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A novel calculation strategy for optimized prediction of the reduction of electrochemical window at anode |
| Guochen Sun(孙国宸)1,2, Jian Gao(高健)3,†, and Hong Li(李泓)1,‡ |
1 Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China;
2 College of Materials Sciences and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China;
3 College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China |
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Abstract The reduction of the electrochemical window (EW) of electrolytes plays a significant role in assessing their compatibility with the anode in lithium-ion batteries. However, the accurate calculation of the reduction of EW is still challenging due to missing the solvation effects, condensation effects, kinetic factors, and the passivation on anodes. The theoretical prediction of the intrinsic and apparent EW is confirmed by a comprehensive experimental analysis of ethylene carbonate-dimethyl carbonate (EC-DMC) electrolytes, combining linear sweep voltammetry (LSV) and gas chromatography-mass spectrometry (GC-MS). The proposed novel kinetic normal distribution theory model can quantitatively explain the current density from LSV and affirm acetaldehyde (MeCHO) as one of the primary reduction products of EC. The solvent effect restricts the intrinsic EW of EC-DMC without lithium salt to 2.6 V (vs. Li+/Li) arising from the Marcus-Gerischer theory and the passivation of MeCHO on the anode broadens the apparent EW to 0.3 V (vs. Li+/Li) arising from the normal distribution of the lowest unoccupied molecular orbital (LUMO) for MeCHO produced by thermal motion. In addition, the passivation on the anode depends intensively on the lithium salt, resulting in more complicated influences on the apparent EW.
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Received: 20 March 2023
Revised: 13 April 2023
Accepted manuscript online: 16 April 2023
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PACS:
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82.47.Aa
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(Lithium-ion batteries)
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82.45.Gj
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(Electrolytes)
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65.40.gk
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(Electrochemical properties)
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87.15.R-
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(Reactions and kinetics)
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| Fund: Project supported by the National Natural Science Foundation of China (Grant Nos. U1964205 and 22109005), the National Key Research and Development Program of China (Grant No. 2016YFB0100100), and Beijing Municipal Science & Technology Commission, China (Grant No. Z191100004719001). |
Corresponding Authors:
Jian Gao, Hong Li
E-mail: gaojian@mail.buct.edu.cn;hli@iphy.ac.cn
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Cite this article:
Guochen Sun(孙国宸), Jian Gao(高健), and Hong Li(李泓) A novel calculation strategy for optimized prediction of the reduction of electrochemical window at anode 2023 Chin. Phys. B 32 078201
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