Oxidation decomposition mechanism of fluoroethylene carbonate-based electrolytes for high-voltage lithium ion batteries: a DFT calculation and experimental study

Xia, Lan and Tang, Bencan and Yao, Linbin and Wang, Kai and Cheris, Anastasia and Pan, Yueyang and Lee, Saixi and Xia, Yonggao and Chen, George Z. and Liu, Zhaoping (2017) Oxidation decomposition mechanism of fluoroethylene carbonate-based electrolytes for high-voltage lithium ion batteries: a DFT calculation and experimental study. ChemistrySelect, 2 (24). pp. 7353-7361. ISSN 2365-6549

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Abstract

The oxidative decomposition mechanism of fluoroethylene carbonate (FEC) used in high-voltage batteries is investigated by using density functional theory (DFT). Radical cation FEC•+ is formed from FEC by transferring one electron to electrode and the most likely decomposition products are CO2 and 2-fluoroacetaldehyde radical cation. Other possible products are CO, formaldehyde and formyl fluoride radical cations. These radical cations are surrounded by much FEC solvent and their radical center may attack the carbonyl carbon of FEC to form aldehyde and oligomers of alkyl carbonates, which is similar with the oxidative decomposition of EC. Then, our experimental result reveals that FEC-based electrolyte has rather high anodic stability. It can form a robust SEI film on the positive electrode surface, which can inhibit unwanted electrolyte solvent and LiPF6 salts decomposition, alleviate Mn/Ni dissolution and therefore, improve the coulombic efficiency and the cycling stability of high voltage LiNi0.5Mn1.5O4 positive electrodes. This work displays that FEC-based electrolyte systems have considerable potential replacement of the EC-based electrolyte for the applications in 5 V Li-ion batteries.

Item Type: Article
Additional Information: This is the peer reviewed version of the following article: L. Xia, B. Tang, L. Yao, K. Wang, A. Cheris, Y. Pan, S. Lee, Y. Xia, G. Z. Chen, Z. Liu, ChemistrySelect 2017, 2, 7353, which has been published in final form at http://dx.doi.org/10.1002/slct.201700938. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving.
Schools/Departments: University of Nottingham Ningbo China > Faculty of Science and Engineering > Department of Chemical and Environmental Engineering
University of Nottingham, UK > Faculty of Engineering > Department of Chemical and Environmental Engineering
Identification Number: 10.1002/slct.201700938
Depositing User: Eprints, Support
Date Deposited: 11 Sep 2017 08:55
Last Modified: 24 Nov 2017 12:37
URI: http://eprints.nottingham.ac.uk/id/eprint/45688

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