Apparatus and process for forming semi-solid electrode having high active solids loading and electrochemical cell including the same

Abstract

To provide a method of forming higher-density semi-solid electrodes.SOLUTION: A method includes: mixing an active material and a conductive material in a liquid electrolyte to form a semi-solid electrode material; disposing the semi-solid electrode material onto a current collector; extracting part of the liquid electrolyte; and compressing the semi-solid electrode material to form a higher-density semi-solid electrode, wherein the higher-density semi-solid electrode includes about 60 to about 85 vol.% of the active material.SELECTED DRAWING: Figure 2A-2E

Description

[Technical Field]

[0001] CROSS-REFERENCE TO RELATED APPLICATIONS

[0001] This application claims priority to and benefit of U.S. Provisional Patent Application No. 62 / 963,908, filed January 21, 2020, entitled "APPARATUSES AND PROCESSES FOR FORMING A SEMI-SOLID ELECTRODE HAVING HIGH ACTIVE SOLIDS LOADING AND ELECTROCHEMICAL CELLS INCLUDING THE SAME," the disclosure of which is hereby incorporated by reference in its entirety. [Background technology]

[0002]

[0002] Semi-solid electrodes can sometimes have lower energy densities than conventional electrodes, where the electrode material is often calendared after being applied to a current collector. As a result, semi-solid electrodes, which can have improved conductivity and reduced risk of ion entrapment within the electrode material compared to conventional electrodes, are often made thicker to achieve the same capacity. Summary of the Invention

[0003]

[0003] Embodiments described herein generally relate to apparatus and processes for forming semi-solid electrodes with increased active solids loading by removing excess electrolyte. In some embodiments, a method for converting a semi-solid electrode material from a first composition to a second composition includes removing a portion of the electrolyte from the semi-solid electrode material. In some embodiments, the semi-solid electrode material can be disposed on a current collector, thereby forming an intermediate electrode. In some embodiments, the method further includes removing a portion of the electrolyte from the semi-solid electrode material by mechanically compressing the intermediate electrode. In some embodiments, the method can include disposing the intermediate electrode between a die and a base of a mechanical press and moving the die toward the base until a compressive force is applied to the intermediate electrode. In some embodiments, an absorbent material can be disposed within the mechanical press, for example, between at least one of the die and the base, to absorb the portion of the electrolyte removed from the intermediate electrode. In some embodiments, removing a portion of the electrolyte from the intermediate electrode forms a finished electrode having a higher active solids loading than the aforementioned semi-solid electrode material and electrodes constructed therefrom.

[0004] In some embodiments, a semi-solid electrode material can be formed by mixing an active material and optionally a conductive material in a liquid electrolyte to form an electrode material comprising a mixture of solid and liquid phases. In some embodiments, the semi-solid electrode material can be disposed on a current collector to form an intermediate electrode. In some embodiments, the intermediate electrode can include a semi-solid electrode material having a first composition in which the ratio of active material to electrolyte is about 10:1 to about 1:1. In some embodiments, the intermediate electrode can be mechanically compressed to form a finished electrode comprising a semi-solid electrode material having a second composition in which the ratio of active material to electrolyte is about 5:1 to about 1:3. [Brief explanation of the drawings]

[0005] [Figure 1]

[0005] According to one embodiment, a method for fabricating a semi-solid electrode is presented. [Figures 2A-2E]

[0006] 1 illustrates a method for fabricating a semi-solid electrode, according to an embodiment. [Figures 3A-3E]

[0007] 1 illustrates a method for fabricating a semi-solid electrode, according to an embodiment. [Figures 4A-4E]

[0008] 1 illustrates a method for fabricating a semi-solid electrode, according to an embodiment. [Figure 4F]

[0008] According to one embodiment, a method for fabricating a semi-solid electrode is presented. [Figure 5A-5B]

[0009] 10 illustrates a method of further use of a semi-solid electrode, according to an embodiment. DETAILED DESCRIPTION OF THE INVENTION

[0006]

[0010] Embodiments described herein generally relate to methods for forming semi-solid electrode materials with high active solids loadings and methods for forming electrochemical cells including the same. In some embodiments, the semi-solid electrode can be formed by mechanically compressing a semi-solid electrode material of an active material and a conductive material in a liquid electrolyte. In some embodiments, the active material can include particles of the active material. In some embodiments, the active particles can be substantially free of a coating layer. In some embodiments, the conductive material can include particles of a conductive material. In some embodiments, the conductive material can be free or substantially free of conductive fibers. In some embodiments, the semi-solid electrode material can include a first volume of liquid electrolyte such that the semi-solid electrode material is flowable during fabrication of the semi-solid electrode. In some embodiments, the semi-solid electrode material can be mechanically compressed to extract a portion of the liquid electrolyte and form a semi-solid electrode material having a second volume of liquid electrolyte that is less than the first volume of liquid electrolyte. In some embodiments, the mechanical compression includes compressing the semi-solid electrode material between a die and a base. In some embodiments, a semi-permeable membrane may be disposed between the semi-solid electrode material and at least one of the base and the die so that a portion of the liquid electrolyte may be extracted without removing any of the active material or conductive material. In some embodiments, removing a portion of the liquid electrolyte from the semi-solid electrode material may form a semi-solid electrode material having a higher active solids content (e.g., greater than about 70 wt% active material).

[0007]

[0011] Conventional electrode materials are generally manufactured by coating a metal substrate (e.g., a current collector) with an electrode slurry composed of an active material, a conductive additive, and a binder dissolved or dispersed in a solvent or water, evaporating the solvent or water, and calendaring the dry solid matrix to a specified thickness. The electrode is then cut and packaged with other components, impregnated with an electrolyte, and the entire package is sealed. Such methods generally involve complex and expensive manufacturing steps, such as casting the electrode. These methods for manufacturing electrodes result in batteries with low capacity, low energy density, and a high ratio of inactive components to active material. Furthermore, binders used in known electrode manufacturing methods can increase tortuosity and reduce the ionic conductivity of the electrode. In some embodiments, the electrodes described herein may be binder-free or substantially binder-free.

[0008]

[0012] Because the electrolyte is injected into conventional electrode materials after calendering, it typically requires significant effort to inject the electrolyte after the formation of an electrochemical cell. Conventional methods for infusing a liquid electrolyte into a calendered electrode material involve the use of high pressure or long infusion times to fully infiltrate the liquid electrolyte into the electrode material. As a result, conventional electrodes are typically calendered to a porosity of only about 20% to facilitate the infusion of the electrolyte into the calendered electrode material. Therefore, there is a trade-off between the energy density of the finished electrode and the degree of densification of the electrode material. That is, conventional electrode materials after calendering are generally denser, and therefore may be more difficult to infiltrate with a liquid electrolyte. Therefore, conventional electrode materials are often not completely wetted with the electrolyte after infusion, which means that the realized energy density may be substantially lower than the theoretical energy density.

[0009]

[0013] Semi-solid electrodes and batteries formed therefrom can often be made thicker (with higher capacity) without experiencing the conductivity problems of thicker conventional electrodes. However, the energy density of semi-solid electrodes can be lower than conventional electrodes, in part because conventional electrodes are typically calendered, and the slurry solvent is removed during a drying step. Semi-solid electrodes are generally not dried or calendered because these electrodes are formed from slurries of active material and optionally conductive material in a liquid electrolyte, in which case the drying or calendering step would remove all, or substantially all, of the electrolyte from the electrode. Thus, there is a continuing need for semi-solid electrodes and electrochemical cells formed therefrom with higher active solids loadings.

[0010]

[0014] As described herein, in some embodiments, a semi-solid electrode is prepared by first slurrying an active material, an optional conductive material, and a liquid electrolyte into a semi-solid electrode material. Because the semi-solid electrode material already contains the liquid electrolyte in contact with the active material, the realized energy density of the finished electrode can be substantially similar to the theoretical energy density.

[0011]

[0015] As used herein, the singular forms "a," "an," and "the" include plural referents unless the context clearly dictates otherwise. Thus, for example, the term "a member" is intended to mean a single member or a combination of members, and "a material" is intended to mean one or more materials, or a combination thereof.

[0012]

[0016] The term "substantially" when used in connection with "cylindrical," "linear," and / or other geometric relationships is intended to mean that the structure so defined is nominally cylindrical, linear, or the like. As an example, a portion of a support member described as "substantially linear" is intended to mean that while linearity of the portion is desired, some nonlinearity may occur in the "substantially linear" portion. Such nonlinearity may result from manufacturing tolerances or other practical considerations (e.g., pressure or force applied to the support member). Thus, a geometric structure modified by the term "substantially" includes such geometric characteristics within a plus or minus 5% tolerance of the described geometric structure. For example, a "substantially linear" portion is one that defines an axis or centerline that is within plus or minus 5% of being linear.

[0013]

[0017] As used herein, the terms "set" and "plurality" can refer to multiple features or a single feature having multiple parts. For example, when referring to a set of electrodes, the set of electrodes can be considered as one electrode having multiple portions, or the set of electrodes can be considered as multiple separate electrodes. Additionally, for example, when referring to multiple electrochemical cells, the multiple electrochemical cells can be considered as multiple separate electrochemical cells or one electrochemical cell having multiple portions. Thus, a set of portions or multiple portions can include multiple portions that are contiguous or discontinuous with one another. Multiple particles or multiple materials can also be made from multiple items that are manufactured separately and later brought together (e.g., by mixing, adhesive, or any suitable method).

[0014]

[0018] As used herein, the terms "about" and "approximately" generally mean plus or minus 10% of the stated value; for example, about 250 μm includes 225 μm to 275 μm, and about 1,000 μm includes 900 μm to 1,100 μm.

[0015]

[0019] As used herein, the term "semi-solid" refers to a material that is a mixture of liquid and solid phases, such as, for example, a particle suspension, a slurry, a colloidal suspension, an emulsion, a gel, or a micelle. As used herein, the term "semi-solid electrode material" refers to a mixture of at least a solid active material and a liquid electrolyte.

[0016]

[0020] As used herein, the terms "activated carbon network" and "networked carbon" refer to the general qualitative state of an electrode. For example, an electrode having an activated carbon network (or networked carbon) is one in which the carbon particles within the electrode assume an individual particle morphology and arrangement relative to one another that promotes electrical contact and electrical conductivity between the particles. Conversely, the terms "unactivated carbon network" and "unnetworked carbon" refer to an electrode in which the carbon particles exist as individual particle islands or multi-particle agglomerate islands that may not be sufficiently connected to provide adequate electrical conduction through the electrode.

[0017]

[0021] In some embodiments, a method for manufacturing a semi-solid electrode with a high active solids loading includes forming a semi-solid electrode material by mixing an active material and a conductive material with a liquid electrolyte and disposing the semi-solid electrode material on a current collector. The method may further include disposing a semi-permeable membrane on an exposed surface of the semi-solid electrode material and compressing the semi-solid electrode material to extract a portion of the liquid electrolyte. In some embodiments, the semi-solid electrode can be compressed using a mechanical press. In some embodiments, the semi-permeable membrane can be configured to absorb a portion of the liquid electrolyte extracted during compression. In some embodiments, an absorbent material may be used to absorb at least a portion of the liquid electrolyte extracted during mechanical pressing of the semi-solid electrode. In some embodiments, mechanically compressing the semi-solid electrode material includes compressing the semi-solid material between a die and a base. In some embodiments, the absorbent material may be disposed on the exposed surface of the semi-permeable membrane, on a contact surface of the die, on a contact surface of the base, or any combination thereof. In some embodiments, the compressed semi-solid electrode material comprises greater than about 70 wt% active material. In some embodiments, the semi-solid electrode material after mixing has a first composition in which the liquid electrolyte is about 50 wt% to about 80 wt% of the semi-solid electrode material, and the compressed semi-solid electrode material has a second composition in which the liquid electrolyte is about 10 wt% to about 45 wt% of the semi-solid electrode material. In some embodiments, the semi-solid electrode material after mixing has a first ratio of liquid electrolyte to active material of about 10:1 to about 1:1, and the compressed semi-solid electrode material has a second ratio of liquid electrolyte to active material of about 5:1 to about 1:3. In some embodiments, the semi-solid electrode material after mixing has a first active material molarity of about 5 M to about 15 M, and the compressed semi-solid electrode material has a second active material molarity of about 16 M to about 24 M. In some embodiments, the semi-solid electrode material after mixing has a first energy density of about 3 mAh / g to about 5 mAh / g, and the semi-solid electrode material after compaction has a second energy density of about 6 mAh / g to about 14 mAh / g.

[0018]

[0022] In some embodiments, a method for fabricating a semi-solid electrode with a high active solids loading includes forming a semi-solid electrode material having a first thickness by mixing an active material and a conductive material with a liquid electrolyte; inserting a semi-solid electrode material between a current collector and a semi-permeable membrane; and mechanically compressing the semi-solid electrode material such that the semi-solid electrode material has a second thickness that is less than the first thickness; In some embodiments, the first thickness is from about 100 μm to about 2,000 μm. In some embodiments, the second thickness is from about 5 μm to about 50 μm. In some embodiments, the mechanical compression is achieved by mechanically compressing the semi-solid electrode material between a base and a die of a mechanical press.

[0019]

[0023] In some embodiments, a method of fabricating a semi-solid electrode with a high active solids loading may include forming a semi-solid electrode material having a first volume by mixing an active substance and a conductive material with a liquid electrolyte, inserting the semi-solid electrode material between a current collector and a semi-permeable membrane, and mechanically compressing the semi-solid electrode material such that the semi-solid electrode material has a second volume that is smaller than the first volume.

[0020]

[0024] In some embodiments, a method of fabricating a semi-solid electrode with a high active solids loading can include mixing an active substance and a conductive material with a liquid electrolyte to form a semi-solid electrode material having a first composition comprising about 50 wt % to about 80 wt % liquid electrolyte; interposing the semi-solid electrode material between a current collector and a semi-permeable membrane; and mechanically compressing the semi-solid electrode material until the semi-solid electrode material has a second composition comprising about 10 wt % to about 45 wt % liquid electrolyte.

[0021]

[0025] In some embodiments, a method for fabricating a semi-solid electrode with a high active solids loading can include forming a first semi-solid electrode material having a first density by mixing an active substance and a conductive material with a liquid electrolyte, interposing the first semi-solid electrode material between a current collector and a semi-permeable membrane, and mechanically compressing the first semi-solid electrode material to form a second semi-solid electrode material having a second density greater than the first density. In some embodiments, the first density is about 2 g / cm. 3 Less than 1.9g / cm 3 Less than 1.8g / cm 3 Less than 1.7g / cm 3 Less than 1.6g / cm 3 Less than 1.5g / cm 3 Less than 1.4g / cm 3 Less than 1.3g / cm 3 Less than 1.2g / cm 3 Less than 1.1g / cm 3 Less than or about 1 g / cm 3 In some embodiments, the second density may be less than about 2.1 g / cm (including all values ​​and ranges therebetween). 3 ~about 5g / cm 3 , about 2.2g / cm 3 ~Approx. 4.5g / cm 3 , about 2.3g / cm 3 ~ approx. 4g / cm 3 , approximately 2.4 g / cm 3 ~Approx. 3.5g / cm 3 , about 2.5g / cm 3 ~About 3g / cm 3 , about 2.5g / cm 3 ~about 5g / cm 3 , about 3g / cm 3 ~about 5g / cm 3 , about 3.5g / cm 3 ~about 5g / cm 3 , about 4g / cm 3 ~about 5g / cm 3 , about 4.5g / cm 3 ~About 5g / cm 3 , about 2.1g / cm 3 ~Approx. 4.5g / cm 3 , about 2.1g / cm 3~ approx. 4g / cm 3 , about 2.1g / cm 3 ~Approx. 3.5g / cm 3 , about 2.1g / cm 3 ~About 3g / cm 3 , or about 2.1 g / cm 3 ~Approx. 2.5g / cm 3 (including all values ​​and ranges therebetween). In some embodiments, the second density is about 2.1 g / cm 3 Larger, about 2.5g / cm 3 Larger, about 3g / cm 3 Larger, about 3.5g / cm 3 Larger, about 4g / cm 3 Larger, about 4.5g / cm 3 Larger, about 5g / cm 3 Larger, about 5.5g / cm 3 Greater than or about 6 g / cm 3 In some embodiments, the energy density of the second semi-solid electrode material is greater than about 5 mAh / g, greater than about 6 mAh / g, greater than about 7 mAh / g, greater than about 8 mAh / g, greater than about 9 mAh / g, greater than about 10 mAh / g, greater than about 11 mAh / g, greater than about 12 mAh / g, greater than about 13 mAh / g, greater than about 14 mAh / g, or greater than about 15 mAh / g, including all values ​​and ranges therebetween.

