High‐Valence‐Cation‐Induced Lattice Expansion for Activating Li <sub>2</sub> S Cathode in All‐Solid‐State Lithium‐Sulfur Batteries
Abstract
ABSTRACT The practical deployment of lithium sulfide (Li 2 S) cathodes in all‐solid‐state lithium‐sulfur batteries (ASSLSBs) is challenged by their poor innate conductivities and high activation barriers. Here, we demonstrate a lattice engineering strategy using Zr 4+ substitution to fundamentally activate Li 2 S. The introduced Zr 4 + expands the lattice, creating lithium vacancies that enhance ionic conductivity by two orders of magnitude. Simultaneously, Zr─S orbital hybridization narrows the bandgap for superior electronic conductivity and weakens Li─S bonds to lower the activation energy. This synergistic effect enables a highly reversible solid‐state sulfur conversion. As a result, our ASSLSB delivers an ultrahigh energy density of 996.2 Wh kg −1 based on the cathode with a record 65 wt.% electrode‐level Li 2 S content and maintains stability for over 100 cycles, far exceeding the conventional configuration of ∼40 wt.% loading. This strategy establishes a viable pathway toward practical high‐energy‐density ASSLSBs by fundamentally activating Li 2 S electrochemistry.
Article Details
Authors (14)
Shuang Hong
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 Integration Platform of Energy Storage and Collaborative Innovation Center of Chemical Science and Engineering Tianjin University Tianjin China
Yun Cao
Key Laboratory of Evolution and Marine Biodiversity (Ministry of Education) and Institute of Evolution and Marine Biodiversity, Ocean University of China, Qingdao, 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)
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)
Ruiqing Ye
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)
Lingjing Wei
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 Integration Platform of Energy Storage and Collaborative Innovation Center of Chemical Science and Engineering Tianjin University Tianjin China
Yanyan Wang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry
Boya Zhang
Yu Long
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
Chen Zhang
Shenzhen Institute for Quantum Science and Engineering, Department of Chemistry, and Department of Physics
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