Lithium metal electrode

Abstract

Lithium metal electrodes are generally described. There is provided an article for inclusion in an electrochemical cell, comprising: a layer comprising lithium metal; and a passivation layer disposed on the lithium metal-containing layer, in which the passivation layer includes a plurality of columnar structures having an aspect ratio of greater than or equal to 0.5 and less than or equal to 5.

Description

[0001] This application is a divisional application of the Chinese patent application filed on June 17, 2022, with application number 202080088085.7 and invention name “Lithium Metal Electrode”. The international application date of the parent application is December 17, 2020, the international application number is PCT / US2020 / 065584, and the earliest priority date is December 20, 2019.

[0002] Related Applications

[0003] Pursuant to 35 U.S.C. §119(e), this application claims priority to U.S. Provisional Application No. 62 / 952,206, filed on December 20, 2019, entitled “Lithium Metal Electrodes,” U.S. Provisional Application No. 62 / 952,197, filed on December 20, 2019, entitled “Lithium Metal Electrodes and Methods,” and U.S. Provisional Application No. 62 / 952,204, filed on December 20, 2019, entitled “Systems and Methods for Fabricating Lithium Metal Electrodes,” each of which is incorporated herein by reference in its entirety. Technical Field

[0004] The present disclosure generally relates to lithium metal electrodes, modular lithium deposition systems, and associated articles and methods. Background Art

[0005] Lithium metal electrodes are suitable for use in lithium batteries because of their high energy density. However, lithium metal electrodes are often susceptible to undesirable reactions during electrochemical cell manufacturing and cycling. Therefore, there is a need for improved lithium metal electrodes, modular lithium deposition systems, and associated articles and methods. Summary of the invention

[0006] The present disclosure generally relates to lithium metal electrodes, modular lithium deposition systems, and associated articles and methods. The subject matter disclosed herein in some cases relates to related products, alternative solutions to specific problems, and / or a variety of different uses of one or more systems and / or articles.

[0007] In some embodiments, an article for inclusion in an electrochemical cell is provided. The article for inclusion in an electrochemical cell comprises: a layer comprising lithium metal and a passivation layer disposed on the layer comprising lithium metal. The passivation layer comprises boron, phosphorus, antimony, selenium tellurium, hydrogen and / or halogen.

[0008] In some embodiments, an article for inclusion in an electrochemical cell includes: a layer including lithium metal and a passivation layer disposed on the layer including lithium metal. The passivation layer includes a plurality of columnar structures having an aspect ratio greater than or equal to 0.5 and less than or equal to 5.

[0009] In some embodiments, an article for inclusion in an electrochemical cell includes an electroactive layer comprising lithium metal. The layer is porous. The layer also includes boron, phosphorus, antimony, selenium, tellurium, hydrogen, and / or halogen.

[0010] In some embodiments, a method is provided. The method includes exposing a layer comprising lithium metal to a gas to form a passivation layer disposed on the layer comprising lithium metal. The gas includes a substance containing boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogen.

[0011] In some embodiments, a method includes exposing a layer comprising lithium metal to a gas to form a passivation layer disposed on the layer comprising lithium metal. The passivation layer includes a plurality of pillars having an aspect ratio greater than or equal to 0.5 and less than or equal to 1.

[0012] In some embodiments, the method includes depositing an electroactive layer from a plurality of gases, the electroactive layer is porous, the plurality of gases include lithium, and the plurality of gases include a substance including boron, phosphorus, antimony, selenium, tellurium, hydrogen, and / or a halogen.

[0013] In some embodiments, the method includes depositing a layer comprising lithium and / or a reaction product of lithium onto a first portion of a substrate in a first module in a modular lithium deposition system. The layer comprising lithium metal and / or a reaction product of lithium metal is deposited by a gas, a second portion of the substrate in a second module is not exposed to the gas, and the modular lithium deposition system further includes a lithium metal source and a roll-to-roll processing system that passes through the first module and the second module.

[0014] In some embodiments, a method includes depositing a layer comprising lithium onto a substrate from a first lithium metal source, and depositing lithium metal onto the first layer comprising lithium metal from a second lithium metal source to form a final layer comprising lithium metal. The first lithium metal source is contained in a first container, the second lithium metal source is contained in a second container, the final layer comprising lithium metal has a smaller thickness variation in a cross-web direction than the first layer comprising lithium metal, and the method is performed in a vacuum chamber located in a modular lithium deposition system, the modular lithium deposition system also including a roll-to-roll processing system passing through the vacuum chamber.

[0015] Some embodiments relate to a modular lithium deposition system. In some embodiments, the modular lithium deposition system includes a first module, a second module, a lithium source, and a roll-to-roll processing system passing through the first module and the second module. The first module and the second module are configured to be reversibly placed in fluid communication with each other.

[0016] In some embodiments, a modular lithium deposition system includes a plurality of modules, a lithium source, and a roll-to-roll processing system that passes through the plurality of modules. The roll-to-roll processing system includes a plurality of drums configured to translate a substrate through the plurality of modules, each of the plurality of drums being in thermal communication with a cooling system, and the cooling system being configured to maintain each of the plurality of drums at a temperature greater than or equal to -35°C and less than or equal to 60°C.

[0017] In some embodiments, a modular lithium deposition system includes a vacuum chamber, a lithium metal source, and a roll-to-roll processing system passing through the vacuum chamber. The lithium metal source is contained in a container, the container includes a cooling system, the cooling system includes a plurality of cooling channels arranged in one or more walls of the container, and the cooling channels are configured to cool the outer surface of the container to a temperature less than or equal to 50° C. and greater than or equal to 15° C.

[0018] In some embodiments, a modular lithium deposition system includes a vacuum chamber, a lithium metal source, and a roll-to-roll processing system passing through the vacuum chamber. The lithium metal source is contained in a container including a shutter, and the shutter is configured to reversibly place the vacuum chamber and the interior of the container containing lithium in fluid communication with each other.

[0019] In some embodiments, the modular lithium deposition system includes a plurality of modules, a plurality of lithium metal sources, a plurality of wire feeding systems, and a roll-to-roll processing system passing through the plurality of modules. The plurality of lithium metal sources are arranged in a plurality of crucibles thermally connected to the heating system. Each wire feeding system is configured to feed a wire containing lithium into one of the plurality of crucibles.

[0020] In some embodiments, an article for inclusion in an electrochemical cell is provided, comprising: a layer comprising lithium metal; and a passivation layer disposed on the layer comprising lithium metal, wherein the passivation layer comprises a plurality of columnar structures having an aspect ratio greater than or equal to 0.5 and less than or equal to 5.

[0021] In some embodiments, an article for inclusion in an electrochemical cell is provided, comprising: an electroactive layer comprising lithium metal, wherein: the layer is porous, and the layer further comprises boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogens.

[0022] In some embodiments, a method for depositing an electroactive layer is provided, comprising: depositing the electroactive layer from a plurality of gases, wherein: the electroactive layer is porous; the plurality of gases comprises lithium; and the plurality of gases comprises a substance containing boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogens.

[0023] In some embodiments, a modular lithium deposition system is provided, comprising: a first module; a second module; a lithium source; and a roll-to-roll processing system passing through the first module and the second module, wherein the first module and the second module are configured to be reversibly placed in fluid communication with each other.

[0024] In some embodiments, a method is provided, comprising: depositing a layer comprising lithium and / or reaction products of lithium onto a first portion of a substrate in a first module in a modular lithium deposition system, wherein: the layer comprising lithium metal and / or reaction products of lithium metal is deposited by a gas, a second portion of the substrate in a second module is not exposed to the gas, and the modular lithium deposition system further comprises a lithium metal source and a roll-to-roll processing system passing through the first module and the second module.

[0025] In some embodiments, a modular lithium deposition system is provided, comprising: a plurality of modules; a lithium source; and a roll-to-roll processing system passing through the plurality of modules, wherein: the roll-to-roll processing system comprises a plurality of rollers, the plurality of rollers being configured to translate a substrate through the plurality of modules, each of the plurality of rollers being thermally connected to a cooling system, and the cooling system being configured to maintain each of the plurality of rollers at a temperature greater than or equal to -35°C and less than or equal to 60°C.

[0026] In some embodiments, a modular lithium deposition system is provided, comprising: a vacuum chamber; a lithium metal source; and a roll-to-roll processing system passing through the vacuum chamber, wherein: the lithium metal source is contained in a container, the container comprises a cooling system, the cooling system comprises a plurality of cooling channels arranged in one or more walls of the container, and the cooling channels are configured to cool the outer surface of the container to a temperature less than or equal to 50°C and greater than or equal to 15°C.

[0027] In some embodiments, a modular lithium deposition system is provided, comprising: a vacuum chamber; a lithium metal source; and a roll-to-roll processing system passing through the vacuum chamber, wherein: the lithium metal source is contained in a container including an opener and the opener is configured to reversibly place the vacuum chamber and the interior of the container containing lithium in fluid communication with each other.

[0028] In some embodiments, a modular lithium deposition system is provided, comprising: a plurality of modules; a plurality of lithium metal sources, wherein the plurality of lithium metal sources are arranged in a plurality of crucibles thermally connected to a heating system; a plurality of wire feeding systems, wherein each wire feeding system is configured to feed a wire containing lithium into one of the plurality of crucibles; and a roll-to-roll processing system passing through the plurality of modules.

[0029] In some embodiments, a method is provided, comprising: depositing a layer comprising lithium onto a substrate from a first lithium metal source, wherein the first lithium metal source is contained in a first container; and depositing lithium metal from a second lithium metal source onto the first layer comprising lithium metal to form a final layer comprising lithium metal, wherein: the final layer comprising lithium metal has a smaller thickness variation in a cross-web direction than the first layer comprising lithium metal, the second lithium metal source is contained in a second container, and the method is performed in a vacuum chamber located in a modular lithium deposition system, the modular lithium deposition system also comprising a roll-to-roll processing system passing through the vacuum chamber.

[0030] Other advantages and novel features of the present invention will become apparent from the following detailed description of various non-limiting embodiments of the present invention when considered in conjunction with the accompanying drawings. In the event that this specification and a document incorporated by reference include conflicting and / or inconsistent disclosures, this specification shall prevail. If two or more documents incorporated by reference include conflicting and / or inconsistent disclosures relative to each other, the document with the later effective date shall prevail. BRIEF DESCRIPTION OF THE DRAWINGS

[0031] Non-limiting embodiments of the present invention will be described by way of example with reference to the accompanying drawings, which are schematic and are not intended to be drawn to scale. In the drawings, each identical or nearly identical component shown is generally represented by a single reference numeral. For the sake of clarity, not every component is labeled in every drawing, nor is every component of every embodiment of the invention shown, where the illustration is not necessary to enable one of ordinary skill in the art to understand the present invention. In the drawings:

[0032] Figure 1 is a schematic depiction of a modular lithium deposition system according to some embodiments;

[0033] Figure 2 is a schematic depiction of a modular lithium deposition system including a connector between two modules according to some embodiments;

[0034] Figure 3 is a schematic depiction of a modular lithium deposition system including a roll-to-roll processing system according to some embodiments;

[0035] Figure 4is a schematic depiction of a roll-to-roll processing system including two rollers according to some embodiments;

[0036] Figure 5 is a schematic depiction of a drum on which a substrate is conveyed by two rollers according to some embodiments;

[0037] Figure 6 is a schematic depiction of an arrangement of a drum, a substrate, and a shield positioned proximate to the substrate according to some embodiments;

[0038] Figure 7 is a schematic depiction of an arrangement of a drum, a substrate, a shield positioned proximate to the substrate, and two ports configured to introduce a gas, according to some embodiments;

[0039] Figure 8 is a schematic depiction of a source located in a container according to some embodiments;

[0040] Fig. 9 is a schematic depiction of a cooling system including a wall having channels disposed therein, according to some embodiments;

[0041] Fig.10 is a schematic depiction of a container for a source including a shutter according to some embodiments;

[0042] Fig.11 is a schematic depiction of a module including three sources of the same type according to some embodiments;

[0043] Fig.12 is a schematic depiction of a module including a vacuum chamber in which a first roller and a second roller are located according to some embodiments;

[0044] Fig.13 is a schematic depiction of a container including a plurality of sources according to some embodiments;

[0045] Fig.14 is a photograph of multiple sources and a heated crucible according to some embodiments;

[0046] Fig.15 is a schematic depiction of an article including a layer comprising lithium metal according to some embodiments;

[0047] Fig.16 is a schematic depiction of a layer comprising lithium metal according to some embodiments;

[0048] Fig.17 is a schematic depiction of an article including both a layer comprising lithium metal and a layer disposed on the layer comprising lithium metal, according to some embodiments;

[0049] Fig.18 is a schematic depiction of a porous layer according to some embodiments;

[0050] Fig.19 and Fig. 20 is a schematic depiction of an article including a layer including a plurality of columnar structures according to some embodiments;

[0051] Fig.21A and Fig.21B is a schematic depiction of a color space according to some embodiments;

[0052] Fig. 22 is a micrograph of a layer comprising lithium according to some embodiments;

[0053] Figure 23 to Figure 28 is a micrograph of a layer comprising lithium metal after exposure to CO2 according to some embodiments;

[0054] Figures 29 to 34 is a graph showing the chemical composition of a passivation layer according to some embodiments;

[0055] Figure 35 to Figure 37 is a graph showing discharge capacity as a function of cycling of an electrochemical cell according to some embodiments;

[0056] Figures 38 to 43 is a micrograph of a layer comprising lithium metal after exposure to CO2 according to some embodiments;

[0057] Figure 44 to Figure 45 is a micrograph of a layer comprising lithium metal exposed to SO 2 according to some embodiments;

[0058] Figure 46 to Figure 47 is a micrograph of a layer comprising lithium metal exposed to COS according to some embodiments;

[0059] Fig.48 is a micrograph of a layer comprising lithium metal exposed to SF6 according to some embodiments;

[0060] Fig.49 is a micrograph of a layer comprising lithium metal exposed to acetylene according to some embodiments;

[0061] Figure 50 to Figure 53 is a micrograph of a layer formed by gaseous lithium metal and gaseous CO2 according to some embodiments;

[0062] Figure 54 to Figure 56 is a micrograph of a layer formed from gaseous lithium metal and gaseous CO2 in the presence of argon according to some embodiments; and

[0063] Figure 57 to Figure 59is a schematic depiction of a modular lithium deposition system according to some embodiments. DETAILED DESCRIPTION

[0064] Articles containing lithium metal for inclusion in electrochemical cells, methods of forming and / or altering such articles, and modular lithium deposition systems are generally described. In some embodiments, the articles described herein may be suitable for use as lithium metal anodes and / or for use in lithium metal anodes. Similarly, the methods and / or modular lithium deposition systems described herein may be suitable for forming lithium metal anodes and / or components thereof.

[0065] Some systems described herein are suitable for forming articles for inclusion in electrochemical cells in a desired manner. In some embodiments, the system includes two or more modules, each of which is capable of and / or configured to perform one or more manufacturing processes. As an example, the system may include one or more modules capable of and / or configured to deposit a material (e.g., lithium metal, a substance that passivates lithium metal) onto a substrate. As another example, the system may include one or more modules capable of and / or configured to perform a reaction on the article therein (e.g., a passivation reaction is performed on the lithium metal present in the article therein). These modules may be capable of and / or configured to be reversibly placed in fluid communication and non-fluid communication with each other. Advantageously, this can enable separate processes to be performed in separate modules without cross-contamination between the modules, and enable a single article (or a portion of a single article) to be transported to different modules through the system (e.g., different processes and / or subsequent identical processes can be performed in the different modules). In some embodiments, one or more features of the modular system may be advantageous for depositing lithium metal. These features are described in more detail below.

[0066] In some embodiments, the article for inclusion in the electrochemical cell comprises lithium metal and further comprises one or more passivating substances. The passivating substance can passivate the lithium metal, thereby reducing the reactivity of the lithium metal. There are several time points during which the lithium metal is expected to be passivated. As an example, when subjected to one or more other manufacturing processes, it may be expected that the lithium metal is passivated, and the one or more other manufacturing processes expose the lithium metal deposited during the previous manufacturing process to a substance reactive with the lithium metal. As another example, in some embodiments, when the lithium metal is present in the electrochemical cell being cycled, it may be expected that the lithium metal is passivated. During these processes, the passivated lithium metal may be ideally less reactive and more stable than the unpassivated lithium metal. For this reason, when all other factors are the same, the chemical reaction may lose less lithium metal than the electrochemical cell without passivated lithium, so that less lithium metal can be used. Additionally or alternatively, the use of passivated lithium can lead to the formation of an electrochemical cell including a lower level of non-functional substances.

[0067] Some embodiments relate to methods of forming articles for inclusion in electrochemical cells and / or to methods of using the modular deposition systems described herein. Such methods can advantageously result in the formation of a lithium metal-containing layer having a desired type and / or amount of passivation, arrangement of passivating species, morphology, and / or other chemical and / or physical characteristics of interest.

[0068] Figure 1 A non-limiting example of a modular lithium deposition system is shown. Figure 1 , the modular lithium deposition system 100 includes a first module 200 and a second module 250. In some embodiments, the first module and the second module may be capable of and / or configured to be reversibly placed in fluid communication with each other. Figure 2 A non-limiting example of a modular lithium deposition system 102 having this feature is shown, where a connector 302 (e.g., an electrically conductive seal; a valve, such as a gate valve) is located between the first module 202 and the second module 252 and is capable of reversibly placing the modules in fluid communication with each other. The valve (or other portion of the modular lithium deposition system capable of placing the two modules in fluid communication with each other) can be opened to allow a substrate on which an article for inclusion in an electrochemical cell is being formed to pass between the modules, and the valve can be closed to fluidly isolate the modules from each other.

[0069] In some embodiments, Figure 1As in the exemplary embodiment shown in the figure, the modular lithium deposition system includes two modules. The modular lithium deposition system may also include three modules, four modules, or even more modules. Such modules may include two or more modules that are identical to each other and / or may include two or more modules that are different from each other.

[0070] A variety of suitable modules may be included in the modular lithium deposition system described herein. In some embodiments, the modular lithium deposition system includes one or more modules, and the one or more modules include a vacuum chamber. The vacuum chamber may be a vessel capable of maintaining an indefinite period of time under a vacuum of less than or equal to 1 millitorr. It may be formed by a material and / or a combination of materials that can withstand a relatively large pressure difference between the inside of the vacuum chamber and the outside of the vacuum chamber (e.g., the pressure difference between atmospheric pressure and 1 millitorr). Similarly, it may be formed by a material and / or a combination of materials that can seal the inside of the vacuum chamber relative to the environment outside the vacuum chamber to a perceptible degree (e.g., so that the pressure difference between atmospheric pressure and the pressure inside the vacuum chamber can be maintained for a period of seconds, minutes, hours or longer without pumping and / or with minimal pumping). The vacuum chamber may be made of a rigid material and / or a combination of materials (e.g., a material and / or a combination of materials that maintains substantially the same shape when subjected to the above-mentioned pressure difference) and / or a deformable material and / or a combination of materials (e.g., a material and / or a combination of materials that do not maintain substantially the same shape when subjected to the above-mentioned pressure difference).

[0071] In some embodiments, the vacuum chamber also includes one or more other system components (e.g., within a module, in another module), and / or can be placed in fluid communication with one or more other system components. Such a vacuum chamber may be advantageous for a system in which it is desired to perform one or more processes in the vacuum chamber that require more than just exposure to a vacuum. For example, in some embodiments, the vacuum chamber may also include a source of material to be deposited on a substrate and / or a source of material reactive with the substrate and / or the material deposited on the substrate, and / or can be placed in fluid communication with the above-mentioned sources. The vacuum chamber may be capable of and / or configured to be placed in fluid communication with other system components when maintained under reduced pressure. This is advantageous for, for example, a process in which it is desired to deposit a material onto a substrate located in the vacuum chamber under reduced pressure and / or it is desired to perform a reaction on a material located in the vacuum chamber under reduced pressure.

[0072] Some modular lithium deposition systems described herein are capable of and / or configured to operate in a roll-to-roll manner. Advantageously, this mode of operation can enable the use of modular lithium deposition systems in a more efficient manner. As an example, in some embodiments, the roll-to-roll operation of a modular lithium deposition system enables two (or more) different modules to perform two (or more) different processes on two (or more) different parts of a substrate at the same time. This can enable different substrates to be manufactured efficiently because they can be sequentially passed through modules that operate simultaneously. As another example, in some embodiments, the roll-to-roll operation of a modular lithium deposition system can enable a single module to perform processes on different parts of a substrate sequentially while minimizing the exposure of the module to its external environment. When the substrate is translated through the module, the module may only need to be exposed to the environment outside it, and in an embodiment where the entire roll-to-roll processing system is located in a vacuum chamber or other desired environment, the environment to which the module is exposed during the process can be relatively similar to the environment during the process in which the module is configured to perform (e.g., it can be a vacuum environment, which may lack and / or only include one or more components that are not desired in the earth's atmosphere in small amounts, such as substances that are reactive with lithium metal).

[0073] Figure 3 An example of a modular lithium deposition system including a roll-to-roll processing system is shown. Figure 3 , the roll-to-roll processing system 504 includes a first roller 604, a second roller 654, and a chamber 704 located between the first module and the second module. The roll-to-roll processing system can be capable of conveying a substrate from a first roller and / or be configured to unwind a substrate from a first roller, convey it through the system (e.g., through the modules, through any chambers located between the modules), and wind it onto a second roller. The substrate can be long enough that it can simultaneously include a portion disposed on a first roller, a portion located in one or more modules of the modular lithium deposition system, and a portion disposed on a second roller. Thus, as described above, different portions of the substrate can be located in different environments and / or different processes can be performed on different portions of the substrate simultaneously. In some embodiments, the rollers of the roll-to-roll processing system can be located outside of a module in a lithium deposition system (e.g., such as Figure 3 In other embodiments, one or more rollers in the roll-to-roll processing system are located inside a module. As an example, the rollers can be located inside a vacuum chamber. In some embodiments, a first roller is located inside a first module and a second roller is located inside a second different module.

[0074] As used herein, when a component is referred to as being "on" or "adjacent" another component, it can be directly on or directly adjacent to the component, or intervening components may also be present. A component "directly on," "directly adjacent to," or "in contact with" another component means that there are no intervening components.

[0075] In some embodiments, the roll-to-roll processing system further comprises a plurality of rollers. The roll-to-roll processing system can be configured such that it is configured to pass the substrate over the rollers as the substrate is transported through the modular lithium deposition system. For example, the rollers can be configured to translate the substrate through the modular lithium deposition system and / or a plurality of modules in the system. The roll-to-roll processing system can also include rollers configured to translate the substrate through the modular lithium deposition system (e.g., in combination with and / or in place of the rollers). Figure 4 A non-limiting example of a roll-to-roll processing system is shown, which includes two rollers, one roller in each module. Figure 4 8, the first chamber 206 includes a drum 806, and the second chamber 256 includes a drum 856. It should also be understood that some modules may lack drums and / or rollers, and some modules may include two or more drums and / or two or more rollers. Figure 5 Another example of a drum 808 is shown over which a substrate 908 passes via two rollers 1008 and 1058. The rollers and / or drums may be configured to rotate to translate the substrate forward and / or backward.

[0076] Some rollers may be able to and / or configured to be cooled and / or heated. The cooled or heated roller may then cool or heat any portion of the substrate arranged thereon. This may be advantageous for rollers located in the following environment, which, if not able to and / or not configured to be cooled and / or heated, may be heated or cooled by their surroundings to a temperature that is undesirable for the portion of the substrate arranged thereon and / or configured to be arranged thereon. For example, the surroundings in the module where the roller is located may be heated by the process performed therein. As an example, a module in which a layer is deposited by a gas may be heated by a gas and / or a solid source (heated to form a gas) of a substance that forms the gas. For various reasons, it may not be desirable to heat the substrate to the same temperature. For example, heating the substrate to the same temperature may undesirably cause the substrate with a low melting point to melt and / or cause a thermally unstable substrate to begin to degrade. As another example, it may be easier to condense the gas to form a layer on a cooled substrate, and / or the cooled substrate may help form a layer containing a gas with a desired morphology.

[0077] Cooling and / or heating the drum can be achieved by using a cooling and / or heating system that is thermally connected to the drum. The cooling and / or heating system can be configured to remove heat from the drum and / or provide heat to the drum. In some embodiments, the cooling and / or heating system can be configured to maintain the drum at a set temperature, within 1 ° C of the set temperature, or within a range that is less than or equal to the resolution of the temperature sensor used by the cooling and / or heating system. Cooling and / or heating the drum can be achieved by a variety of suitable types of cooling systems, including a system that circulates a cooled and / or heated fluid through one or more surfaces of the drum and / or through one or more walls of the drum. In some embodiments, the drum is heated by a heating system that uses resistive heating. The cooling and / or heating system can also include a temperature sensor (e.g., as part of a feedback loop configured to maintain the cooling and / or heating system at a set temperature and / or within a set temperature range). Non-limiting examples of suitable temperature sensors include thermocouples and RTD sensors. Each roller in the modular lithium deposition system can be independently cooled and / or heated by a different cooling and / or heating system, or two or more (or all) rollers in the modular lithium deposition system can be cooled and / or heated by a common cooling and / or heating system. Similarly, each roller in the modular lithium deposition system can be cooled and / or heated to a different temperature, or two or more (or all) rollers in the modular lithium deposition system can be cooled and / or heated to a common temperature.

[0078] In some embodiments, one or more features other than the roller can help maintain the substrate at a desired temperature. As an example, the substrate can be cooled and / or heated by being exposed to a gas having a temperature lower than or higher than the substrate. For example, the temperature of the substrate can be changed by being exposed to an inert gas. An inert gas can be provided simultaneously with a gas provided at a temperature higher than the substrate temperature, such as a gas that can condense on the substrate to form a layer arranged on the substrate. When exposed to the substrate, it can have a temperature lower than the temperature of the substrate surface exposed thereto, or can have a temperature similar to or higher than the temperature of the substrate surface exposed thereto. In the former case, the inert gas can directly cool the substrate. In the latter, the inert gas can cool the gas provided therewith, which can reduce or eliminate any thermal damage to the substrate caused by being exposed to the gas. As described in more detail elsewhere herein, exposing the substrate to both an inert gas (e.g., an inert gas for cooling) and another gas simultaneously can have other advantages.

[0079] In some embodiments, as another example of a feature of a module that can help maintain the substrate at a desired temperature, a shield is positioned proximate the substrate (and / or the location where the substrate is configured to be located, such as a drum). In some embodiments, the shield can be located between the substrate or the location where the substrate is configured to be located (e.g., a drum) and a heat source (e.g., a container containing a source and / or a source (e.g., a source of lithium metal and / or a source of gas)). Figure 6 One non-limiting embodiment of an arrangement of a drum 810, a substrate 910, and a shield 1110 positioned proximate to the substrate 910 is shown. The shield can restrict the flow of any gas between the shield and the substrate and / or can tend to maintain a relatively constant atmosphere at that location. Thus, the cooling gas introduced into the space between the shield and the substrate can be used to cool the substrate for a considerable period of time and / or can block the introduction of hotter substances therein. Figure 7 As shown in , in some embodiments, a cooling gas (e.g., a cooling inert gas) can be introduced into the space through one or more ports. Figure 7 , ports 1212 and 1262 are configured to introduce cooling gaseous species into a space 1312 between substrate 912 and shield 1112. The ports may be in fluid communication with a source of cooling gas and may be capable of reversibly placing the source of cooling gas in fluid communication with the space between the substrate and shield.

[0080] The shield may also be configured so that one or more other substances may be introduced into the space between the shield and the substrate. As an example, as described in more detail elsewhere herein, the shield may have an opening positioned proximate to a source and / or positioned proximate to a shutter of a container including a source.

[0081] In some embodiments, the modular lithium deposition system includes a source of one or more materials configured to be introduced into one or more modules in the system. Such a source can be located in one or more modules in the module (e.g., in a vacuum chamber), outside the module (e.g., in a position that can be reversibly placed in fluid communication with a module and / or its components (e.g., a vacuum chamber), and / or can form their own module (e.g., in a module that can be reversibly placed in fluid communication with another module and / or its components (e.g., a vacuum chamber). In some embodiments, the source is located in a container (e.g., a container located in one or more of the above positions). Figure 8 One non-limiting embodiment of source 1414 positioned within container 1514 is shown.

[0082] Some sources may include a substance that is configured to be incorporated into a layer deposited therein and / or configured to undergo a reaction in the module to form a reaction product to be incorporated into a layer deposited therein. Non-limiting examples of such sources include a source of lithium metal and a source of a substance reactive with lithium metal. The source of lithium metal may be suitable for forming a layer (e.g., a passivation layer) containing lithium metal and / or its reaction products, and the source of a substance reactive with lithium metal may be configured to form a layer (e.g., a passivation layer) disposed on the lithium metal and / or containing the reaction products of the lithium metal.

[0083] Some sources may include materials that are not configured to be incorporated into a layer deposited therein, or are configured not to undergo a reaction in a module to form a reaction product to be incorporated into a layer deposited therein. As an example, some sources may be sources of gases that are inert to lithium metal and / or gases that are generally considered to be inert gases (e.g., argon, helium, other rare gases). Such gases may be configured to regulate the interaction of one or more other types of gases (e.g., gases containing lithium, gases reactive with lithium) with each other and / or with one or more components of the module. For example, as described above, in some embodiments, an inert gas may help cool one or more parts of a module. As another example, an inert gas may affect the morphology of one or more layers deposited on a substrate. Without wishing to be bound by any particular theory, it is believed that an inert gas may interact with a gas containing lithium and / or a gas containing a substance reactive with lithium to reduce the tendency of these gases to form a porous layer and enhance the tendency of these gases to form a denser, more crystalline layer. It is believed that this effect is enhanced when the inert gas has a temperature sufficient to cool the associated gases deposited to form the layer (e.g., the gas is provided at a lower temperature than these gases). It is also believed that this effect is enhanced when the inert gas is present in a manner sufficient to cause the local pressure at the location where the associated layer is deposited to have characteristics that promote the formation of such a layer.

