Solid-state bipolar battery containing ion gel

Abstract

A high temperature stable solid bipolar battery is provided. The battery includes two or more electrodes, one or more solid electrolyte layers, and an ion gel disposed in a void space in the battery. Each electrode includes a plurality of solid electroactive particles. Each solid electrolyte layer includes a plurality of solid electrolyte particles, and a first solid electrolyte layer in the one or more solid electrolyte layers may be disposed between a first electrode and a second electrode of the two or more electrodes. The ion gel is disposed in the void space between the two or more electrodes, the solid electroactive particles of the two or more electrodes, the solid electrolyte particles of the one or more solid electrolyte layers, and the one or more solid electrolyte layers, so that the battery has a reduced inter-particle porosity. The ion gel may have an ionic conductivity of about 0.1 mS / Cm to about 10 mS / Cm.

Description

[0001] introduction

[0002] This section provides background information related to the present disclosure which is not necessarily prior art.

[0003] Electrochemical energy storage devices such as lithium-ion batteries can be used in a variety of products, including automotive products such as start-stop systems (e.g., 12V start-stop systems), battery auxiliary systems ("µBAS"), hybrid electric vehicles ("HEV"), and electric vehicles ("EV"). A typical lithium-ion battery contains two electrodes and an electrolyte assembly and / or a separator. One of the two electrodes can serve as a positive electrode or cathode, and the other electrode can serve as a negative electrode or anode. The lithium-ion battery can also include various terminals and packaging materials. Rechargeable lithium-ion batteries operate by reversibly transferring lithium ions back and forth between a negative electrode and a positive electrode. For example, during charging of the battery, lithium ions can move from the positive electrode to the negative electrode, and move in the opposite direction when the battery is discharged. A separator and / or an electrolyte can be disposed between the negative electrode and the positive electrode. The electrolyte is suitable for conducting lithium ions between the electrodes, and like the two electrodes, can be in solid form, liquid form, or a solid-liquid hybrid form. In the case of a solid-state battery including a solid electrolyte layer disposed between solid electrodes, the solid electrolyte layer physically separates the solid electrodes, thereby eliminating the need for a separate separator.

[0004] Solid-state batteries have advantages over batteries including separators and liquid electrolytes. These advantages may include longer shelf life and lower self-discharge, simpler thermal management, reduced packaging requirements, and the ability to operate in a wider temperature window. For example, solid electrolytes are generally non-volatile and non-flammable, allowing the battery to circulate under more severe conditions without potential reduction or thermal runaway, which may occur when using liquid electrolytes. However, solid-state batteries generally experience relatively low power capacity. For example, such low power capacity may be due to the interface resistance in and / or at the solid-state electrode, and the solid electrolyte layer interface resistance caused by limited contact or void space between solid-state active particles and / or solid-state electrolyte particles. Therefore, it is desirable to develop high-performance solid-state battery materials and methods that can improve the contact and / or interaction (e.g., microinterface) between solid-state active particles and / or solid-state electrolyte particles, the contact and / or interaction (e.g., microinterface) between solid-state electrodes and solid-state electrolyte layers, and / or mitigate the impact of void space in solid-state batteries. SUMMARY OF THE INVENTION

[0005] This section provides a general summary of the disclosure, and is not a comprehensive disclosure of its full scope or all of its features.

[0006] The present disclosure relates to a solid-state battery, such as a solid-state bipolar battery, comprising an ion gel that wets the interface between solid electrolyte particles and / or solid active material particles to reduce interparticle porosity and improve ionic contact. The solid-state battery, such as a bipolar solid-state battery, may further include a polymer blocker configured to contact one or more adjacent current collectors to reduce potential ionic short circuits. The present disclosure also relates to a method for introducing an ion gel and / or a polymer blocker.

[0007] In various aspects, the present disclosure provides a solid-state battery pack comprising two or more electrodes, one or more solid electrolyte layers, and an ion gel disposed in a void space. Each electrode may include a plurality of solid-state electroactive particles. Each solid electrolyte layer may include a plurality of solid electrolyte particles, wherein the first solid electrolyte layer in the one or more solid electrolyte layers is disposed between the first electrode and the second electrode of the two or more electrodes. The ion gel is disposed in the void space between the two or more electrodes, the solid-state electroactive particles of the two or more electrodes, the solid electrolyte particles of the one or more solid electrolyte layers, and the one or more solid electrolyte layers, so that the solid-state battery pack has an inter-particle porosity of less than or equal to about 20% by volume. The ion gel may have an ionic conductivity of greater than or equal to about 0.1 mS / cm to less than or equal to about 10 mS / cm.

[0008] In one aspect, the ionic gel can include greater than or equal to about 30 wt % to less than or equal to about 95 wt % of the ionic liquid and greater than or equal to about 2 wt % to less than or equal to about 40 wt % of the solid component.

[0009] In one aspect, the solid component can include at least one of an organic polymer, an inorganic oxide, a polymer / oxide hybrid, and a metal-organic framework (MOF).

[0010] In one aspect, the organic polymer can be selected from: poly(ethylene oxide) (PEO) (where 1,000≤n≤10,000,000), poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF=HFP) (where 1,000≤x≤10,000,000 and 1,000≤y≤10,000,000), poly(methyl methacrylate) (PMMA) (where 1,000≤n≤10,000,000), carboxymethyl cellulose (CMC) (where 1,000≤n≤10,000,000), polyacrylonitrile (PAN) (where 1,000≤n≤10,000,000), polyvinylidene fluoride (PVDF) (where 1,000≤n≤10,000,000). 0,000), one or more poly(vinyl alcohol) (PVA) (wherein 1,000≤n≤10,000,000), one or more polyvinyl pyrrolidone (PVP) (wherein 1,000≤n≤10,000,000) and combinations thereof; the inorganic oxide may be selected from: SiO2, Al2O3, TiO2, ZrO2 and combinations thereof; the polymer / oxide mixture may include one or more of the organic polymers and one or more of the inorganic oxides; and one or more metal-organic frameworks (MOFs) may be selected from: MIL-101, UiO-67, ZIF-8 and combinations thereof.

[0011] In one aspect, the ionic liquid comprises a cation and an anion. The cation may be selected from: Li(triglyme)methylimidazolium ([Li(G3)] + )、Li(tetraethylene glycol dimethyl ether)([Li(G4) + ])、1-ethyl-3([Emim] + )、1-propyl-3-methylimidazolium([Pmim] + )、1-butyl-3-methylimidazolium([Bmim] + )、1,2-dimethyl-3-butylimidazolium([DMBim])、1-alkyl-3-methylimidazolium([Cnmim] + )、1-allyl-3-methylimidazolium([Amim] + )、1,3-diallylimidazolium([Daim] + )、1-allyl-3-vinylimidazolium([Avim] + ); 1-vinyl-3-ethylimidazolium ([Veim] + )、1-cyanomethyl-3-methylimidazolium([MCNim] + )、1,3-Dicyanomethyl-imidazolium([BCNim] + ), 1-propyl-1-methylpiperidinium ([PP 13 ]+ )、1-butyl-1-methylpiperidinium([PP 14 ] + ), 1-methyl-1-ethylpyrrolidinium ([Pyr 12 ] + ), 1-propyl-1-methylpyrrolidinium ([Pyr 13 ] + )、1-butyl-1-methylpyrrolidinium([Pyr 14 ] + ), methyl-methylcarboxymethyl-pyrrolidinium ([MMMPyr] + ), tetramethylammonium ([N 1111 ] + ), tetraethylammonium ([N 2222 ] + ), tributylmethylammonium ([N 4441 ] + ), diallyldimethylammonium ([DADMA] + ); NN-diethyl-N-methyl-N-(2-methoxyethyl)ammonium ([DEME] + )、N,N-diethyl-N-(2-methacryloylethyl)-N-methylammonium([DEMM] + ), trimethyl isobutyl-phosphonium ([P 111i4 ] + ), triisobutylmethylphosphonium ([P 1i444 ] + ), tributylmethylphosphonium ([P 1444 ] + ), diethylmethylisobutylphosphonium ([P 1224 ] + )、trihexyldecylphosphonium([P 66610 ] + ), trihexyltetradecylphosphonium ([P 66614 ] + ) and combinations thereof. The anion may be selected from the group consisting of hexafluoroarsenate, hexafluorophosphate, bis(fluorosulfonyl)imide (FSI), bis(trifluoromethanesulfonyl)imide (TFSI), perchlorate, tetrafluoroborate, cyclo-difluoromethane-1,1-bis(sulfonyl)imide (DMSI), bis(perfluoroethanesulfonyl)imide (BETI), bis(oxalate)borate (BOB), difluoro(oxalato)borate (DFOB), bis(fluoromalonate)borate (BFMB) and combinations thereof.

[0012] In one aspect, the ionic liquid can further include a low boiling point solvent selected from the group consisting of dimethyl carbonate, ethylene carbonate, ethyl acetate, acetonitrile, acetone, toluene, propylene carbonate, diethyl carbonate, 1,2,2-tetrafluoroethyl, 2,2,3,3-tetrafluoropropyl ether, and combinations thereof.

[0013] In one aspect, the ion gel may further include greater than 0 wt % to less than about 40 wt % of one or more lithium salts. Each lithium salt includes an anion selected from hexafluoroarsenate, hexafluorophosphate, bis(fluorosulfonyl)imide (FSI), perchlorate, tetrafluoroborate, cyclo-difluoromethane-1,1-bis(sulfonyl)imide (DMSI), bis(trifluoromethanesulfonyl)imide (TFSI), bis(perfluoroethanesulfonyl)imide (BETI), bis(oxalate)borate (BOB), difluoro(oxalato)borate (DFOB), and bis(fluoromalonate)borate (BFMB).

[0014] In one aspect, the solid electrolyte layer may include a first layer comprising a first plurality of solid electrolyte particles and a second layer comprising a second plurality of solid electrolyte particles, wherein the first and second plurality of solid electrolyte particles are the same or different, and the first and second plurality of solid electrolyte particles define the plurality of solid electrolyte particles.

[0015] In one aspect, the solid-state battery can further include two or more current collectors, wherein a first current collector of the two or more current collectors is disposed adjacent to the first electrode, and a second current collector of the two or more current collectors is disposed adjacent to the second electrode.

