Self‐Medicating Molten‐Salt Synthesis of Bulk‐Stabilized High‐Energy Cathodes for Li‐Ion Batteries
Abstract
Abstract High‐energy lithium‐ion batteries necessitate stable Ni‐rich layered cathodes, yet critical challenges such as lattice distortion and surface structure collapse remain unresolved. While conventional high‐valence doping greatly alleviates surface degradations, it is ineffective in stabilizing bulk lattice due to dopant segregation. Here, we propose a slightly Li‐rich (SLR) lattice design by partially substituting transition‐metal (TM) ions with Li + ions in TM layers, reducing electrostatic repulsion against high‐valence dopants. Integrated theory‐experiment analyses reveal uniform bulk doping of Mo 6+ in SLR cathodes, realized via a self‐medicating and scalable molten‐salt synthesis route. An optimized high‐energy cathode (880 Wh kg −1 cathode ) achieves 89% retention after 1000 cycles in Ah‐scale pouch cells, sustains 10 C ultrafast charging/discharging for 300 cycles (3.8 min to 80% state‐of‐charge), and operates stably in all‐solid‐state batteries. Multimodal characterizations link uniform Mo 6+ doping to suppressed lattice strain and structural collapse. This work establishes a new paradigm for bulk lattice engineering of advanced battery cathodes.
Article Details
Authors (17)
Xiaoqiao Li
Department of Chemical Engineering Shanghai Electrochemical Energy Devices Research Center School of Chemistry and Chemical Engineering Shanghai Jiao Tong University Shanghai 200240 China
Fanxiu Feng
Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Renewable Energy Conversion and Storage Center College of Chemistry Nankai University Tianjin 300071 China
Taiping Hu
School of Materials Science and Engineering
Yong Wang
Chenji Hu
School of Chemistry and Chemical Engineering, in-situ Center for Physical Sciences, Shanghai Electrochemical Energy Device Research Center (SEED) and Frontiers Science Center for Transformative Molecules
Jingyu Chen
Yilin Chen
School of Urban Planning and Design, Peking University, Shenzhen Graduate School
Chun Cheng
Department of Materials Science and Engineering
Han Wang
Qinfeng Zheng
School of Chemistry and Chemical Engineering, In Situ Center for Physical Sciences, Shanghai Electrochemical Energy Device Research Center (SEED)
Yixiao Zhang
Yu‐Shi He
Department of Chemical Engineering Shanghai Electrochemical Energy Devices Research Center School of Chemistry and Chemical Engineering Shanghai Jiao Tong University Shanghai 200240 China
Shenzhen Xu
School of Materials Science and Engineering
Wei Zhang
Liwei Chen
School of Chemistry and Chemical, In situ Center for Physical Science
Zi‑Feng Ma
Linsen Li
School of Chemistry and Chemical Engineering, in-situ Center for Physical Sciences, Shanghai Electrochemical Energy Device Research Center (SEED) and Frontiers Science Center for Transformative Molecules