Setter body and methods of forming the same

Abstract

In one aspect, the present invention provides a setter body for sintering a solid-state electrolyte material. The setter body comprises a substrate and a coating. The substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface. The substrate comprises nickel. The coating is at least partially disposed on the first surface of the substrate. The coating comprises at least about 1 mole percent of lithium. And, the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate. Another aspect provides a method of forming a setter body. A further aspect provides a method of forming a sintered solid-state electrolyte material.

Description

PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 SETTER BODY AND METHODS OF FORMING THE SAME CROSS REFEREENCE TO RELATED APPLICATION

[0001] This PCT application claims the benefit of U.S. provisional application no.63 / 582,272, filed Sept.13, 2023. This document is incorporated herein by reference in its entirety. FIELD OF THE INVENTION

[0002] The present invention relates to a setter body for sintering a solid-state electrolyte material, methods of forming the same, and methods of using the same. BACKGROUND

[0003] Solid-state batteries typically include one or more solid-state electrolyte materials. The solid-state electrolyte materials may function as, for example, a separator. In other examples, the solid-state electrolyte material may be formed as a bilayer comprising a porous layer and a dense layer. In such examples, the porous layer is a host matrix for receiving an active anode material (e.g., lithium) and the dense layer is a separator. However, manufacturing films comprising layers of varying porosity (e.g., a porous layer and a dense layer) presents challenges. For example, during sintering, each layer may be subject to different degrees of shrinkage, leading to part warping and curling. For this reason, setter bodies are frequently implemented to constrain solid-state electrolyte materials during sintering.

[0004] Typically, setter bodies include a substrate comprising a ceramic material (e.g., alumina, zirconia, magnesium oxide (MgO), and doped or undoped lithium lanthanum zirconium oxide (LLZO) compositions). Although such setter bodies may be used to provide favorable part flatness, there are drawbacks associated with the use of such setter bodies. Specifically, setter bodies including a substrate comprising a ceramic material exhibit limited or no reusability and may react with or cause compositional changes to at least a portion (e.g., a surface or a portion of a surface) of solid-state electrolyte materials. The use of such setter bodies may also result in unfavorable cross-diffusion. And, some setter bodies may adhere to the solid-state electrolyte material during processing.

[0005] Accordingly, there remains a need to provide improved setter bodies. 1 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 SUMMARY OF THE INVENTION

[0006] In one aspect, the present invention provides a setter body for sintering a solid-state electrolyte material. The setter body comprises a substrate and a coating. The substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface. The substrate comprises nickel. The coating is at least partially disposed on the first surface of the substrate. The coating comprises at least about 1 mole percent of lithium. And, the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate.

[0007] In some embodiments, the nickel of the substrate is elemental nickel, a nickel oxide, a nickel alloy, or any combination thereof. For example, the substrate may comprise elemental nickel. And, in some embodiments, the substrate comprises a nickel oxide.

[0008] In some embodiments, the substrate comprises a nickel alloy. For example, the nickel alloy may comprise aluminum, iron, copper, molybdenum, chromium, titanium, cobalt, tungsten, or any combination thereof.

[0009] In some embodiments, the substrate is a plate, a foam, or a mesh. For example, the substrate may be a plate. In some embodiments, the plate has a thickness of from about 1,000 µm to about 10,000 µm. And, in some embodiments, the plate has an apparent porosity of less than about 5%.

[0010] In other embodiments, the substrate is a foam. In some embodiments, the foam has a thickness of from about 1 µm to about 1,000 µm. In some embodiments, the foam has an apparent porosity of greater than about 50%. And, in some embodiments, the foam has an apparent porosity of greater than about 5%.

[0011] In other embodiments, the substrate is a mesh. In some embodiments, the mesh has a thickness of from about 1 µm to about 1,000 µm. In some embodiments, the mesh has an apparent porosity of greater than about 5%. And, in some embodiments, the mesh has an apparent porosity of greater than about 50%.

[0012] In some embodiments, the substrate has a weight-to-area ratio of from about 0.01 g / cm2to about 14.0 g / cm2. In other embodiments, the substrate has a weight-to-area ratio of from about 0.1 g / cm2to about 0.5 g / cm2. And, in some embodiments, the substrate has a weight-to- area ratio of from about 0.1 g / cm2to about 0.2 g / cm2. 2 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0013] In some embodiments, the coating has a thickness of from about 1 nm to about 100 µm. In other embodiments, the coating has a thickness of from about 1 nm to about 1 µm.

[0014] In some embodiments, the coating comprises elemental lithium, a lithium oxide, a lithium alloy, or any combination thereof. For example, the coating may comprise elemental lithium. In other embodiments, the coating comprises a lithium oxide. And, in some embodiments, the coating comprises a lithium alloy.

[0015] In some embodiments, the coating comprises at least one nodule extending away from the first surface of the substrate. In other embodiments, the at least one nodule comprises aluminum, silicon, magnesium, titanium, calcium, oxygen, or any combination thereof.

[0016] In some embodiments, the substrate comprises less than about 1 mole percent of lithium. In other embodiments, the substrate comprises less than about 0.5 mole percent of lithium. And, in some embodiments, substrate is free of lithium.

[0017] In some embodiments, the coating comprises at least about 5 mole percent of lithium. In other embodiments, the coating is at least partially disposed on at least one of the second and outer surfaces of the substrate. For example, the coating may be at least partially disposed on the second surface of the substrate. In some embodiments, the coating is at least partially disposed on the second surface of the substrate. And, in some embodiments, the coating is at least partially disposed on the second surface and the outer surface of the substrate.

[0018] In another aspect, the present invention provides a method forming a setter body comprising: (a) disposing a substrate in a heating chamber, wherein the substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, and wherein the substrate comprises nickel; (b) providing a lithium source in the heating chamber; and (c) heating the heating chamber to a temperature of from about 600 °C to about 1,500 °C to form a coating comprising lithium from the lithium source at least partially on the first surface of the substrate, thereby forming the setter body.

[0019] In some implementations, the nickel of the substrate is elemental nickel, a nickel oxide, a nickel alloy, or any combination thereof. For example, the substrate comprises elemental nickel. In other examples, substrate comprises a nickel alloy (e.g., Ni alloy comprising no greater than 3 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 20% iron). In some examples, the nickel alloy comprises aluminum, iron (e.g., at no greater than 20%), copper, molybdenum, chromium, titanium, cobalt, tungsten, or any combination thereof.

[0020] In some implementations, the substrate is a plate, a foam, or a mesh.

[0021] In some implementations, the lithium source comprises lithium lanthanum zirconium oxide (LLZO). In some of these implementations, the LLZO is doped. In alternative implementations, the LLZO is undoped.

[0022] In some implementations, the substrate comprises less than about 0.5 mole percent of lithium.

[0023] In some implementations, the substrate is free of lithium.

[0024] In some implementations, the coating comprises at least about 1 mole percent of lithium.

[0025] In some implementations, the coating comprises at least about 5 mole percent of lithium.

[0026] In some implementations, the coating is at least partially disposed on at least one of the second and outer surfaces of the substrate.

[0027] Some implementations further comprise (d) flowing a gas into the heating chamber.

[0028] In some implementations, the gas comprises a mixture of hydrogen and an inert gas. In other implementations, the gas comprises a mixture of CO and an inert gas.

[0029] In some implementations, the gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 3,000 SCCM.

[0030] In some implementations, step (d) is performed at least partially during step (c).

[0031] In some implementations, an atmosphere inside the heating chamber during step (c) comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof.

[0032] In some implementations, The method of any one of claims 30-48, wherein the method further comprises (e) repeating step (c).

[0033] In some implementations, the lithium source is a first lithium source, and wherein the method further comprises (e-1) replacing the first lithium source in the heating chamber with a second lithium source after step (c); and (e-2) repeating step (c).

[0034] In some implementations, the method further comprises cooling the heating chamber prior to step (e-1). 4 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0035] In a further aspect, the present invention provides a method of forming a sintered solid- state electrolyte material comprising: (aa) disposing a setter body of any one of claims 1-29 in a heating chamber; (bb) disposing a green body on the coating of the setter body, wherein the green body comprises a solid-state electrolyte material; (cc) heating the heating chamber to a temperature of from about 600 °C to about 1,500 °C to form the sintered solid-state electrolyte, wherein the solid-state electrolyte material loses less than about 20 mole percent of lithium during step (cc).

[0036] In some implementations, the solid-state electrolyte material loses less than about 15 mole percent of lithium during step (cc).

[0037] In some implementations, the solid-state electrolyte material loses less than about 10 mole percent of lithium during step (cc).

[0038] In some implementations, the method further comprises (dd) flowing a gas into the heating chamber.

[0039] In some implementations, the gas comprises a mixture of hydrogen and an inert gas.

[0040] In some implementations, the gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 3,000 SCCM.

[0041] In some implementations, step (dd) is performed at least partially during step (cc).

[0042] In some implementations, an atmosphere inside the heating chamber during step (cc) comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof.

[0043] In some implementations, an atmospheric pressure inside the heating chamber during step (cc) is from about 1 Pa to about 10 Mpa.

[0044] In some implementations, the green body further comprises at least one of a pore forming agent and a binder, and wherein step (cc) further comprises (cc-1) heating the heating chamber to a first temperature of from about 400 °C to about 800 °C to burnout the at least one of the pore forming agent and the binder; and (cc-2) heating the heating chamber to a second temperature of from about 600 °C to about 1,500 °C to form the sintered solid-state electrolyte, wherein the second temperature is greater than the first temperature. 5 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0045] In some implementations, wherein the method further comprises (dd) flowing a gas into the heating chamber.

[0046] In some implementations, step (dd) further comprises (dd-1) flowing a first gas into the heating chamber at least partially during step (cc-1); and (dd-2) flowing a second gas into the heating chamber at least partially during step (cc-2).

[0047] In some implementations, the first and second gases are each independently flowed into the heating chamber at a flow rate of from about 1 SCCM to about 3,000 SCCM.

[0048] In some implementations, the first gas comprises oxygen or air, and wherein the second gas comprises a mixture of hydrogen (or CO) and an inert gas. BRIEF DESCRIPTION OF THE DRAWINGS

[0049] The following figures are provided by way of example and are not intended to limit the scope of the claimed invention.

[0050] FIG.1 is a cross-sectional view of a first exemplary embodiment of a setter body for sintering a solid-state electrolyte material.

[0051] FIG.2 is a cross-sectional view of a second exemplary embodiment of a setter body for sintering a solid-state electrolyte material.

[0052] FIG.3 is a cross-sectional view of a third exemplary embodiment of a setter body for sintering a solid-state electrolyte material.

[0053] FIG.4 is a cross-sectional view of a fourth exemplary embodiment of a setter body for sintering a solid-state electrolyte material.

[0054] FIG.5 is a flow chart of a method of forming a setter body according to one implementation of the invention.

[0055] FIG.6 is a flow chart of a method of forming a sintered solid-state electrolyte material according to one implementation of the invention.

[0056] FIG.7A is an image of the nickel-mesh substrate of Example 1 prior to cleaning.

[0057] FIG.7B is an image of the nickel-mesh substrate of Example 1 after cleaning.

[0058] FIG.8 is a front view of a stack for forming setter bodies according to Example 1.

[0059] FIG.9 is an image of a portion of a setter body comprising a nickel-mesh substrate and nodules according to Example 1. 6 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0060] FIG.10 is a graph of the results of the XPS analysis of the setter body comprising a nickel plate according to Example 1, wherein nickel, lithium, oxygen, and carbon atomic concentrations are plotted against the scanning depth of the setter body.

[0061] FIG.11 is a front view of a stack for sintering a solid-state electrolyte material according to Example 2.

[0062] FIG.12A is images of the setter bodies and green body tape of Example 2, prior to sintering.

[0063] FIG.12B is images of the setter bodies of Example 2, after sintering and a cross section of the resulting bilayer LLZO solid state electrolyte material.

[0064] FIG.12C is images of the setter bodies of Example 2 after being recycled for use in six (6) sintering cycles and a cross section of the bilayer LLZO solid state electrolyte material resulting from the sixth sintering cycle.

[0065] FIG.12D is images of the setter bodies of Example 2 after being recycled for use in eleven (11) sintering cycles and a cross section of the bilayer LLZO solid state electrolyte material resulting from the eleventh sintering cycle.

[0066] FIG.13A is an image of cross section of the LLZO bilayer material of Example 3 after treatment with a sintering process.

[0067] FIG.13B is the EDX spectrum of the dense surface of the LLZO bilayer material treated with a sintering process on an iron setter, according to Example 3.

[0068] FIG.14 is an image of cross section of the LLZO bilayer material of Example 6 after treatment with a sintering process.

