Bonding layer for solid-state batteries

Abstract

Set forth herein are electrochemical cells which include a negative electrode current collector, a lithium metal negative electrode, lithium-stuffed garnet solid-state electrolyte separator, a bonding agent layer, a positive electrode, and a positive electrode current collector. The bonding agent layer is between the lithium-stuffed garnet solid-state electrolyte separator and the positive electrode. The bonding agent layer advantageously lowers the interfacial impedance between a lithium-stuffed garnet solid-state electrolyte separator and a positive electrode and also optionally acts as an adhesive between the electrolyte separator and the positive electrode.

Description

Attorney Docket No.114826.00834 415.601 BONDING LAYER FOR SOLID-STATE BATTERIES CROSS-REFERENCE TO RELATED APPLICATIONS

[0001] This application claims the benefit of priority to U.S. Provisional ApplicationNo.63 / 671,447, filed July 15, 2024, the entire contents of which are herein incorporated by reference in their entirety for all purposes. FIELD

[0002] The present disclosure concerns solid-state rechargeable batteries.BACKGROUND

[0003] When a lithium metal negative electrode charges and discharges, it expandsand contracts as lithium strips and plates at the negative electrode. This expansion and contraction can lead to delamination of a solid electrolyte separator from a positive electrode. This results in an increase in interfacial impedance.

[0004] When, for example, a solid separator such as a lithium-stuffed garnetelectrolyte monolith contacts a positive electrode, there may be interfacial impedance between the solid electrolyte and the positive electrode due to poor wetting of the positive electrode, or its catholyte, onto the solid electrolyte surface, low ion-conductivity in either the separator or the electrode, or chemical reactions between the positive electrode and the solid electrolyte which produce side products detrimental to electrochemical performance. To address some of these challenges, certain researchers have attempted to combine liquid and gel electrolytes with lithium-stuffed garnets. See, for example, K. Yoshima, et al., Journal of Power Sources, 302 (2016) 283-290. PCT / US2017 / 032749 filed May 15, 2017, entitled SOLID ELECTROLYTE SEPARATOR BONDING AGENT, PCT / US2017 / 057735 filed October 21, 2017, entitled ELECTROLYTE SEPARATORS INCLUDINIG LITHIUM BOROHYDRIDE AND COMPOSITE ELECTROLYTE SEPARATORS OF LITHIUM- STUFFED GARNET AND LITHIUM BOROHYDRIDE, and PCT / US2017 / 057739 filed October 20, 2017, entitled BOROHYDRIDE-SULFIDE INTERFACIAL LAYER IN ALL SOLID-STATE BATTERY, are incorporated by reference herein in its entirety for all purposes.

[0005] There is therefore a need for improved materials and processes for bondingelectrolyte separators to positive electrodes. What is needed are, for example, new bondingAttorney Docket No.114826.00834 415.601 agents for bonding a solid separator, e.g., a lithium-stuffed garnet separator, to a positive electrode in such a way that the bonding agent, the electrolyte, and the catholyte conduct Li+ions. What is also needed in the relevant field are materials which bond, adhere, or maintain direct contact between, a solid separator and a positive electrode and also lower the interface resistance (measured as impedance and characterized by an Area-specific Resistance). The instant disclosure sets forth such materials and methods, in addition to making and using such materials and processes, and other solutions to problems in the relevant field. SUMMARY

[0006] In an embodiment, the instant disclosure sets forth a solid bonding layercomposition that includes a lithium salt, wherein the lithium salt is LiI, LiBr, LiCl, or combinations thereof, an alcohol, wherein the alcohol is methanol, isopropanol, or combinations thereof, wherein the lithium salt is present at 1 M to 5 M concentration, wherein the composition is solid.

[0007] In an embodiment, the instant disclosure sets forth a lithium salt, wherein thelithium salt is LiI, LiBr, LiCl, or combinations thereof; an organic solubilizer, wherein the solubilizer is 1,3-dioxolate (DOL), dimethoxyethane (DME), or combinations thereof, wherein the lithium salt is present at 1 M to 5 M concentration, and wherein the composition is solid.

[0008] In an embodiment, the instant disclosure sets forth a solid-state batteryincluding a positive electrode layer comprising a cathode active material and a catholyte material; a solid bonding layer, wherein the bonding layer includes a composition including lithium salt and an alcohol, wherein the lithium salt is present at 1 M – 5 M concentration; and an electrolyte separator comprising a lithium-stuffed garnet; wherein the bonding layer is in contact with the positive electrode layer and the electrolyte separator; wherein the lithium salt is LiI, LiBr, LiCl, or combinations thereof; wherein the alcohol is methanol, isopropanol, or combinations thereof.

[0009] In an embodiment, the instant disclosure sets forth a solid-state batteryincluding a positive electrode layer comprising a cathode active material and a catholyte material; a bonding layer, wherein the bonding layer includes a composition including a lithium salt and an organic solubilizer, wherein the solubilizer is 1,3-dioxolane (DOL), dimethoxyethane (DME), or combinations thereof; and an electrolyte separator comprising aAttorney Docket No.114826.00834 415.601 lithium-stuffed garnet; wherein the bonding layer is in contact with the solid-state buffer layer and the electrolyte separator.

[0010] In an embodiment, the instant disclosure sets forth a process for making abonding layer, the process including mixing dried LiI, LiBr, or a combination thereof, with an alcohol, wherein the alcohol is selected from methanol, isopropanol, or a combination thereof, wherein the lithium salt is present at 1 M to 5 M concentration, wherein after mixing, the composition is a solid at standard atmospheric pressure and room temperature.

[0011] In an embodiment, the instant disclosure sets forth an electrochemical stackwhich includes a lithium metal (Li) negative electrode, a positive electrode, an electrolyte separator in direct contact with the Li metal negative electrode, and a solid bonding layer comprising a lithium salt and an alcohol selected from methanol, isopropanol, or combinations thereof, wherein the lithium salt is present at 1 M to 5 M concentration.

[0012] In an embodiment, the bonding layer directly contacts, and is positionedbetween, the electrolyte separator and the positive electrode, and the electrolyte separator protects the Li metal negative electrode from exposure to the bonding layer. As described herein, in some examples, the bonding layer lowers the interfacial impedance at the interface between the electrolyte separator and the positive electrode when compared to the electrolyte separator in direct physical contact with the positive electrode. In some examples, the bonding layer lowers the interfacial impedance at the interface between the electrolyte membrane and the positive electrode by a factor of at least 10, at least 100, or at least 1000 with respect to the interfacial impedance at the interface between the electrolyte membrane and the positive electrode when a bonding layer is not positioned between, the electrolyte membrane and the positive electrode. BRIEF DESCRIPTIONS OF THE DRAWINGS

[0013] FIG. 1 is a differential scanning calorimetry (DSC) plot for LiI-4-isopropanol.

[0014] FIG. 2 is a differential scanning calorimetry (DSC) plot for LiI-4-isopropanolillustrating reversible melting with LSTPS.

[0015] FIGS. 3A-3C are photos of the LiBr-isopropanol (1:4) synthesis.

[0016] FIG. 4 is an x-ray diffraction (XRD) pattern of LSTPS after DOL or DMEtreatment.Attorney Docket No.114826.00834 415.601

[0017] FIG. 5 is a plot of electrochemical impedance spectroscopy (EIS) for LSTPSafter DOL or DME treatment. DETAILED DESCRIPTION Definitions

[0018] If a definition provided in any material incorporated by reference hereinconflicts with a definition provided herein, the definition provided herein controls.

[0019] As used herein, the term “about” when qualifying a number, e.g., about 15 %w / w, refers to the number qualified and optionally the numbers included in a range about that qualified number that includes ± 10% of the number. For example, about 15 % w / w includes 15 % w / w as well as 13.5 % w / w, 14 % w / w, 14.5 % w / w, 15.5 % w / w, 16 % w / w, or 16.5 % w / w. For example, “about 75 °C,” includes 75 °C as well 68 °C, 69 °C, 70 °C, 71 °C, 72 °C, 73 °C, 74 °C, 75 °C, 76 °C, 77 °C, 78 °C, 79 °C, 80 °C, 81 °C, 82 °C, or 83 °C.

[0020] As used herein, the phrase “active material,” refers to a material thatintercalates, or converts with, lithium in a reversible reaction such that the active material is suitable for use in a rechargeable battery. Active materials may include intercalation materials such as NCA or NMC. Active materials may include conversion chemistry materials such as FeF3. For example, active materials may include, but are not limited to, any active material set forth in US US20160211517A1, which published July 21, 2016, and istitled LITHIUM RICH NICKEL MANGANESE COBALT OXIDE.

[0021] As used herein the phrase “applying a pressure,” refers to a process wherebyan external device, e.g., a calender, induces a pressure in another material.

[0022] As used herein, the phrase “at least one member selected from the group,”includes a single member from the group, more than one member from the group, or a combination of members from the group. At least one member selected from the group consisting of A, B, and C includes, for example, A, only, B, only, or C, only, as well as A and B as well as A and C as well as B and C as well as A, B, and C or any other all combinations of A, B, and C.