[0084] Some sources and / or their containers may be configured to be heated and / or cooled. When the source is a material that is not gaseous when provided (e.g., solid or liquid at room temperature and pressure, solid or liquid at the temperature and pressure of the module into which it is introduced) but is desired to be introduced into the module in gaseous form and / or deposited on the substrate by gas, it may be advantageous to heat the source. The source may be heated by a heating system that is thermally connected thereto. The heating system may resistively heat the container in which the source is located and / or the location where the substrate is arranged. In some embodiments, the heating system may heat the container and / or location by providing a heat source at a set temperature (or within 1°C of the set temperature, or within a range of a difference of less than or equal to the resolution of the temperature sensor used by the cooling and / or heating system) in a manner that maintains the source at a set temperature (or within 1°C of the set temperature, or within a range of a difference of less than or equal to the resolution of the temperature sensor used by the cooling and / or heating system). It should also be understood that, as described elsewhere herein, some modules may include one or more sources of materials that are provided as gases (e.g., materials that are gases at room temperature and pressure, materials that are gases at the temperature and pressure of the module into which they are introduced). Such sources may be provided in addition to or in lieu of sources of materials that are not provided as gases.

[0085] When it is desired to operate the modular lithium deposition system at a high speed and / or when it is desired to have a relatively short time between its continuous use, it may be advantageous to cool the source. When the source is at an elevated temperature, it may evaporate and / or sublimate to form a gas, which will not be expected to be introduced into the environment outside the environment where the source is located, such as the environment outside the module and / or its parts (e.g., vacuum chamber) where the source is located. For example, it may not be expected that the molten lithium is placed in fluid communication with the environment outside the module, because the molten lithium may have undesirable reactivity and / or undesirable volatility. Therefore, the ability of the source (e.g., a source comprising lithium) to be rapidly cooled to the temperature at which it experiences minimum evaporation and sublimation can make it possible to place the modules in rapid fluid communication with each other and / or place the modules in fluid communication with the atmosphere after performing a process in which a source in a chamber in the chamber is heated. The source can be cooled by its container (e.g., when its container includes a cooling system and / or is thermally connected to the cooling system). As with a cooling system that can be used to cool one or more rollers, a cooling system that is configured and / or capable of cooling a container for a source can be configured to maintain one or more portions of the container (e.g., one or more outer surfaces of the container, one or more inner surfaces of the container) at or within 1°C of the set temperature and / or within a range from the set temperature that is less than or equal to the resolution of a temperature sensor employed by the cooling and / or heating system.

[0086] Note that some modular lithium deposition systems may include separate cooling and heating systems associated with sources therein (e.g., both a heating system configured to heat the source and a separate cooling system configured to cool the source), and some modular lithium deposition systems may include heating systems and cooling systems capable of and / or configured to operate together to maintain the source at a set temperature.

[0087] In some embodiments, the cooling system of the container for the source includes a plurality of channels arranged in one or more walls and / or arranged across one or more surfaces of the container. A cooling fluid can flow through these channels (e.g., by means of a pump and / or possibly cooled by a cooler), which can cool the container, one or more outer surfaces and / or inner surfaces of the container, and / or the source contained in the container (e.g., by contacting the cooled inner surface of the container). Non-limiting examples of suitable cooling fluids include cooling gases (e.g., cooling inert gases, such as cooling argon, cooling helium, and / or another cooling rare gas) and cooling liquids (e.g., cooling water). In some embodiments, the cooling fluid can be a fluid that does not have a boiling point between the temperature at which it is provided to the channel and the temperature of the source (e.g., the cooling fluid can be provided as a gas and remain as a gas after flowing through the channel, the cooling fluid can be provided as a liquid and remain as a liquid after flowing through the channel).

[0088] Fig. 9 One non-limiting embodiment of a cooling system 1516 is shown, which includes a wall 1616 having a channel 1716 disposed therein. Fig. 9 As with the containers shown in , some containers may include channels in all of their walls. Other containers may include channels in some but not all of their walls. For example, some containers may include channels only in one or more walls that are directly adjacent to the source. Similarly, it should be understood that Fig. 9 The number of channels in each wall, the positioning of the channels within the walls, and the size of the channels relative to the walls shown in FIG. 1 are exemplary, and some embodiments may be different in these (and / or other) ways. Fig. 9 The embodiments shown by way of example are different.

[0089] Some containers suitable for containing sources have one or more features that make the container well suited for use with a lithium metal source and / or other sources having the features described herein. For example, in some embodiments, the container is formed of a material that has a relatively low coefficient of thermal expansion between room temperature and the typical temperature to which the container is heated, has a relatively high hardness, and / or has a relatively high toughness. Steel is an example of a suitable material having these properties.

[0090] As another example, in some embodiments, the container includes a shutter that can and / or is configured to reversibly place the source in fluid communication with another module and / or another component of the module in which the source is located (e.g., by opening and closing). The module can include a vacuum chamber and a source positioned in a container located within the vacuum chamber, and the shutter can be capable of reversibly placing the source in fluid communication with the vacuum chamber. Fig.10 One non-limiting embodiment of a container for a source including a shutter having this feature is shown. Fig.10 In the embodiment, the container 1518 includes a shutter 1818, which can be reversibly opened and closed to place the interior of the container 1518 in fluid communication with the environment outside the container 1518 and out of fluid communication with the environment outside the container 1518.

[0091] In some embodiments, and Fig.10 As in the embodiment exemplarily shown in , the shutter that opens and closes the container can place the entire interior of the container (where the source is located) in fluid communication with another module and / or module component and remove it from fluid communication with another module and / or module component. The opening and closing of the shutter can also place one or more sub-portions of the interior of the container (e.g., the portion where the lithium metal source is located and / or the portion in fluid communication with it) in fluid communication with another module and / or module component and remove it from fluid communication with another module and / or module component, while not affecting the presence or absence of fluid communication between one or more other portions of the interior of the container and another module and / or module component. The presence of the shutter can make it possible to control the exposure of the source to another module and / or module component, so that the source is in fluid communication with another module and / or module component when needed (e.g., when the source is at a temperature suitable for forming a gas to be introduced into the module and / or module component, when the substrate is properly positioned to receive and / or react with a gas generated by the source), and is not in fluid communication with another module and / or module component at other points in time (e.g., when the source is at a temperature that is too low to form a desired gas in an appropriate amount and / or with a desired composition). This can advantageously prevent or reduce the introduction of gas from the source at inappropriate times, thereby preventing or reducing the amount of substrate that behaves as unsuitable for introduction into an electrochemical cell and / or unsuitable for further manufacturing steps.

[0092] In some embodiments, the shutter is configured to be heated. For example, it can be heated by a heating system in thermal communication therewith. The heating system can resistively heat the shutter and / or can provide a heat source at a set temperature (or within 1°C of the set temperature and / or within a range of a difference from the set temperature that is less than or equal to the resolution of the temperature sensor used by the heating system) in a manner that maintains the shutter at a set temperature (or within 1°C of the set temperature and / or within a range of a difference from the set temperature that is less than or equal to the resolution of the temperature sensor used by the heating system).

[0093] Some modular lithium deposition systems and / or modules therein may include more than one source. Each source may be of the same type, each source may be of a different type, or a modular lithium deposition system and / or module may include two or more of at least one type of source, and also include one or more other different types of sources. In some embodiments, it may be advantageous for a single module to include multiple sources of the same type. Different sources of the same type may complement each other. As an example, in some embodiments, a module includes multiple sources at different locations within the module and / or multiple ports at different locations around the module, each of which places the source in fluid communication with the module. Multiple sources can help together form layers from the source and / or layers in a uniform manner to react with gases generated by the source (e.g., having a change in the cross web direction of less than or equal to 0.5 microns between its thickest point and its thinnest point).

[0094] Fig.11 An example of a module comprising three sources of the same type is shown. Fig.11 In the embodiment, module 220 includes vacuum chamber 1920, drum 820, first lithium metal source 1420, second lithium metal source 1450 and third lithium metal source 1480. The three lithium metal sources 1420, 1450 and 1480 are located in vacuum chamber 1920, which also includes drum 820. Although not shown in FIG. Fig.11 However, it should be understood that Fig.11 The three ports configured to reversibly place the three lithium metal sources in fluid communication with the interior of the vacuum chamber at the same location as the three lithium metal sources shown in FIG. 1 are expected to be similar to Fig.11 The embodiment shown in FIG.

[0095] exist Fig.11In the present invention, a portion of a substrate that is passed through a roller (e.g., thereby and / or by means of a modular lithium deposition translation with the aid of multiple rollers) can be sequentially exposed to a gas from a second lithium metal source, exposed to a gas from a first lithium metal source, and then exposed to a gas from a third lithium metal source. If sources are used to deposit a layer on a substrate, a large portion of the layer can be deposited by a gas from one of the three sources (e.g., the first source), and the other two sources can be used to deposit other portions of the layer that enhance its uniformity (e.g., reduce its thickness, chemical composition, and / or porosity variation in the cross-web direction). For example, the gas from the last source to which a portion of the substrate is exposed can adjust the amount of material it deposits based on the amount of material that has been deposited on the portion of the substrate to which it is exposed. It can deposit more material on portions of the substrate where a smaller amount of material has been deposited, and deposit less (or no) material on portions of the substrate where a larger amount of material has been deposited. If not the primary source, the gas from the first source to which the substrate is exposed may deposit more material on portions of the substrate on which the primary source typically deposits less material (e.g., portions of the substrate closer to the edge of the primary source), and deposit less (or no) material on portions of the substrate on which the primary source typically deposits more material (e.g., portions of the substrate closer to the center of the primary source).

[0096] In some embodiments, Fig.11 As with the embodiment shown in , multiple sources (e.g., multiple sources of the same type) can be located around a common drum and / or can be configured to produce gases to be deposited to form a layer on portions of a substrate disposed on a common drum. Multiple sources in a single module can also be positioned near different drums in the module and / or configured to produce gases to be deposited to form layers on portions of substrates disposed on different drums in the module. Fig.12 One example of a module 222 is shown that includes a vacuum chamber 1922 in which are positioned a first roller 822 and a second roller 872. The module 222 also includes a source 1422 positioned proximate the first roller 822 and a second source 1452 of the same type positioned proximate the second roller. Portions of the substrate 922 that translate through the module 222 to first pass through the first roller 822 and then through the second roller 872 will first be exposed to gas originating from the first source 1422 and then to gas originating from the second source 1452.

[0097] In some embodiments, Figure 11 to Figure 12As in the embodiment shown in , each source in the module is contained in its own container. The amount of gas introduced into the module from the source can be controlled by the container (e.g., by opening and closing a shutter on the container, by adjusting the temperature of the container) and / or by a port in fluid communication with the container. A module can also include two or more sources in a common container and / or in fluid communication with a common port. Fig.13 An example of multiple sources with this characteristic is shown. Fig.13 , a single container 1524 includes multiple sources 1424. In some such embodiments, the amount of gas introduced into the module from different sources located in a common container can be independently controlled. This can be achieved by, for example, providing different amounts of heat to different sources (thereby adjusting the temperature, evaporation rate, and / or sublimation rate of the sources differently) and / or by heating different amounts of the sources (thereby limiting the amount of source material that can evaporate and / or sublime). The amount of source that is heated can be varied by varying the amount of source exposed to the heat source. As described above with respect to Figure 11 to Figure 12 As with the described embodiments, the amount of gas produced by any particular source can be selected so that all of the sources together result in the production of gas that is deposited on the substrate in the form of a relatively uniform layer (e.g., having a variation in the cross-web direction of less than or equal to 0.5 microns between its thickest and thinnest points).

[0098] In an exemplary embodiment, a source including multiple parts is provided in the form of a material, and the multiple parts can be relatively easily translated onto a heated crucible. The rate at which the various parts of the source are translated onto the heated crucible can affect the amount of the source that is sublimated and / or evaporated by the heat source. For example, when the various parts of the source are introduced into the heated crucible more quickly, a larger amount of gas can be produced from the source, and when the various parts of the source are introduced into the heated crucible more slowly, a smaller amount of gas can be produced from the source. A type of source that may be particularly suitable for this design is a source in the form of a wire. The wire can initially be wound around a roller and then unrolled onto a heated crucible. Fig.14 One example of multiple sources and heated crucibles having this design is shown.

[0099] In some embodiments, the modular lithium deposition system includes a combination of different types of sources and / or ports that are positioned relative to each other and are in communication with different types of source fluids to facilitate the formation of a desired combination of layers. As an example, in some embodiments, the modular lithium deposition system includes one or more sources of materials other than lithium metal (e.g., reactive with lithium metal) positioned near a source of lithium metal. Similarly, the modular lithium deposition system may include ports that are in communication with one or more source fluids of materials other than lithium metal (e.g., reactive with lithium metal) positioned near a source of lithium metal. Such sources and / or ports may be capable of and / or configured to introduce two types of gases into a common portion of a substrate at a relatively close time point (e.g., simultaneously or nearly simultaneously). When the two sources are simultaneously placed in communication with the internal fluid of the module, a layer containing both reaction products and / or lithium therebetween and condensed gases other than lithium can be deposited on the portion of the substrate.

[0100] As another example, in some embodiments, the modular lithium deposition system includes one or more sources of materials other than lithium metal (e.g., reactive with lithium metal) positioned at an appreciable distance from the source of lithium metal. Similarly, the modular lithium deposition system may include a port connected to one or more source fluids of materials other than lithium metal (e.g., reactive with lithium metal) positioned at an appreciable distance from the source of lithium metal. Such a source and / or port may be capable of and / or configured to introduce two types of gases to a common location at different time points. This may be suitable for embodiments in which two different layers are deposited from two different sources. For example, in some embodiments, a layer containing lithium metal may be deposited first, and then the layer containing lithium metal may be exposed to a gas of a material other than lithium metal. The gas may react with the layer containing lithium metal and / or be deposited on the layer containing lithium metal to form a layer arranged on the layer containing lithium metal, such as a passivation layer.

[0101] In some embodiments, the modular lithium deposition system includes one or more components in addition to the components described above. As an example, in some embodiments, the modular lithium deposition system includes one or more sensors. The sensor can be located in one or more modules in the module. For example, in some embodiments, the sensor is located in a vacuum chamber as a module and / or located in a module. The sensor can be configured to sense one or more characteristics of the modular lithium deposition system, the modules in the system, and / or the layers deposited in the system (e.g., a layer containing lithium metal, a layer containing a substance other than lithium metal, a passivation layer). Non-limiting examples of the characteristics of the modules in the lithium deposition system that can be sensed include temperature and the amount of various gases present. Non-limiting examples of the characteristics of the layers that can be sensed include conductivity, capacitance, color, reflectivity, and thickness. Non-limiting examples of suitable sensors for sensing these (and / or other) characteristics include temperature sensors, conductivity sensors (e.g., rolling four-point probe sensors), capacitance sensors, optical sensors, and thickness sensors (e.g., eddy current sensors, time of flight sensors).

[0102] Advantageously, in some embodiments, the modular lithium deposition system can be configured to enable adjustment of one or more characteristics of a module in the modular lithium deposition based on characteristics sensed by one or more sensors (e.g., based on a feedback system). For example, a sensor can sense a characteristic indicating a layer that includes too much or too little of any particular substance (e.g., lithium metal, a substance other than lithium metal), is deposited too quickly or too slowly, and / or has an undesirable morphology. The sensor can output a signal indicating the relevant defect to an operator of the modular lithium deposition system and enable the operator to adjust one or more characteristics of the relevant module to compensate for it, and / or can cause the modular lithium deposition system to self-adjust to do so. Non-limiting examples of parameters that can be adjusted by an operator and / or by the modular lithium deposition system in response to characteristics sensed by sensors include: the flow rate of gas entering a module in which the relevant layer is being deposited (e.g., from a source), the temperature of one or more locations (e.g., the temperature of a container holding the source, the temperature of the location where the source is located, the temperature in a vacuum chamber in which the relevant layer is being deposited, the temperature of a roller on which the substrate on which the relevant layer is being deposited is arranged), the state of a shutter (e.g., open, closed), and the speed at which a substrate passes through a relevant module (e.g., through a vacuum chamber in a module).

[0103] Another example of another component that the modular lithium deposition system may include is a module (e.g., an oxygen plasma source) configured to generate oxygen plasma. The module may include a vacuum chamber, and the vacuum chamber may be configured to generate oxygen plasma (e.g., by allowing a controlled flow of oxygen to enter the vacuum chamber and applying a high-frequency voltage to the oxygen). In some embodiments, oxygen plasma may be particularly useful for cleaning a substrate and / or increasing the adhesion of a substrate to a layer deposited thereon before depositing a layer on the substrate. To this end, it may be advantageous to position the module configured to generate oxygen plasma so that a substrate passing through the modular lithium deposition system passes through a module configured to generate oxygen plasma before entering a module configured to deposit one or more layers on the substrate.

[0104] Some embodiments relate to articles for inclusion in an electrochemical cell, such as those that can be manufactured in a modular lithium deposition system described herein. In some embodiments, the article for inclusion in an electrochemical cell includes a layer comprising lithium metal. Fig.15 An example of an article having this property is shown. Fig.15 In the embodiment of the present invention, the article 2026 includes a layer 2126 containing lithium metal. The article suitable for inclusion in an electrochemical cell and containing lithium metal may also include one or more additional substances. The additional substances may be located in the layer containing lithium metal and / or may be located at a position other than the layer containing lithium metal. Fig.16 An example of an article having the former property is shown, and Fig.17 An example of an article having the latter property is shown.

[0105] exist Fig.16 , layer 2228 contains both lithium metal and another non-lithium metal species. The non-lithium metal species can passivate the lithium metal. For this reason, a layer containing both lithium metal and another non-lithium metal species can be understood as "bulk passivated," or containing a species that passivates lithium dispersed throughout the bulk of the layer.

[0106] exist Fig.17 In the embodiment, the article 2030 includes a layer 2130 containing lithium metal and a layer 2330 disposed on the layer containing lithium metal and containing a substance other than lithium metal. In some embodiments, the layer disposed on the layer containing lithium metal is a layer that passivates the layer containing lithium metal. That is, it can be a passivation layer. For this reason, the layer containing lithium located below the layer can be understood as "surface passivated", or passivated at its surface.

[0107] When the layer contains both lithium metal and substances other than lithium metal, the lithium metal component and substances other than lithium metal can be located in the layer in a variety of suitable ways. In some embodiments, lithium metal and one or more substances other than lithium metal form a single phase (e.g., alloy) together. One or more substances other than lithium metal can also be separated from the phase containing lithium metal (e.g., with the phase containing pure lithium metal, with the phase containing lithium metal alloy). The phase other than the phase containing lithium metal can contain ceramics. Two or more phases can be distributed in the layer so that they form a relatively uniform mixture (e.g., so that when the density of each phase is evaluated on a length scale of tens of nanometers, hundreds of nanometers and / or microns, each phase is relatively uniformly distributed throughout the layer). Two or more phases can also be distributed in the layer so that they do not form a relatively uniform mixture (e.g., so that when the density of each phase is evaluated on a length scale of tens of nanometers, hundreds of nanometers or microns, one or more parts of the layer are enriched in one of these phases and / or insufficient in one of these phases).

[0108] The layer containing both lithium metal and a substance other than lithium metal can be electroactive as a whole. That is, if the layer as a whole is appropriately stimulated, the lithium metal in the layer can be able to and / or configured to undergo a redox process. For example, in some embodiments, a layer containing both lithium metal and a substance other than lithium metal can be configured to be placed in an electrochemical cell, and the lithium metal in the layer can be configured to act as an anode and / or as a component of an anode, which anode or a component of an anode undergoes an oxidation process during discharge and / or undergoes a reduction process during charging. Such a layer may include an electroactive portion (e.g., a portion containing lithium metal) and a non-electroactive portion. The non-electroactive portion may include a ceramic (e.g., as described above).

[0109] The layer comprising lithium metal can have a variety of suitable morphologies. Some layers comprising lithium metal (e.g., a layer consisting of and / or consisting essentially of lithium metal, and a layer further comprising one or more non-lithium metal substances) can be relatively dense and / or non-porous. Some layers comprising lithium metal (e.g., a layer consisting of and / or consisting essentially of lithium metal, and a layer further comprising one or more non-lithium metal substances) can include pores. Fig.18 A non-limiting example of an article 2032 is shown, which includes a layer 2232 containing lithium metal and non-lithium metal substances. Fig.18 As can be seen in FIG. 2 , the layer 2232 containing lithium metal and non-lithium metal substances includes a plurality of pores 2432. Some layers containing lithium metal and including a plurality of pores, Fig.18, including pores that are open pores (i.e., pores that are in communication with an ambient fluid external to the layer containing lithium metal). Similarly, some layers containing lithium metal and including a plurality of pores, as exemplarily shown in Fig.18 As with the types of layers shown in , the porous layer containing lithium metal includes pores that are closed pores (i.e., pores that are not in communication with an ambient fluid external to the layer containing lithium metal, such as some pores in the bulk of the layer). Some open pores may extend through the thickness of the layer containing lithium metal, while some open pores may not extend through. The porous layer containing lithium metal may include all of the above types of pores, include some of the above types of pores but lack other types of pores, and / or include pores of types other than those described above.

[0110] Similarly, a layer disposed on the layer containing lithium metal (eg, a layer containing a substance other than lithium metal, a passivation layer) may also have a variety of suitable morphologies. In some embodiments, the layer disposed on the layer containing lithium metal includes a plurality of columnar structures. Fig.19 An example of an article 2034 is shown, which includes a layer 2134 including lithium metal and a layer 2334 including a plurality of columnar structures 2534 disposed on the layer 2134. When present, the plurality of columnar structures can constitute the entire layer (e.g., as Fig.19 ), or the layer may also include one or more components that are not columnar. When present, the plurality of columnar structures may include columnar structures that are topologically contacted with each other by a layer arranged on a layer comprising lithium metal. As an example, refer to Fig.19 , columnar structures 2534A and 2534B are topologically in contact with each other on top of a layer disposed on a layer comprising lithium metal. Such embodiments may also include columnar structures that are not topologically in contact with any other columnar structure through a layer disposed on a layer comprising lithium metal (e.g., Fig.19 In some embodiments, the layer disposed on the layer comprising lithium metal lacks a columnar structure that is topologically in contact with other columnar structures through the layer.

[0111] The columnar structure present in a layer disposed on a layer containing lithium metal (e.g., a layer containing a substance other than lithium metal, a passivation layer) can have a morphology that can be characterized by one or more of the regions described in a Thornton diagram. For example, in some embodiments, the layer disposed on the layer containing lithium metal includes a porous structure having a morphology consistent with region I of the Thornton diagram (e.g., including conical crystallites separated by voids), region T of the Thornton diagram (e.g., including densely packed fibrous particles), region II of the Thornton diagram (e.g., including columnar particles), and / or region III of the Thornton diagram (e.g., including recrystallized particles). Such a columnar structure can be in the form of a dense film and / or can include fine-grained nanocrystals (e.g., having a preferred orientation). The Thornton diagram is described in Anders, AStructure Zone Diagram Including Plasma Based Deposition and Ion Etching, Thin Solid Films 2010; 518 (15); 4087-90, which is incorporated herein by reference in its entirety for all purposes.

[0112] As from Fig.19 It can be seen that the layer (e.g., a layer containing a substance other than lithium metal, a passivation layer) disposed on the layer containing lithium metal and comprising a plurality of columnar structures can be porous. For example, the spaces between the columnar structures can take the form of holes and / or the columnar structures themselves can include holes. These holes can include open holes (e.g., holes that pass through the entire layer, holes that do not pass through the entire layer) and / or closed holes.

[0113] In some embodiments, a layer disposed on a layer containing lithium metal (e.g., a layer containing a substance other than lithium metal, a passivation layer) includes a plurality of columnar structures and / or a plurality of pores that extend partially but not entirely through the layer. Fig. 20 An example of a layer having this property is shown. Fig. 20 , article 2036 includes layer 2136 including lithium and layer 2336 disposed on layer 2136. Layer 2336 includes a plurality of columnar structures 2536 extending partially through the layer from an upper surface of layer 2336 and a plurality of pores 2636 also extending partially through the layer from an upper surface of the layer. The lower portion of layer 2336 lacks columnar structures and pores.

[0114] It should also be noted that some layers disposed on the layer containing lithium metal (eg, a layer containing a substance other than lithium metal, a passivation layer) may lack columnar structures and / or pores.

[0115] In some embodiments, the article for inclusion in the electrochemical cell includes two or more of the above layers. As an example, in some embodiments, the article for inclusion in the electrochemical cell includes a layer (e.g., a passivation layer) containing a substance other than lithium metal disposed on a layer containing lithium metal. As another example, the article for inclusion in the electrochemical cell may include a layer containing lithium metal disposed on a layer (e.g., a passivation layer) containing a substance other than lithium metal. As a third example, some embodiments may relate to an article including a layer (e.g., a layer containing lithium metal, a layer containing a substance other than lithium metal, a passivation layer) located between two layers of different types (e.g., between two layers containing lithium metal, between two layers containing substances other than lithium metal, between two passivation layers). Other arrangements (e.g., including four or more layers, including two adjacent layers having the same composition) are also contemplated.

[0116] It should also be understood that some articles for inclusion in electrochemical cells may include Figures 15 to 20 As an example, in some embodiments, the article for inclusion in an electrochemical cell further includes a substrate, a current collector, a release layer, or any other suitable component.

[0117] Some embodiments herein relate to methods. Examples of contemplated methods include methods that may be performed in a modular lithium deposition system and / or methods that may be used to form a layer comprising lithium metal and / or a layer disposed on a layer comprising lithium metal.

[0118] For example, some embodiments relate to a method comprising depositing a layer onto a substrate in a module located in a modular lithium deposition chamber. The modular lithium deposition system and / or the module may have one or more of the features described elsewhere herein. As an example, the module may include a vacuum chamber (and in some embodiments, a layer is deposited on a portion of a substrate located in a vacuum chamber). As another example, the module may have an environment different from different parts of the modular lithium deposition system where the layer is not deposited. For example, in some embodiments, during the deposition of the layer onto the first portion of the substrate, the second portion of the substrate is not exposed to the gas used to deposit the layer. This can be achieved by, for example, positioning the first and second portions of the substrate in a module that is fluidically isolated from each other (e.g., a vacuum chamber that is fluidically isolated from each other).

[0119] As another example of a suitable method, in some embodiments, a method includes depositing a layer comprising lithium metal in a modular deposition system that includes two or more lithium metal sources located in two or more containers. The method can include depositing lithium metal from the two sources (e.g., sequentially) to form a final layer comprising lithium metal that has a higher uniformity (e.g., having a reduced variation in thickness, chemical composition, and / or porosity in a cross-web direction) than a layer comprising lithium metal deposited from only one of the two or more sources would have. For example, depositing lithium metal from a first lithium metal source can produce a first layer comprising lithium metal, and depositing lithium metal from a second lithium metal source on the first layer can result in the formation of a final, more uniform lithium metal layer that includes the first lithium metal layer and lithium metal deposited from the second lithium metal source on the first lithium metal layer.

[0120] As a third example of a suitable method, in some embodiments, a method includes depositing an electroactive layer from a gas containing lithium and a gas containing a non-lithium species. These gases can react with each other to form a layer containing both lithium metal and a species other than lithium metal.

[0121] As a fourth example of a suitable method, in some embodiments, a method includes forming a passivation layer disposed on a layer comprising lithium metal. The passivation layer may be formed by exposing the layer comprising lithium metal to a gas reactive therewith. The gas may react with the lithium metal at a surface of the layer comprising lithium metal to form a passivation layer disposed on the layer comprising lithium metal. The passivation layer may include a reaction product of the lithium metal in the layer comprising lithium metal and the gas.

[0122] As described elsewhere herein, in some embodiments, one or more components of the modular lithium deposition system are configured to be heated, cooled, and / or maintained at a temperature within a temperature range. Examples of suitable such temperature ranges are provided below.

[0123] A component of a modular lithium deposition system that can be configured to be cooled to a temperature within a range and / or maintained at a temperature within a range is a drum. In some embodiments, the drum is configured to be cooled to and / or maintained at a temperature (e.g., by a cooling system) of less than or equal to 60°C, less than or equal to 55°C, less than or equal to 50°C, less than or equal to 45°C, less than or equal to 40°C, less than or equal to 35°C, less than or equal to 30°C, less than or equal to 25°C, less than or equal to 20°C, less than or equal to 15°C, less than or equal to 10°C, less than or equal to 5°C, less than or equal to 0°C, less than or equal to -5°C, less than or equal to -10°C, less than or equal to -15°C, less than or equal to -20°C, less than or equal to -25°C, or less than or equal to -30°C. In some embodiments, the drum is configured to be cooled (e.g., by a cooling system) to and / or maintained at a temperature of greater than or equal to -35°C, greater than or equal to -30°C, greater than or equal to -25°C, greater than or equal to -20°C, greater than or equal to -15°C, greater than or equal to -10°C, greater than or equal to -5°C, greater than or equal to 0°C, greater than or equal to 5°C, greater than or equal to 10°C, greater than or equal to 15°C, greater than or equal to 20°C, greater than or equal to 25°C, greater than or equal to 30°C, greater than or equal to 35°C, greater than or equal to 40°C, greater than or equal to 45°C, greater than or equal to 50°C, or greater than or equal to 55°C. Combinations of the above ranges are also possible (e.g., less than or equal to 60°C and greater than or equal to -35°C). Other ranges are also possible. The temperature of the drum can be determined by an IR temperature sensor.

[0124] When the modular lithium deposition system includes two or more drums, each drum can be independently configured to be cooled to a temperature within one or more of the above ranges and / or maintained at a temperature within one or more of the above ranges. In some embodiments, the cooling fluid circulated across one or more surfaces of one or more drums and / or through one or more walls of one or more drums has a temperature within one or more of the above ranges.