[0069] Like reference numerals in the various drawings indicate like elements. For example, the substrate may be referred to as 102 in FIG.1, as 302 in FIG.3, and 802a and 802b in FIG.8. DETAILED DESCRIPTION

[0070] The present invention provides a setter body, methods of forming such a setter body, and methods of using such a setter body.

[0071] As used herein, the following definitions shall apply unless otherwise indicated.

[0072] I. DEFINITIONS

[0073] The terminology used herein is for the purpose of describing particular exemplary configurations only and is not intended to be limiting. As used herein, the singular articles "a," "an," and "the" may be intended to include the plural forms as well, unless the context clearly 7 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 indicates otherwise. The terms "comprises," "comprising," "including," and "having," are inclusive and therefore specify the presence of features, steps, operations, elements, and / or components, but do not preclude the presence or addition of one or more other features, steps, operations, elements, components, and / or groups thereof. The method steps, processes, and operations described herein are not to be construed as necessarily requiring their performance in the particular order discussed or illustrated, unless specifically identified as an order of performance. Additional or alternative steps may be employed.

[0074] The terms first, second, third, etc. may be used herein to describe various elements, components, regions, layers and / or sections. These elements, components, regions, layers and / or sections should not be limited by these terms. These terms may be only used to distinguish one element, component, region, layer or section from another region, layer or section. Terms such as "first," "second," and other numerical terms do not imply a sequence or order unless clearly indicated by the context. Thus, a first element, component, region, layer or section discussed below could be termed a second element, component, region, layer or section without departing from the teachings of the example configurations.

[0075] As used herein, when an element is referred to as being "on," "engaged to," "connected to," "attached to," or "coupled to" another element, it may be directly on, engaged, connected, attached, or coupled to the other element, or intervening elements may be present. In contrast, when an element is referred to as being "directly on," "directly engaged to," "directly connected to," "directly attached to," or "directly coupled to" another element, there may be no intervening elements or layers present. Other words used to describe the relationship between elements should be interpreted in a like fashion (e.g., "between" versus "directly between," "adjacent" versus "directly adjacent," etc.). As used herein, the term "and / or" includes any and all combinations of one or more of the associated listed items.

[0076] As used herein, the term "setter body" refers to a body comprising a substrate and a coating. The substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface. The substrate comprises nickel. The coating is at least partially disposed on the first surface of the substrate. In some embodiments, the coating comprises at least about 1 mole percent of lithium. In other embodiments, the coating comprises at least about 1 wt% of lithium based on the total weight of the coating. 8 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0077] As used herein, the term "mole percent (mol %)" of a constituent (or element) refers to a percentage of the constituent (or element), expressed in moles, that is present in an article (e.g., the substrate or the coating) based on the total amount of all constituents, expressed in moles, present in the article. For example, in the context of an amount of lithium present in a coating, the mole percent of lithium is calculated according to the following formula: " Mole percent (mol %) of lithium in the coating =&%)$%*'")()#&x 100% wherein nlithiumis the number of moles of lithium in the coating; and ntotal is the number of total moles of all constituents in the coating.

[0078] It will be appreciated that the mole percent of lithium in the coating and / or the substrate includes elemental lithium in addition to lithium that is covalently and / or ionically bonded in lithium-containing compounds present in the coating and / or the substrate. Lithium-containing compounds include lithium oxides and lithium alloys.

[0079] As used herein, it will be appreciated that a "wt% of lithium" in the coating and / or the substrate includes elemental lithium in addition to lithium that is covalently and / or ionically bonded in lithium-containing compounds present in the coating and / or the substrate.

[0080] As used herein, the term "solid-state electrolyte material" refers to a material that is suitable for use in a solid-state battery cell, such as LLZO materials.

[0081] As used herein, the term "green body" refers to an unsintered body (e.g., a tape and / or film) that comprises a solid-state electrolyte material.

[0082] As used herein, the term "apparent porosity" refers to the open (or accessible) porosity (i.e., porosity that excludes volume(s) from sealed or closed pores, cells, or voids). Apparent porosity can be represented as a fraction or percentage of the volume of open pores, cells, or voids over the total volume.

[0083] As used herein, the term "doping" and other forms of the word (e.g., "doped") refer to the presence or placement of atoms other than the base atoms in the crystal structure of the garnet material. For example, for the base structure of Li7La3Zr2O12(a LLZO material), an atom can be substituted for a portion or all of the lithium, a portion or all of the lanthanum, a portion or all of the zirconium and / or a portion or all of the oxygen. Such substitution can be made after forming the base structure or during the formation of the base structure. Similar substitutions can be made for other garnet-based structures. 9 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0084] As used herein, the term "powder bed" refers to a powder that contains lithium that is near the component being thermally processed. The powder can be composed of undoped LLZO, doped LLZO, or another material containing lithium. The powder bed may act as a source of lithium during thermal processing.

[0085] II. SETTER BODY

[0086] In one aspect, the present invention provides a setter body for sintering a solid-state electrolyte material. As shown in FIG.1, the setter body 100 comprises a substrate 102 and a coating 104.

[0087] A. Substrate

[0088] With continued reference to FIG.1, the substrate has a first surface 106, a second surface 108 opposite the first surface, and an outer surface 110 extending from the first surface to the second surface.

[0089] Materials suitable as substrates of the present invention do not substantially deplete SSE materials (e.g., LLZO materials) of lithium when such SSE materials are sintered and do not adhere to the SSE material (e.g., LLZO material) during or after sintering.

[0090] Metal oxides and other oxide materials react with lithium containing materials (e.g., SSE materials (e.g., LLZO materials)) under sintering conditions (e.g., elevated temperatures between from about 600°C to about 900°C). This undesired reaction can consume lithium and cause depletion of lithium from the SSE material. The reaction may also cause the SSE material to adhere to or fuse with the setter. Moreover, the sintering process may also facilitate undesired cross-diffusion of chemical species between the oxide material and the SSE material.

[0091] Metals and metal alloys commonly possess a native metal oxide coating formed by exposure of the metal or alloy to atmospheric conditions. Metals and metal alloys possessing native metal oxide coatings will react with lithium containing materials (e.g., SSE materials (e.g., LLZO materials)), unless the native oxide coating is substantially or completely removed. Thus, suitable metals and metal alloys useful for substrates of the present invention are those capable of shedding substantially all or all of the oxygen of their native metal oxide coatings when heated under reducing conditions (e.g., heating at elevated temperatures between from about 600°C to about 900°C in an atmosphere comprising hydrogen, carbon monoxide, combinations thereof, and the like; or heating at elevated temperatures between from about 600°C to about 900°C and contacting the metal and / or metal alloy with solid carbon). 10 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0092] In some embodiments, the native oxide coating can be removed by heating the substrate material (e.g., heating at a temperature of from about 600°C to about 900°C) in a reducing environment by using, for example, an atmosphere comprising hydrogen or carbon monoxide, or using solid carbon in contact with the metal. In some examples, the material is heated at a temperature of from about 600°C to about 900°C under an atmosphere of about 0.3% H2 to about 0.9% H2in argon (or other inert gas) to remove all or substantially all of the native metal oxide coating.

[0093] 0E 2CCBE@A:D =B:@H:D BI : GCFJ F? JA> 3B;;I ?H>> >E>H@O #T3$ L>HIKI J>DG>H:JKH>' 8BE<> >EJHFGO #T4$ :E= >EJA:CGO #T8$ :H> >II>EJB:CCO <FEIJ:EJ MBJA J>DG>H:JKH> KEC>II : GA:I> <A:E@> F<<KHI% JA> ?H>> >E>H@O L>HIKI J>DG>H:JKH> GCFJ BI =H:ME :I : I>HB>I F? IJH:B@AJ CBE>I% MA>H> T8 BI JA> ICFG> :E= T4 BI JA> O&BEJ>H<>GJ' 9A> ICFG> F? JA> CBE> <A:E@>I MA>E :EO F? JA> D:J>HB:CI involved melt or vaporize. Free energy of formation is negative for most metal oxides, and so JA> =B:@H:D BI =H:ME MBJA T3 / 6 :J JA> JFG F? JA> =B:@H:D% :E= JA> L:CK>I F? T3 IAFME :H> :CC negative numbers. Temperatures where either the metal or oxide melt or vaporize can be marked on the diagram. In the Ellingham diagram for metals reacting to form oxides, the oxygen partial pressure is taken as 1 atmosphere, and all of the reactions are normalized to consume one mole of O2. Thus Ellingham diagrams for metals illustrate which metals can reduce their native oxide coating at a temperature of from about 600° to about 900°C. For instance, in an Ellingham diagram depicting the free energy of formation for nickel (II) oxide from nickel metal and oxygen is an upward sloping line as temperature increases. The line depicting the free energy of formation for water from hydrogen and oxygen is an upward sloping line as temperature increases and is below the line for nickel to nickel (II) oxide. This indicates that the formation of water is more favorable thermodynamically at a temperature of from about 600°C to about 900°C and therefore hydrogen can be used to reduce the native oxide to metallic nickel. Nickel is therefore a suitable substrate. Similarly, other metals having an Ellingham diagram line above hydrogen in this temperature range (i.e., at a temperature of from about 600°C to about 900°C) would also be suitable substrates. For example, cobalt, copper, and alloys thereof are also suitable substrates. However, the line for iron is below that for hydrogen, so if hydrogen is used as the reducing agent then the native oxide coating for iron will not be removed at a temperature of from about 600°C to about 900°C; thus iron is not a suitable substrate, as shown in Example 4 below. However, as demonstrated in Examples 4 and 5 below, metal alloys formed of less than 11 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 about 20 wt% (e.g., less than about 15 wt%, less than about 10 wt%, or less than about 5 wt%) of iron are suitable alloys. In Example 4, Invar (containing 64 wt% iron) did not form a suitable substrate; but, in Example 5, Monel 400 (containing ~65 wt% Ni, ~33 wt% Cu, and ~2 wt% Fe) was shown to be a suitable substrate. Consequently, alloys possessing at least about 80 wt% (e.g., from about 80% to 100%, from about 85% to 100%, from about 90% to 100%, or from about 95% to 100%) of one or more metals having a Ellingham diagram line above hydrogen at a temperature range of from about 600°C to about 900°C are suitable substrate materials. Table 1 describes certain examples of suitable substrate materials of the present invention.

[0094] Table 1: Examples of Substrate Materials Material Composition (wt%) Suitable Setter Material ' "

[0095] In some embodiments, the substrate comprises nickel. In some embodiments, the nickel of the substrate is elemental nickel, a nickel oxide, a nickel alloy, or any combination thereof. For example, the substrate may comprise elemental nickel. And, in some embodiments, the substrate comprises a nickel oxide (e.g., nickel(II) oxide (NiO), nickel (III) oxide (Ni2O3), and other oxides containing nickel).

[0096] In some embodiments, the substrate comprises a nickel alloy. For example, the nickel alloy may comprise aluminum, iron, copper, molybdenum, chromium, titanium, cobalt, tungsten, platinum, or any combination thereof. In some embodiments, the nickel alloy comprises aluminum. In some embodiments, the nickel alloy comprises less than about 20 wt% (e.g., less 12 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 than about 15 wt%, less than about 10 wt%, or less than about 5 wt%) of iron. For example, the Ni alloy comprises from about 0.01 wt% to about 18 wt% (e.g., from about 0.05 wt% to about 15wt%, from about 0.05 wt% to about 10 wt%, or from about 0.05 wt% to about 5 wt%) of Fe. In other embodiments, the nickel alloy comprises copper. In some embodiments, the nickel alloy comprises molybdenum. In some embodiments, the nickel alloy comprises chromium. In other embodiments, the nickel alloy comprises titanium. In some embodiments, the nickel alloy comprises cobalt. In some embodiments, the nickel alloy comprises tungsten. And, in some embodiments, the nickel alloy comprises copper and cobalt. Non-limiting examples of nickel alloys include nickel alloy 400 (UNS N04400), alloy B-2 (UNS N10665), nichrome 70 (UNS N06008), nickel alloy 600 (UNS N06600), nickel alloy 601 (UNS N06601), nickel alloy X-750 (UNS N07750), nickel alloy 825 (UNS N08825), alloy G-3 (UNS N06985), nickel alloy 800 (UNS N08800), alloy C-276 (UNS N10276), alloy C-22 (UNS N06022), nickel alloy 59 (UNS N06059), alloy C-2000 (UNS N06200), nickel alloy 686 (UNS N06686), nickel alloy 617 (UNS N06617), nickel alloy HR-160 (UNS N12160), nickel alloy 602 CA, and nitinol (UNS N01555).

[0097] In some embodiments, the nickel alloy comprises one or more inert metals. In other embodiments, the nickel alloy has a melting point of at least about 1,300 °C. For example, the nickel alloy may have a melting point of at least about 1,400 °C. And, in other embodiments, the nickel alloy has a melting point of at least about 1,500 °C.

