Enhancing in SITU polymerizable solid polymer electrolytes with exfoliated hexagonal boron nitride or fluorine-functionalized hexagonal boron nitride

Abstract

An exemplary embodiment of the present disclosure provides a method for making an electrolyte, comprising: providing a solid polymer electrolyte (SPE); incorporating boron nitride with the SPE to form a composite polymer electrolyte (CPE), wherein the boron nitride is at least one of exfoliated hexagonal boron nitride (ex-BN) or fluorine-fimctionalized hexagonal boron nitride (BN-F).

Description

Attorney Docket No: 011529.114794 ENHANCING IN SITU POLYMERIZABLE SOLID POLYMER ELECTROLYTES WITH EXFOLIATED HEXAGONAL BORON NITRIDE OR FLUORINE- FUNCTIONALIZED HEXAGONAL BORON NITRIDE CROSS-REFERENCE TO RELATED APPLICATIONS

[0001] This application claims the benefit of U.S. Provisional Application Serial No.63 / 675,936, filed on 26 July 2024, which is incorporated herein by reference in its entirety as if fully set forth below FIELD OF THE INVENTION

[0002] The various embodiments of the present disclosure relate generally to rechargeablebatteries, and more particularly, to enhancing in situ polymerizable solid polymer electrolytes for lithium-ion batteries using exfoliated hexagonal boron nitride or fluorine-functionalized hexagonal boron nitride. BACKGROUND

[0003] Advancing next-generation rechargeable batteries with higher energy density, longer cyclelife, and improved safety is critical for electric vehicles (EVs), smart grids, and flexible electronics. Lithium-ion Batteries (LIBs), which use intercalation-based graphite anodes with a capacity of 372 mAh·gb*, are widely used, but their limited electrochemical capacity restricts their effectiveness in extended-range EVs and advanced electronics. As a result, Lithium Metal Batteries (LMBs) have gained interest due to their ultrahigh theoretical energy densities, potentially enhancing energy densities by 35% in weight and 50% in volume. However, LMBs face significant challenges, mainly the severe growth of Lithium (Li) dendrites, which can breach the separator and cause short circuits. Additionally, conventional organic liquid electrolytes are toxic, flammable, prone to leakage, and exhibit poor thermal stability, posing serious safety concerns.

[0004] To achieve high-energy-density LIBs, innovative electrolytes that resist dendrite growth andensure safety are essential. Solid-state electrolytes (SSEs) are particularly promising due to their mechanical strength, which mitigates dendrite growth, and their low flammability and non-leakage properties, enhancing battery safety. SSEs include inorganic solid electrolytes (ISEs), solid polymer electrolytes (SPEs), and composite polymer electrolytes (CPEs). Despite their high Lithium ionicIUTJZIYO[OY^ #e=O+) and mechanical strength, ISEs face challenges such as high interfacial resistance316687865v5Attorney Docket No: 011529.114794 between the cathode and electrolyte and difficulties in forming effective Li-ion pathways within the cathode. Poor contact and chemical incompatibility lead to significant energy losses, and their rigidity hinders continuous Li-ion pathways, reducing battery performance.

[0005] SPEs, made from polymer matrices like poly(ethylene oxide) (PEO), polyacrylonitrile (PAN),and poly(vinylidene fluoride) (PVDF), offer flexibility, good processability, low cost, and excellent interfacial contact with electrodes. In situ polymerizable SPEs have been further developed to achieve a conformal interface with electrodes. Initially, the liquid-state electrolyte precursor is conformally applied to the electrodes and then solidified after integration, ensuring optimal contact and enhancedVKWLUWSGTIK( ;U\K[KW& BA8X MKTKWGRR^ K]NOHOY RU\ e=O+ at room temperature (<10b- BjISb*).>UJOL^OTM YNK VUR^SKW SGYWO] XYWZIYZWK NGX XNU\T VWUMWKXX& HZY ROSOYKJ e=O+ remains challenging. ForOTXYGTIK& A8@'HGXKJ KRKIYWUR^YKX IUTYGOTOTM =O XGRYX K]NOHOY RU\ e=O+ (<1×10b / BjISb* at 25 °C) due totheir crystalline phases.

[0006] Recently, propylene carbonate (PC) electrolytes, where Li salts are dissolved in PC, haveGYYWGIYKJ GYYKTYOUT LUW YNKOW NOMN e=O+, exceeding 1×10b, BjISb* at 25 °C. However, succinonitrile (SN)-based PC electrolytes lack mechanical strength and electrochemical stability, making them impractical.

[0007] Accordingly, there is a need for improved electrolytes addressing one or more of thedisadvantages discussed above. SUMMARY OF THE INVENTION

[0008] To address the challenges of increasing energy and power densities in rechargeable batteries,certain embodiments of the present disclosure focus on enhancing in situ polymerizable solid polymer electrolytes (SPEs) for next-generation rechargeable lithium (Li)-ion batteries (LIBs) using exfoliated hexagonal boron nitride (ex-BN) or fluorine-functionalized hexagonal boron nitride (BN-F). The incorporation of ex-BN or BN-F significantly improves the electrochemical and mechanical properties of in situ polymerizable SPEs through Li-ion transport enhancement and mechanical robustness, along with a high surface area. The present disclosure encompasses the synthesis, characterization, and performance evaluation of ex-BN- or BN-F-incorporated PC-based SPEs, demonstrating improved Li- ion transport properties, mechanical strength, and chemical stability. The practical applications of these composite polymer electrolytes (CPEs) in Li metal batteries (LMBs) are also explored, highlighting their potential to enhance battery performance, safety, and longevity. This development aims to enhance the commercial viability and sustainability of LMBs, particularly all-solid-state LMBs (ASSLMBs), for widespread use in electric vehicles (EVs) and beyond. 316687865v5Attorney Docket No: 011529.114794

[0009] To enhance the efficiency and reduce production costs of LMBs, particularly ASSLMBs,the present disclosure introduces high-performance CPEs utilizing in situ polymerizable SPEs with 0.5 wt.% or less of high-surface-area functional inorganic fillers, such as ex-BN and BN-F. Hexagonal BN (h-BN) is a promising filler due to its chemical inertness, mechanical strength, electrical insulation, and ability to immobilize anions, thereby increasing the Li-ion selectivity. BN-F can further enhance electrolyte stability with electrodes, preventing decomposition and ensuring a longer battery lifespan. Integrating ex-BN and BN-F into in situ polymerizable SPEs can result in CPEs with improved mechanical properties and enhanced electrochemical properties, ultimately boosting ASSLMB performance and reducing production costs.

