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首页> 外文期刊>Advanced functional materials >Molecular-level Designed Polymer Electrolyte for High-Voltage Lithium–Metal Solid-State Batteries
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Molecular-level Designed Polymer Electrolyte for High-Voltage Lithium–Metal Solid-State Batteries

机译：Molecular-level Designed Polymer Electrolyte for High-Voltage Lithium–Metal Solid-State Batteries

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摘要

In solid polymer electrolytes (SPEs) based Li–metal batteries, the inhomogeneousmigration of dual-ion in the cell results in large concentration polarizationand reduces interfacial stability during cycling. A special molecular-leveldesigned polymer electrolyte (MDPE) is proposed by embedding a specialfunctional group (4-vinylbenzotrifluoride) in the polycarbonate base. InMDPE, the polymer matrix obtained by copolymerization of vinylidene carbonateand 4-vinylbenzotrifluoride is coupled with the anion of lithium-saltby hydrogen bonding and the “σ-hole” effect of the CF bond. This intermolecularinteraction limits the migration of the anion and increases the ionictransfer number of MDPE (t_(Li)~+ = 0.76). The mechanisms of the enhanced t_(Li)~+of MDPE are profoundly understood by conducting first-principles densityfunctional theory calculation. Furthermore, MDPE has an electrochemicalstability window (4.9 V) and excellent electrochemical stability with Li–metaldue to the C=O group and trifluoromethylbenzene (ph-CF_3) of the polymermatrix. Benefited from these merits, LiNi_(0.8)Co_(0.1)Mn_(0.1)O_2-based solid-statecells with the MDPE as both the electrolyte host and electrode binder exhibitgood rate and cycling performance. This study demonstrates that polymerelectrolytes designed at the molecular level can provide a broader platformfor the high-performance design needs of lithium batteries.

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