[0022]

[0026] In some embodiments, methods for producing semi-solid electrodes with high active solids loading can include the use of recycled electrochemical cell materials. In some embodiments, the recycled electrochemical cell materials can include spent electrochemical cell materials, partially used electrochemical cell materials, conductive electrochemical cell waste, and / or other electrochemical cell materials that can be repurposed. In some embodiments, mechanically compressing the recycled electrochemical cell materials can improve the overall conductivity and / or active material fraction of the recycled electrochemical cell materials. In some embodiments, methods for producing semi-solid electrodes with high active solids loading may include the use of at least about 5 wt%, at least about 10 wt%, at least about 15 wt%, at least about 20 wt%, at least about 25 wt%, at least about 30 wt%, at least about 35 wt%, at least about 40 wt%, at least about 45 wt%, at least about 50 wt%, at least about 55 wt%, at least about 60 wt%, at least about 65 wt%, at least about 70 wt%, at least about 75 wt%, at least about 80 wt%, at least about 85 wt%, at least about 90 wt%, or at least about 95 wt% recycled electrochemical cell material.

[0023]

[0027] FIG. 1 illustrates a method 10 for forming a semi-solid electrode containing a higher active solids loading than conventional electrodes while maintaining flowability during electrode fabrication. The method 10 may include, at 11, forming an intermediate electrode by dispensing a semi-solid electrode material onto a current collector. In some embodiments, dispensing the semi-solid electrode material may include forming or substantially forming the electrode by drop-casting the semi-solid electrode material onto a moving current collector. In some embodiments, dispensing the semi-solid electrode material may include extruding the semi-solid electrode material onto a fixed current collector, such as from a moving extrusion nozzle. In some embodiments, the semi-solid electrode material may be dispensed onto a fixed current collector, e.g., in discrete portions, by a fixed dispensing mechanism, and the discrete portions of the semi-solid electrode material may then be spread across the surface of the current collector by any suitable method to form or substantially form the electrode. In some embodiments, the current collector material may be distributed onto multiple current collectors such that each of the multiple current collectors is separated from the other current collectors. Discrete portions of the semi-solid electrode material may then be disposed on the surface of each of the individualized current collectors to form or substantially form an electrode. In some embodiments, the electrode formed according to step 11 of method 10 includes an intermediate electrode material such that the electrode may be operable in an electrochemical cell but has a lower active solids loading than desired in the finished electrode. The formed electrode may be a positive electrode, an anode, a negative electrode, a cathode, or other electrode or component of an electrochemical cell. As described herein, the electrode may be a semi-solid electrode comprising at least an active material and / or a conductive material in a liquid electrolyte.

[0024]

[0028] In some embodiments, the semi-solid electrode material may comprise any suitable composition of active and / or conductive materials in a liquid electrolyte, such as those compositions described in more detail in U.S. Pat. Nos. 8,993,159, 9,178,200, 9,184,464, 9,203,092, 9,362,583, 9,385,392, 9,401,501, 9,437,864, 9,484,569, 9,812,674, 9,825,280, 9,831,518, and 9,831,522, the disclosures of which are hereby incorporated by reference in their entireties. Examples of methods for manufacturing semi-solid electrodes and electrochemical cells having semi-solid electrodes are described in further detail in U.S. Provisional Patent Application No. 62 / 695,483, entitled "Continuous and Semi-Continuous Methods of Semi-Solid Electrode and Battery Manufacturing," filed July 9, 2018 (hereinafter the "'483 Application"), the entire disclosure of which is hereby incorporated by reference.

[0025]

[0029] In some embodiments, to form a semi-solid electrode material that can be more easily disposed on a current collector, the semi-solid electrode material has an electrolyte to active material ratio of about 10:1 to about 1:1, about 9:1 to about 2:1, about 8:1 to about 3:1, about 7:1 to about 4:1, about 6:1 to about 5:1, about 10:1 to about 2:1, about 10:1 to about 3:1, about 10:1 to about 4:1, about 10:1 to about 5:1, about 10:1 to about 6:1, about 10:1 to about 7:1, about 10:1 to about 8:1, about 10:1 to about 9:1, about 10:1 to about 11:1, about 10:1 to about 12:1, about 10:1 to about 13:1, about 10:1 to about 14 The semi-solid electrode material may have a first composition that is about 5:1, about 10:1 to about 6:1, about 10:1 to about 7:1, about 10:1 to about 8:1, about 10:1 to about 9:1, about 9:1 to about 1:1, about 8:1 to about 1:1, about 7:1 to about 1:1, about 6:1 to about 1:1, about 5:1 to about 1:1, about 4:1 to about 1:1, about 3:1 to about 1:1, or about 2:1 to about 1:1 (including all values ​​and ranges therebetween). In some embodiments, when the semi-solid electrode material has the first composition, the semi-solid electrode material can be more easily handled and dispensed onto a current collector due to its relatively low viscosity compared to the desired viscosity of the semi-solid electrode material in the finished electrode.

[0026]

[0030] In some embodiments, the first composition of the semi-solid electrode material has a saturation rate of about 0.1 mAh / g to about 10 mAh / g, about 0.5 mAh / g to about 9.5 mAh / g, about 1 mAh / g to about 9 mAh / g, about 1.5 mAh / g to about 8.5 mAh / g, about 2 mAh / g to about 8 mAh / g, about 2.5 mAh / g to about 7.5 mAh / g, about 3 mAh / g to about 7.5 mAh / g, or about 4 mAh / g to about 5 mAh / g. mAh / g, approximately 0.1mAh / g to approximately 9.5mAh / g, approximately 0.1mAh / g to approximately 9mAh / g, approximately 0.1mAh / g to approximately 8.5 / mAh / g, approximately 0.1mAh / g to approximately 8mAh / g, approximately 0.1mAh / g to approximately 7.5mAh / g, approximately 0.1mAh / g to approximately 7mAh / g, approximately 0.1mAh / g to approximately 6.5mAh / g, approximately 0.1mAh / g ~ approx. 6mAh / g, approx. 0.5mAh / g ~ approx. 10mAh / g, approx. 1mAh / g ~ approx. 10mAh / g, approx. 1.5mAh / g ~ approx. 10mAh / g, approx. 2mAh / g ~ approx. The energy density may be 0 mAh / g, about 4.5 mAh / g to about 10 mAh / g, about 5 mAh / g to about 10 mAh / g, about 5.5 mAh / g to about 10 mAh / g, about 6 mAh / g to about 10 mAh / g, about 6.5 mAh / g to about 10 mAh / g, or about 7 mAh / g to about 10 mAh / g (including all values ​​and ranges therebetween). In some embodiments, the first composition of the semi-solid electrode material can have an energy density of less than about 10 mAh / g, about 9.5 mAh / g, about 9 mAh / g, about 8.5 mAh / g, about 8 mAh / g, about 7.5 mAh / g, about 7 mAh / g, about 6.5 mAh / g, about 6 mAh / g, about 5.5 mAh / g, about 5 mAh / g, about 4.5 mAh / g, about 4 mAh / g, about 3.5 mAh / g, about 3 mAh / g, about 2.5 mAh / g, about 2 mAh / g, about 1.5 mAh / g, about 1 mAh / g, about 0.5 mAh / g, or about 0.1 mAh / g (including all values ​​and ranges therebetween).

[0027]

[0031] In some embodiments, the semi-solid electrode material disposed on the surface of the current collector may have a thickness, where the thickness is the dimension of the semi-solid electrode material in a direction perpendicular to the surface of the current collector. In some embodiments, the semi-solid electrode material may have a thickness of about 51 μm to about 3,000 μm, about 75 μm to about 2,500 μm, about 100 μm to about 2,000 μm, about 150 μm to about 1,500 μm, about 200 μm to about 1,000 μm, about 250 μm to about 750 μm, about 51 μm to about 2,500 μm, about 51 μm to about 2,000 μm, about 51 μm to about 1,500 μm, about 51 μm to about 1,000 μm, about 100 μm to about 3,000 μm, or about The thickness before mechanical compression may be 200 μm to about 3,000 μm, about 300 μm to about 3,000 μm, about 400 μm to about 3,000 μm, about 500 μm to about 3,000 μm, about 750 μm to about 3,000 μm, about 1,000 μm to about 3,000 μm, about 1,500 μm to about 3,000 μm, about 2,000 μm to about 3,000 μm, or about 2,500 μm to about 3,000 μm (including all values ​​and ranges therebetween). In some embodiments, the semi-solid electrode material may have a thickness before being mechanically compressed that is greater than about 51 μm, about 75 μm, about 100 μm, about 150 μm, about 200 μm, about 250 μm, about 300 μm, about 400 μm, about 500 μm, about 750 μm, about 1,000 μm, about 1,500 μm, about 2,000 μm, about 2,500 μm, or about 3,000 μm (including all values ​​and ranges therebetween).

[0028]

[0032] Method 10 may include, at 12, mechanically compressing the semi-solid electrode material to extract a portion of the liquid electrolyte. In some embodiments, the semi-solid electrode material may have a second composition after extracting a portion of the liquid electrolyte. In some embodiments, mechanical compression of the semi-solid electrode material may result in deformation of at least a portion of the semi-solid electrode material (e.g., a reduction in volume, a reduction in thickness, a reduction in length, a reduction in height, a combination thereof, etc.), and may result in no or substantially no deformation of the current collector. In some embodiments, mechanical compression of the intermediate electrode material may result in removal of a portion of the electrolyte from the semi-solid electrode material.

[0029]

[0033] In some embodiments, mechanical compression may include placing an intermediate electrode between a die and a base of a mechanical press and moving the die toward the base until a compressive force is applied to the intermediate electrode. In some embodiments, the die and base may be configured to be the same or substantially the same shape and size as the intermediate electrode. In some embodiments, the mechanical press may be a stamp press including a motor and a piston configured to apply a motive force to the die, and the die is sized and configured to apply a compressive force to the intermediate electrode held in place by the base. In some embodiments, the intermediate electrode may be positioned within the mechanical press such that an exposed surface or a portion of an exposed surface of the semi-solid electrode material is adjacent to the die, while an exposed surface or a portion of an exposed surface of the current collector is adjacent to the base. In some embodiments, the intermediate electrode may be positioned within the mechanical press such that an exposed surface or a portion of an exposed surface of the current collector is adjacent to the die, while an exposed surface or a portion of an exposed surface of the semi-solid electrode material is adjacent to the base. In some embodiments, the base and / or die may have contact surfaces. In some embodiments, the base and / or die can have an interface region between a contact surface of the base and / or a contact surface of the die and a current collector and / or semi-solid electrode material.

[0030]

[0034] In some embodiments, the contact surface of the die and / or the contact surface of the base may include a cavity such that, during mechanical compression of the intermediate electrode, removed electrolyte, or a portion thereof, may be retained within or transmitted through the cavity. In some embodiments, during mechanical compression of the intermediate electrode, removed electrolyte, or a portion thereof, may exit the semi-solid electrode material and be transmitted through the porous current collector into or through the cavity. In some embodiments, removed electrolyte, or a portion thereof, may exit the semi-solid electrode material and be transmitted out between the base and the die around the end or edge of the current collector. In some embodiments, removed electrolyte, or a portion thereof, may exit the semi-solid electrode material in a direction opposite the current collector and be transmitted into or through the cavity. In some embodiments, removed electrolyte, or a portion thereof, may be transmitted out of the semi-solid electrode material by more than one of the paths described herein. In some embodiments, the cavity may be fluidly coupled to a drain so that removed electrolyte transferred into or through the cavity can be removed from the mechanical press via the drain. In some embodiments, the cavity may be fluidly coupled to a reservoir so that removed electrolyte transferred into or through the cavity can be removed from the mechanical press via the reservoir. In some embodiments, the removed electrolyte held in the reservoir may be reusable and / or recyclable for use in other semi-solid electrodes or elsewhere.

[0031]

[0035] In some embodiments, a semi-permeable membrane can be disposed on or near the semi-solid electrode material such that during mechanical compression of the intermediate electrode, the semi-permeable membrane does not allow transmission of active substances, conductive materials, etc., out of the semi-solid electrode material, but does allow transmission of electrolyte out of the semi-solid electrode material. In some embodiments, the semi-permeable membrane can be a sheet or other planar structure configured to be removed from on or near the semi-solid electrode material before or after removal of the intermediate electrode from the mechanical press and before incorporating the mechanically compressed electrode into an electrochemical cell or the like. In some embodiments, the semi-permeable membrane can be a conventional separator material configured to allow at least some flow of liquid electrolyte therethrough. In some embodiments, the semi-permeable membrane can be any material that is completely or substantially chemically inert with respect to the composition of the semi-solid electrode material and / or current collector, while allowing at least some flow of liquid electrolyte therethrough. In some embodiments, the semi-permeable membrane can absorb at least a portion of the extracted liquid electrolyte such that the liquid electrolyte cannot be reabsorbed into the semi-solid electrode material, is substantially unable to be reabsorbed into the semi-solid electrode material, or may only be only partially reabsorbed into the semi-solid electrode material.

[0032]

[0036] In some embodiments, removing a portion of the electrolyte from the intermediate electrode forms a finished electrode having a higher active solids loading than the aforementioned semi-solid electrode materials and electrodes constructed therefrom. Without wishing to be bound by any particular theory, removing a portion of the electrolyte (e.g., an excess portion of the liquid electrolyte) can reduce the volume of the semi-solid electrode material on the current collector by removing the electrolyte and by compressing and removing voids and porosity without a corresponding reduction in conductivity throughout the semi-solid electrode material. In some embodiments, the reduction in porosity can include a reduction in porosity from approximately about 20% to about 50% to about 5% to about 30%, including all values ​​and ranges therebetween.

[0033]

[0037] In some embodiments, the second composition of the semi-solid electrode material can have a lower ratio of electrolyte to active material than the first composition. In some embodiments, the second composition of the semi-solid electrode material can have a ratio of electrolyte to active material of about 5:1 to about 1:3, about 4:1 to about 1:2, about 3:1 to about 1:1, about 5:1 to about 1:2, about 5:1 to about 1:1, about 5:1 to about 2:1, about 5:1 to about 3:1, about 5:1 to about 4:1, about 4:1 to about 1:3, about 3:1 to about 1:3, about 2:1 to about 1:3, about 1:1 to about 1:3, or about 1:2 to about 1:3 (including all values ​​and ranges therebetween).