[0016] In one aspect, at least one of the first and second current collectors includes a first half comprising a first material and a second half comprising a second material, wherein the second half is substantially parallel to the first half, and the first and second materials are different.

[0017] In one aspect, the solid-state battery pack may further include a polymer barrier, wherein the polymer barrier contacts the first current collector to the second current collector. The polymer barrier may have a thickness of greater than or equal to about 2 μm to less than or equal to about 200 μm. The polymer barrier includes an insulating material selected from the group consisting of polyurethane resin, polyamide resin, polyolefin resin, polyethylene resin, polypropylene resin, ethylene, propylene, butylene, silicone, polyimide resin, epoxy resin, acrylic resin, ethylene-propylene diene rubber (EPDM), isocyanate adhesive, acrylic resin adhesive, cyanoacrylate adhesive, and combinations thereof.

[0018] In one aspect, the solid-state battery can be a bipolar battery, wherein the two or more electrodes include a first electrode, a second electrode and one or more bipolar electrodes, the plurality of solid-state electroactive particles include a first plurality of solid-state electroactive particles and a second plurality of solid-state electroactive particles, and the one or more solid-state electrolyte layers include a first solid-state electrolyte layer and a second solid-state electrolyte layer. Each bipolar electrode may include a current collector. The first plurality of solid-state electroactive particles may be disposed on a first side of the current collector, and the second plurality of solid-state electroactive particles may be disposed on a second side of the current collector. The first solid-state electrolyte layer may be disposed between the first electrode and the first side of the one or more bipolar electrodes, and the second solid-state electrolyte may be disposed between the second side of the one or more bipolar electrodes and the second electrode. The ion gel may be further disposed in the void space between the first plurality of solid-state electroactive particles and the second plurality of solid-state electroactive particles, the first solid-state electrolyte layer and the first electrode, one or more bipolar electrodes, one or more bipolar electrodes and the first solid-state electrolyte layer, one or more bipolar electrodes and the second solid-state electrolyte layer, and the second solid-state electrolyte layer and the second electrode.

[0019] In various other aspects, the present disclosure provides a solid-state electrode comprising a plurality of solid-state electroactive particles and an ion gel disposed in the void spaces between the solid-state electroactive particles, such that the solid-state electrode has an inter-particle porosity of less than or equal to about 20% by volume. The ion gel may have an ionic conductivity of greater than or equal to about 0.1 mS / cm to less than or equal to about 10 mS / cm.

[0020] In one aspect, the plurality of solid electroactive particles may define an electrode layer. The solid electrode may further include a solid electrolyte layer disposed adjacent to the electrode layer. The solid electrolyte layer may include a plurality of solid electrolyte particles. The ion gel may further be disposed in gaps between the solid electrolyte particles and between the solid electrolyte layer and the electrode layer.

[0021] In one aspect, the ion gel may include greater than or equal to about 30 wt % to less than or equal to about 95 wt % of an ionic liquid and greater than or equal to about 2 wt % to less than or equal to about 40 wt % of a solid component. The ionic liquid may include cations and anions, and the solid component may include at least one of an organic polymer, an inorganic oxide, a polymer / oxide mixture, and a metal-organic framework (MOF).

[0022] In one aspect, the ionic liquid may include a cation selected from the group consisting of: Li(triglyme)methylimidazolium ([Li(G3)] + )、Li(tetraethylene glycol dimethyl ether)([Li(G4) +])、1-ethyl-3([Emim] + )、1-propyl-3-methylimidazolium([Pmim] + )、1-butyl-3-methylimidazolium([Bmim] + )、1,2-dimethyl-3-butylimidazolium([DMBim])、1-alkyl-3-methylimidazolium([Cnmim] + )、1-allyl-3-methylimidazolium([Amim] + )、1,3-diallylimidazolium([Daim] + )、1-allyl-3-vinylimidazolium([Avim] + ); 1-vinyl-3-ethylimidazolium ([Veim] + )、1-cyanomethyl-3-methylimidazolium([MCNim] + )、1,3-Dicyanomethyl-imidazolium([BCNim] + ), 1-propyl-1-methylpiperidinium ([PP 13 ] + )、1-butyl-1-methylpiperidinium([PP 14 ] + ), 1-methyl-1-ethylpyrrolidinium ([Pyr 12 ] + ), 1-propyl-1-methylpyrrolidinium ([Pyr 13 ] + )、1-butyl-1-methylpyrrolidinium([Pyr 14 ] + ), methyl-methylcarboxymethyl-pyrrolidinium ([MMMPyr] + ), tetramethylammonium ([N 1111 ] + ), tetraethylammonium ([N 2222 ] + ), tributylmethylammonium ([N 4441 ] + ), diallyldimethylammonium ([DADMA] + ); NN-diethyl-N-methyl-N-(2-methoxyethyl)ammonium ([DEME] + )、N,N-diethyl-N-(2-methacryloylethyl)-N-methylammonium([DEMM] + ), trimethyl isobutyl-phosphonium ([P 111i4 ] + ), triisobutylmethylphosphonium ([P 1i444 ] + ), tributylmethylphosphonium ([P 1444 ] +), diethylmethylisobutylphosphonium ([P 1224 ] + )、Trihexyldecylphosphonium([P 66610 ] + ), trihexyltetradecylphosphonium ([P 66614 ] + ) and their combinations.

[0023] In one aspect, the ionic liquid may include an anion selected from the group consisting of hexafluoroarsenate, hexafluorophosphate, bis(fluorosulfonyl)imide (FSI), bis(trifluoromethanesulfonyl)imide (TFSI), perchlorate, tetrafluoroborate, cyclo-difluoromethane-1,1-bis(sulfonyl)imide (DMSI), bis(perfluoroethanesulfonyl)imide (BETI), bis(oxalato)borate (BOB), difluoro(oxalato)borate (DFOB), bis(fluoromalonato)borate (BFMB), and combinations thereof.

[0024] In one aspect, the ionic liquid may further include a low boiling point solvent. The low boiling point solvent may be selected from the group consisting of dimethyl carbonate, ethylene carbonate, ethyl acetate, acetonitrile, acetone, toluene, propylene carbonate, diethyl carbonate, 1,2,2-tetrafluoroethyl, 2,2,3,3-tetrafluoropropyl ether and combinations thereof.

[0025] In one aspect, the ion gel may further include greater than 0 wt % to less than about 40 wt % of one or more lithium salts. Each lithium salt includes an anion selected from hexafluoroarsenate, hexafluorophosphate, bis(fluorosulfonyl)imide (FSI), perchlorate, tetrafluoroborate, cyclo-difluoromethane-1,1-bis(sulfonyl)imide (DMSI), bis(trifluoromethanesulfonyl)imide (TFSI), bis(perfluoroethanesulfonyl)imide (BETI), bis(oxalate)borate (BOB), difluoro(oxalato)borate (DFOB), and bis(fluoromalonate)borate (BFMB).

[0026] Further areas of applicability will become apparent from the description provided herein.The description and specific examples in this summary are intended for purposes of illustration only and are not intended to limit the scope of the present disclosure. BRIEF DESCRIPTION OF THE DRAWINGS

[0027] The drawings described herein are illustrative only of selected embodiments and not all possible implementations, and are not intended to limit the scope of the present disclosure.

[0028] Figure 1A is a diagram of an example solid-state battery pack;

[0029] Figure 1B is a diagram of an example solid-state battery with an ion gel according to various aspects of the present technology;

[0030] Figure 2A is an illustration of an example negative electrode including a solid electrolyte layer disposed on an exposed surface thereof in accordance with various aspects of the present technology;

[0031] Figure 2B is an illustration of an example positive electrode including a solid electrolyte layer disposed on an exposed surface thereof in accordance with various aspects of the present technology;

[0032] Figure 2C is an illustration of an example solid-state battery according to various aspects of the present technology, wherein the solid-state electrolyte layer comprises a first solid-state electrolyte layer disposed on an exposed surface of a negative electrode and a second solid-state electrolyte layer disposed on an exposed surface of a positive electrode;

[0033] Figure 3 is an illustration of an example method of forming an electrode having an ion gel according to various aspects of the present technology;

[0034] Figure 4A is a diagram of an example bipolar solid-state battery with an ion gel according to various aspects of the present technology;

[0035] Figure 4B is a diagram of an example bipolar solid-state battery with ion gel and dual current collectors according to various aspects of the present technology;

[0036] Figure 4C is a diagram of an example bipolar solid-state battery with ion gel and polymer barriers according to various aspects of the present technology;

[0037] Figure 5A is a graphical illustration of a 1C charge-discharge curve of a comparative battery; and

[0038] Figure 5B It is a graph comparing the 1C cycle capacity of the batteries.

[0039] Corresponding reference numerals indicate corresponding parts throughout the several views of the drawings. DETAILED DESCRIPTION OF THE INVENTION

[0040] Exemplary embodiments are provided so that the present disclosure will be thorough and the scope will be fully conveyed to those skilled in the art. Many specific details are set forth, such as examples of specific compositions, components, devices, and methods to provide a thorough understanding of the embodiments of the present disclosure. It will be apparent to those skilled in the art that specific details need not be employed, that exemplary embodiments may be embodied in many different forms, and that none should be construed as limiting the scope of the present disclosure. In some exemplary embodiments, well-known processes, well-known equipment structures, and well-known techniques are not described in detail.

[0041] The terms used herein are only for the purpose of describing specific exemplary embodiments, and are not intended to be restrictive. Unless the context clearly indicates, the singular forms "one", "a kind of" and "the" used herein may also be intended to include plural forms. The terms "comprise", "include", "contain" and "have" are inclusive, thus specifying the presence of the features, elements, compositions, steps, integers, operations and / or components, without excluding the presence or increase of one or more other features, integers, steps, operations, elements, components and / or groups thereof. Although the open term "comprising" should be understood as a non-limiting term for describing and claiming the various embodiments described herein, in some aspects, the term may be alternatively understood as a more restrictive and constraining term, such as "consisting of..." or "consisting essentially of..." Thus, for any given embodiment describing a composition, material, component, element, feature, integer, operation and / or process step, the present disclosure also specifically includes an embodiment consisting of or essentially consisting of such described compositions, materials, components, elements, features, integers, operations and / or process steps. In the case of “consisting of,” the alternative embodiment excludes any additional compositions, materials, components, elements, features, integers, operations and / or process steps, while in the case of “consisting essentially of,” any additional compositions, materials, components, elements, features, integers, operations and / or process steps that substantially affect the basic and novel characteristics are excluded from such embodiments, but any compositions, materials, components, elements, features, integers, operations and / or process steps that do not substantially affect the basic and novel characteristics may be included in the embodiment.