[0098] In some embodiments, the substrate is a plate, a foam, or a mesh. In other embodiments, the substrate is a plate. When the substrate is a plate, the plate may have a thickness of from about 1 µm (e.g., the substrate plate is a foil) to about 10,000 µm. In some embodiments, the plate has a thickness of from about 1,000 µm to about 10,000 µm. In some embodiments, the plate has a thickness of from about 1,000 µm to about 2,000 µm. In other embodiments, the plate has a thickness of from about 2,000 µm to about 3,000 µm. In some embodiments, the plate has a thickness of from about 3,000 µm to about 4,000 µm. In some embodiments, the plate has a thickness of from about 4,000 µm to about 5,000 µm. In other embodiments, the plate has a thickness of from about 5,000 µm to about 6,000 µm. In some embodiments, the plate has a thickness of from about 6,000 µm to about 7,000 µm. In some embodiments, the plate has a thickness of from about 7,000 µm to about 8,000 µm. In other embodiments, the plate has a thickness of from about 8,000 µm to about 9,000 µm. In some embodiments, the 13 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 plate has a thickness of from about 2,500 µm to about 7,500 µm. And, in some embodiments, the plate has a thickness of from about 9,000 µm to about 10,000 µm.

[0099] In some embodiments, the plate has an apparent porosity of less than about 5%. For example, the plate may have an apparent porosity of less than 2.5 percent. In other embodiments, the plate has an apparent porosity of less than about 1%. And, in some embodiments, the plate is substantially free of (or free of) pores.

[0100] In some embodiments, the plate comprises a cladding, wherein the cladding comprises elemental nickel, a nickel oxide, a nickel alloy, or any combination thereof. For example, the plate comprises a ceramic clad with elemental nickel, a nickel oxide, a nickel alloy, or any combination thereof. In other examples, the plate comprises a ceramic (e.g., an aluminum oxide ceramic, a zirconium oxide ceramic, or other ceramic) and a cladding comprising elemental nickel, a nickel oxide (such as any nickel oxide described herein), a nickel alloy (such as any nickel alloy described herein), or any combination thereof. In other embodiments, the plate comprises aluminum, iron, copper, tin, or any combination thereof, clad with elemental nickel, a nickel oxide, a nickel alloy, or any combination thereof. For example, the plate comprises copper with nickel cladding, iron with nickel cladding, tin with nickel cladding, or aluminum with nickel cladding.

[0101] In some embodiments, the plate comprises a nickel layer, wherein the nickel layer comprises elemental nickel, a nickel oxide, a nickel alloy, or any combination thereof, wherein the nickel layer is disposed on the surface of a ceramic as an annealed paste, by sputtering, or by vapor deposition. In some examples, the plate comprises a ceramic (e.g., an aluminum oxide ceramic, a zirconium oxide ceramic, or other ceramic) and a nickel layer, wherein the nickel layer comprises elemental nickel, a nickel oxide (such as any nickel oxide described herein), a nickel alloy (such as any nickel alloy described herein), or any combination thereof, and wherein the nickel layer has a thickness of at least about 50 µm.

[0102] In some embodiments, the substrate is a foam. When the substrate is a foam, the foam may have thickness of from about 1 µm to about 1,000 µm. For example, the foam may have a thickness of from about 1 µm to about 100 µm. In other embodiments, the foam may have a thickness of from about 100 µm to about 200 µm. In some embodiments, the foam may have a thickness of from about 200 µm to about 300 µm. In some embodiments, the foam may have a thickness of from about 300 µm to about 400 µm. In other embodiments, the foam may have a 14 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 thickness of from about 400 µm to about 500 µm. In some embodiments, the foam may have a thickness of from about 500 µm to about 600 µm. In some embodiments, the foam may have a thickness of from about 600 µm to about 700 µm. In other embodiments, the foam may have a thickness of from about 700 µm to about 800 µm. In some embodiments, the foam may have a thickness of from about 800 µm to about 900 µm. In some embodiments, the foam may have a thickness of from about 250 µm to about 750 µm. And, in some embodiments, the foam may have a thickness of from about 900 µm to about 1,000 µm.

[0103] In some embodiments, the foam has an apparent porosity of greater than about 5%. For example, the foam may have an apparent porosity of greater than about 10%. In other embodiments, the foam has an apparent porosity of greater than about 20%. In some embodiments, the foam has an apparent porosity of greater than about 30%. In some embodiments, the foam has an apparent porosity of greater than about 40%. In other embodiments, the foam has an apparent porosity of greater than about 50%. In some embodiments, the foam has an apparent porosity of greater than about 60%. In some embodiments, the foam has an apparent porosity of greater than about 70%. In other embodiments, the foam has an apparent porosity of greater than about 80%. And, in some embodiments, the foam has an apparent porosity of greater than about 90%.

[0104] In some embodiments, the foam has an apparent porosity of from about 20% to about 80%. In other embodiments, the foam has an apparent porosity of from about 35% to about 75%. In some embodiments, the foam has an apparent porosity of from about 45% to about 65%. In some embodiments, the foam has an apparent porosity of from about 50% to about 60%. In some embodiments, the foam has an apparent porosity of from about 60% to about 80%. In some embodiments, the foam has an apparent porosity of from about 20% to about 95%. And, in some embodiments, the foam has an apparent porosity of from about 50% to about 90%.

[0105] In some embodiments, the substrate is a mesh. When the substrate is a mesh, the mesh may have thickness of from about 1 µm to about 1,000 µm. For example, the mesh may have a thickness of from about 1 µm to about 100 µm. In other embodiments, the mesh may have a thickness of from about 100 µm to about 200 µm. In some embodiments, the mesh may have a thickness of from about 200 µm to about 300 µm. In some embodiments, the mesh may have a thickness of from about 300 µm to about 400 µm. In other embodiments, the mesh may have a 15 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 thickness of from about 400 µm to about 500 µm. In some embodiments, the mesh may have a thickness of from about 500 µm to about 600 µm. In some embodiments, the mesh may have a thickness of from about 600 µm to about 700 µm. In other embodiments, the mesh may have a thickness of from about 700 µm to about 800 µm. In some embodiments, the mesh may have a thickness of from about 800 µm to about 900 µm. In some embodiments, the mesh may have a thickness of from about 250 µm to about 750 µm. And, in some embodiments, the mesh may have a thickness of from about 900 µm to about 1,000 µm.

[0106] In some embodiments, the mesh has an apparent porosity of greater than about 5%. For example, the mesh may have an apparent porosity of greater than about 10%. In other embodiments, the mesh has an apparent porosity of greater than about 20%. In some embodiments, the mesh has an apparent porosity of greater than about 30%. In some embodiments, the mesh has an apparent porosity of greater than about 40%. In other embodiments, the mesh has an apparent porosity of greater than about 50%. In some embodiments, the mesh has an apparent porosity of greater than about 60%. In some embodiments, the mesh has an apparent porosity of greater than about 70%. In other embodiments, the mesh has an apparent porosity of greater than about 80%. And, in some embodiments, the mesh has an apparent porosity of greater than about 90%.

[0107] In some embodiments, the mesh has an apparent porosity of from about 20% to about 80%. In other embodiments, the mesh has an apparent porosity of from about 35% to about 75%. In some embodiments, the mesh has an apparent porosity of from about 45% to about 65%. In some embodiments, the mesh has an apparent porosity of from about 50% to about 60%. In some embodiments, the mesh has an apparent porosity of from about 60% to about 80%. In some embodiments, the mesh has an apparent porosity of from about 20% to about 95%. And, in some embodiments, the mesh has an apparent porosity of from about 50% to about 90%.

[0108] In some embodiments, the substrate (e.g., the mesh) has a weight-to-area ratio of from about 0.01 g / cm2to about 14.0 g / cm2(e.g., from about 0.05 g / cm2to about 1.0 g / cm2). For example, the substrate may have a weight-to-area ratio of from about 0.01 g / cm2to about 0.5 g / cm2. In some embodiments, the substrate has a weight-to-area ratio of from about 0.1 g / cm2to about 0.5 g / cm2. In other embodiments, the substrate has a weight-to-area ratio of from about 0.1 g / cm2to about 0.4 g / cm2. In some embodiments, the substrate has a weight-to-area ratio of 16 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 from about 0.1 g / cm2to about 0.3 g / cm2. And, in some embodiments, the substrate has a weight- to-area ratio of from about 0.1 g / cm2to about 0.2 g / cm2.

[0109] In some embodiments, the substrate comprises less than about 1 mole percent of lithium. In other embodiments, the substrate comprises less than about 0.5 mole percent of lithium. In additional embodiments, the substrate comprises less than about 0.25 mole percent (e.g., less than about 0.10 mole percent) of lithium. And, in some embodiments, substrate is free of lithium.

[0110] B. Coating

[0111] When lithium containing materials such as LLZO are sintered, they volatilize lithium and generate a vapor pressure of lithium at high temperatures. If the vapor pressure of lithium in the immediate vicinity to the article being sintered does not reach an equilibrium or saturation point, then the lithium containing material (LLZO) will become depleted of lithium, which is undesirable for generating sintered SSE materials. In the case of LLZO, depletion of lithium before or during sintering can prevent the LLZO from densifying leading to undersintering, or it may generate undesirable secondary phases that are lithium poor, such as La2Zr2O7. Setter materials used with lithium-containing materials, and specifically LLZO, adsorb lithium on their surfaces on first use and act as lithium sinks in the furnace and deplete the sintering article of lithium. By coating the substrate with a coating comprising lithium before sintering, the vapor pressure of lithium in the immediate vicinity of the sintering article can reach an equilibrium point and reduce lithium depletion from the sintering article. The coating enables the setters to be used repeatedly and indefinitely.

[0112] With reference again to FIG.1, the coating is at least partially disposed on the first surface of the substrate. The coating comprises at least about 1 mole percent of lithium. And, the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate.

[0113] In some embodiments, as shown in FIG.1, the coating is disposed on the entire first surface of the substrate. In other embodiments, the coating is disposed on substantially all (e.g., at least about 60 %, at least about 70%, at least about 80%, at least about 90%, or at least about 95%) of the first surface of the substrate. And, in other embodiments, the coating is disposed only on a portion of the first surface of the substrate (e.g., from about 10% to about 55% of the first surface of the substrate). 17 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0114] In some embodiments, the coating has a thickness of from about 1 nm to about 100 µm. In some embodiments, the coating has a thickness of from about 10 nm to about 100 nm (e.g., from about 20 nm to about 75 nm). In other embodiments, the coating has a thickness of from about 1 nm to about 50 µm. In some embodiments, the coating has a thickness of from about 1 nm to about 1 µm. For example, the coating may have a thickness of from about 1 nm to about 100 nm. In some embodiments, the coating has a thickness of from about 100 nm to about 200 nm. In some embodiments, the coating has a thickness of from about 200 nm to about 300 nm. In other embodiments, the coating has a thickness of from about 300 nm to about 400 nm. In some embodiments, the coating has a thickness of from about 400 nm to about 500 nm. In some embodiments, the coating has a thickness of from about 500 nm to about 600 nm. In other embodiments, the coating has a thickness of from about 600 nm to about 700 nm. In some embodiments, the coating has a thickness of from about 700 nm to about 800 nm. In some embodiments, the coating has a thickness of from about 800 nm to about 900 nm. In other embodiments, the coating has a thickness of from about 250 nm to about 750 nm. And, in some embodiments, the coating has a thickness of from about 900 nm to about 1 µm.

[0115] In some embodiments, the coating comprises elemental lithium, a lithium oxide, lithium peroxide, lithium carbonate, a lithium carbonate, a lithium alloy, or any combination thereof. For example, the coating may comprise elemental lithium. In other examples, the coating comprises elemental an oxide, peroxide, or hydroxide of lithium. In some embodiments, the coating comprises a lithium oxide. And, in some embodiments, the coating comprises a lithium alloy.

[0116] In some embodiments, the coating may comprise at least one nodule extending away from the first surface of the substrate. In other embodiments, the coating comprises one nodule. And, in some embodiments, the coating comprises a plurality of nodules.