[0034]

[0038] In some embodiments, the second composition of the semi-solid electrode material has a capacitance of about 5 mAh / g to about 24 mAh / g, about 6 mAh / g to about 23 mAh / g, about 7 mAh / g to about 22 mAh / g, about 8 mAh / g to about 21 mAh / g, about 9 mAh / g to about 20 mAh / g, about 10 mAh / g to about 19 mAh / g, about 11 mAh / g to about 18 mAh / g, about 12 mAh / g to about 17 mAh / g, about 13 mAh / g to about 16 mAh / g, about 14 mAh / g to about 15 mAh / g, about 5 mAh / g to about 23 mAh / g, or about 16 mAh / g to about 24 mAh / g. h / g, about 5mAh / g to about 22mAh / g, about 5mAh / g to about 21mAh / g, about 5mAh / g to about 20mAh / g, about 5mAh / g to about 19mAh / g, about 5mAh / g to about 18mAh / g, about 5mAh / g to about 17mAh / g, about 5mAh / g to approx. 16mAh / g, approx. 5mAh / g to approx. 15mAh / g, approx. 5mAh / g to approx. 14mAh / g, approx. 5mAh / g to approx. 13mAh / g, approx. 5mAh / g to approx. 12mAh / g, approx. 5mAh / g to approx. 11mAh / g, approx. g ~ about 10mAh / g, about 5mAh / g - about 9mAh / g, about 5mAh / g - about 8mAh / g, about 5mAh / g - about 7mAh / g, about 5mAh / g - about 6mAh / g, about 6mAh / g - about 24mAh / g, about 7mAh / g - about 24mAh / g, about 8mAh / g to about 24mAh / g, about 9mAh / g to about 24mAh / g, about 10mAh / g to about 24mAh / g, about 11mAh / g to about 24mAh / g, about 12mAh / g to about 24mAh / g, about 13mAh / g to about 24mAh / g , about 14 mAh / g to about 24 mAh / g, about 15 mAh / g to about 24 mAh / g, about 16 mAh / g to about 24 mAh / g, about 17 mAh / g to about 24 mAh / g, about 18 mAh / g to about 24 mAh / g, about 19 mAh / g to about 24 mAh / g, about 20 mAh / g to about 24 mAh / g, about 21 mAh / g to about 24 mAh / g, about 22 mAh / g to about 24 mAh / g, or about 23 mAh / g to about 24 mAh / g (including all values ​​and ranges therebetween).In some embodiments, the first composition of the semi-solid electrode material can have an energy density greater than about 5 mAh / g, about 6 mAh / g, about 7 mAh / g, about 8 mAh / g, about 9 mAh / g, about 10 mAh / g, about 11 mAh / g, about 12 mAh / g, about 13 mAh / g, about 14 mAh / g, about 15 mAh / g, about 16 mAh / g, about 17 mAh / g, about 18 mAh / g, about 19 mAh / g, about 20 mAh / g, about 21 mAh / g, about 22 mAh / g, about 23 mAh / g, or about 24 mAh / g (including all values ​​and ranges therebetween).

[0035]

[0039] In some embodiments, the semi-solid electrode material has a diameter of about 1 μm to about 50 μm, about 2 μm to about 49 μm, about 3 μm to about 48 μm, about 4 μm to about 47 μm, about 5 μm to about 46 μm, about 6 μm to about 45 μm, about 7 μm to about 44 μm, about 8 μm to about 43 μm, about 9 μm to about 42 μm, about 10 μm to about 41 μm, about 15 μm to about 40 μm, about 20 μm to about 30 μm, about 2 μm to about 50 μm, about 3 μm to about 50 μm, about 4 μm to about 50 μm, about 5 μm to about 50 μm, about 6 μm to about 50 μm, about 7 μm to about 50 ...50 μm, about 9 μm to about 50 μm, about 10 μm to about 50 μm, about 15 μm to about 40 μm, about 20 μm to about 30 μm, about 2 μm to about 50 μm, about 3 μm to about 50 μm, about 4 μm to about 50 μm, about 5 μm to about The thickness after mechanical compression may be from about 10 μm to about 50 μm, from about 8 μm to about 50 μm, from about 9 μm to about 50 μm, from about 10 μm to about 50 μm, from about 11 μm to about 50 μm, from about 12 μm to about 50 μm, from about 13 μm to about 50 μm, from about 14 μm to about 50 μm, from about 15 μm to about 50 μm, from about 20 μm to about 50 μm, from about 25 μm to about 50 μm, from about 30 μm to about 50 μm, from about 35 μm to about 50 μm, from about 40 μm to about 50 μm, or from about 45 μm to about 50 μm (including all values ​​and ranges therebetween). In some embodiments, the semi-solid electrode material has a thickness of about 50 μm, about 49 μm, about 48 μm, about 47 μm, about 46 μm, about 45 μm, about 44 μm, about 43 μm, about 42 μm, about 41 μm, about 40 μm, about 39 μm, about 38 μm, about 37 μm, about 36 μm, about 35 μm, about 34 μm, about 33 μm, about 32 μm, about 31 μm, about 30 μm, about 29 μm, about 28 μm, about 27 μm, about 26 μm, about 25 μm, It may have a thickness after mechanical compression of less than about 24 μm, about 23 μm, about 22 μm, about 21 μm, about 20 μm, about 19 μm, about 18 μm, about 17 μm, about 16 μm, about 15 μm, about 14 μm, about 13 μm, about 12 μm, about 11 μm, about 10 μm, about 9 μm, about 8 μm, about 7 μm, about 6 μm, about 5 μm, about 4 μm, about 3 μm, about 2 μm, or about 1 μm (including all values ​​and ranges therebetween).

[0036]

[0040] Method 10 may optionally include, at 13, absorbing the extracted portion of the liquid electrolyte using an absorbent material. In some embodiments, the absorbent material may be disposed within the mechanical press, for example, between the intermediate electrode and at least one of the die and base, to absorb at least a portion of the electrolyte removed from the intermediate electrode. In some embodiments, the absorbent material may be an integral component of the mechanical press. In some embodiments, the absorbent material may be bonded to the die of the mechanical press such that the extracted liquid electrolyte is absorbed by the absorbent material when the die compresses the semi-solid electrode material against a current collector positioned on the base. In some embodiments, the absorbent material may be bonded to the base of the mechanical press. In some embodiments, the current collector may be at least partially porous such that liquid electrolyte removed from the semi-solid electrode material during compression of the intermediate electrode can be transferred through the current collector and into the absorbent material. In some embodiments, the absorbent material may be reusable. In some embodiments, a first intermediate electrode can be mechanically compressed, and the removed liquid electrolyte can be absorbed by the absorbent material. After mechanically compressing the intermediate electrode, the completed electrode can be removed from the mechanical press. The mechanical press can then be operated to a closed position such that the die and / or base are moved to remove the extracted liquid electrolyte from the absorbent material by compressing it between the die and base. In some embodiments, after the extracted liquid electrolyte has been removed from the absorbent material, the mechanical press can be returned to an open position and a second intermediate electrode can be placed between the base and die for mechanical compression. In some embodiments, after pressing the intermediate electrode with the mechanical press, the extracted liquid electrolyte can be removed from the absorbent material, and the same intermediate electrode can be pressed a second time until a sufficient amount of liquid electrolyte has been removed to achieve the desired composition for the finished electrode.

[0037]

[0041] In some embodiments, the absorbent material may include any of fibrous materials, cotton, rice hulls, superhydrophobic sawdust, cellulosic materials, superabsorbent polymers, zeolite materials, aerogels, nanocellulose aerogels, hydrogels, polyurethanes, polypropylene, polyethylene, and cross-linked polymers, nanoparticles, carbon nanotubes, poly(dimethylsiloxane), sepiolite, talc, montmorillonite, sphagnum peat moss, charcoal, and sawdust mixtures, combinations thereof, and the like.

[0038]

[0042] In some embodiments, an absorbent material may be used in addition to the base and / or die having a cavity. In some embodiments, an absorbent material may be used instead of the base and / or die having a cavity. In some embodiments, the cavity may be at least partially filled with the absorbent material such that when extracted electrolyte is transferred into the cavity, the absorbent material can capture all, substantially all, most, some, or a portion of the extracted electrolyte to prevent at least that portion from being reabsorbed into the semi-solid electrode material. In some embodiments, the absorbent material may be positioned such that when extracted electrolyte or a portion thereof is transferred through the cavity, for example, through the cavity into a reservoir or drain fluidly coupled to the cavity, the absorbent material can capture all, substantially all, most, some, or a portion of the extracted electrolyte to prevent at least that portion from being transferred back into the cavity and / or reabsorbed into the semi-solid electrode material. In some embodiments, the absorbent material may be positioned near the edges of the base, die, and / or intermediate electrode such that a portion of the electrolyte removed from the semi-solid electrode material through the edge of the intermediate electrode can be captured, substantially captured, or at least partially captured by the absorbent material. In some embodiments, the absorbent material may be inserted between the die or base and the semi-permeable membrane. In some embodiments, the absorbent material may be inserted between the porous current collector and the base or die. In some embodiments, the absorbent material may be positioned in more than one of the configurations described herein; for example, the absorbent material may be disposed between the base and the current collector, between the die and the semi-permeable membrane positioned on the exposed surface of the semi-solid electrode material, and near the edge of the intermediate electrode such that all or substantially all of the removed excess electrolyte can be captured by the absorbent material.

[0039]

[0043] In some embodiments, once the composition of the semi-solid electrode material matches or substantially matches the desired composition of the semi-solid electrode material in the finished electrode, the electrode can be removed from the mechanical press. In some embodiments, the electrode can be weighed before being mechanically pressed, then mechanically pressed for a first period of time to remove a first portion of the electrolyte, and then weighed again, with the difference between the first and second weights being usable to determine the mass of the electrolyte removed. If the mass of the removed electrolyte sufficiently matches the desired volume or mass of the electrolyte to be removed, the electrode can be considered a finished electrode and is ready for further processing or incorporation into an electrochemical cell. If the mass of the removed electrolyte does not sufficiently match the desired volume or mass of the electrolyte to be removed, the electrode can be mechanically pressed for a second period of time to remove a second portion of the electrolyte, and then weighed a third time, with the difference between the second and third weights being usable to determine the mass of the electrolyte removed during the second period of time. The electrode can be considered a finished electrode when the mass of electrolyte removed during the first time period plus the mass of electrolyte removed during the second time period equals or substantially equals the desired mass of electrolyte to be removed from the semi-solid electrode material. Mechanical compression of the intermediate electrode can continue in this repetitive manner until the total volume or mass of electrolyte removed equals or substantially equals the desired volume or mass of electrolyte to be removed. In some embodiments, if more than the desired amount of electrolyte has been removed from the electrode, electrolyte can be reapplied to the semi-solid electrode. In some embodiments, reapplication of electrolyte can be by spraying, dripping, or other suitable application method.

[0040]

[0044] In some embodiments, the completed electrode may include an electrode tab electrically connected to the current collector and configured to transport electrons into or out of the electrode. In some embodiments, the electrode tab may extend beyond the current collector and / or insulating material. In some embodiments, the electrode tab may be electrically coupled to the current collector before the semi-solid electrode material is disposed on the current collector. In some embodiments, the cell may include integrated electrical tabbing, which can eliminate the need for (i) a separate tab component (e.g., electrical lead), (ii) connecting a dedicated tab to the current collector, and (iii) a dedicated tab sealing operation. Alternatively, in some embodiments, the electrical tab or lead may be provided as an extension of the current collector that is integral with the current collector. In some embodiments, the tab or lead may be defined by removing material from a larger area of ​​the current collector material, thereby defining the current collector and the tab or lead.

[0041]

[0045] Method 10 optionally includes smoothing and / or planarizing the surface of the electrode (e.g., cathode) (14) to prevent voids between the electrode and the separator in the completed electrochemical cell. Contact between the electrode and the absorbent material can leave the surface of the electrode uneven and uneven. Smoothing and / or planarizing the electrode surface can make the surface of the electrode flush with the surface that will ultimately contact it (e.g., the separator surface, the current collector surface, the surface of the second electrode). Configuring these surfaces to be flush with each other can help prevent overvoltage losses due to voids between these surfaces. In some embodiments, smoothing and / or planarizing the electrode surface can be performed using a doctor blade, spatula, or other suitable smoothing device.

[0042]

[0046] Method 10 optionally includes forming a completed electrochemical cell by joining the completed electrode (e.g., cathode) with a second completed electrode (e.g., anode) with a separator interposed therebetween (15). That is, once the completed electrode is singulated and excess electrolyte is removed, the completed electrode can be assembled into an electrochemical cell with a second completed electrode exhibiting the opposite redox reaction. That is, the cathode and anode can be joined together with a separator disposed therebetween.

[0043]

[0047] In some embodiments, a separator may be disposed between the anode and the cathode. In some embodiments, the separator may be bonded to at least one of the anode and the cathode using an adhesive. In some embodiments, one anode, one cathode, and one separator may be stacked together to form a unit cell assembly. Each unit cell assembly may also include conductive tabs (also called wires) for coupling the electrodes to an external circuit. Multiple unit cell assemblies are then stacked or arranged together to form a battery cell. In some embodiments, the number of unit cell assemblies in a battery cell may vary depending, for example, on the desired capacity and / or thickness of the resulting battery cell. These stacked unit cell assemblies are electrically connected in parallel, and the respective tabs of each unit cell assembly are typically welded together by a welding process such as resistance welding, laser welding, ultrasonic welding, seam welding, or electric beam welding, among others.

[0044]

[0048] Method 10 optionally includes pressing the electrochemical cell or electrochemical cell stack to ensure contact throughout the electrochemical cell or electrochemical cell stack. Applying force to the electrochemical cell or electrochemical cell stack can help reduce or substantially eliminate voids in the electrochemical cell or electrochemical cell stack. These voids may exist at interfaces between electrodes and separators, between electrodes and current collectors, and / or between electrochemical cells.

[0045]

[0049] In some embodiments, the prepared electrochemical cell may be vacuum-sealed in a prismatic pouch, which can provide airtight isolation of the electrochemical cell materials from the environment. The pouch can thus help prevent leakage of harmful substances, such as electrolyte solvents and / or corrosive salts, into the surrounding environment and prevent ingress of water and / or oxygen into the cell. Other functions of the pouch may include, for example, compressive packaging of the inner layers, voltage isolation for safety and handling, and mechanical protection of the electrochemical cell assembly. In some embodiments, electrolyte may be injected into the stacked unit cell assembly during vacuum pouch sealing, and the unit cell assembly and electrolyte may then be sealed within the pouch. In some embodiments, electrolyte is not added during the pouch sealing step if the semi-solid electrode material may already contain the desired total amount of electrolyte.

[0046]

[0050] In some embodiments, the sealed battery cell may then undergo a formation process, during which an initial charging operation may be performed, to create a stable solid-electrolyte interphase (SEI) layer that can passivate the electrode-electrolyte interface and prevent side reactions. In some embodiments, several charge and discharge cycles may be performed to ensure that the battery's capacity meets required specifications. In some embodiments, a degassing step may be performed to release gases introduced or generated during the initial charging stage or during the electrochemical reactions of the battery formation step. The presence of trapped gas in the electrode generally reduces the electrode's conductivity and density, limits the amount of active electrochemical material that can be installed in the battery cell, and can cause dendrite growth in lithium batteries, which can impair battery performance. In some embodiments, dendrite formation can cause reduced cycle life and overall safety performance. In some embodiments, a resealing step may be performed to reseal the battery cell after release of trapped gases.

[0047]

[0051] 2A-2E illustrate a method 20 for forming a semi-solid electrode material 230b having a higher active material concentration and a higher energy density without the need for electrolyte injection and / or drying steps. The method 20 includes, at 21, first forming an intermediate electrode by placing stencils 220a, 220b (collectively, "stencil 220") on a current collector 210 (e.g., a foil current collector). The current collector 210 may be any suitably conductive material configured to transport ions / electrons between the electrode material and a source or sink. In some embodiments, the stencil 220 may comprise any material that is impervious to the transport of semi-solid electrode material therethrough. In some embodiments, the stencil 220 may be sized and configured to extend near, or substantially near, the perimeter of the current collector 210 or near the outer dimensions of the current collector 210. In some embodiments, the stencil 220 may have the same or substantially the same dimensions as the current collector 210. In some embodiments, stencil 220 can include a masking material, such as the masking materials described in the '483 application. In some embodiments, the masking material can be a tape or similar material that can be applied on or near current collector 210 to contain the semi-solid electrode material during deposition of the semi-solid electrode material on current collector 210, during the laser step of manufacturing the electrochemical cell, and / or during use of the electrochemical cell.

[0048]

[0052] In some embodiments, instead of or in addition to a masking material as described above, an endo frame structure may be placed on the current collector 210 before the semi-solid electrode material is placed on the current collector 210. In some embodiments, the endo frame may hold the current collector 210 in place or substantially in place during deposition of the semi-solid electrode material. In some embodiments, the endo frame may have at least some z-direction thickness such that the endo frame at least partially defines an interior region within which the semi-solid electrode material may be placed and held on the surface of the current collector 210.