[0042] Any method steps, processes, and operations described herein should not be construed as necessarily requiring their performance in the particular order discussed or shown, unless expressly identified as an order of performance. It should also be understood that additional or alternative steps may be employed unless otherwise stated.

[0043] When a component, element or layer is referred to as being "located on," "engaged to," "connected to," or "coupled to" another element or layer "on," it may be directly located on, engaged to, connected to, or coupled to the other component, element or layer, or there may be intermediate elements or layers. In contrast, when an element is referred to as being "directly located on," "directly engaged to," "directly connected to," or "directly coupled to" another element or layer "on," there may be no intermediate elements or layers. Other words used to describe the relationship between elements should be interpreted in a similar manner (e.g., "between" versus "directly between," "adjacent" versus "directly adjacent," etc.). The term "and / or" as used herein includes any and all combinations of one or more of the associated listed items.

[0044] Although the term first, second, third etc. can be used in this article to describe various steps, elements, components, regions, layers and / or parts, unless otherwise specified, these steps, elements, components, regions, layers and / or parts should not be limited by these terms. These terms can only be used to distinguish a step, element, component, region, layer or part from another step, element, component, region, layer or part. Unless the context clearly indicates, otherwise the terms such as "first", "second" and other numerical terms do not imply order or sequence when used in this article. Thus, the first step, element, component, region, layer or part discussed below can be referred to as the second step, element, component, region, layer or part, without leaving the teaching of this exemplary embodiment.

[0045] Spatially or temporally relative terms, such as "before", "after", "inside", "outside", "below", "below", "lower", "above", "upper", etc., are used herein for ease of description to describe the relationship of one element or feature to another element or feature as shown in the figures. Spatially or temporally relative terms may be intended to encompass different orientations of the device or system in use or operation in addition to the orientation depicted in the figures.

[0046] Throughout this disclosure, numerical values ​​represent approximate measures or boundaries of ranges to cover minor deviations from a given value and embodiments with approximately the stated value and embodiments with the exact stated value. Except in the working examples provided at the end of the detailed description, the numerical values ​​of all parameters (such as amounts or conditions) in this specification (including the appended claims) should be understood to be modified by the term "approximately" in all cases, regardless of whether "approximately" actually appears before the numerical value. "Approximately" means that the numerical value allows some slight imprecision (the accuracy of the value is achieved by some methods; approximately or reasonably close to the value; nearly). If the imprecision provided by "approximately" is not understood in the art with this common meaning, then the "approximately" used herein at least represents the changes that may be caused by the general methods of measuring and using such parameters. For example, "approximately" can include less than or equal to 5%, optionally less than or equal to 4%, optionally less than or equal to 3%, optionally less than or equal to 2%, optionally less than or equal to 1%, optionally less than or equal to 0.5%, and optionally less than or equal to 0.1% in some aspects.

[0047] Furthermore, the disclosure of ranges includes disclosure of all values ​​within the entire range and further subdivided ranges, including endpoints and subranges given for that range.

[0048] Example embodiments will now be described more fully with reference to the accompanying drawings.

[0049] The present technology relates to solid-state batteries (SSBs) comprising ion gels, such as bipolar solid-state batteries. The solid-state battery may have a bipolar stack design comprising a plurality of bipolar electrodes, wherein a first mixture of solid electroactive material particles (and optionally solid electrolyte particles) is disposed on a first side of a current collector, and a second mixture of solid electroactive material particles (and optionally solid electrolyte particles) is disposed on a second side of the current collector parallel to the first side. As solid electroactive material particles, the first mixture may include cathode material particles. As solid electroactive material particles, the second mixture may include anode material particles. The solid electrolyte particles may be the same or different in each case.

[0050] In each case, the ion gel can wet the interface between the solid electrolyte particles and / or the solid electroactive material particles and / or fill the void space between the solid electrolyte particles and / or the solid electroactive material particles to reduce the interparticle porosity and improve ionic contact; and / or the polymer barrier can contact or connect one or more adjacent current collectors to mitigate potential ionic short circuits. Such bipolar solid-state batteries can be incorporated into energy storage devices, such as rechargeable lithium-ion batteries, which can be used in automotive transportation applications (e.g., motorcycles, boats, tractors, buses, mobile homes, campers, and tanks). However, the present technology can also be used in a variety of other industries and applications, including aerospace parts, consumer products, devices as non-limiting examples. Buildings (e.g., houses, offices, sheds, and warehouses), office equipment and furniture, and industrial equipment machinery, agricultural or farm equipment, or heavy machinery. In various aspects, the present disclosure provides a rechargeable lithium-ion battery that exhibits high temperature stability and improved safety and excellent power capacity and life performance.

[0051] An exemplary and schematic diagram of an all-solid-state electrochemical cell (also referred to as a "solid-state battery" and / or "battery") 20 for cycling lithium ions is shown in Figure 1A and 1B The battery pack 20 includes a negative electrode (ie, an anode) 22 , a positive electrode (ie, a cathode) 24 , and a solid electrolyte layer 26 .

[0052] The solid electrolyte layer 26 is a separator that physically separates the negative electrode 22 from the positive electrode (i.e., cathode) 24. The solid electrolyte layer 26 can be defined by a first plurality of solid electrolyte particles 30. A second plurality of solid electrolyte particles 90 can be mixed with the solid negative electroactive particles 50 in the negative electrode 22, and a third plurality of solid electrolyte particles 92 can be mixed with the solid positive electroactive particles 60 in the positive electrode 24 to form a continuous electrolyte network, which can be a continuous solid electrolyte network. For example, the solid negative electroactive particles 50 and the solid positive electroactive particles 60 are independently not mixed with the electrolyte, or are independently mixed with the second / third plurality of solid electrolyte particles 90, 92.

[0053] Negative electrode current collector 32 may be located at or near negative electrode 22. Figure 4B As discussed in the context of , the negative electrode current collector 32 may be formed of copper or any other suitable conductive material known to those skilled in the art. The positive electrode current collector 34 may be located at or near the positive electrode 24. As described below in Figure 4B As discussed in the context of FIG. 1 , the positive electrode current collector 34 can be formed of aluminum or any other conductive material known to those skilled in the art. The negative electrode current collector 32 and the positive electrode current collector 34 respectively collect free electrons and move them to and from the external circuit 40 (as indicated by the solid arrows). For example, the interruptible external circuit 40 and the load device 42 can connect the negative electrode 22 (through the negative electrode current collector 32) and the positive electrode 24 (through the positive electrode current collector 34).

[0054] Although the illustrated example includes a single positive electrode (i.e., cathode) 24 and a single negative electrode (i.e., anode) 22, those skilled in the art will recognize that the present teachings are applicable to a variety of other configurations, including those having one or more cathodes and one or more anodes, and various current collectors having a layer of electroactive particles disposed on or adjacent to one or more surfaces thereof.

[0055] The battery 20 can generate current (e.g., 20 ) during discharge by a reversible electrochemical reaction that occurs when the external circuit 40 is closed (to connect the negative electrode 22 and the positive electrode 24) and when the negative electrode 22 has a lower potential than the positive electrode 24. Figure 1A and 1B). The chemical potential difference between the negative electrode 22 and the positive electrode 24 drives the electrons generated at the negative electrode 22 by a reaction such as oxidation of the intercalated lithium toward the positive electrode 24 through the external circuit 40. The lithium ions also generated at the negative electrode 22 are simultaneously transferred toward the positive electrode 24 through the solid electrolyte layer 26. The electrons flow through the external circuit 40, and the lithium ions migrate across the solid electrolyte layer 26 to the positive electrode 24, where the ions are plated, reacted, or intercalated. The current through the external circuit 40 can be harnessed and directed through the load device 42 (in the direction of the arrow) until the lithium in the negative electrode 22 is depleted and the capacity of the battery pack 20 is reduced.

[0056] An external power source (e.g., a charging device) can be connected to the battery pack 20 to reverse the electrochemical reactions that occur during the battery pack discharge process, thereby charging or re-energizing the battery pack 20 at any time. The external power source that can be used to charge the battery pack 20 can vary depending on the size, construction, and specific end use of the battery pack 20. Some notable and exemplary external power sources include, but are not limited to, AC-DC converters and automotive alternators that are connected to the AC power grid through a wall outlet. Connecting an external power source to the battery pack 20 promotes reactions at the positive electrode 24, such as non-spontaneous oxidation of embedded lithium, thereby generating electrons and lithium ions. Electrons (which flow back to the negative electrode 22 through the external circuit 40) and lithium ions (which move back to the negative electrode 22 across the solid electrolyte layer 26) recombine at the negative electrode 22 and replenish it with lithium so that it can be consumed during the next battery pack discharge cycle. Thus, a complete discharge event followed by a complete charging event is considered to be a cycle in which lithium ions circulate between the positive electrode 24 and the negative electrode 22.

[0057] In many configurations of the battery 20, the negative electrode current collector 32, the negative electrode 22, the solid electrolyte layer 26, the positive electrode 24, and the positive electrode current collector 34 are each prepared as relatively thin layers (e.g., a thickness of a few microns to a millimeter or less) and assembled into layers electrically connected in parallel to provide suitable electrical energy and power packages. In various other cases, the battery 20 may include electrodes 22, 24 electrically connected in series.

[0058] In various aspects, the battery pack 20 may include a variety of other components that are not depicted herein but are known to those skilled in the art. For example, the battery pack 20 may include a housing, a gasket, a terminal cover, and any other conventional components or materials that may be located in the battery pack 20 (including between or near the negative electrode 22, the positive electrode 24, and / or the solid electrolyte layer 26).