[0117] When present, the at least one nodule comprises aluminum, silicon, magnesium, calcium, titanium, oxygen, or any combination thereof. For example, the at least one nodule may comprise aluminum. In other embodiments, the at least one nodule comprises silicon. In some embodiments, the at least one nodule comprises magnesium. In some embodiments, the at least one nodule comprises calcium. In some embodiments, the at least one nodule comprises oxygen (i.e., oxygen is present in one or more oxide forms). And, in some embodiments, the at least one nodule comprises aluminum, silicon, magnesium, calcium, and oxygen. 18 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0118] In some embodiments, the coating comprises at least about 2.5 mole percent of lithium. In other embodiments, the coating comprises at least about 5 mole percent of lithium. For example, the coating may comprise at least about 10 mole percent of lithium. In other embodiments, the coating comprises at least about 15 mole percent of lithium. In some embodiments, the coating comprises at least about 20 mole percent of lithium. In some embodiments, the coating comprises at least about 25 mole percent of lithium. In other embodiments, the coating comprises at least about 30 mole percent of lithium. In some embodiments, the coating comprises at least about 35 mole percent of lithium. In some embodiments, the coating comprises at least about 40 mole percent of lithium. In other embodiments, the coating comprises at least about 45 mole percent of lithium. In some embodiments, the coating comprises at least about 50 mole percent of lithium. In some embodiments, the coating comprises at least about 55 mole percent of lithium. In other embodiments, the coating comprises at least about 60 mole percent of lithium. In some embodiments, the coating comprises at least about 65 mole percent of lithium. In some embodiments, the coating comprises at least about 70 mole percent of lithium. In other embodiments, the coating comprises at least about 75 mole percent of lithium. And, in some embodiments, the coating comprises at least about 80 mole percent of lithium.

[0119] In some embodiments, the coating comprises at least about 1 wt% of lithium based on the total weight of the coating. In other embodiments, the coating comprises at least about 2.5 wt% of lithium based on the total weight of the coating. For example, the coating may comprise at least about 5 wt% of lithium based on the total weight of the coating. In some embodiments, the coating comprises at least about 10 wt% of lithium based on the total weight of the coating. In some embodiments, the coating comprises at least about 15 wt% of lithium based on the total weight of the coating. In other embodiments, the coating comprises at least about 20 wt% of lithium based on the total weight of the coating. In some embodiments, the coating comprises at least about 25 wt% of lithium based on the total weight of the coating. In some embodiments, the coating comprises at least about 30 wt% of lithium based on the total weight of the coating. In other embodiments, the coating comprises at least about 35 wt% of lithium based on the total weight of the coating. In some embodiments, the coating comprises at least about 40 wt% of lithium based on the total weight of the coating. In some embodiments, the coating comprises at least about 45 wt% of lithium based on the total weight of the coating. In other embodiments, 19 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 the coating comprises at least about 50 wt% of lithium based on the total weight of the coating. In some embodiments, the coating comprises at least about 55 wt% of lithium based on the total weight of the coating. In some embodiments, the coating comprises at least about 60 wt% of lithium based on the total weight of the coating. In other embodiments, the coating comprises at least about 65 wt% of lithium based on the total weight of the coating. In some embodiments, the coating comprises at least about 70 wt% of lithium based on the total weight of the coating. In some embodiments, the coating comprises at least about 75 wt% of lithium based on the total weight of the coating. And, in some embodiments, the coating comprises at least about 80 wt% of lithium based on the total weight of the coating.

[0120] In some embodiments, the coating is at least partially disposed on at least one of the second and outer surfaces of the substrate. For example, as shown in FIG.2, the coating 204 may be at least partially disposed on the outer surface 210 of the substrate 202. In the illustrated embodiment, the coating is disposed on the entire outer surface of the substrate. In other embodiments, the coating is disposed on substantially all (e.g., at least 60 %, at least 70%, at least 80%, at least 90%, or at least 95%) of the outer surface of the substrate. And, in some embodiments, the coating is disposed only on a portion of the outer surface of the substrate.

[0121] With reference to FIG.3, in other embodiments, the coating 304 is at least partially disposed on the second surface 308 of the substrate 302. In some embodiments, the coating is disposed on the entire second surface of the substrate. In other embodiments, the coating is disposed on substantially all (e.g., at least 60 %, at least 70%, at least 80%, at least 90%, or at least 95%) of the second surface of the substrate. And, in some embodiments, the coating is disposed only on a portion of the second surface of the substrate.

[0122] As shown in FIG.4, the coating 404 may be disposed on each of the first, second, and outer surfaces of the substrate 402. In some embodiments, the coating is disposed on the entire first, second, and outer surfaces of the substrate. In other embodiments, the coating is disposed on substantially all (e.g., at least 60 %, at least 70%, at least 80%, at least 90%, or at least 95%) of the first, second, and outer surfaces of the substrate. And, in some embodiments, the coating is disposed only on a portion of the first, second, and outer surfaces of the substrate.

[0123] Referring to FIGs 8 and 9, in some embodiments, wherein the substrate is a mesh or a foam (no pictured), the coating may be on portions one or more external surface(s) of the mesh or foam. For example, the coating may be disposed on substantially all of the external surfaces 20 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 of the mesh substrate, so that each of the wires or filaments forming the mesh are substantially coated with the coating.

[0124] C. Alternative Embodiments

[0125] In another aspect, the present invention provides a setter body for sintering a solid-state electrolyte material. The setter body comprises a substrate and a coating. The substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface. The substrate comprises nickel. The coating is at least partially disposed on the first surface of the substrate. The coating comprises at least about 1 wt% of lithium based on the total weight of the coating. And, the wt% percent of lithium in the coating is greater than a wt% percent of lithium in the substrate.

[0126] In a further aspect, the present invention provides a setter body for sintering a solid-state electrolyte material. The setter body comprises a substrate and a coating. The substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface. The substrate comprises a mesh further comprising nickel. The coating is at least partially disposed on the first surface of the mesh substrate. The coating comprises at least about 5 mole percent of lithium (e.g., from about 5 mole percent to about 50 mole percent). And, the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate.

[0127] In yet another aspect, the present invention provides a setter body for sintering a solid- state electrolyte material. The setter body comprises a substrate and a coating. The substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface. The substrate comprises nickel. The coating is at least partially disposed on two or more surfaces selected from the first surface, the second surface, and the outer surface of the substrate. The coating comprises at least about 1 mole percent of lithium (e.g., from about 5 mole percent to about 50 mole percent). And, the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate.

[0128] In another aspect, the present invention provides a setter body for sintering a solid-state electrolyte material. The setter body comprises a substrate and a coating. The substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface. The substrate comprises nickel. The coating is at least partially disposed on two or more surfaces selected from the first surface, the second surface, and 21 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 the outer surface of the substrate. The coating comprises at least about 5 mole percent of lithium (e.g., from about 5 mole percent to about 50 mole percent). And, the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate.

[0129] In another aspect, the present invention provides a setter body for sintering a solid-state electrolyte material. The setter body comprises a substrate and a coating. The substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface. The substrate comprises nickel. The coating is at least partially disposed on two or more surfaces selected from the first surface, the second surface, and the outer surface of the substrate, and the coating is partially disposed between the first surface and the second surface (i.e., the coating is at least partially embedded within the substrate between the first and second surfaces). The coating comprises at least about 5 mole percent of lithium (e.g., from about 5 mole percent to about 50 mole percent). And, the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate.

[0130] In one aspect, the present invention provides a setter body for sintering a solid-state electrolyte material. The setter body comprises a substrate and a coating. The substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface. The substrate comprises mesh further comprising nickel. The substrate is free of lithium. The coating is at least partially disposed on the first surface of the substrate. The coating comprises at least about 5 mole percent of lithium. And, the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate.

[0131] In one aspect, the present invention provides a setter body for sintering a solid-state electrolyte material. The setter body comprises a substrate and a coating. The substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface. The substrate comprises mesh further comprising nickel. The coating is at least partially disposed on the first surface of the substrate and between the first surface and the second surface of the substrate. The coating comprises at least about 5 mole 22 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 percent of lithium (e.g., from about 5 mole percent to about 50 mole percent). And, the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate.

[0132] III. METHODS OF FORMING A SETTER BODY

[0133] Another aspect of the present invention provides a method of forming a setter body. With reference to FIG.5, a flow chart depicting an example method for forming a setter body, the method comprises (a) disposing a substrate in a heating chamber, wherein the substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, and wherein the substrate comprises nickel (5002); (b) providing a lithium source in the heating chamber (5004); and (c) heating the heating chamber to a temperature of from about 600 °C to about 1,500 °C to form a coating comprising lithium from the lithium source at least partially on the first surface of the substrate, thereby forming the setter body (5006).

[0134] The substrate may be any substrate described herein. For example, in some implementations, the nickel of the substrate is elemental nickel, a nickel oxide, a nickel alloy, or any combination thereof. In other examples, the substrate comprises nickel cladding (e.g., copper with nickel cladding, iron with nickel cladding, tin with nickel cladding, or aluminum with nickel cladding). In other implementations, the substrate comprises elemental nickel. In some implementations, the substrate comprises a nickel alloy. And, in some implementations, the nickel alloy comprises aluminum, iron, copper, molybdenum, chromium, titanium, cobalt, tungsten, or any combination thereof.

[0135] In some implementations, the substrate is a plate, a foam, or a mesh. For example, the substrate may be a plate. In other implementations, the substrate is a foam. And, in some implementations, the substrate is a mesh.

[0136] In some implementations, the substrate comprises less than about 1 mole percent of lithium. In other implementations, the substrate comprises less than about 0.5 mole percent of lithium. And, in some examples and implementations, the substrate is free of lithium.

[0137] In some implementations, step (a) may comprise disposing a plurality of substrates in the heating chamber. For example, step (a) may comprise disposing 2, 5, 10, 20, or more substrates in the heating chamber. In some implementations, the plurality of substrates may be arranged as a stack of substrates in the heating chamber. 23 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0138] In some implementations, the heating chamber is an oven or a furnace.

[0139] In some implementations, the lithium source comprises lithium lanthanum zirconium oxide (LLZO). For example, in some implementations, the lithium source may be provided as a powder bed comprising LLZO. When the lithium source comprises LLZO, the LLZO may be doped, undoped, or a mixture of doped and undoped LLZO. In some implementations, the LLZO is doped. In other implementations, the LLZO is undoped. And, in some implementations, the lithium source comprises residual lithium remaining in the heating chamber from previous iterations of the method. In some implementations, the lithium source comprises lithium metal, an oxide of lithium, a hydroxide of lithium, a halogen salt of lithium, a carbonate of lithium, a nitrate of lithium, or any combination thereof. For example, the lithium source comprises Li2O, LiOH, LiOH•H2O, LiCl, Li2CO3, LiNO3, or any combination thereof. In some implementations, the lithium source comprises LiO2. In some implementations, the lithium source comprises LiOH. In other implementations, the lithium source comprises LiOH•H2O. In some implementations, the lithium source comprises LiCl. In some implementations, the lithium source comprises Li2CO3. And, in some implementations, the lithium source comprises LiNO3.

[0140] In some implementations, the lithium source comprises or is provided as a powder bed, a sacrificial tape, a method artifact in the furnace, or any combination thereof.

[0141] In some implementations, step (c) comprises heating the heating chamber to a temperature of from about 700 °C to about 1,500 °C. In other implementations, step (c) comprises heating the heating chamber to a temperature of from about 800 °C to about 1,500 °C (e.g., from about 800 °C to about 1,200 °C). In some implementations, step (c) comprises heating the heating chamber to a temperature of from about 900 °C to about 1,500 °C. And, in some implementations, step (c) comprises heating the heating chamber to a temperature of from about 1,000 °C to about 1,500 °C.

[0142] In some implementations, the coating comprises at least about 1 mole percent of lithium. In other implementations, the coating comprises at least about 5 mole percent of lithium. In some implementations, the coating comprises at least about 1 wt% of lithium based on the total weight of the coating. And, in some implementations, the coating comprises at least about 5 wt% of lithium based on the total weight of the coating.

[0143] In some implementations, the coating is at least partially disposed on at least one of the second and outer surfaces of the substrate. In other implementations, the coating is at least 24 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 partially disposed on the second surface of the substrate. In some implementations, the coating is at least partially disposed on the outer surface of the substrate. And, in some implementations, the coating is at least partially disposed on the second surface and the outer surface of the substrate.

[0144] In some implementations, step (c) is performed for at least about 1 minute. In other implementations, step (c) is performed for at least about 1 hour (e.g., from about 1 hour to about 3 hours, from about 1.5 hrs to about 2.5 hrs, or about 2 hrs). In some implementations, step (c) is performed for at least about 2 hours. And, in some implementations, step (c) is performed for from about 1 minute to about 5 hours.

[0145] In some implementations, the method further comprises (d) flowing a gas into the heating chamber.

[0146] In some implementations, the gas comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof. In other implementations, the gas comprises a mixture of hydrogen and an inert gas (e.g., nitrogen). For example, the gas may comprise carbon monoxide. In some implementations, the gas comprises carbon dioxide. In some implementations, the gas comprises ammonia. In other implementations, the gas comprises hydrogen sulfide. In some implementations, the gas comprises methane. In some implementations, the gas comprises hydrogen. In other implementations, the gas comprises nitrogen. In some implementations, the gas comprises argon. And, in some implementations, the gas comprises helium.