[0010] Certain embodiments of the present disclosure address these challenges by employing ascalable and efficient process to incorporate ex-BN or BN-F into in situ polymerizable CPEs, which significantly enhances their performance. In particular, the present disclosure provides processes for synthesizing ex-BN or BN-F-incorporated in situ polymerizable CPEs by, for example, synthesizing ex-BN and BN-F and incorporating these into the polymer matrix to form high-performance CPEs. The electrochemical and mechanical properties of the ex-BN or BN-F-incorporated CPEs are thenK]GSOTKJ& OTIRZJOTM3 #O$ GXXKXXOTM YNK OUTOI IUTJZIYO[OY^ #e=O+) and Li-ion transference number (tLi+)of the in situ polymerizable CPEs with ex-BN or BN-F; (ii) conducting linear sweep voltammetry (LSV) to evaluate the electrochemical stability and performance; and (iii) investigating the mechanical properties of CPEs with the addition of ex-BN or BN-F by utilizing nanoindentation to demonstrate the improvements in strength. Additionally, the electrochemical performance of the LMBs is assessed. This includes constructing full-cell LMBs with CPEs and performing rate capability and cycling stability tests to demonstrate the practical application and benefits of BN-F- based CPEs. Finally, the structures of cycled Li metal anodes and NMC811 (Lithium Nickel>GTMGTKXK 6UHGRY @]OJK$ IGYNUJKX \KWK K]GSOTKJ GLYKW .)iI^IRKX YU HKYYKW ZTJKWXYGTJ YNK I^IROTMstability of BN-F-based CPEs, and the role of fluorine in interfacial stability was investigated. The implementation of these in situ polymerizable CPEs can revolutionize the manufacturing landscape by reducing energy requirements and production time, while enhancing the performance and safety of LMBs. Specifically, various embodiments disclosed herein promote more uniform Li deposition, a critical factor in improving battery performance, with minimal decrease in both volumetric and gravimetric energy densities. 316687865v5Attorney Docket No: 011529.114794

[0011] An exemplary embodiment of the present disclosure provides a composite polymerelectrolyte (CPE) for use in a solid-state battery, comprising: a solid polymer electrolyte matrix; and boron nitride disposed within the solid-polymer electrolyte matrix, wherein the boron nitride is at least one of exfoliated hexagonal boron nitride (ex-BN) or fluorine-functionalized hexagonal boron nitride (BN-F).

[0012] In any of the embodiments disclosed herein, the CPE, can comprise a solid polymerelectrolyte matrix comprising a polymer monomer, a plasticizer, a polymerization initiator, a crosslinker, and a lithium salt.

[0013] In any of the embodiments disclosed herein, the CPE can comprise a solid polymerelectrolyte matrix wherein the monomer comprises ethyl acrylate (EA).

[0014] In any of the embodiments disclosed herein, the CPE can comprise a solid polymerelectrolyte matrix wherein the plasticizer comprises succinonitrile (SN).

[0015] In any of the embodiments disclosed herein, the CPE can comprise a solid polymerelectrolyte matrix wherein the polymerization initiator comprises azobisisobutyronitrile (AIBN).

[0016] In any of the embodiments disclosed herein, the CPE can comprise a solid polymerelectrolyte matrix wherein the crosslinker comprises ethylene glycol dimethacrylate (EGDMA).

[0017] In any of the embodiments disclosed herein, the CPE can comprise a solid polymerelectrolyte matrix wherein the lithium salt comprises Li bis(trifluoromethanesulfonyl)imide (LiTFSI).

[0018] In any of the embodiments disclosed herein, the CPE can comprise no more than 0.5 wt.%of the boron nitride.

[0019] In any of the embodiments disclosed herein, the CPE can comprise no more than 0.3 wt.%of the boron nitride.

[0020] In any of the embodiments disclosed herein, the CPE can comprise no more than 0.1 wt.%of the boron nitride.

[0021] In any of the embodiments disclosed herein, the CPE can be incorporated into a solid-statebattery.

[0022] An exemplary embodiment of the present disclosure provides a method for making anelectrolyte, comprising: providing a solid polymer electrolyte (SPE) precursor solution; incorporating boron nitride into the SPE precursor solution, wherein the boron nitride is at least one of exfoliated hexagonal boron nitride (ex-BN) or fluorine-functionalized hexagonal boron nitride 316687865v5Attorney Docket No: 011529.114794 (BN-F); and polymerizing the SPE precursor solution to form a composite polymer electrolyte (CPE).

[0023] In any of the embodiments disclosed herein, the method for making an electrolyte whereinthe polymerizable SPE precursor solution can comprise a polymer monomer, a plasticizer, a polymerization initiator, a crosslinker, and a lithium salt.

[0024] In any of the embodiments disclosed herein, the method for making an electrolyte whereinthe boron nitride can be ex-BN, wherein incorporating the ex-BN can comprise dispersing bulk hexagonal boron nitride (h-BN) in N-methyl-2-pyrrolidone (NMP) to create a dispersed composition; and energizing the dispersed composition to exfoliate the ex-BN.

[0025] In any of the embodiments disclosed herein, energizing the dispersed composition cancomprise exposing the dispersed composition to ultrasonic energy.

[0026] In any of the embodiments disclosed herein, the method for making an electrolyte whereinthe boron nitride can be BN-F, wherein incorporating the BN-F can comprise dispersing bulk hexagonal boron nitride (h-BN) with a sulfonated tetrafluoroethylene-based fluoropolymer- copolymer and dimethylformamide (DMF) to form a dispersion mixture; and heating the dispersion mixture to generate the BN-F.

[0027] In any of the embodiments disclosed herein, the method for making an electrolyte cancomprise heating the dispersion mixture in an autoclave at 200°C for 12 hours.

[0028] In any of the embodiments disclosed herein, the SPE precursor solution can comprise oneor more polymer monomers, including, but not limited to, ethyl acrylate, ethylene oxide, vinylidene fluoride, hexafluoropropylene, acrylonitrile, methyl methacrylate, methyl siloxane, dimethyl siloxane, vinyl alcohol, vinyl chloride, aliphatic polycarbonates, ethylene carbonate, propylene carbonate, trimethylene carbonate, vinylene carbonate, propylene carbonate, fluoroethylene carbonate, bis((methoxyethoxy)ethoxy)phosphazene, methyl vinyl sulfone, ethyl vinyl sulfone,SKYN^R SKYNGIW^RGYK& [OT^R GIKYGYK& d'IGVWURGIYUTK& RGIYOI GIOJ& GIW^ROI GIOJ& KYN^RKTK MR^IUR&acrylamide, maleimide compounds, maleic anhydride compounds, 1,3-dioxolane, diallyl carbonate, diallyl adipate, diallyl maleate, diallyl phthalate, the like, and any sulfonated derivates thereof.

[0029] In any of the embodiments disclosed herein, the SPE precursor solution can comprise oneor crosslinkers, including, but not limited to, ethylene glycol dimethacrylate, ethylene glycol, ethylene glycol diacrylate, ethylene oxide, glycidyl methacrylate, methyl methacrylate, ethylene 316687865v5Attorney Docket No: 011529.114794 glycol diglycidyl ether, 2,2,3,3,4,4,5,5-octafluoro-1,6-hexanediol diacrylate, trimethylolpropane trimethacrylate, trimethylolpropane triglycidyl ether, acrylic acid, acryloyl chloride, pentaerythritol acrylate, glycerol, boric acid, carboxylic acid, sodium trimetaphosphate, N,N’- methylene bisacrylamide, carbodiimide, diazide compounds, genipin, vinyl carbonate compounds, and the like.

