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Tuning Reaction Kinetics of Fluorinated Molecules to Construct Robust Solid Electrolyte Interphases on SiOx Anode.

Created on 21 Sep 2024

Authors

Shiming Chen, Zhikang Deng, Jiangxiao Li, Wenguang Zhao, Bowen Nan, Yue Zuo, Jianjun Fang, Yuxiang Huang, Zu-Wei Yin, Feng Pan, Luyi Yang

Published in

Angewandte Chemie (International ed. in English). Pages e202413927. Sep 20, 2024. Epub Sep 20, 2024.

Abstract

Introducing fluorinated electrolyte additives to construct LiF-rich solid-electrolyte interphase (SEI) on Si-based anodes is proven an effective strategy for coping with its massive volume changes during cycling. However, most current research on fluorine-containing additives focuses on their thermodynamics of decomposition, lacking studies on the correlation between the molecular structure of additives and their decomposition kinetics. Herein, two fluorinated ester additives, diethyl fluoromalonate (F1DEM) and diethyl 2,2-difluoromalonate (F2DEM) were designed and synthesized. Through combining a wealth of characterizations and simulations, it is revealed that despite the similar reduction thermodynamics, the favorable reduction kinetics of single-fluorinated F1DEM facilitate a LiF-rich layer during the early stage of SEI formation, contributing to the formation of a more robust SEI on SiOx anode compared to the difluorinated F2DEM. Consequently, the proposed additive achieves excellent cycling stability (84 % capacity retention after 1000 cycles) for 5 Ah 21700 cylindrical batteries under practical testing conditions. By unveiling the role of reaction kinetics, a long-overlooked aspect for the study of electrolyte additives, this work sheds light on how to construct a stable SEI on Si-based anodes.

PMID:
39304910
Bibliographic data and abstract were imported from PubMed on 21 Sep 2024.

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