[0147] In some implementations, the gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 3,000 SCCM. For example, the gas may be flowed into the heating chamber at a flow rate of from about 1,000 SCCM to about 3,000 SCCM. In other implementations, the gas is flowed into the heating chamber at a flow rate of from about 1,500 SCCM to about 2,500 SCCM. In some implementations, the gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 1,500 SCCM. And, in some implementations, the gas is flowed into the heating chamber at a flow rate of from about 1,500 SCCM to about 3,000 SCCM.

[0148] In some implementations, step (d) is performed at least partially during step (c). In other implementations, an atmosphere inside the heating chamber during step (c) comprises carbon 25 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof.

[0149] In some implementations, the method further comprises (e) repeating step (c).

[0150] In some implementations, the lithium source is further defined as a first lithium source, and step (e) comprises (e-1) replacing the first lithium source in the heating chamber with a second lithium source after step (c); and (e-2) repeating step (c).

[0151] In some implementations, the method further comprises cooling the heating chamber prior to step (e-1). For example, the method may comprise cooling the heating chamber to about room temperature prior to step (e-1). In other implementations, the method may comprise cooling the heating chamber to less than about 100 °C prior to step (e-1). And, in some implementations, the method may comprise cooling the heating chamber to less than about 50 °C prior to step (e-1).

[0152] In some implementations, the method further comprises (f) cleaning the substrate prior to step (a).

[0153] It will be appreciated that the substrate may be cleaned in any suitable manner sufficient to prepare surfaces of the substrate to receive a coating. For example, step (f) may comprise cleaning the substrate prior to step (a) with a sonicator (e.g., an ultrasonicator). The substrate may be disposed in a solvent (e.g., isopropanol) for cleaning with the sonicator.

[0154] In some implementations, the method further comprises (g) cleaning the setter body after step (c).

[0155] It will be appreciated that the setter body may be cleaned in any suitable manner. For example, step (g) may comprise cleaning the setter body after step (c) with a sonicator (e.g., an ultrasonicator). The setter body may be disposed in a solvent (e.g., water) for cleaning with the sonicator.

[0156] In another aspect, the present invention provides a method of forming a setter body for sintering a solid-state electrolyte material. The method comprises 26 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 (I-a) disposing a substrate in a heating chamber, wherein the substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, and wherein the substrate comprises nickel; (I-b) providing a lithium source in the heating chamber; and (I-c) heating the heating chamber to a temperature of from about 800 °C to about 1,200 °C to form a coating comprising lithium from the lithium source at least partially on the first surface of the substrate, thereby forming the setter body, wherein the coating comprises at least about 1 mole percent (e.g., at least about 5 mole percent or from about 5 mole percent to about 50 mole percent) of lithium.

[0157] In a further aspect, the present invention provides a method of forming a setter body for sintering a solid-state electrolyte material. The method comprises (II-a) disposing a substrate in a heating chamber, wherein the substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, and wherein the substrate comprises nickel; (II-b) providing a lithium source in the heating chamber, wherein the lithium source comprises LLZO; and (II-c) heating the heating chamber to a temperature of from about 600 °C to about 1,500 °C to form a coating comprising lithium from the lithium source at least partially on the first surface of the substrate, thereby forming the setter body, wherein the coating comprises at least about 1 mole percent (e.g., at least about 5 mole percent or from about 5 mole percent to about 50 mole percent) of lithium.

[0158] In yet another aspect, the present invention provides a method of forming a setter body for sintering a solid-state electrolyte material. The method comprises (III-a) disposing a substrate in a heating chamber, wherein the substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, and wherein the substrate comprises nickel; (III-b) providing a lithium source in the heating chamber; (III-c) heating the heating chamber to a temperature of from about 600 °C to about 1,500 °C to form a coating comprising lithium from the lithium source at least partially on the first surface of the substrate, thereby forming the setter body, wherein the coating comprises at least 27 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 about 1 mole percent (e.g., at least about 5 mole percent or from about 5 mole percent to about 50 mole percent) of lithium; and (III-d) flowing a gas into the heating chamber at least partially during step (c), wherein the gas comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof.

[0159] In another aspect, the present invention provides a method of forming a setter body for sintering a solid-state electrolyte material. The method comprises (IV-a) disposing a substrate in a heating chamber, wherein the substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, and wherein the substrate comprises nickel; (IV-b) providing a lithium source in the heating chamber; (IV-c) heating the heating chamber to a temperature of from about 600 °C to about 1,500 °C to form a coating comprising lithium from the lithium source at least partially on the first surface of the substrate, thereby forming the setter body, wherein the coating comprises at least about 1 mole percent of lithium; (IV-d) flowing a gas into the heating chamber at least partially during step (c), wherein the gas comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof; and (IV-f) cleaning the substrate prior to step (a).

[0160] In one aspect, the present invention provides a method of forming a setter body for sintering a solid-state electrolyte material. The method comprises (V-a) disposing a substrate in a heating chamber, wherein the substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, and wherein the substrate comprises nickel; (V-b) providing a lithium source in the heating chamber, wherein the lithium source comprises LLZO; (V-c) heating the heating chamber to a temperature of from about 600 °C to about 1,500 °C to form a coating comprising lithium from the lithium source at least partially on the first surface of the substrate, thereby forming the setter body, wherein the coating comprises at least about 1 mole percent (e.g., at least about 5 mole percent or from about 5 mole percent to about 50 mole percent) of lithium; 28 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 (V-d) flowing a gas into the heating chamber at least partially during step (c), wherein the gas comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof; and (V-f) cleaning the substrate prior to step (a).

[0161] IV. METHODS OF FORMING A SINTERED SOLID-STATE ELECTROLYTE MATERIAL

[0162] Another aspect of the present invention provides a method of forming a sintered solid- state electrolyte material. With reference to FIG.6, a flow chart depicting an exemplary implementation of forming a sintered solid-state electrolyte material is provided. The method comprises (aa) disposing a setter body in a heating chamber, wherein the setter body comprises a substrate having a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, wherein the substrate comprises nickel, and a coating at least partially disposed on the first surface of the substrate, wherein the coating comprises at least about 1 mole percent (e.g., at least about 5 mole percent or from about 5 mole percent to about 50 mole percent) of lithium, and wherein the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate (6002); (bb) disposing a green body on the coating of the setter body, wherein the green body comprises a solid-state electrolyte material (6004); and (cc) heating the heating chamber to a temperature of from about 600 °C to about 1,500 °C to form the sintered solid-state electrolyte (6006), wherein the solid-state electrolyte material loses less than about 20 mole percent of lithium during step (cc).

[0163] The setter body may be any setter body described herein. In some implementations, step (aa) comprises disposing a plurality of setter bodies in a heating chamber. And, in some implementations, the plurality of setter bodies may be arranged as a stack of setter bodies in the heating chamber.

[0164] In some implementations, the green body is a tape or a film. The green body may comprise any suitable solid-state electrolyte material for use in a solid-state battery cell. For 29 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 example, in some implementations, the solid-state electrolyte material may comprise a garnet material. Non-limiting examples of garnet materials include lithium garnet materials, doped lithium garnet materials, lithium garnet composite materials, and combinations thereof. Non- limiting examples of lithium garnet materials include Li3-phase lithium garnet solid-state electrolyte materials (e.g., Li3M1Te2O12, where M1is a lanthanide such as Y, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Zr, Ta, or a combination thereof and Li3+xNd3Te2-xO12, where x is 0.05 to 1.5; Li5-phase lithium garnet solid-state electrolyte materials (e.g., Li5La3M22O12, where M2is Nb, Zr, Ta, Sb, or a combination thereof, cation-substituted Li 2 5La3M 2O12 such as, for example, Li M1La M2 O , where M1is Mg, Ca, Sr, B 2 6 3 2 12 a, or combinations thereof, and Li7La3M2O12, where M2is Zr, Sn, or a combination thereof); Li6-phase lithium garnet solid-state electrolyte materials (e.g., Li6M1La 2 2M 2O12, where M1is Mg, Ca, Sr, Ba, or a combination thereof and M2is Nb, Ta, or a combination thereof); cation-doped Li6La2BaTa2O12; cation-doped Li6BaY2M22O12, where M2is Nb, Ta, or a combination thereof and the cation dopants are barium, yttrium, zinc, or combinations thereof, an Li7-phase lithium garnet solid-state electrolyte material (e.g., cubic Li7La3Zr2O12 and Li7Y3Zr2O12); cation-doped Li7La3Zr2O12; Li5+2xLa3, Ta2-xO2, where x is 0.1 to 1, Li6.8(La2.95,Ca0.5)(Zr1.75,Nb0.25)O12(LLCZN), Li6.4Y3Zr1.4Ta0.6O12, Li6.5La2.5Ba0.5TaZrO12, Li6BaY2M12O12, Li7Y3Zr2O12, Li6.75BaLa2Nb1.75Zn0.25O12, or Li6.75BaLa2Ta1.75Zn0.25O12), lithium garnet composite materials (e.g., lithium garnet-conductive carbon matrix or composites with other materials). Other examples of lithium-ion-conducting solid-state electrolyte materials include cubic garnet-type materials such as 3 mol % YSZ-doped Li7.6La3Zr1.94Y0.06O12 and 8 mol % YSZ-doped Li7.16La3Zr1.94Y0.06O12. Additional examples of suitable lithium garnet solid-state electrolyte materials include, but are not limited to, Li5La3Nb2O12, Li5La3Ta2O12, Li7La3Zr2O12, Li6La2SrNb2O12, Li6La2BaNb2O12, Li6La2SrTa2O12, Li6La2BaTa2O12, Li7Y3Zr2O12, Li6.4Y3Zr1.4Ta0.6O12, Li6.5La2.5Ba0.5TaZrO12, Li7Y3Zr2O12, Li6.75BaLa2Nb1.75Zn0.25O12, or Li6.75BaLa2Ta1.75Zn0.25O12. In some embodiments, the garnet material is, for example, Li7-xLa3-yM1yZr2-zM2zO12, wherein x greater than 0 and less than 2, M1is chosen from Ba, Ca, Y, and combinations thereof, and M2is chosen from Nb, Ta, and combinations thereof. In some embodiments, the garnet material is Li6.75La3Zr1.75Ta0.25O12 (LLZT), Li6.75La2.75Zr1.75Ca0.25Nb0.25O12 (LLZCN), Li5La3Nb2O12 (LLZNO), Li7La3Zr2O12 (LLZ), Li5La3Ta2O12, Li6La2SrNb2O12, Li6La2BaNb2O12, Li6La2SrTa2O12, Li6La2BaTa2O12, 30 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 Li Y Zr O , Li Y Zr Ta O , Li L 1 7 3 2 12 6.4 3 1.4 0.6 12 6.5 a2.5Ba0.5TaZrO12, Li6BaY2M 2O12, Li6.75BaLa2Nb1.75Zn0.25O12, Li6.75BaLa2Ta1.75Zn0.25O12, or any combination thereof.

[0165] In some embodiments, the garnet material comprises a composition of Formula (I): M17-xD1aM23-yD2bM32-zD3cO12-wD4d (I), wherein: M1 is Li; M2 is La; M3 is Zr; D1 is H, Be, B, Al, Fe, Zn, Ga, Ge, or any combination thereof; D2 is Na, K, Ca, Rb, Sr, Y, Ag, Ba, Bi, Pr, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Tm, Zn, Ce, or any combination thereof; D3 is Mg, Si, Sc, Ti, V, Cr, Mn, Co, Ni, Cu, Ge, As, Se, Nb, Mo, Tc, Ru, Rh, Pd, Cd, In, Sn, Sb, Hf, Ta, W, Ir, Pt, Au, Hg, Tl, Pb, Ce, Eu, Te, Y, Sr, Ca, Ba, Gd, Ge, or any combination thereof; D4 is F, Cl, Br, I, S, Se, Te, N, P, or any combination thereof; ( Q M Q )- &('+ . N Q *- ( Q O Q *- ( Q P Q )- ( Q : Q )- ( Q ; Q *- ( Q < Q )- :E= ( Q = Q )% wherein at least one of a, b, c, and d is not zero.

[0166] In some implementations, the green body comprises at least one of a pore forming agent and a binder. In some implementations, the green body comprises a pore forming agent. In other implementations, the green body comprises a binder. And, in some implementations, the green body comprises a binder and a pore forming agent. The binder and pore forming agents may be any binder and pore forming agents suitable for use in a solid-state electrolyte material for a battery cell. 31 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0167] In some implementations, the solid-state electrolyte material loses less than about 15 mole percent of lithium during step (cc). In other implementations, the solid-state electrolyte material loses less than about 10 mole percent of lithium during step (cc). And, in some implementations, the solid-state electrolyte material loses less than about 7.5 mole percent of lithium during step (cc).

