Gel electrolyte

Abstract

a polymer, a gel solvent, and a compound of formula (I): [Formula 1] TIFF2026508079000020.tif41147, wherein X is Al or B, and R 1 is independently a substituent in each occurrence, and two R 1 groups may be joined to form a ring, M + is a cation. The gel electrolyte can be used in metal batteries or metal-ion batteries.

Description

[Background technology]

[0001] WO 99 / 12938 discloses polyfluorinated alkoxides coordinated to a transition metal or an element of Group III, IV, or V. The use of the compounds in batteries is disclosed.

[0002] Nolan et al., "Nonaqueous Lithium Battery Electrolytes Based on Bis(polyfluorodiolato)borates," 2003 J. Electrochem. Soc. 150 A1726, discloses lithium salts for use as battery electrolytes.

[0003] JP 2002 / 260734 A discloses an electrolyte of formula (1). [ka]

[0004] US Pat. No. 6,783,896 discloses compounds of formula (I). [ka]

[0005] EP 1075036 discloses compounds of formula (1). [ka]

[0006] Takahiro Aoki et al., "Lithium ion conductivity of gel polymer electrolytes containing insoluble lithium tetrakis(pentafluorobenzenethiolato)borate," Journal of Power Sources, Volume 156, Issue 2, June 1, 2006, Pages 589-593, discloses a lithium ion conductive gel polymer electrolyte composed of insoluble lithium tetrakis(pentafluorobenzenethiolato)borate (LiTPSB), poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), and an ethylene carbonate-propylene carbonate mixed solvent (EC-PC).

[0007] WO 2022 / 243470 discloses an electrolyte comprising solvated lithium ions. Summary of the Invention

[0008] The present disclosure provides a method for producing a gel comprising the steps of: [ka] wherein X is Al or B, and R 1 is independently a substituent in each occurrence, and two R 1 groups may be joined to form a ring, M + is a cation.

[0009] Optionally, the compound of formula (I) has formula (Ia): [ka] wherein R 2 is independently in each occurrence a divalent organic group.

[0010] Optionally, each R 2 is represented by formula (II): [ka] where R 3 is, in each occurrence, H or a substituent, and Ar 1 is C 6-20 It is an arylene group.

[0011] Optionally, Ar 1 is unsubstituted or substituted 1,2-phenylene.

[0012] Optionally, the mass of the polymer in the gel is no more than 30% of the mass of the compound of Formula (I).

[0013] Optionally, M + is lithium ion.

[0014] Optionally, the polymer is a crosslinkable polymer.

[0015] Optionally, the polymer is a cross-linked polymer.

[0016] The present disclosure provides a battery that includes a negative electrode, a positive electrode, and a gel electrolyte described herein disposed between the negative electrode and the positive electrode.

[0017] Optionally, the metal battery contains no more than 16 moles of total solvent per mole of M+.

[0018] The present disclosure provides a method of forming a metal battery or battery precursor thereof as described herein, wherein forming a gel electrolyte comprises depositing a formulation comprising a polymer, a gel solvent, a compound of Formula (I), and a depositing solvent onto a surface, and evaporating the depositing solvent.

[0019] Optionally, the polymer is crosslinkable and the method further comprises crosslinking the crosslinkable polymer.

[0020] Optionally, the surface is a surface of an electrode or an electrode current collector.

[0021] Optionally, after evaporation of the deposition solvent, the gel electrolyte is separated from the surface and applied to an electrode or electrode current collector surface. [Brief explanation of the drawings]

[0022] [Figure 1] FIG. 1 is a schematic diagram of a battery having a gel electrolyte as described herein. [Figure 2] 1 shows a Nyquist plot for a cell containing a gel electrolyte according to some embodiments of the present disclosure. DETAILED DESCRIPTION OF THE INVENTION