[0023] As used herein “ASR” refers to area-specific resistance. ASR is measuredusing electrochemical impedance spectroscopy (EIS). EIS can be performed on a Biologic VMP3 instrument or an equivalent thereof. In an ASR measurement, lithium contacts areAttorney Docket No.114826.00834 415.601 deposited on two sides of a sample. An AC voltage of 25mV rms is applied across a frequency of 300kHz-0.1mHz while the current is measured. EIS partitions the ASR into the bulk contribution and the interfacial ASR contribution, by resolving two semicircles in a Nyquist plot. As used herein, the phrase “lithium interfacial resistance,” refers to the interfacial resistance of a material towards the incorporation of Li+ions. A lithium interfacial ASR (ASRinterface) is calculated from the interfacial resistance (Rinterface), by the equation ASRinterface=Rinterface*A / 2, where A is the area of the electrodes in contact with the separator and the factor of 2 accounts for 2 interfaces when measured in a symmetric cell and Rinterface=Rtotal-Rbulk, wherein Rtotal is total resistance and Rbulk is bulk resistance.

[0024] As used herein the phrase “bonding layer” refers to a layer which adheres alithium-stuffed garnet layer to an electrolyte layer or buffer layer. A layer herein is a material which covers the face of the lithium-stuffed garnet layer. The bonding layer is not a perimeter seal around the edges of the lithium stuffed-garnet.

[0025] As used herein, a “binder” refers to a material that assists in or increases theadhesion and / or cohesion of another material. For example, as used herein, polyvinyl butyral is a binder because it is useful for adhering garnet materials. Other binders may include polycarbonates. Other binders may include polyacrylates and polymethacrylates. These examples of binders are not limiting as to the entire scope of binders contemplated here but merely serve as examples. Binders useful in the present disclosure include, but are not limited to, polypropylene (PP), polyethylene, atactic polypropylene (aPP), isotactic polypropylene (iPP), ethylene propylene rubber (EPR), ethylene pentene copolymer (EPC), polyisobutylene (PIB), styrene butadiene rubber (SBR), polyolefins, polyethylene-co-poly-1-octene (PE-co- PO), polyethylene-co-poly(methylene cyclopentane) (PE-co-PMCP), poly(methyl methacrylate) (and other acrylics), acrylic, polyvinylacetacetal resin, polyvinyl butyral resin, PVB, polyvinyl acetal resin, stereoblock polypropylenes, polypropylene polymethylpentene copolymer, polyethylene oxide (PEO), PEO block copolymers, silicone, and the like. In some examples, including any of the foregoing, the binder is a polymer is selected from the group consisting of polyacrylonitrile (PAN), polypropylene, polyethylene, polyethylene oxide (PEO), polymethyl methacrylate (PMMA), polyvinyl chloride (PVC), polyvinyl pyrrolidone (PVP), polyethylene oxide poly(allyl glycidyl ether) PEO-AGE, polyethylene oxide 2-methoxyethoxyethyl glycidyl ether (PEO-MEEGE), polyethylene oxide 2-methoxyethoxyethyl glycidyl poly(allyl glycidyl ether) (PEO-MEEGE- AGE), polysiloxane, polyvinylidene fluoride (PVDF),Attorney Docket No.114826.00834 415.601 polyvinylidene fluoride hexafluoropropylene (PVDF-HFP), ethylene propylene (EPR), nitrile rubber (NPR), styrene-butadiene-rubber (SBR), polybutadiene polymer, polybutadiene rubber (PB), polyisobutadiene rubber (PIB), polyolefin, alpha-polyolefin, ethylene alpha- polyolefin, polyisoprene rubber (PI), polychloroprene rubber (CR), acrylonitrile-butadiene rubber (NBR), and polyethyl acrylate (PEA).As used herein, “selected from the group consisting of” refers to a single member from the group, more than one member from the group, or a combination of members from the group. A member selected from the group consisting of A, B, and C includes, for example, A only, B only, or C only, as well as A and B, A and C, B and C, as well as A, B, and C.

[0026] As used herein, the term “buffer” refers to a single ion conducting, solid-stateelectrolyte that is finely mixed within or combined with the positive electrode components or is a layer which is in direct contact with the positive electrode, e.g., an electrolyte layer laminated to the positive electrode layer. Single ion conducting means that the material only conducts one type of ion, e.g., a Li+ion with a transference number of greater than 0.9. Solid- state means that the buffer exists in the solid phase at ambient temperatures and pressures. The

[0027] As used herein, the phrase “buffer is mixed within the positive electrodelayer,” means that the buffer material is ground up, e.g., milled, and then mixed with the other positive electrode layer compounds, e.g., active material and conductive carbon, when the positive electrode layer is formed.

[0028] As used herein the phrase “casting a film,” refers to the process of deliveringor transferring a liquid or a slurry into a mold, or onto a substrate, such that the liquid or the slurry forms, or is formed into, a film. Casting may be done via doctor blade, meyer rod, comma coater, gravure coater, microgravure, reverse comma coater, slot die, slip and / or tape casting, and other methods.

[0029] As used herein, the phrase “characterized by the formula” refers to adescription of a chemical compound by its chemical formula.

[0030] As used herein, the phrase “current collector” refers to a component or layer ina secondary battery through which electrons conduct, to or from an electrode in order to complete an external circuit, and which are in direct contact with the electrode to or from which the electrons conduct. In some examples, the current collector is a metal (e.g., Al, Cu, or Ni, steel, alloys thereof, or combinations thereof) layer which is laminated to a positive orAttorney Docket No.114826.00834 415.601 negative electrode. In some examples, the current collector is Al. In some examples, the current collector is Cu. In some examples, the current collector is Ni. In some examples, the current collector is steel. In some examples, the current collector is an alloy of Al. In some examples, the current collector is an alloy of Cu. In some examples, the current collector is an alloy of steel. In some examples, the current collector is Al. In some examples, the current collector is coated with carbon. In some examples, the current collector comprises a combination of the above metals. During charging and discharging, electrons move in the opposite direction to the flow of Li ions and pass through the current collector when entering or exiting an electrode.

[0031] As used herein, the term “diameter (D50)” includes the characteristicdimension at which 50% of the total particle area (or volume) is representative of particles smaller than the recited size. Similarly, the term “diameter (D10)” includes the characteristic dimension at which 10% of the total particle area (or volume) is representative of particles smaller than the recited size. These figures may be calculated on a per-volume or per-area basis. Per-volume basis is assumed if neither is explicitly recited.

[0032] As used herein, the term “contact” means direct contact unless specifiedotherwise. For electrically conductive materials, contact means contact sufficient for electrical conduction to occur between the contacting materials. For ionically conductive materials, contact means contact sufficient for ionic conduction to occur between the contacting materials. Two materials which are in direct contact are positioned without an interleaving layer between the two materials. As used herein, the phrase “electrical contact,” refers to contact sufficient for electrical conduction to occur between the contacting materials.

[0033] As used herein, the phrase “direct contact,” means that two materials are insufficient physical contact to conduct an electronic or ionic current therebetween, if the materials are electrically or ionically conductive. Direct contact between two materials, one of which is electrically or ionically insulating, means that the two materials share an interface that transmits an applied force or pressure.

[0034] As used herein, the phrase “electrical contact” means that two materials are indirect contact and can conduct an electrical current through the point(s) of direct contact.

[0035] As used herein, the terms “cathode” and “anode” refer to the electrodes of abattery. During a charge cycle in a Li-secondary battery, Li ions leave the cathode and moveAttorney Docket No.114826.00834 415.601 through an electrolyte and to the anode. During a charge cycle, electrons leave the cathode and move through an external circuit to the anode. During a discharge cycle in a Li-secondary battery, Li ions migrate towards the cathode through an electrolyte and from the anode. During a discharge cycle, electrons leave the anode and move through an external circuit to the cathode.

[0036] As used herein, the phrases “electrochemical cell” or “battery cell” shall,unless specified to the contrary, mean a single cell including a positive electrode and a negative electrode, which have ionic communication with each other by way of an electrolyte. In some embodiments, a battery or module may include multiple positive electrodes and / or multiple negative electrodes enclosed in one container or otherwise put together one on top of another, e.g., a stack of electrochemical cells. A stack of electrochemical cells or “electrochemical stack,” may be referred to as a multi-layered cell. A symmetric cell may be a cell having two Li metal anodes separated by a solid-state electrolyte.

[0037] As used herein, the phrase “electrochemical device” refers to an energystorage device, such as, but not limited to a Li-secondary battery that operates or produces electricity or an electrical current by an electrochemical reaction, e.g., a conversion chemistry reaction such as 3Li + FeF3↔ 3LiF + Fe.

[0038] As used herein, the term “electrolyte,” refers to a material that allows ions,e.g., Li+, to migrate therethrough, but which does not allow electrons to conduct therethrough. The ionic conductivity is greater than the electronic conductivity by a factor of at least 1000. Electrolytes are useful for electrically insulating the cathode and anode of a secondary battery while allowing ions, e.g., Li+, to transmit through the electrolyte. Solid electrolytes, in some examples, rely on ion hopping and / or diffusion through rigid structures. Solid electrolytes may be also referred to as fast ion conductors or super-ionic conductors. In this case, a solid electrolyte layer may be also referred to as a solid electrolyte separator or a solid-state electrolyte separator.

[0039] As used herein, the phrase “film thickness” refers to the distance, or medianmeasured distance, between the top and bottom faces of a film. As used herein, the term “thickness” when referring to a layer refers to the distance, or median measured distance, between the top and bottom faces of the layer. As used herein, the top and bottom faces referAttorney Docket No.114826.00834 415.601 to the sides of the film having the largest surface area. Scanning electron microscopy is used to measure thickness unless specified otherwise explicitly.

[0040] As used herein, the term “thin film” refers to a film having the components,compositions, or materials described herein where the film has an average thickness dimension of about 10 nm to about 100 μm. In some examples, thin refers to a film that is less than about 1 μm, 10 μm, or 50 μm in thickness.