[0125] Another component of the modular lithium deposition system that can be configured to be cooled to a temperature within a certain range and / or maintained at a temperature within a certain range is the outer surface of the container for the lithium metal source. In some embodiments, the outer surface of the container is configured to be cooled to the following temperature and / or maintained at the following temperature (e.g., through multiple cooling channels): less than or equal to 50°C, less than or equal to 45°C, less than or equal to 40°C, less than or equal to 35°C, less than or equal to 30°C, less than or equal to 25°C, or less than or equal to 20°C. In some embodiments, the outer surface of the container is configured to be cooled to the following temperature and / or maintained at the following temperature (e.g., through multiple cooling channels): greater than or equal to 15°C, greater than or equal to 20°C, greater than or equal to 25°C, greater than or equal to 30°C, greater than or equal to 35°C, greater than or equal to 40°C, or greater than or equal to 45°C. Combinations of the above ranges are also possible (e.g., less than or equal to 50°C and greater than or equal to 15°C). Other ranges are also possible. The temperature of the outer surface of the container for the lithium source can be determined by a thermocouple located on the outer surface.

[0126] When the modular lithium deposition system includes two or more containers for a lithium metal source, each container for a lithium metal source can be independently configured to be cooled to a temperature within one or more of the above ranges and / or maintained at a temperature within one or more of the above ranges.

[0127] Some containers for lithium metal sources may be configured to be heated (e.g., in addition to being cooled). In some embodiments, the inner surface of the container is configured to be heated (e.g., by a heating system, such as a resistive heating system) to and / or maintained at a temperature greater than or equal to 550°C, greater than or equal to 560°C, greater than or equal to 570°C, greater than or equal to 580°C, greater than or equal to 590°C, greater than or equal to 600°C, greater than or equal to 610°C, greater than or equal to 620°C, or greater than or equal to 630°C. In some embodiments, the inner surface of the container is configured to be heated (e.g., by a heating system, such as a resistive heating system) to and / or maintained at a temperature less than or equal to 635°C, less than or equal to 630°C, less than or equal to 620°C, less than or equal to 610°C, less than or equal to 600°C, less than or equal to 590°C, less than or equal to 580°C, less than or equal to 570°C, or less than or equal to 560°C. Combinations of the above ranges are also possible (e.g., greater than or equal to 550°C and less than or equal to 635°C). Other ranges are also possible. The temperature of the inner surface of the container for the lithium source can be determined by a thermocouple located on the inner surface. In some embodiments, the inner surface configured to be heated to a temperature within one or more of the above ranges and / or maintained within a temperature within one or more of the above ranges is an inner surface in direct contact with the lithium metal source.

[0128] When the modular lithium deposition system includes two or more containers for a lithium metal source, each container for a lithium metal source can be independently configured to be heated to a temperature within one or more of the above ranges and / or maintained at a temperature within one or more of the above ranges.

[0129] Another component of the modular lithium deposition system that can be configured to be heated to a temperature within a certain range and / or maintained at a temperature within a certain range is a shutter of a container containing a lithium metal source. In some embodiments, the shutter is configured to be heated to and / or maintained at a temperature greater than or equal to 550°C, greater than or equal to 560°C, greater than or equal to 570°C, greater than or equal to 580°C, greater than or equal to 590°C, greater than or equal to 600°C, greater than or equal to 610°C, greater than or equal to 620°C, greater than or equal to 630°C, or greater than or equal to 640°C (e.g., by a heating system, such as a resistive heating system). In some embodiments, the shutter is configured to be heated to and / or maintained at a temperature less than or equal to 645°C, less than or equal to 640°C, less than or equal to 630°C, less than or equal to 620°C, less than or equal to 610°C, less than or equal to 600°C, less than or equal to 590°C, less than or equal to 580°C, less than or equal to 570°C, or less than or equal to 560°C (e.g., greater than or equal to 550°C and less than or equal to 645°C). Other ranges are also possible. The temperature of the shutter of the container for the lithium source can be determined by a thermocouple located on the shutter.

[0130] When the modular lithium deposition system includes two or more containers for a lithium metal source, each container for the lithium metal source can independently include a shutter configured to be heated to a temperature within one or more of the above ranges and / or maintained at a temperature within one or more of the above ranges.

[0131] As described elsewhere herein, in some embodiments, the modular lithium deposition system includes one or more vacuum chambers. The vacuum chambers can be configured to be maintained at a pressure less than atmospheric pressure. As an example, in some embodiments, the vacuum chambers are configured to be maintained at a pressure less than or equal to 10 -4 Support, less than or equal to 5*10 -5 Support, less than or equal to 2*10 -5 Support, less than or equal to 10 -5 Support, less than or equal to 5*10 -6 Support, less than or equal to 2*10 -6 Support, less than or equal to 10 -6 Support, less than or equal to 5*10 -7 Support, or less than or equal to 2*10 -7 In some embodiments, the vacuum chamber is configured to be maintained at a pressure greater than or equal to 10 -7 Support, greater than or equal to 2*10 -7Support, greater than or equal to 5*10 -7 Support, greater than or equal to 10 -6 Support, greater than or equal to 2*10 -6 Support, greater than or equal to 5*10 -6 Support, greater than or equal to 10 -5 Support, greater than or equal to 2*10 -5 Support, or greater than or equal to 5*10 -5 Combinations of the above ranges are also possible (e.g., less than or equal to 10 -6 Support and greater than or equal to 10 -7 Torr, or less than or equal to 10 -4 Support and greater than or equal to 10 -5 Torr). Other ranges are also possible. The pressure of the vacuum chamber can be determined by a pressure gauge located in the vacuum chamber.

[0132] When the modular lithium deposition system includes two or more vacuum chambers, each vacuum chamber may be independently configured to be maintained at a pressure within one or more of the ranges described above.

[0133] As described elsewhere herein, some embodiments relate to a modular lithium deposition system comprising a source, such as a source of a gas reactive with lithium metal and / or a source of a gas configured to be deposited to form a layer disposed on a layer comprising lithium metal. Also as described elsewhere herein, some embodiments relate to a method of depositing a layer (e.g., a passivation layer) on a layer comprising lithium metal. In some embodiments, the layer is deposited by condensing a gas on a layer comprising lithium metal. It is also possible that the reaction products of the gases with each other and / or with lithium metal (e.g., in a lithium metal layer) can condense to form the associated layer. A variety of suitable gases are suitable for such purposes, including CO2, O2, H2O, COS, SO2, CS2, H2, N2, N2O, NH3, SF6, Freon, fluorobenzene, SiF4, C2H2, air (e.g., clean dry air, artificial air), substances containing boron (e.g., borates), substances containing phosphorus (e.g., phosphates), substances containing selenium, substances containing tellurium and / or substances containing halogens (e.g., substances containing fluorine, bromine and / or iodine, including those mentioned above). In some embodiments, one or more gases suitable for use in atomic layer deposition are used to deposit a layer containing lithium metal and / or a layer thereon. Some gases that can be used to deposit a layer containing lithium metal and / or a layer thereon can be activated (e.g., by plasma) before and / or while being used to deposit the layer.

[0134] In some embodiments, two or more gases are used in combination. For example, in some embodiments, it may be desirable to deposit a layer from a combination of gases that include both H2O and another different gas. As another example, in some embodiments, a combination of CO2 with N2 and / or O2 may be particularly advantageous. In some embodiments, as described elsewhere herein, a layer disposed on a layer comprising lithium metal may be deposited in the further presence of an inert gas such as argon and / or helium.

[0135] When a layer is deposited by a combination of gases including both H2O and another different gas, the relative humidity of the combination of gases can be various suitable values. That is, the ratio of the amount of H2O in the combination of gases to the amount of H2O soluble in the combination of gases can be selected as needed. In some embodiments, the relative humidity of the combination of gases is similar to the relative humidity of a typical dry room (e.g., less than or equal to 10%). The relative humidity of the combination of gases can also have another value (e.g., exceeding the value in a typical dry room). In some embodiments, a layer is deposited by a combination of gases having the following relative humidities: greater than or equal to 0%, greater than or equal to 1%, greater than or equal to 2%, greater than or equal to 5%, greater than or equal to 7.5%, greater than or equal to 10%, greater than or equal to 12.5%, greater than or equal to 15%, greater than or equal to 20%, greater than or equal to 25%, greater than or equal to 30%, greater than or equal to 35%, greater than or equal to 40%, or greater than or equal to 45%. In some embodiments, the layer is deposited from a combination of gases having a relative humidity of less than or equal to 50%, less than or equal to 45%, less than or equal to 40%, less than or equal to 35%, less than or equal to 30%, less than or equal to 25%, less than or equal to 20%, less than or equal to 15%, less than or equal to 12.5%, less than or equal to 10%, less than or equal to 7.5%. Less than or equal to 5%, less than or equal to 2%, or less than or equal to 1%. Combinations of the above ranges are also possible (e.g., greater than or equal to 0% and less than or equal to 50%, greater than or equal to 0% and less than or equal to 30%, or greater than or equal to 0% and less than or equal to 10%). Other ranges are also possible.

[0136] As described elsewhere herein, some embodiments relate to layers comprising lithium metal (e.g., electroactive layers comprising lithium metal). For example, some embodiments relate to the deposition of such layers, some embodiments relate to articles comprising such layers for inclusion in electrochemical cells, and some embodiments relate to modular lithium deposition systems configured to deposit such layers. Other characteristics of layers comprising lithium metal are described in more detail below.

[0137] The layer containing lithium metal can have various suitable thicknesses. In some embodiments, the layer containing lithium metal has the following thickness: greater than or equal to 1 micron, greater than or equal to 2 microns, greater than or equal to 5 microns, greater than or equal to 7.5 microns, greater than or equal to 10 microns, greater than or equal to 15 microns, greater than or equal to 20 microns, greater than or equal to 25 microns, greater than or equal to 30 microns, greater than or equal to 35 microns, greater than or equal to 40 microns, or greater than or equal to 45 microns. In some embodiments, the layer containing lithium metal has the following thickness: less than or equal to 50 microns, less than or equal to 45 microns, less than or equal to 40 microns, less than or equal to 35 microns, less than or equal to 30 microns, less than or equal to 25 microns, less than or equal to 20 microns, less than or equal to 15 microns, less than or equal to 10 microns, less than or equal to 7.5 microns, less than or equal to 5 microns, or less than or equal to 2 microns. Combinations of the above ranges are also possible (e.g., greater than or equal to 1 micron and less than or equal to 50 microns, or greater than or equal to 2 microns and less than or equal to 30 microns). Other ranges are also possible. The thickness of the layer containing lithium metal can be determined by eddy current sensing.

[0138] When the article for inclusion in an electrochemical cell includes two or more layers comprising lithium metal, each layer comprising lithium metal can independently have a thickness within one or more of the above ranges.

[0139] The layer containing lithium metal can have a variety of suitable porosities. As described elsewhere herein, some layers containing lithium metal can be relatively dense (e.g., they can have a porosity greater than or equal to 0% and less than or equal to 5%), or can include a plurality of pores occupying a significant volume fraction thereof (e.g., they can have a porosity greater than or equal to 5% and less than or equal to 25%, or greater than or equal to 5% and less than or equal to 15%). In some embodiments, the layer containing lithium metal has the following porosity: greater than or equal to 0%, greater than or equal to 0.5%, greater than or equal to 1%, greater than or equal to 1.5%, greater than or equal to 2%, greater than or equal to 3%, greater than or equal to 4%, greater than or equal to 5%, greater than or equal to 7.5%, greater than or equal to 10%, greater than or equal to 12.5%, greater than or equal to 15%, greater than or equal to 17.5%, greater than or equal to 20%, or greater than or equal to 22.5%. In some embodiments, the layer comprising lithium metal has a porosity of less than or equal to 25%, less than or equal to 22.5%, less than or equal to 20%, less than or equal to 17.5%, less than or equal to 15%, less than or equal to 12.5%, less than or equal to 10%, less than or equal to 7.5%, less than or equal to 5%, less than or equal to 4%, less than or equal to 3%, less than or equal to 2%, less than or equal to 1.5%, less than or equal to 1%, or less than or equal to 0.5%. Combinations of the above ranges are also possible (e.g., greater than or equal to 0% and less than or equal to 25%, greater than or equal to 0% and less than or equal to 5%, greater than or equal to 5% and less than or equal to 25%, or greater than or equal to 5% and less than or equal to 25%). Other ranges are also possible.

[0140] The layer containing lithium metal may have a porosity in one or more of the above ranges as determined by dividing the measured density of the layer containing lithium metal by the theoretical density of the layer containing lithium metal. The measured density of the layer containing lithium metal can be determined by the following formula: measured density of the layer containing lithium metal = [weight of the layer containing lithium metal] / [(area of ​​the layer containing lithium metal) * (thickness of the layer containing lithium metal as measured by a drop meter)].

[0141] The layer comprising lithium can also have a porosity in one or more of the above ranges as measured by a scanning electron microscope. In short, a scanning electron microscope operated in immersion mode at an accelerating voltage of 5kV, a working distance of 5mm, a spot size of 3.5 and a magnification of 25,000 can be used to image the layer comprising lithium. The image can be analyzed using ImageJ configured to have an 8-bit type, 255 gray levels, a width of 27.43 inches, a height of 19.69 inches, an image size of 1.6MB and a resolution of 56 pixels per inch. In ImageJ, the brightness / contrast minimum value can be set to 0, the brightness / contrast maximum value can be set to 255, the threshold lower limit value can be set to 0, and the threshold upper limit value can be set to a value that makes the hole look black. Then, ImageJ can be used to analyze the resulting image to determine the percentage of black area. This percentage can be regarded as being equivalent to the porosity of the layer comprising lithium.

[0142] When the article for inclusion in an electrochemical cell comprises two or more layers comprising lithium metal, each layer comprising lithium metal can independently have a porosity within one or more of the above ranges as measured by one or both of the above measurement techniques.

[0143] In some embodiments, information about the morphology of the layer comprising lithium metal can be obtained from its color space. Color space is a combination of brightness, saturation, chroma, and hue that characterizes the visual appearance of an object. Fig.21A and Fig.21B It is shown how these parameters together describe the visual appearance of an object.It will also be appreciated that a layer comprising lithium may appear visually to have various colours, such as red, yellow, green and / or blue.

[0144] In some embodiments, the layer comprising lithium has a brightness greater than or equal to 10, greater than or equal to 12.5, greater than or equal to 15, greater than or equal to 17.5, greater than or equal to 20, greater than or equal to 22.5, greater than or equal to 25, greater than or equal to 27.5, greater than or equal to 30, greater than or equal to 35, greater than or equal to 40, greater than or equal to 45, greater than or equal to 50, greater than or equal to 55, greater than or equal to 60, greater than or equal to 65, greater than or equal to 70, greater than or equal to 75, or greater than or equal to 80. In some embodiments, the layer comprising lithium has a brightness of less than or equal to 85, less than or equal to 80, less than or equal to 75, less than or equal to 70, less than or equal to 65, less than or equal to 60, less than or equal to 55, less than or equal to 50, less than or equal to 45, less than or equal to 40, less than or equal to 35, less than or equal to 30, less than or equal to 27.5, less than or equal to 25, less than or equal to 22.5, less than or equal to 20, less than or equal to 17.5, less than or equal to 15, or less than or equal to 12.5. Combinations of the above ranges are also possible (e.g., greater than or equal to 10 and less than or equal to 85, or greater than or equal to 20 and less than or equal to 60). Other ranges are also possible.

[0145] When the article for inclusion in an electrochemical cell includes two or more layers comprising lithium metal, each layer comprising lithium metal can independently have a brightness within one or more of the above ranges.

[0146] In some embodiments, the layer comprising lithium has a red / green saturation ("a" saturation): greater than or equal to -3, greater than or equal to -2.5, greater than or equal to -2, greater than or equal to -1.5, greater than or equal to -1, greater than or equal to -0.5, greater than or equal to 0, greater than or equal to 0.5, greater than or equal to 1, greater than or equal to 1.5, greater than or equal to 2, greater than or equal to 2.5, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, greater than or equal to 4.5, greater than or equal to 5, greater than or equal to 6, greater than or equal to 8, greater than or equal to 10, greater than or equal to 12.5, or greater than or equal to 15. In some embodiments, the layer comprising lithium has the following red / green saturation: less than or equal to 20, less than or equal to 15, less than or equal to 12.5, less than or equal to 10, less than or equal to 8, less than or equal to 6, less than or equal to 5, less than or equal to 4.5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, less than or equal to 2.5, less than or equal to 2, less than or equal to 1.5, less than or equal to 1, less than or equal to 0.5, less than or equal to 0, less than or equal to -0.5, less than or equal to -1, less than or equal to -1.5, less than or equal to -2, or less than or equal to -2.5. Combinations of the above ranges are also possible (e.g., greater than or equal to -3 and less than or equal to 20, or greater than or equal to -1 and less than or equal to 4). Other ranges are also possible.

[0147] When the article for inclusion in an electrochemical cell includes two or more layers comprising lithium metal, each layer comprising lithium metal can independently have a red / green saturation within one or more of the above ranges.

[0148] In some embodiments, the layer comprising lithium has a yellow / blue saturation ("b" saturation): greater than or equal to -3, greater than or equal to -2.5, greater than or equal to -2, greater than or equal to -1.5, greater than or equal to -1, greater than or equal to -0.5, greater than or equal to 0, greater than or equal to 0.5, greater than or equal to 1, greater than or equal to 1.5, greater than or equal to 2, greater than or equal to 2.5, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, greater than or equal to 4.5, greater than or equal to 5, greater than or equal to 6, greater than or equal to 8, greater than or equal to 10, greater than or equal to 12.5, or greater than or equal to 15. In some embodiments, the layer comprising lithium has the following yellow / blue saturation: less than or equal to 20, less than or equal to 15, less than or equal to 12.5, less than or equal to 10, less than or equal to 8, less than or equal to 6, less than or equal to 5, less than or equal to 4.5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, less than or equal to 2.5, less than or equal to 2, less than or equal to 1.5, less than or equal to 1, less than or equal to 0.5, less than or equal to 0, less than or equal to -0.5, less than or equal to -1, less than or equal to -1.5, less than or equal to -2, or less than or equal to -2.5. Combinations of the above ranges are also possible (e.g., greater than or equal to -3 and less than or equal to 20, or greater than or equal to -1 and less than or equal to 4). Other ranges are also possible.

[0149] When the article for inclusion in an electrochemical cell includes two or more layers comprising lithium metal, each layer comprising lithium metal can independently have a yellow / blue saturation within one or more of the above ranges.

[0150] In some embodiments, the layer comprising lithium has a chromaticity of greater than or equal to -2, greater than or equal to -1.5, greater than or equal to -1, greater than or equal to -0.5, greater than or equal to 0, greater than or equal to 0.5, greater than or equal to 1, greater than or equal to 1.5, greater than or equal to 2, greater than or equal to 2.5, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, greater than or equal to 4.5, greater than or equal to 5, greater than or equal to 6, greater than or equal to 8, greater than or equal to 10, greater than or equal to 12.5, or greater than or equal to 15. In some embodiments, the layer comprising lithium has a chromaticity of less than or equal to 20, less than or equal to 15, less than or equal to 12.5, less than or equal to 10, less than or equal to 8, less than or equal to 6, less than or equal to 5, less than or equal to 4.5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, less than or equal to 2.5, less than or equal to 2, less than or equal to 1.5, less than or equal to 1, less than or equal to 0.5, less than or equal to 0, less than or equal to -0.5, less than or equal to -1, or less than or equal to -1.5. Combinations of the above ranges are also possible (e.g., greater than or equal to -2 and less than or equal to 20, or greater than or equal to -1 and less than or equal to 5). Other ranges are also possible.

[0151] When the article for inclusion in an electrochemical cell includes two or more layers comprising lithium metal, each layer comprising lithium metal can independently have a chromaticity within one or more of the above ranges.

[0152] In some embodiments, the layer comprising lithium has a hue of greater than or equal to -2°, greater than or equal to 0°, greater than or equal to 2°, greater than or equal to 5°, greater than or equal to 7.5°, greater than or equal to 10°, greater than or equal to 20°, greater than or equal to 50°, greater than or equal to 75°, greater than or equal to 100°, greater than or equal to 125°, greater than or equal to 150°, greater than or equal to 175°, greater than or equal to 200°, greater than or equal to 225°, greater than or equal to 250°, greater than or equal to 275°, greater than or equal to 300°, or greater than or equal to 325°. In some embodiments, the layer comprising lithium has a hue of less than or equal to 360°, less than or equal to 325°, less than or equal to 300°, less than or equal to 275°, less than or equal to 250°, less than or equal to 225°, less than or equal to 200°, less than or equal to 175°, less than or equal to 150°, less than or equal to 125°, less than or equal to 100°, less than or equal to 75°, less than or equal to 50°, less than or equal to 20°, less than or equal to 10°, less than or equal to 7.5°, less than or equal to 5°, less than or equal to 2°, or less than or equal to 0°. Combinations of the above ranges are also possible (e.g., greater than or equal to -2° and less than or equal to 360°, or greater than or equal to 10° and less than or equal to 350°). Other ranges are also possible.

[0153] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal can independently have a hue within one or more of the above ranges.

[0154] In some embodiments, the layer containing lithium metal is relatively smooth. The smoothness or roughness of the layer containing lithium metal can be characterized in a variety of ways. Suitable parameters that can be used to characterize the roughness of the layer containing lithium metal and suitable values ​​of these parameters are described in more detail below. Some of the following techniques can be used with reference to the cross-section of the layer containing lithium metal, and it should be understood that some layers containing lithium metal may include at least one cross-section having one or more of the characteristics described below, some layers containing lithium metal may be composed only of cross-sections having one or more of the characteristics described below, and some layers containing lithium metal may have a morphology that makes most of the cross-sections (e.g., at least 50% of the cross-sections, at least 75% of the cross-sections, at least 90% of the cross-sections, at least 95% of the cross-sections, or at least 99% of the cross-sections) have one or more of the following characteristics.

[0155] An example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is R a, which is the arithmetic mean deviation of a cross section across the height of the layer from a mean line of the cross section (i.e., a line parallel to the surface and dividing the cross section such that the area between the surface topography and the line below it is equal to the area between the surface topography and the line above it). In some embodiments, the layer comprising lithium metal has the following R a Value: less than or equal to 1.5 microns, less than or equal to 1.25 microns, less than or equal to 1 micron, less than or equal to 0.75 microns, less than or equal to 0.5 microns, less than or equal to 0.25 microns, less than or equal to 0.2 microns, less than or equal to 0.18 microns, less than or equal to 0.15 microns, less than or equal to 0.125 microns, less than or equal to 0.1 microns, or less than or equal to 0.075 microns. In some embodiments, the layer comprising lithium metal has the following R a Values: greater than or equal to 0.05 microns, greater than or equal to 0.075 microns, greater than or equal to 0.1 microns, greater than or equal to 0.125 microns, greater than or equal to 0.15 microns, greater than or equal to 0.18 microns, greater than or equal to 0.2 microns, greater than or equal to 0.25 microns, greater than or equal to 0.5 microns, greater than or equal to 0.75 microns, greater than or equal to 1 micron, or greater than or equal to 1.25 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 1.5 microns and greater than or equal to 0.05 microns, or less than or equal to 1.5 microns and greater than or equal to 0.18 microns). Other ranges are also possible.

[0156] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal may independently have an R in one or more of the above ranges. a value.

[0157] A second example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is R q , which is the root mean square deviation of the cross section across the height of the layer from the mean line of the cross section. In some embodiments, the layer comprising lithium metal has the following R q Value: less than or equal to 2.5 microns, less than or equal to 2.25 microns, less than or equal to 2 microns, less than or equal to 1.75 microns, less than or equal to 1.5 microns, less than or equal to 1.25 microns, less than or equal to 1 micron, less than or equal to 0.75 microns, less than or equal to 0.5 microns, less than or equal to 0.4 microns, less than or equal to 0.3 microns, or less than or equal to 0.2 microns. In some embodiments, the layer comprising lithium metal has the following R qValues: greater than or equal to 0.1 microns, greater than or equal to 0.2 microns, greater than or equal to 0.3 microns, greater than or equal to 0.4 microns, greater than or equal to 0.5 microns, greater than or equal to 0.75 microns, greater than or equal to 1 micron, greater than or equal to 1.25 microns, greater than or equal to 1.5 microns, greater than or equal to 1.75 microns, greater than or equal to 2 microns, or greater than or equal to 2.25 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 2.5 microns and greater than or equal to 0.1 microns, or less than or equal to 2 microns and greater than or equal to 0.2 microns). Other ranges are also possible.

[0158] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal may independently have an R in one or more of the above ranges. q value.

[0159] A third example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is R p , which is the difference between the maximum height in the cross section and the height of the average line. In some embodiments, the layer containing lithium metal has the following R p Value: less than or equal to 15 microns, less than or equal to 12.5 microns, less than or equal to 10 microns, less than or equal to 7.5 microns, less than or equal to 5 microns, less than or equal to 2.5 microns, less than or equal to 2 microns, less than or equal to 1.5 microns, or less than or equal to 1 micron. In some embodiments, the layer comprising lithium metal has the following R p Values: greater than or equal to 0.5 microns, greater than or equal to 1 micron, greater than or equal to 1.5 microns, greater than or equal to 2 microns, greater than or equal to 2.5 microns, greater than or equal to 5 microns, greater than or equal to 7.5 microns, greater than or equal to 10 microns, or greater than or equal to 12.5 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 15 microns and greater than or equal to 0.5 microns, or less than or equal to 15 microns and greater than or equal to 1 micron). Other ranges are also possible.

[0160] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal may independently have an R in one or more of the above ranges. p value.

[0161] Another example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is R v , which is the difference between the minimum height in the cross section and the height of the average line. In some embodiments, the layer containing lithium metal has the following R vValue: greater than or equal to less than or equal to -15 microns, greater than or equal to -12.5 microns, greater than or equal to -10 microns, greater than or equal to -7.5 microns, greater than or equal to -5 microns, greater than or equal to -2.5 microns, greater than or equal to -2 microns, greater than or equal to -1.5 microns, or greater than or equal to -1 micron. In some embodiments, the layer comprising lithium metal has the following R v Values: less than or equal to -0.5 microns, less than or equal to -1 microns, less than or equal to -1.5 microns, less than or equal to -2 microns, less than or equal to -2.5 microns, less than or equal to -5 microns, less than or equal to -7.5 microns, less than or equal to -10 microns, or less than or equal to -12.5 microns. Combinations of the above ranges are also possible (e.g., greater than or equal to -15 microns and less than or equal to -0.5 microns, or greater than or equal to -15 microns and less than or equal to -1 micron). Other ranges are also possible.

[0162] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal may independently have an R in one or more of the above ranges. v value.

[0163] Another example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is R t , which is R p The absolute value and R v In some embodiments, the layer comprising lithium metal has the following R t Value: less than or equal to 30 microns, less than or equal to 25 microns, less than or equal to 20 microns, less than or equal to 15 microns, less than or equal to 10 microns, less than or equal to 7.5 microns, less than or equal to 5 microns, less than or equal to 4 microns, less than or equal to 3 microns, less than or equal to 2.5 microns, less than or equal to 2 microns, or less than or equal to 1.5 microns. In some embodiments, the layer comprising lithium metal has the following R t Values: greater than or equal to 1 micron, greater than or equal to 1.5 microns, greater than or equal to 2 microns, greater than or equal to 2.5 microns, greater than or equal to 3 microns, greater than or equal to 4 microns, greater than or equal to 5 microns, greater than or equal to 7.5 microns, greater than or equal to 10 microns, greater than or equal to 15 microns, greater than or equal to 20 microns, or greater than or equal to 25 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 25 microns and greater than or equal to 1 micron, or less than or equal to 30 microns and greater than or equal to 2 microns). Other ranges are also possible.

[0164] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal may independently have an R in one or more of the above ranges. t value.

[0165] Another example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is R pm , which is the average height of the peaks in the cross section relative to the average line. In some embodiments, the layer containing lithium metal has the following R pm Value: less than or equal to 15 microns, less than or equal to 12.5 microns, less than or equal to 10 microns, less than or equal to 7.5 microns, less than or equal to 5 microns, less than or equal to 3 microns, less than or equal to 2 microns, less than or equal to 1.5 microns, less than or equal to 1 micron, or less than or equal to 0.75 microns. In some embodiments, the layer comprising lithium metal has the following R pm Values: greater than or equal to 0.5 microns, greater than or equal to 0.75 microns, greater than or equal to 1 micron, greater than or equal to 1.5 microns, greater than or equal to 2 microns, greater than or equal to 3 microns, greater than or equal to 5 microns, greater than or equal to 7.5 microns, greater than or equal to 10 microns, or greater than or equal to 12.5 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 15 microns and greater than or equal to 0.5 microns, or less than or equal to 10 microns and greater than or equal to 1 micron). Other ranges are also possible.

[0166] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal may independently have an R in one or more of the above ranges. pm value.

[0167] Another example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is R vm , which is the average height of the valleys in the cross section relative to the average line. In some embodiments, the layer comprising lithium metal has the following R vm Value: greater than or equal to -15 microns, greater than or equal to -12.5 microns, greater than or equal to -10 microns, greater than or equal to -7.5 microns, greater than or equal to -5 microns, greater than or equal to -3 microns, greater than or equal to -2 microns, greater than or equal to -1.5 microns, greater than or equal to -1 micron, or greater than or equal to -0.75 microns. In some embodiments, the layer comprising lithium metal has the following R vmValues: less than or equal to -0.5 microns, less than or equal to -0.75 microns, less than or equal to -1 microns, less than or equal to -1.5 microns, less than or equal to -2 microns, less than or equal to -3 microns, less than or equal to -5 microns, less than or equal to -7.5 microns, less than or equal to -10 microns, or less than or equal to -12.5 microns. Combinations of the above ranges are also possible (e.g., greater than or equal to -15 microns and less than or equal to -1 micron, or greater than or equal to -10 microns and less than or equal to -0.5 microns). Other ranges are also possible.

[0168] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal may independently have an R in one or more of the above ranges. vm value.

