Competitive Adsorption and Structural Reinforcement Synergy Stabilizes High‐Voltage Quasi‐Solid‐State Batteries
Abstract
ABSTRACT Quasi‐solid‐state batteries (QSSBs) employing high‐voltage cathodes promise high energy density and safety, yet suffer from unstable cathode/electrolyte interfaces and cathode degradation. Here, we propose a competitive adsorption and structural reinforcement synergy (CASR) strategy to address these challenges. Specifically, a Cu‐centered self‐adsorption molecule is incorporate into the polymer electrolyte, which preferentially adsorbs at the cathode/electrolyte interface through competitive adsorption against solvent molecules, thereby reducing the solvent content on the cathode surface while promoting anion enrichment. This process induces the formation of a uniform F‐rich cathode/electrolyte interphase with a LiF‐rich outer layer and an inner layer containing Cu─F bonds, thereby effectively suppressing cathode degradation. Cathode structural stability is further reinforced through dynamic Cu doping into TM‐deficient lattice sites during cycling. Under low‐loading coin‐cell conditions (2.0 mg cm −2 ), the resulting Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 QSSBs retain 80% of their initial capacity after 400 cycles at 4.6 V, and achieve 80% capacity retention over 1000 cycles under 10C and 4.5 V. A 1 Ah‐level pouch‐cell tested under 4.3 V and 1C charge/0.5C discharge conditions supports the potential of the CASR strategy. This work provides a promising pathway for synchronously stabilizing cathode/electrolyte interface and cathode structure in high‐voltage QSSBs.
Article Details
Authors (15)
Lifen Zhang
College of Chemical Engineering, Institute of New Energy Materials and Engineering, College of Materials Science and Engineering, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems
Zongtao Lu
Institute of New Energy Materials and Engineering, College of Materials Science and Engineering, State Key Laboratory of Green and Efficient Development of Phosphorus Resources, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems
Song Duan
Institute of New Energy Materials and Engineering, College of Materials Science and Engineering, State Key Laboratory of Green and Efficient Development of Phosphorus Resources, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems
Bingsen Qin
Institute of New Energy Materials and Engineering, College of Materials Science and Engineering, State Key Laboratory of Green and Efficient Development of Phosphorus Resources, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems
Hongyao Wang
Institute of New Energy Materials and Engineering, College of Materials Science and Engineering, State Key Laboratory of Green and Efficient Development of Phosphorus Resources, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems
Peng Wang
Zhenghao Li
Institute of New Energy Materials and Engineering, College of Materials Science and Engineering, State Key Laboratory of Green and Efficient Development of Phosphorus Resources, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems
Junfei Zhu
Institute of New Energy Materials and Engineering, College of Materials Science and Engineering, State Key Laboratory of Green and Efficient Development of Phosphorus Resources Fuzhou University Fuzhou P.R. China
Junwen Fu
Zhiyang Yu
State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry
Sijie Liu
Research Institute of Tsinghua University in Shenzhen
Can Liao
Department of Chemistry
Wei Yan
Jiujun Zhang
Institute of New Energy Materials and Engineering, College of Materials Science and Engineering, State Key Laboratory of Green and Efficient Development of Phosphorus Resources, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems
Yun Zheng