[0030] In any of the embodiments disclosed herein, the SPE precursor solution can comprise oneor more plasticizers, including, but not limited to, succinonitrile (SN), sebaconitrile, 1-ethyl-1- methylpyrrolidinium bis(trifluoromethylsulfonyl)imide, N,N-diethylpyrrolidinium bis(fluorosulfonyl)amide, N-ethyl-N-methylpyrrolidinium bis(fluorosulfonyl)imide, bis(trifluoromethylsulfonyl)imide, bis(fluorosulfonyl)imide, imidazolium, phosphonium, pyrrolidinium, ammonium, BF4, PF6, B(CN)4, FeCl4, B(CH2CH3)3(CH3), perfluorobutane sulfonate, propylene carbonate, ethylene carbonate, dimethyl carbonate, dioctyl sebacate, dibutylXKHGIGYK& JOSKYN^R LUWSGSOJK& JOSKYN^R XZRLU]OJK& f'HZY^WURGIYUTK& JOKYN^R VNYNGRGYK& JOSKYN^Rphthalate, dimethyl isophthalate, dimethylglycol phthalate, tris(2-ethylhexyl)trimellitate, polyethylene glycol, poly(ethylene glycol) dimethyl ether, montmorillonite, glycerol, and the like.

[0031] In any of the embodiments disclosed herein, the SPE precursor solution can comprise oneor more thermal initiators, including, but not limited to, azobisisobutyronitrile (AIBN), 2,2'- azobis[2-(2-imidazolin-2-yl)propane] dihydrochloride, benzoyl peroxide, lauroyl peroxide, tert- butyl hydroperoxide, di-tert-butyl peroxide, dicumyl peroxide, cumene hydroperoxide, sodium persulfate, tetraphenyl-1,2-ethanediol, tris(trimethylsilyl)silane, n-tert-butyl-n-(2-methyl-1- phenylpropyl)-o-(1-phenylethyl)hydroxylamine, n-tert-butyl-o-[1-[4-(chloromethyl) phenyl]ethyl]- n-(2-methyl-1-phenylpropyl)hydroxylamine, benzenesulfonic acid esters, alkyl sulfonium salts, and phenyl-triazine-containing initiators such as 3,3-dimethyl-1-phenyltriazene (BTAM), 3,3- diethyl-1-phenyltriazene (BTAE), 2,2,6,6-tetramethyl-1-(phenyldiazenyl)piperidine (BTACM), 2,2,6,6-tetramethyl-1-(phenyldiazenyl)piperidin-4-ol (BTACH OH), and 2,2,6- tetramethyl-1-(phenyldiazenyl)piperidin-4-ol (BTACM OH), and the like.

[0032] In any of the embodiments disclosed herein, the SPE precursor solution can comprise oneor more chemical initiators, including, but not limited to, Al(OTf)3, Sn(Otf)2, SnF2, AlI3, SnCl4, Sc(SO3CF3)3, BF3, LiPF6, LiDFOB, LiN(SO2F)2, iodonium borates, tris(pentafluorophenyl) borane (TB), lauroyl peroxide, benzoyl peroxide, cumene hydroperoxide, 2,2'-azobis(2- 316687865v5Attorney Docket No: 011529.114794 methylpropionamidine) dihydrochloride (AIBA), potassium persulfate, tert-butyl peroxybenzoate, tert-butyl peroxyacetate, dicumyl peroxide, and the like.

[0033] In any of the embodiments disclosed herein, the SPE precursor solution can comprise oneor more photoinitiators, which may or may not be used with an alcohol or amine-based co-initiator, including, but not limited to, acylphosphine oxides, alpha-aminoalkylphenones, alpha- dialkoxyacetophenones, alpha-hydroxyalkylphenones, benzoin ethers, benzil ketals, hydroxyacetophenones, phosphone oxide, alpha hydroxy ketones, irgacure series, 2-hydroxy-2- methylpropiophenone, phenylpropanedione, lithium phenyl-2,4,6-trimethylbenzoylphosphinate, phenylpropanedione, diphenyl(2,4,6-trimethylbenzoyl)phosphine oxide , 2,2-dimethoxy-2- phenylacetophenone, eosin y, ivocerin, benzophenone, camphorquinone, phenathrenequinone, thioxanthones, riboflavin, iodonium salts, and the like.

[0034] In any of the embodiments disclosed herein, the SPE precursor solution can comprise oneor more Lithium salts, including, but not limited to, LiPF6, LiCTFSI, LiBETI, LiTDI, LiBF4, LiClO4, LiAsF6, LiBOB, LiDFOB, LiFSI, LiBr, LiCl, LiF, LiCF3SO3, LiCF3CO2, LiAlCl4, LiTFSI, ionic liquid-based lithium salts, and the like.

[0035] In any of the embodiments disclosed herein, the SPE precursor solution can comprise apropylene carbonate (PC).

[0036] In any of the embodiments disclosed herein, the SPE precursor solution can comprisesuccinonitrile (SN), azobisisobutyronitrile (AIBN), ethylene glycol dimethacrylate (EGDMA), and Li bis(trifluoromethanesulfonyl)imide (LiTFSI).

[0037] In any of the embodiments disclosed herein, the method for making the electrolyte canfurther comprise polymerizing the SPE precursor solution.

[0038] In any of the embodiments disclosed herein, polymerizing the SPE precursor solution cancomprise thermally treating the SPE precursor solution.

[0039] In any of the embodiments disclosed herein, thermally treating the SPE precursor solutioncan comprise heating the SPE precursor solution at about 65 °C for 12 hours.

[0040] In any of the embodiments disclosed herein, polymerizing the SPE precursor solutioncan comprise photopolymerizing the SPE precursor solution.

[0041] In any of the embodiments disclosed herein, polymerizing the SPE precursor solutioncan comprise chemically initiated polymerization. 316687865v5Attorney Docket No: 011529.114794

[0042] In any of the embodiments disclosed herein, polymerizing the SPE precursor solutioncan comprise pouring the SPE precursor solution into a porous framework prior to polymerizing.

[0043] In any of the embodiments disclosed herein, polymerizing the SPE precursor solutioncan comprise direct deposition onto the electrode surface.

[0044] In any of the embodiments disclosed herein, the method of making the CPE can comprisepolymerizing the SPE precursor solution.

[0045] In any of the embodiments disclosed herein, the method of making the CPE can comprise3D printing a polymer matrix as a framework, infiltrating with precursor solution plus at least one of ex-BN or BN-F, and then polymerizing the SPE precursor solution.