[0169] Another example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is R z , which is the height difference between the average height of the five highest peaks in the cross section and the average height of the five deepest valleys in the cross section. In some embodiments, the layer comprising lithium metal has the following R z Value: less than or equal to 20 microns, less than or equal to 17.5 microns, less than or equal to 15 microns, less than or equal to 12.5 microns, less than or equal to 10 microns, less than or equal to 7.5 microns, less than or equal to 5 microns, or less than or equal to 2.5 microns. In some embodiments, the layer comprising lithium metal has the following R z Values: greater than or equal to 1 micron, greater than or equal to 2.5 microns, greater than or equal to 5 microns, greater than or equal to 7.5 microns, greater than or equal to 10 microns, greater than or equal to 12.5 microns, greater than or equal to 15 microns, or greater than or equal to 17.5 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 20 microns and greater than or equal to 1 micron). Other ranges are also possible.

[0170] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal may independently have an R in one or more of the above ranges. z value.

[0171] Another example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is S m , which is the area of ​​material in the cross section that exists between the top of the cross section and the 90th percentile cross-sectional height (i.e., a height value greater than 90% of the height in the cross section). In some embodiments, the layer comprising lithium metal has the following S mValue: less than or equal to 1 square micron, less than or equal to 0.75 square micron, less than or equal to 0.5 square micron, less than or equal to 0.3 square micron, less than or equal to 0.2 square micron, less than or equal to 0.15 square micron, less than or equal to 0.1 square micron, less than or equal to 0.075 square micron, less than or equal to 0.05 square micron, less than or equal to 0.03 square micron, less than or equal to 0.02 square micron, less than or equal to 0.015 square micron, less than or equal to 0.01 square micron, less than or equal to 0.0075 square micron, less than or equal to 0.005 square micron, less than or equal to 0.003 square micron, or less than or equal to 0.002 square micron. In some embodiments, the layer comprising lithium metal has the following S m Values: greater than or equal to 0.001 square microns, greater than or equal to 0.002 square microns, greater than or equal to 0.003 square microns, greater than or equal to 0.005 square microns, greater than or equal to 0.0075 square microns, greater than or equal to 0.01 square microns, greater than or equal to 0.02 square microns, greater than or equal to 0.05 square microns, greater than or equal to 0.075 square microns, greater than or equal to 0.1 square microns, greater than or equal to 0.15 square microns, greater than or equal to 0.2 square microns, greater than or equal to 0.3 square microns, greater than or equal to 0.5 square microns, or greater than or equal to 0.75 square microns. Combinations of the above ranges are also possible (e.g., less than or equal to 1 square micron and greater than or equal to 0.001 square microns, or less than or equal to 0.2 square microns and greater than or equal to 0.01 square microns). Other ranges are also possible.

[0172] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal can independently have an S in one or more of the above ranges. m value.

[0173] Another example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is S bi , which is the height difference between the 95th percentile cross-sectional height (i.e., the height value greater than 95% of the heights in the cross section) and the height of the average line. In some embodiments, the layer containing lithium metal has the following S biValue: less than or equal to 2 microns, less than or equal to 1.75 microns, less than or equal to 1.5 microns, less than or equal to 1.25 microns, less than or equal to 1.1 microns, less than or equal to 1 micron, less than or equal to 0.95 microns, less than or equal to 0.9 microns, less than or equal to 0.85 microns, less than or equal to 0.8 microns, less than or equal to 0.6 microns, less than or equal to 0.4 microns, less than or equal to 0.35 microns, less than or equal to 0.3 microns, less than or equal to 0.25 microns, less than or equal to 0.2 microns, less than or equal to 0.15 microns, or less than or equal to 0.125 microns. In some embodiments, the layer comprising lithium metal has the following S bi Values: greater than or equal to 0.1 micron, greater than or equal to 0.125 micron, greater than or equal to 0.15 micron, greater than or equal to 0.2 micron, greater than or equal to 0.25 micron, greater than or equal to 0.3 micron, greater than or equal to 0.35 micron, greater than or equal to 0.4 micron, greater than or equal to 0.6 micron, greater than or equal to 0.8 micron, greater than or equal to 0.85 micron, greater than or equal to 0.9 micron, greater than or equal to 0.95 micron, greater than or equal to 1 micron, greater than or equal to 1.1 micron, greater than or equal to 1.25 micron, greater than or equal to 1.5 micron, or greater than or equal to 1.75 micron. Combinations of the above ranges are also possible (e.g., less than or equal to 2 microns and greater than or equal to 0.1 micron, or less than or equal to 0.9 micron and greater than or equal to 0.3 micron). Other ranges are also possible.

[0174] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal can independently have an S in one or more of the above ranges. bi value.

[0175] Another example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is S dq , which is the root mean square of the slope of the surface of the layer. In some embodiments, the layer comprising lithium metal has the following S dq Value: less than or equal to 100, less than or equal to 90, less than or equal to 80, less than or equal to 70, less than or equal to 60, less than or equal to 50, less than or equal to 40, less than or equal to 30, or less than or equal to 20. In some embodiments, the layer comprising lithium metal has the following S dq Values: greater than or equal to 10, greater than or equal to 20, greater than or equal to 30, greater than or equal to 40, greater than or equal to 50, greater than or equal to 60, greater than or equal to 70, greater than or equal to 80, or greater than or equal to 90. Combinations of the above ranges are also possible (e.g., less than or equal to 100 and greater than or equal to 10, or less than or equal to 80 and greater than or equal to 20). Other ranges are also possible.

[0176] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal can independently have an S in one or more of the above ranges. dq value.

[0177] Another example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is S ku , which is the kurtosis of the height distribution of the cross section. In some embodiments, the layer comprising lithium metal has the following S ku Value: less than or equal to 70, less than or equal to 60, less than or equal to 50, less than or equal to 40, less than or equal to 30, less than or equal to 25, less than or equal to 20, less than or equal to 15, less than or equal to 12.5, less than or equal to 10, less than or equal to 8, less than or equal to 6, less than or equal to 5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, or less than or equal to 2.5. In some embodiments, the layer comprising lithium metal has the following S ku Values: greater than or equal to 2, greater than or equal to 2.5, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, greater than or equal to 5, greater than or equal to 6, greater than or equal to 8, greater than or equal to 10, greater than or equal to 12.5, greater than or equal to 15, greater than or equal to 20, greater than or equal to 25, greater than or equal to 30, greater than or equal to 40, greater than or equal to 50, or greater than or equal to 60. Combinations of the above ranges are also possible (for example, less than or equal to 70 and greater than or equal to 2, or less than or equal to 15 and greater than or equal to 2). Other ranges are also possible.

[0178] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal can independently have an S in one or more of the above ranges. ku value.

[0179] Another example of a parameter that can be used to characterize the roughness of a layer comprising lithium metal is S sk , which is the skewness of the height distribution of the cross section. In some embodiments, the layer comprising lithium metal has the following S skValue: less than or equal to 5, less than or equal to 4.5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, less than or equal to 2.5, less than or equal to 2, less than or equal to 1.5, less than or equal to 1, less than or equal to 0.75, less than or equal to 0.5, less than or equal to 0.3, less than or equal to 0.2, less than or equal to 0.1, less than or equal to 0, less than or equal to -0.1, less than or equal to -0.2, less than or equal to -0.3, less than or equal to -0.5, less than or equal to -0.75, less than or equal to -1, or less than or equal to -1.5. In some embodiments, the layer comprising lithium metal has the following S sk Values: greater than or equal to -2, greater than or equal to -1.5, greater than or equal to -1, greater than or equal to -0.75, greater than or equal to -0.5, greater than or equal to -0.3, greater than or equal to -0.2, greater than or equal to -0.1, greater than or equal to 0, greater than or equal to 0.1, greater than or equal to 0.2, greater than or equal to 0.3, greater than or equal to 0.5, greater than or equal to 0.75, greater than or equal to 1, greater than or equal to 1.5, greater than or equal to 2, greater than or equal to 2.5, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, or greater than or equal to 4.5. Combinations of the above ranges are also possible (e.g., less than or equal to 5 and greater than or equal to -2, or less than or equal to 3 and greater than or equal to -0.2). Other ranges are also possible.

[0180] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal can independently have an S in one or more of the above ranges. ku value.

[0181] As described above, in some embodiments, the layer containing lithium metal also contains one or more substances other than lithium metal. For example, the layer containing lithium can also contain metals, non-metals and / or metalloids. Suitable metals include aluminum, magnesium, indium and / or tin (for example, one or more such metals can form alloys with lithium metal). Suitable non-metals include carbon, oxygen, hydrogen (for example, in the form of hydrides, covalently bonded to carbon), sulfur, nitrogen, selenium and various halogens (for example, fluorine, bromine, iodine). Suitable metalloids include boron, silicon, antimony and tellurium. In some embodiments, the layer containing lithium contains lithium and also contains two or more other substances (for example, two or more non-metals). Also as described above, such substances can form a single phase with lithium metal (for example, in the form of an alloy) or a phase (for example, a non-electroactive phase, a phase containing ceramics) present in the layer in addition to the phase containing lithium metal. The phase separated from the phase containing lithium metal can have one or more features (for example, chemical composition) described elsewhere herein about the passivation layer.

[0182] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal can independently include one or more of the above-described substances.

[0183] In some embodiments, the first electrode comprises an electroactive material comprising at least 50% lithium by weight. In some cases, the electroactive material comprises at least 75%, at least 90%, at least 95%, or at least 99% lithium by weight.

[0184] When the article for inclusion in an electrochemical cell includes two or more layers comprising lithium metal, each layer comprising lithium metal can independently include an amount of lithium within one or more of the above ranges.

[0185] In some embodiments, the layer comprising lithium metal also comprises both carbon and oxygen. In such a layer, the ratio of carbon to oxygen can generally be selected as desired. For example, the ratio of carbon to oxygen can be greater than or equal to 0, greater than or equal to 0.01, greater than or equal to 0.02, greater than or equal to 0.05, greater than or equal to 0.075, greater than or equal to 0.1, greater than or equal to 0.15, greater than or equal to 0.2, greater than or equal to 0.25, greater than or equal to 0.3, greater than or equal to 0.35, greater than or equal to 0.4, or greater than or equal to 0.45. In some embodiments, the ratio of carbon to oxygen in the layer containing lithium metal is less than or equal to 0.5, less than or equal to 0.45, less than or equal to 0.4, less than or equal to 0.35, less than or equal to 0.3, less than or equal to 0.25, less than or equal to 0.2, less than or equal to 0.15, less than or equal to 0.1, less than or equal to 0.075, less than or equal to 0.05, less than or equal to 0.02, or less than or equal to 0.01. Combinations of the above ranges are also possible (e.g., greater than or equal to 0 and less than or equal to 0.1, or greater than or equal to 0.01 and less than or equal to 0.5). Other ranges are also possible. The ratio of carbon to oxygen in the layer containing lithium metal can be determined by energy dispersive spectroscopy.

[0186] When the article for inclusion in an electrochemical cell includes two or more layers comprising lithium metal, each layer comprising lithium metal can independently have a carbon to oxygen ratio within one or more of the above ranges.

[0187] In some embodiments, the layer containing lithium metal also contains both carbon and sulfur. In such a layer, the ratio of carbon to sulfur can generally be selected as desired. For example, the ratio of carbon to sulfur can be greater than or equal to 0, greater than or equal to 0.01, greater than or equal to 0.02, greater than or equal to 0.05, greater than or equal to 0.075, greater than or equal to 0.1, greater than or equal to 0.15, greater than or equal to 0.2, greater than or equal to 0.25, greater than or equal to 0.3, greater than or equal to 0.35, or greater than or equal to 0.4. In some embodiments, the ratio of carbon to sulfur in the layer containing lithium metal is less than or equal to 0.45, less than or equal to 0.4, less than or equal to 0.35, less than or equal to 0.3, less than or equal to 0.25, less than or equal to 0.2, less than or equal to 0.15, less than or equal to 0.1, less than or equal to 0.075, less than or equal to 0.05, less than or equal to 0.02, or less than or equal to 0.01. Combinations of the above ranges are also possible (e.g., greater than or equal to 0 and less than or equal to 0.1, or greater than or equal to 0.01 and less than or equal to 0.45). Other ranges are also possible. The ratio of carbon to sulfur in the layer comprising lithium metal can be determined by energy dispersive spectroscopy.

[0188] When the article for inclusion in an electrochemical cell includes two or more layers comprising lithium metal, each layer comprising lithium metal can independently have a carbon to sulfur ratio within one or more of the above ranges.

[0189] In some embodiments, the layer containing lithium metal also contains both carbon and fluorine. In such a layer, the ratio of carbon to fluorine can generally be selected as needed. For example, the ratio of carbon to fluorine can be greater than or equal to 0, greater than or equal to 0.01, greater than or equal to 0.02, greater than or equal to 0.05, greater than or equal to 0.075, greater than or equal to 0.1, greater than or equal to 0.15, greater than or equal to 0.2, greater than or equal to 0.25, greater than or equal to 0.3, or greater than or equal to 0.35. In some embodiments, the ratio of carbon to fluorine in the layer containing lithium metal is less than or equal to 0.4, less than or equal to 0.35, less than or equal to 0.3, less than or equal to 0.25, less than or equal to 0.2, less than or equal to 0.15, less than or equal to 0.1, less than or equal to 0.075, less than or equal to 0.05, less than or equal to 0.02, or less than or equal to 0.01. Combinations of the above ranges are also possible (e.g., greater than or equal to 0 and less than or equal to 0.1, or greater than or equal to 0.01 and less than or equal to 0.4). Other ranges are also possible. The ratio of carbon to fluorine in the layer comprising lithium metal can be determined by energy dispersive spectroscopy.

[0190] When the article for inclusion in an electrochemical cell includes two or more layers comprising lithium metal, each layer comprising lithium metal can independently have a carbon to fluorine ratio within one or more of the above ranges.

[0191] Advantageously, some layers containing lithium may have a relatively low elastic modulus. A low elastic modulus may indicate a relatively deformable (e.g., deformed when a relatively small amount of force is applied) layer containing lithium. This may advantageously enable the layer containing lithium to be compacted in a relatively easy manner to produce a layer containing lithium with a relatively low surface area. Since lithium present at the surface of the layer containing lithium may undesirably undergo depletion reactions with the electrolyte, it is believed that a layer containing lithium with a relatively low surface area advantageously reduces the rate at which such reactions occur and / or reduces the total amount of such reactions that occur during the life of the electrochemical cell.

[0192] In some embodiments, the layer comprising lithium metal has an elastic modulus of less than 4.9 GPa, less than or equal to 4.5 GPa, less than or equal to 4.25 GPa, less than or equal to 4 GPa, less than or equal to 3.75 GPa, less than or equal to 3.5 GPa, less than or equal to 3.25 GPa, less than or equal to 3 GPa, less than or equal to 2.75 GPa, less than or equal to 2.5 GPa, less than or equal to 2.25 GPa, less than or equal to 2 GPa, less than or equal to 1.75 GPa, less than or equal to 1.5 GPa, less than or equal to 1.25 GPa, or less than or equal to 1 GPa. In some embodiments, the layer comprising lithium metal has an elastic modulus greater than or equal to 0.75 GPa, greater than or equal to 1 GPa, greater than or equal to 1.25 GPa, greater than or equal to 1.5 GPa, greater than or equal to 1.75 GPa, greater than or equal to 2 GPa, greater than or equal to 2.25 GPa, greater than or equal to 2.5 GPa, greater than or equal to 2.75 GPa, greater than or equal to 3 GPa, greater than or equal to 3.25 GPa, greater than or equal to 3.5 GPa, greater than or equal to 3.75 GPa, greater than or equal to 4 GPa, greater than or equal to 4.25 GPa, or greater than or equal to 4.5 GPa. Combinations of the above ranges are also possible (e.g., less than 4.9 GPa and greater than or equal to 0.75 GPa, or less than or equal to 4 GPa and greater than or equal to 0.75 GPa). Other ranges are also possible.

[0193] The elastic modulus of the layer containing lithium metal can be determined by performing the procedure described in ASTM E2546 using the following parameters: (1) an approach speed of 1 micron / minute; (2) a contact load of 0.03 mN; (3) a load between 1-2.5 mN; (4) a load rate of twice the load; and (5) an indentation depth of 1 micron.

[0194] When the article for inclusion in an electrochemical cell includes two or more layers containing lithium metal, each layer containing lithium metal can independently have an elastic modulus within one or more of the above ranges.

[0195] In some embodiments, the layer comprising lithium metal exhibits desirable behavior during the tape test described in ASTM 3359. For example, in some embodiments, the layer comprising lithium metal does not crack, delaminate, and / or peel off the substrate on which the layer is disposed during the tape test.

[0196] When the article for inclusion in an electrochemical cell includes two or more lithium metal-containing layers, each lithium metal-containing layer may independently exhibit one or more of the characteristics described above during the tape test.

[0197] As described elsewhere herein, some embodiments relate to an article for inclusion in an electrochemical cell, the article comprising a layer comprising lithium metal and a second layer disposed on the layer comprising lithium metal. Such a second layer can be a passivation layer. Additional details about the passivation layer are provided below.

[0198] The passivation layer can passivate the layer containing lithium metal on which the passivation layer is arranged by reducing the reactivity of the layer containing lithium metal with substances to which the article for inclusion in the electrochemical cell is exposed. For example, the passivation layer can be used as a physical barrier between the surrounding environment and the layer containing lithium metal. Substances reactive with lithium metal can be transmitted through in relatively small (or zero) amounts and / or at relatively slow (or zero) speeds, thereby reducing the rate at which lithium reacts with such substances. It should be understood that although the passivation layer may be relatively impermeable to some substances reactive with lithium, such a layer may be relatively permeable to other substances. For example, the passivation layer is generally permeable to lithium ions.

[0199] The passivation layer can have various suitable thicknesses. In some embodiments, the passivation layer has a thickness of 0.01 micrometer, greater than or equal to 0.02 micrometer, greater than or equal to 0.05 micrometer, greater than or equal to 0.075 micrometer, greater than or equal to 0.1 micrometer, greater than or equal to 0.2 micrometer, greater than or equal to 0.5 micrometer, greater than or equal to 0.75 micrometer, greater than or equal to 1 micrometer, greater than or equal to 1.5 micrometers, greater than or equal to 2 micrometers, greater than or equal to 2.5 micrometers, greater than or equal to 3 micrometers, or greater than or equal to 4 micrometers. In some embodiments, the passivation layer has a thickness of less than or equal to 5 microns, less than or equal to 4 microns, less than or equal to 3 microns, less than or equal to 2.5 microns, less than or equal to 2 microns, less than or equal to 1.5 microns, less than or equal to 1 micron, less than or equal to 0.75 microns, less than or equal to 0.5 microns, less than or equal to 0.2 microns, less than or equal to 0.1 microns, less than or equal to 0.075 microns, less than or equal to 0.05 microns, or less than or equal to 0.02 microns. Combinations of the above ranges are also possible (e.g., greater than or equal to 0.01 microns and less than or equal to 5 microns). Other ranges are also possible. The thickness of the passivation layer can be determined by cross-sectional scanning electron microscopy.

[0200] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer can independently have a thickness within one or more of the above ranges.

[0201] As described above, in some embodiments, the passivation layer includes a plurality of columnar structures. When present, such structures can have various suitable aspect ratios. As used herein, aspect ratio refers to the ratio of a "first" line segment to a "second" line segment, both of which are oriented parallel to the main axis of the columnar structure and have a length equal to the length of the columnar structure projected on the main axis. The "first" line segment is a line segment that has the longest such projected length and is oriented in a direction different from that parallel to the substrate or layer on which the columnar structure is directly arranged. The "second" line segment is a line segment having the second longest such projected length. In some embodiments, the first line may correspond to the length of the columnar structure, and the second line may correspond to the width of the columnar structure.

[0202] In some embodiments, the columnar structure has an aspect ratio of greater than or equal to 0.5, greater than or equal to 0.75, greater than or equal to 1, greater than or equal to 1.25, greater than or equal to 1.5, greater than or equal to 1.75, greater than or equal to 2, greater than or equal to 2.25, greater than or equal to 2.5, greater than or equal to 2.75, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, or greater than or equal to 4.5. In some embodiments, the columnar structure has an aspect ratio of less than or equal to 5, less than or equal to 4.5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, less than or equal to 2.75, less than or equal to 2.5, less than or equal to 2.25, less than or equal to 2, less than or equal to 1.75, less than or equal to 1.5, less than or equal to 1.25, less than or equal to 1, or less than or equal to 0.75. Combinations of the above ranges are also possible (eg, greater than or equal to 0.5 and less than or equal to 5, or greater than or equal to 1 and less than or equal to 3). Other ranges are also possible. The aspect ratio of the columnar structure can be determined by cross-sectional scanning electron microscopy.

[0203] In some embodiments, the passivation layer may include one or more columnar structures having an aspect ratio within one or more of the above ranges. The passivation layer may also include a plurality of columnar structures, each of the plurality of columnar structures (or at least 50% of the plurality of columnar structures, at least 75% of the plurality of columnar structures, at least 90% of the plurality of columnar structures, or at least 95% of the plurality of columnar structures) having an aspect ratio within one or more of the above ranges. In some embodiments, the plurality of columnar structures have an average aspect ratio within one or more of the above ranges. When an article for inclusion in an electrochemical cell includes two or more passivation layers, one or more of the above features may be independently applicable to each layer.

[0204] In some embodiments, the passivation layer is porous. For example, the passivation layer can have a porosity greater than or equal to 5%, greater than or equal to 7.5%, greater than or equal to 10%, greater than or equal to 12.5%, greater than or equal to 15%, or greater than or equal to 17.5%. In some embodiments, the passivation layer has a porosity less than or equal to 20%, less than or equal to 17.5%, less than or equal to 15%, less than or equal to 12.5%, less than or equal to 10%, or less than or equal to 7.5%. Combinations of the above ranges are also possible (e.g., greater than or equal to 5% and less than or equal to 20%). Other ranges are also possible.

[0205] The porosity of the passivation layer can be determined by measuring the volume enclosed by the outer boundary of the composite passivation layer (e.g., by using an electron microscope); measuring the pore volume of the passivation layer by adopting ASTM Standard D4284-07 as described below; dividing the measured pore volume by the volume enclosed by the passivation layer and multiplying by 100%. ASTM Standard D4284-07, which is incorporated herein by reference in its entirety, can be used to generate a pore size distribution, which is plotted as the cumulative intruded pore volume according to the pore size. To calculate the porosity, the area under the curve spanning a given range on the x-axis can be calculated. Alternatively, in the case where the article includes pore sizes outside the range of pore sizes that can be accurately measured using ASTM Standard D4284-07, BET surface analysis can be used to supplement porosimetry measurements, such as described, for example, in S. Brunauer, P. H. Emmett and E. Teller, J. Am. Chem. Soc., 1938, 60, 309, which is incorporated herein by reference in its entirety.

[0206] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer can independently have a porosity within one or more of the above ranges.

[0207] The passivation layers described herein may have a variety of color spaces and a variety of one or more parameters constituting the color spaces. The passivation layers described herein may also appear visually to have a variety of colors, such as red, yellow, green, and / or blue.

[0208] In some embodiments, the passivation layer has a brightness greater than or equal to 10, greater than or equal to 12.5, greater than or equal to 15, greater than or equal to 17.5, greater than or equal to 20, greater than or equal to 22.5, greater than or equal to 25, greater than or equal to 27.5, greater than or equal to 30, greater than or equal to 35, greater than or equal to 40, greater than or equal to 45, greater than or equal to 50, greater than or equal to 55, greater than or equal to 60, greater than or equal to 65, greater than or equal to 70, greater than or equal to 75, or greater than or equal to 80. In some embodiments, the passivation layer has a brightness of less than or equal to 85, less than or equal to 80, less than or equal to 75, less than or equal to 70, less than or equal to 65, less than or equal to 60, less than or equal to 55, less than or equal to 50, less than or equal to 45, less than or equal to 40, less than or equal to 35, less than or equal to 30, less than or equal to 27.5, less than or equal to 25, less than or equal to 22.5, less than or equal to 20, less than or equal to 17.5, less than or equal to 15, or less than or equal to 12.5. Combinations of the above ranges are also possible (e.g., greater than or equal to 10 and less than or equal to 85, or greater than or equal to 20 and less than or equal to 60). Other ranges are also possible.

[0209] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer can independently have a brightness within one or more of the above ranges.

[0210] In some embodiments, the passivation layer has a red / green saturation ("a" saturation) of greater than or equal to -3, greater than or equal to -2.5, greater than or equal to -2, greater than or equal to -1.5, greater than or equal to -1, greater than or equal to -0.5, greater than or equal to 0, greater than or equal to 0.5, greater than or equal to 1, greater than or equal to 1.5, greater than or equal to 2, greater than or equal to 2.5, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, greater than or equal to 4.5, greater than or equal to 5, greater than or equal to 6, greater than or equal to 8, greater than or equal to 10, greater than or equal to 12.5, or greater than or equal to 15. In some embodiments, the passivation layer has the following red / green saturation: less than or equal to 20, less than or equal to 15, less than or equal to 12.5, less than or equal to 10, less than or equal to 8, less than or equal to 6, less than or equal to 5, less than or equal to 4.5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, less than or equal to 2.5, less than or equal to 2, less than or equal to 1.5, less than or equal to 1, less than or equal to 0.5, less than or equal to 0, less than or equal to -0.5, less than or equal to -1, less than or equal to -1.5, less than or equal to -2, or less than or equal to -2.5. Combinations of the above ranges are also possible (e.g., greater than or equal to -3 and less than or equal to 20, or greater than or equal to -1 and less than or equal to 4). Other ranges are also possible.

[0211] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer can independently have a red / green saturation within one or more of the above ranges.

[0212] In some embodiments, the passivation layer has a yellow / blue saturation ("b" saturation) of greater than or equal to -3, greater than or equal to -2.5, greater than or equal to -2, greater than or equal to -1.5, greater than or equal to -1, greater than or equal to -0.5, greater than or equal to 0, greater than or equal to 0.5, greater than or equal to 1, greater than or equal to 1.5, greater than or equal to 2, greater than or equal to 2.5, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, greater than or equal to 4.5, greater than or equal to 5, greater than or equal to 6, greater than or equal to 8, greater than or equal to 10, greater than or equal to 12.5, or greater than or equal to 15. In some embodiments, the passivation layer has the following yellow / blue saturation: less than or equal to 20, less than or equal to 15, less than or equal to 12.5, less than or equal to 10, less than or equal to 8, less than or equal to 6, less than or equal to 5, less than or equal to 4.5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, less than or equal to 2.5, less than or equal to 2, less than or equal to 1.5, less than or equal to 1, less than or equal to 0.5, less than or equal to 0, less than or equal to -0.5, less than or equal to -1, less than or equal to -1.5, less than or equal to -2, or less than or equal to -2.5. Combinations of the above ranges are also possible (e.g., greater than or equal to -3 and less than or equal to 20, or greater than or equal to -1 and less than or equal to 4). Other ranges are also possible.

[0213] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer can independently have a yellow / blue saturation within one or more of the above ranges.

[0214] In some embodiments, the passivation layer has a chromaticity of greater than or equal to -2, greater than or equal to -1.5, greater than or equal to -1, greater than or equal to -0.5, greater than or equal to 0, greater than or equal to 0.5, greater than or equal to 1, greater than or equal to 1.5, greater than or equal to 2, greater than or equal to 2.5, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, greater than or equal to 4.5, greater than or equal to 5, greater than or equal to 6, greater than or equal to 8, greater than or equal to 10, greater than or equal to 12.5, or greater than or equal to 15. In some embodiments, the passivation layer has a chromaticity of less than or equal to 20, less than or equal to 15, less than or equal to 12.5, less than or equal to 10, less than or equal to 8, less than or equal to 6, less than or equal to 5, less than or equal to 4.5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, less than or equal to 2.5, less than or equal to 2, less than or equal to 1.5, less than or equal to 1, less than or equal to 0.5, less than or equal to 0, less than or equal to -0.5, less than or equal to -1, or less than or equal to -1.5. Combinations of the above ranges are also possible (e.g., greater than or equal to -2 and less than or equal to 20, or greater than or equal to -1 and less than or equal to 5). Other ranges are also possible.

[0215] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer can independently have a chromaticity within one or more of the above ranges.

[0216] In some embodiments, the passivation layer has a hue of greater than or equal to -2°, greater than or equal to 0°, greater than or equal to 2°, greater than or equal to 5°, greater than or equal to 7.5°, greater than or equal to 10°, greater than or equal to 20°, greater than or equal to 50°, greater than or equal to 75°, greater than or equal to 100°, greater than or equal to 125°, greater than or equal to 150°, greater than or equal to 175°, greater than or equal to 200°, greater than or equal to 225°, greater than or equal to 250°, greater than or equal to 275°, greater than or equal to 300°, or greater than or equal to 325°. In some embodiments, the passivation layer has a hue of less than or equal to 360°, less than or equal to 325°, less than or equal to 300°, less than or equal to 275°, less than or equal to 250°, less than or equal to 225°, less than or equal to 200°, less than or equal to 175°, less than or equal to 150°, less than or equal to 125°, less than or equal to 100°, less than or equal to 75°, less than or equal to 50°, less than or equal to 20°, less than or equal to 10°, less than or equal to 7.5°, less than or equal to 5°, less than or equal to 2°, or less than or equal to 0°. Combinations of the above ranges are also possible (e.g., greater than or equal to -2° and less than or equal to 360°, or greater than or equal to 10° and less than or equal to 350°). Other ranges are also possible.

[0217] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer can independently have a hue within one or more of the above ranges.

[0218] In some embodiments, the passivation layer is relatively smooth. The smoothness or roughness of the passivation layer can be characterized in a variety of ways similar to those described elsewhere herein for layers containing lithium metal. The following techniques can be employed with reference to cross-sections of the passivation layer, and it should be understood that some passivation layers may include at least one cross-section having one or more of the characteristics described below, some passivation layers may consist only of cross-sections having one or more of the characteristics described below, and some passivation layers may have a morphology such that a majority of the cross-sections (e.g., at least 50% of the cross-sections, at least 75% of the cross-sections, at least 90% of the cross-sections, at least 95% of the cross-sections, or at least 99% of the cross-sections) have one or more of the following characteristics.

