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

作者：Xinpeng Li, Menghao Li, Yue Liu, Yulin Jie, Wanxia Li, Yawei Chen, Fanyang Huang, Yuchen Zhang, Tahir Muhammad Sohail, Shiyang Wang, Xingbao Zhu, Tao Cheng, Meng Gu, Shuhong Jiao, Ruiguo Cao · 发表于：Journal of the American Chemical Society · 年份：2024 · DOI：10.1021/jacs.3c14667 · 被引用次数：56 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Advanced Battery Technologies Research

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 ∼99.63% at a low temperature of -30 °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 ...