Molecular anchoring of free solvents for high-voltage and high-safety lithium metal batteries

被引：68

作者：

Cui, Zhuangzhuang ^{[1
]}

Jia, Zhuangzhuang ^{[2
]}

Ruan, Digen ^{[1
]}

Nian, Qingshun ^{[1
]}

Fan, Jiajia ^{[1
]}

Chen, Shunqiang ^{[1
]}

He, Zixu ^{[1
]}

Wang, Dazhuang ^{[1
]}

Jiang, Jinyu ^{[1
]}

Ma, Jun ^{[1
]}

Ou, Xing ^{[3
]}

Jiao, Shuhong ^{[1
]}

Wang, Qingsong ^{[2
]}

Ren, Xiaodi ^{[1
]}

机构：

[1] Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Dept Mat Sci & Engn, CAS Key Lab Mat Energy Convers, Hefei 230026, Anhui, Peoples R China

[2] Univ Sci & Technol China, State Key Lab Fire Sci, Hefei 230026, Anhui, Peoples R China

[3] Cent South Univ, Engn Res Ctr, Sch Met & Environm, Minist Educ Adv Battery Mat, 932 South Lushan Rd, Changsha 410083, Hunan, Peoples R China

来源：

NATURE COMMUNICATIONS | 2024年 / 15卷 / 01期

基金：

中国国家自然科学基金;

关键词：

LIQUID ELECTROLYTE; THERMAL RUNAWAY; HYDROGEN-BOND; ION BATTERY; ANODES; MODEL;

D O I：

10.1038/s41467-024-46186-y

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Constraining the electrochemical reactivity of free solvent molecules is pivotal for developing high-voltage lithium metal batteries, especially for ether solvents with high Li metal compatibility but low oxidation stability ( <4.0 V vs Li+/Li). The typical high concentration electrolyte approach relies on nearly saturated Li+ coordination to ether molecules, which is confronted with severe side reactions under high voltages ( >4.4 V) and extensive exothermic reactions between Li metal and reactive anions. Herein, we propose a molecular anchoring approach to restrict the interfacial reactivity of free ether solvents in diluted electrolytes. The hydrogen-bonding interactions from the anchoring solvent effectively suppress excessive ether side reactions and enhances the stability of nickel rich cathodes at 4.7 V, despite the extremely low Li+/ether molar ratio (1:9) and the absence of typical anion-derived interphase. Furthermore, the exothermic processes under thermal abuse conditions are mitigated due to the reduced reactivity of anions, which effectively postpones the battery thermal runaway.

引用

页数：12

共 61 条

[41] HYDROGEN-BONDING EFFECTS ON OXYGEN-17 CHEMICAL SHIFTS [J].