[0046] In any of the embodiments disclosed herein, the method of making the CPE can comprise3D printing a solution containing and at least one of ex-BN or BN-F as a framework, infiltrating with precursor solution, and then polymerizing the SPE precursor solution.

[0047] In any of the embodiments disclosed herein, the method of making the CPE can comprise3D printing a polymer matrix containing at least one of ex-BN or BN-F as a framework, infiltrating with precursor solution, and then polymerizing the SPE precursor solution.

[0048] In any of the embodiments disclosed herein, the SPE can be an in situ polymerizableSPE.

[0049] In any of the embodiments disclosed herein, the CPE can have one or more of theperformance characteristics disclosed herein.

[0050] In any of the embodiments disclosed herein, the method for making the electrolyte canfurther comprise incorporating the CPE into a solid-state battery.

[0051] In any of the embodiments disclosed herein, the method for making the electrolyte canfurther comprise incorporating the CPE into a lithium battery.

[0052] Another embodiment of the present disclosure provides a CPE comprising an in situpolymerizable SPE incorporated with an exfoliated hexagonal boron nitride.

[0053] Another embodiment of the present disclosure provides a CPE comprising an in situpolymerizable SPE incorporated with a fluorine-functionalized hexagonal boron nitride.

[0054] These and other aspects of the present disclosure are described in the Detailed Descriptionbelow and the accompanying drawings. Other aspects and features of embodiments will become apparent to those of ordinary skill in the art upon reviewing the following description of specific, exemplary embodiments in concert with the drawings. While features of the present disclosure may 316687865v5Attorney Docket No: 011529.114794 be discussed relative to certain embodiments and figures (FIGs.), all embodiments of the present disclosure can include one or more of the features discussed herein. Further, while one or more embodiments may be discussed as having certain advantageous features, one or more of such features may also be used with the various embodiments discussed herein. In similar fashion, while exemplary embodiments may be discussed below as device, system, or method embodiments, it is to be understood that such exemplary embodiments can be implemented in various devices, systems, and methods of the present disclosure. BRIEF DESCRIPTION OF THE DRAWINGS

[0055] The patent or application file contains at least one drawing executed in color. Copies ofthis patent or patent application publication with color drawing(s) will be provided by the Office upon request and payment of the necessary fee.

[0056] FIG. 1 depicts Transmission Electron Microscopy (TEM) images of hexagonal boronnitride (h-BN). The left image shows bulk h-BN, characterized by stacked layers. The right imagedisplays exfoliated h-BN, where the layers have been successfully separated into few-layer sheets. This exfoliation process increases the specific surface area, enabling h-BN to interact more effectively with the electrolyte matrix.

[0057] FIG. 2 shows morphological variation in PC-based SPE with and without fillers. (Leftto right) Images of SPE with no additive filler, with raw BN 0.3 wt.% and exfoliated BN 0.3 wt.%.

[0058] FIG. 3 depicts the Fourier Transform Infrared Spectroscopy (FTIR) spectra showing thebroad B-N-B bending vibrations in h-BN (bottom) and F-BN (top). In F-BN, the F-B peaks can beclearly seen interspersed with the broad B-N peak.

[0059] FIGs. 4A-4D depicts the electrochemical and mechanical characterizations of PC-basedSPE with ex-BN filler (0 wt.%, 0.1 wt.%, 0.3 wt.%, and 0.5 wt.%). (FIG. 4A) Lithium-iontransference number (tLi+), determined using the Bruce-Vincent method; (FIG. 4B) Lithium ionicIUTJZIYO[OY^ #e=O+); (FIG.4C) Linear Sweep Voltammetry (LSV) curves demonstrating theelectrochemical stability of the electrolytes; and (FIG.4D) nanoindentation analysis of PC-based SPEs with varied exBN.

[0060] FIGs. 5A-5D depicts the electrochemical and mechanical characterizations of PC-basedSPE with BN-F filler. (FIG.5A) Lithium-ion transference number (tLi+), (FIG.5B) Lithium ionicIUTJZIYO[OY^ #e=O+), (FIG. 5C) Linear Sweep Voltammetry (LSV), and (FIG. 5D) Young’smodulus of SPE and CPE with BN-F filters. 316687865v5Attorney Docket No: 011529.114794

[0061] FIGs. 6A-6B shows the electrochemical performance of CPEs with ex-BN filler in LMBfull-cell systems. (FIG. 6A) Rate performance of full-cell batteries at room temperature. (FIG. 6B)Rate performance and cycling stability of full-cell batteries at 30°C paired with NMC811 cathodes.

[0062] FIGs. 7A-7D shows the electrochemical performance of CPEs with BN-F filler in LMBfull-cell systems compared to CPE without addition of boron nitride. (FIG.7A) Rate performance of full-cell batteries at room temperature. (FIG. 7B) Rate performance and cycling stability of full-cell batteries at 30°C paired with NMC811 cathodes. (FIG.7C) Cycling stability test using a high-capacity NMC 811 cathode, a low N / P ratio (< 2), achieving energy density of 454.90Wh / kg. (FIG. 7D) Charge-discharge voltage profiles from the cycling stability test.

[0063] FIG. 8 shows Scanning Electron Microscopy (SEM) micrographs of Li metal anodeXZWLGIKX GLYKW .) I^IRKX OT =Oh?>61** LZRR IKRR LUW BA8 #RKLY$& 6A8'5? #SOJJRK$& GTJ 6A8'95?(right).

[0064] FIG. 9 depicts X-ray Photoelectron Spectroscopy (XPS) in-depth profiling analysis ofYNK B8< RG^KW LUWSKJ UT =O GTUJKX GLYKW .) I^IRKX UL =Oh?>61** LZRR IKRR( CNK XVKIYWG LUW =O *X(left) and F 1s (right) reveal differences in SEI composition.

[0065] FIG. 10 shows High-Resolution Transmission Electron Microscopy (HRTEM)SOIWUMWGVNX UL YNK 68< UT ?>61** VGWYOIRKX GLYKW .) I^IRKX UL =Oh?>61** LZRR IKRR LUW YNKcathode-electrolyte interphase (CEI) for SPE (left), CPE-BN (middle), and CPE-FBN (right). The dotted lines mark the boundaries of the CEI, where the width of the interphase is given.

[0066] FIGs. 11A-11D demonstrates full cell performance under high voltage and high-loadingconditions. (FIGs. 11A-11B) Active material’s loading is 1 ~ 2 mg / cm2. (FIG. 11A) cyclabilityVKWLUWSGTIK UL =Oh?>61** GY )(.6 OT YNK [URYGMK WGTMK UL ,() ' -(.D( #FIG. 11B) Corresponding:67 [URYGMK VWULORKX UL =Oh6A8'5?h?>61** IKRR( #FIG. 11C) Schematic illustration of full cellconfiguration designed to achieve high energy density ASSLMBs. Active material’s loading is 20mg / cm2. (FIG. 11D$ 6^IROTM VKWLUWSGTIK UL =Oh6A8'95?h?>61** GY )(+ S4cIS-2,demonstrating high energy density. DETAILED DESCRIPTION

[0067] Although preferred exemplary embodiments of the disclosure are explained in detail, itis to be understood that other exemplary embodiments are contemplated. Accordingly, it is not intended that the disclosure is limited in its scope to the details of construction and arrangement 316687865v5Attorney Docket No: 011529.114794 of components set forth in the following description or illustrated in the drawings. The disclosure is capable of other exemplary embodiments and of being practiced or carried out in various ways. Also, in describing the preferred exemplary embodiments, specific terminology will be resorted to for the sake of clarity.

