Diverse polymer structure design: a key enabler for advanced lithium-based batteries

Sijeong Park , Hyeju Shin , Sinho Choi , Gyujin Song

Microstructures ›› 2026, Vol. 6 ›› Issue (1) -2026014.

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Microstructures ›› 2026, Vol. 6 ›› Issue (1) -2026014. DOI: 10.20517/microstructures.2025.64
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Diverse polymer structure design: a key enabler for advanced lithium-based batteries
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Abstract

The growing demand for batteries with higher energy density and improved safety necessitates the development of advanced electrode materials beyond conventional systems. Although high-energy electrodes offer superior theoretical capacities, they encounter major challenges, including structural instability caused by volume changes and uncontrollable dissolution. These issues contribute to performance degradation and safety risks at both the electrode and cell levels. Addressing these persistent problems is therefore essential to achieving safe, high-energy-density batteries. Polymers, with their versatile functionalities, present significant opportunities in this regard. The strategic design and deployment of tailored polymer architectures can enhance structural stability and improve cell configurations. In this work, we highlight the role of polymer chemistry in governing electrochemical behavior and demonstrate how it can drive substantial improvements in both performance metrics and the critical safety features required for reliable battery operation.

Keywords

Polymer structure / interface engineering / battery safety / electrochemical stability / high-energy-density / lithium-based batteries

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Sijeong Park, Hyeju Shin, Sinho Choi, Gyujin Song. Diverse polymer structure design: a key enabler for advanced lithium-based batteries. Microstructures, 2026, 6(1): -2026014 DOI:10.20517/microstructures.2025.64

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References

[1]

Machala ML,Bunke SP.Life cycle comparison of industrial-scale lithium-ion battery recycling and mining supply chains.Nat Commun2025;16:988 PMCID:PMC11761346

[2]

Song IT,Koh J.Thermal runaway prevention through scalable fabrication of safety reinforced layer in practical Li-ion batteries.Nat Commun2024;15:8294 PMCID:PMC11437208

[3]

Duan J,Dai H.Building safe lithium-ion batteries for electric vehicles: a review.Electrochem Energ Rev2020;3:1-42

[4]

Schmuch R,Hörpel G,Winter M.Performance and cost of materials for lithium-based rechargeable automotive batteries.Nat Energy2018;3:267-78

[5]

Eshetu GG,Judez X.Production of high-energy Li-ion batteries comprising silicon-containing anodes and insertion-type cathodes.Nat Commun2021;12:5459 PMCID:PMC8443554

[6]

Kim S,Miara L.High-energy and durable lithium metal batteries using garnet-type solid electrolytes with tailored lithium-metal compatibility.Nat Commun2022;13:1883 PMCID:PMC8986853

[7]

Xu J,Cai S.High-energy lithium-ion batteries: recent progress and a promising future in applications.Energy Environ Mater2023;6:e12450

[8]

Liu W,Chau K.Overview of batteries and battery management for electric vehicles.Energy Rep2022;8:4058-84

[9]

Zeng Y,Fu Y.Extreme fast charging of commercial Li-ion batteries via combined thermal switching and self-heating approaches.Nat Commun2023;14:3229 PMCID:PMC10239438

[10]

Frith JT,Ulissi U.A non-academic perspective on the future of lithium-based batteries.Nat Commun2023;14:420 PMCID:PMC9879955

[11]

Zhao S,Yan K.Towards high-energy-density lithium-ion batteries: Strategies for developing high-capacity lithium-rich cathode materials.Energy Storage Mater2021;34:716-34

[12]

Zhang S,Hu N.Tackling realistic Li+ flux for high-energy lithium metal batteries.Nat Commun2022;13:5431 PMCID:PMC9481556

[13]

Ou X,Zhong W.Enabling high energy lithium metal batteries via single-crystal Ni-rich cathode material co-doping strategy.Nat Commun2022;13:2319 PMCID:PMC9050889

[14]

Lee BJ,Yu JH.Development of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy.Nat Commun2022;13:4629 PMCID:PMC9360432

[15]

Huo H,Bai Y.Chemo-mechanical failure mechanisms of the silicon anode in solid-state batteries.Nat Mater2024;23:543-51 PMCID:PMC10990934

[16]