[0023] Unless the context clearly requires otherwise, throughout the specification and claims, words such as "comprise," "comprising," and the like shall be construed in an inclusive sense, i.e., "including, but not limited to," as opposed to an exclusive or exhaustive sense. Furthermore, the words "herein," "on," "under," and words of similar import, when used in this application, refer to this application as a whole and not to particular portions of this application. Where the context permits, words in the Detailed Description using the singular or plural may also include the plural or singular, respectively. The word "or" in connection with a list of two or more items encompasses all of the following interpretations of that word: any of the items in the list, all of the items in the list, and any combination of the items in the list. As used in this application, a reference to a layer "over" another layer means that the layers may be in direct contact, or that there may be one or more intervening layers. As used in this application, a reference to a layer "on" another layer means that the layers are in direct contact. A reference to an element of the periodic table includes any isotopes of that element.

[0024] The teachings of the technology provided herein may be applied to other systems, not necessarily the systems described below. Elements and acts of the various examples described below can be combined to provide further implementations of the technology. Some alternative implementations of the technology may include additional elements as well as fewer elements relative to those implementations described below.

[0025] These and other changes can be made to the technology in light of the following detailed description. While the description illustrates certain examples of the technology and explains the best mode contemplated, no matter how detailed the description may appear, the technology can be practiced in many ways. As described above, a particular term used when describing a particular feature or aspect of the technology should not be construed as meaning that the term is redefined herein to be limited to any particular feature, characteristic, or aspect of the technology associated with that term. In general, the terms used in the following claims should not be construed as limiting the technology to the particular embodiments disclosed herein, unless such terms are otherwise expressly defined in the "Description of Embodiments" section. Thus, the actual scope of the technology encompasses not only the disclosed embodiments but also all equivalent ways of practicing or implementing the technology according to the claims.

[0026] In order to reduce the number of claims, certain aspects of the technology are presented below in certain claim forms, but applicant contemplates various aspects of the technology in any number of claim forms.

[0027] In the following description, for purposes of explanation, numerous specific details are set forth in order to provide a thorough understanding of implementations of the disclosed technology. However, it will be apparent to one skilled in the art that embodiments of the disclosed technology may be practiced without some of these specific details.

[0028] Figure 1 shows a battery, which may be a metal battery or a metal ion battery, preferably a lithium battery or a lithium ion battery.

[0029] The battery includes an anode current collector 101 in contact on its surface with an anode 103, a cathode current collector 109 in contact with a cathode 107, and a layer 105 disposed between the anode and cathode, the layer including or consisting of a gel electrolyte as described herein.

[0030] In some embodiments, layer 105 is a gel layer comprising a polymer, a solvent, and a compound of formula (I).

[0031] In some embodiments, layer 105 is a porous separator that includes a gel as described herein imbibed into the porous separator.

[0032] In the case of metal ion batteries, such as lithium ion batteries, the negative electrode comprises an active material, such as graphite, for absorption of metal ions.

[0033] In a metal battery, the negative electrode 103 is a layer of metal (eg, lithium) that forms on the negative electrode current collector during charging of the battery and is removed during discharge of the battery.

[0034] The positive electrode may be selected from any positive electrode known to those skilled in the art.

[0035] The negative and positive current collectors can be any suitable conductive material known to those skilled in the art, for example, one or more layers of a metal or metal alloy such as aluminum or copper.

[0036] For simplicity, FIG. 1 shows a battery in which the negative and positive electrodes are separated only by a layer containing or consisting of gel, although it will be understood that in use, a solid electrolyte interface typically forms on the negative electrode surface.

[0037] In other embodiments, one or more additional layers may be disposed between the negative electrode and the gel and / or between the positive electrode and the gel.

[0038] Compounds of formula (I) Formula (I) is [ka] And, X is Al or B.

[0039] R 1 is independently a substituent in each occurrence, and two R 1 The groups may be joined to form a ring.

[0040] M + is a cation. M + is preferably an alkali metal cation, more preferably lithium.