[0068] To facilitate an understanding of the principles and features of the present disclosure,various illustrative embodiments are explained below. The components, steps, and materials described hereinafter as making up various elements of the embodiments disclosed herein are intended to be illustrative and not restrictive. Many suitable components, steps, and materials that would perform the same or similar functions as the components, steps, and materials described herein are intended to be embraced within the scope of the disclosure. Such other components, steps, and materials not described herein can include, but are not limited to, similar components or steps that are developed after development of the embodiments disclosed herein.

[0069] As used in the specification and the appended claims, the singular forms “a,” “an” and“the” include plural referents unless the context clearly dictates otherwise.

[0070] Also, in describing the preferred exemplary embodiments, terminology will be resortedto for the sake of clarity. It is intended that each term contemplates its broadest meaning as understood by those skilled in the art and includes all technical equivalents which operate in a similar manner to accomplish a similar purpose.

[0071] Ranges can be expressed herein as from “about” or “approximately” one particular valueand / or to “about” or “approximately” another particular value. When such a range is expressed, another exemplary embodiment includes from the one particular value and / or to the other particular value.

[0072] Similarly, as used herein, “substantially free” of something, or “substantially pure”, andlike characterizations, can include both being “at least substantially free” of something, or “at least substantially pure”, and being “completely free” of something, or “completely pure”.

[0073] By “comprising” or “containing” or “including” is meant that at least the namedcompound, member, particle, or method step is present in the composition or article or method, but does not exclude the presence of other compounds, materials, particles, method steps, even if the other such compounds, material, particles, method steps have the same function as what is named. 316687865v5Attorney Docket No: 011529.114794

[0074] Mention of one or more method steps does not preclude the presence of additionalmethod steps or intervening method steps between those steps expressly identified. Similarly, it is also to be understood that the mention of one or more components in a device or system does not preclude the presence of additional components or intervening components between those components expressly identified.

[0075] The materials described as making up the various members of the invention are intendedto be illustrative and not restrictive. Many suitable materials that would perform the same or a similar function as the materials described herein are intended to be embraced within the scope of the invention. Such other materials not described herein can include, but are not limited to, for example, materials that are developed after the time of the development of the invention.

[0076] Reference will now be made in detail to exemplary embodiments of the disclosedtechnology, examples of which are illustrated in the accompanying drawings and disclosed herein. Wherever convenient, the same references numbers will be used throughout the drawings to refer to the same or like parts.

[0077] To address the disadvantages of conventional electrolytes discussed above, disclosedherein are in situ polymerizable PC-based SPEs, which combine the flexibility of SPEs with the highe=O% UL A6& \NORK GINOK[OTM G IUTLUWSGR OTYKWLGIK \OYN KRKIYWUJKX( 6A8X \OYN OTUWMGTOI LORRKWX ULLKWa promising solution by merging the benefits of both inorganic fillers and SPEs. Incorporating functional inorganic fillers into SPEs allows CPEs to achieve superior electrochemical properties and enhanced mechanical strength.

[0078] Hexagonal boron nitride (h-BN), especially when exfoliated into nanosheets (ex-BN) orfunctionalized with fluorine (BN-F), provides a high surface area that significantly enhances the properties of in situ polymerizable CPEs. Incorporating ex-BN or BN-F into in situ polymerizable CPEs offers multiple benefits: improved Li-ion transport properties due to better interaction with Li ions, enhanced mechanical strength to prevent dendritic growth, excellent insulating properties to prevent electron crossover, and improved electrochemical stability for high-voltage applications. Additionally, fluorine functionalization of the filler further enhances the interfacial stability between electrolytes and electrodes, preventing decomposition and allowing more effective Li-ion transport. Using high surface area materials like ex-BN and BN-F allows for the development of lighter and thinner electrolytes that effectively suppress Li dendrite growth, thereby achieving higher gravimetric and volumetric energy densities. 316687865v5Attorney Docket No: 011529.114794

[0079] Moreover, high-density fillers in the liquid precursor of in situ polymerizable SPEs cansettle due to gravity, leading to non-uniform distribution. In contrast, 2D materials like ex-BN and BN-F remain well-dispersed, ensuring efficient and uniform application in LMBs.

[0080] The development and implementation of high-performance CPEs incorporating ex-BNand BN-F will significantly advance the field of energy storage. This technology will enable the production of safer, more efficient, and higher-performing ASSLMBs, which are crucial for the widespread adoption of EVs, renewable energy systems, and advanced electronic devices. TheGHOROY^ YU KTNGTIK e=O+, mechanical strength, and thermal stability in these batteries addresses thecritical challenges faced by current energy storage technologies.

[0081] By utilizing a small amount of high-surface-area materials like ex-BN and BN-F, thisdisclosure ensures that CPEs remain lightweight and efficient, achieving higher gravimetric and volumetric energy densities. This not only improves the performance and safety of LMBs but also reduces the complexity of battery manufacturing processes. Additionally, the scalable and efficient synthesis process developed for these CPEs will streamline production, lower energy consumption, and minimize production time, further promoting the commercial viability of advanced LMBs.

[0082] The principles and methods described herein, although demonstrated with specific SPEs,can be easily adapted to various other types of SPEs, thereby broadening the applicability of this technology across different solid-state battery systems. In addition to thermal polymerization, the in- situ polymerization of these CPEs can be achieved through photoinitiation, which offers several advantages, including faster polymerization rates, reduced thermal stress on materials, and more precise control over the polymerization process. Highlighting this capability enhances the versatility and appeal of the technology, showcasing its adaptability to different manufacturing conditions and requirements. The successful integration of these CPEs into full-cell configurations underscores their practical applicability and potential for large-scale implementation. By enhancing the performance and safety of LMBs, this technology can contribute to the development of more sustainable and efficient energy storage solutions, supporting the transition to a low-carbon economy and reducing dependence on fossil fuels. The widespread adoption of advanced LMBs enabled by embodiments of the present disclosure can play a pivotal role in meeting the growing demand for high-energy- density applications, driving innovation in the energy sector, and promoting a cleaner, more sustainable future. 316687865v5Attorney Docket No: 011529.114794

[0083] The present disclosure introduces a scalable and efficient process for synthesizing ex-BNand BN-F-based CPEs. By optimizing and functionalizing h-BN and incorporating it into the in situ polymerizable polymer matrix, high-performance CPEs are created that enhance the performance and safety of LMBs. This technology can revolutionize manufacturing, reduce energy requirements and production time, and promote more uniform Li deposition. Ultimately, this development advances LMB technology, making it more viable and sustainable for widespread applications, particularly in EVs and beyond. EXAMPLES

[0084] The following examples are provided for illustrative purposes only and should not beconstrued as limiting the scope of the present disclosure. The various methods and systems disclosed herein can include one or more of the steps and components, respectively disclosed in the below examples.