[0049]

[0053] In some embodiments, the inner frame can at least partially define the surface area of ​​the finished electrode (e.g., as the inner extent of the inner frame). In some embodiments, the inner frame can at least partially define the thickness of the semi-solid electrode material on the current collector 210 based on the z-direction height of the inner frame.

[0050]

[0054] In some embodiments, the stencil 220 may include two inner frames, where a first inner frame 220a may be placed directly on the current collector 210 or on a masking material placed on the current collector 210, and a second inner frame 220b may be placed on the first inner frame 220a.

[0051]

[0055] Method 20 further includes, at 22, depositing a semi-solid electrode material into the cavity and, optionally, spreading the semi-solid electrode material uniformly across the current collector foil. In some embodiments, depositing the semi-solid electrode material onto the current collector 210 can form a semi-solid electrode material 230a having a first composition. In some embodiments, dispensing the semi-solid electrode material can include forming or substantially forming an intermediate electrode by drop-casting the material onto a moving current collector. In some embodiments, dispensing the semi-solid electrode material can include extruding the semi-solid electrode material onto the fixed current collector 210 from a moving extrusion nozzle or the like. In some embodiments, the semi-solid electrode material can be dispensed onto the fixed current collector 210 by a fixed dispensing mechanism, e.g., in discrete portions, and then the discrete portions of the semi-solid electrode material can be spread across the surface of the current collector 210 by any suitable method to form or substantially form the intermediate electrode. In some embodiments, the current collector material may be distributed among multiple current collectors 210 such that each of the multiple current collectors 210 is isolated from the other current collectors. Discrete portions of semi-solid electrode material may then be disposed on the surface of each of the individualized current collectors 210 to form, or substantially form, an intermediate electrode. In some embodiments, the intermediate electrode formed according to step 22 of method 20 includes an intermediate electrode material (e.g., 230a) such that the intermediate electrode may be operable in an electrochemical cell but has a lower active solids loading than desired for the finished electrode. The formed intermediate electrode may be a positive electrode, an anode, a negative electrode, a cathode, or other electrode or component of an electrochemical cell. As described herein, the electrode may be a semi-solid electrode that includes at least an active material and / or a conductive material in a liquid electrolyte.

[0052]

[0056] In some embodiments, the semi-solid electrode material may be smoothed or spread along the surface of the exposed portion of the current collector 210. In some embodiments, a blade (also referred to herein as a "doctor blade") or other straight-edged implement may be used to spread the semi-solid electrode material. In some embodiments, the blade and / or inner frame may be operably coupled to a vibration source for vibrating the blade or inner frame during deposition or smoothing of the semi-solid electrode material. The vibration may facilitate distribution of the semi-solid electrode material during or after the semi-solid electrode material deposition step.

[0053]

[0057] Method 20 further includes removing the stencil at 23 to define the electrode and form the electrode edges. In some embodiments, step 23 may include removing the inner frame, the masking material, or both. In some embodiments, removing the stencil material may result in an intermediate electrode with smoother edges, with less edge breakdown, substantially no edge breakdown, or no edge breakdown. In some embodiments, a portion of the stencil may be removed, for example, the top layer or top half of the stencil, and the bottom layer or bottom half may be left in place on current collector 210.

[0054]

[0058] In some embodiments, once the stencil or a portion thereof is removed, the intermediate electrode may be weighed and / or the thickness of the intermediate electrode may be measured. In some embodiments, the weight of the intermediate electrode may be compared to a predetermined weight desired for the intermediate electrode. In some embodiments, the thickness (e.g., in the z-direction) of the intermediate electrode may be compared to a predetermined thickness desired for the intermediate electrode. In some embodiments, the predetermined weight and / or predetermined thickness may be a first weight or a first thickness.

[0055]

[0059] The method 20 further includes, at 24, placing the electrode in a mechanical press and applying a compressive force to extract a portion of the electrolyte from the semi-solid electrode material. In some embodiments, the mechanical press may include a base 250 a and a die 250 b, and moving the base and / or die applies a compressive force F to the intermediate electrode sufficient to extract a portion of the electrolyte from the semi-solid electrode material 230 a. In some embodiments, the mechanical press may include a press guide 260, such as a channel or multiple walls, to control the movement of the base 250 a and / or die 250 b during mechanical pressing. In some embodiments, once the portion of the electrolyte is removed by mechanical compression of the intermediate electrode, the electrode may include a semi-solid electrode material 230 b having a second composition in which the ratio of active material to electrolyte is higher than when the semi-solid electrode material 230 a has a first composition.

[0056]

[0060] In some embodiments, at least one of the base 250a and the die 250b may include a cavity such that removed electrolyte, or a portion thereof, may be retained within or transmitted through the cavity during mechanical compression of the intermediate electrode. In some embodiments, removed electrolyte, or a portion thereof, may exit the semi-solid electrode material and be transmitted through the porous current collector into or through the cavity during mechanical compression of the intermediate electrode. In some embodiments, removed electrolyte, or a portion thereof, may exit the semi-solid electrode material and be transmitted between the base and the die around the end or edge of the current collector. In some embodiments, removed electrolyte, or a portion thereof, may exit the semi-solid electrode material in a direction opposite the current collector 210 and be transmitted into or through the cavity. In some embodiments, removed electrolyte, or a portion thereof, may be transmitted out of the semi-solid electrode material 230a by more than one of the paths described herein. In some embodiments, the cavity may be fluidly coupled to a drain so that removed electrolyte transferred into or through the cavity can be removed from the mechanical press via the drain. In some embodiments, the cavity may be fluidly coupled to a reservoir so that removed electrolyte transferred into or through the cavity can be removed from the mechanical press via the reservoir. In some embodiments, the removed electrolyte held in the reservoir may be reusable and / or recyclable for use in other semi-solid electrodes or elsewhere.

[0057]

[0061] In some embodiments, a semi-permeable membrane (not shown) may be disposed on or near the semi-solid electrode material such that during mechanical compression of the intermediate electrode, the semi-permeable membrane does not allow transmission of active substances, conductive materials, etc., out of the semi-solid electrode material, but does allow transmission of electrolyte out of the semi-solid electrode material. In some embodiments, the semi-permeable membrane may be a sheet or other planar structure configured to be removed from on or near the semi-solid electrode material before or after removal of the intermediate electrode from the mechanical press and before incorporating the mechanically compressed electrode into an electrochemical cell or the like. In some embodiments, the semi-permeable membrane may be a conventional separator material configured to allow at least some flow of liquid electrolyte therethrough. In some embodiments, the semi-permeable membrane may be any material that is completely or substantially chemically inert with respect to the composition of the semi-solid electrode material 230a and / or current collector 210, while allowing at least some flow of liquid electrolyte therethrough. In some embodiments, the semi-permeable membrane may remain on or near the semi-solid electrode material throughout mechanical compression and construction of the electrochemical cell, such that the semi-permeable membrane is included in the finished electrochemical cell.

[0058]

[0062] In some embodiments, prior to mechanically pressing the intermediate electrode, e.g., at 24, absorbent material 240 may be disposed between a portion of the intermediate electrode and a component of the mechanical press. In some embodiments, absorbent material 240 may be disposed within the mechanical press, e.g., between the intermediate electrode and at least one of die 250b and base 250a, to absorb at least a portion of the electrolyte removed from the intermediate electrode. In some embodiments, absorbent material 240 may include any of fibrous materials, cotton, rice hulls, superhydrophobic sawdust, cellulosic materials, superabsorbent polymers, zeolite materials, aerogels, nanocellulose aerogels, hydrogels, polyurethane, polypropylene, polyethylene, and cross-linked polymers, nanoparticles, carbon nanotubes, poly(dimethylsiloxane), sepiolite, talc, montmorillonite, sphagnum peat moss, charcoal, and sawdust mixtures, combinations thereof, and the like.

[0059]

[0063] In some embodiments, the absorbent material 240 may be used in addition to the base and / or die having a cavity. In some embodiments, the absorbent material 240 may be used instead of the base and / or die having a cavity. In some embodiments, the cavity may be at least partially filled with the absorbent material such that when extracted electrolyte is transferred into the cavity, the absorbent material 240 can capture all, substantially all, most, some, or a portion of the extracted electrolyte to prevent at least that portion from being reabsorbed into the semi-solid electrode material 230b. In some embodiments, the absorbent material 240 may be positioned such that when extracted electrolyte or a portion thereof is transferred through the cavity, for example, through the cavity into a reservoir or drain fluidly coupled to the cavity, the absorbent material 240 can capture all, substantially all, most, some, or a portion of the extracted electrolyte to prevent at least that portion from being transferred back into the cavity and / or reabsorption into the semi-solid electrode material 230b. In some embodiments, the absorbent material 240 may be positioned near the base 250a, the die 250b, and / or the edge of the intermediate electrode such that a portion of the electrolyte removed from the semi-solid electrode material 230a through the edge of the intermediate electrode can be captured, substantially captured, or at least partially captured by the absorbent material 240. In some embodiments, the absorbent material 240 may be inserted between the die 250b or the base 250a and the semi-permeable membrane. In some embodiments, the absorbent material 240 may be inserted between the porous current collector 210 and the base 250a or the die 250b. In some embodiments, the absorbent material 240 may be positioned in more than one of the configurations described herein; for example, the absorbent material 240 may be disposed between the base 250a and the current collector 210, between the die 250b and the semi-permeable membrane positioned on the exposed surface of the semi-solid electrode material 230a, and near the edge of the intermediate electrode such that all or substantially all of the removed excess electrolyte can be captured by the absorbent material 240.

[0060]

[0064] Method 20 further includes disassembling the mechanical press assembly and removing the absorbent material 240, the semi-permeable membrane, and / or any remaining stencil material (e.g., first inner frame 220a) to form a finished semi-solid electrode having a higher active solids loading. In some embodiments, removing a portion of the electrolyte from the intermediate electrode forms a finished electrode having a higher active solids loading than the aforementioned semi-solid electrode material and electrode constructed therefrom. Without wishing to be bound by any particular theory, removing a portion of the electrolyte (e.g., an excess portion of liquid electrolyte) can reduce the volume of the semi-solid electrode material on the current collector by removing the electrolyte and by compressing and removing voids and porosity without a corresponding decrease in conductivity throughout the semi-solid electrode material. In some embodiments, the reduction in porosity can include a reduction in porosity from approximately about 20% to about 50% to about 5% to about 30%, including all values ​​and ranges therebetween.

[0061]

[0065] In some embodiments, the first composition of the semi-solid electrode material 230a can include between about 20% and about 80% by volume of active material. In some embodiments, the first composition of the semi-solid electrode material 230a can include between about 40% and about 80% by volume, or between about 50% and about 80% by volume of active material. In some embodiments, the first composition of the semi-solid electrode material 230a can include at least about 20%, at least about 25%, at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%, at least about 65%, at least about 70%, or at least about 75% by volume of active material. In some embodiments, the first composition of the semi-solid electrode material 230a can include about 80% or less, about 75% or less, about 70% or less, about 65% or less, about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, about 35% or less, about 30% or less, or about 25% or less by volume of active material. Combinations of the above volume percentages of active material in the first composition of the semi-solid electrode material 230a are also possible (e.g., at least about 20% by volume and about 80% or less by volume, or at least about 30% by volume and about 60% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the first composition of the semi-solid electrode material 230a can include about 20%, about 25%, about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, about 60%, about 65%, about 70%, about 75%, or about 80% active material by volume.

[0062]

[0066] In some embodiments, the first composition of the semi-solid electrode material 230a can include between about 0.5% and about 25% by volume of conductive material. In some embodiments, the first composition of the semi-solid electrode material 230a can include between about 1.0% and about 6% by volume of conductive material. In some embodiments, the first composition of the semi-solid electrode material 230a can include at least about 0.5%, at least about 1%, at least about 1.5%, at least about 2%, at least about 2.5%, at least about 3%, at least about 3.5%, at least about 4%, at least about 4.5%, at least about 5%, at least about 5.5%, at least about 6%, at least about 6.5%, at least about 7%, at least about 7.5%, at least about 8%, at least about 8.5%, at least about 9%, at least about 9.5%, at least about 10%, at least about 15%, or at least about 20% by volume of conductive material. In some embodiments, the first composition of the semi-solid electrode material 230a can include about 25% or less, about 20% or less, about 15% or less, about 10% or less, about 9.5% or less, about 9% or less, about 8.5% or less, about 8% or less, about 7.5% or less, about 7% or less, about 6.5% or less, about 6% or less, about 5.5% or less, about 5% or less, about 4.5% or less, about 4% or less, about 3.5% or less, about 3% or less, about 2.5% or less, about 2% or less, about 1.5% or less, or about 1% or less by volume of conductive material. Combinations of the above volume percentages of conductive material in the first composition of the semi-solid electrode material 230a are also possible (e.g., at least about 0.5% by volume and about 25% or less by volume, or at least about 3% by volume and about 10% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the first composition of the semi-solid electrode material 230a can include about 0.5%, about 1%, about 1.5%, about 2%, about 2.5%, about 3%, about 3.5%, about 4%, about 4.5%, about 5%, about 5.5%, about 6%, about 6.5%, about 7%, about 7.5%, about 8%, about 8.5%, about 9%, about 9.5%, about 10%, about 15%, about 20%, or about 25% conductive material by volume.

[0063]

[0067] In some embodiments, the first composition of the semi-solid electrode material 230a can include about 25% to about 70% electrolyte by volume. In some embodiments, the first composition of the semi-solid electrode material 230a can include about 30% to about 50%, or about 20% to about 40% electrolyte by volume. In some embodiments, the first composition of the semi-solid electrode material 230a can include at least about 25%, at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%, or at least about 65% electrolyte by volume. In some embodiments, the first composition of the semi-solid electrode material 230a can be about 70% or less, about 65% or less, about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, about 35% or less, or about 30% or less electrolyte by volume. Combinations of the above volume percentages of electrolyte in the first composition of the semi-solid electrode material 230a are also possible (e.g., at least about 25% and not more than about 70%, or at least about 30% and not more than about 50%), including all values ​​and ranges therebetween. In some embodiments, the first composition of the semi-solid electrode material 230a can include about 25%, about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, about 60%, about 65%, or about 70% electrolyte by volume.

[0064]

[0068] In some embodiments, the second composition of semi-solid electrode material 230b can include about 30% to about 85% by volume of active material. In some embodiments, the second composition of semi-solid electrode material 230b can include about 50% to about 85% by volume, or 60% to about 85% by volume of active material. In some embodiments, the second composition of semi-solid electrode material 230b can include at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%, at least about 65%, at least about 70%, at least about 75%, or at least about 80% by volume of active material. In some embodiments, the second composition of the semi-solid electrode material 230b can include about 85% or less, about 80% or less, about 75% or less, about 70% or less, about 65% or less, about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, or about 35% or less by volume of active material. Combinations of the above volume percentages of active material in the second composition of the semi-solid electrode material 230b are also possible (e.g., at least about 30% by volume and about 85% or less by volume, or at least about 40% by volume and about 70% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the second composition of the semi-solid electrode material 230b can include about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, about 60%, about 65%, about 70%, about 75%, about 80%, or about 85% active material by volume.