[0041] As used herein, the phrase “lithium stuffed garnet” refers to oxides that arecharacterized by a crystal structure related to a garnet crystal structure. U.S. Patent Application Publication No. U.S.2015 / 0099190, which published Apr.9, 2015 and was filed Oct.7, 2014 as Ser. No.14 / 509,029, is incorporated by reference herein in its entirety for all purposes. This application describes Li-stuffed garnet solid-state electrolytes used in solid- state lithium rechargeable batteries.

[0042] Unless stated otherwise to the contrary, lithium-stuffed garnets includecompounds having the formula LiALaBM′CM″DZrEOF, LiALaBM′CM″DTaEOF, or LiALaBM′CM″DNbEOF, wherein 4<A<8.5, 1.5<B<4, 0≦C≦2, 0≦D≦2; 0≦E≦2, 10<F<13, and M″ and M″ are each, independently in each instance selected from Al, Mo, W, Nb, Sb, Ca, Ba, Sr, Ce, Hf, Rb, Nb, Ga, or Ta, or LiaLabZrCAldMe″eOf, wherein 5<a<7.7; 2<b<4; 0≦c≦2.5; 0≦d≦2; 0≦e≦2, 10<f<13 and Me″ is a metal selected from Nb, Ta, V, W, Mo, Ga, or Sb and as described herein.

[0043] Li-stuffed garnets may also be a composition according toLiALaBM′CM″DZrEOF, LiALaBM′CM″DTaEOF, or LiALaBM′CM″DNbEOF, wherein 4<A<8.5, 1.5<B<4, 0≤C≤2, 0≤D≤2; 0≤E<3, 10<F<13, and M′ and M″ are each, independently in each instance selected from Ga, Al, Mo, W, Nb, Sb, Ca, Ba, Sr, Ce, Hf, Rb, Nb, Ga, or Ta, or LiaLabZrcAldMe″eOf, wherein 5<a<8.5; 2<b<4; 0<c≤2.5; 0≤d<2; 0≤e<2, and 10<f<13 and Me″ is a metal selected from Ga, Nb, Ta, V, W, Mo, or Sb and as otherwise described in U.S. Patent Application Publication No. U.S.2015 / 0099190. As used herein, lithium-stuffed garnets, and garnets, generally, include, but are not limited to, Li7.0La3(Zrt1+Nbt2+Tat3)O12+0.35Al12O3; wherein (t1+t2+t3=2) so that the La:(Zr / Nb / Ta) ratio is 3:2. Also, garnets used herein include, but are not limited to, LixLa3Zr2OF+yAl2O3, wherein x ranges from 5.5 to 9; and y ranges from 0.05 to 1. In these examples, subscripts x, y, and F are selected so that the garnet is charge neutral. In some examples x is 7 and y is 1.0. In some examples, x is 5 and y is 1.0. In some examples, x is 6 and y is 1.0. In someAttorney Docket No.114826.00834 415.601 examples, x is 8 and y is 1.0. In some examples, x is 9 and y is 1.0. In some examples x is 7 and y is 0.35. In some examples, x is 5 and y is 0.35. In some examples, x is 6 and y is 0.35. In some examples, x is 8 and y is 0.35. In some examples, x is 9 and y is 0.35. In some examples x is 7 and y is 0.7. In some examples, x is 5 and y is 0.7. In some examples, x is 6 and y is 0.7. In some examples, x is 8 and y is 0.7. In some examples, x is 9 and y is 0.7. In some examples x is 7 and y is 0.75. In some examples, x is 5 and y is 0.75. In some examples, x is 6 and y is 0.75. In some examples, x is 8 and y is 0.75. In some examples, x is 9 and y is 0.75. In some examples x is 7 and y is 0.8. In some examples, x is 5 and y is 0.8. In some examples, x is 6 and y is 0.8. In some examples, x is 8 and y is 0.8. In some examples, x is 9 and y is 0.8. In some examples x is 7 and y is 0.5. In some examples, x is 5 and y is 0.5. In some examples, x is 6 and y is 0.5. In some examples, x is 8 and y is 0.5. In some examples, x is 9 and y is 0.5. In some examples x is 7 and y is 0.4. In some examples, x is 5 and y is 0.4. In some examples, x is 6 and y is 0.4. In some examples, x is 8 and y is 0.4. In some examples, x is 9 and y is 0.4. In some examples x is 7 and y is 0.3. In some examples, x is 5 and y is 0.3. In some examples, x is 6 and y is 0.3. In some examples, x is 8 and y is 0.3. In some examples, x is 9 and y is 0.3. In some examples x is 7 and y is 0.22. In some examples, x is 5 and y is 0.22. In some examples, x is 6 and y is 0.22. In some examples, x is 8 and y is 0.22. In some examples, x is 9 and y is 0.22. Also, garnets as used herein include, but are not limited to, LixLa3Zr2O12+yAl2O3. In one embodiment, the Li-stuffed garnet herein has a composition of Li7Li3Zr2O12. In another embodiment, the Li-stuffed garnet herein has a composition of Li7Li3Zr2O12.Al2O3. In yet another embodiment, the Li-stuffed garnet herein has a composition of Li7Li3Zr2O12.0.22Al2O3. In yet another embodiment, the Li-stuffed garnet herein has a composition of Li7Li3Zr2O12.0.35Al2O3. In certain other embodiments, the Li-stuffed garnet herein has a composition of Li7Li3Zr2O12.0.5Al2O3. In another embodiment, the Li-stuffed garnet herein has a composition of Li7Li3Zr2O12.0.75Al2O3.

[0044] As used herein, garnet does not include YAG-garnets (i.e., yttrium aluminumgarnets, or, e.g., Y3Al5O12). As used herein, garnet does not include silicate-based garnets such as pyrope, almandine, spessartine, grossular, hessonite, or cinnamon-stone, tsavorite, uvarovite and andradite and the solid solutions pyrope-almandine-spessarite and uvarovite- grossular-andradite. Garnets herein do not include nesosilicates having the general formula X3Y2(SiO4)3 wherein X is Ca, Mg, Fe, and, or, Mn; and Y is Al, Fe, and, or, Cr.Attorney Docket No.114826.00834 415.601

[0045] As used herein, the term “LSTPS” refers to an electrolyte material having Li,Si, P, Sn, and S chemical constituents. In an example, “LSTPS” can refer to Li4-x(SidSn1-d)- (1-x)PxS4, wherein 0.5<d<1.0 and 0.1<x<1.0 (e.g., d=0.8 and x=0.55).

[0046] As used herein, “LSPSO,” refers to LSPS that is doped with, or has, O present.In some examples, “LSPSO,” is a LSPS material with an oxygen content between 0.01 and 10 atomic %.

[0047] As used herein, the term “LXPS” or “LPS+X” refers to a lithium conductingelectrolyte comprising Li, P, S, and X, where X = Cl, Br, and / or I. For example, “LSPI” refers to a lithium conducting electrolyte comprising Li, P, S, and I. More generally, it is understood to include aLi2S+bP2Sy+cLiX where X = Cl, Br, and / or I and wherein y=3-5, wherein a / b=2.5-4.5, and where (a+b) / c=0.5-15.

[0048] As used herein, the term “LPSCl” refers to an electrolyte material having Li,P, S, and Cl chemical constituents. As used herein, the term “LPSBr” refers to an electrolyte material having Li, P, S, and Br chemical constituents. As used herein, the term “LPSI” refers to an electrolyte material having Li, P, S, and I chemical constituents. LXPSO refers to LXPS, as defined above, and having oxygen doping at from 0.1 to about 10 atomic %. LPSO refers to LPS, as defined above, and having oxygen doping at from 0.1 to about 10 atomic %.

[0049] As used herein, the term “LBHI” or “LiBHI” refers to a lithium conductingelectrolyte having Li, B, H, and I. More generally, it is understood to include aLiBH4+bLiX where X = Cl, Br, and / or I and where a:b=7:1, 6:1, 5:1, 4:1, 3:1, 2:1, or within the range a / b = 2-4. LBHI may further include nitrogen in the form of aLiBH4+bLiX+cLiNH2 where (a+c) / b = 2-4 and c / a = 0-10.

[0050] As used herein, the term “LBHXN” refers to a composition characterized asA·(LiBH4)·B·(LiX)·C·(LiNH2) wherein X is fluorine (F), bromine (Br), chloride (Cl), iodine(I), or a combination thereof, and wherein 0≤A≤6, 2≤B≤5, and 0≤C≤9. As used herein, theterm “LBHFN” refers to a composition characterized as A·(LiBH4)·B·(LiF)·C·(LiNH2) and wherein 0≤A≤6, 2≤B≤5, and 0≤C≤9. As used herein, the term “LBHBrN” refers to acomposition characterized as A·(LiBH4)·B·(LiBr)·C·(LiNH2) and wherein 0≤A≤6, 2≤B≤5,and 0≤C≤9. As used herein, the term “LBHClN” refers to a composition characterized asA·(LiBH4)·B·(LiCl)·C·(LiNH2) and wherein 0≤A≤6, 2≤B≤5, and 0≤C≤9. As used herein, theterm “LBHIN” refers to a composition characterized as A·(LiBH4)·B·(LiI)·C·(LiNH2) and wherein 0≤A≤6, 2≤B≤5, and 0≤C≤9.Attorney Docket No.114826.00834 415.601

[0051] As used herein, the term “LBHXN” refers to a composition characterized asA·(LiBH4)·B·(LiX)·C·(LiNH2) wherein X is fluorine (F), bromine (Br), chloride (Cl), iodine(I), or a combination thereof, and wherein 3≤A≤6, 2≤B≤5, and 0≤C≤9. As used herein, theterm “LBHFN” refers to a composition characterized as A·(LiBH4)·B·(LiF)·C·(LiNH2) and wherein 3≤A≤6, 2≤B≤5, and 0≤C≤9. As used herein, the term “LBHBrN” refers to acomposition characterized as A·(LiBH4)·B·(LiBr)·C·(LiNH2) and wherein 3≤A≤6, 2≤B≤5,and 0≤C≤9. As used herein, the term “LBHClN” refers to a composition characterized asA·(LiBH4)·B·(LiCl)·C·(LiNH2) and wherein 3≤A≤6, 2≤B≤5, and 0≤C≤9. As used herein, theterm “LBHIN” refers to a composition characterized as A·(LiBH4)·B·(LiI)·C·(LiNH2) and wherein 3≤A≤6, 2≤B≤5, and 0≤C≤9.

