Revisiting Dipole-Induced Fluorinated-Anion Decomposition Reaction for Promoting a LiF-Rich Interphase in Lithium-Metal Batteries  

作　　者：Liu Wang Jiahui Guo Qi Qi Xiaotong Li Yuanmeng Ge Haoyi Li Yunfeng Chao Jiang Du Xinwei Cui 

机构地区：[1]Henan Institutes of Advanced Technology,Zhengzhou University,Zhengzhou 450003,People’s Republic of China [2]College of Materials Science and Engineering,Zhengzhou University,Zhengzhou 450001,People’s Republic of China [3]State Key Laboratory of Coking Coal Resources Green Exploitation,Zhengzhou University,Zhengzhou 450001,People’s Republic of China

出　　处：《Nano-Micro Letters》2025年第5期263-280,共18页纳微快报(英文版)

基　　金：the financial support from the National Natural Science Foundation of China(Nos.52272242,52174387,and 52403339);Key Research and Development Program of Henan Province(No.231111240600)。

摘　　要：Building anion-derived solid electrolyte interphase(SEI)with enriched LiF is considered the most promising strategy to address inferior safety features and poor cyclability of lithium-metal batteries(LMBs).Herein,we discover that,instead of direct electron transfer from surface polar groups to bis(trifluoromethanesulfonyl)imide(TFSI-)for inducing a LiF-rich SEI,the dipole-induced fluorinated-anion decomposition reaction begins with the adsorption of Li ions and is highly dependent on their mobility on the polar surface.To demonstrate this,a single-layer graphdiyne on MXene(sGDY@MXene)heterostructure has been successfully fabricated and integrated into polypropylene separators.It is found that the adsorbed Li ions connect electron-donating sGDY@MXene to TFSI-,facilitating interfacial charge transfer for TFSI-decomposition.However,this does not capture the entire picture.The sGDY@MXene also renders the adsorbed Li ions with high mobility,enabling them to reach optimal reaction sites and expedite their coordination processes with O on O=S=O and F on the broken–CF_3~-,facilitating bond cleavage.In contrast,immobilized Li ions on the more lithiophilic pristine MXene retard these cleavage processes.Consequently,the decomposition reaction is accelerated on [e-mail] work highlights the dedicate balance between lithiophilicity and Li-ion mobility in effectively promoting a LiF-rich SEI for the long-term stability of LMBs.

关 键 词：LiF-rich SEI Li-ion mobility Lithiophilicity MXene Graphdiyne 

分 类 号：TM912[电气工程—电力电子与电力传动] TB383.2[一般工业技术—材料科学与工程] O646[理学—物理化学]