Constructing Durable High‐Voltage PVDF‐Based Solid‐State Lithium Metal Batteries via an All‐in‐One Design
Abstract
ABSTRACT Poly(vinylidene fluoride) (PVDF)‐based solid electrolytes represent a compelling frontier for solid‐state lithium metal batteries. Unfortunately, their practical implementation is severely impeded by high Li + migration energy barrier and pronounced interfacial instabilities, arising from α‐phase‐rich conformations and undesired Li + ‐solvation environments. In this study, an ‘all‐in‐one’ regulation strategy enabled by N‐methylimidazolium bis((trifluoromethyl)sulfonyl)imide (MimTFSI) is proposed, which synergistically engineers a β‐phase polymer matrix for shortened pathways and constructs an anion‐rich solvation sheath for lowered energy barriers, ultimately unlocking fast and stable Li + transport coupled with exceptional interfacial compatibility. Consequently, this integrated solid‐state electrolyte demonstrates a high ionic conductivity of 0.84 mS cm − 1 , supports stable cycling of Li symmetric cells for over 4000 h at 0.1 mA cm − 2 , and delivers outstanding cycling performance in Li/LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cells, retaining 93.8% of its initial capacity after 930 cycles at 0.5 C and 95% over 500 cycles at 1 C. Even under expanded voltage windows, it retains 80% after 580 cycles at 4.4 V and 84% after 160 cycles at 4.5 V. Furthermore, the pouch cell is capable of delivering a discharge capacity of 3.26 mAh cm −2 , demonstrating the strong applicability for next‐generation solid‐state lithium metal batteries.
Article Details
Authors (9)
Yuchen Wang
State Key Laboratory of Animal Biodiversity Conservation and Integrated Pest Management, Institute of Zoology, Chinese Academy of Sciences
Xinpeng Han
Guangxi Key Laboratory of Processing for Non‐ferrous Metals and Featured Materials MOE Key Laboratory of New Processing Technology for Non‐ferrous Metals and Materials Guangxi Key Laboratory of Electrochemical Energy Materials Guangxi Key Lab of Petrochemical Resource Processing and Process Intensification Technology School of Chemistry and Chemical Engineering School of Resources Environment and Materials Guangxi Key Laboratory of Advanced Rare Earth Materials Guangxi University Nanning China
Keyan Li
State Key Laboratory of Fine Chemicals Frontier Science Center For Smart Materials PSU‐DUT Joint Center for Energy Research School of Chemical Engineering Dalian University of Technology Dalian China
Wantao Meng
Guangxi Key Laboratory of Processing for Non‐ferrous Metals and Featured Materials MOE Key Laboratory of New Processing Technology for Non‐ferrous Metals and Materials Guangxi Key Laboratory of Electrochemical Energy Materials Guangxi Key Lab of Petrochemical Resource Processing and Process Intensification Technology School of Chemistry and Chemical Engineering School of Resources Environment and Materials Guangxi Key Laboratory of Advanced Rare Earth Materials Guangxi University Nanning China
Henghui Xiao
Guangxi Key Laboratory of Processing for Non‐ferrous Metals and Featured Materials MOE Key Laboratory of New Processing Technology for Non‐ferrous Metals and Materials Guangxi Key Laboratory of Electrochemical Energy Materials Guangxi Key Lab of Petrochemical Resource Processing and Process Intensification Technology School of Chemistry and Chemical Engineering School of Resources Environment and Materials Guangxi Key Laboratory of Advanced Rare Earth Materials Guangxi University Nanning China
Jiaxin Wei
Dong Yang
Xinwen Guo
State Key Laboratory of Fine Chemicals, Frontier Science Center for Smart Materials, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering
Meinan Liu
-Lab & CAS Key Laboratory of Nanophotonic Materials and Devices