[0052] As used herein, the phrase “made of the same type of material,” refers to twoor more different physical forms of a material but which includes same composition. For example, lithium-stuffed garnet powder and a lithium-stuffed garnet thin film are made of the same type of material. For example, LSTPS powder and an LSTPS thin film are made of the same type of material.

[0053] As used herein the term “making,” refers to the process or method of formingor causing to form the object that is made. For example, making an energy storage electrode includes the process, process steps, or method of causing the electrode of an energy storage device to be formed. The end result of the steps constituting the making of the energy storage electrode is the production of a material that is functional as an electrode

[0054] As used herein, the phrase “positive electrode” refers to the electrode in asecondary battery towards which positive ions, e.g., Li+, conduct, flow, or move during discharge of the battery. As used herein, the phrase “negative electrode” refers to the electrode in a secondary battery from which positive ions, e.g., Li+flow, or move during discharge of the battery. In a battery comprised of a Li-metal electrode and a conversion chemistry, intercalation chemistry, or combination of conversion / intercalation chemistry- including electrode (i.e., cathode active material), the electrode having the conversion chemistry, intercalation chemistry, or combination of conversion / intercalation chemistry material is referred to as the positive electrode. In some usage, cathode is used in place of positive electrode, and anode is used in place of negative electrode. When a Li-secondary battery is charged, Li ions move from the positive electrode (e.g., NiFx, NMC, NCA) towardsAttorney Docket No.114826.00834 415.601 the negative electrode (e.g., Li-metal). When a Li-secondary battery is discharged, Li ions move towards the positive electrode and from the negative electrode.

[0055] As used herein, the phrase “organic component (at 10%)” refers to the weightpercent amount of an organic species in a host. For example, if the buffer layer includes LSTPS and a polymer but wherein the organic component (at 10%), this means that the total amount of polymer in the combination of LSTPS and polymer is 10 weight %, with the remaining 90% being non-organic, e.g., LSTPS.

[0056] As used herein, the phrase “porosity as determined by SEM” refers tomeasurement of density by using image analysis software to analyze a scanning electron micrograph. For example, first, a user or software assigns pixels and / or regions of an image as porosity. Second, the area fraction of those regions is summed. Finally, the porosity fraction determined by SEM is equal to the area fraction of the porous region of the image.

[0057] As used herein, the phrase “providing” refers to the provision of, generationor, presentation of, or delivery of that which is provided.

[0058] As used here, the phrase “solid-state electrolyte separator” is usedinterchangeably with the phrase “solid separator,” and refers to a material which does not include carbon and which conducts atomic ions (e.g., Li+) but does not conduct electrons. A solid-state electrolyte separator is a solid material suitable for electrically isolating the positive and negative electrodes of a lithium secondary battery while also providing a conduction pathway for lithium ions. Examples of solid-state electrolytes include oxide electrolytes and sulfide electrolytes, which are further defined below. Non-limiting examples of sulfide electrolytes are found, for example, in U.S. Pat. No.9,172,114, which issued Oct. 27, 2015, and also in US Patent Application Publication No.2017-0162901 A1, which published Jun.8, 2017. Non-limiting examples of oxide electrolytes are found, for example, in US Patent Application Publication No.2015-0200420 A1, which published Jul.16, 2015, and issued as U.S. Pat. No.9,806,372 on Oct.31, 2017. In some examples, the solid-state electrolyte also includes a polymer and is referred to as a composite electrolyte. Composite electrolytes are found for example in U.S. Patent No.9,666,870. The entire contents of the just-mentioned US patents and published US patent applications are incorporated herein by reference in their entirety for all purposes.

[0059] As used herein, the terms “separator” refers short-hand reference for Li+ ion-conducting electrolyte separator, unless explicitly specified otherwise.Attorney Docket No.114826.00834 415.601

[0060] As used herein, the phrase “solid-state cathode” or “solid-state positiveelectrode” refers to a type of “positive electrode” defined herein. In certain examples, all components in this solid-state cathode film are in solid form. The solid-state cathode includes active cathode materials as defined herein, solid-state catholyte as defined herein, optionally a conductive additive, and optionally binders. The solid-state cathode are in some examples densified films.

[0061] As used here, the phrase “solid-state electrolyte,” is used interchangeably withthe phrase “solid separator” refers to a material which does not include carbon and which conducts atomic ions (e.g., Li+) but does not conduct electrons. An inorganic solid-state electrolyte is a solid material suitable for electrically isolating the positive and negative electrodes of a lithium secondary battery while also providing a conduction pathway for lithium ions. Example inorganic solid-state electrolytes include oxide electrolytes and sulfide electrolytes, which are further defined below. Non-limiting example sulfide electrolytes are found, for example, in US Patent No.9,172,114, which issued October 27, 2015, and also in US Patent Application Publication No.2017-0162901 A1, which published June 8, 2017, and was filed as US Patent Application No.15 / 367,103 on December 1, 2016, the entire contents of which are herein incorporated by reference in its entirety for all purposes. Non-limiting example oxide electrolytes are found, for example, in US Patent Application Publication No. 2015-0200420 A1, which published July 16, 2015, the entire contents of which are herein incorporated by reference in its entirety for all purposes. In some examples, the inorganic solid-state electrolyte also includes a polymer.

[0062] As used herein, the term “sulfide” refers to refers to a chemical compound thatincludes at least one sulfur atom and one other element in the chemical formula for the chemical compound. For example, a “sulfide” is interchangeable with “sulfide electrolytes.” Non-limiting examples of sulfide electrolytes are found, for example, in US Patent No. 9,172,114, issued October 27, 2015, and also in US Patent Application Publication No.2017- 0162901 A1, which published June 8, 2017, and was filed as US Patent Application No. 15 / 367,103 on December 1, 2016, the entire contents of which are herein incorporated by reference in its entirety for all purposes. As used herein, a sulfide catholyte is a catholyte that comprises or consists essentially of a sulfide.

[0063] As used here, the phrase “sulfide electrolyte,” or “lithium sulfide” includes,but is not limited to, electrolytes referred to herein as LSS, LTS, LXPS, or LXPSO, where XAttorney Docket No.114826.00834 415.601 is Si, Ge, Sn, As, Al, or Li-Sn-Si-P-S, or Li-As-Sn-S. In these acronyms (LSS, LTS, LXPS, or LXPSO), S refers to the element S, Si, or combinations thereof, and T refers to the element Sn. “Sulfide electrolyte” may also include LiaPbScXd, LiaBbScXd, LiaSnbScXdor LiaSibScXdwhere X=F, Cl, Br, I, and 10%≤a≤50%, 10%≤b≤44%, 24%≤c≤70%, 0≤d≤18%; % are atomic %. Up to 10 at% oxygen may be present in the sulfide electrolytes, either by design or as a contaminant species.

[0064] As used herein, the term “sulfide-halide” refers to a chemical compound thatincludes at least one sulfur atom, at least one halogen atom, and one other element in the chemical formula for the chemical compound.

[0065] As used herein, voltage is set forth with respect to lithium (i.e., V vs. Li) metalunless stated otherwise.

[0066] As used herein, “module” and “battery module” mean a unit that houses one ormore electrochemical cell and may, but does not necessarily, include the following elements: (i) mechanical structural components (e.g., outer module housing / structure, means for spacing and securing the cells, cell pressure distributors, cell swelling compensation); (ii) thermal management components (e.g., battery cell thermal contacts / interface, venting, cooling channels, and thermal barriers, all at least partially within the module housing); (iii) high voltage components (e.g., busbars, cables, couplings, electrical insulation, and terminals, all at least partially enclosed by the module housing); and (iv) electrical hardware components for cell monitoring and identification (e.g., cell supervision electronics, electrical connectors, wireless or wired communication devices, RFIDs, thermocouples, current sensors, and voltage sensors). An electrochemical stack may include several of these aforementioned units arranged in electrical communication (e.g., serial or parallel electrical connection). In some examples, when the electrochemical stack includes several units, the units may be layered, laminated together, or otherwise adhered to each other, in a column. In some examples, when the electrochemical stack includes several units, the units may be layered, laminated together, or otherwise adhered to each other in an array. In some examples, when the electrochemical stack includes several units, the stack may be arranged such that one negative electrode current collector is shared with two or more positive electrodes. Alternatively, in some examples, when the electrochemical stack includes several units, the stack may be arranged such that one positive electrode current collector is shared with two or more negative electrodes. Where appropriate or necessary, adhesives or otherAttorney Docket No.114826.00834 415.601 bonding materials may be provided among the various layers in a stack. Optionally or additionally, when cells are provided together to form a stack, the cells simply may be set one on top of another, or alternatively one or more of the cells may be adhered to one or both immediately adjacent cells.