[0059] As described above, the size and shape of the battery pack 20 can vary depending on the specific application for which it is designed. Battery-powered vehicles and handheld consumer electronic devices are two examples in which the battery pack 20 is most likely to be designed with different sizes, capacities, and power output specifications. As described above, the battery pack 20 can also be connected in series or in parallel with other similar lithium-ion cells or battery packs to produce greater voltage output, energy, and power (if the load device 42 requires it). The battery pack 20 can generate a current toward the load device 42, which can be operably connected to the external circuit 40. The load device 42 can be powered in whole or in part by the current through the external circuit 40 when the battery pack 20 is discharged. Although the load device 42 can be any number of known electric devices, as non-limiting examples, some specific examples of power-consuming load devices include electric motors for hybrid electric vehicles or all-electric vehicles, laptop computers, tablet computers, cellular phones, and cordless power tools or appliances. The load device 42 can also be a power generation device that charges the battery pack 20 for the purpose of storing electrical energy.

[0060] Refer to Figure 1A and 1B , the solid electrolyte layer 26 provides electrical separation between the negative electrode 22 (ie, the anode) and the positive electrode 24 (ie, the cathode) - preventing physical contact. The solid electrolyte layer 26 also provides a path of minimum resistance for the ions to pass through the interior. In various aspects, as described above, the solid electrolyte layer 26 can be defined by a first plurality of solid electrolyte particles 30. For example, the solid electrolyte layer 26 can be in the form of a layer or composite material containing a first plurality of solid electrolyte particles 30. The solid electrolyte particles 30 can have an average particle size of greater than or equal to about 0.02 μm to less than or equal to about 20 μm, and in some aspects, optionally greater than or equal to about 0.1 μm to less than or equal to about 1 μm. Although not shown, those skilled in the art will recognize that in some cases, one or more binder particles can be mixed with the solid electrolyte particles 30. For example, in some aspects, the solid electrolyte layer 26 can include greater than or equal to about 0.5 wt % to less than or equal to about 10 wt % of one or more binders. The one or more binders may include, for example, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), ethylene propylene diene monomer (EPDM) rubber, nitrile rubber (NBR), styrene-butadiene rubber (SBR), and lithium polyacrylate (LiPAA).

[0061] The solid electrolyte layer 26 may be in the form of a layer having a thickness of greater than or equal to about 5 μm to less than or equal to about 200 μm, optionally greater than or equal to about 10 μm to less than or equal to about 100 μm, optionally about 40 μm, and in some aspects optionally about 20 μm. Figure 1A As shown in , such a solid electrolyte layer 26 can have an inter-particle porosity 80 (defined herein as the fraction of the total volume of pores to the total volume of the layer or membrane) between the first plurality of solid electrolyte particles 30 of greater than 0 volume % to less than or equal to about 50 volume %, greater than or equal to about 1 volume % to less than or equal to about 40 volume %, or greater than or equal to about 2 volume % to less than or equal to about 20 volume %.

[0062] The first plurality of solid electrolyte particles 30 may include one or more oxide-based particles, metal-doped or aliovalent-substituted oxide particles, sulfide-based particles, nitride-based particles, hydride-based particles, halide-based particles, and borate-based particles.

[0063] In certain variations, the oxide-based particles may comprise one or more garnet ceramics, LISICON-type oxides, NASICON-type oxides, and perovskite-type ceramics. For example, the garnet ceramic may be selected from: Li7La3Zr2O 12 , Li 6.2 Ga 0.3 La 2.95 R 0.05 Zr2O 12 , Li 6.85 La 2.9 Ca 0.1 Zr 1.75 Nb 0.25 O 12 , Li 6.25 Al 0.25 La3Zr2O 12 , Li 6.75 LqCy 1.75 Nb 0.25 O 12 And combinations thereof. The LISICON type oxide may be selected from: Li 2+2x Zn 1-x GeO4 (where 0 < x < 1), Li 14 Zn(GeO4)4、Li 3+x (P 1−x Si x )O4 (where 0 < x < 1), Li 3+x Ge x V 1-xO4 (where 0 < x < 1) and combinations thereof. The NASICON-type oxide may be defined by LiMM'(PO4)3, where M and M' are independently selected from Al, Ge, Ti, Sn, Hf, Zr and La. For example, in certain variations, the NASICON-type oxide may be selected from: Li 1+x Al x Ge 2-x (PO4)3 (LAGP) (where 0 ≤ x ≤ 2), Li 1.4 Al 0.4 Ti 1.6 (PO4)3、Li 1.3 Al 0.3 Ti 1.7 (PO4)3, LiTi2(PO4)3, LiGeTi(PO4)3, LiGe2(PO4)3, LiHf2(PO4)3 and combinations thereof. The perovskite ceramic may be selected from: Li 3.3 La 0.53 TiO3、LiSr 1.65 Zr 1.3 Ta 1.7 O9, Li 2x-y Sr 1-x Ta y Zr 1-y O3 (where x = 0.75y and 0.60 < y < 0.75), Li 3 / 8 Sr 7 / 16 Nb 3 / 4 Zr 1 / 4 O3、Li 3x La (2 / 3-x) TiO3 (where 0 < x < 0.25) and combinations thereof.

[0064] In certain variations, the metal-doped or alivalently substituted oxide particles may include, for example, aluminum (Al) or niobium (Nb) doped Li7La3Zr2O 12 , Antimony (Sb) doped Li7La3Zr2O 12 , Gallium (Ga) doped Li7La3Zr2O 12 , chromium (Cr) and / or vanadium (V) substituted LiSn2P3O 12 , Li substituted by aluminum (Al) 1+x+y Al x Ti 2-x Si Y P 3-y O 12 (where 0 < x < 2 and 0 < y < 3) and their combinations.

[0065] In certain variations, the sulfide-based particles may include, for example, a Li2S-P2S5 system, a Li2S-P2S5-MO x System (where 1 < x < 7), Li2S-P2S5-MS x system (where 1 < x < 7), Li 10 GeP2S 12 (LGPS), Li6PS5X (where X is Cl, Br or I) (including lithium argyrodite), Li7P2S8I, Li 10.35 Ge 1.35 P 1.65 S 12 , Li 3.25 Ge 0.25 P 0.75 S4 (sulfur LISICON), Li 10 SnP2S 12 , Li 10 SiP2S 12 , Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 、(1-x)P2S5-xLi2S(where 0.5≤x≤0.7)、Li 3.4 Si 0.4 P 0.6 S4、PLi 10 GeP2S 11.7 O 0.3 , Li 9.6 P3S 12 、Li7P3S 11 、Li9P3S9O3、Li 10.35 Ge 1.35 P 1.63 S 12 , Li 9.81 Sn 0.81 P 2.19 S 12 , Li 10 (Si 0.5 Ge 0.5 )P2S 12 , Li 10 (Ge 0.5 Sn 0.5 )P2S 12 , Li 10 (Si 0.5 Sn 0.5 )P2S 12 , Li 3.833 Sn 0.833 As0.16 S4, LiI–Li4SnS4, Li4SnS4 and combinations thereof.

[0066] In certain variations, the nitride-based particles may include, for example, Li3N, Li7PN4, LiSi2N3, and combinations thereof; the hydride-based particles may include, for example, LiBH4, LiBH4–LiX (wherein x = Cl, Br, or I), LiNH2, Li2NH, LiBH4-LiNH2, Li3AlH6, and combinations thereof; the halide-based particles may include, for example, LiI, Li3InCl6, Li2CdCl4, Li2MgCl4, LiCdI4, Li2ZnI4, Li3OCl, and combinations thereof; and the borate-based particles may include, for example, Li2B4O7, Li2O–B2O3–P2O5, and combinations thereof.

[0067] In this manner, in various aspects, the first plurality of solid electrolyte particles 30 may include one or more electrolyte materials selected from the group consisting of: Li7La3Zr2O 12 , Li 6.2 Ga 0.3 La 2.95 R 0.05 Zr2O 12 , Li 6.85 La 2.9 Ca 0.1 Zr 1.75 Nb 0.25 O 12 , Li 6.25 Al 0.25 La3Zr2O 12 , Li 6.75 Ln3Z 1.75 Nb 0.25 O 12 , Li 6.75 Ln3Z 1.75 Nb 0.25 O 12 , Li 2+2x Zn 1-x GeO4 (where 0 < x < 1), Li 14 Zn(GeO4)4、Li 3+x (P 1−x Si x )O4 (where 0 < x < 1), Li 3+x Ge x V 1-x O4 (where 0 < x < 1), LiMM'(PO4)3 (where M and M' are independently selected from Al, Ge, Ti, Sn, Hf, Zr and La), Li 3.3 La0.53 TiO3、LiSr 1.65 Zr 1.3 Ta 1.7 O9, Li 2x-y Sr 1-x Ta y Zr 1-y O3 (where x = 0.75y and 0.60 < y < 0.75), Li 3 / 8 Sr 7 / 16 Nb 3 / 4 Zr 1 / 4 O3、Li 3x La (2 / 3-x) TiO3 (where 0 < x < 0.25), aluminum (Al), or niobium (Nb) doped Li7La3Zr2O 12 , Antimony (Sb) doped Li7La3Zr2O 12 , Gallium (Ga) doped Li7La3Zr2O 12 , chromium (Cr) and / or vanadium (V) substituted LiSn2P3O 12 , Li substituted by aluminum (Al) 1+x+y Al x Ti 2-x Si Y P 3-y O 12 (where 0 < x < 2 and 0 < y < 3), Li2S-P2S5 system, Li2S-P2S5-MO x System (where 1 < x < 7), Li2S-P2S5-MS x system (where 1 < x < 7), Li 10 GeP2S 12 (LGPS), Li6PS5X (where X is Cl, Br or I) (containing lithium argyrodite), Li7P2S8I, Li 10.35 Ge 1.35 P 1.65 S 12 , Li 3.25 Ge 0.25 P 0.75 S4 (sulfur LISICON), Li 10 SnP2S 12 , Li 10 SiP2S 12 , Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 、(1-x)P2S5-xLi2S(where 0.5≤x≤0.7)、Li3.4 Si 0.4 P 0.6 S4、PLi 10 GeP2S 11.7 O 0.3 , Li 9.6 P3S 12 、Li7P3S 11 、Li9P3S9O3、Li 10.35 Ge 1.35 P 1.63 S 12 , Li 9.81 Sn 0.81 P 2.19 S 12 , Li 10 (Si 0.5 Ge 0.5 )P2S 12 , Li 10 (Ge 0.5 Sn 0.5 )P2S 12 , Li 10 (Si 0.5 Sn 0.5 )P2S 12 , Li 3.833 Sn 0.833 As 0.16 S4, LiI–Li4SnS4, Li4SnS4, Li3N, Li7PN4, LiSi2N3, LiBH4, LiBH4–LiX (wherein x = Cl, Br or I), LiNH2, Li2NH, LiBH4-LiNH2, Li3AlH6, LiI, Li3InCl6, Li2CdCl4, Li2MgCl4, LiCdI4, Li2ZnI4, Li3OCl, Li2B4O7, Li2O–B2O3–P2O5 and combinations thereof.