[0041] In some embodiments, two pairs of R 1 The groups are attached so that the compound of formula (I) has the formula (Ia): [ka] wherein R 2 is independently in each occurrence a divalent organic group.

[0042] R 1 If no groups are attached, then preferably each R 1 is independently C at each occurrence. 1-20 It is an alkyl group, wherein one or more non-adjacent C atoms of the alkyl group can be substituted by O, S, CO, or COO, and one or more H atoms of the alkyl group can be substituted by F.

[0043] Preferred R 1 The group is C 1-20 Contains alkyl, OR 1 One or more C atoms other than the C atom bonded to O or terminal C atoms may be substituted with O, and one or more H atoms may be substituted with F.

[0044] In the case of formula (Ia), R 2 is preferably Ar 1 and Ar 1is independently at each occurrence an optionally substituted C which may be unsubstituted or substituted with one or more substituents, e.g., 1,2-phenylene; 6-20 Arylene groups, Ar 1 , which may be unsubstituted or substituted with one or more substituents, for example, 2,2'-linked biphenylene; 1 -Ar 1 Biarylene groups of the formula (II): [ka] where R 3 is H or a substituent in each occurrence, and Ar 1 C 6-20 an arylene group, preferably unsubstituted or substituted 1,2-phenylene, of formula (II)

[0045] Preferably, R 3 independently at each occurrence represents H, or C in which one or more H atoms may be replaced by F and one or more non-terminal C atoms may be replaced by O. 1-6 It is an alkyl group.

[0046] In a preferred embodiment, at least one R 3 , optionally each R 3 is C 1-6 It is a perfluoroalkyl group.

[0047] Preferably, each Ar of formula (I) 1 is phenylene, more preferably 1,2-linked phenylene that is unsubstituted or substituted with one or more substituents.

[0048] If present, Ar 1 The substituents in are preferably, and independently, F and C 1-12 alkyl, and one or more non-adjacent C 1-12 Non-terminal C atoms of alkyl are O, S, NR 4 , CO COO or CONR 4 wherein R 4 is independently C1-12 is a hydrocarbyl group, C 1-12 One or more H atoms of the alkyl group may be replaced with F.

[0049] As used herein, a "non-terminal C atom" of an alkyl group means one of the methyl groups at the chain end of a linear alkyl chain or at the chain end of a branched alkyl group, respectively.

[0050] C anywhere in this specification 1-12 The hydrocarbyl group is preferably C 1-12 Alkyl, phenyl, and one or more C 1-6 phenyl substituted with an alkyl group.

[0051] The compound of formula (I) can be prepared by reacting a compound of formula (III) with R 1 If the group is not attached, it may be formed by reacting a compound of either formula (IVa) or (IVb), or in the case of a compound of formula (Ia), with a compound of formula (V). [ka]

[0052] The compound of formula (IVa) may be a primary, secondary, or tertiary alcohol.

[0053] The compound of formula (IVb) may be an aldehyde or a ketone.

[0054] Exemplary compounds of formula (III) include, but are not limited to, lithium aluminum hydride (LiAlH4) and lithium borohydride (LiBH4).

[0055] polymer The polymer may be selected from any known ion-conducting polymer, including, but not limited to, poly(alkylene oxides), such as poly(ethylene oxide) and poly(propylene oxide), and fluorinated polymers, such as polyvinylidene fluoride, PVDF-HFP, PMMA, polyacrylonitrile, polycarbonate, polyethylene, polypropylene, poly(vinyl methyl ketone), polyvinylpyrrolidone, polyether ether ketone, polyisoprene, polybutadiene, polystyrene-block-polyisoprene-block-polystyrene, poly(1-vinylpyrrolidone-co-vinyl acetate), polystyrene-block-polybutadiene-block-polystyrene, polystyrene-block-poly(ethylene oxide)-block-polystyrene, copolymers, and mixtures thereof.

[0056] The polymer is preferably a neutral polymer, ie not a polymer substituted with ionic groups, and particularly preferably not a single-ion conducting polymer containing anionic groups.