[0219] In some embodiments, the passivation layer has the following R aValue: less than or equal to 1.5 microns, less than or equal to 1.25 microns, less than or equal to 1 micron, less than or equal to 0.75 microns, less than or equal to 0.5 microns, less than or equal to 0.25 microns, less than or equal to 0.2 microns, less than or equal to 0.18 microns, less than or equal to 0.15 microns, less than or equal to 0.125 microns, less than or equal to 0.1 microns, or less than or equal to 0.075 microns. In some embodiments, the passivation layer has the following R a Values: greater than or equal to 0.05 microns, greater than or equal to 0.075 microns, greater than or equal to 0.1 microns, greater than or equal to 0.125 microns, greater than or equal to 0.15 microns, greater than or equal to 0.18 microns, greater than or equal to 0.2 microns, greater than or equal to 0.25 microns, greater than or equal to 0.5 microns, greater than or equal to 0.75 microns, greater than or equal to 1 micron, or greater than or equal to 1.25 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 1.5 microns and greater than or equal to 0.05 microns, or less than or equal to 1.5 microns and greater than or equal to 0.18 microns). Other ranges are also possible.

[0220] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an R in one or more of the above ranges. a value.

[0221] In some embodiments, the passivation layer has the following R q Value: less than or equal to 2.5 microns, less than or equal to 2.25 microns, less than or equal to 2 microns, less than or equal to 1.75 microns, less than or equal to 1.5 microns, less than or equal to 1.25 microns, less than or equal to 1 micron, less than or equal to 0.75 microns, less than or equal to 0.5 microns, less than or equal to 0.4 microns, less than or equal to 0.3 microns, or less than or equal to 0.2 microns. In some embodiments, the passivation layer has the following R q Values: greater than or equal to 0.1 microns, greater than or equal to 0.2 microns, greater than or equal to 0.3 microns, greater than or equal to 0.4 microns, greater than or equal to 0.5 microns, greater than or equal to 0.75 microns, greater than or equal to 1 micron, greater than or equal to 1.25 microns, greater than or equal to 1.5 microns, greater than or equal to 1.75 microns, greater than or equal to 2 microns, or greater than or equal to 2.25 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 2.5 microns and greater than or equal to 0.1 microns, or less than or equal to 2 microns and greater than or equal to 0.2 microns). Other ranges are also possible.

[0222] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an R in one or more of the above ranges. q value.

[0223] In some embodiments, the passivation layer has the following R p Value: less than or equal to 15 microns, less than or equal to 12.5 microns, less than or equal to 10 microns, less than or equal to 7.5 microns, less than or equal to 5 microns, less than or equal to 2.5 microns, less than or equal to 2 microns, less than or equal to 1.5 microns, or less than or equal to 1 micron. In some embodiments, the passivation layer has the following R p Values: greater than or equal to 0.5 microns, greater than or equal to 1 micron, greater than or equal to 1.5 microns, greater than or equal to 2 microns, greater than or equal to 2.5 microns, greater than or equal to 5 microns, greater than or equal to 7.5 microns, greater than or equal to 10 microns, or greater than or equal to 12.5 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 15 microns and greater than or equal to 0.5 microns, or less than or equal to 15 microns and greater than or equal to 1 micron). Other ranges are also possible.

[0224] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an R in one or more of the above ranges. p value.

[0225] In some embodiments, the passivation layer has the following R v Value: greater than or equal to less than or equal to -15 microns, greater than or equal to -12.5 microns, greater than or equal to -10 microns, greater than or equal to -7.5 microns, greater than or equal to -5 microns, greater than or equal to -2.5 microns, greater than or equal to -2 microns, greater than or equal to -1.5 microns, or greater than or equal to -1 micron. In some embodiments, the passivation layer has the following R v Values: less than or equal to -0.5 microns, less than or equal to -1 microns, less than or equal to -1.5 microns, less than or equal to -2 microns, less than or equal to -2.5 microns, less than or equal to -5 microns, less than or equal to -7.5 microns, less than or equal to -10 microns, or less than or equal to -12.5 microns. Combinations of the above ranges are also possible (e.g., greater than or equal to -15 microns and less than or equal to -0.5 microns, or greater than or equal to -15 microns and less than or equal to -1 micron). Other ranges are also possible.

[0226] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an R in one or more of the above ranges. v value.

[0227] In some embodiments, the passivation layer has the following R t Value: less than or equal to 30 microns, less than or equal to 25 microns, less than or equal to 20 microns, less than or equal to 15 microns, less than or equal to 10 microns, less than or equal to 7.5 microns, less than or equal to 5 microns, less than or equal to 4 microns, less than or equal to 3 microns, less than or equal to 2.5 microns, less than or equal to 2 microns, or less than or equal to 1.5 microns. In some embodiments, the passivation layer has the following R t Values: greater than or equal to 1 micron, greater than or equal to 1.5 microns, greater than or equal to 2 microns, greater than or equal to 2.5 microns, greater than or equal to 3 microns, greater than or equal to 4 microns, greater than or equal to 5 microns, greater than or equal to 7.5 microns, greater than or equal to 10 microns, greater than or equal to 15 microns, greater than or equal to 20 microns, or greater than or equal to 25 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 25 microns and greater than or equal to 1 micron, or less than or equal to 30 microns and greater than or equal to 2 microns). Other ranges are also possible.

[0228] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an R in one or more of the above ranges. t value.

[0229] In some embodiments, the passivation layer has the following R pm Value: less than or equal to 15 microns, less than or equal to 12.5 microns, less than or equal to 10 microns, less than or equal to 7.5 microns, less than or equal to 5 microns, less than or equal to 3 microns, less than or equal to 2 microns, less than or equal to 1.5 microns, less than or equal to 1 micron, or less than or equal to 0.75 microns. In some embodiments, the passivation layer has the following R pm Values: greater than or equal to 0.5 microns, greater than or equal to 0.75 microns, greater than or equal to 1 micron, greater than or equal to 1.5 microns, greater than or equal to 2 microns, greater than or equal to 3 microns, greater than or equal to 5 microns, greater than or equal to 7.5 microns, greater than or equal to 10 microns, or greater than or equal to 12.5 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 15 microns and greater than or equal to 0.5 microns, or less than or equal to 10 microns and greater than or equal to 1 micron). Other ranges are also possible.

[0230] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an R in one or more of the above ranges. pm value.

[0231] In some embodiments, the passivation layer has the following R vm Value: greater than or equal to -15 microns, greater than or equal to -12.5 microns, greater than or equal to -10 microns, greater than or equal to -7.5 microns, greater than or equal to -5 microns, greater than or equal to -3 microns, greater than or equal to -2 microns, greater than or equal to -1.5 microns, greater than or equal to 1 micron, or greater than or equal to -0.75 microns. In some embodiments, the passivation layer has the following R vm Values: less than or equal to -0.5 microns, less than or equal to -0.75 microns, less than or equal to -1 microns, less than or equal to -1.5 microns, less than or equal to -2 microns, less than or equal to -3 microns, less than or equal to -5 microns, less than or equal to -7.5 microns, less than or equal to -10 microns, or less than or equal to -12.5 microns. Combinations of the above ranges are also possible (e.g., greater than or equal to -15 microns and less than or equal to -1 micron, or greater than or equal to -10 microns and less than or equal to -0.5 microns). Other ranges are also possible.

[0232] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an R in one or more of the above ranges. vm value.

[0233] In some embodiments, the passivation layer has the following R z Value: less than or equal to 20 microns, less than or equal to 17.5 microns, less than or equal to 15 microns, less than or equal to 12.5 microns, less than or equal to 10 microns, less than or equal to 7.5 microns, less than or equal to 5 microns, or less than or equal to 2.5 microns. In some embodiments, the passivation layer has the following R z Values: greater than or equal to 1 micron, greater than or equal to 2.5 microns, greater than or equal to 5 microns, greater than or equal to 7.5 microns, greater than or equal to 10 microns, greater than or equal to 12.5 microns, greater than or equal to 15 microns, or greater than or equal to 17.5 microns. Combinations of the above ranges are also possible (e.g., less than or equal to 20 microns and greater than or equal to 1 micron). Other ranges are also possible.

[0234] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an R in one or more of the above ranges. z value.

[0235] In some embodiments, the passivation layer has the following S mValue: less than or equal to 1 square micron, less than or equal to 0.75 square micron, less than or equal to 0.5 square micron, less than or equal to 0.3 square micron, less than or equal to 0.2 square micron, less than or equal to 0.15 square micron, less than or equal to 0.1 square micron, less than or equal to 0.075 square micron, less than or equal to 0.05 square micron, less than or equal to 0.03 square micron, less than or equal to 0.02 square micron, less than or equal to 0.015 square micron, less than or equal to 0.01 square micron, less than or equal to 0.0075 square micron, less than or equal to 0.005 square micron, less than or equal to 0.003 square micron, or less than or equal to 0.002 square micron. In some embodiments, the passivation layer has the following S m Values: greater than or equal to 0.001 square microns, greater than or equal to 0.002 square microns, greater than or equal to 0.003 square microns, greater than or equal to 0.005 square microns, greater than or equal to 0.0075 square microns, greater than or equal to 0.01 square microns, greater than or equal to 0.02 square microns, greater than or equal to 0.05 square microns, greater than or equal to 0.075 square microns, greater than or equal to 0.1 square microns, greater than or equal to 0.15 square microns, greater than or equal to 0.2 square microns, greater than or equal to 0.3 square microns, greater than or equal to 0.5 square microns, or greater than or equal to 0.75 square microns. Combinations of the above ranges are also possible (e.g., less than or equal to 1 square micron and greater than or equal to 0.001 square microns, or less than or equal to 0.2 square microns and greater than or equal to 0.01 square microns). Other ranges are also possible.

[0236] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an S in one or more of the above ranges. m value.

[0237] In some embodiments, the passivation layer has the following S bi Value: less than or equal to 2 microns, less than or equal to 1.75 microns, less than or equal to 1.5 microns, less than or equal to 1.25 microns, less than or equal to 1.1 microns, less than or equal to 1 micron, less than or equal to 0.95 microns, less than or equal to 0.9 microns, less than or equal to 0.85 microns, less than or equal to 0.8 microns, less than or equal to 0.6 microns, less than or equal to 0.4 microns, less than or equal to 0.35 microns, less than or equal to 0.3 microns, less than or equal to 0.25 microns, less than or equal to 0.2 microns, less than or equal to 0.15 microns, or less than or equal to 0.125 microns. In some embodiments, the passivation layer has the following S biValues: greater than or equal to 0.1 micron, greater than or equal to 0.125 micron, greater than or equal to 0.15 micron, greater than or equal to 0.2 micron, greater than or equal to 0.25 micron, greater than or equal to 0.3 micron, greater than or equal to 0.35 micron, greater than or equal to 0.4 micron, greater than or equal to 0.6 micron, greater than or equal to 0.8 micron, greater than or equal to 0.85 micron, greater than or equal to 0.9 micron, greater than or equal to 0.95 micron, greater than or equal to 1 micron, greater than or equal to 1.1 micron, greater than or equal to 1.25 micron, greater than or equal to 1.5 micron, or greater than or equal to 1.75 micron. Combinations of the above ranges are also possible (e.g., less than or equal to 2 microns and greater than or equal to 0.1 micron, or less than or equal to 0.9 micron and greater than or equal to 0.3 micron). Other ranges are also possible.

[0238] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an S in one or more of the above ranges. bi value.

[0239] In some embodiments, the passivation layer has the following S dq Value: less than or equal to 100, less than or equal to 90, less than or equal to 80, less than or equal to 70, less than or equal to 60, less than or equal to 50, less than or equal to 40, less than or equal to 30, or less than or equal to 20. In some embodiments, the passivation layer has the following S dq Values: greater than or equal to 10, greater than or equal to 20, greater than or equal to 30, greater than or equal to 40, greater than or equal to 50, greater than or equal to 60, greater than or equal to 70, greater than or equal to 80, or greater than or equal to 90. Combinations of the above ranges are also possible (e.g., less than or equal to 100 and greater than or equal to 10, or less than or equal to 80 and greater than or equal to 20). Other ranges are also possible.

[0240] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an S in one or more of the above ranges. dq value.

[0241] In some embodiments, the passivation layer has the following S ku Value: less than or equal to 70, less than or equal to 60, less than or equal to 50, less than or equal to 40, less than or equal to 30, less than or equal to 25, less than or equal to 20, less than or equal to 15, less than or equal to 12.5, less than or equal to 10, less than or equal to 8, less than or equal to 6, less than or equal to 5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, or less than or equal to 2.5. In some embodiments, the passivation layer has the following Sku Values: greater than or equal to 2, greater than or equal to 2.5, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, greater than or equal to 5, greater than or equal to 6, greater than or equal to 8, greater than or equal to 10, greater than or equal to 12.5, greater than or equal to 15, greater than or equal to 20, greater than or equal to 25, greater than or equal to 30, greater than or equal to 40, greater than or equal to 50, or greater than or equal to 60. Combinations of the above ranges are also possible (for example, less than or equal to 70 and greater than or equal to 2, or less than or equal to 15 and greater than or equal to 2). Other ranges are also possible.

[0242] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an S in one or more of the above ranges. ku value.

[0243] In some embodiments, the passivation layer has the following S sk Value: less than or equal to 5, less than or equal to 4.5, less than or equal to 4, less than or equal to 3.5, less than or equal to 3, less than or equal to 2.5, less than or equal to 2, less than or equal to 1.5, less than or equal to 1, less than or equal to 0.75, less than or equal to 0.5, less than or equal to 0.3, less than or equal to 0.2, less than or equal to 0.1, less than or equal to 0, less than or equal to -0.1, less than or equal to -0.2, less than or equal to -0.3, less than or equal to -0.5, less than or equal to -0.75, less than or equal to -1, or less than or equal to -1.5. In some embodiments, the passivation layer has the following S sk Values: greater than or equal to -2, greater than or equal to -1.5, greater than or equal to -1, greater than or equal to -0.75, greater than or equal to -0.5, greater than or equal to -0.3, greater than or equal to -0.2, greater than or equal to -0.1, greater than or equal to 0, greater than or equal to 0.1, greater than or equal to 0.2, greater than or equal to 0.3, greater than or equal to 0.5, greater than or equal to 0.75, greater than or equal to 1, greater than or equal to 1.5, greater than or equal to 2, greater than or equal to 2.5, greater than or equal to 3, greater than or equal to 3.5, greater than or equal to 4, or greater than or equal to 4.5. Combinations of the above ranges are also possible (e.g., less than or equal to 5 and greater than or equal to -2, or less than or equal to 3 and greater than or equal to -0.2). Other ranges are also possible.

[0244] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer may independently have an S in one or more of the above ranges. ku value.

[0245] When present, the passivation layer can have a variety of suitable compositions. In some embodiments, the passivation layer comprises the reaction product of lithium metal and gas reactive with lithium metal. Therefore, in some embodiments, the passivation layer comprises one or more forms of lithium (e.g., lithium ions, ceramics comprising lithium). The passivation layer can also be deposited by a gas that has not undergone a reaction with lithium metal and / or has undergone such a reaction to a relatively low degree. Such a passivation layer can lack lithium and / or can contain a relatively small amount of lithium. For example, they can include ceramics lacking lithium and / or including a relatively small amount of lithium. Some passivation layers can include, for example, non-metals and / or metalloids. Suitable non-metals include carbon, oxygen, hydrogen, sulfur, nitrogen, selenium and various halogens (e.g., fluorine, bromine, iodine). Suitable metalloids include boron, silicon, antimony and tellurium. In some embodiments, the passivation layer includes two or more substances (e.g., two or more non-metals). Non-limiting examples of such combinations of species include: oxygen and carbon; oxygen and hydrogen; sulfur and oxygen; sulfur and carbon; sulfur, oxygen, and carbon; nitrogen and oxygen; nitrogen and hydrogen; fluorine and sulfur; fluorine, carbon, and hydrogen; fluorine and silicon; and carbon and hydrogen.

[0246] When the article for inclusion in an electrochemical cell comprises two or more passivation layers, each passivation layer may independently comprise one or more of the above-described materials.

[0247] When the passivation layer contains both carbon and oxygen, the ratio of carbon to oxygen can generally be selected as desired. For example, the ratio of carbon to oxygen can be greater than or equal to 0.01, greater than or equal to 0.02, greater than or equal to 0.05, greater than or equal to 0.075, greater than or equal to 0.1, greater than or equal to 0.15, greater than or equal to 0.2, greater than or equal to 0.25, greater than or equal to 0.3, greater than or equal to 0.35, greater than or equal to 0.4, or greater than or equal to 0.45. In some embodiments, the ratio of carbon to oxygen in the passivation layer is less than or equal to 0.5, less than or equal to 0.45, less than or equal to 0.4, less than or equal to 0.35, less than or equal to 0.3, less than or equal to 0.25, less than or equal to 0.2, less than or equal to 0.15, less than or equal to 0.1, less than or equal to 0.075, less than or equal to 0.05, or less than or equal to 0.02. Combinations of the above-referenced ranges are also possible (eg, greater than or equal to 0.01 and less than or equal to 0.5). Other ranges are also possible. The ratio of carbon to oxygen in the passivation layer can be determined by energy dispersive spectroscopy.

[0248] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer can independently have a carbon to oxygen ratio within one or more of the above ranges.

[0249] In some embodiments, the passivation layer contains both carbon and sulfur. In such a layer, the ratio of carbon to sulfur can generally be selected as needed. For example, the ratio of carbon to sulfur can be greater than or equal to 0.01, greater than or equal to 0.02, greater than or equal to 0.05, greater than or equal to 0.075, greater than or equal to 0.1, greater than or equal to 0.15, greater than or equal to 0.2, greater than or equal to 0.25, greater than or equal to 0.3, greater than or equal to 0.35, or greater than or equal to 0.4. In some embodiments, the ratio of carbon to sulfur in the passivation layer is less than or equal to 0.45, less than or equal to 0.4, less than or equal to 0.35, less than or equal to 0.3, less than or equal to 0.25, less than or equal to 0.2, less than or equal to 0.15, less than or equal to 0.1, less than or equal to 0.075, less than or equal to 0.05, or less than or equal to 0.02. Combinations of the above ranges are also possible (e.g., greater than or equal to 0.01 and less than or equal to 0.45). Other ranges are possible.The ratio of carbon to sulfur in the passivation layer can be determined by energy dispersive spectroscopy.

[0250] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer can independently have a carbon to sulfur ratio within one or more of the above ranges.

[0251] In some embodiments, the passivation layer includes both carbon and fluorine. In such a layer, the ratio of carbon to fluorine can generally be selected as needed. For example, the ratio of carbon to fluorine can be greater than or equal to 0.01, greater than or equal to 0.02, greater than or equal to 0.05, greater than or equal to 0.075, greater than or equal to 0.1, greater than or equal to 0.15, greater than or equal to 0.2, greater than or equal to 0.25, greater than or equal to 0.3, or greater than or equal to 0.35. In some embodiments, the ratio of carbon to fluorine in the passivation layer is less than or equal to 0.4, less than or equal to 0.35, less than or equal to 0.3, less than or equal to 0.25, less than or equal to 0.2, less than or equal to 0.15, less than or equal to 0.1, less than or equal to 0.075, less than or equal to 0.05, or less than or equal to 0.02. Combinations of the above ranges are also possible (e.g., greater than or equal to 0.01 and less than or equal to 0.4). Other ranges are also possible. The ratio of carbon to fluorine in the passivation layer can be determined by energy dispersive spectroscopy.

[0252] When the article for inclusion in an electrochemical cell includes two or more passivation layers, each passivation layer can independently have a carbon to fluorine ratio within one or more of the above ranges.

[0253] As described elsewhere herein, in some embodiments, the layer comprising lithium metal and / or a layer disposed thereon (eg, a passivation layer) is deposited and / or disposed on a substrate. Additional details of such substrates are provided below.

[0254] Substrates suitable for use in conjunction with modular lithium deposition systems, articles for inclusion in electrochemical cells, and methods described herein can have a variety of suitable thicknesses. In some embodiments, the substrate has a thickness of greater than or equal to 3 mils, greater than or equal to 3.5 mils, greater than or equal to 4 mils, or greater than or equal to 4.5 mils. In some embodiments, the substrate has a thickness of less than or equal to 5 mils, less than or equal to 4.5 mils, less than or equal to 4 mils, or less than or equal to 3.5 mils. Combinations of the above ranges are also possible (e.g., greater than or equal to 3 mils and less than or equal to 5 mils). Other ranges are also possible. The thickness of the substrate can be determined by a drop gauge.

[0255] The substrate can have a variety of suitable compositions. In some embodiments, the substrate comprises a polymer, such as poly(ester) (e.g., poly(ethylene terephthalate), such as optical grade poly(ethylene terephthalate)). Other examples of suitable polymers include polyolefins, polypropylene, nylon, polyvinyl chloride, and polyethylene (which may be optionally metallized). In some cases, the substrate comprises a metal (e.g., a foil such as nickel foil and / or aluminum foil), a glass, or a ceramic material. In some embodiments, the substrate includes a film that may be optionally arranged on a thicker substrate material. For example, in certain embodiments, the substrate includes one or more films, such as a polymer film (e.g., poly(ethylene terephthalate) film) and / or a metallized polymer film (using various metals such as aluminum and copper). The substrate may also include additional components, such as fillers, adhesives, and / or surfactants.

[0256] Typically, the substrate described herein is configured to be removed from the article for incorporation into the electrochemical cell before being incorporated into the electrochemical cell. In certain embodiments, the substrate can remain intact with such an article after its manufacture, but can be layered before the article is incorporated into the electrochemical cell. For example, the article for incorporation into the electrochemical cell can be packaged and shipped to the manufacturer, which can then be incorporated into the electrochemical cell. In such an embodiment, the article for incorporation into the electrochemical cell can be inserted into an airtight and / or moisture-proof package to prevent or suppress the degradation and / or contamination of one or more components of the article. Enabling the substrate to remain attached can facilitate the handling and transportation of the article for incorporation into the electrochemical cell. For example, the substrate can be relatively thick and / or can have sufficient relative rigidity and / or hardness to prevent or suppress deformation of the article for incorporation into the electrochemical cell during processing. In such an embodiment, the substrate can be removed by the manufacturer before, during, or after the assembly of the electrochemical cell.

[0257] In some embodiments, an article for inclusion in an electrochemical cell can be disposed on or deposited onto a release layer. For example, a release layer can be disposed on a substrate onto which a layer comprising lithium metal is deposited (e.g., in a modular lithium deposition system). Suitable release layers and their characteristics are described in more detail below.

[0258] The peeling layer contemplated for use with the systems, articles, and methods described herein can have a variety of suitable thicknesses. In some embodiments, the peeling layer has a thickness of greater than or equal to 2 microns, greater than or equal to 2.25 microns, greater than or equal to 2.5 microns, greater than or equal to 2.75 microns, greater than or equal to 3 microns, greater than or equal to 3.25 microns, greater than or equal to 3.5 microns, or greater than or equal to 3.75 microns. In some embodiments, the peeling layer has a thickness of less than or equal to 4 microns, less than or equal to 3.75 microns, less than or equal to 3.5 microns, less than or equal to 3.25 microns, less than or equal to 3 microns, less than or equal to 2.75 microns, less than or equal to 2.5 microns, or less than or equal to 2.25 microns. Combinations of the above ranges are also possible (e.g., greater than or equal to 2 microns and less than or equal to 4 microns). Other ranges are also possible. The thickness of the peeling layer can be determined by a drop gauge.

[0259] As described above, in some embodiments, it may be beneficial to deposit a layer comprising lithium metal onto a substrate, but it is not desirable to incorporate the substrate into an electrochemical cell comprising the resulting layer. In such embodiments, it is advantageous to position the release layer between the substrate (and any layers disposed on the substrate that are not configured to be included in the resulting electrochemical cell) and any layers that are configured to be included in the resulting electrochemical cell. When the release layer is adjacent to the substrate, the release layer may be partially or completely delaminated from the layer comprising lithium metal during subsequent steps in the formation of the electrochemical cell (e.g., if not configured to remain in the final electrochemical cell), and / or it may be partially or completely delaminated from the carrier substrate during subsequent steps in the formation of the electrochemical cell (e.g., if configured to remain in the final electrochemical cell).

[0260] In some embodiments, the release layer may have one or more features of the release layer described in U.S. Patent Publication No. 2014 / 272,565, U.S. Patent Publication No. 2014 / 272,597, and U.S. Patent Publication No. 2011 / 068,001, each of which is incorporated herein by reference in its entirety. In some embodiments, the release layer may preferably be a release layer comprising a hydroxyl functional group (e.g., comprising poly(vinyl alcohol) (PVOH) and / or EVAL) and having one of the structures described above.

[0261] In one set of embodiments, the release layer is formed of a polymer material. Specific examples of suitable polymers include, but are not limited to, polyoxides, poly(alkyl oxides) / polyalkylene oxides (e.g., polyethylene oxide, polypropylene oxide, polybutylene oxide), polyvinyl alcohol, polyvinyl butyral, polyvinyl formal, vinyl acetate-vinyl alcohol copolymers, ethylene-vinyl alcohol copolymers, vinyl alcohol-methyl methacrylate copolymers, polysiloxanes, and fluorinated polymers. Further examples of polymer materials include polysulfones, polyethersulfones, polyphenylsulfones (e.g., poly(vinyl ether sulfone) available from BASF, S 6010, S 3010 and S2010,), polyethersulfone-polyalkylene oxide copolymers, polyphenylsulfone-polyalkylene oxide copolymers, polysulfone-polyalkylene oxide copolymers, polyisobutylene (e.g., available from BASF B10, B15, B30, B80, B150 and B200), polyisobutylene succinic anhydride (PIBSA), polyisobutylene-polyalkylene oxide copolymers, polyamide 6 (e.g., available from BASF B33) (e.g., extrusion of a 2 μm polyamide layer on a polyolefin support or solution casting of a PA layer on a polyolefin support substrate), polyvinylpyrrolidone, polyvinylpyrrolidone-polyvinylimidazole copolymer (e.g., HP56), polyvinylpyrrolidone-polyvinyl acetate copolymer (e.g., available from BASF ), maleimide-vinyl ether copolymers, polyacrylamides, fluorinated polyacrylates (optionally including surface reactive comonomers), polyethylene-polyvinyl alcohol copolymers (e.g., available from BASF ), polyethylene-polyvinyl acetate copolymers, polyvinyl alcohol and polyvinyl acetate copolymers, polyoxymethylene (e.g., extruded), polyvinyl butyral (e.g., available from BASF ), polyureas (e.g., branched), photopolymerized polymers based on acrolein derivatives (CH2=CR-C(O)R), polysulfone-polyalkylene oxide copolymers, polyvinylidene fluoride (e.g., available from BASF D155) and combinations thereof.

[0262] In one embodiment, the peeling layer comprises a polyethersulfone-polyalkylene oxide copolymer. In a specific embodiment, the polyethersulfone-polyalkylene oxide copolymer is a polyarylethersulfone-polyalkylene oxide copolymer (PPC) obtained by polycondensation of a reaction mixture (RG), the reaction mixture (RG) comprising the following components: (A1) at least one aromatic dihalogen compound, (B1) at least one aromatic dihydroxy compound, and (B2) at least one polyalkylene oxide having at least two hydroxyl groups. The reaction mixture may also include (C) at least one aprotic polar solvent and (D) at least one metal carbonate, wherein the reaction mixture (RG) does not include any substance that forms an azeotrope with water. The resulting copolymer may be a random copolymer or a block copolymer. For example, the resulting copolymer may include an A1-B1 block and an A1-B2 block. In some cases, the resulting copolymer may include a block of A1-B1-A1-B2.

[0263] Other examples of polymeric materials include polyimide (e.g., ); siliconized polyester film (e.g., Mitsubishi polyester), metallized polyester film (e.g., available from Mitsubishi or Sion Power), polybenzimidazole (PBI; e.g., low molecular weight PBI - available from Celanese), polybenzoxazole (e.g., available from Foster-miller, Toyobo), ethylene-acrylic acid copolymer (e.g., available from BASF ), acrylate-based polymers (e.g., available from BASF ), (charged) polyvinylpyrrolidone-polyvinylimidazole copolymers (e.g., available from BASF HP56, ), polyacrylonitrile (PAN), styrene-acrylonitrile (SAN), thermoplastic polyurethane (e.g., available from BASF 1195A 10), polysulfone-poly(alkylene oxide) copolymers, benzophenone-modified polysulfone (PSU) polymers, polyvinyl pyrrolidone-polyvinyl acetate copolymers (e.g., available from BASF ) and their combinations.

[0264] In some embodiments, the exfoliation layer includes a substantially conductive polymer. Examples of such materials include conductive polymers (also referred to as electronic polymers or conductive polymers) doped with lithium salts (e.g., LiSCN, LiBr, LiI, LiClO4, LiAsF6, LiSO3CF3, LiSO3CH3, LiBF4, LiB(Ph)4, LiPF6, LiC(SO2CF3)3, and LiN(SO2CF3)2). Examples of conductive polymers include, but are not limited to, poly(acetylene), poly(pyrrole), poly(thiophene), poly(aniline), poly(fluorene), polynaphthalene, poly(p-phenylene sulfide), and poly(p-phenylene vinylene). Conductive additives may also be added to the polymer to form a conductive polymer.