[0085] The disclosure below provides a comprehensive technical approach to enhance theperformance and safety of in situ polymerizable CPEs by incorporating ex-BN and BN-F. The technical approach is structured around four main objectives: synthesis of ex-BN and BN-F-based CPEs, electrochemical and mechanical properties enhancement, and full cell performance evaluation. Example 1. Synthesis of ex-BN and BN-F-incorporated In Situ Polymerizable CPEs

[0086] To exfoliate the ex-BN, bulk h-BN was dispersed in N-methyl-2-pyrrolidone (NMP) andsubjected to ultrasonic energy. This method effectively breaks down the stacked layers of bulk h- BN into few-layer sheets, as confirmed by transmission electron microscopy (TEM) images (FIG. 1). The resulting ex-BN was then incorporated into in situ polymerizable PC-based SPEs, designed to enhance the electrochemical and mechanical properties for high-energy LMBs.

[0087] For the synthesis, a series of PC-based SPEs were prepared by incorporating differentweight percentages of ex-BN (0 wt.%, 0.1 wt.%, 0.3 wt.%, and 0.5 wt.%). It was observed that adding more than 0.5 wt.% of ex-BN led to sedimentation in the precursor solution, thus it was not included in the optimization process. The in-situ polymerizable PC-based SPE precursor solution contained ethyl acrylate (EA), succinonitrile (SN), azobisisobutyronitrile (AIBN) as a thermal initiator, ethylene glycol dimethacrylate (EGDMA) for cross-linking, and Li bis(trifluoromethanesulfonyl)imide (LiTFSI) as the Li salt. This mixture was infused into porous frameworks with a thickness of 25 µm and thermally treated at 65°C for 12 hours to initiate 316687865v5Attorney Docket No: 011529.114794 polymerization, forming PC-based SPEs with ex-BN fillers. Scanning electron microscopy (SEM) images revealed uniform dispersion of ex-BN in the SPEs, whereas bulk h-BN tended to form agglomerates (FIG. 2).

[0088] To functionalize BN with fluorine, bulk h-BN was dispersed in a mixture of sulfonatedtetrafluoroethylene-based fluoropolymer-copolymer and dimethylformamide (DMF). This mixture was then heated in an autoclave at 200°C for 12 hours to generate fluorine radicals. The resulting BN-F and polymer fragments were washed with acetone to isolate BN-F. Successful functionalization was confirmed by Fourier Transform Infrared Spectroscopy (FTIR) analysis, which displayed multiple bands corresponding to the broad B-N transverse optical (TO) mode around 1380 Additional bands associated with fluorine-bonded boron and nitrogen included primary vibrational modes of covalent B-F bonds at 1053 and 1235 cmb*, and N-F bond vibrations at 633 cmb*, overlapping with B-N-B out-of-plane bending vibrations (FIG.3). The development of SPEs incorporating BN-F aims to further enhance both electrochemical and mechanical properties. A 0.3 wt.% BN-F was incorporated into an in-situ polymerizable SPE precursor solution containing EA, SN, AIBN, EGDMA, and LiTFSI. This mixture was filled into porous frameworks with a thickness of 25 µm and thermally treated at 65°C for 12 hours to initiate polymerization, resulting in PC-based SPEs with BN-F fillers. Example 2. Characterization of the Electrochemical and Mechanical Properties of the ex-BNor BN-F-incorporated CPEs

[0089] The electrochemical properties of the in situ polymerizable CPEs with ex-BN filler wereassessed, focusing on essential metrics such as tLi+& e=O+, and electrochemical stability (FIGs. 4A-4D). The tLi+, determined using the Bruce-Vincent method, across different compositions showed that in situ polymerizable CPEs with ex-BN at 0%, 0.1%, 0.3%, and 0.5% exhibited tLi+values of 0.569, 0.571, 0.610, and 0.637, respectively (FIG. 4A). As the content of ex-BN, which captures anions to increase Li-ion selectivity, increased, the tLi+also increased. However, as the ex-BN content increased,YNK e=O+ exhibited the values of 0.877 mS·cm-1, 1.296 mS·cm-1, 0.429 mS·cm-1, and 0.500 mS·cm-1,respectively, with the highest value observed at exBN_0.3% (FIG. 4B). This is because ex-BN itself is a non-conductive material, and excessive amounts of ex-BN in the electrolyte hinder Li-ion conduction. LSV tests for electrochemical stability identified that as the content of ex-BN increased, the stability improved (FIG.4C). In this study, exBN_0.3% and exBN 0.5% showed nearly identical stability values. The mechanical properties of the PC-based SPE with and without ex-BN fillers were 316687865v5Attorney Docket No: 011529.114794 investigated using a nanoindenter. This study confirmed that 2D nanosheet forms of ex-BN can effectively enhance the mechanical properties of the electrolyte. An increase in the ex-BN content correlated with an increase in the modulus of the electrolyte, indicating that even a small amount of ex-BN can effectively improve the modulus (FIG.4D).

[0090] The tLi+ was assessed via the Bruce-Vincent method, revealing a notable increase for theBN-F 0.3 wt.% sample. While the bare SPE showed a lower tLi+of 0.569, the BN-F 0.3 wt.% sample exhibited a significantly higher tLi+of 0.715, indicating efficient Li-ion transport andreduced anion mobility (FIG.5A$( e=O+ of the CPEs, measured through electrochemical impedanceXVKIYWUXIUV^ #8<B$& XNU\KJ YNGY YNK 5?'9F)(," XGSVRK NGJ G SGWQKJR^ NOMNKW e=O+ (1.700 mS / cm)compared to the SPE and CPE-exBN 0.3% (FIG. 5B). This enhancement is due to the increased dissociation of Li salts and the efficient ion transport pathways provided by the F functional groups. Electrochemical stability evaluated using LSV demonstrated that the BN-F_0.3% had superior electrochemical stability compared to the bare CPE, which had lower stability (FIG. 5C). This improved stability indicates that the BN-F_0.3% is more suitable for high-voltage applications. The mechanical properties of the PC-based SPE with BN-F were also explored using a nanoindenter. The findings demonstrated that the inclusion of 2D nanosheet forms of BN-F enhances the mechanical properties of the electrolyte due to the strong interactions between BN-F and the polymer matrix (FIG.5D). Example 3. Assessment of the Electrochemical Performance of the LMBs

