Self-Regulating Interfacial Space Charge through Polyanion Repulsion Effect towards Dendrite-Free Polymer Lithium-Metal Batteries

被引:20
作者
Cui, Manying [1 ]
Gao, Na [1 ]
Zhao, Wenshan [1 ]
Zhao, Hongyang [1 ]
Cao, Zhenjiang [1 ]
Qin, Yanyang [1 ]
Gao, Guoxin [1 ]
Xi, Kai [1 ]
Su, Yaqiong [1 ]
Ding, Shujiang [1 ]
机构
[1] Xi An Jiao Tong Univ, Engn Res Ctr Energy Storage Mat & Devices, Sch Chem, State Key Lab Mech Behav Mat,Minist Educ, 28 Xianning West Rd, Xian 710049, Peoples R China
基金
中国国家自然科学基金;
关键词
concentration polarization; ion transport regulation; lithium-metal battery; polymer electrolyte; single-ion conductor; ELECTROLYTES;
D O I
10.1002/aenm.202303834
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Uncontrolled transport of anions leads to many issues, including concentration polarization, excessive interface side reactions, and space charge-induced lithium dendrites at the anode/electrolyte interface, which severely deteriorates the cycling stability of lithium metal batteries. Herein, an asymmetrical polymer electrolyte modified by a boron-containing single-ion conductor (LiPVAOB), is designed to inhibit the nonuniform aggregation of free anions in the vicinity of the lithium anode through the repulsion effect improving the lithium-ion transference number to 0.63. This LiPVAOB exerts a repulsion interaction with free anions even at a long distance and a selective effect for free anions transport, which diminishes uneven aggregation of free anions at the interface and suppresses space charges-induced lithium dendrites growth. Consequently, the assembled Li||Li cell delivers an ultra-long cycle for over 5400 h. The Li||LiFePO4 cell exhibits outstanding cycle performance with a capacity retention of 93% over 4500 cycles. In particular, the assembled high-voltage Li||Li1.2Ni0.2Mn0.6O2 cell (charged to 4.8 V) exhibits good cycle stability with a high specific capacity of 245 mAh g-1. This designed polymer electrolyte provides a promising strategy for regulating ion transport to inhibit space charge-induced lithium dendrite growth for high-performance lithium metal batteries. An asymmetrical polymer electrolyte modified by a boron-containing single-ion conductor (LiPVAOB) is designed to inhibit the nonuniform aggregation of free anions in the vicinity of the lithium anode. This LiPVAOB exerts a repulsion interaction with free anions even at a long distance, which diminishes uneven aggregation of free anions at the interface and suppresses space charges-induced lithium dendrites growth.image
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页数:10
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