Molecular‐level Designed Polymer Electrolyte for High‐Voltage Lithium–Metal Solid‐State Batteries

• DOI: 10.1002/adfm.202209828
• Publication Date: 2022-11-14T11:02:34Z
• Authors: Chao Wang; Hong Liu; Yuhao Liang; Dabing Li; Xiaoxue Zhao; Jiaxin Chen; Weiwei Huang; Lei Gao; Li‐Zhen Fan
• Keywords: Polycarbonate

Abstract In solid polymer electrolytes (SPEs) based Li–metal batteries, the inhomogeneous migration of dual‐ion in cell results large concentration polarization and reduces interfacial stability during cycling. A special molecular‐level designed electrolyte (MDPE) is proposed by embedding a functional group (4‐vinylbenzotrifluoride) polycarbonate base. MDPE, matrix obtained copolymerization vinylidene carbonate 4‐vinylbenzotrifluoride coupled with anion lithium‐salt hydrogen bonding “σ‐hole” effect CF bond. This intermolecular interaction limits increases ionic transfer number MDPE ( t Li + = 0.76). The mechanisms enhanced are profoundly understood conducting first‐principles density theory calculation. Furthermore, has an electrochemical window (4.9 V) excellent due to CO trifluoromethylbenzene (ph‐CF 3 ) matrix. Benefited from these merits, LiNi 0.8 Co 0.1 Mn O 2 ‐based solid‐state cells as both host electrode binder exhibit good rate cycling performance. study demonstrates that at molecular level can provide broader platform for high‐performance design needs lithium batteries.