[0065]

[0069] In some embodiments, the second composition of the semi-solid electrode material 230b can include between about 0.5% and about 30% by volume of conductive material. In some embodiments, the second composition of the semi-solid electrode material 230b can include between about 1.0% and about 6% by volume of conductive material. In some embodiments, the second composition of the semi-solid electrode material 230b can include at least about 0.5%, at least about 1%, at least about 1.5%, at least about 2%, at least about 2.5%, at least about 3%, at least about 3.5%, at least about 4%, at least about 4.5%, at least about 5%, at least about 5.5%, at least about 6%, at least about 6.5%, at least about 7%, at least about 7.5%, at least about 8%, at least about 8.5%, at least about 9%, at least about 9.5%, at least about 10%, at least about 15%, at least about 20%, or at least about 25% by volume of conductive material. In some embodiments, the second composition of the semi-solid electrode material 230b can include about 30% or less, about 25% or less, about 20% or less, about 15% or less, about 10% or less, about 9.5% or less, about 9% or less, about 8.5% or less, about 8% or less, about 7.5% or less, about 7% or less, about 6.5% or less, about 6% or less, about 5.5% or less, about 5% or less, about 4.5% or less, about 4% or less, about 3.5% or less, about 3% or less, about 2.5% or less, about 2% or less, about 1.5% or less, or about 1% or less by volume of conductive material. Combinations of the above volume percentages of conductive material in the second composition of the semi-solid electrode material 230b are also possible (e.g., at least about 0.5% by volume and about 30% or less by volume, or at least about 5% by volume and about 10% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the second composition of the semi-solid electrode material 230b can include about 0.5%, about 1%, about 1.5%, about 2%, about 2.5%, about 3%, about 3.5%, about 4%, about 4.5%, about 5%, about 5.5%, about 6%, about 6.5%, about 7%, about 7.5%, about 8%, about 8.5%, about 9%, about 9.5%, about 10%, about 15%, about 20%, about 25%, or about 30% conductive material by volume.

[0066]

[0070] In some embodiments, the second composition of semi-solid electrode material 230b can include about 15% to about 60% electrolyte by volume. In some embodiments, the second composition of semi-solid electrode material 230b can include about 20% to about 40% or about 10% to about 30% electrolyte by volume. In some embodiments, the second composition of semi-solid electrode material 230b can include at least about 15%, at least about 20%, at least about 25%, at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, or at least about 55% electrolyte by volume. In some embodiments, the second composition of semi-solid electrode material 230b can be about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, about 35% or less, about 30% or less, about 25% or less, or about 20% or less electrolyte by volume. Combinations of the above volume percentages of electrolyte in the second composition of semi-solid electrode material 230b are also possible (e.g., at least about 15% and not more than about 60%, or at least about 20% and not more than about 40%, including all values ​​and ranges therebetween). In some embodiments, the second composition of semi-solid electrode material 230b can include about 15%, about 20%, about 25%, about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, or about 60% electrolyte by volume.

[0067]

[0071] In some embodiments, the second composition of semi-solid electrode material 230b can have a lower ratio of electrolyte to active material than the first composition of semi-solid electrode material 230a. In some embodiments, the second composition of semi-solid electrode material 230b can have a ratio of electrolyte to active material of about 5:1 to about 1:6, about 5:1 to about 1:5, about 5:1 to about 1:4, about 5:1 to about 1:3, about 4:1 to about 1:2, about 3:1 to about 1:1, about 5:1 to about 1:2, about 5:1 to about 1:1, about 5:1 to about 2:1, about 5:1 to about 3:1, about 5:1 to about 4:1, or about 4:1 to about The active agent may have a v / v ratio of electrolyte to active agent of 1:3, about 3:1 to about 1:3, about 2:1 to about 1:3, about 1:1 to about 1:3, about 1:2 to about 1:3, about 1:2 to about 1:4, about 1:2 to about 1:5, about 1:2 to about 1:6, about 1:3 to about 1:6, about 1:4 to about 1:6, or about 1:5 to about 1:6 (including all values ​​and ranges therebetween).

[0068]

[0072] In some embodiments, the weight and / or thickness of the semi-solid electrode can be measured at various points throughout the process of mechanically pressing the intermediate electrode to form the finished electrode. For example, in some embodiments, the weight of the finished electrode can be a second weight and compared to the first weight to determine the mass of electrolyte removed during mechanical pressing. In some embodiments, the thickness of the finished electrode can be a second thickness and compared to the first thickness to determine the volume of electrolyte removed during mechanical pressing. In some embodiments, if the difference between the first and second weights or the difference between the first and second thicknesses of the semi-solid electrode material 230b is not sufficient, the absorbent material 240 and / or semi-permeable membrane can be placed again on the semi-solid electrode, and the intermediate electrode can be further mechanically compressed to remove a second portion of the electrolyte from the semi-solid electrode material 230b. In some embodiments, the volume or mass of the electrolyte removed during mechanical pressing can be used to determine the relative volume or mass percentage of the active material, conductive material, and electrolyte in the semi-solid electrode material 230b.

[0069]

[0073] In some embodiments, once the composition of the semi-solid electrode material 230b matches or substantially matches the desired composition of the semi-solid electrode material 230b in the finished electrode, the electrode can be removed from the mechanical press. In some embodiments, the electrode can be weighed before being mechanically pressed, then mechanically pressed for a first period of time to remove a first portion of the electrolyte, and then weighed again, with the difference between the first and second weights being usable to determine the mass of the removed electrolyte. If the mass of the removed electrolyte sufficiently matches the desired volume or mass of electrolyte to be removed, the electrode can be considered a finished electrode and is ready for further processing or incorporation into an electrochemical cell (not shown). If the mass of the removed electrolyte does not sufficiently match the desired volume or mass of electrolyte to be removed, the electrode may be mechanically pressed for a second period of time to remove a second portion of the electrolyte, and then weighed a third time; the difference between the second and third weights can be used to determine the mass of electrolyte removed during the second period of time. When the mass of electrolyte removed during the first period of time plus the mass of electrolyte removed during the second period of time equals or substantially equals the desired mass of electrolyte to be removed from the semi-solid electrode material, the electrode may be considered a finished electrode. Mechanical compression of the intermediate electrode may continue in this iterative manner until the total volume or mass of removed electrolyte equals or substantially equals the desired volume or mass of electrolyte to be removed.

[0070]

[0074] In some embodiments, the completed electrode may include an electrode tab electrically connected to the current collector and configured to transport electrons into or out of the electrode. In some embodiments, the electrode tab may extend beyond the current collector and / or insulating material. In some embodiments, the electrode tab may be electrically coupled to the current collector before the semi-solid electrode material is disposed on the current collector. In some embodiments, the cell may include integrated electrical tabs, which may eliminate the need for (i) separate tab components (e.g., electrical leads), (ii) connecting a dedicated tab to the current collector, and (iii) a dedicated tab sealing operation. Instead, in some embodiments, the electrical tab or lead may be provided as an extension of the current collector that is integral with the current collector. In some embodiments, the tab or lead may be defined by removing material from a larger area of ​​the current collector material, thereby defining the current collector and the tab or lead.

[0071]

[0075] Method 20 optionally includes forming a completed electrochemical cell by joining a completed electrode (e.g., a cathode) with a second completed electrode (e.g., an anode) with a separator interposed therebetween. That is, once the completed electrode is singulated and excess electrolyte is removed, the completed electrode can be assembled into an electrochemical cell with a second completed electrode exhibiting the opposite redox reaction. That is, the cathode and anode can be joined together with a separator disposed therebetween.

[0072]

[0076] In some embodiments, a separator may be disposed between the anode and the cathode. In some embodiments, the separator may be bonded to at least one of the anode and the cathode using an adhesive. In some embodiments, one anode, one cathode, and one separator may be stacked together to form a unit cell assembly. Each unit cell assembly may also include conductive tabs (also called wires) for coupling the electrodes to an external circuit. Multiple unit cell assemblies are then stacked or arranged together to form a battery cell. In some embodiments, the number of unit cell assemblies in a battery cell may vary depending, for example, on the desired capacity and / or thickness of the resulting battery cell. These stacked unit cell assemblies are electrically connected in parallel, and the respective tabs of each unit cell assembly are typically welded together by a welding process such as resistance welding, laser welding, ultrasonic welding, seam welding, or electric beam welding, among others.

[0073]

[0077] In some embodiments, the prepared electrochemical cell may be vacuum-sealed in a prismatic pouch, which can provide airtight isolation of the electrochemical cell materials from the environment. The pouch can thus help prevent leakage of harmful substances, such as electrolyte solvents and / or corrosive salts, into the surrounding environment and prevent ingress of water and / or oxygen into the cell. Other functions of the pouch may include, for example, compressive packaging of the inner layers, voltage isolation for safety and handling, and mechanical protection of the electrochemical cell assembly. In some embodiments, electrolyte may be injected into the stacked unit cell assembly during vacuum pouch sealing, and the unit cell assembly and electrolyte may then be sealed within the pouch. In some embodiments, electrolyte is not added during the pouch sealing step if the semi-solid electrode material may already contain the desired total amount of electrolyte.

[0074]

[0078] In some embodiments, the sealed battery cell may then undergo a formation process, during which an initial charging operation may be performed to create a stable SEI layer that can passivate the electrode-electrolyte interface and prevent side reactions. In some embodiments, several charge and discharge cycles may be performed to ensure that the battery's capacity meets required specifications. In some embodiments, a degassing step may be performed to release gases introduced or generated during the initial charging stage or during the electrochemical reactions of the battery formation step. The presence of trapped gases in the electrode generally reduces the electrode's conductivity and density, limits the amount of active electrochemical material that can be installed in the battery cell, and can cause dendrite growth in lithium batteries, which can impair battery performance. In some embodiments, dendrite formation can cause reduced cycle life and overall safety performance. In some embodiments, a resealing step may be performed to reseal the battery cell after the release of trapped gases.

[0075]

[0079] 3A-3E illustrate a method 30 for forming a semi-solid electrode material with a higher active material concentration and a higher energy density without the need for an electrolyte injection step and / or a drying step. The method 30 includes, at 31, first forming an intermediate electrode by placing stencils 320a, 320b (collectively "stencil 320") on a current collector 310 (e.g., a foil current collector). The current collector 310 may be any suitably conductive material configured to transport ions / electrons between the electrode material and a source or sink. In some embodiments, the stencil 320 may comprise any material that is impervious to the transport of the semi-solid electrode material therethrough. In some embodiments, the stencil 320 may be sized and configured to extend near or substantially near the perimeter of the current collector 310. In some embodiments, the stencil 320 may have the same or substantially the same dimensions as the current collector 310. In some embodiments, the stencil 320 may include a masking material, such as the masking materials described in the '483 application. In some embodiments, the masking material may be a tape or similar material that may be applied on or near the current collector 310 to contain the semi-solid electrode material during deposition of the semi-solid electrode material onto the current collector 310.

[0076]

[0080] In some embodiments, instead of or in addition to a masking material as described above, an inner frame structure may be placed on the current collector 310 before the semi-solid electrode material is placed on the current collector 310. In some embodiments, the inner frame may hold the current collector 310 in place, or substantially in place, during deposition of the semi-solid electrode material. In some embodiments, the inner frame may have at least some z-direction thickness such that the inner frame at least partially defines an interior region within which the semi-solid electrode material may be placed and held on the surface of the current collector 310.

[0077]

[0081] In some embodiments, the inner frame can at least partially define the surface area of ​​the finished electrode (e.g., as the inner extent of the inner frame). In some embodiments, the inner frame can at least partially define the thickness of the semi-solid electrode material on the current collector 310 based on the z-direction height of the inner frame.

[0078]

[0082] In some embodiments, the stencil 320 may include two inner frames, where a first inner frame 320a may be placed directly on the current collector 310 or on a masking material placed on the current collector 310, and a second inner frame 320b may be placed on the first inner frame 320a.

[0079]

[0083] The method 30 further includes, at 32, depositing a semi-solid electrode material into the cavity and, optionally, spreading the semi-solid electrode material uniformly across the current collector foil. In some embodiments, depositing the semi-solid electrode material onto the current collector 310 can form a semi-solid electrode material 330a having a first composition. In some embodiments, dispensing the semi-solid electrode material can include forming or substantially forming an intermediate electrode by drop-casting the semi-solid electrode material onto a moving current collector. In some embodiments, dispensing the semi-solid electrode material can include extruding the semi-solid electrode material onto the fixed current collector 310 from a moving extrusion nozzle or the like. In some embodiments, the semi-solid electrode material can be dispensed onto the fixed current collector 310 by a fixed dispensing mechanism, e.g., in discrete portions, and then the discrete portions of the semi-solid electrode material can be spread across the surface of the current collector 310 by any suitable method to form or substantially form the intermediate electrode. In some embodiments, the current collector material may be distributed among multiple current collectors 310 such that each of the multiple current collectors 310 is isolated from the other current collectors. Discrete portions of semi-solid electrode material may then be disposed on the surface of each of the individualized current collectors 310 to form, or substantially form, an intermediate electrode. In some embodiments, the intermediate electrode formed according to step 32 of method 30 includes an intermediate electrode material (e.g., 330a) such that the intermediate electrode may be operable in an electrochemical cell but has a lower active solids loading than desired for the finished electrode. The formed intermediate electrode may be a positive electrode, an anode, a negative electrode, a cathode, or other electrode or component of an electrochemical cell. As described herein, the electrode may be a semi-solid electrode comprising at least an active material and / or a conductive material in a liquid electrolyte.

[0080]

[0084] In some embodiments, the semi-solid electrode material may be smoothed or spread along the surface of the exposed portion of the current collector 310. In some embodiments, a blade (also referred to herein as a "doctor blade") or other straight-edged implement may be used to spread the semi-solid electrode material. In some embodiments, the blade and / or inner frame may be operably coupled to a vibration source for vibrating the blade or inner frame during deposition or smoothing of the semi-solid electrode material. The vibration may facilitate distribution of the semi-solid electrode material during or after the semi-solid electrode material deposition step.

[0081]

[0085] Method 30 further includes removing the stencil at 33 to define the electrode and form the electrode edges. In some embodiments, step 33 may include removing the inner frame, the masking material, or both. In some embodiments, removing the stencil material may result in an intermediate electrode with smoother edges, with less edge breakdown, substantially no edge breakdown, or no edge breakdown. In some embodiments, a portion of the stencil may be removed, for example, the top layer or top half of the stencil, and the bottom layer or bottom half may be left in place on the current collector 310.

[0082]

[0086] In some embodiments, once the stencil or a portion thereof is removed, the intermediate electrode may be weighed and / or the thickness of the intermediate electrode may be measured. In some embodiments, the weight of the intermediate electrode may be compared to a predetermined weight desired for the intermediate electrode. In some embodiments, the thickness (e.g., in the z-direction) of the intermediate electrode may be compared to a predetermined thickness desired for the intermediate electrode. In some embodiments, the predetermined weight and / or predetermined thickness may be a first weight or a first thickness.

[0083]

[0087] The method 30 further includes, at 34, applying a compressive force F to extract a portion of the electrolyte from the semi-solid electrode material. In some embodiments, the compressive force may be applied to the semi-solid electrode material by a roller or the like. As shown, the roller rotates along direction R. In some embodiments, the roller may be moved across a surface of a fixed intermediate electrode to apply the compressive force F. In some embodiments, the intermediate electrode may be positioned on a base (not shown), and the roller may be moved across the surface of the fixed intermediate electrode. In some embodiments, the intermediate electrode may be moved through, past, or under the roller so that the roller can apply the compressive force F. In some embodiments, the intermediate electrode may be transported along a conveyor below the roller. In some embodiments, the intermediate electrode may be moved through multiple rollers so that multiple rollers apply the compressive force F. In some embodiments, when a portion of the electrolyte is removed by mechanical compression of the intermediate electrode, the electrode may include a semi-solid electrode material 330b having a second composition in which the ratio of active material to electrolyte is higher than when the semi-solid electrode material 330a has the first composition.

[0084]

[0088] In some embodiments, the base, the roller, one of the rollers, and / or each of the rollers may include a cavity such that removed electrolyte, or a portion thereof, may be retained within or transmitted through the cavity during mechanical compression of the intermediate electrode. In some embodiments, removed electrolyte, or a portion thereof, may exit the semi-solid electrode material and be transmitted through the porous current collector into or through the cavity during mechanical compression of the intermediate electrode. In some embodiments, removed electrolyte, or a portion thereof, may exit the semi-solid electrode material and be transmitted between the base and the roller or rollers around an end or edge of the current collector. In some embodiments, removed electrolyte, or a portion thereof, may exit the semi-solid electrode material in a direction opposite the current collector 310 and be transmitted into or through the cavity. In some embodiments, removed electrolyte, or a portion thereof, may be transmitted out of the semi-solid electrode material 330a by more than one of the paths described herein. In some embodiments, the cavity may be fluidly coupled to a drain so that removed electrolyte transferred into or through the cavity can be removed from the mechanical press via the drain. In some embodiments, the cavity may be fluidly coupled to a reservoir so that removed electrolyte transferred into or through the cavity can be removed from the mechanical press via the reservoir. In some embodiments, the removed electrolyte held in the reservoir may be reusable and / or recyclable for use in other semi-solid electrodes or elsewhere.