[0057] Preferably, the mass of the polymer in the gel is 3 to 90% by weight, more preferably 5 to 30% by weight, of the mass of the compound of formula (I).

[0058] In some embodiments, the gel polymer is crosslinked. In some embodiments, the crosslinked gel polymer may be formed by the reaction of an uncrosslinked polymer substituted with a substituent comprising a crosslinkable group. The crosslinkable group may be represented by formula (VI): [ka] may be a group In the formula, Sp is a spacer group, x is 0 or 1, and XL is a crosslinkable group.

[0059] Optionally, XL: (i) Formula -CR 5 acyclic units of the formula =CH2, where R 5 is H or a substituent, preferably C, such as vinyl, styryl acrylate or methacrylate.1-6 an alkyl group of the formula -CR 5 =CH2 acyclic units, (ii) a cyclic alkene, preferably an optionally substituted norbornene, cyclopropene, or cyclobutene; (iii) an optionally substituted epoxide, and (iv) optionally substituted benzocyclobutene.

[0060] The optionally substituted benzocyclobutene-containing bridging group has the formula (VI): [ka] wherein R 6 is H or a substituent at each occurrence, q is 0, 1, 2 or 3, preferably 0, and R 7 is a substituent at each occurrence.

[0061] Preferably, two R are bonded to the same carbon atom. 6 At least one of the groups R 6 is H. Optionally, each R in formula (VI) 6 is H or only one R of formula (IV) 6 is not H. Exemplary non-H groups R 6 is C 1-6 Alkyl and C 1-6 It is an alkoxy.

[0062] R 7 When present, preferably F, Cl, NO, CN, C 1-6 Alkyl and C 1-6 Alkoxy is selected from:

[0063] Sp is preferably optionally substituted phenylene, and C 1-20 alkylene, C 1-20 One or more H atoms of the alkylene can be replaced by F, and one or more non-adjacent C atoms can be replaced by O, S, NR 4 , Si(R 8 )2, CO, COO or CONR 4and R 4 is H or a substituent as defined above, and each R 8 are independently a substituent, optionally C 1-20 It is a hydrocarbyl group.

[0064] Optional substituents of the phenylene group Sp include F, CN, NO2, and one or more H atoms may be replaced by F, and one or more non-adjacent C atoms may be replaced by O, S, NR 4 , Si(R 8 )2, CO, COO or CONR 4 C can be substituted with 1-20 It is alkylene.

[0065] In some embodiments, the crosslinked gel polymer can be formed by reacting a composition comprising a compound of Formula (I), a gel solvent, and a monomer for forming the crosslinked polymer. The composition can contain only one type of monomer. The composition can contain two or more different types of monomer. The composition can include an initiator.

[0066] solvent The gel comprises at least one solvent.

[0067] The one or more solvents may be, for example, C 2 carbonates such as propylene carbonate, ethylene carbonate, and dimethyl carbonate. 2-10 Alkylene carbonate, di(C 1-10 alkyl)carbonates, such as glyme, diglyme, triglyme and tetraglyme, linear, branched or cyclic compounds containing two or more ether groups, such as 1,3-dioxolane, 2,5-dimethoxytetrahydrofuran, succinonitrile, cyclic lactones, such as gamma-butyrolactone, and mixtures thereof.

[0068] Preferably, the one or more solvents have a boiling point of at least 200°C.

[0069] Preferably, the gel contains no more than 16 moles, and optionally no more than 10 moles, of total solvent per mole of M+. The solvent / M+ ratio is determined by the ratio of the solvent to the total solvent in the finished gel prior to battery formation.1 It can be determined from the integration of the 1 H NMR spectrum.

[0070] The presence of a solvent has been found to significantly increase the ionic conductivity of compounds of formula (I). Without wishing to be bound by any theory, this increase is believed to be due to the + This is due to the solvation of the cation.