[0068] In various aspects, such as Figure 2A –2C for solid-state battery packs (e.g. Figure 1A and 1BThe solid electrolyte layers 200A, 200B, 200C described above can be respectively formed by: a single (first) layer 230 comprising a first plurality of solid electrolyte particles 240 disposed on an exposed surface 216 of a negative electrode 210 (i.e., an anode), the negative electrode being defined by a plurality of solid negative electroactive particles 212 disposed adjacent to a negative electrode current collector 214 (and in some cases, as described above, another plurality of solid electrolyte particles (not shown)); a single (second) layer 250 comprising a second plurality of solid electrolyte particles 260 disposed on an exposed surface 226 of a positive electrode 220 (i.e., a cathode), the positive electrode being defined by a plurality of solid positive electroactive particles 222 disposed adjacent to a positive electrode current collector 224 (and in some cases, as described above, another plurality of solid electrolyte particles (not shown)); or a combination thereof - that is, a first layer 230 comprising a first plurality of solid electrolyte particles 240 disposed on the negative electrode 210 and a second layer 250 comprising a second plurality of solid electrolyte particles 260 disposed on the positive electrode 220.

[0069] In various cases, the solid electrolyte particles 240, 260 may include one or more of the solid electrolytes described in detail above. The solid electrolyte materials defining each layer 230, 250 may be the same or different. The solid electrolyte layers 200A, 200B, 200C may each have a thickness of greater than or equal to about 5 μm to less than or equal to about 200 μm, optionally greater than or equal to about 10 μm to less than or equal to about 100 μm, optionally about 40 μm, and optionally about 20 μm in some aspects. The first and second layers 230, 250 have a certain thickness to define a solid electrolyte layer 200A, 200B, 200C having a thickness of greater than or equal to about 5 μm to less than or equal to about 200 μm, optionally greater than or equal to about 10 μm to less than or equal to about 100 μm, optionally about 40 μm, and optionally about 20 μm in some aspects.

[0070] Refer to Figure 1A and 1B, the negative electrode 22 can be formed of a lithium matrix material that is capable of serving as a negative terminal of a lithium-ion battery pack. For example, in certain variations, the negative electrode 22 can be defined by a plurality of solid negatively electroactive particles 50. In some cases, as shown, the negative electrode 22 is a composite material comprising a mixture of solid negatively electroactive particles 50 and a second plurality of solid electrolyte particles 90. For example, the negative electrode 22 may include greater than or equal to about 30% by weight to less than or equal to about 98% by weight, and in some aspects optionally greater than or equal to about 50% by weight to less than or equal to about 95% by weight of solid negatively electroactive particles 50, and greater than or equal to about 0% by weight to less than or equal to about 50% by weight, and in some aspects optionally greater than or equal to about 5% by weight to less than or equal to about 20% by weight of a second plurality of solid electrolyte particles 90. Such a negative electrode 22 may have greater than or equal to about 0% by volume to less than or equal to about 20% by volume such as Figure 1A The inter-particle porosity 82 between the solid negatively electroactive particles 50 and / or the second plurality of solid electrolyte particles 90 is shown in FIG.

[0071] The second plurality of solid electrolyte particles 90 may be the same as or different from the first plurality of solid electrolyte particles 30. In certain variations, the solid negatively electroactive particles 50 may be lithium-based, such as lithium alloys. In other variations, the solid negatively electroactive particles 50 may be silicon-based, including, for example, silicon alloys and / or silicon-graphite mixtures. In still other variations, the negative electrode 22 may be a carbonaceous anode, and the solid negatively electroactive particles 50 may include one or more negatively electroactive materials, such as graphite, graphene, hard carbon, soft carbon, and carbon nanotubes (CNTs). In still other variations, the negative electrode 22 may include one or more negatively electroactive materials, such as lithium titanium oxide (Li4Ti5O 12 ); one or more metal oxides, such as TiO2 and / or V2O5; and metal sulfides, such as FeS. Thus, the solid negatively electroactive particles 50 can be selected from, for example, lithium, graphite, graphene, hard carbon, soft carbon, carbon nanotubes, silicon, silicon-containing alloys, tin-containing alloys, and combinations thereof.

[0072] In some variations, the negative electrode 22 may further include one or more conductive additives and / or binder materials. For example, the solid negative electroactive particles 50 (and / or the second plurality of solid electrolyte particles 90) may optionally be mixed with one or more conductive materials (not shown) that provide an electronic conduction path and / or at least one polymer binder material (not shown) that improves the structural integrity of the negative electrode 22.

[0073] For example, the solid negatively charged particles 50 (and / or the second plurality of solid electrolyte particles 90) may optionally be mixed with a binder, such as polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), ethylene propylene diene monomer (EPDM) rubber, nitrile rubber (NBR), styrene-butadiene rubber (SBR) and / or lithium polyacrylate (LiPAA) binder. The conductive material may include, for example, a carbon-based material or a conductive polymer. The carbon-based material may include, for example, graphite, acetylene black (such as KETCHEN TM Black or DENKA TM Black), carbon fibers and nanotubes, graphene (such as graphene oxide), carbon black (such as Super P), etc. Examples of conductive polymers may include polyaniline, polythiophene, polyacetylene, polypyrrole, etc. In some aspects, a mixture of conductive additives and / or binder materials may be used.

[0074] The negative electrode 22 can include greater than or equal to about 0 wt % to less than or equal to about 30 wt %, and in some aspects optionally greater than or equal to about 2 wt % to less than or equal to about 10 wt % of one or more conductive additives; and greater than or equal to about 0 wt % to less than or equal to about 20 wt %, and in some aspects optionally greater than or equal to about 1 wt % to less than or equal to about 10 wt % of one or more binders.

[0075] The positive electrode 24 can be formed of a lithium-based or electroactive material that can undergo lithium insertion and deinsertion while serving as the positive terminal of the battery 20. For example, in certain variations, the positive electrode 24 can be defined by a plurality of solid positive electroactive particles 60. In some cases, as shown, the positive electrode 24 is a composite material comprising a mixture of solid positive electroactive particles 60 and a third plurality of solid electrolyte particles 92. For example, the positive electrode 24 can include greater than or equal to about 30% by weight to less than or equal to about 98% by weight, and in some aspects optionally greater than or equal to about 50% by weight to less than or equal to about 95% by weight of solid positive electroactive particles 60, and greater than or equal to about 0% by weight to less than or equal to about 50% by weight, and in some aspects optionally greater than or equal to about 5% by weight to less than or equal to about 20% by weight of the third plurality of solid electrolyte particles 92. Such a positive electrode 24 can have greater than or equal to about 1% by volume to less than or equal to about 20% by volume, and optionally greater than or equal to 5% by volume to less than or equal to about 10% by volume. Figure 1A The inter-particle porosity 84 between the solid positive electroactive particles 60 and / or the third plurality of solid electrolyte particles 92 is shown in FIG.

[0076] The third plurality of solid electrolyte particles 92 may be the same or different from the first and / or second plurality of solid electrolyte particles 30, 90. In some variations, the positive electrode 24 may be one of a layered oxide cathode, a spinel cathode, and a polyanion cathode. For example, in the case of a layered oxide cathode (e.g., a rock salt layered oxide), the solid positive electroactive particles 60 may include one or more positive electroactive materials, and for a solid-state lithium-ion battery, the positive electroactive materials are selected from LiCoO2, LiNi x Mn y Co 1-x-y O2 (where 0 ≤ x ≤ 1 and 0 ≤ y ≤ 1), LiNi x Mn y Al 1-x-y O2 (where 0< x ≤ 1 and 0 < y ≤ 1), LiNi x Mn 1-x O2 (where 0 ≤ x ≤ 1) and Li 1+x MO2 (where 0 ≤ x ≤ 1). The spinel cathode may include one or more positive electroactive materials, such as LiMn2O4 and LiNi 0.5 Mn 1.5 O4. The polyanion cathode may include phosphates such as LiFePO4, LiVPO4, LiV2(PO4)3, Li2FePO4F, Li3Fe3(PO4)4 or Li3V2(PO4)F3 for lithium-ion batteries, and / or silicates such as LiFeSiO4 for lithium-ion batteries. In this manner, in various aspects, the solid-state positively electroactive particles 60 may include one or more positively electroactive materials selected from LiCoO2, LiNi x Mn y Co 1-x-y O2 (where 0 ≤ x ≤ 1 and 0 ≤ y ≤ 1), LiNi x Mn 1-x O2 (where 0 ≤ x ≤ 1), Li 1+x MO2 (where 0 ≤ x ≤ 1), LiMn2O4, LiNi x Mn 1.5 O4, LiFePO4, LiVPO4, LiV2(PO4)3, Li2FePO4F, Li3Fe3(PO4)4, Li3V2(PO4)F3, LiFeSiO4 and combinations thereof. In certain aspects, the solid positive electroactive particles 60 can be coated (e.g., with LiNbO3 and / or Al2O3) and / or the positive electroactive material can be doped (e.g., with aluminum and / or magnesium).

[0077] In some variations, the positive electrode 24 may further include one or more conductive additives and / or binder materials. For example, the solid positive electroactive particles 60 (and / or the third plurality of solid electrolyte particles 92) may optionally be mixed with one or more conductive materials (not shown) that provide an electronic conduction path and / or at least one polymer binder material (not shown) that improves the structural integrity of the positive electrode 24.

[0078] For example, the solid positively charged particles 60 (and / or the third plurality of solid electrolyte particles 92) may be optionally mixed with a binder, such as polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), ethylene propylene diene monomer (EPDM) rubber, nitrile rubber (NBR), styrene-butadiene rubber (SBR) and / or lithium polyacrylate (LiPAA) binder. The conductive material may include, for example, a carbon-based material or a conductive polymer. The carbon-based material may include, for example, graphite, acetylene black (such as KETCHEN TM Black or DENKA TM Black), carbon fibers and nanotubes, graphene (such as graphene oxide), carbon black (such as Super P), etc. Examples of conductive polymers may include polyaniline, polythiophene, polyacetylene, polypyrrole, etc. In some aspects, a mixture of conductive additives and / or binder materials may be used.

