Anion competition for Li+solvated coordination environments in poly(1,3 dioxolane)electrolyte to enable high-voltage lithium metal solid-state batteries

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外文摘要：Gel-based polymer electrolytes are limited by the polarity of the residual solvent,which restricts the coupling-breaking behaviour during Li+conduction,resulting in the Li+transport kinetics being greatly affected.Here,we designed anion competitive gel polymer electrolyte(ACPE)by introducing lithium difluoro(oxalato)borate(LiDFOB)anion into the 1,3-dioxolane(DOL)in situ polymerisation system.ACPE enhances the ionic dipole interaction between Li+and the solvent molecules and synergizes with Li+across the solvation site of the polymer ethylene oxide(EO)unit,combination that greatly improves the Li+transport efficiency.As a result,ACPE exhibits 1.12 mS cm-1 ionic conductivity and 0.75 Li+trans-fer number at room temperature.Additionally,this intra-polymer solvation sheath allows preferential desolvation of DFOB-,which contributes to the formation of kinetically stable anion-derived interphase and effectively mitigates side reactions.Our results demonstrate that the assembled Li||NCM622 solid-state battery exhibits lifespan of over 300 cycles with average Coulombic efficiency of 98.8％and capacity retention of 80.3％.This study introduces a novel approach for ion migration and interface design,paving the way for high-safety and high-energy-density batteries.

外文关键词：

Li-metal batteriesPoly(1,3-dioxolane)In situ polymerizationSolid-state polymer electrolytesAnion competition

作者：

Qiujun Wang、Yanqiang Ma、Xiaomeng Jia、Di Zhang、Zhaojin Li、Huilan Sun、Qujiang Sun、Bo Wang、Li-Zhen Fan

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作者单位：

Hebei Key Laboratory of Flexible Functional Materials,School of Materials Science and Engineering,Hebei University of Science and Technology,Shijiazhuang 050000,Hebei,China

Beijing Advanced Innovation Center for Materials Genome Engineering,Institute of Advanced Materials and Technology,University of Science and Technology Beijing,Beijing 100083,China

基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNatural Science Foundation of Hebei ProvinceNatural Science Foundation of Hebei ProvinceNatural Science Foundation of Hebei ProvinceBeijing Natural Science Foundation

项目编号：

2200805352002111B2021208061B2022208006B2023208014Z200011

出版年：

2024

DOI：

10.1016/j.jechem.2024.05.028

能源化学

中国科学院大连化学物理研究所中国科学院成都有机化学研究所

能源化学

CSTPCDEI

影响因子：0.654

ISSN：2095-4956

年,卷(期)：2024.96(9)