[0091] The practical application of ex-BN-based CPEs in LMBs was evaluated by constructingfull-cell batteries with LiNi0.8Co0.1Mn0.1O2(NMC811) cathodes using the synthesized CPEs as electrolytes (FIGs. 6A-6D). The cells were tested under various conditions: at room temperature (RT) and at 30°C. At RT, initial rate tests revealed that cells incorporating exBN_0.3%-based CPEs exhibited significantly enhanced capacities of 189.7 mAh·gb*at 0.2C, while the SPE showed only 165.6 mAh·gb*(FIG. 6A). Moreover, as the current density increased, the performance improvement of exBN 0.3%-based CPEs became more pronounced. The bare CPE exhibited lower capacities and poor performance at high current densities, whereas the exBN_0.3% sample demonstrated exceptional performance with high capacities and excellent performance at high current densities. Rate capability and cyclability were also tested at 30°C, showing a slight increaseOT IGVGIOY^ \OYN K]5? JZK YU YNK OTIWKGXKJ e=O+ of the SPE itself at 30°C, which diminishes therelative impact of the exBN (FIG.6B). 316687865v5Attorney Docket No: 011529.114794

[0092] The practical application of BN-F-based CPEs in LMBs was evaluated by constructingfull-cell batteries with NMC811 cathodes using the synthesized CPEs as electrolytes (FIGs. 7A- 7D). At RT, initial rate tests revealed that cells incorporating exBN 0.3%-based and BN-F 0.3%- based CPEs exhibited similarly high capacities of 190 mAh·gb*at 0.2C, while the SPE with no boron nitride added showed only 166 mAh·gb*(FIG. 7A). However, as the current density increased, the performance improvement of CPE-BN-F 0.3% was significantly more pronounced. This sample showed superior rate capability and cycling stability, which can be attributed to the efficient ion transport and enhanced mechanical properties provided by the BN-F. At 30°C, the performance improvement attributed to the ex-BN filler was less significant compared to RT (FIG.7B$( 6UT[KWXKR^& YNK 5?'9'HGXKJ 6A8& QTU\T LUW OYX XZVKWOUW e=O+, exhibited exceptionally highcapacities, achieving nearly the theoretical capacity with 221 mAh·gb*at 0.2C. Moreover, the CPE-BN-F 0.3% demonstrated a smaller reduction in capacity at higher rates compared to the other two groups, further highlighting its efficacy.

[0093] To highlight the suitability of CPE-BN-F 0.3% for high-energy and power ASSLMBs,full cells were tested under demanding conditions, including a low N / P ratio (<2), a high-capacity NMC 811 cathode (~4 mAh·cmb+), a 25 .im-thick CPE, and a thin Li foil (35 .im; 7 mAh·cmb+) (FIGs. 7C-7D). The cell demonstrated impressive capacities of 214 mAh·gb*(4.2 mAh·cmb+) at0.05 mA·cmb+ GTJ +). S4NcMb* (4.1 mAh·cmb+) at 0.2 mA·cmb+, with a maintained capacity of193 mAh·gb*and 94% capacity retention after 20 cycles at 0.2 mA·cmb+. Additionally, it exhibited a high gravimetric energy density of 454.90 \Vh·kg(anode + cathode + electrolyte)-1and high volumetric energy density of 1032.4 \Vh·L(anode + cathode + electrolyte)-1. The practical application of BN-F-incorporated CPEs in LMBs demonstrated significant performance improvements, attributed to the unique properties of fluorinations. The presence of fluorine facilitates enhanced interaction between h-BN and the polymer matrix, resulting in better filler dispersion and mechanical integrity. Additionally, fluorine improves the electrolyte's performance by enhancing oxidation stability, forming a stable solid electrolyte interface (SEI), reducing sideWKGIYOUTX& SGOTYGOTOTM MUUJ e=O+, suppressing dendrite growth, and ensuring compatibility withhigh-voltage cathodes. These factors collectively contribute to the improved cycle life, safety, and efficiency of LMBs. Comprehensive testing at RT and 30°C revealed that BN-F-based CPEs exhibited high capacities and superior rate capability, with minimal capacity reduction at higher rates. Full cells tested under demanding conditions also showed impressive capacities and energy 316687865v5Attorney Docket No: 011529.114794 densities, affirming the potential of BN-F- incorporated CPEs for high-energy and power ASSLMBs. These findings underscore the critical roles played by fluorine in achieving superior electrochemical and mechanical properties, positioning BN-F-incorporated CPEs as promising candidates for advanced ASSLMBs.

[0094] The implementation of these technical approaches can produce high-performance CPEsthat enhance the efficiency, safety, and commercial viability of LMBs. By optimizing the synthesis, mechanical, and electrochemical properties, and thoroughly testing full-cell performance, this technology aims to revolutionize the manufacturing and application of LMBs, making them suitable for widespread use in EVs and other high-energy-density applications. Example 4. Evaluation of the Stability of the Solid Electrolyte Interface for High-energy Applications

[0095] To further understand the superior cycling stability of the cell with CPE-FBN, theXYWZIYZWKX UL I^IRKJ =O SKYGR GTUJKX GTJ ?6>1** IGYNUJKX \KWK K]GSOTKJ GLYKW .)iI^IRKX( B8>images revealed a highly porous structure with Li whiskers in the Li|SPE|NCM811 anode, while the Li|CPE-FBN|NCM811 anode displayed a dense, chunk-like Li deposition with no signs of dendritic growth (*,+#.&). This favorable morphology contributed to improved cycling performance and reduced impedance growth. X-ray photoelectron spectroscopy (XPS) analysis indicated that the SEI formed by CPE-FBN contained higher concentrations of inorganic compounds such as LiF and Li-O, effectively suppressing dendrite formation (*,+#.'). The fluorine to oxygen (F / O) ratio for CPE-FBN was 2.65, compared to 0.73 for CPE-BN and 0.69 for the SPE, further confirming the superior SEI characteristics and stable Li deposition in the CPE- FBN system. Furthermore, TEM images of the cycled NCM811 cathodes revealed that the incorporation of CPE-FBN resulted in a significantly thinner cathode-electrolyte interphase (CEI) layer compared to that observed with conventional SPE (*,+#.%$). This finding indicates improved interfacial stability and a substantial reduction in side reactions at the CEI, highlighting the effectiveness of CPE-FBN in maintaining a stable and durable interface. Example 5. Examination of the Role of Fluorine in Interfacial Stability under High-Voltage Conditions.

