Breaking Solvation Dominance Effect Enabled by Ion-Dipole Interaction Toward Long-Spanlife Silicon Oxide Anodes in Lithium-Ion Batteries

Shengwei Dong; Lingfeng Shi; Shenglu Geng; Yanbin Ning; Cong Kang; Yan Zhang; Ziwei Liu; Jiaming Zhu; Zhuomin Qiang; Lin Zhou; Geping Yin; Dalong Li; Tiansheng Mu; Shuaifeng Lou

doi:10.1007/s40820-024-01592-1

Breaking Solvation Dominance Effect Enabled by Ion-Dipole Interaction Toward Long-Spanlife Silicon Oxide Anodes in Lithium-Ion Batteries

Nanomicro Lett. 2024 Dec 26;17(1):95. doi: 10.1007/s40820-024-01592-1.

Authors

Shengwei Dong¹, Lingfeng Shi¹, Shenglu Geng¹, Yanbin Ning¹, Cong Kang¹, Yan Zhang¹, Ziwei Liu¹, Jiaming Zhu¹, Zhuomin Qiang¹, Lin Zhou², Geping Yin¹, Dalong Li³, Tiansheng Mu⁴, Shuaifeng Lou^{5

6}

Affiliations

¹ State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, People's Republic of China.
² School of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai, 264200, People's Republic of China.
³ School of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai, 264200, People's Republic of China. lidalong@hit.edu.cn.
⁴ State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, People's Republic of China. mutiansheng@hit.edu.cn.
⁵ State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, People's Republic of China. shuaifeng.lou@hit.edu.cn.
⁶ Chongqing Research Institute of HIT, Chongqing, 401135, People's Republic of China. shuaifeng.lou@hit.edu.cn.

PMID: 39724233
DOI: 10.1007/s40820-024-01592-1

Abstract

Micrometer-sized silicon oxide (SiO) anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process. Herein, an innovative deep eutectic electrolyte derived from succinonitrile is introduced to enhance the cycling stability of SiO anodes. Density functional theory calculations validate a robust ion-dipole interaction between lithium ions (Li⁺) and succinonitrile (SN). The cosolvent fluoroethylene carbonate (FEC) optimizes the Li⁺ solvation structure in the SN-based electrolyte with its weakly solvating ability. Molecular dynamics simulations investigate the regulating mechanism of ion-dipole and cation-anion interaction. The unique Li⁺ solvation structure, enriched with FEC and TFSI^-, facilitates the formation of an inorganic-organic composite solid electrolyte interphase on SiO anodes. Micro-CT further detects the inhibiting effect on the SiO volume expansion. As a result, the SiO|LiCoO₂ full cells exhibit excellent electrochemical performance in deep eutectic-based electrolytes. This work presents an effective strategy for extending the cycle life of SiO anodes by designing a new SN-based deep eutectic electrolyte.

Keywords: Ion-dipole interaction; Lithium-ion batteries; Long-term cycling; Micrometer-sized silicon oxide.