Liang B,Xu Y.Silicon-based materials as high capacity anodes for next generation lithium ion batteries.J Power Sources2014;267:469-90

[17]

Li Z,Zhang Z.A 3D conducting scaffold with lithiophilic carbon nanoparticles for stable lithium metal battery anodes.J Power Sources2024;618:235183

[18]

Long K,Wang H.High interfacial capacitance enabled stable lithium metal anode for practical lithium metal pouch cells.Energy Storage Mater2023;58:142-54

[19]

Wen Y,Zhu Y.Expanded graphite as superior anode for sodium-ion batteries.Nat Commun2014;5:4033

[20]

Moon J,Jung H.Interplay between electrochemical reactions and mechanical responses in silicon-graphite anodes and its impact on degradation.Nat Commun2021;12:2714 PMCID:PMC8113583

[21]

Jia T,Lv Y.Prelithiation strategies for silicon-based anode in high energy density lithium-ion battery.Green Energy Environ2023;8:1325-40

[22]

Qian J,Xu W.High rate and stable cycling of lithium metal anode.Nat Commun2015;6:6362 PMCID:PMC4346622

[23]

Toki GFI,Rehman WU,Wang L.Recent progress and challenges in silicon-based anode materials for lithium-ion batteries.Ind Chem Mater2024;2:226-69

[24]

Ye H,Yin YX,Guo YG.An outlook on low-volume-change lithium metal anodes for long-life batteries.ACS Cent Sci2020;6:661-71 PMCID:PMC7256944

[25]

Li AM,Pollard TP.High voltage electrolytes for lithium-ion batteries with micro-sized silicon anodes.Nat Commun2024;15:1206 PMCID:PMC10853533

[26]

Foss CEL,Ulvestad A.Revisiting mechanism of silicon degradation in Li-ion batteries: effect of delithiation examined by microscopy combined with ReaxFF.J Phys Chem Lett2025;16:2238-44 PMCID:PMC11891961

[27]

Taiwo OO,Hall SA.Microstructural degradation of silicon electrodes during lithiation observed via operando X-ray tomographic imaging.J Power Sources2017;342:904-12

[28]

Baek M,Jeong K.Naked metallic skin for homo-epitaxial deposition in lithium metal batteries.Nat Commun2023;14:1296 PMCID:PMC9998607

[29]

Ko S,Shimada T.Electrode potential influences the reversibility of lithium-metal anodes.Nat Energy2022;7:1217-24

[30]

Jiao S,Li Q.Behavior of lithium metal anodes under various capacity utilization and high current density in lithium metal batteries.Joule2018;2:110-24

[31]

Qi X,Pang J.Unveiling micro internal short circuit mechanism in a 60 Ah high-energy-density Li-ion pouch cell.Nano Energy2021;84:105908

[32]

Song Y,Sheng L.The significance of mitigating crosstalk in lithium-ion batteries: a review.Energy Environ Sci2023;16:1943-63

[33]

Wu Z,Yuan F.Ni-rich cathode materials for stable high-energy lithium-ion batteries.Nano Energy2024;126:109620

[34]

Cho H,Kim M,Min K.A review of problems and solutions in Ni-rich cathode-based Li-ion batteries from two research aspects: Experimental studies and computational insights.J Power Sources2024;597:234132

[35]

Ryu H,Kim J,Yoon CS.Capacity fading mechanisms in Ni-rich single-crystal NCM cathodes.ACS Energy Lett2021;6:2726-34

[36]

Zhao Z,Wen Z.Cation mixing effect regulation by niobium for high voltage single-crystalline nickel-rich cathodes.Chem Eng J2023;461:142093

[37]

Lee GH,Shin J,Yang W.Towards commercialization of fluorinated cation-disordered rock-salt Li-ion cathodes.Front Chem2023;11:1098460 PMCID:PMC9880041

[38]

Cai J,Li L.Kinetically dormant Ni-rich layered cathode during high-voltage operation.Adv Mater2025;37:e2419253 PMCID:PMC11983239

[39]

Dong X,Zhu W.Enhanced high-voltage cycling stability of Ni-rich cathode materials via the self-assembly of Mn-rich shells.J Mater Chem A2019;7:20262-73

[40]

Pathak AD,Choi W.Towards the commercialization of Li-S battery: from lab to industry.Energy Storage Mater2024;72:103711

