journal article·2025-09Open access

Atypical Hydrogen Bond Interaction Enables Anion‐Rich Solvation Structure in Polymer Electrolytes for High‐Voltage Flexible Lithium Metal Batteries

Shujing Wen, Junhua Zhou, Guangzhao Zhang, Qingrong Wang, Chao Luo, Ruo Wang, Pengxian Li, Chaoyang Wang, Xiaoxiong Xu, Yonghong Deng, Jian Chang, Zijian Zheng

Advanced Science· Volume 12· Issue 34

Abstract

Abstract Flexible lithium metal batteries (LMBs) using polymer‐based solid‐state electrolytes (PSSEs) are highly desirable for wearable applications because of the potential advantages in energy density and safety. Recently, ether‐based polyelectrolytes have received extensive attention because of their good stability, high ionic conductivity, and Li metal anode compatibility. However, it typically forms organic‐rich cathode electrolyte interphase (CEI) at the cathode, which is still a pain point that impedes the high‐voltage performance. To address this challenge, herein a fluorinated plasticizer, bis(2‐fluoroethyl) ether (BFE) is reported, which can be easily blended into ether‐based PSSE and enables high‐voltage‐stable flexible LMBs. The BFE and PSSE molecules form an atypical hydrogen bond interaction, which weakens the interaction between PSSE and lithium ions. This leads to the formation of an anion‐rich solvation structure that generates inorganic‐rich and high‐voltage‐stable CEI. The oxidation stability of PSSE is improved from 4.4 V to over 4.7 V after introducing the BFE molecules. LMBs using BFE‐blended PSSE can couple with high‐voltage cathode and retain 80% capacity after 480 cycles at 1C. Full cells show high energy density (752.2 Wh L −1 ) outstanding capacity retention per cycle (99.88%), and high flexibility with almost identic charge/discharge characteristics after 4000 bending cycles.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced Battery Technologies Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Applied Biology and Chemical Technology Faculty of Science The Hong Kong Polytechnic University Hung Hom Hong Kong SAR 999077 China

Department of Materials Science and Engineering, School of Innovation and Entrepreneurship Key University Laboratory of Highly Efficient Utilization of Solar Energy and Sustainable Development of Guangdong Southern University of Science and Technology Shenzhen 518055 China

Dongguan Key Laboratory of Interdisciplinary Science for Advanced Materials and Large‐Scale Scientific Facilities School of Physical Sciences Great Bay University Dongguan Guangdong 523000 China

Research Institute of Materials Science South China University of Technology Guangzhou 510640 China

Research Institute for Smart Energy The Hong Kong Polytechnic University Hung Hom Hong Kong SAR 999077 China

Research Institute for Intelligent Wearable Systems The Hong Kong Polytechnic University Hung Hom Hong Kong SAR 999077 China

PolyU‐Daya Bay Technology and Innovation Research Institute Huizhou Guangdong 516083 China

PolyU‐Wenzhou Technology and Innovation Research Institute Wenzhou Zhejiang 325024 China

Funding

National Natural Science Foundation of China · Basic and Applied Basic Research Foundation of Guangdong Province · Shenzhen Science and Technology Innovation Program · Hong Kong Polytechnic University

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