Patching Solid Electrolyte Interphase via Modulating Anion Decomposition Reactions for Stable Lithium Metal Batteries

J Jia‐Lin Li (School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China) X Xue‐Qiang Zhang (School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China) P Pei‐Ping Yu (Institute of Functional Nano and Soft Materials Jiangsu Key Laboratory for Carbon‐based Functional Materials and Devices Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215006 P.R. China) S Shu‐Yu Sun (Beijing Key Laboratory of Complex Solid State Batteries Department of Chemical Engineering Tsinghua University Beijing 100084 P.R. China) L Lin‐Kun Yang (School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China) Y Ya‐Nan Wang (School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China) Z Zhao Zheng (Beijing Key Laboratory of Complex Solid State Batteries & Tsinghua Center for Green Chemical Engineering Electrification, Department of Chemical Engineering) X Xue‐Yi Yan (School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China) W Wen‐Jun Feng (Beijing Key Laboratory of Complex Solid State Batteries Department of Chemical Engineering Tsinghua University Beijing 100084 P.R. China) X Xiaoru Chen (Research Institute of Tsinghua University Shenzhen 518057 P.R. China) T Tao Cheng (Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Jiangsu Key Laboratory of Advanced Negative Carbon Technologies) J Jia‐Qi Huang (School of Interdisciplinary Science Beijing Institute of Technology Beijing P. R. China)

Abstract

Abstract Solid electrolyte interphase (SEI) on lithium (Li) metal anodes undergoes repeated rupture and patching during cycles, which induces the formation of inactive Li and the rapid failure of Li metal batteries. The inactive Li compounds used to patch SEI dominate inactive Li for highly reversible Li metal anodes. Herein, patching SEI rapidly by modulating decomposition reactions of bis(fluorosulfonyl)imide anion (FSI − ) in the electrolyte is proposed to decrease the amount of inactive Li compounds. Increasing overpotential of anodes can promote the fast and complete decomposition reactions of FSI − , which increases the amount of insoluble inorganic components in the decomposition products of one FSI − . Abundant insoluble inorganic components can build SEI efficiently to avoid the further decomposition of the electrolyte. Then, a protocol is proposed to increase overpotential of anodes by applying a high current density within a short time during the final stage of Li deposition in Li metal batteries. With the proposed protocol, the amount of inactive Li compounds decreases by 62.2%. Furthermore, a prototype pouch cell of 411 Wh kg −1 achieves 202 stable cycles. This work provides a fresh understanding of SEI formation and inspires a new strategy to stabilize SEI.

Article Details

Volume / Issue Vol. 65, Issue 5
Published January 28, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (12)

J

Jia‐Lin Li

School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China

X

Xue‐Qiang Zhang

School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China

P

Pei‐Ping Yu

Institute of Functional Nano and Soft Materials Jiangsu Key Laboratory for Carbon‐based Functional Materials and Devices Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215006 P.R. China

S

Shu‐Yu Sun

Beijing Key Laboratory of Complex Solid State Batteries Department of Chemical Engineering Tsinghua University Beijing 100084 P.R. China

L

Lin‐Kun Yang

School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China

Y

Ya‐Nan Wang

School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China

Z

Zhao Zheng

Beijing Key Laboratory of Complex Solid State Batteries & Tsinghua Center for Green Chemical Engineering Electrification, Department of Chemical Engineering

X

Xue‐Yi Yan

School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China

W

Wen‐Jun Feng

Beijing Key Laboratory of Complex Solid State Batteries Department of Chemical Engineering Tsinghua University Beijing 100084 P.R. China

X

Xiaoru Chen

Research Institute of Tsinghua University Shenzhen 518057 P.R. China

T

Tao Cheng

Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Jiangsu Key Laboratory of Advanced Negative Carbon Technologies

J

Jia‐Qi Huang

School of Interdisciplinary Science Beijing Institute of Technology Beijing P. R. China