[0067] Electrochemical stack assemblies refer to multiple electrochemical cellsconnected together.

[0068] As used herein, the phrase “positive electrode terminal” refers to an electricalconnection to the positive electrode. A positive electrode terminal may also be referred to as a positive electrode current collector.

[0069] As used herein, the phrase “negative electrode terminal” refers to an electricalconnection to the negative electrode. A negative electrode terminal may also be referred to as a negative electrode current collector.

[0070] As used herein, the phrase “cathode active material” refers to a material whichcan intercalate lithium ions or react with lithium ions in a reversible manner. Examples include LiMPO4(M=Fe, Ni, Co, Mn); LixTiyOz, wherein x is from 0 to 8, y is from 1 to 12, z is from 1 to 24; LiMn2aNiaO4, wherein a is from 0 to 2; a nickel cobalt aluminum oxide; LiNixMnyCozO2, x+y+z=1, 0≤x≤1, 0≤y≤1, and 0≤z≤1; and LiNixCoyAlzO2, wherein x+y+z=1, and 0≤x≤1, 0≤y≤1, and 0≤z≤1. In these formula, x, y, and z are chosen so that the formula is charge neutral.

[0071] As used herein, the phrase “thickness” or “film thickness” refers to thedistance, or median measured distance between top and bottom major surfaces of a layer or film. As used herein, the top and bottom major surfaces refer to the layer or film sides having the largest geometric surface area.

[0072] As used herein, “thin” means, when qualifying a solid-state electrolyte, athickness dimension less than 200 μm, sometimes less than 100 μm and in some cases between 0.1 and 60 μm, and in other cases between about 10 nm to about 100 μm; in other cases about 1 μm, 10 μm, or 50 μm in thickness.

[0073] As used herein, the term “lithium salt” refers to a lithium-containingcompound that is a solid at room temperature that at least partially dissociates when immersed in a solvent such as EMC. Lithium salts may include but are not limited to LiPF6, LiBOB, LiTFSi, LiFSI, LiAsF6, LiClO4, LiI, LiBETI, LiBF4.As used herein, the termAttorney Docket No.114826.00834 415.601 “carbonate solvent” refers to a class of solvents containing a carbonate group C(=O)(O–)2. Carbonate solvents include but are not limited to ethylene carbonate, dimethyl carbonate, propylene carbonate, diethyl carbonate, ethyl methyl carbonate, dimethyl ethylene carbonate, isobutylene carbonate, nitroethyl carbonate, Monofluoroethylene carbonate, fluoromethyl ethylene carbonate, 1,2-butylene carbonate, methyl propyl carbonate, isopropyl methyl carbonate, etc

[0074] As used herein, the term “alcohol” is a C1-C6 alcohol.

[0075] As used herein, the term “bonding layer” is a layer that is both adhesive andconductive. The layer is not limited to a perimeter seal, but includes coating the face of the positive electrode layer, buffer layer, and / or solid-state separator.

[0076] As used herein, the term “solid-state buffer layer” is a buffer layer that is solidas described herein, wherein the solid-state buffer layer is spread across the face of the positive electrolyte layer, bonding layer, and / or solid-state separator. The layer is not limited to a perimeter seal.

[0077] As used herein, the term “LiX-alcohol” wherein X is Cl, Br, or I, refers to acomposition comprising a lithium halide and short chain alcohol (e.g., C1-C6 alcohol). In an example, the LiX-alcohol can be LiI-isopropyl alcohol, LiBr-methanol, among others. The ratio of lithium halide to alcohol can be from 1:5 to 5:1. The composition can be a solid composition.

[0078] As used herein, the term “LBHIN” refers to a composition characterized asA·(LiBH4)·B·(LiI)·C·(LiNH2) and wherein 0≤A≤6, 2≤B≤5, and 0≤C≤9, for example,wherein 3≤A≤6, 2≤B≤5, and 0≤C≤9. Electrochemical cells

[0079] One example electrochemical cell is schematically illustrated in FIG. 1. Asshown, the solid-state battery can include a positive current collector layer in contact with a positive electrode layer. The positive electrode layer can include a cathode active material, a binder, and a catholyte material. The positive electrode layer can be solvent-free. In some examples, the positive electrode layer does not include an additional electronically conductive additive.

[0080] The positive electrode layer is in contact with a solid-state buffer layer. In anexample, the solid-state buffer layer can comprise the same material as the catholyte of theAttorney Docket No.114826.00834 415.601 positive electrode layer. In an example, the solid-state buffer layer can comprise a different material as the catholyte of the positive electrode layer. The solid-state buffer layer can be bound to a separator layer via a bonding layer. The separator layer can be a lithium-stuffed garnet layer. The separator layer can be in contact with a negative current collector.

[0081] In some examples, the electrochemical cell further includes a positiveelectrode current collector layer. In some examples, the electrochemical cell further includes a negative electrode current collector layer. In some examples, the negative electrode current collector layer is a sintered metal. In some examples, the sintered metal is selected from the group consisting of Al, Cu, Ni, Ag, Au, Pt, Pd, or Sn. In some examples, the metal is Ni. Bonding Layer Composition

[0082] In an example, the solid bonding layer composition includes a lithium salt.The lithium salt can be LiTFSI, LiFSI, LiPF6, LiClO4, LiAsF6, LiBOB, LiBETI, LiBF4, LiI, LiBr, LiCl, or combinations thereof. In an example, the lithium salt is LiI, LiBr, LiCl, or combinations thereof. The solid bonding layer composition includes an alcohol, wherein the alcohol is methanol, isopropanol, or combinations thereof. The lithium salt can be present at 1 M to 5 M concentration. In an example, the composition is solid.

[0083] In an example, the bonding layer composition can include a lithium salt and aorganic solubilizer. The lithium salt can be LiTFSI, LiFSI, LiPF6, LiClO4, LiAsF6, LiBOB, LiBETI, LiBF4, LiI, LiBr, LiCl, or combinations thereof. For example, the lithium salt can be LiTFSI, LiFSI, LiPF6, or combinations thereof. The organic solubilizer can be 1,3-dioxolane, dimethoxyethane, or combinations thereof. The bonding layer can be in the form of a gel.

[0084] In certain examples, the lithium salt is selected from LiPF6, Lithiumbis(oxalato)borate (LiBOB), Lithium bis(perfluoroethanesulfonyl)imide (LIBETI), LiTFSi, LiBF4, LiClO4, LiAsF6, LiFSI, LiAsF6, or LiI. In certain examples, the lithium salt is LiPF6. In certain examples, the lithium salt is LiBOB.In certain examples, the lithium salt is LiTFSi. In certain examples, the lithium salt is LiBF4. In certain examples, the lithium salt is LiClO4. In certain examples, the lithium salt is LiAsF6. In certain examples, the lithium salt is LiI. In certain examples, the lithium salt is LiBF4.

[0085] In certain examples, several lithium salts may be present simultaneously indifferent concentrations. In some examples, the concentration is about 0.5, about 0.6, about 0.7, about 0.8, about 0.9, about 1.0, about 1.1, about 1.2, about 1.3, about 1.4, about 1.5, about 1.6, about 1.7, about 1.8, about 1.9 or about 2.0M. In certain examples, the bondingAttorney Docket No.114826.00834 415.601 layer may contain two salts selected from LiBr, LiCl, LiI, LiPF6, LiBOB, LiTFSi, LiBF4,LiClO4, LiAsF6, LiFSI, or LiAsF6. In certain examples, the gel electrolyte may contain threesalts selected from LiPF6, LiBOB, LiTFSi, LiBF4, LiClO4, LiAsF6, LiFSI, LiAsF6, LiBr, LiCl, or LiI.

[0086] In certain examples, the lithium salt is a lithium salt is selected from LiPF6,LiBOB, and LFTSi.

[0087] In certain examples, the lithium salt is LiPF6 at a concentration of 0.5 M to2M. In some examples, the concentration is 0.5, 0.6, 0.7, 0.8, 0.9, 1.0, 1.1, 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8, 1.9 or 2.0M.

[0088] In certain examples, the lithium salt is LiTFSI at a concentration of 0.5 M to2M. In some examples, the concentration is 0.5, 0.6, 0.7, 0.8, 0.9, 1.0, 1.1, 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8, 1.9 or 2.0M

[0089] In certain examples, the lithium salt is present at a concentration from 0.01 Mto 10 M. In some examples, the concentration is 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1.0, 1.1, 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8, 1.9, 2.0, 2.1, 2.2, 2.3, 2.4, 2.5, 2.6, 2.7, 2.8, 2.9, 3.0, 3.3, 3.2, 3.3, 3.4, 3.5, 3.6, 3.7, 3.8, 3.9, 2.0, 0.3, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 3.0, 3.1, 3.2, 3.3, 3.4, 3.5, 3.6, 3.7, 3.8, 3.9, 4.0, 5.1, 5.2, 5.3, 5.4, 5.5, 5.6, 5.7, 5.8, 5.9, 6.0, 6.1, 6.2, 6.3, 6.4, 6.5, 6.6, 6.7, 6.8, 6.9, 7.0, 7.1, 7.2, 7.3, 7.4, 7.5, 7.6, 7.7, 7.8, 7.9, 8.0, 8.1, 8.2, 8.8, 8.4, 8.5, 8.6, 8.7, 8.8, 8.9, 9.9, 9.1, 9.2, 9.3, 9.4, 9.5, 9.6, 9.7, 9.8, 9.9, 10.0 M.