[0265] In some embodiments, the release layer includes a cross-linkable polymer. Non-limiting examples of cross-linkable polymers include polyvinyl alcohol, polyvinyl butyral, polyvinyl pyridine, polyvinyl pyrrolidone, polyvinyl acetate, acrylonitrile butadiene styrene (ABS), ethylene propylene rubber (EPDM), EPR, chlorinated polyethylene (CPE), ethylene bisacrylamide (EBA), acrylates (e.g., alkyl acrylates, ethylene glycol acrylates, polyethylene glycol acrylates, ethylene ethyl acrylate (EEA)), hydrogenated nitrile rubber (HNBR), natural rubber, nitrile rubber (NBR), certain Fluoropolymers, silicone rubber, polyisoprene, ethylene vinyl acetate (EVA), chlorosulfonyl rubber, fluorinated poly(arylene ether) (FPAE), polyetherketone, polysulfone, polyetherimide, diepoxide, diisocyanate, diisothiocyanate, formaldehyde resin, amino resin, polyurethane, unsaturated polyether, polyethylene glycol vinyl ether, polyethylene glycol divinyl ether, their copolymers, and polymers for protective coating layers of isolation layers described in U.S. Pat. No. 6,183.901 to Ying et al., assigned to common assignee.

[0266] Additional examples of cross-linkable or cross-linked polymers include UV / E beam cross-linked or similar polymers (i.e., polymers comprising an amorphous blend of one or more of poly(sulfone), poly(ethersulfone), and poly(phenylsulfone)), UV cross-linked -Polyalkylene oxide copolymer, UV / E beam cross-linked - acrylamide blends, cross-linked polyisobutylene-polyalkylene oxide copolymers, cross-linked branched polyimide (BPI), cross-linked maleimide-polyetheramine (Jeffamine) polymers (MSI gel), cross-linked acrylamide, and combinations thereof.

[0267] Based on the general knowledge in the art and the description herein, a person skilled in the art can select an appropriate cross-linkable polymer and a suitable cross-linking method. The cross-linked polymer material can also include a salt such as a lithium salt to enhance lithium ion conductivity.

[0268] If a cross-linkable polymer is used, the polymer (or polymer precursor) may include one or more cross-linking agents. A cross-linking agent is a molecule having a reactive portion that is designed to interact with functional groups on a polymer chain in a manner that will form cross-links between one or more polymer chains. Examples of cross-linking agents that can be used to cross-link the polymer materials of the support layer described herein include, but are not limited to: polyamide-epichlorohydrin (polycup 172); aldehydes (e.g., formaldehyde and urea formaldehyde); dialdehydes (e.g., glyoxal glutaraldehyde and hydroxyhexadecaldehyde); acrylates (e.g., ethylene glycol diacrylate, di(ethylene glycol) diacrylate, tetra(ethylene glycol) diacrylate, methacrylate, ethylene glycol dimethacrylate, di(ethylene glycol) dimethacrylate, tri(ethylene glycol) dimethacrylate); amides (e.g., N,N'-methylenebisacrylamide, N,N'- ... silanes (e.g., methyltrimethoxysilane, methyltriethoxysilane, tetramethoxysilane (TMOS), tetraethoxysilane (TEOS), tetrapropoxysilane, methyltri(methylethylketoxime)silane, methyltri(acetoneoxime)silane, methyltri(methylisobutylketoxime)silane, dimethyldimethoxysilane ...ethoxysilane, tetramethoxysilane (TMOS), tetraethoxysilane (TEOS), tetrapropoxysilane, methyltri(methylethylketoxime)silane, methyltri(methylethylketoxime)silane, methyltri(acetoneoxime)silane, methyltri(methylisobutylketoxime)silane, dimethyldimethoxysilane, methyltriethoxysilane, tetramethoxysilane (TMOS), tetraethoxysilane (TEOS), tetrapropoxysilane, methyltri(methylethylketoxime)silane, methyltri(methylethylketoxime)silane, methyltri (methyl ethyl ketoxime) silane, trimethyl (methyl ethyl ketoxime) silane, vinyl tri (methyl ethyl ketoxime) silane, methyl vinyl bis (methyl ethyl ketoxime) silane, methyl vinyl bis (cyclohexane ketoxime) silane, vinyl tri (methyl isobutyl ketoxime) silane, methyl triacetoxy silane, tetraacetoxy silane and phenyl tri (methyl ethyl ketoxime) silane); divinylbenzene; melamine; ammonium zirconium carbonate; dicyclohexylcarbodiimide / dimethylaminopyridine (D CC / DMAP); 2-chloropyridinium ion; 1-hydroxycyclohexyl phenyl ketone; acetophenone dimethyl ketal; benzoyl methyl ether; aryl trifluorovinyl ether; benzocyclobutene; phenolic resins (e.g., condensates of phenol with formaldehyde and lower alcohols such as methanol, ethanol, butanol and isobutanol), epoxides; melamine resins (e.g., condensates of melamine with formaldehyde and lower alcohols such as methanol, ethanol, butanol and isobutanol); polyisocyanates; and dialdehydes.

[0269] Other types of polymers that may be suitable for use in the release layer may include, but are not limited to: polyamines (e.g., poly(ethyleneimine) and polypropyleneimine (PPI)); polyamides (e.g., poly( -caprolactam) (nylon 6), poly(hexamethylene adipamide) (nylon 66)), polyimides (e.g., polyimide, polynitrile, and poly(pyromellitimide-1,4-diphenyl ether) (Kapton)); vinyl polymers (e.g., polyacrylamide, poly(2-vinylpyridine), poly(N-vinylpyrrolidone), poly(methyl cyanoacrylate), poly(ethyl cyanoacrylate), poly(butyl cyanoacrylate), poly(isobutyl cyanoacrylate), poly(vinyl acetate), poly(vinyl alcohol) , poly(vinyl chloride), poly(vinyl fluoride), poly(2-vinylpyridine), polychlorotrifluoroethylene, and poly(isohexylcyanoacrylate)); polyacetals; polyolefins (e.g., poly(butene-1), poly(n-pentene-2), polypropylene, polytetrafluoroethylene); polyesters (e.g., polycarbonate, polybutylene terephthalate, polyhydroxybutyrate); polyethers (poly(ethylene oxide) (PEO), poly(propylene oxide) (PPO), poly(tetramethylene oxide) (PTMO)); vinylidene polymers (e.g., polyisobutylene poly(vinylidene chloride), poly(vinylidene fluoride), poly(vinylidene fluoride, poly(vinylidene fluoride) block copolymer); polyaromatic amides (e.g., poly(imino-1,3-phenyleneiminoisophthaloyl) and poly(imino-1,4-phenyleneiminoterephthaloyl)); polyheteroaromatic compounds (e.g., polybenzimidazole (PBI), polybenzobisoxazole (PBO), and polybenzobisthiazole (PBT)); polyheterocyclic compounds (e.g., polypyrrole); polyurethane; phenolic polymers (e.g., phenol formaldehyde); polyalkynes (e.g., polyacetylene); polydienes (e.g., 1,2-polybutadiene, cis- or trans-1,4-polybutadiene); polysiloxanes (e.g., poly(dimethylsiloxane) (PDMS), poly(diethylsiloxane) (PDES), polydiphenylsiloxane (PDPS), and polymethylphenylsiloxane (PMPS)); and inorganic polymers (e.g., polyphosphazenes, polyphosphonates, polysilanes, polysilazanes).

[0270] In some embodiments, the molecular weight of the polymer can be selected to achieve a specific adhesive affinity and can vary in the release layer. In some embodiments, the molecular weight of the polymer used in the release layer can be greater than or equal to 1,000 g / mol, greater than or equal to 5,000 g / mol, greater than or equal to 10,000 g / mol, greater than or equal to 15,000 g / mol, greater than or equal to 20,000 g / mol, greater than or equal to 25,000 g / mol, greater than or equal to 30,000 g / mol, greater than or equal to 50,000 g / mol, greater than or equal to 100,000 g / mol, or greater than or equal to 150,000 g / mol. In certain embodiments, the molecular weight of the polymer used in the release layer can be less than or equal to 150,000 g / mol, less than or equal to 100,000 g / mol, less than or equal to 50,000 g / mol, less than or equal to 30,000 g / mol, less than or equal to 25,000 g / mol, less than or equal to 20,000 g / mol, less than or equal to 10,000 g / mol, less than or equal to 5,000 g / mol, or less than or equal to 1,000 g / mol. Other ranges are also possible. Combinations of the above ranges are also possible (e.g., greater than or equal to 5,000 g / mol and less than or equal to 50,000 g / mol).

[0271] When a polymer is used, the polymer may be substantially cross-linked, substantially uncross-linked, or partially cross-linked, as the disclosure is not limited in this manner. Additionally, the polymer may be substantially crystalline, partially crystalline, or substantially amorphous. Without wishing to be bound by theory, embodiments in which the polymer is amorphous may exhibit a smoother surface, as crystallization of the polymer may result in increased surface roughness. In certain embodiments, the release layer is formed of or includes a wax.

[0272] As described elsewhere herein, in some embodiments, a layer comprising lithium metal and / or a layer disposed thereon (eg, a passivation layer) is deposited and / or disposed on a current collector. Further details of such current collectors are provided below.

[0273] When present, the current collector may take the form of a layer arranged on a substrate (e.g., arranged on a peeling layer on a substrate). The thickness of such a layer may generally be selected as desired. In some embodiments, the current collector has a thickness of greater than or equal to 0.1 micron, greater than or equal to 0.15 micron, greater than or equal to 0.2 micron, greater than or equal to 0.25 micron, greater than or equal to 0.3 micron, greater than or equal to 0.35 micron, greater than or equal to 0.4 micron, or greater than or equal to 0.45 micron. In some embodiments, the current collector has a thickness of less than or equal to 0.5 micron, less than or equal to 0.45 micron, less than or equal to 0.4 micron, less than or equal to 0.35 micron, less than or equal to 0.3 micron, less than or equal to 0.25 micron, less than or equal to 0.2 micron, or less than or equal to 0.15 micron. Combinations of the above ranges are also possible (e.g., greater than or equal to 0.1 micron and less than or equal to 0.5 micron). Other ranges are also possible. The thickness of the current collector may be determined by optical profilometry.

[0274] The current collector generally comprises a conductive material. For example, the current collector may comprise a metal (e.g., copper, nickel, aluminum, a passivation metal), a metallized polymer (e.g., metallized poly(ethylene terephthalate)), a conductive polymer, and / or a polymer comprising conductive particles dispersed therein.

[0275] The current collector can be formed in a variety of ways. For example, the current collector can be deposited on the electrode by physical vapor deposition, chemical vapor deposition, electrochemical deposition, sputtering, scraping, flash evaporation or any other appropriate deposition technique for the selected material. Some such processes (e.g., physical vapor deposition, chemical vapor deposition, sputtering) can be performed in the modular lithium deposition system described herein and / or can be performed on the substrate before the substrate is introduced into the modular lithium deposition system. In some embodiments, the current collector is formed separately from the article (e.g., for being incorporated into the article in the electrochemical cell) to be incorporated therein, and then incorporated into the article (and / or incorporated into the parts of the article, such as layers). However, it should be understood that in some embodiments, the article for being incorporated into the electrochemical cell may lack a current collector. This may be true when the article itself (and / or the electroactive material therein) is conductive.

[0276] As described elsewhere herein, some embodiments relate to articles for incorporation into electrochemical cells. In some embodiments, an article for incorporation into an electrochemical cell includes an anode and / or a portion of an anode (e.g., for a lithium metal electrochemical cell). Additional details of an electrochemical cell into which such an article may be incorporated are described below.

[0277] Some electrochemical cells may also include an electrolyte. In some embodiments, the electrolyte is a non-aqueous electrolyte. Suitable non-aqueous electrolytes may include organic electrolytes, such as liquid electrolytes, gel polymer electrolytes, and solid polymer electrolytes. These electrolytes may optionally include one or more ionic electrolyte salts (e.g., to provide or enhance ionic conductivity). Examples of useful non-aqueous liquid electrolyte solvents include, but are not limited to, non-aqueous organic solvents such as N-methylacetamide, acetonitrile, acetals, ketals, esters (e.g., esters of carbonic acid), carbonates (e.g., dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, propylene carbonate, ethylene carbonate, fluoroethylene carbonate, difluoroethylene carbonate), sulfones, sulfites, cyclopentanes, sulfonimides (e.g., lithium bis(trifluoromethane)sulfonyl imide), aliphatic ethers, acyclic ethers, cyclic ethers, glycol dimethyl ethers, polyethers, phosphates (e.g., hexafluorophosphates), siloxanes, dioxolanes, N-alkylpyrrolidones, nitrate-containing compounds, substituted forms of the foregoing, and blends thereof. Examples of usable acyclic ethers include, but are not limited to, diethyl ether, dipropyl ether, dibutyl ether, dimethoxymethane, trimethoxymethane, 1,2-dimethoxyethane, diethoxyethane, 1,2-dimethoxypropane and 1,3-dimethoxypropane. Examples of usable cyclic ethers include, but are not limited to, tetrahydrofuran, tetrahydropyran, 2-methyltetrahydrofuran, 1,4-dioxane, 1,3-dioxolane and trioxane. Examples of usable polyethers include, but are not limited to, diethylene glycol dimethyl ether (diglyme), triethylene glycol dimethyl ether (triglyme), tetraethylene glycol dimethyl ether (tetraglyme), higher glyme, ethylene glycol divinyl ether, diethylene glycol divinyl ether, triethylene glycol divinyl ether, dipropylene glycol dimethyl ether and butanediol ether. Examples of usable sulfones include, but are not limited to, cyclopentane sulfone, 3-methylcyclopentane sulfone and 3-cyclopentane sulfone. Fluorinated derivatives of the foregoing can also be used as liquid electrolyte solvents.

[0278] In some cases, a mixture of solvents described herein can also be used. For example, in some embodiments, the mixture of solvents is selected from the group including 1,3-dioxolane and dimethoxyethane, 1,3-dioxolane and diethylene glycol dimethyl ether, 1,3-dioxolane and triethylene glycol dimethyl ether, and 1,3-dioxolane and sulfolane. In some embodiments, the mixture of solvents includes dimethyl carbonate and ethylene carbonate. In some embodiments, the mixture of solvents includes ethylene carbonate and ethyl methyl carbonate. In some cases, the weight ratio of the two solvents in the mixture can range from about 5 weight %: 95 weight % to 95 weight %: 5 weight %. For example, in some embodiments, the electrolyte includes a mixture of 50 weight % of dimethyl carbonate: 50 weight % of ethylene carbonate. In some other embodiments, the electrolyte includes a mixture of 30 weight % of ethylene carbonate: 70 weight % of ethyl methyl carbonate. The electrolyte may include a mixture of dimethyl carbonate:ethylene carbonate having a ratio of dimethyl carbonate:ethylene carbonate of less than or equal to 50 wt %:50 wt % and greater than or equal to 30 wt %:70 wt %.

[0279] In some embodiments, the electrolyte may include a mixture of fluoroethylene carbonate and dimethyl carbonate. The weight ratio of fluoroethylene carbonate to dimethyl carbonate may be 20 wt %: 80 wt % or 25 wt %: 75 wt %. The weight ratio of fluoroethylene carbonate to dimethyl carbonate may be greater than or equal to 20 wt %: 80 wt % and less than or equal to 25 wt %: 75 wt %.

[0280] Non-limiting examples of suitable gel polymer electrolytes include polyethylene oxide, polypropylene oxide, polyacrylonitrile, polysiloxane, polyimide, polyphosphazene, polyether, sulfonated polyimide, perfluorinated membrane (NAFION resin), polydivinyl polyethylene glycol, polyethylene glycol diacrylate, polyethylene glycol dimethacrylate, derivatives of the foregoing, copolymers of the foregoing, crosslinked and network structures of the foregoing, and blends of the foregoing.

[0281] Non-limiting examples of suitable solid polymer electrolytes include polyethers, polyethylene oxides, polypropylene oxides, polyimides, polyphosphazenes, polyacrylonitrile, polysiloxanes, derivatives of the foregoing, copolymers of the foregoing, crosslinked and network structures of the foregoing, and blends of the foregoing.

[0282] In some embodiments, the electrolyte is in the form of a layer with a specific thickness. The electrolyte layer can have, for example, the following thickness: at least 1 micron, at least 5 microns, at least 10 microns, at least 15 microns, at least 20 microns, at least 25 microns, at least 30 microns, at least 40 microns, at least 50 microns, at least 70 microns, at least 100 microns, at least 200 microns, at least 500 microns or at least 1mm. In some embodiments, the thickness of the electrolyte layer is less than or equal to 1mm, less than or equal to 500 microns, less than or equal to 200 microns, less than or equal to 100 microns, less than or equal to 70 microns, less than or equal to 50 microns, less than or equal to 40 microns, less than or equal to 30 microns, less than or equal to 20 microns, less than or equal to 10 microns, or less than or equal to 5 microns. Other values ​​are also possible. Combinations of the above ranges are also possible. The thickness of the electrolyte layer can be determined by a drip gauge.

[0283] In some embodiments, the electrolyte comprises at least one lithium salt. For example, in some cases, the at least one lithium salt is selected from the group consisting of LiSCN, LiBr, LiI, LiSO3CH3, LiNO3, LiPF6, LiBF4, LiB(Ph)4, LiClO4, LiAsF6, Li2SiF6, LiSbF6, LiAlCl4, lithium bis(oxalate)borate, lithium difluoro(oxalate)borate, salts containing tri(oxalate)phosphate anions (e.g., lithium tri(oxalate)phosphate), LiCF3SO3, LiN(SO2F)2, LiN(SO2CF3)2, LiC(CnF) 2n+1 SO2)3 (wherein n is an integer ranging from 1 to 20), and (CnF 2n+1 SO2) m XLi (wherein n is an integer ranging from 1 to 20, when X is selected from oxygen or sulfur, m is 1, when X is selected from nitrogen or phosphorus, m is 2, and when X is selected from carbon or silicon, m is 3).

[0284] When present, the lithium salt may be present in the electrolyte at various suitable concentrations. In some embodiments, the lithium salt is present in the electrolyte at a concentration greater than or equal to 0.01M, greater than or equal to 0.02M, greater than or equal to 0.05M, greater than or equal to 0.1M, greater than or equal to 0.2M, greater than or equal to 0.5M, greater than or equal to 1M, greater than or equal to 2M, or greater than or equal to 5M. The lithium salt may be present in the electrolyte at a concentration less than or equal to 10M, less than or equal to 5M, less than or equal to 2M, less than or equal to 1M, less than or equal to 0.5M, less than or equal to 0.2M, less than or equal to 0.1M, less than or equal to 0.05M, or less than or equal to 0.02M. Combinations of the above ranges are also possible (e.g., greater than or equal to 0.01M and less than or equal to 10M, or greater than or equal to 0.01M and less than or equal to 5M). Other ranges are also possible.

[0285] In some embodiments, the electrolyte may include a favorable amount of LiPF6. In some embodiments, the electrolyte includes the following concentration of LiPF6: greater than or equal to 0.01M, greater than or equal to 0.02M, greater than or equal to 0.05M, greater than or equal to 0.1M, greater than or equal to 0.2M, greater than or equal to 0.5M, greater than or equal to 1M, or greater than or equal to 2M. The electrolyte may include the following concentration of LiPF6: less than or equal to 5M, less than or equal to 2M, less than or equal to 1M, less than or equal to 0.5M, less than or equal to 0.2M, less than or equal to 0.1M, less than or equal to 0.05M, or less than or equal to 0.02M. Combinations of the above ranges are also possible (e.g., greater than or equal to 0.01M and less than or equal to 5M). Other ranges are also possible.

[0286] In some embodiments, the electrolyte comprises a substance having an oxalate (borate) group (e.g., LiBOB, lithium difluoro(oxalate)borate), and the total weight of the substance having an (oxalate) borate group in the electrochemical cell may be less than or equal to 30 wt%, less than or equal to 28 wt%, less than or equal to 25 wt%, less than or equal to 22 wt%, less than or equal to 20 wt%, less than or equal to 18 wt%, less than or equal to 15 wt%, less than or equal to 12 wt%, less than or equal to 10 wt%, less than or equal to 8 wt%, less than or equal to 6 wt%, less than or equal to 5 wt%, less than or equal to 4 wt%, less than or equal to 3 wt%, less than or equal to 2 wt%, or less than or equal to 1 wt%. In some embodiments, the total weight of the material having (oxalate) borate in the electrochemical cell relative to the total weight of the electrolyte is greater than 0.2 wt%, greater than 0.5 wt%, greater than 1 wt%, greater than 2 wt%, greater than 3 wt%, greater than 4 wt%, greater than 6 wt%, greater than 8 wt%, greater than 10 wt%, greater than 15 wt%, greater than 18 wt%, greater than 20 wt%, greater than 22 wt%, greater than 25 wt%, or greater than 28 wt%. Combinations of the above ranges are also possible (e.g., greater than 0.2 wt% and less than or equal to 30 wt%, greater than 0.2 wt% and less than or equal to 20 wt%, greater than 0.5 wt% and less than or equal to 20 wt%, greater than 1 wt% and less than or equal to 8 wt%, greater than 1 wt% and less than or equal to 6 wt%, greater than 4 wt% and less than or equal to 10 wt%, greater than 6 wt% and less than or equal to 15 wt%, or greater than 8 wt% and less than or equal to 20 wt%). Other ranges are also possible.

[0287] In some embodiments, the electrolyte comprises fluoroethylene carbonate, and the total weight of fluoroethylene carbonate in the electrochemical cell, relative to the total weight of the electrolyte, can be less than or equal to 30 weight %, less than or equal to 28 weight %, less than or equal to 25 weight %, less than or equal to 22 weight %, less than or equal to 20 weight %, less than or equal to 18 weight %, less than or equal to 15 weight %, less than or equal to 12 weight %, less than or equal to 10 weight %, less than or equal to 8 weight %, less than or equal to 6 weight %, less than or equal to 5 weight %, less than or equal to 4 weight %, less than or equal to 3 weight %, less than or equal to 2 weight %, or less than or equal to 1 weight %. In some embodiments, the total weight of fluoroethylene carbonate in the electrolyte is greater than 0.2 wt %, greater than 0.5 wt %, greater than 1 wt %, greater than 2 wt %, greater than 3 wt %, greater than 4 wt %, greater than 6 wt %, greater than 8 wt %, greater than 10 wt %, greater than 15 wt %, greater than 18 wt %, greater than 20 wt %, greater than 22 wt %, greater than 25 wt %, or greater than 28 wt %. Combinations of the above ranges are also possible (e.g., less than or equal to 0.2 wt % and greater than 30 wt %, less than or equal to 15 wt % and greater than 20 wt %, or less than or equal to 20 wt % and greater than 25 wt %). Other ranges are also possible.

[0288] In some embodiments, the weight percent of one or more electrolyte components is measured prior to the first use or first discharge of the electrochemical cell using known amounts of the various components. In other embodiments, the weight percent is measured at some point during the cycle life of the cell. In some such embodiments, the cycling of the electrochemical cell can be stopped and the weight percent of the relevant components in the electrolyte can be determined using, for example, gas chromatography-mass spectrometry. Other methods, such as NMR, inductively coupled plasma mass spectrometry (ICP-MS), and elemental analysis can also be used.

[0289] In some embodiments, the electrolyte can simultaneously include multiple substances that are particularly beneficial in combination. For example, in some embodiments, the electrolyte includes fluoroethylene carbonate, dimethyl carbonate and LiPF6. The weight ratio of fluoroethylene carbonate to dimethyl carbonate can be between 20 weight %: 80 weight % and 25 weight %: 75 weight %, and the concentration of LiPF6 in the electrolyte can be about 1M (for example, between 0.05M and 2M). The electrolyte can also include lithium bis (oxalate) borate (for example, in the electrolyte, the concentration is between 0.1 weight % and 6 weight %, between 0.5 weight % and 6 weight %, or between 1 weight % and 6 weight %), and / or lithium tris (oxalate) phosphate (for example, in the electrolyte, the concentration is between 1 weight % and 6 weight %).

[0290] In some embodiments, the electrochemical devices described herein include an electrode other than an electrode comprising lithium. The electrode may be a cathode and / or a positive electrode (eg, an electrode that is reduced during discharge and oxidized during charge).

[0291] The cathode and / or the positive electrode may comprise an electroactive material comprising a lithium intercalation compound (e.g., a compound capable of reversibly inserting lithium ions at lattice sites and / or interstitial sites). In some cases, the electroactive material comprises a lithium transition metal oxygen compound (i.e., a lithium transition metal oxide or a lithium transition metal oxo acid salt). The electroactive material may be a layered oxide (e.g., a layered oxide that is also a lithium transition metal oxygen compound). A layered oxide generally refers to an oxide having a layered structure (e.g., multiple sheets or layers stacked on top of each other). Non-limiting examples of suitable layered oxides include lithium cobalt oxide (LiCoO2), lithium nickel oxide (LiNiO2), and lithium manganese oxide (LiMnO2).

[0292] In some embodiments, the cathode and / or the positive electrode comprises a layered oxide that is lithium nickel manganese cobalt oxide (LiNi x Mn y Co z O2, also referred to as "NMC" or "NCM"). In some such embodiments, the sum of x, y, and z is 1. For example, a non-limiting example of a suitable NMC compound is LiNi 1 / 3 Mn 1 / 3 Co 1 / 3 O2. Other non-limiting examples of suitable NMC compounds include LiNi 3 / 5 Mn 1 / 5 Co 1 / 5 O2 and LiNi 7 / 10 Mn 1 / 10 Co 1 / 5 O2.

[0293] In some embodiments, the cathode and / or positive electrode comprises a layered oxide that is lithium nickel cobalt aluminum oxide (LiNi x Co y Al z O2, also referred to as "NCA"). In some such embodiments, the sum of x, y, and z is 1. For example, a non-limiting example of a suitable NCA compound is LiNi 0.8 Co 0.15 Al 0.05 O2.

[0294] In some embodiments, the electroactive material comprises a transition metal polyanion oxide (e.g., a compound comprising a transition metal, oxygen, and / or an anion having an absolute value greater than 1). A non-limiting example of a suitable transition metal polyanion oxide is lithium iron phosphate (LiFePO4, also referred to as "LFP"). Another non-limiting example of a suitable transition metal polyanion oxide is lithium manganese iron phosphate (LiMn x Fe 1-x PO4, also referred to as "LMFP"). A non-limiting example of a suitable LMFP compound is LiMn 0.8 Fe 0.2 PO4.

[0295] In some embodiments, the electroactive material includes a spinel (e.g., a compound having the structure AB2O4, where A can be Li, Mg, Fe, Mn, Zn, Cu, Ni, Ti, or Si, and B can be Al, Fe, Cr, Mn, or V). A non-limiting example of a suitable spinel is lithium manganese oxide (LiMn2O4, also referred to as "LMO"). Another non-limiting example is lithium manganese nickel oxide (LiNi x M 2-x O4, also referred to as "LMNO"). A non-limiting example of a suitable LMNO compound is LiNi 0.5 Mn 1.5 O4. In some cases, the electroactive material comprises Li 1.14 Mn 0.42 Ni 0.25 Co 0.29 O2 ("HC-MNC"), lithium carbonate (Li2CO3), lithium carbides (e.g., Li2C2, Li4C, Li6C2, Li8C3, Li6C3, Li4C3, Li4C5), vanadium oxides (e.g., V2O5, V2O3, V6O 13 ) and / or vanadium phosphate (e.g., lithium vanadium phosphate, such as Li3V2(PO4)3), or any combination thereof.

[0296] In some embodiments, the electroactive material in the cathode and / or the positive electrode comprises a conversion compound. For example, the electroactive material may be a lithium conversion material. It has been recognized that a cathode comprising a conversion compound may have a relatively large specific capacity. Without wishing to be bound by a particular theory, a relatively large specific capacity may be achieved by utilizing all possible oxidation states of the compound via a conversion reaction in which more than one electron transfer occurs per transition metal (e.g., compared to 0.1 to 1 electron transfers embedded in the compound). Suitable conversion compounds include, but are not limited to, transition metal oxides (e.g., Co3O4), transition metal hydrides, transition metal sulfides, transition metal nitrides, and transition metal fluorides (e.g., CuF2, FeF2, FeF3). Transition metals generally refer to elements whose atoms have partially filled d subshells (e.g., Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, Cd, Hf, Ta, W, Re, Os, Ir, Pt, Au, Hg, Rf, Db, Sg, Bh, Hs).

[0297] In some cases, the electroactive material may include a material doped with one or more dopants to change the electrical properties (eg, conductivity) of the electroactive material. Non-limiting examples of suitable dopants include aluminum, niobium, silver, and zirconium.

[0298] In some embodiments, the electroactive material in the cathode and / or the positive electrode may include sulfur. In some embodiments, the electrode as the cathode may include an electroactive sulfur-containing material. As used herein, "electroactive sulfur-containing material" refers to an electroactive material comprising elemental sulfur in any form, wherein the electrochemical activity involves oxidation or reduction of sulfur atoms or parts. As an example, the electroactive sulfur-containing material may include elemental sulfur (e.g., S8). In some embodiments, the electroactive sulfur-containing material includes a mixture of elemental sulfur and sulfur-containing polymers. Therefore, suitable electroactive sulfur-containing materials may include, but are not limited to, elemental sulfur, organic or inorganic sulfides or polysulfides (e.g., alkali metals), and organic materials comprising sulfur atoms and carbon atoms, which may or may not be polymerized. Suitable organic materials include, but are not limited to, those that also include heteroatoms, conductive polymer segments, composite materials, and conductive polymers. In some embodiments, the electroactive sulfur-containing material in the second electrode (e.g., cathode) includes at least 40% by weight of sulfur. In some cases, the electroactive sulfur-containing material includes at least 50% by weight, at least 75% by weight, or at least 90% by weight of sulfur.

[0299] Examples of sulfur-containing polymers include those described in U.S. Pat. Nos. 5,601,947 and 5,690,702 to Skotheim et al., U.S. Pat. Nos. 5,529,860 and 6,117,590 to Skotheim et al., U.S. Pat. No. 6,201,100 issued March 13, 2001 to Gorkovenko et al., and PCT Publication No. WO99 / 33130. Other suitable electroactive sulfur-containing materials containing polysulfide bonds are described in U.S. Pat. No. 5,441,831 to Skotheim et al., U.S. Pat. No. 4,664,991 to Perichaud et al., and U.S. Pat. Nos. 5,723,230, 5,783,330, 5,792,575, and 5,882,819 to Naoi et al. Still further examples of electroactive sulfur-containing materials include those containing disulfide groups as described, for example, in U.S. Pat. No. 4,739,018 to Armand et al.; U.S. Pat. Nos. 4,833,048 and 4,917,974 both to De Jonghe et al.; U.S. Pat. Nos. 5,162,175 and 5,516,598 both to Visco et al.; and U.S. Pat. No. 5,324,599 to Oyama et al.

