Fast Interfacial Defluorination Kinetics Enables Stable Cycling of Low-Temperature Lithium Metal Batteries

Li, Xinpeng1; Li, Menghao2,3; Liu, Yue4; Jie, Yulin1; Li, Wanxia1; Chen, Yawei1; Huang, Fanyang1; Zhang, Yuchen1; Sohail, Tahir Muhammad1; Wang, Shiyang1; Zhu, Xingbao5; Cheng, Tao4; Gu, M. Danny2; Jiao, Shuhong1; Cao, Ruiguo1

2024-05-16

10.1021/jacs.3c14667

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY   影响因子和分区

0002-7863

1520-5126

The development of low-temperature lithium metal batteries (LMBs) encounters significant challenges because of severe dendritic lithium growth during the charging/discharging processes. To date, the precise origin of lithium dendrite formation still remains elusive due to the intricate interplay between the highly reactive lithium metal anode and organic electrolytes. Herein, we unveil the critical role of interfacial defluorination kinetics of localized high-concentration electrolytes (LHCEs) in regulating lithium dendrite formation, thereby determining the performance of low-temperature LMBs. We investigate the impact of solvation structures of LHCEs on low-temperature LMBs by employing tetrahydrofuran (THF) and 2-methyltetrahydrofuran (2-MeTHF) as comparative solvents. The combination of comprehensive characterizations and theoretical simulations reveals that the THF-based LHCE featured with a strong solvation strength exhibits fast interfacial defluorination reaction kinetics, thus leading to the formation of an amorphous and inorganic-rich solid-electrolyte interphase (SEI) that can effectively suppress the growth of lithium dendrites. As a result, the highly reversible Li metal anode achieves an exceptional Coulombic efficiency (CE) of up to similar to 99.63% at a low temperature of -30 degrees C, thereby enabling stable cycling of low-temperature LMB full cells. These findings underscore the crucial role of electrolyte interfacial reaction kinetics in shaping SEI formation and provide valuable insights into the fundamental understanding of electrolyte chemistry in LMBs.

SCI ; EI

英语

其他

National Natural Science Foundation of China[52225105] ; National Key Research and Development Program of China["2022YFA1504102","2022YFB2502200"] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDB0450302] ; National Natural Science Foundation of China["22279127","52072358","U21A2082","52273225","22173066","22303058"] ; Guangdong Fundamental Research Association[2022B1515120013] ; Guangdong scientific program[2019QN01L057] ; Natural Science Foundation of Jiangsu Province[BK20230475]

Chemistry

Chemistry, Multidisciplinary

WOS:001226075900001

AMER CHEMICAL SOC

Web of Science

1.Univ Sci & Technol China, Dept Mat Sci & Engn, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
2.Eastern Inst Adv Study, Eastern Inst Technol, Ningbo 315000, Peoples R China
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
4.Soochow Univ, Inst Funct Nano & Soft Mat FUNSOM, Suzhou 215123, Peoples R China
5.Got High Tech Co Ltd, Hefei 230026, Peoples R China

Li, Xinpeng,Li, Menghao,Liu, Yue,et al. Fast Interfacial Defluorination Kinetics Enables Stable Cycling of Low-Temperature Lithium Metal Batteries[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024,146(25).

Li, Xinpeng.,Li, Menghao.,Liu, Yue.,Jie, Yulin.,Li, Wanxia.,...&Cao, Ruiguo.(2024).Fast Interfacial Defluorination Kinetics Enables Stable Cycling of Low-Temperature Lithium Metal Batteries.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,146(25).

Li, Xinpeng,et al."Fast Interfacial Defluorination Kinetics Enables Stable Cycling of Low-Temperature Lithium Metal Batteries".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146.25(2024).