[0090] In certain examples, the solvent in bonding layer is selected from 1,3-dioxolane, dimethoxyethane, ethylene carbonate (EC), diethylene carbonate, diethyl carbonate, dimethyl carbonate (DMC), ethyl-methyl carbonate (EMC), propylmethyl carbonate, nitroethyl carbonate, propylene carbonate (PC), diethyl carbonate (DEC), methyl propyl carbonate (MPC), 2,5-Dioxahexanedioic Acid Dimethyl Ester, tetrahydrofuran (THF), γ-Butyrolactone (GBL), fluoroethylene carbonate (FEC), fluoromethyl ethylene carbonate (FMEC), trifluoroethyl methyl carbonate (F-EMC), fluorinated 3-(1,1,2,2-tetrafluoroethoxy)- 1,1,2,2-tetrafluoropropane / 1,1,2,2-Tetrafluoro-3-(1,1,2,2-tetrafluoroethoxy)propane (F- EPE), fluorinated cyclic carbonate (F-AEC), dioxolane, prop-1-ene-1,3-sultone (PES), sulfolane, acetonitrile (ACN), succinonitrile (SN), Pimelonitrile, Suberonitrile, propionitrile, Propanedinitrile, glutaronitrile (GLN), adiponitrile (ADN), hexanedinitrile, pentanedinitrile, acetophenone, isophorone, benzonitrile, Methylene methanedisulfonate, dimethyl sulfate, dimethyl sulfoxide (DMSO), ethyl acetate, methyl butyrate, dimethyl ether (DME), diethylAttorney Docket No.114826.00834 415.601 ether, dioxolane, gamma butyl-lactone, Methyl benzoate, 2-methyl-5-oxooxolane-2- carbonitrile, or combinations thereof.

[0091] In certain examples, the solvent is selected from methylene carbonate (EC). Incertain examples, the solvent is a mixture of EC with sulfolane, EC with EMC, EC with PC, EC with DMC, EC with MPC, EC with DEC, EC with GBL, or EC with PES. The mixture ratio of EC to the other component may be about 8:2, about 7:3, about 6:4, about 5:5, about 4:6, about 3:7, or about 2:8.

[0092] In certain examples, the solvent is present in the bonding layer as a residualamount. In some examples, the residual amount is the amount of solvent remaining after the bonding layer is dried. In some examples, the residual amount is the amount of solvent remaining after the bonding layer is dried after the bonding layer is made. In some examples, the residual amount is the amount of solvent remaining after the bonding layer is spin-coated onto a substrate and dried. In some examples, the residual amount is the minimum amount of solvent required to solvate the lithium salt. For example, in certain examples, the lithium salt in the gel electrolyte is LiPF6 at a concentration of 0.5 M to 2M. To prepare this gel electrolyte, a solvent such as a combination of EC:DMC in a 1:1 v / v ratio may be used. In this solvent, LiPF6 is dissolved at a concentration of 0.5 M to 2M. Next, the bonding layer is deposited onto a substrate or onto a solid state electrolyte and allowed to dry. Once the evaporation of solvent is no longer appreciable at room temperature, the amount of solvent remaining in the gel is considered the residual amount.

[0093] In some examples, the bonding layer can include a polymer is selected fromthe group consisting of polyacrylonitrile (PAN), polypropylene, polyethylene oxide (PEO), polymethyl methacrylate (PMMA), polyvinyl chloride (PVC), polyvinyl pyrrolidone (PVP), polyethylene oxide poly(allyl glycidyl ether) PEO-AGE, polyethylene oxide 2- methoxyethoxy)ethyl glycidyl ether (PEO-MEEGE), polyethylene oxide 2- methoxyethoxy)ethyl glycidyl poly(allyl glycidyl ether) (PEO-MEEGE-AGE), polysiloxane, polyvinylidene fluoride (PVDF), polyvinylidene fluoride hexafluoropropylene (PVDF -HFP), and rubbers such as ethylene propylene (EPR), nitrile rubber (NPR), styrene-butadiene- rubber (SBR), polybutadiene polymer, polybutadiene rubber (PB), polyisobutadiene rubber (PIB), polyisoprene rubber (PI), polychloroprene rubber (CR), acrylonitrile-butadiene rubber (NBR), polyethyl acrylate (PEA), polyvinylidene fluoride (PVDF), or polyethylene (e.g., low density linear polyethylene).Attorney Docket No.114826.00834 415.601

[0094] In certain examples, the bonding layer can include a polymer includingpolyacrylonitrile (PAN) or polyvinylidene fluoride hexafluoropropylene (PVDF-HFP). In certain examples, the polymer in the gel electrolyte is a combination of polyacrylonitrile (PAN) and polyvinylidene fluoride hexafluoropropylene (PVDF-HFP). In certain examples, the polymer is PAN, PVDF-HFP, PVDF-HFP and PAN, PMMA, PVC, PVP, PEO, or combinations thereof. In certain examples, the polymer is PAN. In certain examples, the polymer in the gel electrolyte is PVDF-HFP. In certain examples, the polymer is PVDF-HFP. In certain examples, the polymer is PMMA. In certain examples, the polymer is PVC. In certain examples, the polymer is PVP. In certain examples, the polymer is PEO.

[0095] In some examples, the bonding layer may further include additives for thepurpose of mitigating gas production during cycling or storage, for improving voltage or thermal stability, or for passivating active materials, current collectors, or other components. Additives are known in the art. Some examples may include vinylene carbonate (VC), methylene methane disulfonate (MMDS), tris(trimethylsilyl) phosphate, fluoroethylene carbonate (FEC), bis(2,2,2-trifluoroethyl) carbonate (TFEC) and / or other compounds known in the art. In some examples, the water content in the solvents is less than 200ppm, or less than 150ppm, or less than 100ppm, or less than 60ppm, or less than 50ppm, or less than 40ppm, or less than 30ppm, or less than 20ppm, or less than 10ppm.

[0096] In yet other examples, the bonding layer lowers the interfacial impedancebetween an electrolyte separator and a positive electrode, when positioned between and directly in contact with an electrolyte separator and a positive electrode.

[0097] The bonding layer may be gel, semi-liquid, semi-solid, polymer, and / or solid.With respect to a gel, PCT / US2019 / 030038, filed April 30, 2019, and PCT / US2017 / 032749, filed May 15, 2017, the contents of which are incorporated by reference in their entirety. Electrolyte Separator

[0098] In some examples, the electrolyte separator is selected from the groupconsisting of a lithium-stuffed garnet, a sulfide electrolyte doped with oxygen, a sulfide electrolyte comprising oxygen, a lithium aluminum titanium oxide, a lithium aluminum titanium phosphate, a lithium aluminum germanium phosphate, a lithium aluminum titanium oxy-phosphate, a lithium lanthanum titanium oxide perovskite, a lithium lanthanum tantalum oxide perovskite, a lithium lanthanum titanium oxide perovskite, an antiperovskite, a LISICON, a LI-S-O-N, lithium aluminum silicon oxide , a Thio-LISICON, a lithium-Attorney Docket No.114826.00834 415.601 substituted NASICON, a LIPON, or a combination, mixture, or multilayer thereof. In some examples, the electrolyte separator is an oxide electrolyte separator.