[0071] Gel formation The gel may be formed by depositing a solution containing a compound of formula (I), a gel solvent, a gel polymer, or a crosslinkable gel polymer (which may be a crosslinkable monomer or polymer) and a film-forming solvent onto a surface, followed by evaporation of the film-forming solvent and, in the case of a crosslinkable gel polymer, crosslinking the crosslinkable gel polymer to form a crosslinked gel polymer.

[0072] Crosslinking of the crosslinkable polymer can be achieved by any method known to those skilled in the art, including heat treatment or radiation, e.g., UV radiation, with heat treatment being preferred given that the cell casing is typically opaque if crosslinking is performed after the cell is assembled.

[0073] The casting solvent(s) suitably have a lower boiling point than the gel solvent, preferably at least 100° C. lower than the gel solvent(s). Exemplary casting solvents include, but are not limited to, tetrahydrofuran, dimethoxyethane, acetone, acetonitrile, dimethyl carbonate, and mixtures thereof.

[0074] battery formation A battery can be formed by providing a gel described herein on the surface of one of the negative and positive electrodes, and by providing the other of the negative and positive electrodes and associated current collectors on top of the gel.

[0075] A metal battery precursor can be formed by providing a gel described herein on the surface of a negative electrode current collector, and by providing a positive electrode and a positive electrode current collector over the gel. Upon application of a charging bias, a lithium negative electrode can be formed between the gel and the negative electrode current collector.

[0076] In some embodiments, the gel may be formed by depositing the solution onto an electrode or current collector, followed by evaporation of the deposition solvent and, in the case of a crosslinkable polymer, crosslinking the polymer.

[0077] In some embodiments, a preformed gel is deposited onto an electrode or current collector. [Example]

[0078] Preparation of electrolytes All solutions were prepared in a nitrogen-filled glove box (O2<0.1 ppm, H2O<3 ppm).

[0079] A stock solution of PVDF-HFP (Mn=110 kDa, Mw=455) in tetrahydrofuran:propylene carbonate (THF:PC, 90:10, v:v) was prepared at a concentration of 100 mg / ml.

[0080] Solution 1 containing Compound Example 1 and PC was prepared with 1.93 molecules of PC per molecule of lithium cation.

[0081] Solution 2 containing Compound Example 2, PC, and THF was prepared with 5.83 molecules of PC and 0.55 molecules of THF per molecule of lithium cation. [ka]

[0082] Gel Example 1 163 mg of Solution 1 was weighed into a 2 ml clear glass vial. 0.15 ml of the PVDF-HFP stock solution was added to it. After homogenization, the mixture gelled. An additional 0.15 ml of THF:PC (9:1) solution was added to it to obtain a clear, free-flowing solution.

[0083] Gel Example 2 73 mg of Solution 1 was weighed into a 2 ml clear glass vial. 0.2 ml of PVDF-HFP stock solution was added to it. After mixing, a clear, free-flowing solution was obtained.

[0084] Gel Example 3 30 mg of Solution 1 was weighed into a 2 ml clear glass vial. 0.25 ml of PVDF-HFP stock solution was added to it. After mixing, a clear, free-flowing solution was obtained.

[0085] Gel Example 4 11 mg of Solution 1 was weighed into a 2 ml clear glass vial. 0.25 ml of PVDF-HFP stock solution was added to it. After mixing, a clear, free-flowing solution was obtained.

[0086] Gel Example 5 3.5 mg of Solution 1 was weighed into a 2 ml clear glass vial. 0.25 ml of PVDF-HFP stock solution was added to it. After mixing, a clear, free-flowing solution was obtained.

[0087] Gel Example 6 230 mg of Solution 1 was weighed into a 2 ml clear glass vial. 0.10 ml of the PVDF-HFP stock solution was added to it. After homogenization, the mixture gelled. An additional 0.12 ml of THF:PC (9:1) solution was added to it to obtain a clear, free-flowing solution.