[41]

He B,Cheng Z.Rationally design a sulfur cathode with solid-phase conversion mechanism for high cycle-stable Li-S batteries.Adv Energy Mater2021;11:2003690

[42]

Wang Z,Ji H,Qian T.Unity of opposites between soluble and insoluble lithium polysulfides in lithium-sulfur batteries.Adv Mater2022;34:e2203699

[43]

Huang S,Hu J.Mechanism investigation of high-performance Li-polysulfide batteries enabled by tungsten disulfide nanopetals.ACS Nano2018;12:9504-12

[44]

Zhang Y,Crompton KR,Zhao K.A sulfur cathode design strategy for polysulfide restrictions and kinetic enhancements in Li-S batteries through oxidative chemical vapor deposition.Nano Energy2023;115:108756

[45]

Gao X,Wang J.Electrolytes with moderate lithium polysulfide solubility for high-performance long-calendar-life lithium-sulfur batteries.Proc Natl Acad Sci USA2023;120:e2301260120 PMCID:PMC10400945

[46]

Kim SC,Liao SL.Solvation-property relationship of lithium-sulphur battery electrolytes.Nat Commun2024;15:1268 PMCID:PMC10858963

[47]

Zhang Y,Yin X.Application of anticorrosive materials in cement slurry: Progress and prospect.Front Mater2022;9:1110692

[48]

Pei F,Lin W.Progress and perspectives on molecular design of crosslinked polymer electrolytes for solid-state lithium batteries.Rev Mater Res2025;1:100013

[49]

Zhang J,Liu Y,Takeoka Y.Covalent design of ionogels: bridging with hydrogels and covalent adaptable networks.Polym Chem2025;16:2327-57

[50]

Li Z,Zhou X.In situ chemical lithiation transforms diamond-like carbon into an ultrastrong ion conductor for dendrite-free lithium-metal anodes.Adv Mater2021;33:e2100793

[51]

Meunier V,Morcrette M.Design of workflows for crosstalk detection and lifetime deviation onset in Li-ion batteries.Joule2023;7:42-56

[52]

Du H,Kang Y.Side reactions/changes in lithium-ion batteries: mechanisms and strategies for creating safer and better batteries.Adv Mater2024;36:e2401482

[53]

Xu K.Nonaqueous liquid electrolytes for lithium-based rechargeable batteries.Chem Rev2004;104:4303-417

[54]

Adhitama E,Brake T.Assessing key issues contributing to the degradation of NCM-622 || Cu cells: competition between transition metal dissolution and “dead Li” formation.Adv Energy Mater2024;14:2303468

[55]

Hogrefe C,Hölzle M.Direct observation of internal short circuits by lithium dendrites in cross-sectional lithium-ion in situ full cells.J Power Sources2023;556:232391

[56]

Wang Y,Hu J,Zhang L.Research on internal short circuit detection method for lithium-ion batteries based on battery expansion characteristics.J Power Sources2023;587:233673

[57]

Liu K,Lin D,Cui Y.Materials for lithium-ion battery safety.Sci Adv2018;4:eaas9820 PMCID:PMC6014713

[58]

Silveri F,Esnault V.Multiscale modelling of Si based Li-ion battery anodes.J Power Sources2024;598:234109

[59]

Chae S,Kim K,Cho J.Confronting issues of the practical implementation of Si anode in high-energy lithium-ion batteries.Joule2017;1:47-60

[60]

Zhang S,Xie J.An elastic cross-linked binder for silicon anodes in lithium-ion batteries with a high mass loading.ACS Appl Mater Interfaces2023;15:6594-602

[61]

Choi S,Coskun A.Highly elastic binders integrating polyrotaxanes for silicon microparticle anodes in lithium ion batteries.Science2017;357:279-83

[62]

Jang W,Kang Y,Kim T.A high-performance self-healing polymer binder for Si anodes based on dynamic carbon radicals in cross-linked poly(acrylic acid).Chem Eng J2023;469:143949

[63]

Wang C,Chen Z,Cui Y.Self-healing chemistry enables the stable operation of silicon microparticle anodes for high-energy lithium-ion batteries.Nat Chem2013;5:1042-8

[64]

