Microenvironment Regulation Unlocks High Li⁺ Conduction in Polyether Electrolytes for High‐Performance Quasi‐Solid‐State Batteries
Abstract
Abstract Polyether electrolytes (PEs) have attracted significant research and industrial interest for high‐performance lithium metal batteries (LMBs). However, traditional PEs are limited by their low lithium‐ion (Li + ) conductivity primary due to strong Li⁺–polymer interactions (i.e. Li + ‐oxygen coordination). Current approaches of modifying polymer molecular structures are largely challenged by the inherent molecular structural constraints of specific polymers and the complexity of the required structural engineering processes. Herein, a novel and straightforward strategy i proposed to reduce the Li + −polymer interaction, increase free‐Li + concentration, and introduce ion‐channels by regulating the microenvironment of PEs through introducing Ge 4+ sites with weak Lewis acidity during in situ polymerization. In this way, the microenvironment regulates PE with a high ionic conductivity of 1.83 mS cm −1 at 25 °C and a Li + transference number of 0.8 is achieved. Remarkably, the electrolyte exhibits extraordinary cycling stability in Li||Li symmetric cells for over 2000 h, demonstrating dendrite‐free Li metal deposition during prolonged cycling. Moreover, the assembled Li||LiFePO 4 cells achieve an impressive capacity retention of 92.1% and ≈100% Coulombic efficiency after a long‐term stability of 2190 cycles at 5 C. This work provides new insight into the design of polymer electrolytes for high‐performance LMBs through microenvironment regulation.
Article Details
Authors (11)
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
Lanting Qian
Department of Chemistry and the Waterloo Institute for Nanotechnology
Yun Zheng
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
Zewen Liu
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
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
Qianyi Ma
Department of Chemical Engineering, Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue West, Waterloo, Ontario N2L 3G1, Canada
Yidong Jiang
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