[0088] Gel Example 7 343 mg of Solution 1 was weighed into a 2 ml clear glass vial. 0.5 ml of the PVDF-HFP stock solution was added to it. After homogenization, the mixture gelled. An additional 0.20 ml of THF:PC (9:1) solution was added to it to obtain a clear, free-flowing solution.

[0089] Gel Example 8 0.220 ml of Gel Example 7 solution was placed in a 2 ml clear glass vial. 0.033 ml of PC was added to it. After mixing, a clear, free-flowing solution was obtained.

[0090] Gel Example 9 0.220 ml of Gel Example 7 solution was placed in a 2 ml clear glass vial. 0.066 ml of 1,2-dimethoxyethane (1,2-DME) was added to it. After mixing, a clear, free-flowing solution was obtained.

[0091] Gel Example 10 0.180 ml of Gel Example 7 solution was placed in a 2 ml clear glass vial. 0.0405 ml of PC and 0.054 ml of 1,2-DME were added to it. After mixing, a clear, free-flowing solution was obtained.

[0092] Gel Example 11 295 mg of Solution 2 was weighed into a 2 ml clear glass vial. 0.15 ml of the PVDF-HFP stock solution was added to it. After homogenization, the mixture gelled. An additional 0.10 ml of THF:PC (9:1) solution was added to it to obtain a clear, free-flowing solution.

[0093] Gel Example 12 620 mg of Solution 2 was weighed into a 2 ml clear glass vial. 0.5 ml of PVDF-HFP stock solution was added to it. After mixing, a clear, free-flowing solution was obtained.

[0094] Gel Example 13 0.220 ml of Gel Example 12 solution was placed in a 2 ml clear glass vial. 0.033 ml of PC was added to it. After mixing, a clear, free-flowing solution was obtained.

[0095] Gel Example 14 11.7 mg of PEG 400 was placed in a 2 ml clear glass vial. 0.220 ml of Gel Example 12 solution was added to it. After mixing, a clear, free-flowing solution was obtained.

[0096] Gel Example 15 0.200 ml of the gel example 12 solution was placed in a 2 ml clear glass vial. 0.030 ml of PC and 0.060 ml of 1,2-DME were added to it. After mixing, a clear, free-flowing solution was obtained.

[0097] Cell formation - gel electrolyte 0.2 ml of each of gel Examples 1-15 was drop-cast using a micropipette onto a stainless steel disc on a hot plate set at 30°C.

[0098] After 15 minutes, the temperature was increased to 40°C and the film was allowed to dry for 1 hour, after which the hotplate was turned off and the disc was allowed to cool to room temperature.

[0099] All solutions resulted in films with gel-like consistencies, ranging from very soft gels to gels that could be removed from stainless steel discs and remained intact.

[0100] The film supported on the stainless steel disk was then transferred under inert atmosphere to an argon-filled glove box for cell assembly.

[0101] The film, supported on a stainless steel disk, was cut into an 8 mm disk diameter using a manual cutter. The outer portion was peeled off from the surface of the stainless steel disk and saved for NMR analysis to determine the solvent content. Any remaining material was removed using a THF-impregnated swab.

[0102] A 200 micron thick silicone spacer shaped as a 16 mm diameter disk with a 9 mm diameter circular hole cut in its center was placed on the stainless steel disk surrounding the 8 mm diameter film.

[0103] To form a coin cell, the stainless steel disk carrying the gel film and silicone spacer was placed on top of another stainless steel disk at the bottom of the coin cell, and a second stainless steel disk was placed on top of the spacer, plus the wave spring and top of the coin cell, followed by crimping.

[0104] The silicone spacer ensures that the gel film is 200 microns thick after crimping, allowing for accurate conductivity calculations and preventing the gel film from being compressed to a smaller thickness after crimping, which could cause a short circuit.