[0300] As described herein, in some embodiments, the electrochemical cell includes a separator. The separator generally comprises a polymer material (e.g., a polymer material that swells or does not swell when exposed to an electrolyte). In some embodiments, the separator is located between the electrolyte and the electrode (e.g., between the electrolyte and the electrode comprising a layer comprising lithium and / or a passivation layer, between the electrolyte and the anode and / or the negative electrode, between the electrolyte and the cathode and / or the positive electrode) and / or between two electrodes (e.g., between the anode and the cathode, between the positive electrode and the negative electrode).

[0301] The separator can be configured to inhibit (e.g., prevent) physical contact between two electrodes (e.g., between an anode and a cathode, between a positive electrode and a negative electrode), which may result in a short circuit in the electrochemical cell. The separator can be configured to be substantially non-conductive, which can reduce the tendency of current to flow through the separator, thereby reducing the likelihood of a short circuit through the separator. In some embodiments, all or one or more portions of the separator can be made of a material having at least 10 4 Ohm meter, at least 10 5 Ohm meter, at least 10 10 Ohm meter, at least 10 15 Ohm meter or at least 10 20 The bulk electronic resistivity of the material is formed in ohms per meter. The bulk electronic resistivity can be measured at room temperature (eg, 25° C.).

[0302] In some embodiments, the separator can be ionically conductive, while in other embodiments, the separator is substantially non-ionically conductive. In some embodiments, the separator has an average ionic conductivity of at least 10 -7 S / cm, at least 10 -6 S / cm, at least 10 -5 S / cm, at least 10 -4 S / cm, at least 10 -2 S / cm or at least 10 -1 In some embodiments, the average ionic conductivity of the separator may be less than or equal to 1 S / cm, less than or equal to 10 -1 S / cm, less than or equal to 10 -2 S / cm, less than or equal to 10 -3 S / cm, less than or equal to 10 -4 S / cm, less than or equal to 10 -5 S / cm, less than or equal to 10 -6 S / cm, less than or equal to 10 -7 S / cm, or less than or equal to 10 -8 S / cm. Combinations of the above-referenced ranges are also possible (e.g., an average ionic conductivity of at least 10 -8 S / cm and less than or equal to 10 -1 S / cm). Other values ​​of ionic conductivity are also possible.

[0303] The average ionic conductivity of the separator can be determined by measuring the average resistivity of the separator under a series of increasing pressures using a conductivity bridge (i.e., an impedance measurement circuit) until the average resistivity of the separator does not change with increasing pressure. This value is considered to be the average resistivity of the separator, and its reciprocal is considered to be the average conductivity of the separator. The conductivity bridge can be operated at 1 kHz. The average ionic conductivity of the separator can be determined by two copper cylinders positioned on opposite sides of the separator at 500 kg / cm 2 The two copper cylinders are capable of applying at least 3 tons / cm to the isolation member. 2 The average ionic conductivity can be measured at room temperature (eg, 25° C.).

[0304] In some embodiments, the separator may be solid. The separator may be sufficiently porous so that it allows the electrolyte solvent to pass through it. In some embodiments, the separator contains substantially no solvent (e.g., which may be different from a gel that contains solvent throughout its volume) other than the solvent that may pass through the pores of the separator or reside in the pores of the separator. In other embodiments, the separator may be in the form of a gel.

[0305] The spacer may comprise a variety of materials. The spacer may comprise one or more polymers (e.g., the spacer may be a polymer, the spacer may be formed from one or more polymers), and / or may comprise an inorganic material (e.g., the spacer may be inorganic, the spacer may be formed from one or more inorganic materials).

[0306] Examples of suitable polymers that may be used in the separator include, but are not limited to, polyolefins (e.g., polyethylene, poly(butene-1), poly(n-pentene-2), polypropylene, polytetrafluoroethylene); polyamines (e.g., poly(ethyleneimine) and polypropyleneimine (PPI)); polyamides (e.g., polyamide (nylon), poly( -caprolactam) (nylon 6), poly(hexamethylene adipamide) (nylon 66)); polyimides (e.g., polyimide, polynitrile, and poly(pyromellitimide-1,4-diphenyl ether) ); polyetheretherketone (PEEK); vinyl polymers (e.g., polyacrylamide, poly(2-vinylpyridine), poly(N-vinylpyrrolidone), poly(methyl cyanoacrylate), poly(ethyl cyanoacrylate), poly(butyl cyanoacrylate), poly(isobutyl cyanoacrylate), poly(vinyl acetate), poly(vinyl alcohol), poly(vinyl chloride), poly(vinyl fluoride), poly(2-vinylpyridine), vinyl polymers, polychlorotrifluoroethylene, and poly(isohexylcyanoacrylate)); polyacetals; polyesters (e.g., polycarbonate, polybutylene terephthalate, polyhydroxybutyrate); polyethers (poly(ethylene oxide) (PEO), poly(propylene oxide) (PPO), poly(tetramethylene oxide) (PTMO)); vinylidene polymers (e.g., polyisobutylene, poly(methyl styrene), poly(methyl methacrylate) (PMMA), poly(vinylidene chloride), poly(vinyl fluoride), poly(vinyl fluoride), poly(vinyl fluoride), poly(2-vinylpyridine), vinyl polymers, polychlorotrifluoroethylene, and poly(isohexylcyanoacrylate)); poly(vinylidene fluoride)); polyaromatic amides (e.g., poly(imino-1,3-phenyleneiminoisophthaloyl) and poly(imino-1,4-phenyleneiminoterephthaloyl)); polyheteroaromatic compounds (e.g., polybenzimidazole (PBI), polybenzobisoxazole (PBO), and polybenzobithiazole (PBT)); polyheterocyclic compounds (e.g., polypyrrole); polyurethane; phenolic polymers (e.g., phenol-formaldehyde); polyalkynes (e.g., polyacetylene); polydienes (e.g., 1,2-polybutadiene, cis- or trans-1,4-polybutadiene); polysiloxanes (e.g., poly(dimethylsiloxane) (PDMS), poly(diethylsiloxane) (PDES), polydiphenylsiloxane (PDPS), and polymethylphenylsiloxane (PMPS)); and inorganic polymers (e.g., polyphosphazenes, polyphosphonates, polysilanes, polysilazanes). In some embodiments, the polymer can be selected from poly (n-pentene-2), polypropylene, polytetrafluoroethylene, polyamide (e.g., polyamide (nylon), poly ( -caprolactam) (nylon 6), poly(hexamethylene adipamide) (nylon 66)), polyimides (e.g., polynitrile and poly(pyromellitimide-1,4-diphenyl ether) ), polyetheretherketone (PEEK) and combinations thereof.

[0307] Non-limiting examples of suitable inorganic separator materials include glass fibers.For example, in some embodiments, the electrochemical cell includes a separator that is a glass fiber filter paper.

[0308] When present, the separator can be porous. In some embodiments, the pore size of the separator is less than or equal to 5 microns, less than or equal to 3 microns, less than or equal to 1 micron, less than or equal to 500nm, less than or equal to 300nm, less than or equal to 100nm, or less than or equal to 50nm. In some embodiments, the pore size of the separator is greater than or equal to 50nm, greater than or equal to 100nm, greater than or equal to 300nm, greater than or equal to 500nm, greater than or equal to 1 micron, or greater than or equal to 3 microns. Other values ​​are also possible. Combinations of the above ranges are also possible (e.g., less than or equal to 5 microns and greater than or equal to 50nm, less than or equal to 300nm and greater than or equal to 100nm, less than or equal to 1 micron and greater than or equal to 300nm, or less than or equal to 5 microns and greater than or equal to 500nm). In some embodiments, the separator is substantially non-porous. That is, the separator may be free of holes, include a minimum number of holes, and / or do not include holes in most of them.

[0309] The electrochemical cells described herein and articles for inclusion in the electrochemical cells described herein can be subjected to applied anisotropic forces (e.g., for articles for inclusion in the electrochemical cells described herein, after being included in the electrochemical cell). As understood in the art, an "anisotropic force" is a force that is unequal in all directions. In some embodiments, the electrochemical cell and / or the article for inclusion in the electrochemical cell can be configured to withstand the applied anisotropic forces while maintaining their structural integrity (e.g., for articles for inclusion in the electrochemical cell, after being included in the electrochemical cell). The applied anisotropic forces can also enhance the morphology of the article for inclusion in the electrochemical cell (e.g., for the article for inclusion in the electrochemical cell, after being included in the electrochemical cell) and / or the morphology of the electrodes in the electrochemical cell (e.g., including articles for inclusion in the electrochemical cells described elsewhere herein and / or electrodes formed by articles for inclusion in the electrochemical cells described elsewhere herein). The electrochemical cells described herein can be adapted and arranged such that during at least one time period during charging and / or discharging thereof, an anisotropic force having a component perpendicular to the active surface of an electrode within the electrochemical cell (e.g., an electrode comprising and / or formed from an article for inclusion in an electrochemical cell described elsewhere herein) is applied to the cell.

[0310] In some such cases, the anisotropic force includes a component perpendicular to the active surface of an electrode within an electrochemical cell (e.g., including an article for inclusion in an electrochemical cell described elsewhere herein and / or an electrode formed by an article for inclusion in an electrochemical cell described elsewhere herein). As used herein, the term "active surface" is used to describe the surface of an electrode on which an electrochemical reaction can occur. Forces having a "normal component" relative to a surface are given their ordinary meaning as understood by those of ordinary skill in the art, and include, for example, forces that exert themselves at least partially in a direction substantially perpendicular to the surface. For example, in the case of a horizontal table, where an object rests on the table and is affected only by gravity, the object exerts a force that is substantially completely perpendicular to the surface of the table. If the object is also pushed laterally through the horizontal table surface, it exerts a force on the table that, while not completely perpendicular to the horizontal surface, includes a component perpendicular to the table surface. Other examples of these terms will be understood by those of ordinary skill in the art, particularly as applied in the specification of the present disclosure. In the case of a curved surface (e.g., a concave surface or a convex surface), the component of the anisotropic force perpendicular to the active surface of the electrode can correspond to the component perpendicular to the plane tangent to the curved surface at the point where the anisotropic force is applied. In some cases, the anisotropic force can be applied at one or more predetermined locations, and in some cases can be distributed over the active surface of the electrode. In some embodiments, the anisotropic force is uniformly applied to the active surface of the electrode, the electrode comprising an article for inclusion in an electrochemical cell described elsewhere herein and / or formed by an article for inclusion in an electrochemical cell described elsewhere herein.

[0311] When an anisotropic force is applied to the electrochemical cell (e.g., during charging and / or discharging of the cell), any of the electrochemical cell characteristics and / or performance metrics described herein can be achieved alone or in combination with each other. In some embodiments, the anisotropic force applied to an electrode (e.g., an electrode including an article for inclusion in an electrochemical cell described elsewhere herein and / or formed by an article for inclusion in an electrochemical cell described elsewhere herein) and / or an electrochemical cell (e.g., during at least one time period during charging and / or discharging of the cell) can include a component perpendicular to the active surface of the electrode.

[0312] In some embodiments, the component of the anisotropic force perpendicular to the active surface of an electrode (e.g., an electrode comprising and / or formed from an article for inclusion in an electrochemical cell described elsewhere herein) defines a pressure of greater than or equal to 1 kg f / cm 2 , greater than or equal to 2kg f / cm 2 , greater than or equal to 4kgf / cm 2 , greater than or equal to 6kg f / cm 2 , greater than or equal to 7.5kg f / cm 2 , greater than or equal to 8kg f / cm 2 , greater than or equal to 10kg f / cm 2 , greater than or equal to 12kg f / cm 2 , greater than or equal to 14kg f / cm 2 , greater than or equal to 16kg f / cm 2 , greater than or equal to 18kg f / cm 2 , greater than or equal to 20kg f / cm 2 , greater than or equal to 22kg f / cm 2 , greater than or equal to 24kg f / cm 2 , greater than or equal to 26kg f / cm 2 , greater than or equal to 28kg f / cm 2 , greater than or equal to 30kg f / cm 2 , greater than or equal to 32kg f / cm 2 , greater than or equal to 34kg f / cm 2 , greater than or equal to 36kg f / cm 2 , greater than or equal to 38kg f / cm 2 , greater than or equal to 40kg f / cm 2 , greater than or equal to 42kg f / cm 2 , greater than or equal to 44kg f / cm 2 , greater than or equal to 46kg f / cm 2 , greater than or equal to 48kg f / cm 2 In some embodiments, the component of the anisotropic force perpendicular to the active surface may, for example, define a pressure of less than or equal to 50 kg f / cm 2, less than or equal to 48 kg f / cm 2 , less than or equal to 46 kg f / cm 2 , less than or equal to 44kg f / cm 2 , less than or equal to 42 kg f / cm 2 , less than or equal to 40 kg f / cm 2 , less than or equal to 38kg f / cm 2 , less than or equal to 36 kg f / cm 2 , less than or equal to 34 kg f / cm 2 , less than or equal to 32kg f / cm 2 , less than or equal to 30 kg f / cm 2 , less than or equal to 28 kg f / cm 2 , less than or equal to 26kg f / cm 2 , less than or equal to 24 kg f / cm 2 , less than or equal to 22 kg f / cm 2 , less than or equal to 20kg f / cm 2 , less than or equal to 18 kg f / cm 2 , less than or equal to 16 kg f / cm 2 , less than or equal to 14kg f / cm 2 , less than or equal to 12 kg f / cm 2 , less than or equal to 10 kg f / cm 2 , less than or equal to 8kg f / cm 2 , less than or equal to 6kg f / cm 2 , less than or equal to 4kg f / cm 2 , less than or equal to 2kg f / cm 2 or less. Combinations of the above ranges are also possible (e.g., greater than or equal to 1 kg f / cm2 And less than or equal to 50kg f / cm 2 ). Other ranges are also possible.

[0313] The anisotropic force applied during at least a portion of the charge and / or discharge can be applied using any method known in the art. In some embodiments, a compression spring can be used to apply the force. Other elements (inside or outside the container structure) can be used to apply the force, and the other elements include but are not limited to Belle's washers, machine screws, pneumatic devices and / or weights, etc. In some cases, the battery can be pre-compressed before being inserted into the container structure, and once inserted into the container structure, they can expand to generate a net force on the battery. For example, a suitable method for applying such a force is described in detail in U.S. Patent No. 9,105,938, which is incorporated herein by reference in its entirety.

[0314] The following applications are incorporated herein by reference in their entirety for all purposes: U.S. Patent Publication No. US2007 / 0221265, published on September 27, 2007, filed as Application No. 11 / 400,781 on April 6, 2006, and entitled “Rechargeable Lithium / Water, Lithium / Air Batteries”; U.S. Patent Publication No. US2009 / 0035646, published on February 5, 2009, filed as Application No. 11 / 888,339 on July 31, 2007, and entitled “Swelling Inhibition in Batteries”; U.S. Patent Publication No. US2010 / 0129699, published on May 17, 2010, filed as Application No. 12 / 312,674 on February 2, 2010, patented as U.S. Patent No. 8,617,748 on December 31, 2013, and entitled “Separation of Electrolytes”; U.S. Patent Publication No. US2010 / 0291442, published on November 18, 2010, filed as Application No. 12 / 682,011 on July 30, 2010, patented as U.S. Patent No. 8,871,387 on October 28, 2014, and entitled “Primer for Battery Electrode”; U.S. Patent Publication No. US2009 / 0200986, published on August 31, 2009, filed as Application No. 12 / 069,335 on February 8, 2008, patented as U.S. Patent No. 8,264,205 on September 11, 2012, and entitled “Circuit for Charge and / or Discharge Protection in an Energy-Storage Device”; U.S. Patent Publication No. US2007 / 0224502, published on September 27, 2007, filed as Application No. 11 / 400,025 on April 6, 2006, patented as U.S. Patent No. 7,771,870 on August 10, 2010, and entitled “Electrode Protection in Both Aqueous and Non-Aqueous Electrochemical cells, Including Rechargeable Lithium Batteries”;U.S. Patent Publication No. US2008 / 0318128, published on December 25, 2008, filed as Application No. 11 / 821,576 on June 22, 2007, and entitled “Lithium Alloy / Sulfur Batteries”; U.S. Patent Publication No. US2002 / 0055040, published on May 9, 2002, filed as Application No. 09 / 795,915 on February 27, 2001, patented on May 10, 2011 as U.S. Patent No. 7,939,198, and entitled “Novel Composite Cathodes, Electrochemical Cells Comprising Novel Composite Cathodes, and Processes for Fabricating Same”; U.S. Patent Publication No. US2006 / 0238203, published on October 26, 2006, filed as Application No. 11 / 111,262 on April 20, 2005, issued as U.S. Patent No. 7,688,075 on March 30, 2010, and entitled “Lithium Sulfur Rechargeable Battery Fuel Gauge Systems and Methods”; U.S. Patent Publication No. US2008 / 0187663, published on August 7, 2008, filed as Application No. 11 / 728,197 on March 23, 2007, issued as U.S. Patent No. 8,084,102 on December 27, 2011, and entitled “Methods for Co-Flash Evaporation of Polymerizable Monomers and Non-Polymerizable Carrier Solvent / Salt Mixtures / Solutions”; U.S. Patent Publication No. US2011 / 0006738, published on January 13, 2011, filed as Application No. 12 / 679,371 on September 23, 2010, and entitled “Electrolyte Additives for Lithium Batteries and Related Methods”;U.S. Patent Publication No. US2011 / 0008531, published on January 13, 2011, filed as Application No. 12 / 811,576 on September 23, 2010, issued as U.S. Patent No. 9,034,421 on May 19, 2015, and entitled “Methods of Forming Electrodes Comprising Sulfur and Porous Material Comprising Carbon”; U.S. Patent Publication No. US2010 / 0035128, published on February 11, 2010, filed as Application No. 12 / 535,328 on August 4, 2009, issued as U.S. Patent No. 9,105,938 on August 11, 2015, and entitled “Application of Force in Electrochemical Cells”; U.S. Patent Publication No. US2011 / 0165471, published on July 15, 2011, filed as Application No. 12 / 180,379 on July 25, 2008, and entitled “Protection of Anodes for Electrochemical Cells”; U.S. Patent Publication No. US2006 / 0222954, published on October 5, 2006, filed as Application No. 11 / 452,445 on June 13, 2006, patented on April 9, 2013 as U.S. Patent No. 8,415,054, and entitled “Lithium Anodes for Electrochemical ... September 23, 2010, filed as Application No. US2011 / 0165471 No. 2010 / 0239914, filed on March 19, 2010 as Application No. 12 / 727,862, and entitled “Cathode for Lithium Battery”; U.S. Patent Publication No. US2010 / 0294049, published on November 25, 2010, filed on May 22, 2009 as Application No. 12 / 471,095, issued on January 3, 2012 as U.S. Patent No. 8,087,309, and entitled “Hermetic Sample Holder and Method for Performing Microanalysis under Controlled Atmosphere Environment”;US Patent Publication No. US2011 / 00765560, published on March 31, 2011, filed as Application No. 12 / 862,581 on August 24, 2010, and entitled “Electrochemical Cells Comprising Porous Structures Comprising Sulfur”; US Patent Publication No. US2011 / 0068001, published on March 24, 2011, filed as Application No. 12 / 862,513 on August 24, 2010, and entitled “Release System for Electrochemical Cells”; US Patent Publication No. US2012 / 0048729, published on March 1, 2012, filed as Application No. 13 / 216,559 on August 24, 2011, and entitled “Electrically Non-Conductive Materials for Electrochemical Cells Comprising Sulfur”; Cells”; U.S. Patent Publication No. US2011 / 0177398, published on July 21, 2011, filed as Application No. 12 / 862,528 on August 24, 2010, and entitled “Electrochemical Cell”; U.S. Patent Publication No. US2011 / 0070494, published on March 24, 2011, filed as Application No. 12 / 862,563 on August 24, 2010, and entitled “Electrochemical Cells Comprising Porous Structures Comprising Sulfur”; U.S. Patent Publication No. US2011 / 0070491, published on March 24, 2011, filed as Application No. 12 / 862,551 on August 24, 2010, and entitled “Electrochemical Cells Comprising Porous Structures Comprising Sulfur” Sulfur"; U.S. Patent Publication No. US2011 / 0059361, published on March 10, 2011, filed as Application No. 12 / 862,576 on August 24, 2010, issued as U.S. Patent No. 9,005,009 on April 14, 2015, and entitled "Electrochemical Cells Comprising Porous Structures Comprising Sulfur";U.S. Patent Publication No. US2012 / 0070746, published on March 22, 2012, filed as Application No. 13 / 240,113 on September 22, 2011, and entitled “Low Electrolyte Electrochemical Cells”; U.S. Patent Publication No. US2011 / 0206992, published on August 25, 2011, filed as Application No. 13 / 033,419 on February 23, 2011, and entitled “Porous Structures for Energy Storage Devices”; U.S. Patent Publication No. 2013 / 0017441, published on January 17, 2013, filed as Application No. 13 / 524,662 on June 15, 2012, patented on January 17, 2017 as U.S. Patent No. 9,548,492, and entitled “Plating No. 13 / 766,862 filed on February 14, 2013, issued as U.S. Patent No. 9,077,041 on July 7, 2015, and entitled “Electrode Structure for Electrochemical Cell”; No. 13 / 789,783 filed on March 8, 2013, issued as U.S. Patent No. 9,214,678 on December 15, 2015, and entitled “Porous Support Structures, Electrodes Containing Same, and Associated Methods”; U.S. Patent Publication No. US2013 / 0095380, published on April 18, 2013, filed as Application No. 13 / 644,933 on October 4, 2012, issued on January 20, 2015 as U.S. Patent No. 8,936,870, and entitled “Electrode Structure and Method for Making the Same”;U.S. Patent Publication No. US2014 / 0123477, published on May 8, 2014, filed as Application No. 14 / 069,698 on November 1, 2013, issued as U.S. Patent No. 9,005,311 on April 14, 2015, and entitled “Electrode Active Surface Pretreatment”; U.S. Patent Publication No. US2014 / 0193723, published on July 10, 2014, filed as Application No. 14 / 150,156 on January 8, 2014, issued as U.S. Patent No. 9,559,348 on January 31, 2017, and entitled “Conductivity Control in Electrochemical Cells”; U.S. Patent Publication No. US2014 / 0255780, published on September 11, 2014, filed as Application No. 14 / 197,782 on March 5, 2014, patented on November 6, 2016 as U.S. Patent No. 9,490,478, and entitled “Electrochemical Cells Comprising Fibril Materials”; U.S. Patent Publication No. US2014 / 0272594, published on September 18, 2014, filed as Application No. 13 / 833,377 on March 15, 2013, and entitled “Protective Structures for Electrodes”; U.S. Patent Publication No. US2014 / 0272597, published on September 18, 2014, filed as Application No. 14 / 209,274 on March 13, 2014, and entitled “Protected Electrode Structures and Methods”; U.S. Patent Publication No. US2014 / 0193713, published on July 10, 2014, filed as Application No. 14 / 150,196 on January 8, 2014, patented on December 27, 2016 as U.S. Patent No. 9,531,009, and entitled “Passivation of Electrodes in Electrochemical Cells”; 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[0315] Example 1

[0316] This example describes the formation of various passivation layers by reacting a layer containing lithium metal with CO2 in a modular lithium deposition system, their chemical composition, and their performance in an electrochemical cell.

[0317] A layer containing lithium metal having a thickness of 25 micrometers was deposited onto the substrate using a modular lithium deposition system. The layer containing lithium metal was then exposed to a gas reactive with lithium to form a passivation layer disposed on the layer containing lithium metal.

[0318] These layers are Figure 22 to Figure 28 Shown in. Fig. 22 is a scanning electron micrograph of a layer containing lithium metal before forming a passivation layer disposed on the layer containing lithium metal. Figure 23 to Figure 24is a scanning electron micrograph of a layer comprising lithium metal after exposure to CO 2 , which results in the formation of a passivation layer disposed on the layer comprising lithium metal. Fig.23 Compared to the layer containing lithium metal shown in Fig.24 The layer containing lithium metal shown in is exposed to a larger amount of CO2. Figure 25 to Figure 28 is a scanning electron micrograph of an additional layer comprising lithium metal that has been exposed to CO2 to form a passivation layer disposed thereon.

[0319] Determined by energy dispersive spectroscopy Figure 22 to Figure 24 The chemical composition of both the surface and the bulk of the article depicted in FIG. Figures 29 to 34 Table 1 below summarizes the data shown in these graphs.

[0320] Table 1

[0321]

[0322] The article including a layer comprising lithium metal and a passivation layer disposed on the layer of lithium metal was incorporated into an electrochemical cell as an anode therein. One set of electrochemical cells also included a lithium iron phosphate cathode and an electrolyte comprising ethylene carbonate. The electrochemical cells were cycled. Fig.35 The discharge capacity according to the cycles of these batteries is shown. Fig.35 In FIG. 1 , data from an electrochemical cell including a layer containing lithium metal that has been exposed to a lower amount of CO2 (e.g., having a similar Fig.23 ); data from an electrochemical cell including a layer containing lithium metal that has been exposed to a higher amount of CO2 (e.g., having a morphology similar to Fig.24 The morphology shown in ). was obtained by cycling the electrochemical cell at a rate of 120 mA discharge and 30 mA recharge. Fig.35 The upper data set in , and the lower data set was obtained by cycling the electrochemical cell at a rate of 300 mA discharge and 75 mA recharge.

[0323] Another set of electrochemical cells also included a lithium cobalt oxide cathode and an ethylene carbonate electrolyte. These electrochemical cells were cycled, and Fig.36 The discharge capacity of these batteries according to the cycle is shown. Fig.35 As in FIG. 1 , data from an electrochemical cell including a layer containing lithium metal that has been exposed to a lower amount of CO2 (e.g., having a similar Fig.23); data from an electrochemical cell including a layer containing lithium metal that has been exposed to a relatively high amount of CO2 (e.g., having a similar Fig.24 ). Fig.35 As in, the upper data set for each type of electrochemical cell was obtained by cycling the electrochemical cell at a rate of 120 mA discharge and 30 mA recharge, and the lower data set was obtained by cycling the electrochemical cell at a rate of 300 mA discharge and 75 mA recharge.

[0324] The third set of electrochemical cells also included a nickel cobalt manganese (NCM 622) cathode and an ethylene carbonate electrolyte. These electrochemical cells were cycled at a rate of 300 mA discharge and 100 mA recharge. Fig.37 The discharge capacities according to the cycles of these batteries are shown.

[0325] Example 2

[0326] This example describes the morphology of various passivation layers formed by reacting a layer containing lithium metal with CO2 in a modular lithium deposition system.

[0327] A series of passivation layers were formed by reacting layers containing lithium metal with varying amounts of CO2. Figures 38 to 41 is a scanning electron micrograph of a series of such passivation layers in order of increasing CO2 exposure. Fig.42 and Fig.43 Other examples of passivation layers formed by reacting a layer containing lithium metal with CO 2 are shown.

[0328] Example 3

[0329] This example describes the morphologies of various passivation layers formed by reacting a layer containing lithium metal with various gases in a modular lithium deposition system.

[0330] The layer containing lithium metal reacts with various gases. Fig.44 and Fig.45 is a scanning electron micrograph of a layer containing lithium metal exposed to SO2 ( Fig.45 The product ratio shown in Fig.44 The article shown in is exposed to more SO2). Fig.46 and Fig.47 is a scanning electron micrograph of a layer containing lithium metal exposed to COS ( Fig.47 The product ratio shown in Fig.46 The articles shown in are exposed to more COS). Fig.48 is a scanning electron micrograph of a layer containing lithium metal exposed to SF6. Fig.49 is a scanning electron micrograph of a layer containing lithium metal exposed to acetylene.

[0331] Example 4

[0332] This example describes the morphology of various passivation layers formed by depositing the layer from a mixture of a gas containing lithium metal and a gas reactive with lithium metal to form a single layer containing both lithium metal and a ceramic that passivates the lithium metal.

[0333] In a first experiment, gaseous lithium metal and CO2 were introduced together into a module in a modular lithium deposition system to form a layer containing both lithium metal and a ceramic formed by the reaction of the lithium metal and CO2. Figure 50 to Figure 51 A side view of the resulting layer is shown, and Figure 52 to Figure 53 A top view is shown.

[0334] In a second experiment, gaseous lithium metal, CO 2 , and argon were introduced together into a module in a modular lithium deposition system to form a layer comprising lithium metal and a ceramic formed by the reaction of the lithium metal with the CO 2 . Figure 54 to Figure 55 A side view of the resulting layer is shown, and Fig.56 Example 5 shows a top view

[0335] This example illustrates several specific configurations of a modular lithium deposition system that may have specific uses.

[0336] Fig.57 A cross-section of an example of a modular lithium deposition system is shown that includes three modules, from left to right: a chamber in which a substrate is configured to be unrolled from a roll, two vacuum chambers in which one or more layers can be deposited, and a chamber in which the substrate is configured to be wrapped around a roll. Fig.58 An exploded view of this same modular lithium deposition system is shown.

[0337] Fig.59 One possible arrangement of multiple rollers, sources of lithium metal (called "deposition sources" and "lithium 'trimming' sources"), sources of gas (called "gas manifolds"), and thickness sensors is shown.