[0096] To further elucidate the role of fluorine, Li|SPE|NCM811, Li|CPE-BN|NCM811, and=O_6A8'95?_?6>1** IKRRX \KWK I^IRKJ GY G NOMN'[URYGMK \OTJU\ UL ,() ' -(.iD GY )(.6 #FIGs.11A-11B). CNK =O_6A8'95?_?6>1** IKRR K]NOHOYKJ G NOMN OTOYOGR IGVGIOY^ UL +*)()iS4NcM-1 and316687865v5Attorney Docket No: 011529.114794WKYGOTKJ 1)" UL OYX IGVGIOY^ GLYKW *+)iI^IRKX( <T IUTYWGXY& YNK =O_BA8_?6>1** IKRR XNU\KJ WGVOJIGVGIOY^ LGJOTM& WKYGOTOTM UTR^ 1)" UL OYX OTOYOGR IGVGIOY^ GLYKW / )iI^IRKX& \NORK YNK =O_6A8'5?_?6>1** IKRR WKGINKJ 1) " WKYKTYOUT GLYKW PZXY 0)iI^IRKX( CNKXK LOTJOTMX ZTJKWXIUWK YNK IWZIOGRrole of fluorine in enhancing interfacial and structural stability under high-voltage conditions. To further assess its practical viability, Li|CPE-FBN|NCM811 cells were evaluated using a highRUGJOTM ?6>1** IGYNUJK #`-iS4NcIS-2$ GTJ G YNOT =>4 #,.iaS$ #*,+-#.%%(")). Even underYNKXK XYWOTMKTY IUTJOYOUTX& YNK IKRR JKRO[KWKJ GT OTOYOGR IGVGIOY^ UL +).()iS4NcM-1 and maintained2,( / " UL OYX IGVGIOY^ GLYKW +)iI^IRKX( 4JJOYOUTGRR^& OY GINOK[KJ WKSGWQGHRK KTKWM^ JKTXOYOKX UL-.-(2iENcQM-1anode+cathode+electrolyte GTJ *),+iENc=-1 anode+cathode+electrolyte (Table 1), highlighting the strong potential of the CPE-FBN system for high-energy-density Li metal batteries. Table 1. Calculation basis for energy density of a protype cell with CPE-FBN.

[0097] It is to be understood that the embodiments and claims disclosed herein are not limitedin their application to the details of construction and arrangement of the components set forth in the description and illustrated in the drawings. Rather, the description and the drawings provide examples of the embodiments envisioned. The embodiments and claims disclosed herein are further capable of other embodiments and of being practiced and carried out in various ways. Also, it is to be understood that the phraseology and terminology employed herein are for the purposes of description and should not be regarded as limiting the claims.

[0098] Accordingly, those skilled in the art will appreciate that the conception upon which theapplication and claims are based may be readily utilized as a basis for the design of other structures, 316687865v5Attorney Docket No: 011529.114794 methods, and systems for carrying out the several purposes of the embodiments and claims presented in this application. It is important, therefore, that the claims be regarded as including such equivalent constructions.

[0099] Furthermore, the purpose of the foregoing Abstract is to enable the United States Patentand Trademark Office and the public generally, and especially including the practitioners in the art who are not familiar with patent and legal terms or phraseology, to determine quickly from a cursory inspection the nature and essence of the technical disclosure of the application. The Abstract is neither intended to define the claims of the application, nor is it intended to be limiting to the scope of the claims in any way. 316687865v5

Claims

Attorney Docket No: 011529.114794 CLAIMS 1. A composite polymer electrolyte (CPE) for use in a solid-state battery, comprising:a solid polymer electrolyte matrix; and boron nitride disposed within the solid-polymer electrolyte matrix, wherein the boron nitride is at least one of exfoliated hexagonal boron nitride (ex-BN) or fluorine-functionalized hexagonal boron nitride (BN-F).

2. The CPE of claim 1, wherein the solid polymer electrolyte matrix comprises a polymermonomer, a plasticizer, a polymerization initiator, a crosslinker, and a lithium salt.

3. The CPE of claim 2, wherein the monomer comprises ethyl acrylate (EA).

4. The CPE of claim 2, wherein the plasticizer comprises succinonitrile (SN).

5. The CPE of claim 2, wherein the polymerization initiator comprises azobisisobutyronitrile(AIBN).

6. The CPE of claim 2, wherein the crosslinker comprises ethylene glycol dimethacrylate(EGDMA).

7. The CPE of claim 2, wherein the lithium salt comprises Libis(trifluoromethanesulfonyl)imide (LiTFSI).

8. The CPE of claim 1, wherein the CPE comprises no more than 0.5 wt.% of the boronnitride.

9. The CPE of claim 1, wherein the CPE comprises no more than 0.3 wt.% of the boronnitride.

10. The CPE of claim 1, wherein the CPE comprises no more than 0.1 wt.% of the boronnitride.

11. The CPE of claim 1, wherein the CPE is incorporated into a solid-state battery.

12. A method for making an electrolyte, comprising:providing a solid polymer electrolyte (SPE) precursor solution; incorporating boron nitride into the SPE precursor solution, wherein the boron nitride is at least one of exfoliated hexagonal boron nitride (ex-BN) or fluorine-functionalized hexagonal boron nitride (BN-F); and polymerizing the SPE precursor solution to form a composite polymer electrolyte (CPE).

13. The method of claim 12, wherein the polymerizable precursor solution comprises a polymermonomer, a plasticizer, a polymerization initiator, a crosslinker, and a lithium salt. 316687865v5Attorney Docket No: 011529.114794 14. The method of claim 12, wherein the boron nitride is ex-BN, wherein incorporating the ex-BN comprises: dispersing bulk hexagonal boron nitride (h-BN) in N-methyl-2-pyrrolidone (NMP) to create a dispersed composition; and energizing the dispersed composition to exfoliate the ex-BN.

15. The method of claim 14, wherein energizing the dispersed composition comprises exposingthe dispersed composition to ultrasonic energy.

16. The method of claim 12, wherein the boron nitride is BN-F, wherein incorporating the BN-F comprises: dispersing bulk hexagonal boron nitride (h-BN) with a sulfonated tetrafluoroethylene-based fluoropolymer-copolymer and dimethylformamide (DMF) to form a dispersion mixture; and heating the dispersion mixture to generate the BN-F.

17. The method of claim 12, wherein the SPE precursor solution comprises a propylenecarbonate (PC).

18. The method of claim 17, wherein the SPE precursor solution further comprisessuccinonitrile (SN), azobisisobutyronitrile (AIBN), ethylene glycol dimethacrylate (EGDMA), and Li bis(trifluoromethanesulfonyl)imide (LiTFSI).

19. The method of claim 12, wherein polymerizing the SPE precursor solution comprisesthermally treating the SPE precursor solution.

20. The method of claim 19, wherein the SPE precursor solution is thermally treated at about65 °C for 12 hours.

21. The method of claim 12, further comprising, prior to polymerizing the SPE precursorsolution, pouring the SPE precursor solution into a porous framework.

22. The method of claim 12, wherein the CPE comprises no more than 0.5 wt.% of the boronnitride.

23. The method of claim 12, wherein the CPE comprises no more than 0.3 wt.% of the boronnitride.

24. The method of claim 12, wherein the CPE comprises no more than 0.1 wt.% of the boronnitride.

25. The method of claim 12, further comprising incorporating the CPE into a solid-statebattery. 316687865v5

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