Size‐Dependent Trade‐off between Sulfur Catalysis and Sulfide Electrolyte Decomposition for Room‐Temperature Ultrahigh‐Rate All‐Solid‐State Li–S Batteries
Abstract
ABSTRACT All‐solid‐state lithium‐sulfur batteries (ASSLSBs) hold immense promise for next‐generation safe and high‐energy storage, yet their power capability is fundamentally limited by sluggish solid‐state sulfur redox kinetics. While catalysis is effective in accelerating these reactions, we reveal for the first time that under overlapping potentials, such catalytic acceleration inevitably triggers severe parasitic decomposition of sulfide solid‐state electrolytes (SSEs), a critical yet overlooked bottleneck that disrupts Li + transport and limits high‐rate performance. To decouple efficient sulfur conversion from interfacial degradation, we devise a spatially selective catalyst architecture. Precisely sized cobalt clusters are confined within an ultra‐microporous carbon host. This design ensures intimate sulfur‐catalyst contact for rapid conversion while physically isolating the catalytic surfaces from the bulk SSE, thereby suppressing its catalytic decomposition. Consequently, the continuous Li + transport network is preserved. The resulting ASSLSB achieves an unprecedented room‐temperature rate capability, stably cycling at an ultrahigh current density of 25.0 mA cm −2 (15 C) for over 15,000 cycles. This work provides a general design principle for reconciling catalysis with interfacial stability in high‐power solid‐state batteries.
Article Details
Authors (14)
Junjie Wang
State Key Laboratory of Quantum Functional Materials, School of Physical Science and Technology
Chuannan Geng
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, State Key Laboratory of Chemical Engineering and Low-Carbon Technology, School of Chemical Engineering and Technology, National Industry-Education Platform for Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
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)
Haotian Yang
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, State Key Laboratory of Chemical Engineering and Low-Carbon Technology, School of Chemical Engineering and Technology, National Industry-Education Platform for Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Shuoyi Chen
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, National Industry‐Education Platform for Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) 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)
Mingyang Jiang
Shenzhen Geim Graphene Center, Shenzhen Key Laboratory for Graphene-Based Materials, Tsinghua Shenzhen International Graduate School
Ying Liu
Luwei Hu
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, National Industry‐Education Platform for Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin University Tianjin China
Qiang Li
Jiwei Shi
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, State Key Laboratory of Chemical Engineering and Low-Carbon Technology, School of Chemical Engineering and Technology, National Industry-Education Platform for Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Li Wang
The Affiliated Cancer Hospital of Zhengzhou University and Henan Cancer Hospital Zhengzhou China
Wei Lv
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