Zhang D,Wang Y.A gradient-distributed binder with high energy dissipation for stable silicon anode.J Colloid Interface Sci2024;673:312-20

[65]

Cheng D,Zeng Y.Dynamic self-adaption supramolecular binder for silicon anodes: anhydride activation enabling practical lithium-ion battery.Adv Funct Mater2025;2507041

[66]

Cai Y,Yu Z.Slidable and highly ionic conductive polymer binder for high-performance Si anodes in lithium-ion batteries.Adv Sci2023;10:e2205590 PMCID:PMC9951352

[67]

Kim J,Lim EY.Stress-dissipative elastic waterborne polyurethane binders for silicon anodes with high structural integrity in lithium-ion batteries.ACS Appl Energy Mater2024;7:1629-39

[68]

Wang Y,Yuan Y,Zhang H.N-rich solid electrolyte interface constructed in situ via a binder strategy for highly stable silicon anode.Adv Funct Mater2023;33:2301716

[69]

Kozen AC,Zhao O,Rubloff GW.Stabilization of lithium metal anodes by hybrid artificial solid electrolyte interphase.Chem Mater2017;29:6298-307

[70]

Song G,Song WJ.Breathable artificial interphase for dendrite-free and chemo-resistive lithium metal anode.Small2022;18:e2105724

[71]

Hwang C,Song G.A three-dimensional nano-web scaffold of ferroelectric beta-PVDF fibers for lithium metal plating and stripping.ACS Appl Mater Interfaces2020;12:29235-41

[72]

Lee S,Song W.Integration of deformable matrix and lithiophilic sites for stable and stretchable lithium metal batteries.Energy Storage Mater2024;73:103850

[73]

Cheng Y,Chen Y.Lithium host: advanced architecture components for lithium metal anode.Energy Storage Mater2021;38:276-98

[74]

Zhao Y,Mensi M,Coskun A.Electrolyte engineering via ether solvent fluorination for developing stable non-aqueous lithium metal batteries.Nat Commun2023;14:299 PMCID:PMC9849263

[75]

Park S,Lee JA,Choi NS.Liquid electrolyte chemistries for solid electrolyte interphase construction on silicon and lithium-metal anodes.Chem Sci2023;14:9996-10024 PMCID:PMC10530773

[76]

Kim K,Park S.Electrolyte-additive-driven interfacial engineering for high-capacity electrodes in lithium-ion batteries: promise and challenges.ACS Energy Lett2020;5:1537-53

[77]

Han D,Kim S.Dual-functional stacked polymer fibers for stable lithium metal batteries in carbonate-based electrolytes.Small Struct2022;3:2200120

[78]

Bai P,Brushett FR.Transition of lithium growth mechanisms in liquid electrolytes.Energy Environ Sci2016;9:3221-9

[79]

Kang H,Hwang G.Stabilizing a lithium metal anode through the sustainable release of a multi-functional AgNO3 additive.Chem Eng J2024;484:149510

[80]

Han DY,Nam S.Facile lithium densification kinetics by hyperporous/hybrid conductor for high-energy-density lithium metal batteries.Adv Sci2024;11:e2402156 PMCID:PMC11220661

[81]

Jung JT,Wang HH,Drioli E.Understanding the non-solvent induced phase separation (NIPS) effect during the fabrication of microporous PVDF membranes via thermally induced phase separation (TIPS).J Membr Sci2016;514:250-63

[82]

Kim M,Kim J.New continuous process developed for synthesizing sponge-type polyimide membrane and its pore size control method via non-solvent induced phase separation (NIPS).Microporous Mesoporous Mater2017;242:166-72

[83]

Park N,Kim S,Park B.Degradation mechanism of Ni-rich cathode materials: focusing on particle interior.ACS Energy Lett2022;7:2362-9

[84]

Wen Y,Tang Y.Mitigating fast-charging degradation in Ni-rich cathodes via enhancing kinetic-mechanical properties.J Energy Chem2025;107:296-304

[85]

Li X,Banis MN.Atomic layer deposition of solid-state electrolyte coated cathode materials with superior high-voltage cycling behavior for lithium ion battery application.Energy Environ Sci2014;7:768-78

[86]

