Stress‐Lensed Electrochemical Sintering Enables Fast and Stable Lithium‐Silicon Alloy Chemistry in All‐Solid‐State Batteries
Abstract
ABSTRACT The fundamental challenge in all‐solid‐state batteries (ASSBs) lies in regulating the dynamic reconstruction of solid‐solid interfaces under electro‐chemo‐mechanical conditions. Currently, no mechanism exists to reconcile the conflicting requirements of structural stability and rapid ion transport for high‐capacity silicon (Si) anodes: expansion‐accommodated encapsulation strategies preserve integrity but block interparticle ionic contact, while intrinsic electrochemical sintering restores conduction but creates excessive agglomeration that fractures the electrode. Here, we propose a stress‐lensed electrochemical sintering (SLES) strategy to guide selective interfacial bonding by depositing Si conformally into a porous carbon host, specifically utilizing its high‐curvature pore entrances as geometric constrictions. During cycling, these constrictions act as “stress lenses”, concentrating the volumetric expansion stress of Si precisely at interparticle contacts. This focused mechanical energy locally lowers the atomic diffusion barrier, guiding the formation of a robust, percolating Si network while preserving internal voids to buffer volume changes. The resulting Si‐SLES anode resolves the stability‐transport conflict, achieving ∼100% capacity retention after 100 cycles with superior rate capability and demonstrating practical viability in full cells over 700 cycles.
Article Details
Authors (16)
Tianze Xu
Jiangsu Co-Innovation Centre of Efficient Processing and Utilization of Forest Resources, College of Chemical Engineering
Qingdong Gao
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, National Industry‐Education Integration Platform of Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering Tianjin University Tianjin China
Jiaxing He
Department of Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong 99077, China
Jiangshan Qi
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, National Industry-Education Integration Platform of Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Michael Häusler
Materials Center Leoben Forschung GmbH Leoben Austria
Zhenshen Li
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, National Industry‐Education Integration Platform of Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering Tianjin University Tianjin China
Fangbing Li
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, National Industry-Education Integration Platform of Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Sijia Chi
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, National Industry-Education Integration Platform of Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Deyuan Li
Junwei Han
Shandong Key Laboratory of Advanced Electrochemical Energy Storage Technologies, College of New Energy
Jing Xiao
School of Materials Science and Engineering, Sun Yat-sen University
Wei Wei
Ziyun Zhao
Roland Brunner
Shichao Wu
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, National Industry-Education Integration Platform of Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Quan‐hong Yang
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin University Tianjin 300072 China