[0079] The positive electrode 24 may include greater than or equal to about 0 wt % to less than or equal to about 30 wt %, and in some aspects optionally greater than or equal to about 2 wt % to less than or equal to about 10 wt % of one or more conductive additives; and greater than or equal to about 0 wt % to less than or equal to about 20 wt %, and in some aspects optionally greater than or equal to about 1 wt % to less than or equal to about 10 wt % of one or more binders.

[0080] Due to the inter-particle porosity 80, 82, 84 between particles in the battery 20 (e.g., the battery 20 in green form can have a solid electrolyte inter-particle porosity of greater than or equal to about 0 vol % to less than or equal to about 30 vol %), direct contact between the solid electroactive particles 50, 60 and the plurality of solid electrolyte particles 30, 90, 92 can be much less than the contact between the liquid electrolyte and the solid electroactive particles in a comparable non-solid state battery. In various aspects, such as Figure 1BAs shown in , the present disclosure provides an ion gel 100. The ion gel 100 can be disposed in a battery pack to wet the interface between the solid electrolyte particles 50, 60 and / or the solid active material particles 30, 90, 92 and / or fill the void space between the solid electrolyte particles 50, 60 and / or the solid active material particles 30, 90, 92, so as to, for example, reduce the inter-particle porosity 80, 82, 84 and improve ion contact and / or enable higher thermal stability. The battery pack 20 may include greater than or equal to about 0 wt% to less than or equal to about 30 wt%, and in some aspects greater than or equal to about 5 wt% to less than or equal to about 20 wt% of the ion gel 100.

[0081] The ion gel 100 is a soft ion gel formed by fixing an ionic liquid in a solid component so that the ion gel 100 maintains the properties of the ionic liquid. For example, the ion gel 100 may have an ionic conductivity of greater than or equal to about 0.1 mS / cm to less than or equal to about 10 mS / cm, optionally greater than or equal to about 1 mS / cm to less than or equal to about 10 mS / cm, and in some aspects optionally about 1 mS / cm and a decomposition temperature greater than about 200°C. The ion gel 100 may include, for example, greater than or equal to about 30 wt% to less than or equal to about 98 wt%, and in some aspects optionally greater than or equal to about 50 wt% to less than or equal to about 95 wt% of the ionic liquid; greater than or equal to about 2 wt% to less than or equal to about 40 wt%, and in some aspects optionally greater than or equal to about 5 wt% to less than or equal to about 20 wt% of the solid component.

[0082] The ionic liquid comprises, for example, a cation and an anion, and in certain variations, an optional diluent solvent.

[0083] The cation may include, for example, Li(triglyme)methylimidazolium ([Li(G3)] + )、Li(tetraethylene glycol dimethyl ether)([Li(G4) + ])、1-ethyl-3([Emim] + )、1-propyl-3-methylimidazolium([Pmim] + )、1-butyl-3-methylimidazolium([Bmim] + )、1,2-dimethyl-3-butylimidazolium([DMBim])、1-alkyl-3-methylimidazolium([Cnmim] + )、1-allyl-3-methylimidazolium([Amim] + )、1,3-diallylimidazolium([Daim] + )、1-allyl-3-vinylimidazolium([Avim] +); 1-vinyl-3-ethylimidazolium ([Veim] + )、1-cyanomethyl-3-methylimidazolium([MCNim] + )、1,3-Dicyanomethyl-imidazolium([BCNim] + ), 1-propyl-1-methylpiperidinium ([PP 13 ] + )、1-butyl-1-methylpiperidinium([PP 14 ] + ), 1-methyl-1-ethylpyrrolidinium ([Pyr 12 ] + ), 1-propyl-1-methylpyrrolidinium ([Pyr 13 ] + )、1-butyl-1-methylpyrrolidinium([Pyr 14 ] + ), methyl-methylcarboxymethyl-pyrrolidinium ([MMMPyr] + ), tetramethylammonium ([N 1111 ] + ), tetraethylammonium ([N 2222 ] + ), tributylmethylammonium ([N 4441 ] + ), diallyldimethylammonium ([DADMA] + ); NN-diethyl-N-methyl-N-(2-methoxyethyl)ammonium ([DEME] + )、N,N-diethyl-N-(2-methacryloylethyl)-N-methylammonium([DEMM] + ), trimethyl isobutyl-phosphonium ([P 111i4 ] + ), triisobutylmethylphosphonium ([P 1i444 ] + ), tributylmethylphosphonium ([P 1444 ] + ), diethylmethylisobutylphosphonium ([P 1224 ] + )、Trihexyldecylphosphonium([P 66610 ] + ), trihexyltetradecylphosphonium ([P 66614 ] + ) and their combinations.

[0084] The anion may include, for example, hexafluoroarsenate, hexafluorophosphate, bis(fluorosulfonyl)imide (FSI), bis(trifluoromethanesulfonyl)imide (TFSI), perchlorate, tetrafluoroborate, cyclo-difluoromethane-1,1-bis(sulfonyl)imide (DMSI), bis(perfluoroethanesulfonyl)imide (BETI), bis(oxalato)borate (BOB), difluoro(oxalato)borate (DFOB), bis(fluoromalonato)borate (BFMB), and combinations thereof.

[0085] An optional diluent solvent may be added to reduce viscosity and / or improve the lithium ion conductivity of the ionic liquid. The optional diluent solvent may be a solvent having a low boiling point. For example, the solvent may have a boiling point of less than or equal to about 150° C., and in some aspects optionally less than or equal to about 100° C. The optional diluent solvent may include, for example, dimethyl carbonate, ethylene carbonate, ethyl acetate, acetonitrile, acetone, toluene, propylene carbonate, diethyl carbonate, 1,2,2-tetrafluoroethyl, 2,2,3,3-tetrafluoropropyl ether, and combinations thereof.

[0086] The solid component may include, for example, one or more organic polymers, inorganic oxides, organic polymer / inorganic oxide (ie, polymer / oxide) mixtures, metal-organic frameworks (MOFs), etc. The one or more organic polymers may include, for example, poly(ethylene oxide) (PEO)

[0087]

[0088] Where 1000≤ n≤10,000,000; one or more poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF=HFP)

[0089]

[0090] Where 1,000≤x≤10,000,000 and 1,000≤y≤10,000,000; one or more poly(methyl methacrylate) (PMMA)

[0091]

[0092] Of which 1,000≤n≤10,000,000; one or more carboxymethyl cellulose (CMC)

[0093]

[0094] Where 1,000≤n≤10,000,000; one or more polyacrylonitrile (PAN)

[0095]

[0096] Where 1,000≤n≤10,000,000; one or more polyvinylidene fluoride (PVDF)

[0097]

[0098] Where 1,000≤n≤10,000,000; one or more poly(vinyl alcohol) (PVA)

[0099]

[0100] Of which 1,000≤n≤10,000,000; one or more polyvinylpyrrolidone (PVP)

[0101]

[0102] wherein 1,000≤n≤10,000,000; and combinations thereof. The one or more inorganic oxides may include, for example, SiO2, Al2O3, TiO2, ZrO2, and combinations thereof. The one or more metal-organic frameworks (MOFs) may include, for example, MIL-101, UiO-67, ZIF-8, and combinations thereof.

[0103] In certain variations, the ion gel 100 may further include one or more lithium salts. For example, the ion gel 100 may include greater than or equal to 0% to less than or equal to about 40% by weight, and in certain aspects optionally greater than or equal to about 5% by weight to less than or equal to about 20% by weight of one or more lithium salts. As non-limiting examples, the one or more lithium salts include lithium cations and anions such as hexafluoroarsenate, hexafluorophosphate, bis(fluorosulfonyl)imide (FSI), perchlorate, tetrafluoroborate, cyclo-difluoromethane-1,1-bis(sulfonyl)imide (DMSI), bis(trifluoromethanesulfonyl)imide (TFSI), bis(perfluoroethanesulfonyl)imide (BETI), bis(oxalate)borate (BOB), difluoro(oxalato)borate (DFOB) and / or bis(fluoromalonate)borate (BFMB).

[0104] In various aspects, the present disclosure provides methods for preparing Figure 1B A method for a solid-state battery with an ion gel as shown in FIG. Figure 3 As shown in , the method can generally include contacting a first electrode 324 with an ion gel precursor solution 315 (i.e., step 302); contacting a second electrode 322 with an ion gel precursor solution 315 (i.e., step 304); and assembling the first and second electrodes 324, 322 to form a solid-state battery 300 (i.e., step 306). Steps 302 and 304 can be performed simultaneously or sequentially.

[0105] The first electrode 324 may be a positive electrode, similar to Figure 1A and 1B In the case of the positive electrode 24 described in detail, the positive electrode 324 can be defined by a plurality of solid positively electroactive particles 360. In some cases, although not shown Figure 3 In the embodiment of the present invention, the positive electrode 324 can also be a composite material comprising a mixture of solid positive electroactive particles 360 and a first plurality of solid electrolyte particles (not shown). The solid positive electroactive particles 360 (and / or the first plurality of solid electrolyte particles) can be disposed adjacent to the surface of the positive electrode current collector 334 in the form of a layer. Such a positive electrode 324 can have an inter-particle porosity 384. Similar to Figure 1A , such positive electrode 324 can have an inter-particle porosity 384 between the solid positive electroactive particles 360 (and / or the first plurality of solid electrolyte particles) of greater than or equal to about 1 volume % to less than or equal to about 20 volume %, and optionally greater than or equal to 5 volume % to less than or equal to about 10 volume %.

[0106] The second electrode 322 may be a negative electrode and similar to Figure 1A and 1B In the case of the negative electrode 22 described in detail, the negative electrode 322 can be defined by a plurality of solid negatively electroactive particles 350. In some cases, although not shown Figure 3 In the embodiment of the present invention, the negative electrode 322 may also be a composite material comprising a mixture of solid negatively electroactive particles 350 and a second plurality of solid electrolyte particles (not shown). The solid negatively electroactive particles 350 (and / or the second plurality of solid electrolyte particles) may be disposed adjacent to the surface of the negative electrode current collector 332 in the form of a layer. Figure 1A Such negative electrode 322 may have an inter-particle porosity 382 between the solid negative electroactive particles 350 (and / or the second plurality of solid electrolyte particles) of greater than or equal to about 0 vol % to less than or equal to about 20 vol %.

