期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 46, 页码 51374-51386出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c13520
关键词
Lithium metal batteries; high voltage; gel polymer electrolyte; customized frontier orbital energy level; interface compatibility
资金
- Science Foundation for the Strategic Priority Research Program of the Chinese Academy of Sciences [XDA22010600]
- Distinguished Young Scholars of China [51625204]
- National Key R&D Program of China [2018YFB0104300]
- National Natural Science Foundation of China [51803230]
- NSFC-Shandong Joint Fund [U1706229]
The development of gel polymer electrolytes (GPEs) is considered to be an effective strategy to drive practical applications of high-voltage lithium metal batteries (HLMBs). However, rare GPEs that can satisfy the demands of HLMBs have been developed because of the limited compatibility with lithium anodes and high-voltage cathodes simultaneously. Herein, a novel strategy for constructing polymer matrixes with a customized frontier orbital energy for GPEs is proposed. The as-investigated polymer matrix (P(CUMA-NPF6))-based GPE (P(CUMA-NPF6)-GPE) obtained via in situ random polymerization delivers a wide voltage window (0-5.6 V vs Li+/Li), large lithium-ion transference number (t(Li)(+), 0.61), and superior electrode/electrolyte interface compatibility. It is to be noted that such a t(Li)(+) of P(CUMA-NPF6)-GPE, which is one of the largest t(Li)(+) among high-voltage GPEs in a fair comparison, results from the high dissociation of lithium salts and effective anion immobilization abilities of P(CUMA-NPF6). Ultimately, the as-assembled HLMB delivers more enhanced cycle performance than its counterpart of commercial liquid electrolytes. It is also demonstrated that P(CUMA-NPF6) can scavenge the active PF5 intermediate generated in the electrolyte at the anode side, thus suppressing the PF5-mediated decomposition reaction of carbonates. This work will enlighten the rational structure design of GPEs for HLMBs.
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