Issue 44, 2021

The solvation structure, transport properties and reduction behavior of carbonate-based electrolytes of lithium-ion batteries

Abstract

Despite the extensive employment of binary/ternary mixed-carbonate electrolytes (MCEs) for Li-ion batteries, the role of each ingredient with regards to the solvation structure, transport properties, and reduction behavior is not fully understood. Herein, we report the atomistic modeling and transport property measurements of the Gen2 (1.2 M LiPF6 in ethylene carbonate (EC) and ethyl methyl carbonate (EMC)) and EC-base (1.2 M LiPF6 in EC) electrolytes, as well as their mixtures with 10 mol% fluoroethylene carbonate (FEC). Due to the mixing of cyclic and linear carbonates, the Gen2 electrolyte is found to have a 60% lower ion dissociation rate and a 44% faster Li+ self-diffusion rate than the EC-base electrolyte, while the total ionic conductivities are similar. Moreover, we propose for the first time the anion–solvent exchange mechanism in MCEs with identified energetic and electrostatic origins. For electrolytes with additive, up to 25% FEC coordinates with Li+, which exhibits a preferential reduction that helps passivate the anode and facilitates an improved solid electrolyte interphase. The work provides a coherent computational framework for evaluating mixed electrolyte systems.

Graphical abstract: The solvation structure, transport properties and reduction behavior of carbonate-based electrolytes of lithium-ion batteries

Supplementary files

Article information

Article type
Edge Article
Submitted
03 Aug 2021
Accepted
16 Sep 2021
First published
17 Sep 2021
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2021,12, 14740-14751

The solvation structure, transport properties and reduction behavior of carbonate-based electrolytes of lithium-ion batteries

T. Hou, K. D. Fong, J. Wang and K. A. Persson, Chem. Sci., 2021, 12, 14740 DOI: 10.1039/D1SC04265C

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