Dipole–Dipole Interaction Induced Electrolyte Interfacial Model To Stabilize Antimony Anode for High-Safety Lithium-Ion Batteries

Qujiang Sun, Zhen Cao, Zheng Ma, Junli Zhang, Haoran Cheng, Xianrong Guo, Geon-Tae Park, Qian Li, Erqing Xie, Luigi Cavallo, Yang-Kook Sun, Jun Ming

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Electrolyte plays a vital role in determining battery performances, while the effect of solvent molecular interaction on electrode performances is not fully understood yet. Herein, we present an unrevealed dipole–dipole interaction to show the mechanism of solvent interaction effect on stabilizing the electrolyte for high electrode performances. As a paradigm, a new nonflammable triethyl phosphate (TEP)-based electrolyte is designed to stabilize the bulk alloying anode (e.g., Sb), where an interfacial model is constructed according to the solvation structure induced by the dipole–dipole interaction between TEP and the essential 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (HFE). We demonstrate that the Li+–solvent–anion complexes derived from different solvation structures exhibit different kinetic and electrochemical properties, contributing to varied Sb anode performances in different electrolytes. As a result, a high lithium storage capacity of 656 mAh g–1, robust rate capacities over 4 A g–1, and a long lifespan of more than 100 cycles are achieved, which are better than those reported before. This work presents a different insight into understanding electrolyte effects on electrode performances and provides a guideline for electrolyte design to stabilize alloying anodes and beyond in metal-ion batteries.
Original languageEnglish (US)
Pages (from-to)3545-3556
Number of pages12
JournalACS Energy Letters
StatePublished - Sep 26 2022

Bibliographical note

KAUST Repository Item: Exported on 2022-10-20
Acknowledgements: The authors greatly thank the National Natural Science Foundation of China (Grant 22122904) for funding support. This work is also supported by the National Natural Science Foundation of China (Grants 21978281, 11974150, and 22109155) and the Fundamental Research Funds for the Central Universities (Grant lzujbky-2021-pd10). The authors also thank the Bureau of International Cooperation Chinese Academy of Sciences, CAS-NST Joint Research Projects (Grant 121522KYSB20200047), and the Scientific and Technological Developing Project of Jilin Province (Grant YDZJ202101ZYTS022). The computational work was done on the KAUST supercomputer. This work was also supported by Hanyang University.


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