[0107] As shown, a solid electrolyte layer 326 can be disposed adjacent to the exposed surface of the negative electrode 322. The solid electrolyte layer 326 can be defined by a third plurality of solid electrolyte particles 330. Figure 1A , such solid electrolyte layer 326 may have an inter-particle porosity 380 between the third plurality of solid electrolyte particles 330 of greater than 0 vol% to less than or equal to about 50 vol%, greater than or equal to about 1 vol% to less than or equal to about 40 vol%, or greater than or equal to about 2 vol% to less than or equal to about 20 vol%. In addition, similar to the above detailed Figure 1A and 1BIn some cases, the third plurality of solid electrolyte particles 330 may include a solid electrolyte material that is the same as or different from the solid electrolyte material defining the first plurality of solid electrolyte particles and / or the second plurality of solid electrolyte particles, respectively.

[0108] However, although not described, those skilled in the art will recognize that in certain variations, such as Figure 2C As shown in , the first solid electrolyte layer can be disposed on the first electrode 324, and the second solid electrolyte layer can be disposed on the second electrode 322, and the first and second solid electrolyte layers can together define the solid electrolyte layer of the solid-state battery. In such cases, the first and second solid electrolyte layers can be the same or different. Similarly, although not described, those skilled in the art will recognize that in certain variations, such as Figure 2B As shown in , the solid electrolyte layer can be disposed adjacent to the exposed surface of the positive electrode.

[0109] Refer to Figure 3 , method step 302 includes (at 302A) contacting the first electrode 324 with an ion gel precursor solution 315. For example, the ion gel precursor solution 315 can be added to the first electrode 324 in a dropwise or spraying manner so as to impregnate the first electrode 324 with the ion gel precursor solution 315. For example, the ion gel precursor solution 315 can substantially fill the void spaces or pores between the solid positively electroactive particles 360 (and / or the first plurality of solid electrolyte particles). The ion gel precursor solution 315 includes a mixture of an ionic liquid, a solid component, and a diluent solvent in liquid form as described above. Similar to Figure 1B , the method step 302 includes (at 302B) removing the diluting solvent from the ion gel precursor solution 315 to form an ion gel 392 in the first electrode 324. As a non-limiting example, in some variations, the ion gel precursor solution 315 may include Li(G3)TFSI (95 wt%) (4.75 g (G3: triethylene glycol dimethyl ether)); PVDF-HFP (5 wt%) (0.25 g); and THF (100 wt%) (5.0 g). In such cases, THF may be removed to form the ion gel 392.

[0110] Method step 304 includes (at 304A) contacting the second electrode 322 with an ion gel precursor solution 315. For example, the ion gel precursor solution 315 can be added to the second electrode 322 in a dropwise or spraying manner so as to impregnate the second electrode 322 with the ion gel precursor solution 315. For example, the ion gel precursor solution 315 can substantially fill the void spaces or pores between the solid negatively electroactive particles 350 (and / or the second plurality of solid electrolyte particles). Similar to Figure 1B, the method step 304 includes removing (at 304B) the diluting solvent from the ion gel precursor solution 315 to form the ion gel 392 in the second electrode 322 .

[0111] Method step 306 includes contacting the first and second electrodes 324, 322 to define the battery pack 300, similar to the Figure 1B The configuration in question.

[0112] Although the examples shown above ( Figure 1A and 1B ) includes a single positive electrode (i.e., cathode) 24 and a single negative electrode (i.e., anode) 22, and those skilled in the art will recognize that the above teachings are applicable to various other configurations, including those having one or more cathodes and one or more anodes, and various current collectors having a layer of electroactive particles disposed on or adjacent to one or more surfaces thereof. For example, Figure 4A As shown in FIG. 4C , the solid-state battery 400 may include a plurality of electrodes, such as a first bipolar electrode 402A and a second bipolar electrode 402B. Figure 4A The asterisk in -4C means that the battery pack 400 may include one or more additional electrodes, as will be appreciated by those skilled in the art.

[0113] The bipolar electrodes 402A, 402B each include a first plurality of electroactive material particles 450 disposed adjacent to or on a first side or surface 432 of a current collector 436 and a second plurality of electroactive material particles 460 disposed adjacent to or on a second side or surface 434 of the current collector 436. The first plurality of electroactive material particles 450 may be solid negative electroactive material particles, as described in detail above in the context of solid negative electroactive particles 50. The second plurality of electroactive material particles 460 may be solid positive electroactive material particles, as described in detail above in the context of solid positive electroactive particles 60.

[0114] In some variations, as shown, the first plurality of solid electrolyte particles 490 may be mixed or doped with the first plurality of electroactive material particles 450; and the second plurality of solid electrolyte particles 492 may be mixed or doped with the second plurality of electroactive material particles 460. A solid electrolyte layer 426 may be disposed between the consecutive electrodes 402A, 402B. The solid electrolyte layer 426 is a separator that physically separates the first electrode 402A from the second electrode 402B. The solid electrolyte layer 426 may be defined by a third plurality of solid electrolyte particles 430. As in Figure 1A and 1BIn the case of the first, second and third pluralities of electroactive material particles 450, 460, 430 may be the same or different.

[0115] As detailed above, for example Figure 1B In some cases, the ion gel 498 can be disposed in the battery pack 400 to wet the interfaces between the solid electrolyte particles 450, 460 and / or the solid electrolyte material particles 430, 490, 492 and / or fill the void spaces between the solid electrolyte particles 450, 460 and / or the solid electrolyte material particles 430, 490, 492, so as to, for example, reduce the inter-particle porosity and improve ionic contact.

[0116] Refer to Figure 4A , the current collector 436 may have a thickness of greater than or equal to about 2 μm to less than or equal to about 60 μm, and in some aspects optionally greater than or equal to about 5 μm to less than or equal to about 30 μm. The current collector 436 may include at least one of stainless steel, aluminum, nickel, iron, titanium, copper, tin, or any other conductive material known to those skilled in the art. In some variations, the current collector 436 may be a cladding foil (i.e., one side of the current collector (e.g., the first side) contains a metal (e.g., a first metal), and the other side of the current collector (e.g., the second side) contains another metal (e.g., a second metal)), including, for example, aluminum-copper (Al-Cu), nickel-copper (Ni-Cu), stainless steel-copper (SS-Cu), aluminum-nickel (Al-Ni), aluminum-stainless steel (Al-SS), and nickel-stainless steel (Ni-SS). In some variations, the current collector 436 may be pre-coated, such as a carbon-coated aluminum current collector.

[0117] In other variations, such as Figure 4B As shown in , the current collector 436 may include a first current collector 438 and a second current collector 442. As shown, the first current collector 438 may define a first side or surface 432 of the current collector 436, and the second current collector 442 may define a second side or surface 434 of the current collector 436. Thus, the first current collector 438 may be adjacent to or near the first plurality of electroactive material particles 450 (and the first plurality of solid electrolyte particles 490), and the second current collector 442 may be adjacent to or near the second plurality of electroactive material particles 460 (and the second plurality of solid electrolyte particles 492).

[0118] The first current collector 438 may be different from the second current collector 442. In some variations, the first current collector 438 may be a negative electrode current collector, and the second current collector 442 may be a positive electrode current collector. In each case, the first and second current collectors 438, 442 may each include at least one of stainless steel, aluminum, nickel, iron, titanium, copper, tin, or any other conductive material known to those skilled in the art. The first and second current collectors 438, 442 may each have a thickness such that the current collector 436 has a thickness of greater than or equal to about 2 μm to less than or equal to about 60 μm, and in some aspects optionally greater than or equal to about 5 μm to less than or equal to about 20 μm.

[0119] In some variants, such as Figure 4C As shown in , the battery pack 400 may include one or more polymer barriers. The polymer barrier may be applied at or adjacent to the cell boundary to mitigate potential ionic short circuits. For example, the polymer barrier may contact or connect one or more current collectors at or adjacent to the cell boundary. As shown, the first polymer barrier 470A may be disposed at or toward the first end 472 of the current collector 436 of the first electrode 402A, and disposed at or toward the first end 472 of the current collector 436 of the second electrode 402B, so that the first polymer barrier 470A connects the first and second electrodes 402A, 402B. The second polymer barrier 470B can be disposed at or toward the second end 474 of the current collector 436 of the first electrode 402A, and can be disposed at or toward the second end 474 of the current collector 436 of the second electrode 402B, such that the second polymer barrier 470B also connects the first and second electrodes 402A, 402B. Although a single polymer barrier pair (i.e., polymer barrier 470A, 470B) is shown, those skilled in the art will recognize that the present teachings are also applicable to battery packs in which polymer barriers are applied to individual cells and / or alternating cells and / or various other battery packs and battery configurations.

[0120] The polymer stoppers 470A, 470B include ion and / or electronic insulating materials having strong adhesion (e.g., greater than or equal to about 0.01 MPa to less than or equal to about 1000 MPa, and in some aspects, optionally greater than or equal to about 0.1 MPa to less than or equal to about 40 MPa) and excellent thermal stability (e.g., greater than or equal to about 40° C. to less than or equal to about 200° C., and in some aspects, optionally greater than or equal to about 45° C. to less than or equal to about 150° C.). For example, each polymer stopper 470A, 470B may include at least one of the following: a hot melt adhesive (e.g., polyurethane resin, polyamide resin, polyolefin resin); polyethylene resin; polypropylene resin; a resin containing an amorphous polypropylene resin as a main component and obtained by copolymerizing, for example, ethylene, propylene, and butylene; silicone; polyimide resin; epoxy resin; acrylic resin; rubber (e.g., ethylene-propylene diene rubber (EPDM)); isocyanate adhesive; acrylic resin adhesive; and cyanoacrylate adhesive. Each polymer barrier 470A, 470B can have a thickness of greater than or equal to about 2 μm to less than or equal to about 200 μm, and in certain aspects optionally greater than or equal to about 40 μm to less than or equal to about 150 μm. Those skilled in the art will recognize that polymer barriers having various other configurations can also be used in the battery pack 400 to mitigate potential ionic short circuits.

