{"title":"Asymmetric Functional Gel Polymer Electrolyte Enables Superior Interfacial Compatibility for Wide Temperature Lithium Metal Batteries","authors":"Haixia Yang, Jiaxin Yan, Shuyang Gao, Xin Chen, Yuanheng Wang, Hua Huo, Chuankai Fu, Chunyu Du, Pengjian Zuo","doi":"10.1039/d5ee03838c","DOIUrl":null,"url":null,"abstract":"Lithium metal batteries (LMBs) represent a promising candidate for next-generation energy storage systems, yet their practical application is constrained by limited cycle life owing to slow interface Li+ ion transport and severe interfacial side reactions, particularly in extreme temperature conditions. Herein, a novel asymmetric gel polymer electrolyte (GPE) is constructed through sequential electrospinning and Li6.4La3Zr1.4Ta0.6O12 (LLZTO) filler integration to achieve high compatibility with Li anode and high-voltage cathode over wide temperature range. The polyethylene oxide (PEO)/poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix adjacent to the Li anode homogenizes Li⁺ ion flux and facilitates the formation of stable solid electrolyte interphase (SEI) through dynamic interfacial remodeling. At the cathode side, the polyacrylonitrile (PAN)/PVDF-HFP matrix exhibits outstanding high-voltage tolerance, effectively suppressing transition metal dissolution and electrolyte decomposition. The incorporated LLZTO enhances LiPF6 dissociation via selective adsorption. The highly porous asymmetric polymer framework architecture facilitates the elimination of macroscopic interfaces among dissimilar materials, achieving fast Li⁺ ion transport. Consequently, the Li||Ni0.8Co0.1Mn0.1O2 cells exhibit outstanding wide temperature cycling of -30 to 70 °C. This asymmetric structure design of GPE offers valuable insights into interfacial engineering exploration for all-climate LMBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"2 1","pages":""},"PeriodicalIF":30.8000,"publicationDate":"2025-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy & Environmental Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d5ee03838c","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Lithium metal batteries (LMBs) represent a promising candidate for next-generation energy storage systems, yet their practical application is constrained by limited cycle life owing to slow interface Li+ ion transport and severe interfacial side reactions, particularly in extreme temperature conditions. Herein, a novel asymmetric gel polymer electrolyte (GPE) is constructed through sequential electrospinning and Li6.4La3Zr1.4Ta0.6O12 (LLZTO) filler integration to achieve high compatibility with Li anode and high-voltage cathode over wide temperature range. The polyethylene oxide (PEO)/poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix adjacent to the Li anode homogenizes Li⁺ ion flux and facilitates the formation of stable solid electrolyte interphase (SEI) through dynamic interfacial remodeling. At the cathode side, the polyacrylonitrile (PAN)/PVDF-HFP matrix exhibits outstanding high-voltage tolerance, effectively suppressing transition metal dissolution and electrolyte decomposition. The incorporated LLZTO enhances LiPF6 dissociation via selective adsorption. The highly porous asymmetric polymer framework architecture facilitates the elimination of macroscopic interfaces among dissimilar materials, achieving fast Li⁺ ion transport. Consequently, the Li||Ni0.8Co0.1Mn0.1O2 cells exhibit outstanding wide temperature cycling of -30 to 70 °C. This asymmetric structure design of GPE offers valuable insights into interfacial engineering exploration for all-climate LMBs.
期刊介绍:
Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences."
Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).