[0085]

[0089] In some embodiments, a semi-permeable membrane (not shown) may be disposed on or near the semi-solid electrode material such that during mechanical compression of the intermediate electrode, the semi-permeable membrane does not allow transmission of active substances, conductive materials, or the like, out of the semi-solid electrode material, but does allow transmission of electrolyte out of the semi-solid electrode material. In some embodiments, the semi-permeable membrane may be a sheet or other planar structure configured to be removed from on or near the semi-solid electrode material before or after removal of the intermediate electrode from the mechanical press and before incorporating the mechanically compressed electrode into an electrochemical cell or the like. In some embodiments, the semi-permeable membrane may be a conventional separator material configured to allow at least some flow of liquid electrolyte therethrough. In some embodiments, the semi-permeable membrane may be any material that is completely or substantially chemically inert with respect to the composition of the semi-solid electrode material and / or current collector 310, while allowing at least some flow of liquid electrolyte therethrough. In some embodiments, the semi-permeable membrane may remain on or near the semi-solid electrode material throughout mechanical compression and construction of the electrochemical cell, such that the semi-permeable membrane is included in the finished electrochemical cell.

[0086]

[0090] In some embodiments, prior to mechanically pressing the intermediate electrode, e.g., at 34, an absorbent material 340 may be disposed between a portion of the intermediate electrode and at least one of the base, roller, or plurality of rollers. In some embodiments, the absorbent material 340 may be disposed between the intermediate electrode and the roller to absorb at least a portion of the electrolyte removed from the intermediate electrode. In some embodiments, the absorbent material 340 may include any of fibrous materials, cotton, rice hulls, superhydrophobic sawdust, cellulosic materials, superabsorbent polymers, zeolite materials, aerogels, nanocellulose aerogels, hydrogels, polyurethane, polypropylene, polyethylene, and cross-linked polymers, nanoparticles, carbon nanotubes, poly(dimethylsiloxane), sepiolite, talc, montmorillonite, sphagnum peat moss, charcoal, and sawdust mixtures, combinations thereof, and the like.

[0087]

[0091] In some embodiments, the absorbent material 340 may be used in addition to a base, roller, and / or rollers having one or more cavities. In some embodiments, the absorbent material 340 may be used instead of a base, roller, and / or rollers having one or more cavities. In some embodiments, the absorbent material 340 may be circulated by multiple rollers. That is, two or more rollers (or a roller and a pivot point) may keep the flat side of the absorbent material 340 in contact with the semi-solid electrode material 330a. In some embodiments, the absorbent material 340 may remove electrolyte from the semi-solid electrode 330a in a continuous or semi-continuous operation. In some embodiments, the absorbent material 340 may be circulated, and electrolyte may be removed from the absorbent material 340 at locations spaced apart from the semi-solid electrode 330a. That is, the absorbent material 340 may be "rejuvenated" and recirculated to again contact the semi-solid electrode 330a. In some embodiments, the cavity may be at least partially filled with absorbent material such that when extracted electrolyte is transferred into the cavity, the absorbent material 340 can trap all, substantially all, most, some, or a portion of the extracted electrolyte to prevent at least a portion of it from being reabsorbed into the semi-solid electrode material 330 b. In some embodiments, the absorbent material 340 may be positioned such that when extracted electrolyte or a portion thereof is transferred through the cavity, e.g., through the cavity into a reservoir or drain fluidly coupled to the cavity, the absorbent material 340 can trap all, substantially all, most, some, or a portion of the extracted electrolyte to prevent at least a portion of it from being transferred back into the cavity and / or reabsorption into the semi-solid electrode material 330 b. In some embodiments, the absorbent material 340 may be positioned near the base, the roller or rollers, and / or the edge of the intermediate electrode such that any portion of the electrolyte removed from the semi-solid electrode material 330a through the edge of the intermediate electrode can be captured, substantially captured, or at least partially captured by the absorbent material 340.In some embodiments, the absorbent material 340 may be inserted between a roller or base and the semi-permeable membrane. In some embodiments, the absorbent material 340 may be inserted between the porous current collector 310 and the base or roller. In some embodiments, the absorbent material 340 may be positioned in more than one of the configurations described herein, for example, between the base and the current collector 310, between a roller or rollers and a semi-permeable membrane positioned on the exposed surface of the semi-solid electrode material 330a, and near the edge of the intermediate electrode, so that all or substantially all of the removed excess electrolyte can be captured by the absorbent material 340.

[0088]

[0092] The method 30 further includes removing the rollers or the pressed electrode from the roller assembly and removing the absorbent material 340, the semi-permeable membrane, and / or any remaining stencil material (e.g., the first inner frame 320a) to form a finished semi-solid electrode having a higher active solids loading. In some embodiments, removing a portion of the electrolyte from the intermediate electrode forms a finished electrode having a higher active solids loading than the aforementioned semi-solid electrode material and electrode constructed therefrom. Without wishing to be bound by any particular theory, removing a portion of the electrolyte (e.g., an excess portion of the liquid electrolyte) can reduce the volume of the semi-solid electrode material on the current collector by removing the electrolyte and by compressing and removing voids and porosity without a corresponding reduction in conductivity across the semi-solid electrode material. In some embodiments, the reduction in porosity can include a reduction in porosity from about 20% to about 50% to about 5% to about 30%, including all values ​​and ranges therebetween.

[0089]

[0093] In some embodiments, the first composition of the semi-solid electrode material 330a can include about 20% to about 80% by volume of active material. In some embodiments, the first composition of the semi-solid electrode material 330a can include about 40% to about 80% by volume, or about 50% to about 80% by volume of active material. In some embodiments, the first composition of the semi-solid electrode material 330a can include at least about 20%, at least about 25%, at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%, at least about 65%, at least about 70%, or at least about 75% by volume of active material. In some embodiments, the first composition of the semi-solid electrode material 330a can include about 80% or less, about 75% or less, about 70% or less, about 65% or less, about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, about 35% or less, about 30% or less, or about 25% or less by volume of active material. Combinations of the above volume percentages of active material in the first composition of the semi-solid electrode material 330a are also possible (e.g., at least about 20% by volume and about 80% or less by volume, or at least about 30% by volume and about 60% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the first composition of the semi-solid electrode material 330a can include about 20%, about 25%, about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, about 60%, about 65%, about 70%, about 75%, or about 80% active material by volume.

[0090]

[0094] In some embodiments, the first composition of the semi-solid electrode material 330a can include between about 0.5% and about 25% by volume of conductive material. In some embodiments, the first composition of the semi-solid electrode material 330a can include between about 1.0% and about 6% by volume of conductive material. In some embodiments, the first composition of the semi-solid electrode material 330a can include at least about 0.5%, at least about 1%, at least about 1.5%, at least about 2%, at least about 2.5%, at least about 3%, at least about 3.5%, at least about 4%, at least about 4.5%, at least about 5%, at least about 5.5%, at least about 6%, at least about 6.5%, at least about 7%, at least about 7.5%, at least about 8%, at least about 8.5%, at least about 9%, at least about 9.5%, at least about 10%, at least about 15%, or at least about 20% by volume of conductive material. In some embodiments, the first composition of the semi-solid electrode material 330a can include about 25% or less, about 20% or less, about 15% or less, about 10% or less, about 9.5% or less, about 9% or less, about 8.5% or less, about 8% or less, about 7.5% or less, about 7% or less, about 6.5% or less, about 6% or less, about 5.5% or less, about 5% or less, about 4.5% or less, about 4% or less, about 3.5% or less, about 3% or less, about 2.5% or less, about 2% or less, about 1.5% or less, or about 1% or less by volume of conductive material. Combinations of the above volume percentages of conductive material in the first composition of the semi-solid electrode material 330a are also possible (e.g., at least about 0.5% by volume and about 25% or less by volume, or at least about 3% by volume and about 10% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the first composition of the semi-solid electrode material 330a can include about 0.5%, about 1%, about 1.5%, about 2%, about 2.5%, about 3%, about 3.5%, about 4%, about 4.5%, about 5%, about 5.5%, about 6%, about 6.5%, about 7%, about 7.5%, about 8%, about 8.5%, about 9%, about 9.5%, about 10%, about 15%, about 20%, or about 25% conductive material by volume.

[0091]

[0095] In some embodiments, the first composition of the semi-solid electrode material 330a can include about 25% to about 70% electrolyte by volume. In some embodiments, the first composition of the semi-solid electrode material 330a can include about 30% to about 50%, or about 20% to about 40% electrolyte by volume. In some embodiments, the first composition of the semi-solid electrode material 330a can include at least about 25%, at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%, or at least about 65% electrolyte by volume. In some embodiments, the first composition of the semi-solid electrode material 330a can be about 70% or less, about 65% or less, about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, about 35% or less, or about 30% or less electrolyte by volume. Combinations of the above volume percentages of electrolyte in the first composition of the semi-solid electrode material 330a are also possible (e.g., at least about 25% and not more than about 70%, or at least about 30% and not more than about 50%), including all values ​​and ranges therebetween. In some embodiments, the first composition of the semi-solid electrode material 330a can include about 25%, about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, about 60%, about 65%, or about 70% electrolyte by volume.

[0092]

[0096] In some embodiments, the second composition of the semi-solid electrode material 330b can include about 30% to about 85% by volume of active material. In some embodiments, the second composition of the semi-solid electrode material 330b can include about 50% to about 85% by volume, or about 60% to about 85% by volume of active material. In some embodiments, the second composition of the semi-solid electrode material 330b can include at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%, at least about 65%, at least about 70%, at least about 75%, or at least about 80% by volume of active material. In some embodiments, the second composition of the semi-solid electrode material 330b can include about 85% or less, about 80% or less, about 75% or less, about 70% or less, about 65% or less, about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, or about 35% or less by volume of active material. Combinations of the above volume percentages of active material in the second composition of the semi-solid electrode material 330b are also possible (e.g., at least about 30% by volume and about 85% or less by volume, or at least about 40% by volume and about 70% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the second composition of the semi-solid electrode material 330b can include about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, about 60%, about 65%, about 70%, about 75%, about 80%, or about 85% active material by volume.

[0093]

[0097] In some embodiments, the second composition of the semi-solid electrode material 330b can include between about 0.5% and about 30% by volume of the conductive material. In some embodiments, the second composition of the semi-solid electrode material 330b can include between about 1.0% and about 6% by volume of the conductive material. In some embodiments, the second composition of the semi-solid electrode material 330b can include at least about 0.5%, at least about 1%, at least about 1.5%, at least about 2%, at least about 2.5%, at least about 3%, at least about 3.5%, at least about 4%, at least about 4.5%, at least about 5%, at least about 5.5%, at least about 6%, at least about 6.5%, at least about 7%, at least about 7.5%, at least about 8%, at least about 8.5%, at least about 9%, at least about 9.5%, at least about 10%, at least about 15%, at least about 20%, or at least about 25% by volume of the conductive material. In some embodiments, the second composition of the semi-solid electrode material 330b can include about 30% or less, about 25% or less, about 20% or less, about 15% or less, about 10% or less, about 9.5% or less, about 9% or less, about 8.5% or less, about 8% or less, about 7.5% or less, about 7% or less, about 6.5% or less, about 6% or less, about 5.5% or less, about 5% or less, about 4.5% or less, about 4% or less, about 3.5% or less, about 3% or less, about 2.5% or less, about 2% or less, about 1.5% or less, or about 1% or less by volume of conductive material. Combinations of the above volume percentages of conductive material in the second composition of the semi-solid electrode material 330b are also possible (e.g., at least about 0.5% by volume and about 30% or less by volume, or at least about 5% by volume and about 10% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the second composition of the semi-solid electrode material 330b can include about 0.5%, about 1%, about 1.5%, about 2%, about 2.5%, about 3%, about 3.5%, about 4%, about 4.5%, about 5%, about 5.5%, about 6%, about 6.5%, about 7%, about 7.5%, about 8%, about 8.5%, about 9%, about 9.5%, about 10%, about 15%, about 20%, about 25%, or about 30% conductive material by volume.

[0094]

[0098] In some embodiments, the second composition of the semi-solid electrode material 330b can include about 15% to about 60% electrolyte by volume. In some embodiments, the second composition of the semi-solid electrode material 330b can include about 20% to about 40% or about 10% to about 30% electrolyte by volume. In some embodiments, the second composition of the semi-solid electrode material 330b can include at least about 15%, at least about 20%, at least about 25%, at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, or at least about 55% electrolyte by volume. In some embodiments, the second composition of the semi-solid electrode material 330b can be about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, about 35% or less, about 30% or less, about 25% or less, or about 20% or less electrolyte by volume. Combinations of the above volume percentages of electrolyte in the second composition of the semi-solid electrode material 330b are also possible (e.g., at least about 15% and not more than about 60%, or at least about 20% and not more than about 40%), including all values ​​and ranges therebetween. In some embodiments, the second composition of the semi-solid electrode material 330b can include about 15%, about 20%, about 25%, about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, or about 60% electrolyte by volume.

[0095]

[0099] In some embodiments, the second composition of semi-solid electrode material 330b can have a lower ratio of electrolyte to active material than the first composition of semi-solid electrode material 330a. In some embodiments, the second composition of semi-solid electrode material 330b can have a ratio of electrolyte to active material of about 5:1 to about 1:3, about 4:1 to about 1:2, about 3:1 to about 1:1, about 5:1 to about 1:2, about 5:1 to about 1:1, about 5:1 to about 2:1, about 5:1 to about 3:1, about 5:1 to about 4:1, about 4:1 to about 1:3, about 3:1 to about 1:3, about 2:1 to about 1:3, about 1:1 to about 1:3, or about 1:2 to about 1:3 (including all values ​​and ranges therebetween).

[0096]

[0100] In some embodiments, the weight and / or thickness of the semi-solid electrode can be measured at various points throughout the process of mechanically pressing the intermediate electrode to form the finished electrode. For example, in some embodiments, the weight of the finished electrode can be a second weight and compared to the first weight to determine the mass of electrolyte removed during mechanical pressing. In some embodiments, the thickness of the finished electrode can be a second thickness and compared to the first thickness to determine the volume of electrolyte removed during mechanical pressing. In some embodiments, if the difference between the first and second weights or the difference between the first and second thicknesses of the semi-solid electrode material 330b is not sufficient, the absorbent material 340 and / or semi-permeable membrane can be placed again on the semi-solid electrode, and the intermediate electrode can be further mechanically compressed to remove a second portion of the electrolyte from the semi-solid electrode material 330b. In some embodiments, the volume or mass of the electrolyte removed during mechanical pressing can be used to determine the relative volume or mass percentage of the active material, conductive material, and electrolyte in the semi-solid electrode material 330b.

[0097]

[0101] In some embodiments, once the composition of the semi-solid electrode material 330b matches or substantially matches the desired composition of the semi-solid electrode material 330b in the finished electrode, the electrode can be removed from the mechanical press. In some embodiments, the electrode can be weighed before being mechanically pressed, then mechanically pressed for a first period of time to remove a first portion of the electrolyte, and then weighed again, with the difference between the first and second weights being usable to determine the mass of the removed electrolyte. If the mass of the removed electrolyte sufficiently matches the desired volume or mass of electrolyte to be removed, the electrode can be considered a finished electrode and is ready for further processing or incorporation into an electrochemical cell (not shown). If the mass of the removed electrolyte does not sufficiently match the desired volume or mass of electrolyte to be removed, the electrode may be mechanically pressed for a second period of time to remove a second portion of the electrolyte, and then weighed a third time; the difference between the second and third weights can be used to determine the mass of electrolyte removed during the second period of time. When the mass of electrolyte removed during the first period of time plus the mass of electrolyte removed during the second period of time equals or substantially equals the desired mass of electrolyte to be removed from the semi-solid electrode material, the electrode may be considered a finished electrode. Mechanical compression of the intermediate electrode may continue in this iterative manner until the total volume or mass of removed electrolyte equals or substantially equals the desired volume or mass of electrolyte to be removed.