[0121] Certain features of the present technology are further demonstrated in the following non-limiting examples. Example

[0122] An example battery 500 is prepared according to various aspects of the present disclosure. For example, the example battery 500 may include a solid electrode and a solid electrolyte layer disposed therebetween. The solid electrolyte layer may include a first plurality of solid electrolyte particles, such as described above, for example, in Figure 1B For example, the first plurality of solid electrolyte particles may include LATP. The first solid electrode may be a negative electrode including a plurality of solid negatively electroactive particles and a second plurality of solid electrolyte particles, as described above, for example, in Figure 1B For example, the second plurality of solid electrolyte particles may comprise LLZO. The second solid electrode may be a positive electrode comprising a plurality of solid positively electroactive particles and a third plurality of solid electrolyte particles, as described above, for example, in Figure 1B For example, the third plurality of solid electrolyte particles may include LATP. The battery 500 of this embodiment may include an ion gel including PVDF-HFP + Li(G3)TFSI ionic liquid.

[0123] A comparative cell 502 was prepared having the same solid electrode and solid electrolyte layers as the example cell 500, but containing a conventional gel, such as PVDF-HFP + LiPF6-EC / PC / DMC, instead of the ion gel.

[0124] Figure 5A 1C charge-discharge curves at 80°C are shown for each of the example battery 500 and the comparative battery 502. "1C" refers to a battery that can be fully charged and discharged within 1 hour. The x-axis 510 represents time in seconds (s). The y-axis 520 represents voltage (V). As shown, the example battery 500 including the ion gel according to various aspects of the present technology has an improved discharge capacity of 0.874 mAh compared to the comparative battery 502 including the conventional gel having a discharge capacity of 0.792 mAh.

[0125] Figure 5B Comparative 1C cycle capacities of comparative cells 500, 502 are shown. Line 500A represents the charging of the embodiment cell 500. Line 500B represents the discharging of the embodiment cell 500. Line 502A represents the charging of the comparative cell 502. Line 502B represents the discharging of the comparative cell 502. The x-axis 540 represents the number of cycles. The y-axis 520 represents the capacity (Ah). As shown, the embodiment cell 500 including the ion gel according to various aspects of the present technology has improved coulombic efficiency (which is equal to [(discharge capacity / charge capacity)*100]) and long-term cycle stability when compared to the comparative cell 502 including the conventional gel.

[0126] For the purpose of illustration and description, embodiments have been described above. It is not intended to be exhaustive or limit the present disclosure. The individual elements or features of a particular embodiment are generally not limited to that particular embodiment, but are interchangeable where appropriate, and can also be used in selected embodiments even if not specifically shown or described. Also can be changed in many ways. Such changes should not be considered as departing from the present disclosure, and all such modifications are intended to be included in the scope of the present disclosure.

Claims

1. A solid-state battery pack comprising: two or more electrodes, each electrode comprising a plurality of solid electroactive particles; one or more solid electrolyte layers, each solid electrolyte layer comprising a plurality of solid electrolyte particles, wherein a first solid electrolyte layer of the one or more solid electrolyte layers is disposed between a first electrode and a second electrode of the two or more electrodes; and an ion gel disposed in void spaces between two or more electrodes, solid electroactive particles of two or more electrodes, solid electrolyte particles of one or more solid electrolyte layers, and one or more solid electrolyte layers, such that the solid-state battery has an inter-particle porosity of less than or equal to 20% by volume, wherein the ion gel has an ionic conductivity of greater than or equal to 0.1 mS / cm to less than or equal to 10 mS / cm, wherein the ion gel comprises greater than or equal to 30 wt % and less than or equal to 95 wt % of the ionic liquid and greater than or equal to 2 wt % and less than or equal to 40 wt % of the solid component, The solid component is selected from the group consisting of carboxymethyl cellulose (CMC), wherein 1,000≤n≤10,000,000, poly(vinyl alcohol) (PVA), wherein 1,000≤n≤10,000,000, polyvinyl pyrrolidone (PVP), wherein 1,000≤n≤10,000,000, and combinations thereof.

2. The solid-state battery of claim 1, wherein the ionic liquid comprises cations and anions, wherein the cation is selected from: Li(triethylene glycol dimethyl ether)methylimidazolium ([Li(G3)] + )、Li(tetraethylene glycol dimethyl ether)([Li(G4) + ])、1-ethyl-3([Emim] + )、1-propyl-3-methylimidazolium ([Pmim] + )、1-butyl-3-methylimidazolium ([Bmim] + )、1,2-dimethyl-3-butylimidazolium ([DMBim]), 1-alkyl-3-methylimidazolium ([Cnmim] + ), 1-allyl-3-methylimidazolium ([Amim] + )、1,3-diallylimidazolium ([Daim] + ), 1-allyl-3-vinylimidazolium ([Avim] + ); 1-vinyl-3-ethylimidazolium ([Veim] + ), 1-cyanomethyl-3-methylimidazolium ([MCNim] + )、1,3-Dicyanomethyl-imidazolium ([BCNim] + ), 1-propyl-1-methylpiperidinium ([PP 13 ] + ), 1-butyl-1-methylpiperidinium ([PP 14 ] + ), 1-methyl-1-ethylpyrrolidinium ([Pyr 12 ] + ), 1-propyl-1-methylpyrrolidinium ([Pyr 13 ] + ), 1-butyl-1-methylpyrrolidinium ([Pyr 14 ] + ), methyl-methylcarboxymethyl-pyrrolidinium ([MMMPyr] + ), tetramethylammonium ([N 1111 ] + ), tetraethylammonium ([N 2222 ] + ), tributylmethylammonium ([N 4441 ] + ), diallyldimethylammonium ([DADMA] + ); NN-diethyl-N-methyl-N-(2-methoxyethyl)ammonium ([DEME] + )、N,N-diethyl-N-(2-methacryloylethyl)-N-methylammonium ([DEMM] + ), trimethyl isobutyl-phosphonium ([P 111i4 ] + ), triisobutylmethylphosphonium ([P 1i444 ] + ), tributylmethylphosphonium ([P 1444 ] + ), diethylmethylisobutylphosphonium ([P 1224 ] + ), trihexyldecylphosphonium ([P 66610 ] + ), trihexyltetradecylphosphonium ([P 66614 ] + ) and combinations thereof, and The anion is selected from the group consisting of hexafluoroarsenate, hexafluorophosphate, bis(fluorosulfonyl)imide (FSI), bis(trifluoromethanesulfonyl)imide (TFSI), perchlorate, tetrafluoroborate, cyclo-difluoromethane-1,1-bis(sulfonyl)imide (DMSI), bis(perfluoroethanesulfonyl)imide (BETI), bis(oxalato)borate (BOB), difluoro(oxalato)borate (DFOB), bis(fluoromalonato)borate (BFMB) and combinations thereof.

3. The solid-state battery of claim 2, wherein the ionic liquid further comprises a low boiling point solvent selected from the group consisting of dimethyl carbonate, ethylene carbonate, ethyl acetate, acetonitrile, acetone, toluene, propylene carbonate, diethyl carbonate, 1,2,2-tetrafluoroethyl, 2,2,3,3-tetrafluoropropyl ether, and combinations thereof.

4. The solid-state battery of claim 1 , wherein the ion gel further comprises greater than 0 wt % to less than 40 wt % of one or more lithium salts, wherein each lithium salt comprises an anion selected from the group consisting of hexafluoroarsenate, hexafluorophosphate, bis(fluorosulfonyl)imide (FSI), perchlorate, tetrafluoroborate, cyclo-difluoromethane-1,1-bis(sulfonyl)imide (DMSI), bis(trifluoromethanesulfonyl)imide (TFSI), bis(perfluoroethanesulfonyl)imide (BETI), bis(oxalato)borate (BOB), difluoro(oxalato)borate (DFOB), and bis(fluoromalonato)borate (BFMB).

5. The solid-state battery of claim 1, wherein the solid-state electrolyte layer comprises: a first layer comprising a first plurality of solid electrolyte particles, and A second layer includes a second plurality of solid electrolyte particles, wherein the first and second plurality of solid electrolyte particles are the same or different and the first and second plurality of solid electrolyte particles define the plurality of solid electrolyte particles.

6. The solid-state battery of claim 1, further comprising two or more current collectors, wherein a first current collector of the two or more current collectors is disposed adjacent to the first electrode, and a second current collector of the two or more current collectors is disposed adjacent to the second electrode, wherein at least one of the first and second current collectors comprises: a first half comprising a first material, and A second half includes a second material, wherein the second half is substantially parallel to the first half, and the first and second materials are different.

7. The solid-state battery pack of claim 6, further comprising a polymer barrier, wherein the polymer barrier enables the first current collector to contact the second current collector, and wherein the polymer barrier has a thickness greater than or equal to 2 μm to less than or equal to 200 μm, and comprises an insulating material selected from the group consisting of polyurethane resin, polyamide resin, polyolefin resin, polyethylene resin, polypropylene resin, ethylene, propylene, butene, a resin containing amorphous polypropylene resin as a main component and obtained by copolymerization of ethylene and / or propylene and / or butene, silicone, polyimide resin, epoxy resin, acrylic resin, ethylene-propylene-diene rubber (EPDM), isocyanate adhesive, acrylic resin adhesive, cyanoacrylate adhesive, and combinations thereof.

8. The solid-state battery of claim 1, wherein the solid-state battery is a bipolar battery; wherein the two or more electrodes include a first electrode, a second electrode, and one or more bipolar electrodes, the plurality of solid electroactive particles include a first plurality of solid electroactive particles and a second plurality of solid electroactive particles, and the one or more solid electrolyte layers include a first solid electrolyte layer and a second solid electrolyte layer; wherein each bipolar electrode comprises a current collector, and the first plurality of solid electroactive particles are disposed on a first side of the current collector, and the second plurality of solid electroactive particles are disposed on a second side of the current collector; wherein the first solid electrolyte layer is disposed between the first electrode and a first side of the one or more bipolar electrodes, and the second solid electrolyte is disposed between a second side of the one or more bipolar electrodes and the second electrode; and The ion gel is further arranged in the void space between the first plurality of solid electroactive particles and the second plurality of solid electroactive particles, the first solid electrolyte layer and the first electrode, one or more bipolar electrodes, one or more bipolar electrodes and the first solid electrolyte layer, one or more bipolar electrodes and the second solid electrolyte layer, and the second solid electrolyte layer and the second electrode.

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