[0099] In some examples, the electrolyte separator has a surface roughness Ra or Rt,on at least one surface, from about 0.1 µm to 10 µm. In other examples, the electrolyte separator has a surface roughness, on at least one surface, from about 0.1 µm to 5 µm. In other examples, the electrolyte separator has a surface roughness, on at least one surface, from about 0.1 µm to 2 µm. In some examples, the electrolyte has a surface roughness from about 0.1 µm to 10 µm at the surface that interfaces the electrolyte separator and the Li metal negative electrode.[000100] In some examples, the electrolyte separator has a density greater than 95% ofits theoretical density. In other examples, the electrolyte separator has a density greater than 95% of its theoretical density as determined by scanning electron microscopy (SEM).[000101] In certain examples, the electrolyte separator has a density greater than 95% ofits theoretical density as measured by the Archimedes method. In some examples, the electrolyte separator has a surface flatness of 0.1 µm to about 50 µm. Positive Electrode Layer[000102] In some examples, the positive electrode includes a lithium intercalationmaterial, a lithium conversion material, or both a lithium intercalation material and a lithium conversion material. In some examples, the lithium intercalation material is selected from a nickel manganese cobalt oxide Li(NiCoMn)O2, (NMC), a nickel cobalt aluminum oxide (NCA), Li(NiCoAl)O2, a lithium cobalt oxide (LCO), a lithium manganese cobalt oxide (LMCO), a lithium nickel manganese cobalt oxide (LMNCO), a lithium nickel manganese oxide (LNMO), LiMn2O4, LiCoO2,LiMn2-aNiaO4, wherein a is from 0 to 2, or LiMPO4, wherein M is Fe, Ni, Co, or Mn. In others, the lithium conversion material is selected from the group consisting of FeF2, NiF2, FeOxF3-2x, FeF3, MnF3, CoF3, CuF2materials, alloys thereof, and combinations thereof. In others, the conversion material is doped with other transition metal fluorides or oxides.[000103] In some examples, the positive electrode further includes a catholyte. In someexamples, the catholyte is a gel electrolyte. In some examples, the positive electrode includes a gel catholyte. In some examples, the positive electrode includes a gel catholyte comprising, a solvent selected from the group consisting of ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), methylene carbonate, and combinations thereof; a polymerAttorney Docket No.114826.00834 415.601 selected from the group consisting of PVDF-HFP and PAN; and a salt selected from the group consisting of LiPF6, LiBOB, and LFTSi.[000104] In some examples, the positive electrode further includes a binder polymerselected from the group consisting of polypropylene (PP), atactic polypropylene (aPP), isotactive polypropylene (iPP), ethylene propylene rubber (EPR), ethylene pentene copolymer (EPC), polyethylene oxide (PEO), PEO block copolymers, polyethylene glycol, polyisobutylene (PIB), styrene butadiene rubber (SBR), a polyolefin, polyethylene-co-poly-1- octene (PE-co-PO) copolymer, PE-co-poly(methylene cyclopentane) (PE-co-PMCP) copolymer, stereoblock polypropylenes, polypropylene polymethylpentene copolymer, acrylics, acrylates, polyvinyl butyral, vinyl polymers, cellulose polymers, resins, polyvinyl alcohol, polymethyl methacrylate, polyvinyl pyrrolidone, polyacrylamide, silicone, PVDF, PVDF-HFP, PAN and combinations thereof. In some examples, the binder polymer is the same polymer as that which is used as a polymer in the bonding layer. In some examples, the positive electrode and / or bonding layer may include poly-ethylene carbonate, polyphenylene sulfide, and / or poly-propylene carbonate. Method of Making the Bonding Layer[000105] In some examples, set forth herein is a method of making a bonding layer.This method, in some examples, includes mixing a lithium salt (e.g., LiBr, LiI, or both) in a 1:1 by volume ratio of methanol to isopropanol, wherein the solution is dried. The dried composition can be melted at least 90°C for at least 30 minutes, followed by cooling the composition to room temperature (25°C) for at least 30 minutes.[000106] In some examples, to form the gel bonding layer, a solvent is provided andmixed with a polymer and a lithium salt. In some examples, the solvent is volatilized to concentrate the solvent and lithium salt into a gel.[000107] U.S. Provisional Application No. U.S. 63 / 333,501, which was filed April 21,2022, entitled, SOLVENT-LESS CATHODE COMPOSITION AND PROCESS FOR MAKING, is incorporated by reference herein in its entirety for all purposes. EXAMPLES[000108] Differential scanning calorimetry (DSC) was obtained by using Netzsch STA449 F3 Jupiter.Attorney Docket No.114826.00834 415.601[000109] Instruments used for electrochemical measurements were Bio-Logicpotentiostat, Arbin Instruments battery cyclers, and Maccor battery cyclers.[000110] Reagents, chemicals, and materials were commercially purchased unlessspecified otherwise to the contrary.[000111] Pouch cell containers were purchased from Showa Denko.[000112] The Electrochemical potentiostat used was an Arbin potentiostat.[000113] Electrical impedance spectroscopy (EIS) was performed with a BiologicVMP3, VSP, VSP-300, SP- 150, or SP-200.[000114] Milling was performed using a Retsch PM 400 Planetary Ball Mill. Mixingwas performed using a Fischer Scientific vortex mixer, a Flaktek speed mixer, or a Primix filmix homogenizer.[000115] Casting was performed on a TQC drawdown table. Calendering wasperformed on an IMC calender.[000116] Light scattering was performed on a Horiba, model: Partica, Model No.:LA-950V2, which is a laser scattering particle size distribution analyzer.[000117] The Lithium Nickel Cobalt Manganese Oxide (NMC) used in the Exampleswas LiNi0.8Co0.1Mn0.1O2 unless specified otherwise. EXAMPLE 1[000118] FIG. 1 is an SEM image of an example of the electrochemical cell disclosedherein. The image shows a positive electrode layer including a cathode active material (NMC) and catholyte material (LPSCl) with PTFE. A buffer layer of LSTPS is between the positive electrode layer and the electrolyte separator. The bonding layer of LBHIN adheres the buffer layer to the garnet-based electrolyte separator. EXAMPLE 2[000119] A LiI-4-isopropanol (LiI-4-iPrOH) bonding layer was synthesized and coatedon a lithium-stuffed garnet-based electrolyte separator. In one example, LiI was mixed in a 1:1 by volume ratio of methanol to isopropanol. The mixture was then dried. In another example, LiBr was mixed in a 1:1 by volume ratio of methanol to isopropanol. The dried composition was melted at 90°C for 30 minutes in Argon. Then the dried composition was cooled to room temperature (25°C) for 30 minutes. This process was repeated twice. The LiI-Attorney Docket No.114826.00834 415.601 4-isopropanol on the lithium-stuffed garnet electrolyte separator (LiI-4-iPrOH-LSTPS) reversibly melts at 80°C on a hot plate.[000120] FIGS. 1-2 show DSC as a function of temperature for the LiI-4-isopropanolmixture and the LiI-4-iPrOH-LSTPS in Example 1. Samples were scanned from 10 to 110 °C at a ramp rate of 5 °C per minute. Two cycles were run[000121] The graphs illustrate a melting peak at 90°C. The graphs illustrate reversiblemelting for the LiI-4-isopropanol sample (FIG.1) as compared to the LiI-4-isopropanol on LSTPS (FIG.2). EXAMPLE 3[000122] A lithium-stuffed garnet separator was made and co-sintered with a currentcollector. The lithium-stuffed garnet separator was heated to 80 °C. The LiI-4-isopropanol was then added to the lithium-stuffed garnet separator. On top of this, a layer of LSTPS was added. This stack was then hot-pressed. A positive electrode layer was then added on top of the LSTPS layer. ASR was measured at -10°C and 30 °C[000123] A low area-specific resistance (ASR) was achieved at 30 °C and -10 °C for theLiI-4-isopropanol bonding layer. Specifically, the average ASR for the LSTPS, bonding layer of LiI-4-isopropanol, and CSC at 30 °C is 12.6 Ωcm2. The average ASR for the LSTPS, bonding layer of LiI-4-isopropanol, and CSC at -10 °C is 192.2 Ωcm2.[000124] The average activation barrier was determined to be 0.459 eV for the bondinglayer of LiI-4-isopropanol, and 0.76 eV for a bonding layer of LBHIN. This was done using the Arrhenius equation and using multiple ASR measurements at a series of temperatures. EXAMPLE 4[000125] As shown in FIGs. 3A-3C, a mixture of LiBr and isopropanol in a 1:4 ratio byvolume was mixed in the presence of Argon, melted at 70°C for 30 minutes, cooled on a cold plate power 50% for 15 minutes, wherein the heating and cooling steps were repeated two times. The bonding layer was coated on a lithium-stuffed garnet-based electrolyte separator, which is then attached to an LSTPS film.Attorney Docket No.114826.00834 415.601 EXAMPLE 5[000126] A lithium-stuffed garnet separator was made and co-sintered with a currentcollector. This is called a CSC layer. The lithium-stuffed garnet separator was heated to 80 °C. The LiI-4-isopropanol was then added to the lithium-stuffed garnet separator. On top of this, a layer of LSTPS was added. This stack was then hot-pressed. A positive electrode layer was then added on top of the LSTPS layer.[000127] ASR was measured at -10°C and 30 °C. The cell build had an area of 0.5 cm2.The cell build was a circular coin cell.[000128] The average ASR for the LSTPS, bonding layer of LiBr-isopropanol, and CSCat 30°C is 11.7 Ωcm2. The average ASR for the LSTPS, bonding layer of LiBr-isopropanol, and CSC at -10°C is 21765 Ωcm2. EXAMPLE 6[000129] A mixture of LiBr and methanol in a 1:4 ratio by volume was mixed in thepresence of Argon, melted at 70°C for 30 minutes, cooled in a freezer for 30 minutes, wherein the heating and cooling steps were repeated two times. The bonding layer was coated on a garnet-based electrolyte separator at 40°C, which is then attached to an LSTPS film.[000130] The average ASR for the LSTPS, bonding layer of LiBr-methanol, andlithium-stuffed garnet separator co-sintered with a current collector at 30°C is 12.1 Ωcm2. The average ASR for the LSTPS, bonding layer of LiBr-methanol, and lithium-stuffed garnet separator co-sintered with a current collector at -10°C is 100.58 Ωcm2.[000131] The average activation barrier for the LiBr-methanol bonding layer is 0.360eV. The average activation barrier for the LiI-4-isopropanol bonding layer is 0.459. The average activation energy for the LBHIN bonding layer is 0.76 eV.[000132] For the bonding layer of LiBr-MeOH at a ratio of 1:4, no cycling plateau wasobserved below 3.6 V. EXAMPLE 7[000133] A gel bonding layer was synthesized from a mixture of 1 mol / L of LiPF6(dried) and 4 mol / L LiTSFI (dried) in a 1,3-dioxolane (DOL) : dimethoxyethane (DME) (1:1 ratio by volume). The mixture was shaken under Argon, heated under Argon to 70°C for two hours, and cooled to room temperature.Attorney Docket No.114826.00834 415.601 EXAMPLE 8[000134] The XRD pattern of LSTPS is shown in FIG. 4.[000135] LSTPS was immersed in DOL for 12 hours at 60 °C in Ar. The product wasfiltered and dried. The XRD pattern is shown in FIG.4.[000136] LSTPS was immersed in DME for 12 hours at 60 °C in Ar. The product wasfiltered and dried. The XRD pattern is shown in FIG.4.[000137] The polysulfide side products dissolved in the bonding layer such that nofixtures were detected at 30°C or 10°C, nor at 60°C at 51 days.[000138] As shown in FIGS. 4-5, the conductivity as evidenced by XRD and XPS ofLSTPS remains the same after overnight DOL and DME treatment. EXAMPLE 9[000139] An LSTPS was immersed in dioxolane (DOL) overnight at 60 °C underArgon, then filtered and dried. An LSTPS was immersed in dimethoxyethane (DME) overnight at 60 °C under Argon, then filtered and dried. An LSTPS was made as a control. The XPS of the LSTPS immersed in DOL or DME remained the same after overnight.[000140] The embodiments and examples described above are intended to be merelyillustrative and non-limiting. Those skilled in the art will recognize or will be able to ascertain using no more than routine experimentation, numerous equivalents of specific compounds, materials and procedures. All such equivalents are considered to be within the scope and are encompassed by the appended claims.