Liang J,Li X.A gradient oxy-thiophosphate-coated Ni-rich layered oxide cathode for stable all-solid-state Li-ion batteries.Nat Commun2023;14:146 PMCID:PMC9832028

[87]

Chen L,Xin J.High dielectric sulfonyl-containing polyimide binders optimize the long-term stability and safety of NCM811 lithium-ion batteries at high voltages.Chem Eng J2025;503:158670

[88]

Kim JH,Kim JW.Regulating electrostatic phenomena by cationic polymer binder for scalable high-areal-capacity Li battery electrodes.Nat Commun2023;14:5721 PMCID:PMC10504278

[89]

Kang J,Jang S.Bollard-anchored binder system for high-loading cathodes fabricated via dry electrode process for Li-ion batteries.Adv Mater2025;37:e2416872

[90]

Song C,Baek K.Acid- and gas-scavenging electrolyte additive improving the electrochemical reversibility of Ni-rich cathodes in Li-ion batteries.ACS Appl Mater Interfaces2023;15:22157-66

[91]

Zhang D,Ma J.Lithium hexamethyldisilazide as electrolyte additive for efficient cycling of high-voltage non-aqueous lithium metal batteries.Nat Commun2022;13:6966 PMCID:PMC9666536

[92]

Jang J,Ahn J.A fluorine-free binder with organic-inorganic crosslinked networks enabling structural stability of Ni-Rich layered cathodes in lithium-ion batteries.Adv Funct Mater2024;34:2410866

[93]

Jeong D,Kim HJ.Striking a balance: exploring optimal functionalities and composition of highly adhesive and dispersing binders for high-nickel cathodes in lithium-ion batteries.Adv Energy Mater2023;13:2302845

[94]

Vettori K,Ahrens L.Chemical and structural degradation of single crystalline high-nickel cathode materials during high-voltage holds.Adv Energy Mater2025;15:2502148

[95]

Dose WM,Temprano I.Onset potential for electrolyte oxidation and Ni-rich cathode degradation in lithium-ion batteries.ACS Energy Lett2022;7:3524-30 PMCID:PMC9578037

[96]

Fan X,Yin X.One stone for multiple birds: a versatile cross-linked poly(dimethyl siloxane) binder boosts cycling life and rate capability of an NCM 523 cathode at 4.6 V.ACS Appl Mater Interfaces2022;14:16245-57

[97]

Liu Z,Mu P,Liu W.Interfacial chemistry of vinylphenol-grafted PVDF binder ensuring compatible cathode interphase for lithium batteries.Chem Eng J2022;446:136798

[98]

Fu Y,Yuan Y.Switchable encapsulation of polysulfides in the transition between sulfur and lithium sulfide.Nat Commun2020;11:845 PMCID:PMC7016103

[99]

Chen H,Boyle D.Electrode design with integration of high tortuosity and sulfur-philicity for high-performance lithium-sulfur battery.Matter2020;2:1605-20

[100]

Huang Y,Zhang C.Recent advances and strategies toward polysulfides shuttle inhibition for high-performance Li-S batteries.Adv Sci2022;9:e2106004 PMCID:PMC9036004

[101]

Fan Y,Zhang F,Zhao Y.Suppressing the shuttle effect in lithium-sulfur batteries by a UiO-66-modified polypropylene separator.ACS Omega2019;4:10328-35 PMCID:PMC6648104

[102]

Tan J,Dong P,Shen J.Appreciating the role of polysulfides in lithium-sulfur batteries and regulation strategies by electrolytes engineering.Energy Storage Mater2021;42:645-78

[103]

Lin X,Ma D.A zwitterionic polymer binder Integrating multiple dynamic interactions enables high-performance lithium - sulfur batteries.Chem Eng J2025;512:162808

[104]

Yang M,Sun X.Shuttle confinement of lithium polysulfides in borocarbonitride nanotubes with enhanced performance for lithium-sulfur batteries.J Mater Chem A2020;8:296-304

[105]

Zhou L,Eichel R.Host materials anchoring polysulfides in Li-S batteries reviewed.Adv Energy Mater2021;11:2001304

[106]

Wang X,Lai C.Dense-stacking porous conjugated polymer as reactive-type host for high-performance lithium sulfur batteries.Angew Chem Int Ed2021;60:11359-69

[107]