[0338] Although several embodiments of the present invention have been described and illustrated herein, a person of ordinary skill in the art will readily conceive of various other methods and / or structures for performing functions and / or obtaining results and / or one or more of the advantages described herein, and each of such changes and / or modifications is considered to be within the scope of the present invention. More generally, it will be readily understood by those skilled in the art that all parameters, dimensions, materials, and configurations described herein are intended to be exemplary, and that actual parameters, dimensions, materials, and / or configurations will depend on a specific application or multiple specific applications for which the teachings of the present invention are used. Those skilled in the art will recognize or be able to determine many equivalents of the specific embodiments of the present invention described herein using only routine experiments. Therefore, it should be understood that the foregoing embodiments are given only as examples, and within the scope of the appended claims and their equivalents, the present invention may be implemented in a manner different from that specifically described and claimed. The present invention is directed to each individual feature, system, article, material, kit, and / or method described herein. In addition, if such features, systems, articles, materials, kits, and / or methods are not mutually contradictory, any combination of two or more such features, systems, articles, materials, kits, and / or methods is included within the scope of the present invention.

[0339] All definitions, as defined and used herein, should be understood to control over dictionary definitions, definitions in documents incorporated by reference, and / or ordinary meanings of the defined terms.

[0340] Unless explicitly indicated to the contrary, the indefinite articles "a" and "an" used in the specification and claims should be understood to mean "at least one".

[0341] As used in the specification and claims, the phrase "and / or" should be understood to refer to "one or both" of the elements so combined: that is, elements that exist together in some cases and separately in other cases. Multiple elements listed with "and / or" should be interpreted in the same manner, that is, "one or more" of the elements so combined. In addition to those elements specifically identified by the "and / or" phrase, other elements may optionally be present, whether related or unrelated to those specifically identified elements. Thus, as a non-limiting example, when used in conjunction with open language such as "comprising", a reference to "A and / or B" may refer to only A (optionally including elements other than B) in one embodiment; may refer to only B (optionally including elements other than A) in another embodiment; may refer to both A and B (optionally including other elements) in yet another embodiment; and so on.

[0342] As used herein in the specification and in the claims, "or" should be understood to have the same meaning as "and / or" as defined above. For example, when the items in the list are separated, "or" or "and / or" should be interpreted as inclusive, i.e., including at least one of a plurality of elements or a list of elements, but also including more than one, and optional other unlisted items. Only terms such as "only one" or "just one" that are clearly indicated in the opposite direction or when "consisting of..." is used in the claims will refer to including just one element in a plurality of elements or a list of elements. In general, the term "or" used herein in front of an exclusive term (such as "any", "one of", "only one of them" or "just one of them") should only be interpreted as indicating exclusive alternatives (i.e., "one or the other but not both"). When "consisting essentially of..." is used in the claims, it should have the common meaning used in the field of patent law.

[0343] As used herein in the specification and claims, when referring to a list of one or more elements, the phrase "at least one" should be understood to refer to at least one element selected from any one or more elements in the list of elements, but does not necessarily include at least one of each element specifically listed in the list of elements, and does not exclude any combination of elements in the list of elements. This definition also allows that elements other than the elements specifically identified in the list of elements to which the phrase "at least one" refers may optionally be present, whether or not related to those specifically identified elements. Thus, as a non-limiting example, "at least one of A and B" (or, equivalently, "at least one of A or B", or equivalently "at least one of A and / or B") may refer to at least one (optionally including more than one) A without B (and optionally including elements other than B) in one embodiment; to at least one (optionally including more than one) B without A (and optionally including elements other than A) in another embodiment; to at least one (optionally including more than one) A and at least one (optionally including more than one) B (and optionally including other elements) in yet another embodiment; and so on.

[0344] It should also be understood that in any method claimed herein that includes more than one step or action, the order of the method steps or actions is not necessarily limited to the order in which the method steps or actions are listed unless explicitly indicated to the contrary.

[0345] In the claims, as well as in the specification above, all transitional phrases such as "comprises," "comprising," "carrying," "having," "containing," "involving," "having," "consisting of," etc. shall be construed as open-ended, i.e., meaning including but not limited to. Only the transitional phrases "consisting of" and "consisting essentially of" shall be closed or semi-closed transitional phrases, respectively, as provided in Section 2111.03 of the U.S. Patent Office Manual of Patent Examining Procedures.

[0346] The present invention can also be implemented through the following embodiments.

[0347] Embodiment 1. An article for inclusion in an electrochemical cell, comprising:

[0348] a layer comprising lithium metal; and

[0349] A passivation layer is arranged on the layer containing lithium metal, wherein the passivation layer contains boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogen.

[0350] Embodiment 2. An article for inclusion in an electrochemical cell, comprising:

[0351] a layer comprising lithium metal; and

[0352] A passivation layer is disposed on the layer containing lithium metal, wherein the passivation layer includes a plurality of columnar structures having an aspect ratio greater than or equal to 0.5 and less than or equal to 5.

[0353] Embodiment 3. An article for inclusion in an electrochemical cell, comprising:

[0354] An electroactive layer comprising lithium metal, wherein:

[0355] The layer is porous, and

[0356] The layer also contains boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogens.

[0357] Embodiment 4. The article for inclusion in an electrochemical cell according to any of the preceding embodiments, further comprising a passivation layer disposed on the electroactive layer.

[0358] Embodiment 5. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the plurality of pillars comprises at least two pillars in topological contact with each other through the passivation layer.

[0359] Embodiment 6. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the plurality of pillars lack pillars in topological contact with each other through the passivation layer.

[0360] Embodiment 7. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the passivation layer is porous.

[0361] Embodiment 8. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the passivation layer has a thickness greater than or equal to 0.01 microns and less than or equal to 5 microns.

[0362] Embodiment 9. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the electroactive layer comprises a plurality of electroactive regions and a plurality of electroactive regions.

[0363] Embodiment 10. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the electroactive region comprises lithium metal.

[0364] Embodiment 11. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the inactive region comprises a ceramic.

[0365] Embodiment 12. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the ceramic comprises boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogen.

[0366] Embodiment 13. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the electroactive region is intermixed with the inactive region.

[0367] Embodiment 14. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the electroactive layer has a thickness greater than or equal to 1 micrometer and less than or equal to 50 micrometers.

[0368] Embodiment 15. The article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the electroactive layer is disposed directly on a current collector.

[0369] Embodiment 16. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises oxygen.

[0370] Embodiment 17. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises oxygen and carbon.

[0371] Embodiment 18. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises oxygen and hydrogen.

[0372] Embodiment 19. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises sulfur and oxygen.

[0373] Embodiment 20. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises sulfur and carbon.

[0374] Embodiment 21. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises sulfur, oxygen and carbon.

[0375] Embodiment 22. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises hydrogen.

[0376] Embodiment 23. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises nitrogen.

[0377] Embodiment 24. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises nitrogen and oxygen.

[0378] Embodiment 25. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises nitrogen and hydrogen.

[0379] Embodiment 26. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises fluorine and sulfur.

[0380] Embodiment 27. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises fluorine, carbon and hydrogen.

[0381] Embodiment 28. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises fluorine and silicon.

[0382] Embodiment 29. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal, the passivation layer and / or the ceramic comprises carbon and hydrogen.

[0383] Embodiment 30. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the ratio of carbon to oxygen in the layer containing lithium metal is greater than or equal to 0 and less than or equal to 0.1.

[0384] Embodiment 31. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the ratio of carbon to oxygen in the layer containing lithium metal, the passivation layer and / or the ceramic is greater than or equal to 0.01 and less than or equal to 0.5.

[0385] Embodiment 32. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the ratio of carbon to sulfur in the layer containing lithium metal is greater than or equal to 0 and less than or equal to 0.1.

[0386] Embodiment 33. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the ratio of carbon to sulfur in the layer containing lithium metal, the passivation layer and / or the ceramic is greater than or equal to 0.01 and less than or equal to 0.45.

[0387] Embodiment 34. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the ratio of carbon to fluorine in the layer containing lithium metal is greater than or equal to 0 and less than or equal to 0.1.

[0388] Embodiment 35. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the ratio of carbon to fluorine in the layer containing lithium metal, the passivation layer and / or the ceramic is greater than or equal to 0.01 and less than or equal to 40.

[0389] Embodiment 36. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the elastic modulus of the layer comprising lithium metal is less than 4.9 GPa.

[0390] Embodiment 37. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the elastic modulus of the layer comprising lithium metal is less than or equal to 4 GPa.

[0391] Embodiment 38. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium metal does not crack, peel and / or delaminate from the substrate during the tape test described in ASTM 3359.

[0392] Embodiment 39. An article for inclusion in an electrochemical cell according to any of the preceding embodiments, wherein the layer comprising lithium has a thickness greater than or equal to 1 micron and less than or equal to 50 microns.

[0393] Embodiment 40. A method for passivating a layer comprising lithium metal, comprising:

[0394] The layer comprising lithium metal is exposed to a gas to form a passivation layer disposed on the layer comprising lithium metal, wherein the gas comprises a substance containing boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogen.

[0395] Embodiment 41. A method for passivating a layer comprising lithium metal, comprising:

[0396] The layer containing lithium metal is exposed to a gas to form a passivation layer disposed on the layer containing lithium metal, wherein the passivation layer includes a plurality of pillars having an aspect ratio greater than or equal to 0.5 and less than or equal to 1.

[0397] Embodiment 42. A method for depositing an electroactive layer, comprising:

[0398] The electroactive layers are deposited from a variety of gases, among which:

[0399] The electroactive layer is porous;

[0400] The plurality of gases comprises lithium; and

[0401] The plurality of gases includes substances containing boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogens.

[0402] Embodiment 43. The method of any one of Embodiments 40 to 42, further comprising depositing a passivation layer on the electroactive layer.

[0403] Embodiment 44. A method according to any one of Embodiments 40 to 43, wherein the plurality of pillars includes at least two pillars in topological contact with each other through the passivation layer.

[0404] Embodiment 45. A method according to any one of Embodiments 40 to 44, wherein the plurality of pillars lack pillars that are topologically contacted with each other through the passivation layer.

[0405] Embodiment 46. The method of any one of Embodiments 40 to 45, wherein the passivation layer is porous.

[0406] Embodiment 47. A method according to any one of Embodiments 40 to 46, wherein the passivation layer has a thickness greater than or equal to 0.01 microns and less than or equal to 5 microns.

[0407] Embodiment 48. A method according to any one of Embodiments 40 to 47, wherein the electroactive layer comprises a plurality of electroactive regions and a plurality of electroactive regions.

[0408] Embodiment 49. The method of any one of Embodiments 40 to 48, wherein the electroactive region comprises lithium metal.

[0409] Embodiment 50. A method according to any one of Embodiments 40 to 49, wherein the non-electroactive area comprises ceramic.

[0410] Embodiment 51. A method according to any one of Embodiments 40 to 50, wherein the ceramic contains boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogens.

[0411] Embodiment 52. A method according to any one of Embodiments 40 to 51, wherein the electrically active region is mixed with the electrically inactive region.

[0412] Embodiment 53. A method according to any one of Embodiments 40 to 52, wherein the electroactive layer has a thickness greater than or equal to 1 micron and less than or equal to 50 microns.

[0413] Embodiment 54. The method of any one of Embodiments 40 to 53, wherein the electroactive layer is disposed directly on a current collector.

[0414] Embodiment 55. A method according to any one of Embodiments 40 to 54, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains oxygen.

[0415] Embodiment 56. A method according to any one of Embodiments 40 to 55, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains oxygen and carbon.

[0416] Embodiment 57. A method according to any one of Embodiments 40 to 56, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains oxygen and hydrogen.

[0417] Embodiment 58. A method according to any one of Embodiments 40 to 57, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains sulfur and oxygen.

[0418] Embodiment 59. A method according to any one of Embodiments 40 to 58, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains sulfur and carbon.

[0419] Embodiment 60. A method according to any one of Embodiments 40 to 59, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains sulfur, oxygen and carbon.

[0420] Embodiment 61. A method according to any one of Embodiments 40 to 60, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains hydrogen.

[0421] Embodiment 62. A method according to any one of Embodiments 40 to 61, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains nitrogen.

[0422] Embodiment 63. A method according to any one of Embodiments 40 to 62, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains nitrogen and oxygen.

[0423] Embodiment 64. A method according to any one of Embodiments 40 to 63, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contain nitrogen and hydrogen.

[0424] Embodiment 65. A method according to any one of Embodiments 40 to 64, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains fluorine and sulfur.

[0425] Embodiment 66. A method according to any one of Embodiments 40 to 65, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains fluorine, carbon and hydrogen.

[0426] Embodiment 67. A method according to any one of Embodiments 40 to 66, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains fluorine and silicon.

[0427] Embodiment 68. A method according to any one of Embodiments 40 to 67, wherein the layer containing lithium metal, the passivation layer and / or the ceramic contains carbon and hydrogen.

[0428] Embodiment 69. A method according to any one of Embodiments 40 to 68, wherein the ratio of carbon to oxygen in the layer containing lithium metal is greater than or equal to 0 and less than or equal to 0.1.

[0429] Embodiment 70. A method according to any one of Embodiments 40 to 69, wherein the ratio of carbon to oxygen in the layer containing lithium metal, the passivation layer and / or the ceramic is greater than or equal to 0.01 and less than or equal to 0.5.

[0430] Embodiment 71. A method according to any one of Embodiments 40 to 70, wherein the ratio of carbon to sulfur in the layer containing lithium metal is greater than or equal to 0 and less than or equal to 0.1.

[0431] Embodiment 72. A method according to any one of Embodiments 40 to 71, wherein the ratio of carbon to sulfur in the layer containing lithium metal, the passivation layer and / or the ceramic is greater than or equal to 0.01 and less than or equal to 0.45.

[0432] Embodiment 73. A method according to any one of Embodiments 40 to 72, wherein the ratio of carbon to fluorine in the layer containing lithium metal is greater than or equal to 0 and less than or equal to 0.1.

[0433] Embodiment 74. A method according to any one of Embodiments 40 to 73, wherein the ratio of carbon to fluorine in the layer containing lithium metal, the passivation layer and / or the ceramic is greater than or equal to 0.01 and less than or equal to 40.

[0434] Embodiment 75. A method according to any one of Embodiments 40 to 74, wherein the elastic modulus of the layer containing lithium metal is less than 4.9 GPa.

[0435] Embodiment 76. A method according to any one of Embodiments 40 to 75, wherein the elastic modulus of the layer containing lithium metal is less than or equal to 4 GPa.

[0436] Embodiment 77. A method according to any one of Embodiments 40 to 76, wherein the layer comprising lithium metal does not crack, peel and / or delaminate from the substrate during the tape test described in ASTM 3359.

[0437] Embodiment 78. A method according to any one of Embodiments 40 to 77, wherein the plurality of gases further includes an inert gas.

[0438] Embodiment 79. A method according to any one of Embodiments 40 to 78, wherein the plurality of gases further includes helium and / or argon.

[0439] Embodiment 80. A method according to any one of Embodiments 40 to 79, wherein the plurality of gases includes CO2.

[0440] Embodiment 81. A method according to any one of Embodiments 40 to 80, wherein the plurality of gases includes O2.

[0441] Embodiment 82. A method according to any one of Embodiments 40 to 81, wherein the plurality of gases includes H2O.

[0442] Embodiment 83. The method of any one of Embodiments 40 to 82, wherein the plurality of gases comprises COS.

[0443] Embodiment 84. A method according to any one of Embodiments 40 to 83, wherein the plurality of gases includes SO2.

[0444] Embodiment 85. A method according to any one of Embodiments 40 to 84, wherein the plurality of gases includes CS2.

[0445] Embodiment 86. A method according to any one of Embodiments 40 to 85, wherein the plurality of gases includes H2.

[0446] Embodiment 87. A method according to any one of Embodiments 40 to 86, wherein the plurality of gases includes N2.

[0447] Embodiment 88. A method according to any one of Embodiments 40 to 87, wherein the plurality of gases includes N2O.

[0448] Embodiment 89. A method according to any one of Embodiments 40 to 88, wherein the plurality of gases includes NH3.

[0449] Embodiment 90. The method of any one of Embodiments 40 to 89, wherein the plurality of gases comprises SF6.

[0450] Embodiment 91. A method according to any one of Embodiments 40 to 90, wherein the plurality of gases includes Freon.

[0451] Embodiment 92. The method of any one of Embodiments 40 to 91, wherein the plurality of gases comprises fluorobenzene.

[0452] Embodiment 93. A method according to any one of Embodiments 40 to 92, wherein the plurality of gases includes SiF4.

[0453] Embodiment 94. A method according to any one of Embodiments 40 to 93, wherein the plurality of gases includes C2H2.

[0454] Embodiment 95. A method according to any one of Embodiments 40 to 94, wherein the plurality of gases includes gases activated by plasma.

[0455] Embodiment 96. A method according to any one of Embodiments 40 to 95, wherein the layer comprising lithium has a thickness greater than or equal to 1 micron and less than or equal to 50 microns.

[0456] Embodiment 97. A modular lithium deposition system comprising:

[0457] Module 1;

[0458] Module 2;

[0459] A source of lithium; and

[0460] a roll-to-roll processing system passing through said first module and said second module,

[0461] Wherein, the first module and the second module are configured to be reversibly placed in fluid communication with each other.

[0462] Embodiment 98. A method comprising:

[0463] depositing a layer comprising lithium and / or a reaction product of lithium onto a first portion of a substrate in a first module in a modular lithium deposition system, wherein:

[0464] The layer comprising lithium metal and / or reaction products of lithium metal is deposited from a gas,

[0465] A second portion of the substrate in the second module is not exposed to the gas, and the modular lithium deposition system further includes a lithium metal source and a roll-to-roll processing system passing through the first module and the second module.

[0466] Embodiment 99. A modular lithium deposition system comprising:

[0467] Multiple modules;

[0468] A source of lithium; and

[0469] A roll-to-roll processing system through the plurality of modules, wherein:

[0470] The roll-to-roll processing system includes a plurality of rollers configured to translate the substrate through the plurality of modules,

[0471] Each of the plurality of drums is in thermal communication with a cooling system, and

[0472] The cooling system is configured to maintain each of the plurality of drums at a temperature greater than or equal to -35°C and less than or equal to 60°C.

[0473] Embodiment 100. A modular lithium deposition system comprising:

[0474] Vacuum chamber;

[0475] a source of lithium metal; and

[0476] A roll-to-roll processing system passing through said vacuum chamber, wherein:

[0477] The lithium metal source is contained in a container,

[0478] The container comprises a cooling system comprising a plurality of cooling channels arranged in one or more walls of the container, and

[0479] The cooling channel is configured to cool the outer surface of the container to a temperature less than or equal to 50°C and greater than or equal to 15°C.

[0480] Embodiment 101. A modular lithium deposition system comprising:

[0481] Vacuum chamber;

[0482] a source of lithium metal; and

[0483] A roll-to-roll processing system passing through said vacuum chamber, wherein:

[0484] The lithium metal source is contained in a container including a shutter, and

[0485] The shutter is configured to reversibly place the vacuum chamber and the interior of the container containing lithium in fluid communication with each other.

[0486] Embodiment 102. A modular lithium deposition system comprising:

[0487] Multiple modules;

[0488] a plurality of lithium metal sources, wherein the plurality of lithium metal sources are arranged in a plurality of crucibles in thermal communication with a heating system;

[0489] a plurality of wire feeding systems, wherein each wire feeding system is configured to feed a wire comprising lithium into one of the plurality of crucibles; and

[0490] A roll-to-roll processing system passes through the plurality of modules.

[0491] Embodiment 103. A method comprising:

[0492] depositing a layer comprising lithium onto a substrate from a first lithium metal source, wherein the first lithium metal source is contained in a first container; and

[0493] depositing lithium metal from a second lithium metal source onto the first layer comprising lithium metal to form a final layer comprising lithium metal, wherein:

[0494] The final layer comprising lithium metal has a smaller thickness variation in the cross-web direction than the first layer comprising lithium metal,

[0495] The second lithium metal source is contained in a second container, and

[0496] The method is performed in a vacuum chamber located in a modular lithium deposition system, which also includes a roll-to-roll processing system passing through the vacuum chamber.

[0497] Embodiment 104. A modular lithium deposition system or method according to any one of Embodiments 95 to 103, wherein the plurality of modules comprises a vacuum chamber.

[0498] Embodiment 105. A modular lithium deposition system or method according to any one of Embodiments 95 to 104, wherein the first module comprises a vacuum chamber.

[0499] Embodiment 106. A modular lithium deposition system or method according to any one of Embodiments 95 to 105, wherein the second module comprises a vacuum chamber.

[0500] Embodiment 107. A modular lithium deposition system or method according to any one of Embodiments 95 to 106, wherein the plurality of rollers are configured to translate the substrate through a plurality of vacuum chambers located in the plurality of modules.

[0501] Embodiment 108. A modular lithium deposition system or method according to any one of Embodiments 95 to 107, wherein the substrate comprises a polymer.

[0502] Embodiment 109. A modular lithium deposition system or method according to any one of Embodiments 95 to 108, wherein the polymer is a poly(ester).

[0503] Embodiment 110. A modular lithium deposition system or method according to any one of Embodiments 95 to 109, wherein the poly(ester) is poly(ethylene terephthalate).

[0504] Embodiment 111. A modular lithium deposition system or method according to any one of Embodiments 95 to 110, wherein a release layer is disposed on the substrate.

[0505] Embodiment 112. A modular lithium deposition system or method according to any one of Embodiments 95 to 111, wherein the release layer comprises a polymer containing alcohol functional groups.

[0506] Embodiment 113. A modular lithium deposition system or method according to any one of Embodiments 95 to 112, wherein the release layer comprises poly(vinyl alcohol).

[0507] Embodiment 114. A modular lithium deposition system or method according to any one of Embodiments 95 to 113, wherein the exfoliation layer has a thickness greater than or equal to 2 microns and less than or equal to 4 microns.

[0508] Embodiment 115. A modular lithium deposition system or method according to any one of Embodiments 95 to 114, wherein the metal layer is disposed on the release layer.

[0509] Embodiment 116. A modular lithium deposition system or method according to any one of Embodiments 95 to 115, wherein the metal layer includes a current collector.

[0510] Embodiment 117. A modular lithium deposition system or method according to any one of Embodiments 95 to 116, wherein the metal layer comprises copper.

[0511] Embodiment 118. A modular lithium deposition system or method according to any one of Embodiments 95 to 117, wherein the metal layer has a thickness greater than or equal to 0.1 microns and less than or equal to 0.5 microns.

[0512] Embodiment 119. A modular lithium deposition system or method according to any one of Embodiments 95 to 118, wherein the vacuum chamber is configured to maintain a pressure greater than or equal to 10 -6 Support and less than or equal to 10 -7 The pressure point of the support.

[0513] Embodiment 120. A modular lithium deposition system or method according to any one of Embodiments 95 to 119, wherein the vacuum chamber is configured to maintain a pressure greater than or equal to 10 -4 Support and less than or equal to 10 -5 The pressure point of the support.

[0514] Embodiment 121. A modular lithium deposition system or method according to any one of Embodiments 95 to 120, wherein the modular lithium deposition system further includes a vacuum chamber configured to generate oxygen plasma.

[0515] Embodiment 122. A modular lithium deposition system or method according to any one of Embodiments 95 to 121, further comprising cleaning the substrate by oxygen plasma treatment before depositing lithium on the substrate.

[0516] Embodiment 123. A modular lithium deposition system or method according to any one of Embodiments 95 to 122, wherein the vacuum chamber further comprises one or more gas sources.

[0517] Embodiment 124. A modular lithium deposition system or method according to any one of Embodiments 95 to 123, wherein the one or more gas sources include a source of an inert gas.

[0518] Embodiment 125. A modular lithium deposition system or method according to any one of Embodiments 95 to 124, wherein the one or more gas sources include a source of a gas reactive with lithium metal.

[0519] Embodiment 126. A modular lithium deposition system or method according to any one of Embodiments 95 to 125, wherein the source of the gas reactive with lithium metal is positioned to react with lithium metal gas from the container containing lithium to form a passivation layer, wherein the passivation layer comprises lithium and reaction products of lithium metal and the gas reactive with lithium metal.

[0520] Embodiment 127. A modular lithium deposition system or method according to any one of Embodiments 95 to 126, wherein the source of the gas reactive with lithium metal is positioned to react with the lithium metal layer deposited on the substrate to form a passivation layer, and the passivation layer comprises the reaction products of lithium metal and the gas reactive with lithium metal arranged on the lithium metal layer.

[0521] Embodiment 128. A modular lithium deposition system or method according to any one of Embodiments 95 to 127, wherein a shield is positioned proximate to the drum.

[0522] Embodiment 129. A modular lithium deposition system or method according to any one of Embodiments 95 to 128, wherein the shield is located between the container containing lithium metal and the drum.

[0523] Embodiment 130. A modular lithium deposition system or method according to any one of Embodiments 95 to 129, wherein the shield is located between the container and the source of gas.

[0524] Embodiment 131. A modular lithium deposition system or method according to any one of Embodiments 95 to 130, wherein the vacuum chamber further comprises one or more sensors.

[0525] Embodiment 132. A modular lithium deposition system or method according to any one of Embodiments 95 to 131, wherein the one or more sensors include a conductivity sensor, an optical sensor, a capacitance sensor, and a thickness sensor.

[0526] Embodiment 133. A modular lithium deposition system or method according to any one of Embodiments 95 to 132, further comprising adjusting the flow rate of the gas based on the characteristics sensed by the one or more sensors.

[0527] Embodiment 134. A modular lithium deposition system or method according to any one of Embodiments 95 to 133, further comprising adjusting the temperature of the container containing the lithium metal based on the characteristics sensed by the one or more sensors.

[0528] Embodiment 135. A modular lithium deposition system or method according to any one of Embodiments 95 to 134, further comprising opening or closing the shutter based on characteristics sensed by the one or more sensors.

[0529] Embodiment 136. A modular lithium deposition system or method according to any one of Embodiments 95 to 135, further comprising adjusting the speed of the substrate based on the characteristics sensed by the one or more sensors.

[0530] Embodiment 137. A modular lithium deposition system or method according to any one of Embodiments 95 to 136, wherein the lithium container is formed of steel.

[0531] Embodiment 138. A modular lithium deposition system or method according to any one of Embodiments 95 to 137, wherein the lithium container is configured to be heated to a temperature greater than or equal to 550°C and less than or equal to 635°C.

[0532] Embodiment 139. A modular lithium deposition system or method according to any one of Embodiments 95 to 138, wherein the lithium metal container is thermally connected to a heating system.

[0533] Embodiment 140. A modular lithium deposition system or method according to any one of Embodiments 95 to 139, wherein the heating system is a resistive heating system.

[0534] Embodiment 141. A modular lithium deposition system or method according to any one of Embodiments 95 to 140, wherein the shutter is thermally connected to a heating system.

[0535] Embodiment 142. A modular lithium deposition system or method according to an...

Claims

1. An article for inclusion in an electrochemical cell, comprising: a layer comprising lithium metal; as well as A passivation layer is disposed on the layer containing lithium metal, wherein the passivation layer includes a plurality of columnar structures having an aspect ratio greater than or equal to 0.5 and less than or equal to 5.

2. An article for inclusion in an electrochemical cell, comprising: An electroactive layer comprising lithium metal, wherein: The layer is porous, and The layer also contains boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogens.

3. A method for depositing an electroactive layer, comprising: The electroactive layers are deposited from a variety of gases, among which: The electroactive layer is porous; The plurality of gases comprises lithium; and The plurality of gases includes substances containing boron, phosphorus, antimony, selenium, tellurium, hydrogen and / or halogens.

4. A modular lithium deposition system comprising: Module 1; Module 2; Lithium source; as well as a roll-to-roll processing system passing through said first module and said second module, Wherein, the first module and the second module are configured to be reversibly placed in fluid communication with each other.

5. A method comprising: depositing a layer comprising lithium and / or a reaction product of lithium onto a first portion of a substrate in a first module in a modular lithium deposition system, wherein: The layer comprising lithium metal and / or reaction products of lithium metal is deposited from a gas, A second portion of the substrate in the second module is not exposed to the gas, and The modular lithium deposition system also includes a lithium metal source and a roll-to-roll processing system that passes through the first module and the second module.

6. A modular lithium deposition system comprising: Multiple modules; Lithium source; as well as A roll-to-roll processing system through the plurality of modules, wherein: The roll-to-roll processing system includes a plurality of rollers configured to translate the substrate through the plurality of modules, Each of the plurality of drums is in thermal communication with a cooling system, and The cooling system is configured to maintain each of the plurality of drums at a temperature greater than or equal to -35°C and less than or equal to 60°C.

7. A modular lithium deposition system comprising: Vacuum chamber; Lithium metal source; as well as A roll-to-roll processing system passing through said vacuum chamber, wherein: The lithium metal source is contained in a container, The container comprises a cooling system comprising a plurality of cooling channels arranged in one or more walls of the container, and The cooling channel is configured to cool the outer surface of the container to a temperature less than or equal to 50°C and greater than or equal to 15°C.

8. A modular lithium deposition system comprising: Vacuum chamber; Lithium metal source; as well as A roll-to-roll processing system passing through said vacuum chamber, wherein: The lithium metal source is contained in a container including a shutter, and The shutter is configured to reversibly place the vacuum chamber and the interior of the container containing lithium in fluid communication with each other.

9. A modular lithium deposition system comprising: Multiple modules; a plurality of lithium metal sources, wherein the plurality of lithium metal sources are arranged in a plurality of crucibles in thermal communication with a heating system; a plurality of wire feeding systems, wherein each wire feeding system is configured to feed a wire comprising lithium into one of the plurality of crucibles; and A roll-to-roll processing system passes through the plurality of modules.

10. A method comprising: depositing a layer comprising lithium onto a substrate from a first lithium metal source, wherein the first lithium metal source is contained in a first container; and depositing lithium metal from a second lithium metal source onto the first layer comprising lithium metal to form a final layer comprising lithium metal, wherein: The final layer comprising lithium metal has a smaller thickness variation in the cross-web direction than the first layer comprising lithium metal, The second lithium metal source is contained in a second container, and The method is performed in a vacuum chamber located in a modular lithium deposition system, which also includes a roll-to-roll processing system passing through the vacuum chamber.

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