Claims

Attorney Docket No.114826.00834 415.601 CLAIMS1. A composition comprising:a lithium salt, wherein the lithium salt is LiI, LiBr, LiCl, or a combination thereof; and an alcohol, wherein the alcohol is methanol, isopropanol, or a combination thereof; wherein the concentration of the lithium salt is present at 1 M – 5M; wherein the composition is a solid at standard atmospheric pressure and temperatures less than 80 C.

2. The composition of claim 1, wherein the lithium salt is present at 1M concentration.

3. The composition of any one of claims 1-2, wherein the lithium salt is LiI.

4. The composition of any one of claims 1-2, wherein the lithium salt is LiCl.

5. The composition of any one of claims 1-2, wherein the lithium salt is LiBr.

6. The composition of any one of claims 1-5, wherein the lithium salt is a combination ofLiI, LiCl, and LiBr.

7. The composition of claim 3, wherein the composition melts at 80 °C at standardatmospheric pressure (1 atm).

8. The composition of claim 4, wherein the composition melts at 85 °C at standardatmospheric pressure (1 atm).

9. The composition of claim 5, wherein the composition melts at 90 °C at standardatmospheric pressure (1 atm).

10. The composition of any one of claims 1-9, wherein the composition has a DifferentialScanning Calorimetry (DSC) profile substantially as shown in FIG.2.

11. The composition of any one of claims 1-9, wherein the composition has a DSC profilesubstantially as shown in FIG.3.

12. A composition comprising:a lithium salt, wherein the lithium salt is LiTFSI, LiFSI, LiPF6, LiClO4, LiAsF6, LiBOB, LiBETI, LiBF4, or a combination thereof; andAttorney Docket No.114826.00834 415.601 an organic solvent, wherein the organic solvent is 1,3-dioxolane (DOL), dimethoxyethane (DME), or a combination thereof; wherein concentration of the lithium salt is 1 M – 5M; wherein the composition is a solid.

13. The composition of claim 12, wherein the lithium salt is present at 1M concentration.

14. The composition of any one of claims 12-13, wherein volume ratio of DOL:DME is 1:4.

15. The composition of any one of claims 12-13, wherein volume ratio of DOL:DME is1:

1.

16. The composition of any one of claims 12-15, further comprising lithium salts LiPF6and LiTFSi.

17. The composition of any one of claims 12-15, further comprising 1M LiPF6 and 1MLiTFSi.

18. The composition of any one of claims 12-15, wherein further comprising 1M LiPF6and 4M LiTFSi.

19. The composition of any one of claims 12-15, wherein further comprising 4M LiPF6 and4M LiTFSi.

20. A solid-state battery comprising:a positive electrode layer comprising cathode active material and catholyte material; a bonding layer, wherein the bonding layer includes a composition comprising at least one lithium salt and at least one alcohol, wherein the lithium salt is present at 1 M – 5 M concentration, wherein the lithium salt is LiI, LiBr, LiCl, or a combination thereof; wherein the alcohol is methanol, isopropanol, or a combination thereof; and an electrolyte separator comprising a lithium-stuffed garnet; wherein the bonding layer is in contact with the positive electrode layer and the electrolyte separator. .

21. The solid-state battery of claim 20, further comprising a solid-state buffer layer, whereinthe solid-state buffer layer is in contact with the positive electrode layer and the solid bonding layer.Attorney Docket No.114826.00834 415.60122. The solid-state battery of any one of claims 20-21, wherein the composition of thebonding layer is a solid composition of LiI-isopropyl alcohol.

23. The solid-state battery of any one of claims 20-21, wherein the composition of thebonding layer is a solid composition of LiBr-methanol.

24. The solid-state battery of any one of claims 20-21, wherein the composition of thebonding layer is a solid composition of LBHIN.

25. The solid-state battery of any one of claims 20-24, wherein the ratio by volume of thelithium salt to alcohol is 1:3 to 1:6.

26. The solid-state battery of any one of claims 20-25, wherein the cathode active materialcomprises a lithium intercalation material, a lithium conversion material, or a combination thereof27. The solid-state battery of claim 26, wherein the lithium intercalation material is selectedfrom the group consisting of a nickel manganese cobalt oxide (NMC), a nickel cobalt aluminum oxide (NCA), Li(NiCoAl)O2, a lithium cobalt oxide (LCO), a lithium manganese cobalt oxide (LMCO), a lithium nickel manganese cobalt oxide (LMNCO), a lithium nickel manganese oxide (LNMO), Li(NiCoMn)O2, LiMn2O4, LiCoO2, LiMn2-aNiaO4, wherein a is from 0 to 2, or LiMPO4, wherein M is Fe, Ni, Co, and Mn.

28. The solid-state battery of any one of claims 20-27, further comprising a catholytematerial, wherein the catholyte material is LSTPS or LSPSCl.

29. The solid-state battery of any one of claims 20-28, comprising:a. LiI;b. MeOH; andc. iPrOH.

30. The solid-state battery of any one of claims 20-29, having a cathode active loading of 20- 100 mAh / cm2< / sup>.

31. The solid-state battery of any one of claims 20-29, having a cathode active loading of 20mAh / cm2< / sup>.

32. The solid-state battery of any one of claims 20-29, having a cathode active loading of 40mAh / cm2.Attorney Docket No.114826.00834 415.60133. The solid-state battery of any one of claims 20-29, having a cathode active loading of 60mAh / cm2< / sup>.

34. The solid-state battery of any one of claims 20-29, having a cathode active loading of 80mAh / cm2< / sup>.

35. A solid-state battery comprising:a positive electrode layer comprising a cathode active material and a catholyte material; a bonding layer, wherein the bonding layer includes a composition including a lithium salt and an organic solvent, wherein the solvent is 1,3-dioxolane (DOL), dimethoxyethane (DME), or a combination thereof; and an electrolyte separator comprising a lithium-stuffed garnet; wherein the bonding layer is in contact with the solid-state buffer layer and the electrolyte separator.

36. The solid-state battery of claim 35, further comprising a solid-state buffer layer, whereinthe solid-state buffer layer is in contact with the positive electrode layer and the solid bonding layer.

37. The solid-state battery of any one of claims 35-36, wherein the lithium salt is LiTFSI,LiFSI, LiPF6, LiClO4, LiAsF6, LiBOB, LiBETI, LiBF4, or combinations thereof.

38. The solid-state battery of any one of claims 35-37, wherein the lithium salt is LiClO4,LiAsF6, LiBOB, LiBETI, LiBF4, or a combination thereof.

39. The solid-state battery of any one of claims 35-37, wherein the lithium salt is LiTFSI,LiFSI, LiPF6, or combinations thereof.

40. The solid-state battery of any one of claims 35-39, further comprising a solvent selectedfrom 1,3-dioxolane, dimethoxyethane, or combinations thereof.

41. The solid-state battery of any one of claims 35-40, wherein the composition of thebonding layer is a gel composition of LiTFSI at 4 mol / L, LiPF6 at 1 mol / L, and a 1:1 mixture by volume of 1,3-dioxolane and dimethoxyethane.

42. The solid-state battery of any one of claims 35-41 wherein the bonding layer is a gel.Attorney Docket No.114826.00834 415.60143. The solid-state battery of any one of claims 35-42, wherein the cathode active materialcomprises a lithium intercalation material, a lithium conversion material, or a combination thereof.

44. The solid-state battery of claim 43, wherein the lithium intercalation material is selectedfrom the group consisting of a nickel manganese cobalt oxide (NMC), a nickel cobalt aluminum oxide (NCA), Li(NiCoAl)O2, a lithium cobalt oxide (LCO), a lithium manganese cobalt oxide (LMCO), a lithium nickel manganese cobalt oxide (LMNCO), a lithium nickel manganese oxide (LNMO), Li(NiCoMn)O2, LiMn2O4, LiCoO2, LiMn2- aNiaO4, wherein a is from 0 to 2, or LiMPO4,wherein M is Fe, Ni, Co, and Mn.

45. The solid-state battery of any one of claims 35-44, further comprising a catholytematerial, wherein the catholyte material is LSTPS or LSPSCl.

46. A process for making a bonding layer, comprising:mixing dried LiI, LiBr, or a combination thereof, with an alcohol, wherein the alcohol is selected from methanol, isopropanol, or a combination thereof; wherein the lithium salt is present at 1 M – 5M concentration; wherein, after the mixing, the composition is a solid at standard atmospheric pressure and room temperature.

47. A process for making a composition comprising: a lithium salt, wherein the lithium salt is LiTFSI, LiFSI, LiPF6, LiClO4, LiAsF6, LiBOB, LiBETI, LiBF4, or a combination thereof; and an organic solvent, wherein the organic solvent is 1,3-dioxolane (DOL), dimethoxyethane (DME), or a combination thereof; wherein concentration of the lithium salt is 1 M – 5M; wherein the composition is a solid.

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