[0168] In some implementations, step (cc) comprises heating the heating chamber to a temperature of from about 700 °C to about 1,500 °C (e.g., from about 700 °C to about 1,200 °C). In other implementations, step (cc) comprises heating the heating chamber to a temperature of from about 800 °C to about 1,500 °C (e.g., from about 800 °C to about 1,200 °C). In some implementations, step (cc) comprises heating the heating chamber to a temperature of from about 900 °C to about 1,500 °C (e.g., from about 900 °C to about 1,200 °C). And, in some implementations, step (cc) comprises heating the heating chamber to a temperature of from about 1,000 °C to about 1,500 °C (e.g., from about 1000 °C to about 1,200 °C).

[0169] In some implementations, the method further comprises (dd) flowing a gas into the heating chamber.

[0170] In some implementations, the gas comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof. In other implementations, the gas comprises a mixture of hydrogen and an inert gas (e.g., nitrogen). For example, the gas may comprise carbon monoxide. In some implementations, the gas comprises carbon dioxide. In some implementations, the gas comprises ammonia. In other implementations, the gas comprises hydrogen sulfide. In some implementations, the gas comprises methane. In some implementations, the gas comprises hydrogen. In other implementations, the gas comprises nitrogen. In some implementations, the gas comprises argon. And, in some implementations, the gas comprises helium.

[0171] In some implementations, the gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 3,000 SCCM. For example, the gas may be flowed into the heating chamber at a flow rate of from about 1,000 SCCM to about 3,000 SCCM. In other implementations, the gas is flowed into the heating chamber at a flow rate of from about 1,500 SCCM to about 2,500 SCCM. In some implementations, the gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 1,500 SCCM. And, in some 32 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 implementations, the gas is flowed into the heating chamber at a flow rate of from about 1,500 SCCM to about 3,000 SCCM.

[0172] In some implementations, step (dd) is performed at least partially during step (cc). In other implementations, an atmosphere inside the heating chamber during step (cc) comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof.

[0173] In some implementations, an atmospheric pressure inside the heating chamber during step (cc) is from about 1 Pa to about 10 Mpa. In other implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 1 MPa to about 10 Mpa. In some implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 1 Pa to about 1 Mpa. In some implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 1 MPa to about 2 Mpa. In some implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 2 MPa to about 3 Mpa. In other implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 3 MPa to about 4 Mpa. In some implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 4 MPa to about 5 Mpa. In some implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 5 MPa to about 6 Mpa. In other implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 6 MPa to about 7 Mpa. In some implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 7 MPa to about 8 Mpa. In some implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 8 MPa to about 9 Mpa. And, in some implementations, the atmospheric pressure inside the heating chamber during step (cc) is from about 9 MPa to about 10 Mpa.

[0174] In some implementations, when the green body further comprises at least one of the binder and the pore forming agent, step (cc) further comprises (cc-1) heating the heating chamber to a first temperature of from about 400 °C to about 800 °C to burnout the at least one of the pore forming agent and the binder; and (cc-2) heating the heating chamber to a second temperature of from about 600 °C to about 1,500 °C (e.g., from about 600 °C to about 1,200 °C) to form the sintered solid-state electrolyte, wherein the second temperature is greater than the first temperature. 33 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0175] In some implementations, step (cc-1) comprises heating the heating chamber to a temperature of from about 450 °C to about 750 °C. In other implementations, step (cc-1) comprises heating the heating chamber to a temperature of from about 500 °C to about 700 °C. And, in some implementations, step (cc-1) comprises heating the heating chamber to a temperature of from about 600 °C to about 700 °C.

[0176] In some implementations, step (cc-2) comprises heating the heating chamber to a temperature of from about 700 °C to about 1,500 °C (e.g., from about 700 °C to about 1,200 °C). In other implementations, step (cc-2) comprises heating the heating chamber to a temperature of from about 800 °C to about 1,500 °C (e.g., from about 800 °C to about 1,200 °C). In some implementations, step (cc-2) comprises heating the heating chamber to a temperature of from about 900 °C to about 1,500 °C (e.g., from about 900 °C to about 1,200 °C). And, in some implementations, step (cc-2) comprises heating the heating chamber to a temperature of from about 1,000 °C to about 1,200 °C (e.g., from about 1000 °C to about 1,200 °C).

[0177] In some implementations, when step (cc) comprises steps (cc-1) and (cc-2), the method may further comprise (dd-1) flowing a first gas into the heating chamber at least partially during step (cc-1); and (dd-2) flowing a second gas into the heating chamber at least partially during step (cc-2).

[0178] In some implementations, the first gas of step (dd-1) is selected from oxygen, dry air, or air.

[0179] In some implementations, the second gas of step (dd-2) is selected from carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof. In other implementations, the second gas comprises a mixture of hydrogen and an inert gas (e.g., nitrogen). In some implementations, the second gas comprises carbon monoxide. In some implementations, the second gas comprises carbon dioxide. In some implementations, the second gas comprises ammonia. In other implementations, the second gas comprises hydrogen sulfide. In some implementations, the second gas comprises methane. In some implementations, the second gas comprises hydrogen. In other implementations, the second gas comprises nitrogen. In some implementations, the second gas comprises argon. And, in some implementations, the second gas comprises helium. 34 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0180] In some implementations, the first gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 3,000 SCCM. For example, the first gas may be flowed into the heating chamber at a flow rate of from about 1,000 SCCM to about 3,000 SCCM. In other implementations, the first gas is flowed into the heating chamber at a flow rate of from about 1,500 SCCM to about 2,500 SCCM. In some implementations, the first gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 1,500 SCCM. And, in some implementations, the first gas is flowed into the heating chamber at a flow rate of from about 1,500 SCCM to about 3,000 SCCM.

[0181] In some implementations, the second gas comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof. In other implementations, the second gas comprises a mixture of hydrogen and an inert gas (e.g., nitrogen). For example, the second gas may comprise carbon monoxide. In some implementations, the second gas comprises carbon dioxide. In some implementations, the second gas comprises ammonia. In other implementations, the second gas comprises hydrogen sulfide. In some implementations, the second gas comprises methane. In some implementations, the second gas comprises hydrogen. In other implementations, the second gas comprises nitrogen. In some implementations, the second gas comprises argon. And, in some implementations, the second gas comprises helium.

[0182] In some implementations, the second gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 3,000 SCCM. For example, the second gas may be flowed into the heating chamber at a flow rate of from about 1,000 SCCM to about 3,000 SCCM. In other implementations, the second gas is flowed into the heating chamber at a flow rate of from about 1,500 SCCM to about 2,500 SCCM. In some implementations, the second gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 1,500 SCCM. And, in some implementations, the second gas is flowed into the heating chamber at a flow rate of from about 1,500 SCCM to about 3,000 SCCM.

[0183] In some implementations, the method further comprises (ee) cooling the heating chamber after step (cc).

[0184] For example, the method may comprise cooling the heating chamber to about room temperature after step (cc). In other implementations, the method may comprise cooling the 35 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 heating chamber to less than about 100 °C after step (cc). And, in some implementations, the method may comprise cooling the heating chamber to less than about 50 °C after step (cc).

[0185] In another aspect, the present invention provides a method of forming a sintered solid- state electrolyte material. The method comprises (I-aa) disposing a setter body in a heating chamber, wherein the setter body comprises a substrate having a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, wherein the substrate comprises nickel, and a coating at least partially disposed on the first surface of the substrate, wherein the coating comprises at least about 1 wt% of lithium based on the total weight of the coating, and wherein the wt% percent of lithium in the coating is greater than a wt% percent of lithium in the substrate; (I-bb) disposing a green body on the coating of the setter body, wherein the green body comprises a solid-state electrolyte material; and (I-cc) heating the heating chamber to a temperature of from about 600 °C to about 1,200 °C to form the sintered solid-state electrolyte, wherein the solid-state electrolyte material loses less than about 20 mole percent of lithium during step (I-cc).

[0186] In a further aspect, the present invention provides a method of forming a sintered solid- state electrolyte material. The method comprises (II-aa) disposing a setter body in a heating chamber, wherein the setter body comprises a substrate having a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, wherein the substrate comprises nickel, and a coating at least partially disposed on the first surface of the substrate, wherein the coating comprises at least about 1 mole percent of lithium, and wherein the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate; (II-bb) disposing a green body on the coating of the setter body, wherein the green body comprises a solid-state electrolyte material and at least one of a pore forming agent and a binder; 36 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 (II-cc-1) heating the heating chamber to a first temperature of from about 400 °C to about 800 °C to burnout at least one of the pore forming agent and the binder; and (II-cc-2) heating the heating chamber to a second temperature of from about 600 °C to about 1,500 °C to form the sintered solid-state electrolyte, wherein the second temperature is greater than the first temperature, wherein the solid-state electrolyte material loses less than about 20 mole percent of lithium during steps (II-cc-1) and (II-cc-2).

[0187] In yet another aspect, the present invention provides a method of forming a sintered solid-state electrolyte material. The method comprises (III-aa) disposing a setter body in a heating chamber, wherein the setter body comprises a substrate having a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, wherein the substrate comprises nickel, and a coating at least partially disposed on the first surface of the substrate, wherein the coating comprises at least about 1 mole percent of lithium, and wherein the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate; (III-bb) disposing a green body on the coating of the setter body, wherein the green body comprises a solid-state electrolyte material and at least one of a pore forming agent and a binder; (III-cc-1) heating the heating chamber to a first temperature of from about 400 °C to about 800 °C to burnout at least one of the pore forming agent and the binder; (III-cc-2) heating the heating chamber to a second temperature of from about 600 °C to about 1,500 °C to form the sintered solid-state electrolyte, wherein the second temperature is greater than the first temperature; (III-dd-1) flowing a first gas into the heating chamber at least partially during step (cc-1); and (III-dd-2) flowing a second gas into the heating chamber at least partially during step (cc-2), 37 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 wherein the solid-state electrolyte material loses less than about 20 mole percent of lithium during steps (III-cc-1) and (III-cc-2).

[0188] V. EXAMPLES

[0189] In order that the invention described herein may be more fully understood, the following examples are set forth. The examples described in this application are offered to illustrate the methods and setter bodies provided herein and are not to be construed in any way as limiting their scope.

[0190] Example 1: Setter Bodies for Sintering a Solid-State Electrolyte Material

[0191] Two (2) size 100 x 100 nickel-mesh substrates with an area of 8 cm by 11 cm and areal density of 0.13 g / cm2from Belleville Wire Cloth Company (200-grade, > 99% pure Ni, Si < 0.35%, Fe < 0.40%, Ti < 0.01%, Co < 0.01%, Mg < 0.004%) (i.e., the first and second substrates) were cleaned in isopropanol via ultrasonication for 5 minutes. FIGS.7A and 7B present images of representative portions of the first and second nickel-mesh substrates before (FIG.7A) and after (FIG.7B) cleaning. The image in FIG.7A was obtained at a magnification of 1600x, using the following microscope settings / parameters and a background scatter detector: ^ FW (field width) = 374 µm ^ HV = 15 kV, ^ Int. = Map ^ WD (working distance) 4.833 mm, and ^ Pressure = 0.10 Pa. The image in FIG.7B was obtained at a magnification of 1000x, using the following microscope settings / parameters and a background scatter detector: ^ FW (field width) = 519 µm ^ HV = 15 kV, ^ Int. = Map ^ WD (working distance) 6.072 mm, and ^ Pressure = 0.10 Pa.

[0192] Referring to FIG.8, the first substrate 802a was placed on a first nickel plate 812a having a thickness of 1.56 mm (McMaster 200-grade, > 99% pure Ni), and a powder bed 814 of undoped LLZO (18 g) was spread evenly across the first substrate on top of the first nickel plate 812a. The second substrate 802b was placed on top of the powder bed. A second nickel plate 38 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 812b was placed on top of the second substrate 802b. The resultant stack was heated at 1,100 °C for 2 hours (ramped from room temperature at 3 °C / min in forming gas, pO2 < 10-23atm with a flow rate of 2,000 SCCM). The forming gas used was 0.4% H2in Ar.

[0193] Setter Bodies – Nickel-mesh substrates

[0194] The resultant first and second setter bodies, generated from the cleaned nickel-mesh substrates, were removed from the stack and ultrasonically cleaned in water for 5 minutes prior to use. FIG.9 presents an image of a portion of the nickel-mesh setter body formed from the substrate of FIGS.7A and 7B. The image in FIG.9 was obtained at a magnification of 1600x, using the following microscope settings / parameters and a background scatter detector: ^ FW (field width) = 374 µm ^ HV = 15 kV, ^ Int. = Map ^ WD (working distance) 4.860 mm, and ^ Pressure = 0.10 Pa. The nickel-mesh setter body includes a plurality of nodules extending away from surfaces of the substrate. It was determined with SEM-EDX that the nodules comprised aluminum, silicon, magnesium, calcium, and / or oxygen.