[0105] Cell Formation - Solution Electrolyte For comparison purposes, coin cells containing electrolyte solutions with various concentrations of Compound Example 1 or 2 without any polymer were prepared. The cells were fabricated by inserting a stainless steel spacer into the bottom of the coin cell, followed by a fluorosilicone spacer. A stencil was molded as a 155 mm diameter disk with a 5 mm diameter circular hole drilled in its center. 30 μl of electrolyte solution was filled into the spacer opening. Two stainless steel spacers were placed on top of the stencil, along with a wave spring and the top of the coin cell, and then crimped. The thickness of the stencil in the crimped cell was 360 μm.

[0106] All coin cells were assembled in a rigorously dried, oxygen-free, argon-gas-filled MBraun glove box.

[0107] Electrochemical Impedance Spectroscopy EIS measurements of the coin-type cells were carried out at room temperature using a potentiostat (Interface 1010E, Gamry Instruments).

[0108] EIS spectra were performed over a frequency range of 1 Hz to 1 MHz at an amplitude of 5 mV.

[0109] The ionic conductivity was calculated using the following formula:

number

[0110] The impedance of the cell was determined by fitting the equivalent circuit to the Nyquist plot (inset of Figure 2), with resistor 1 corresponding to the x-intercept of the first semicircle on the x-axis of the Nyquist plot (Figure 2).

[0111] Resistor 1 was used to calculate the conductivity of the material according to the above formula. The ionic conductivities are listed in Table 1. [Table 1]

[0112] Compound Example 2 provides higher ionic conductivity than Compound Example 1.

[0113] Ionic conductivity and gel flexibility increase with increasing solvent additive content.

[0114] Increasing the amount of polymer results in a decrease in ionic conductivity, which makes the gel less adhesive to metal and glass surfaces, but also more robust.

Claims

1. a polymer, a gel solvent, and a compound of formula (I): 【Chemistry 1】 A gel electrolyte comprising a compound of In the formula, X is Al or B, and R １ is independently a substituent in each occurrence, and two R １ The groups may be joined to form a ring, and M ＋ is a cation, a gel electrolyte.

2. The compound of formula (I) has the formula (Ia): 【Chemistry 2】 and In the formula, R ２ 10. The gel electrolyte of claim 1, wherein each occurrence of is independently a divalent organic group.

3. Each R ２ is represented by formula (II): 【Transformation 3】 is the basis of In the formula, R ３ is H or a substituent at each occurrence, and Ar １ is C ６－２０ The gel electrolyte according to claim 2 , wherein the group is an arylene group.

4. Ar １ The gel electrolyte according to claim 3, wherein is unsubstituted or substituted 1,2-phenylene.

5. The gel electrolyte according to any one of claims 1 to 4, wherein the mass of the polymer in the gel is 30% or less of the mass of the compound of formula (I).

6. M ＋ The gel electrolyte according to any one of claims 1 to 5, wherein is a lithium ion.

7. The gel electrolyte according to any one of claims 1 to 6, wherein the polymer is a crosslinkable polymer.

8. The gel electrolyte according to any one of claims 1 to 6, wherein the polymer is a cross-linked polymer.

9. A battery comprising a negative electrode, a positive electrode, and the gel electrolyte according to any one of claims 1 to 8, disposed between the negative electrode and the positive electrode.

10. 10. The metal battery of claim 9, wherein the metal battery contains no more than 16 moles of total solvent per mole of M+.

11. 11. A method for forming the metal battery or battery precursor thereof according to any one of claims 1 to 10, wherein forming the gel electrolyte comprises depositing a film on a surface of a formulation comprising the polymer, the gel solvent, the compound of formula (I), and a film-forming solvent, and evaporating the film-forming solvent.

12. The method of claim 11 , wherein the polymer is crosslinkable, and the method further comprises crosslinking the crosslinkable polymer.

13. 13. The method of claim 11 or 12, wherein the surface is a surface of an electrode or an electrode current collector.

14. 13. The method of claim 11 or 12, wherein the gel electrolyte separates from the surface after evaporation of the deposition solvent and is applied to an electrode or electrode current collector surface.

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