Senthil C,Jung HY.Flame retardant high-power Li-S flexible batteries enabled by bio-macromolecular binder integrating conformal fractions.Nat Commun2022;13:145 PMCID:PMC8748741

[108]

Dose WM,Allen JP.Electrolyte reactivity at the charged Ni-rich cathode interface and degradation in Li-ion batteries.ACS Appl Mater Interfaces2022;14:13206-22 PMCID:PMC9098117

[109]

Yoo S,Shin M.Hierarchical multiscale hyperporous block copolymer membranes via tunable dual-phase separation.Sci Adv2015;1:e1500101 PMCID:PMC4646775

[110]

Tu C,Qi X,Yang Z.Heteroelectrocatalyst MoS2@CoS2 modified separator for Li-S battery: unveiling superior polysulfides conversion and reaction kinetics.Chem Eng J2024;499:155915

[111]

Dong Q,Ren X.Dopamine-modified separator anchoring polysulfides via electrostatic interaction for enhanced Lithium-sulfur batteries.J Energy Storage2025;106:114855

[112]

Lin C,Wang D.Safe, facile, and straightforward fabrication of poly(n-vinyl imidazole)/polyacrylonitrile nanofiber modified separator as efficient polysulfide barrier toward durable lithium-sulfur batteries.Adv Funct Mater2025;35:2411872

[113]

Liu X,Ren D.In situ observation of thermal-driven degradation and safety concerns of lithiated graphite anode.Nat Commun2021;12:4235 PMCID:PMC8270978

[114]

Zheng T,Bao H.Gas evolution in Li-ion rechargeable batteries: a review on operando sensing technologies, gassing mechanisms, and emerging trends.ChemElectroChem2024;11:e202400065

[115]

Murali DR,Lin JY.Zeolite membrane separators for fire-safe Li-ion batteries - effects of crystal shape and membrane pore structure.J Membr Sci2023;680:121743

[116]

Zhang X,Zhen C.Recent progress in flame-retardant separators for safe lithium-ion batteries.Energy Storage Mater2021;37:628-47

[117]

Wang K,Wang Y.Dual phase change separator combining cooling and thermal shutdown functions for Li-ion battery with enhanced safety.Chem Eng J2024;481:148538

[118]

Zhang Y,Zhang XD.A smart risk-responding polymer membrane for safer batteries.Sci Adv2023;9:eade5802 PMCID:PMC9891686

[119]

Wang H,Kong X.Liquid electrolyte: the nexus of practical lithium metal batteries.Joule2022;6:588-616

[120]

Liu YK,Du J,Chen AB.Research progresses of liquid electrolytes in lithium-ion batteries.Small2023;19:e2205315

[121]

Ren D,Hua R.Challenges and opportunities of practical sulfide-based all-solid-state batteries.eTransportation2023;18:100272

[122]

Park J,Kim D.Unraveling the limitations of solid oxide electrolytes for all-solid-state electrodes through 3D digital twin structural analysis.Nano Energy2021;79:105456

[123]

Armand M.Building better batteries.Nature2008;451:652-7

[124]

Meng YS,Xu K.Designing better electrolytes.Science2022;378:eabq3750

[125]

Zhou D,Tkacheva A,Wang G.Polymer electrolytes for lithium-based batteries: advances and prospects.Chem2019;5:2326-52

[126]

Pei F,Zhang Y.Interfacial self-healing polymer electrolytes for long-cycle solid-state lithium-sulfur batteries.Nat Commun2024;15:351 PMCID:PMC10774406

[127]

Tang L,Zhang Z.Polyfluorinated crosslinker-based solid polymer electrolytes for long-cycling 4.5 V lithium metal batteries.Nat Commun2023;14:2301 PMCID:PMC10121557

[128]

Han DY,Kwon JY.Covalently interlocked electrode-electrolyte interface for high-energy-density quasi-solid-state lithium-ion batteries.Adv Sci2025;12:e2417143 PMCID:PMC12165079

[129]

Deng K,Wang S.Effective suppression of lithium dendrite growth using a flexible single-ion conducting polymer electrolyte.Small2018;14:e1801420

[130]

Jeong J,Shin H.Fire-inhibiting nonflammable gel polymer electrolyte for lithium-ion batteries.ACS Energy Lett2023;8:4650-7

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