[0195] Setter Bodies – Nickel plate substrates

[0196] One of the resultant nickel plate setter bodies formed from nickel plates 812a and 812b underwent XPS analysis.

[0197] XPS Analysis Methods

[0198] The nickel plate setter body underwent a survey scan followed by a depth profile / high- resolution scan of detected species at depths of 0 nm, 50 nm, 100 nm, and 150 nm with respect to SiO2sputter rate using the following parameters.

[0199] Acquisition Parameters: ^ Dual-beam charge neutralization consisting of electrons and low energy argon ions for all scans; ^ Monochromatic Al KS (1486.6 eV), operated using a 50 W, 200 µm x-ray beam rastering a single point at the center of the sputter crater during depth-profiling; ^ Survey scans: 45° photoelectron takeoff angle, 280 eV analyzer pass energy, 1.0 eV / step; 39 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 ^ High-resolution scans: 45° photoelectron takeoff angle, variable analyzer pass energy and eV step size to maximize analytical signal; and ^ Energy scale of high-resolution spectra was referenced to the C 1s peak position of the carbonate bond at 290.1 eV.

[0200] Depth Profile Sputter Parameters: ^ 4 keV Ar+beam energy, 1 µA beam current, 3 mm x 3 mm raster area at 16.7 min intervals for a total of 50 minutes; and ^ Sputter rate of 100-nm SiO2reference sample: 3.6 nm / min.

[0201] Referring to FIG.10, the XPS analysis detected an absence of nickel at the immediate surface of the setter body, and the scanned surface was almost entirely (or entirely) coated with an oxidized form lithium. The oxygen signals from the XPS scans indicate that the coating comprises Li2CO3with traces of Li2O at the surface. The carbon signal also supports this finding.

[0202] The surface of the setter body was sputtered for a pre-determined interval at an estimated depth of ~160 nm. At this first depth, metallic nickel was detected and no oxidized form of nickel was detected. At increasing depths, the concentration of nickel increases while the total concentration of lithium remains relatively consistent with depth, indicating some penetration of oxidized lithium into the nickel substrate. LiOH, Li2O, and Li2CO3, were all detected under the surface.

[0203] Example 2: Sintering a Solid-State Electrolyte Material

[0204] With reference to FIG.11, a setter body, coated and formed according to Example 1, having a nickel plate substrate 1012 was placed in a furnace and a green body bilayer tape 1016 (8 cm by 11 cm) was placed on the setter body. The green body bilayer tape was comprised of a doped LLZO. The tape further comprised a porous layer 1018 (40 µm thick) including a pore forming agent and a dense layer 1020 comprising excess lithium (i.e., 15% lithium in excess of stoichiometric from Li2CO3). The porous layer was placed in contact with the setter body 1012. One of the setter bodies having a nickel-mesh substrate 1000 from Example 1 was placed on top of the bilayer tape in contact with the dense layer. The resultant stack was heated at 0.4 °C / min from room temperature to 580 °C in UHP O2 and held for 30 minutes at 2,000 SCCM to burnout the binder and the pore forming agent. While maintaining that temperature, argon flowed for 30 minutes through the furnace at 2,000 SCCM. Subsequently, forming gas was flowed for 30 40 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 minutes through the furnace at 2,000 SCCM while maintaining the temperature. The furnace temperature was increased from 580 °C to 725 °C at 1 °C / min and then held for 1 hour. The furnace temperature was then increased at 3 °C / min to 1,100 °C for 2 hours. Finally, the furnace was cooled down at 3 °C / min. For all steps after the debinding step, the pO -23 2 was less than 10 atm. The resulting product was a sintered bilayer solid state electrolyte material comprising a porous layer and a dense layer.

[0205] Referring to FIGS.12A-12D, setter body 1012 and setter body 1000 were recovered and reused in ten (10) additional sintering processes consistent with those set forth above to create sintered, bilayer, solid state electrolyte materials demonstrating that the setter bodies are resilient to (and recyclable for) high temperature sintering processes for LLZO solid state electrolyte materials. The microscope image in FIG.12B was obtained at a magnification of 2500x, using the following microscope settings / parameters and a background scatter detector: ^ FW (field width) = 239 µm ^ HV = 15 kV, ^ Int. = Image ^ WD (working distance) 6.560 mm, and ^ Pressure = 0.10 Pa.

[0206] The microscope image in FIG.12C was obtained at a magnification of 2500x, using the following microscope settings / parameters and a background scatter detector: ^ FW (field width) = 239 µm ^ HV = 15 kV, ^ Int. = Image ^ WD (working distance) 7.057 mm, and Pressure = 0.10 Pa.

[0207] The microscope image in FIG.12D was obtained at a magnification of 2500x, using the following microscope settings / parameters and a background scatter detector: ^ FW (field width) = 239 µm ^ HV = 15 kV, ^ Int. = Image ^ WD (working distance) 6.922 mm, and ^ Pressure = 0.10 Pa. 41 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280

[0208] As shown in FIGs 12A-12D, these coated nickel setter bodies can be used (and / or re- used) in at least 11 sintering processes to generate LLZO solid state electrolyte materials without the requirement of adding excess lithium in the sintering process and without significant lithium depletion in the resulting sintered material.

[0209] Example 3: Setter Bodies for Sintering a Solid-State Electrolyte Material

[0210] Iron metal (99.5% purity) was used to test as setter body substrate. Undoped LLZO powder bed (12 g) was spread evenly across an iron plate with dimensions of 3.25” × 5.5” × 0.005”. The resultant stack was heated at 1,100 °C for 2 hours (ramped from room temperature at 3 °C / min in forming gas, pO2 < 10-23atm with a flow rate of 2,000 SCCM) to generate the coating and form the setter body. The cooled powder bed stuck substantially to the iron plate and the iron plate was discolored brown and black. The plate discoloration indicates oxidation on the plate surface, and powder adhesion to the plate indicates a reaction between the powder and the iron plate.

[0211] The setter body having a iron plate substrate was placed in a furnace and a green body bilayer tape (6 cm by 9 cm) was placed on the setter body as illustrated in FIG.11 and described in Example 1. The green body bilayer tape was comprised of a doped LLZO. The tape further comprised a porous layer (40 µm thick) including a pore forming agent and a dense layer comprising doped LLZO. The porous layer was placed in contact with the setter body. A setter body having a nickel-mesh substrate, generated according to the processes described in Example 1, was placed on top of the bilayer tape in contact with the dense layer. The resultant stack was heated at 0.4 °C / min from room temperature to 640 °C in dried air and held for 30 minutes at 2,000 SCCM to burnout the binder and the pore forming agent. While maintaining that temperature, argon flowed for 30 minutes through the furnace at 2,000 SCCM. Subsequently, forming gas was flowed for 30 minutes through the furnace at 2,000 SCCM while maintaining the temperature. The furnace temperature was then increased at 3 °C / min to 1,100 °C for 2 hours. Finally, the furnace was cooled down at 5 °C / min. For all steps after the binder-removal step, the pO2was less than 10-23atm. The resulting product was an under-sintered bilayer solid state electrolyte material comprising a porous layer and a dense layer. Referring to FIG.13A, the dense layer was not uniform in density and was substantially porous. Additionally, iron was detected in the dense layer by SEM-EDX analysis, as shown in FIG.13B. This Example 3 42 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 demonstrates that the iron in the setter body interacted with LLZO solid-state electrolyte material. Therefore, iron was not a suitable setter substrate for sintering the LLZO material.

[0212] The microscope image in FIG.13A was obtained at a magnification of 2500x, using the following microscope settings / parameters and a background scatter detector: ^ FW (field width) = 239 µm ^ HV = 15 kV, ^ Int. = Image ^ WD (working distance) 6.589 mm, and ^ Pressure = 0.10 Pa.

[0213] Example 4: Invar Alloy Setter Bodies for Sintering a Solid-State Electrolyte Material

[0214] Invar alloy composed of 64 wt% iron and 36 wt% nickel was used to test as setter body substrate. An undoped LLZO powder bed (12 g) was spread evenly across the Invar alloy plate 3.25” × 5.5” × 0.005”. The resultant stack was heated at 1,100 °C for 2 hours (ramped from room temperature at 3 °C / min in forming gas, pO2< 10-23atm with a flow rate of 2,000 SCCM) to generate the coating and form a coated setter body. A portion of the powder bed adhered to the Monel 400 plate but was easily removed. The plate retained a substantially metallic color.

[0215] The setter body having an Invar alloy plate substrate was placed in a furnace and a green body bilayer tape (6 cm by 9 cm) was placed on the setter body as illustrated in FIG.11 and described in Example 1. The green body bilayer tape was comprised of a doped LLZO. The tape further comprised a porous layer (40 µm thick) including a pore forming agent and a dense layer comprising doped LLZO. The porous layer was placed in contact with the setter body. A setter body having a nickel-mesh substrate, generated according to the processes described in Example 1, was placed on top of the bilayer tape in contact with the dense layer. The resultant stack was heated at 0.4 °C / min from room temperature to 640 °C in dried air and held for 30 minutes at 2,000 SCCM to burnout the binder and the pore forming agent. While maintaining that temperature, argon flowed for 30 minutes through the furnace at 2,000 SCCM. Subsequently, forming gas was flowed for 30 minutes through the furnace at 2,000 SCCM while maintaining the temperature. The furnace temperature was then increased at 3 °C / min to 1,100 °C for 2 hours. Finally, the furnace was cooled down at 5 °C / min. For all steps after the binder- removal step, the pO2was less than 10-23atm. The resulting product was a sintered LLZO 43 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 bilayer solid state electrolyte material comprising a porous layer and a dense layer. The dense layer was sufficiently densified. The sintered bilayer was discolored light brown in some areas. However, iron was detected in the dense layer by SEM-EDX analysis. No copper was detected in the SEM-EDX analysis. The example demonstrates that the 64 wt% iron in the setter body interacted with the solid-state electrolyte material. Therefore, Invar was not a suitable setter substrate for sintering the LLZO material.

[0216] Example 5: Monel Alloy Setter Bodies for Sintering a Solid-State Electrolyte Material

[0217] Monel 400 alloy (65 wt% nickel, 33 wt% copper, and 2 wt% iron) was used to test as setter body substrate. Undoped LLZO powder bed (12 g) was spread evenly across the Monel 400 plate (3.25” × 5.5” × 0.005”). The resultant stack was heated at 1,100 °C for 2 hours (ramped from room temperature at 3 °C / min in forming gas, pO2 < 10-23atm with a flow rate of 2,000 SCCM) to generate the coating and form the setter body. A portion of the powder bed adhered to the Monel 400 plate but was easily removed. The plate retained a substantially metallic color.

[0218] The setter body having a Monel 400 alloy plate substrate was placed in a furnace and a green body bilayer tape (6 cm by 9 cm) was placed on the setter body as illustrated in FIG.11 and described in Example 1. The green body bilayer tape was comprised doped LLZO. The tape further comprised a porous layer (40 µm thick) including a pore forming agent and a dense layer comprising doped LLZO. The porous layer was placed in contact with the setter body. One of the setter bodies having a nickel-mesh substrate, generated according to the processes described in Example 1, was placed on top of the bilayer tape in contact with the dense layer. The resultant stack was heated at 0.4 °C / min from room temperature to 640 °C in dried air and held for 30 minutes at 2,000 SCCM to burnout the binder and the pore forming agent. While maintaining that temperature, argon flowed for 30 minutes through the furnace at 2,000 SCCM. Subsequently, forming gas was flowed for 30 minutes through the furnace at 2,000 SCCM while maintaining the temperature. The furnace temperature was then increased at 3 °C / min to 1,100 °C for 2 hours. Finally, the furnace was cooled down at 5 °C / min. For all steps after the binder- removal step, the pO2 was less than 10-23atm. The resulting product was a sintered bilayer solid state electrolyte material comprising a porous layer and a dense layer. The dense layer was sufficiently densified. No iron, copper, or nickel was detected in the dense layer by SEM-EDX 44 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 analysis. The example demonstrates that the 2 wt% iron and 33 wt% copper in the setter body did not substantially interact with the solid-state electrolyte material. Therefore, Monel 400 was a suitable setter substrate.

[0219] Example 6: Uncoated Setter Bodies for Sintering a Solid-State Electrolyte Material

[0220] To demonstrate the importance of the setter body coating, an uncoated nickel plate and uncoated nickel mesh were used to sinter a solid-state electrolyte material. The as-received nickel plate was placed in a furnace and a green body bilayer tape (6 cm by 9 cm) was placed on the plate. The green body bilayer tape was comprised of a doped LLZO. The tape further comprised a porous layer (40 µm thick) including a pore forming agent and a dense layer comprising doped LLZO. The porous layer was placed in contact with the plate. An as-received nickel-mesh was placed on top of the bilayer tape in contact with the dense layer. The resultant stack was heated at 0.4 °C / min from room temperature to 640 °C in dried air and held for 30 minutes at 2,000 SCCM to burnout the binder and the pore forming agent. While maintaining that temperature, argon flowed for 30 minutes through the furnace at 2,000 SCCM. Subsequently, forming gas was flowed for 30 minutes through the furnace at 2,000 SCCM while maintaining the temperature. The furnace temperature was then increased at 3 °C / min to 1,100 °C for 2 hours. Finally, the furnace was cooled down at 5 °C / min. For all steps after the binder- removal step, the pO2 was less than 10-23atm. The resulting product was a poorly-sintered bilayer solid state electrolyte material comprising a porous layer and a dense layer, as shown in FIG.14.