[0098]

[0102] In some embodiments, the completed electrode may include an electrode tab electrically connected to the current collector and configured to transport electrons into or out of the electrode. In some embodiments, the electrode tab may extend beyond the current collector and / or insulating material. In some embodiments, the electrode tab may be electrically coupled to the current collector before the semi-solid electrode material is disposed on the current collector. In some embodiments, the cell may include integrated electrical tabs, which may eliminate the need for (i) separate tab components (e.g., electrical leads), (ii) connecting a dedicated tab to the current collector, and (iii) a dedicated tab sealing operation. Instead, in some embodiments, the electrical tab or lead may be provided as an extension of the current collector that is integral with the current collector. In some embodiments, the tab or lead may be defined by removing material from a larger area of ​​the current collector material, thereby defining the current collector and the tab or lead.

[0099]

[0103] Method 30 optionally includes forming a completed electrochemical cell by joining the completed electrode (e.g., cathode) with a second completed electrode (e.g., anode) with a separator interposed therebetween. That is, once the completed electrode is singulated and excess electrolyte is removed, the completed electrode can be assembled into an electrochemical cell with a second completed electrode exhibiting the opposite redox reaction. That is, the cathode and anode can be joined together with a separator disposed therebetween.

[0100]

[0104] In some embodiments, a separator may be disposed between the anode and the cathode. In some embodiments, the separator may be bonded to at least one of the anode and the cathode using an adhesive. In some embodiments, one anode, one cathode, and one separator may be stacked together to form a unit cell assembly. Each unit cell assembly may also include conductive tabs (also called wires) for coupling the electrodes to an external circuit. Multiple unit cell assemblies are then stacked or arranged together to form a battery cell. In some embodiments, the number of unit cell assemblies in a battery cell may vary depending, for example, on the desired capacity and / or thickness of the resulting battery cell. These stacked unit cell assemblies are electrically connected in parallel, and the respective tabs of each unit cell assembly are typically welded together by a welding process such as resistance welding, laser welding, ultrasonic welding, seam welding, or electric beam welding, among others.

[0101]

[0105] In some embodiments, the prepared electrochemical cell may be vacuum-sealed in a prismatic pouch, which can provide airtight isolation of the electrochemical cell materials from the environment. The pouch can thus help prevent leakage of harmful substances, such as electrolyte solvents and / or corrosive salts, into the surrounding environment and prevent ingress of water and / or oxygen into the cell. Other functions of the pouch may include, for example, compressive packaging of the inner layers, voltage isolation for safety and handling, and mechanical protection of the electrochemical cell assembly. In some embodiments, electrolyte may be injected into the stacked unit cell assembly during vacuum pouch sealing, and the unit cell assembly and electrolyte may then be sealed within the pouch. In some embodiments, electrolyte is not added during the pouch sealing step if the semi-solid electrode material may already contain the desired total amount of electrolyte.

[0102]

[0106] In some embodiments, the sealed battery cell may then undergo a formation process, during which an initial charging operation may be performed to create a stable SEI layer that can passivate the electrode-electrolyte interface and prevent side reactions. In some embodiments, several charge and discharge cycles may be performed to ensure that the battery's capacity meets required specifications. In some embodiments, a degassing step may be performed to release gases introduced or generated during the initial charging stage or during the electrochemical reactions of the battery formation step. The presence of trapped gases in the electrode generally reduces the electrode's conductivity and density, limits the amount of active electrochemical material that can be installed in the battery cell, and can cause dendrite growth in lithium batteries, which can impair battery performance. In some embodiments, dendrite formation can cause reduced cycle life and overall safety performance. In some embodiments, a resealing step may be performed to reseal the battery cell after the release of trapped gases.

[0103]

[0107] 4A-4E illustrate a method 40 for forming a semi-solid electrode material having a higher active material concentration and a higher energy density without requiring an electrolyte injection step and / or a drying step. The method 40 includes, at 41, loading a semi-solid electrode material 430a having a first composition into a press 435. In some embodiments, the press 435 may include a base 436 and a frame 438, where the base 436 and the frame 438 form a cavity 439. In some embodiments, the base 436 may include a watertight seal around its edge such that the semi-solid electrode material 430a does not substantially leak through the interface between the base 436 and the frame 438. In some embodiments, the semi-solid electrode material 430a may have the same or substantially similar properties as the semi-solid electrode material 330a as described above with reference to FIGS. 3A-3E.

[0104]

[0108] In some embodiments, a semi-permeable membrane (not shown) may be disposed on or near the semi-solid electrode material such that during mechanical compression of the intermediate electrode, the semi-permeable membrane does not allow transmission of active substances, conductive materials, or the like, out of the semi-solid electrode material, but does allow transmission of electrolyte out of the semi-solid electrode material. In some embodiments, the semi-permeable membrane may be a sheet or other planar structure configured to be removed from on or near the semi-solid electrode material before or after removal of the intermediate electrode from the mechanical press and before incorporating the mechanically compressed electrode into an electrochemical cell or the like. In some embodiments, the semi-permeable membrane may be a conventional separator material configured to allow at least some flow of liquid electrolyte therethrough. In some embodiments, the semi-permeable membrane may be any material that is completely or substantially chemically inert with respect to the composition of the semi-solid electrode material 430a and / or current collector 410, while allowing at least some flow of liquid electrolyte therethrough. In some embodiments, the semi-permeable membrane may remain on or near the semi-solid electrode material throughout mechanical compression and construction of the electrochemical cell, such that the semi-permeable membrane is included in the finished electrochemical cell.

[0105]

[0109] At 42, semi-solid electrode material 430a is uniformly disposed throughout cavity 439 of press 435 so as to be flush or nearly flush with the top of frame 438. Absorbent material 440 is then placed over the top of frame 438. In some embodiments, absorbent material 440 may be the same as or substantially similar to absorbent material 340 as described above with reference to Figures 3A-3E.

[0106]

[0110] At 43, a force F is applied to the bottom surface of the base 436 to shrink the cavity 439 and extract a portion of the electrolyte from the semi-solid electrode material 430a and into the absorbent material 440. At 44, mechanical compression of the semi-solid electrode material 430a removes a portion of the electrolyte, allowing the semi-solid electrode material 430a to become a semi-solid electrode wafer 430b having a second composition. The semi-solid electrode wafer 430b has a higher active material to electrolyte ratio than the semi-solid electrode material 430a. In some embodiments, the cavity 439 may be fluidly coupled to a drain (not shown) so that removed electrolyte transferred into or through the cavity can be removed from the mechanical press via the drain. In some embodiments, the cavity may be fluidly coupled to a reservoir (not shown) so that removed electrolyte transferred into or through the cavity can be removed from the mechanical press via the reservoir. In some embodiments, the removed electrolyte held in the reservoir may be reusable and / or recyclable for use in other semi-solid electrodes or elsewhere.

[0107]

[0111] At 45, the semi-solid electrode wafer 430b is removed from the press 435, where it may be used to construct an electrochemical cell or may be further processed. Removal of the semi-solid electrode wafer 430b from the press 435 may also include removing any absorbent material in contact with the semi-solid electrode wafer 430b. The semi-solid electrode wafer 430b is a versatile, free-standing material that can be applied to a variety of different applications. In some embodiments, the semi-solid electrode wafer 430b may have compositional characteristics that are the same as or substantially similar to those of the semi-solid electrode material 330b described above with reference to FIGS. 3A-3E. In some embodiments, the method 40 may include the use of a roller to densify the semi-solid electrode material 430a, as described above with reference to FIGS. 3A-3E.

[0108]

[0112] In some embodiments, the first composition of the semi-solid electrode material 430a can include between about 20% and about 80% active material by volume. In some embodiments, the first composition of the semi-solid electrode material 430a can include between about 40% and about 80% active material by volume, or between about 50% and about 80% active material by volume. In some embodiments, the first composition of the semi-solid electrode material 430a can include at least about 20%, at least about 25%, at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%, at least about 65%, at least about 70%, or at least about 75% active material by volume. In some embodiments, the first composition of the semi-solid electrode material 430a can include about 80% or less, about 75% or less, about 70% or less, about 65% or less, about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, about 35% or less, about 30% or less, or about 25% or less by volume of active material. Combinations of the above volume percentages of active material in the first composition of the semi-solid electrode material 430a are also possible (e.g., at least about 20% by volume and about 80% or less by volume, or at least about 30% by volume and about 60% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the first composition of the semi-solid electrode material 430a can include about 20%, about 25%, about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, about 60%, about 65%, about 70%, about 75%, or about 80% active material by volume.

[0109]

[0113] In some embodiments, the first composition of the semi-solid electrode material 430a can include between about 0.5% and about 25% by volume of conductive material. In some embodiments, the first composition of the semi-solid electrode material 430a can include between about 1.0% and about 6% by volume of conductive material. In some embodiments, the first composition of the semi-solid electrode material 430a can include at least about 0.5%, at least about 1%, at least about 1.5%, at least about 2%, at least about 2.5%, at least about 3%, at least about 3.5%, at least about 4%, at least about 4.5%, at least about 5%, at least about 5.5%, at least about 6%, at least about 6.5%, at least about 7%, at least about 7.5%, at least about 8%, at least about 8.5%, at least about 9%, at least about 9.5%, at least about 10%, at least about 15%, or at least about 20% by volume of conductive material. In some embodiments, the first composition of the semi-solid electrode material 430a can include about 25% or less, about 20% or less, about 15% or less, about 10% or less, about 9.5% or less, about 9% or less, about 8.5% or less, about 8% or less, about 7.5% or less, about 7% or less, about 6.5% or less, about 6% or less, about 5.5% or less, about 5% or less, about 4.5% or less, about 4% or less, about 3.5% or less, about 3% or less, about 2.5% or less, about 2% or less, about 1.5% or less, or about 1% or less by volume of conductive material. Combinations of the above volume percentages of conductive material in the first composition of the semi-solid electrode material 430a are also possible (e.g., at least about 0.5% by volume and about 25% or less by volume, or at least about 3% by volume and about 10% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the first composition of the semi-solid electrode material 430a can include about 0.5%, about 1%, about 1.5%, about 2%, about 2.5%, about 3%, about 3.5%, about 4%, about 4.5%, about 5%, about 5.5%, about 6%, about 6.5%, about 7%, about 7.5%, about 8%, about 8.5%, about 9%, about 9.5%, about 10%, about 15%, about 20%, or about 25% conductive material by volume.

[0110]

[0114] In some embodiments, the first composition of semi-solid electrode material 430a can include about 25% to about 70% electrolyte by volume. In some embodiments, the first composition of semi-solid electrode material 430a can include about 30% to about 50%, or about 20% to about 40% electrolyte by volume. In some embodiments, the second composition of semi-solid electrode material 430b can include at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%, at least about 65%, at least about 70%, at least about 75%, or at least about 80% active material by volume. In some embodiments, the second composition of the semi-solid electrode material 430b can include about 85% or less, about 80% or less, about 75% or less, about 70% or less, about 65% or less, about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, or about 35% or less by volume of active material. Combinations of the above volume percentages of active material in the second composition of the semi-solid electrode material 430b are also possible (e.g., at least about 30% by volume and about 85% or less by volume, or at least about 40% by volume and about 70% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the second composition of the semi-solid electrode material 430b can include about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, about 60%, about 65%, about 70%, about 75%, about 80%, or about 85% active material by volume.

[0111]

[0115] In some embodiments, the second composition of the semi-solid electrode wafer 430b can include about 30% to about 85% by volume of active material. In some embodiments, the second composition of the semi-solid electrode wafer 430b can include about 50% to about 85% by volume, or 60% to about 85% by volume of active material. In some embodiments, the second composition of the semi-solid electrode wafer 430b can include at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%, at least about 65%, at least about 70%, at least about 75%, or at least about 80% by volume of active material. In some embodiments, the second composition of the semi-solid electrode material 430b can include about 85% or less, about 80% or less, about 75% or less, about 70% or less, about 65% or less, about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, or about 35% or less by volume of active material. Combinations of the above volume percentages of active material in the second composition of the semi-solid electrode material 430b are also possible (e.g., at least about 30% by volume and about 85% or less by volume, or at least about 40% by volume and about 70% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the second composition of the semi-solid electrode material 430b can include about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, about 60%, about 65%, about 70%, about 75%, about 80%, or about 85% active material by volume.

[0112]

[0116] In some embodiments, the second composition of the semi-solid electrode wafer 430b can include between about 0.5% and about 30% conductive material by volume. In some embodiments, the second composition of the semi-solid electrode wafer 430b can include between about 1.0% and about 6% conductive material by volume. In some embodiments, the second composition of the semi-solid electrode material 430b can include at least about 0.5%, at least about 1%, at least about 1.5%, at least about 2%, at least about 2.5%, at least about 3%, at least about 3.5%, at least about 4%, at least about 4.5%, at least about 5%, at least about 5.5%, at least about 6%, at least about 6.5%, at least about 7%, at least about 7.5%, at least about 8%, at least about 8.5%, at least about 9%, at least about 9.5%, at least about 10%, at least about 15%, at least about 20%, or at least about 25% conductive material by volume. In some embodiments, the second composition of the semi-solid electrode material 430b can include about 30% or less, about 25% or less, about 20% or less, about 15% or less, about 10% or less, about 9.5% or less, about 9% or less, about 8.5% or less, about 8% or less, about 7.5% or less, about 7% or less, about 6.5% or less, about 6% or less, about 5.5% or less, about 5% or less, about 4.5% or less, about 4% or less, about 3.5% or less, about 3% or less, about 2.5% or less, about 2% or less, about 1.5% or less, or about 1% or less by volume of conductive material. Combinations of the above volume percentages of conductive material in the second composition of the semi-solid electrode material 430b are also possible (e.g., at least about 0.5% by volume and about 30% or less by volume, or at least about 5% by volume and about 10% or less by volume), including all values ​​and ranges therebetween. In some embodiments, the second composition of the semi-solid electrode material 430b can include about 0.5%, about 1%, about 1.5%, about 2%, about 2.5%, about 3%, about 3.5%, about 4%, about 4.5%, about 5%, about 5.5%, about 6%, about 6.5%, about 7%, about 7.5%, about 8%, about 8.5%, about 9%, about 9.5%, about 10%, about 15%, about 20%, about 25%, or about 30% conductive material by volume.

[0113]

[0117] In some embodiments, the second composition of the semi-solid electrode wafer 430b can include about 15% to about 60% electrolyte by volume. In some embodiments, the second composition of the semi-solid electrode wafer 430b can include about 20% to about 40% or about 10% to about 30% electrolyte by volume. In some embodiments, the second composition of the semi-solid electrode material 430b can include at least about 15%, at least about 20%, at least about 25%, at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, or at least about 55% electrolyte by volume. In some embodiments, the second composition of the semi-solid electrode material 430b can be about 60% or less, about 55% or less, about 50% or less, about 45% or less, about 40% or less, about 35% or less, about 30% or less, about 25% or less, or about 20% or less electrolyte by volume. Combinations of the above volume percentages of electrolyte in the second composition of semi-solid electrode material 430b are also possible (e.g., at least about 15% and not more than about 60%, or at least about 20% and not more than about 40% (including all values ​​and ranges therebetween). In some embodiments, the second composition of semi-solid electrode material 430b can include about 15%, about 20%, about 25%, about 30%, about 35%, about 40%, about 45%, about 50%, about 55%, or about 60% electrolyte by volume.

[0114]

[0118] In some embodiments, the second composition of the semi-solid electrode material 330b can have a lower ratio of electrolyte to active material than the first composition of the semi-solid electrode material 430a. In some embodiments, the second composition of the semi-solid electrode wafer 430b can have a ratio of electrolyte to active material of about 5:1 to about 1:3, about 4:1 to about 1:2, about 3:1 to about 1:1, about 5:1 to about 1:2, about 5:1 to about 1:1, about 5:1 to about 2:1, about 5:1 to about 3:1, about 5:1 to about 4:1, about 4:1 to about 1:3, about 3:1 to about 1:3, about 2:1 to about 1:3, about 1:1 to about 1:3, or about 1:2 to about 1:3 (including all values ​​and ranges therebetween).