[0221] The microscope image in FIG.14 was obtained at a magnification of 2500x, using the following microscope settings / parameters and a background scatter detector: ^ FW (field width) = 208 µm ^ HV = 15 kV, ^ Int. = Image ^ WD (working distance) 4.900 mm, and ^ Pressure = 0.10 Pa.

[0222] The resulting bilayer solid state electrolyte, sintered using an uncoated Ni plate, was significantly deficient in lithium, as determined by ICP-OES, by 14%. The resulting sintered bilayer solid state electrolyte from Example 3 using the coated setter body was measured for lithium content by ICP-OES and was not measurably deficient (0-1%). 45 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 EQUIVALENTS AND SCOPE

[0223] In the claims articles such as "a," "an," and "the" may mean one or more than one unless indicated to the contrary or otherwise evident from the context. Claims or descriptions that include "or" between one or more members of a group are considered satisfied if one, more than one, or all of the group members are present in, employed in, or otherwise relevant to a given product or process unless indicated to the contrary or otherwise evident from the context. The invention includes embodiments in which exactly one member of the group is present in, employed in, or otherwise relevant to a given product or process. The invention includes embodiments in which more than one, or all of the group members are present in, employed in, or otherwise relevant to a given product or process.

[0224] Furthermore, the invention encompasses all variations, combinations, and permutations in which one or more limitations, elements, clauses, and descriptive terms from one or more of the listed claims is introduced into another claim. For example, any claim that is dependent on another claim can be modified to include one or more limitations found in any other claim that is dependent on the same base claim. Where elements are presented as lists, e.g., in Markush group format, each subgroup of the elements is also disclosed, and any element(s) can be removed from the group. It should it be understood that, in general, where the invention, or aspects of the invention, is / are referred to as comprising particular elements and / or features, certain embodiments of the invention or aspects of the invention consist, or consist essentially of, such elements and / or features. For purposes of simplicity, those embodiments have not been specifically set forth in haec verba herein. It is also noted that the terms "comprising" and "containing" are intended to be open and permits the inclusion of additional elements or steps. Where ranges are given, endpoints are included. Furthermore, unless otherwise indicated or otherwise evident from the context and understanding of one of ordinary skill in the art, values that are expressed as ranges can assume any specific value or sub–range within the stated ranges in different embodiments of the invention, to the tenth of the unit of the lower limit of the range, unless the context clearly dictates otherwise.

[0225] This application refers to certain issued patents, published patent applications, journal articles, and other publications, all of which are incorporated herein by reference. If there is a conflict between any of the incorporated references and the instant specification, the specification shall control. In addition, any particular embodiment of the present invention that 46 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 falls within the prior art may be explicitly excluded from any one or more of the claims. Because such embodiments are deemed to be known to one of ordinary skill in the art, they may be excluded even if the exclusion is not set forth explicitly herein. Any particular embodiment of the invention can be excluded from any claim, for any reason, whether or not related to the existence of prior art.

[0226] Those skilled in the art will recognize or be able to ascertain using no more than routine experimentation many equivalents to the specific embodiments described herein. The scope of the present embodiments described herein is not intended to be limited to the above Description, but rather is as set forth in the appended claims. Those of ordinary skill in the art will appreciate that various changes and modifications to this description may be made without departing from the spirit or scope of the present invention, as defined in the following claims. 47 57098938.1

Claims

PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 WHAT IS CLAIMED IS:

1. A setter body for sintering a solid-state electrolyte material, the setter body comprising: a substrate having a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, wherein the substrate comprises nickel; and a coating at least partially disposed on the first surface of the substrate, wherein the coating comprises at least about 1 mole percent of lithium, and wherein the mole percent of lithium in the coating is greater than a mole percent of lithium in the substrate.

2. The substrate of claim 1, wherein the nickel of the substrate is elemental nickel, a nickel oxide, a nickel alloy, or any combination thereof.

3. The substrate of claim 2, wherein the substrate comprises elemental nickel.

4. The substrate of claim 2, wherein substrate comprises a nickel alloy.

5. The substrate of claim 4, wherein the nickel alloy comprises aluminum, iron, copper, molybdenum, chromium, titanium, cobalt, tungsten, or any combination thereof.

6. The substrate of any one of claims 1-5, wherein the substrate is a plate, a foam, or a mesh.

7. The substrate of claim 6, wherein the substrate is a plate.

8. The substrate of claim 7, wherein the plate has a thickness of from about 1 µm to about 10,000 µm.

9. The substrate of claim 7 or claim 8, wherein the plate has an apparent porosity of less than about 5%. 48 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 10. The substrate of claim 6, wherein the substrate is a foam.

11. The substrate of claim 10, wherein the foam has a thickness of from about 1 µm to about 5,000 µm.

12. The substrate of claim 10 or claim 11, wherein the foam has an apparent porosity of greater than about 5%.

13. The substrate of claim 12, wherein the foam has an apparent porosity of greater than about 50%.

14. The substrate of claim 6, wherein the substrate is a mesh.

15. The substrate of claim 14, wherein the mesh has a thickness of from about 1 µm to about 5,000 µm.

16. The substrate of claim 14 or claim 15, wherein the mesh has an apparent porosity of greater than about 5%.

17. The substrate of claim 16, wherein the mesh has an apparent porosity of greater than about 50%.

18. The substrate of any one of claims 1-17, wherein the substrate has a weight-to-area ratio of from about 0.01 g / cm2to about 14.0 g / cm2.

19. The substrate of any one of claims 1-18, wherein the substrate has a weight-to-area ratio of from about 0.1 g / cm2to about 0.5 g / cm2.

20. The substrate of any one of claims 1-19, wherein the substrate has a weight-to-area ratio of from about 0.1 g / cm2to about 0.2 g / cm2. 49 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 21. The substrate of any one of claims 1-20, wherein the coating has a thickness of from about 1 nm to about 100 µm.

22. The substrate of any one of claims 1-21, wherein the coating has a thickness of from about 1 nm to about 1 µm.

23. The substrate of any one of claims 1-22, wherein the coating comprises elemental lithium, lithium peroxide, lithium hydroxide, a lithium oxide, a lithium carbonate, a lithium alloy, or any combination thereof.

24. The substrate of any one of claims 1-23, wherein the coating comprises at least one nodule extending away from the first surface of the substrate.

25. The substrate of claim 24, wherein the at least one nodule comprises aluminum, silicon, magnesium, calcium, oxygen, or any combination thereof.

26. The substrate of any one of claims 1-25, wherein the substrate comprises less than about 0.5 mole percent of lithium.

27. The substrate of any one of claims 1-26, wherein the substrate is free of lithium.

28. The substrate of any one of claims 1-27, wherein the coating comprises at least about 5 mole percent of lithium.

29. The substrate of any one of claims 1-28, wherein the coating is at least partially disposed on at least one of the second and outer surfaces of the substrate.

30. A method of forming a setter body for sintering a solid-state electrolyte material, the method comprising: 50 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 (a) disposing a substrate in a heating chamber, wherein the substrate has a first surface, a second surface opposite the first surface, and an outer surface extending from the first surface to the second surface, and wherein the substrate comprises nickel; (b) providing a lithium source in the heating chamber; and (c) heating the heating chamber to a temperature of from about 600 °C to about 1,500 °C to form a coating comprising lithium from the lithium source at least partially on the first surface of the substrate, thereby forming the setter body.

31. The method of claim 30, wherein the nickel of the substrate is elemental nickel, a nickel oxide, a nickel alloy, or any combination thereof.

32. The method of claim 31, wherein the substrate comprises elemental nickel.

33. The method of claim 31, wherein substrate comprises a nickel alloy.

34. The method of claim 33, wherein the nickel alloy comprises aluminum, iron, copper, molybdenum, chromium, titanium, cobalt, tungsten, or any combination thereof.

35. The method of any one of claims 30-34, wherein the substrate is a plate, a foam, or a mesh.

36. The method of any one of claims 30-35, wherein the lithium source comprises lithium lanthanum zirconium oxide (LLZO).

37. The method of claim 36, wherein the LLZO is doped.

38. The method of claim 36, wherein the LLZO is undoped.

39. The method of any one of claims 30-38, wherein the substrate comprises less than about 0.5 mole percent of lithium. 51 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 40. The method of any one of claims 30-39, wherein the substrate is free of lithium.

41. The method of any one of claims 30-40, wherein the coating comprises at least about 1 mole percent of lithium.

42. The method of any one of claims 30-41, wherein the coating comprises at least about 5 mole percent of lithium.

43. The method of any one of claims 30-42, wherein the coating is at least partially disposed on at least one of the second and outer surfaces of the substrate.

44. The method of any one of claims 30-43, wherein the method further comprises (d) flowing a gas into the heating chamber.

45. The method of claim 44, wherein the gas comprises a mixture of hydrogen and an inert gas.

46. The method of claim 44 or claim 45, wherein the gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 3,000 SCCM.

47. The method of any one of claims 44-46, wherein step (d) is performed at least partially during step (c).

48. The method of any one of claims 30-47, wherein an atmosphere inside the heating chamber during step (c) comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof.

49. The method of any one of claims 30-48, wherein the method further comprises (e) repeating step (c). 52 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 50. The method of claim 49, wherein the lithium source is a first lithium source, and wherein the method further comprises (e-1) replacing the first lithium source in the heating chamber with a second lithium source after step (c); and (e-2) repeating step (c).

51. The method of claim 50, wherein the method further comprises cooling the heating chamber prior to step (e-1).

52. A method of forming a sintered solid-state electrolyte material, the method comprising: (dd) disposing a setter body of any one of claims 1-29 in a heating chamber; (ee) disposing a green body on the coating of the setter body, wherein the green body comprises a solid-state electrolyte material; (ff) heating the heating chamber to a temperature of from about 600 °C to about 1,500 °C to form the sintered solid-state electrolyte, wherein the solid-state electrolyte material loses less than about 20 mole percent of lithium during step (cc).

53. The method of claim 52, wherein the solid-state electrolyte material loses less than about 15 mole percent of lithium during step (cc).

54. The method of claim 52, wherein the solid-state electrolyte material loses less than about 10 mole percent of lithium during step (cc).

55. The method of any one of claims 52-54, wherein the method further comprises (gg) flowing a gas into the heating chamber.

56. The method of claim 55, wherein the gas comprises a mixture of hydrogen and an inert gas. 53 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 57. The method of claim 55 or claim 56, wherein the gas is flowed into the heating chamber at a flow rate of from about 1 SCCM to about 3,000 SCCM.

58. The method of any one of claims 55-57, wherein step (dd) is performed at least partially during step (cc).

59. The method of any one of claims 52-58, wherein an atmosphere inside the heating chamber during step (cc) comprises carbon monoxide, carbon dioxide, ammonia, hydrogen sulfide, methane, hydrogen, nitrogen, argon, helium, or any combination thereof.

60. The method of any one of claims 52-59, wherein an atmospheric pressure inside the heating chamber during step (cc) is from about 1 Pa to about 10 Mpa.

61. The method of claim 52, wherein the green body further comprises at least one of a pore forming agent and a binder, and wherein step (cc) further comprises (cc-1) heating the heating chamber to a first temperature of from about 400 °C to about 800 °C to burnout the at least one of the pore forming agent and the binder; and (cc-2) heating the heating chamber to a second temperature of from about 600 °C to about 1,500 °C to form the sintered solid-state electrolyte, wherein the second temperature is greater than the first temperature.

62. The method of claim 61, wherein the method further comprises (dd) flowing a gas into the heating chamber.

63. The method of claim 62, wherein step (dd) further comprises (dd-1) flowing a first gas into the heating chamber at least partially during step (cc-1); and (dd-2) flowing a second gas into the heating chamber at least partially during step (cc-2).

64. The method of claim 63, wherein the first and second gases are each independently flowed into the heating chamber at a flow rate of from about 1 SCCM to about 3,000 SCCM. 54 57098938.1PCT Application Attorney Docket No.273679 / ISS-025WO / 551280 65. The method of claim 63 or claim 64, wherein the first gas comprises oxygen or air, and wherein the second gas comprises a mixture of hydrogen and an inert gas. 55 57098938.1

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