[0115]

[0119] 4F is a top view of semi-solid electrode wafer 430b. As shown, semi-solid electrode wafer 430b has a rectangular shape when viewed from above. In some embodiments, semi-solid electrode wafer 430b may have a circular, L-shaped, square, or any other shape suitable for incorporation into an electrochemical cell when viewed from above. Thus, in some embodiments, cavity 439 may have a rectangular, circular, L-shaped, square, or any other shape suitable for fabricating an electrode when viewed from above.

[0116]

[0120] In some embodiments, the weight and / or thickness of the semi-solid electrode can be measured at various points throughout the process of mechanically pressing the intermediate electrode to form the finished electrode. For example, in some embodiments, the weight of the finished electrode can be a second weight and compared to the first weight to determine the mass of electrolyte removed during mechanical pressing. In some embodiments, the thickness of the finished electrode can be a second thickness and compared to the first thickness to determine the volume of electrolyte removed during mechanical pressing. In some embodiments, if the difference between the first and second weights or the difference between the first and second thicknesses of the semi-solid electrode wafer 430b is not sufficient, the absorbent material 440 and / or semi-permeable membrane can be placed again on the semi-solid electrode, and the intermediate electrode can be further mechanically compressed to remove a second portion of the electrolyte from the semi-solid electrode wafer 430b. In some embodiments, the volume or mass of the electrolyte removed during mechanical pressing can be used to determine the relative volume or mass percentage of the active material, conductive material, and electrolyte in the semi-solid electrode wafer 430b.

[0117]

[0121] In some embodiments, once the composition of the semi-solid electrode wafer 430b matches or substantially matches the desired composition of the semi-solid electrode wafer 430b of the finished electrode, the electrode can be removed from the mechanical press. In some embodiments, the electrode can be weighed before being mechanically pressed, then mechanically pressed for a first period of time to remove a first portion of the electrolyte, and then weighed again, with the difference between the first and second weights being usable to determine the mass of the removed electrolyte. If the mass of the removed electrolyte sufficiently matches the desired volume or mass of electrolyte to be removed, the electrode can be considered a finished electrode and is ready for further processing or incorporation into an electrochemical cell (not shown). If the mass of the removed electrolyte does not sufficiently match the desired volume or mass of electrolyte to be removed, the electrode may be mechanically pressed for a second period of time to remove a second portion of the electrolyte, and then weighed a third time; the difference between the second and third weights can be used to determine the mass of electrolyte removed during the second period of time. When the mass of electrolyte removed during the first period of time plus the mass of electrolyte removed during the second period of time equals or substantially equals the desired mass of electrolyte to be removed from the semi-solid electrode material, the electrode may be considered a finished electrode. Mechanical compression of the intermediate electrode may continue in this iterative manner until the total volume or mass of removed electrolyte equals or substantially equals the desired volume or mass of electrolyte to be removed.

[0118]

[0122] 5A and 5B illustrate a method 50 of further use of the aforementioned semi-solid electrode wafer 430b, according to an embodiment. In some embodiments, the semi-solid electrode wafer 430b can be used to form an electrochemical cell, which includes a second electrode 470, a current collector 472, and a separator 474. As shown at 51, the second electrode 470 is disposed on the current collector 472, and the separator 474 is disposed on the second electrode 470. In some embodiments, an electrolyte droplet 476 may be disposed on the separator 474 to wet the surface of the separator 474. At 52, the semi-solid electrode wafer 430b is disposed on the separator 474. Wetting the surface of the separator 474 can prevent voids along the interface between the semi-solid electrode wafer 430b and the separator 474. The voids are filled by the electrolyte droplets 476, and there is substantially no area at the interface between the semi-solid electrode wafer 430b and the separator 474 to block ion migration.

[0119]

[0123] In some embodiments, the semi-solid electrode wafer 430b can be easily transported. In some embodiments, multiple semi-solid electrode wafers 430b can be stacked together. In some embodiments, semi-solid electrode wafers 430b can be stacked on top of other electrodes. In some embodiments, multiple semi-solid electrode wafers 430b having different cell chemistries can be stacked together. That is, a first semi-solid electrode wafer can have a first cell chemistry and a second semi-solid electrode wafer can have a second cell chemistry, where the second cell chemistry is different from the first cell chemistry. In some embodiments, additional semi-solid electrode wafers can have additional chemistries. In some embodiments, the semi-solid electrode wafer 430b can be included in a bi-cell or electrochemical cell system having multiple battery chemistries.

[0120]

[0124] Various concepts may be embodied as one or more methods, at least one example of which is provided. Actions performed as part of a method may be ordered in any suitable manner. Thus, embodiments may be constructed in which actions are performed in an order different from that illustrated, and these embodiments may include performing some actions simultaneously even though they are shown as sequential actions in the illustrative embodiments. In other words, it is understood that such features are not necessarily limited to a particular order of execution, but rather may be any number of threads, processes, services, servers, and / or the like that may execute sequentially, asynchronously, simultaneously, in parallel, simultaneously, synchronously, and / or the like in a manner consistent with this disclosure. Thus, some of these features may be mutually inconsistent in that they cannot coexist in a single embodiment. Similarly, some features may be applicable to one aspect of the innovation but not to other aspects.

[0121]

[0125] Additionally, the present disclosure may include other innovations not currently described. Applicant reserves all rights in such innovations, including the right to embody such innovations and to file additional applications, continuations, continuations-in-part, divisional applications, and / or the like. Accordingly, it is to be understood that the advantages, embodiments, examples, functional aspects, features, logical aspects, operational aspects, organizational aspects, structural aspects, topological aspects, and / or other aspects of the present disclosure are not to be construed as limitations on the present disclosure as defined by the embodiments, or limitations on equivalents of the embodiments. Various embodiments of the technology disclosed herein may be implemented in a manner that allows for great flexibility and customization as described herein, depending on the particular needs and / or characteristics of individual and / or business users, database configurations and / or relational models, data types, data transmission and / or network frameworks, syntax structures, and / or the like.

[0122]

[0126] All definitions, as defined and used herein, shall be understood to take precedence over dictionary definitions, definitions in documents incorporated by reference, and / or ordinary meanings of the defined terms.

[0123]

[0127] As used herein, in certain embodiments, the term "about" or "approximately" preceding a numerical value refers to a range of plus or minus 10% of that value. When a range of values ​​is provided, it is understood that each intervening value between the upper and lower limit of that range (to one-tenth of the unit of the lower limit unless the context clearly dictates otherwise), and any other stated or intervening value within that stated range, is encompassed within the disclosure. It is also encompassed within the disclosure that the upper and lower limits of these smaller ranges may independently be included within the smaller ranges, subject to any specifically excluded limit in the stated range. When a stated range includes one or both of the limits, ranges excluding either or both of those included limits are also included within the disclosure.

[0124]

[0128] The indefinite articles "a" and "an" shall be understood in this specification and embodiments to mean "at least one" unless expressly indicated otherwise.

[0125]

[0129] The term "and / or" shall be understood in this specification and in embodiments to mean "one or both" of the elements so conjuncted, i.e., elements that are conjunctive in some instances and disjunctive in other instances. Multiple elements listed with "and / or" shall be construed in the same manner, i.e., "one or more" of the elements so conjuncted. Other elements, other than the elements specifically identified by the "and / or" clause, may optionally be present, whether related or unrelated to those specifically identified elements. Thus, as a non-limiting example, a reference to "A and / or B," when used in conjunction with open-ended language such as "comprising," may refer in one embodiment to A only (optionally including elements other than B), in another embodiment to B only (optionally including elements other than A), in yet another embodiment to both A and B (optionally including other elements), etc.

[0126]

[0130] In the present specification and embodiments, "or" shall be understood to have the same meaning as "and / or" as defined above. For example, when separating items in a list, "or" or "and / or" shall be construed as being inclusive, i.e., the inclusion of at least one, but also including two or more of several elements or a list of elements, and optionally additional unlisted items. Only terms expressly indicated otherwise, such as "only one of" or "exactly one of," or, when used in the embodiments, "consisting of," shall imply the inclusion of exactly one element of several elements or a list of elements. In general, the term "or" shall be construed herein to indicate exclusive alternatives (i.e., "either / or," "one of," "only one of," or "exactly one of,") only when preceded by terms of exclusivity, such as "either / or," "one of," "only one of," or "exactly one of." When used in the embodiments, "consisting essentially of" shall have its ordinary meaning as used in the field of patent law.

[0127]

[0131] In this specification and embodiments, the phrase "at least one," in reference to a list of one or more elements, shall be understood to mean at least one element selected from any one or more of the elements in the list of elements, but not necessarily including at least one of each and every element specifically listed in the list of elements, and not excluding any combination of elements in the list of elements. This definition also allows that elements other than those specifically identified in the list of elements to which the phrase "at least one" refers may optionally be present, whether related or unrelated 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") can mean, in one embodiment, at least one A (and optionally including elements other than B), optionally including more than one, in the absence of B; in another embodiment, at least one B (and optionally including elements other than A), optionally including more than one, in the absence of A; in yet another embodiment, at least one A, optionally including more than one, and at least one B (and optionally including other elements), optionally including more than one, etc.

[0128]

[0132] In the above embodiments and specification, all transitional phrases such as "comprising," "including," "carrying," "having," "containing," "involving," "holding," "composed of," and the like, shall be understood to be open-ended, i.e., to mean 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 set forth in Section 2111.03 of the U.S. Patent and Trademark Office Manual of Patent Examining Procedures.

[0129]

[0133] While specific embodiments of the present disclosure have been summarized above, many alternatives, modifications, and variations will be apparent to those skilled in the art. Accordingly, the embodiments described herein are intended to aid understanding rather than to be limiting. Various changes can be made without departing from the spirit and scope of the present disclosure. While the methods and steps described above show certain events occurring in a particular order, those skilled in the art, having the benefit of this disclosure, will understand that the ordering of certain steps can be changed and that such changes are in accordance with variations of the present invention. Furthermore, some of the steps, in addition to being performed sequentially as described above, may also be performed simultaneously in a parallel process, where possible. While embodiments have been specifically illustrated and described, it will be understood that various changes in form and detail can be made.

Claims

1. 1. A method for forming a densified semi-solid electrode, the method comprising: forming a semi-solid electrode material by mixing an active material and a conductive material with a liquid electrolyte; disposing the semi-solid electrode material on a current collector; disposing a semi-permeable membrane on an exposed surface of the semi-solid electrode material; compressing the semi-solid electrode material between the current collector and the semi-permeable membrane to extract a portion of the liquid electrolyte and form the densified semi-solid electrode; Including, The method, wherein the densified semi-solid electrode comprises about 60% to about 85% active material by volume.

2. The method of claim 1 , wherein the semi-permeable membrane is configured to absorb the portion of the liquid electrolyte extracted during compression.

3. 10. The method of claim 1, further comprising disposing an absorbent material on an exposed surface of the semipermeable membrane, the absorbent material configured to absorb the portion of the liquid electrolyte extracted during compression.

4. The method of claim 1 , wherein mechanically compressing the semi-solid electrode material comprises compressing the semi-solid material between a die and a base.

5. 10. The method of claim 1, wherein the compressed semi-solid electrode material comprises greater than about 70 wt% of the active material.

6. the semi-solid electrode material after mixing has a first composition in which the liquid electrolyte is about 50 wt % to about 80 wt % of the semi-solid electrode material; 10. The method of claim 1, wherein the semi-solid electrode material after compaction has a second composition in which the liquid electrolyte is about 10 wt % to about 45 wt % of the semi-solid electrode material.

7. the semi-solid electrode material after mixing has a first ratio of liquid electrolyte to active material of about 10:1 to about 1:1; 10. The method of claim 1, wherein the semi-solid electrode material after compression has a second ratio of liquid electrolyte to active material of about 5:1 to about 1:

3.

8. the semi-solid electrode material after mixing has a first active agent molarity of about 5 M to about 15 M; 10. The method of claim 1, wherein the semi-solid electrode material after compaction has a second active agent molarity of about 16M to about 24M.

9. the semi-solid electrode material after mixing has a first energy density of about 3 mAh / g to about 5 mAh / g; 10. The method of claim 1, wherein the semi-solid electrode material after compaction has a second energy density of about 6 mAh / g to about 14 mAh / g.

10. The method of claim 1 , wherein the conductive material comprises conductive particles.

11. the densified semi-solid electrode is a first electrode, the current collector is a first current collector; removing the semi-permeable membrane from the first electrode; placing a second electrode on the second current collector; placing the separator over the second electrode such that a first surface of the separator contacts the second electrode and a second surface of the separator is exposed, the second surface being opposite the first surface; disposing a droplet of electrolyte on the second surface of the separator; forming an electrochemical cell by disposing the first electrode on the separator; The method of claim 1 further comprising:

12. forming a semi-solid electrode material having a first volume by mixing an active material and a conductive material with a liquid electrolyte; Inserting the semi-solid electrode material between a current collector and a semi-permeable membrane; applying a compressive force to the semi-solid electrode material by a roller such that the semi-solid electrode material has a second volume that is smaller than the first volume; A method comprising:

13. 13. The method of claim 12, further comprising exposing the semi-solid electrode material to an absorbent material such that a portion of the liquid electrolyte migrates from the semi-solid electrode material to the absorbent material.

14. The method of claim 13 , wherein the absorbent material is conveyed by one or more rollers.

15. The method of claim 14 , wherein a flat portion of the absorbent material contacts the semi-solid electrode material.

16. The method of claim 12, wherein the second volume is about 50% to about 95% of the first volume.

17. 17. The method of claim 16, wherein the second volume is about 50% to about 80% of the first volume.

18. 17. The method of claim 16, wherein the second volume is about 70% to about 95% of the first volume.

19. forming a semi-solid electrode material having a first thickness by mixing an active material and a conductive material with a liquid electrolyte; Inserting the semi-solid electrode material between a current collector and a semi-permeable membrane; applying a compressive force to the semi-solid electrode material with a roller such that the semi-solid electrode material has a second thickness that is less than the first thickness; A method comprising:

20. 20. The method of claim 19, wherein the first thickness is from about 100 μm to about 2,000 μm.

21. 20. The method of claim 19, wherein the second thickness is from about 5 μm to about 50 μm.

22. 20. The method of claim 19, wherein mechanical compaction is achieved by mechanically compressing the semi-solid electrode material between a base and a die of a mechanical press.

23. mixing an active material and a conductive material with a liquid electrolyte to form a first semi-solid electrode material having a first composition comprising about 50 wt % to about 80 wt % of the liquid electrolyte; inserting the first semi-solid electrode material between a current collector and a semi-permeable membrane; mechanically compressing the first semi-solid electrode material to form a second semi-solid electrode material having a second composition comprising about 10 wt % to about 45 wt % of the liquid electrolyte; A method comprising:

24. forming a first semi-solid electrode material having a first density by mixing an active material and a conductive material with a liquid electrolyte; inserting the first semi-solid electrode material between a current collector and a semi-permeable membrane; mechanically compressing the first semi-solid electrode material to form a second semi-solid electrode material having a second density greater than the first density, the second semi-solid electrode material comprising about 60% to about 85% by volume of the active material; A method comprising:

25. The first density is about 2 g / cm ３ 25. The method of claim 24, wherein the

26. The second density is about 2.1 g / cm ３ ~ about 4 g / cm ３ 26. The method of claim 25, wherein:

27. 27. The method of claim 26, wherein the energy density of the second semi-solid electrode material is greater than about 7 mAh / g.

28. 28. The method of claim 27, wherein the energy density of the second semi-solid electrode material is greater than about 8 mAh / g.

29. 30. The method of claim 28, wherein the energy density of the second semi-solid electrode material is greater than about 9 mAh / g.

30. 30. The method of claim 29, wherein the energy density of the second semi-solid electrode material is greater than about 10 mAh / g.

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