Volume 136, Issue 31 e202406122
Forschungsartikel

Upgrading Electrolyte Antioxidant Chemistry by Constructing Potential Scaling Relationship

Ruhong Li

Ruhong Li

State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou, 311215 China

These authors contributed equally to this paper.

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Zunchun Wu

Zunchun Wu

State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

These authors contributed equally to this paper.

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Shuoqing Zhang

Shuoqing Zhang

State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

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Jia Liu

Jia Liu

State Key Laboratory of Clean Energy Utilization, School of Energy Engineering, Zhejiang University, Hangzhou, 310027 China

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Liwu Fan

Liwu Fan

State Key Laboratory of Clean Energy Utilization, School of Energy Engineering, Zhejiang University, Hangzhou, 310027 China

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Tao Deng

Tao Deng

Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland, USA

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Lixin Chen

Lixin Chen

State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province, Hangzhou, 310013 China

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Xiulin Fan

Corresponding Author

Xiulin Fan

State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

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First published: 14 May 2024
Citations: 4

Abstract

Rational design of advanced electrolytes to improve the high-voltage capability has been attracting wide attention as one critical solution to enable next-generation high-energy-density batteries. However, the limited understanding of electrolyte antioxidant chemistry as well as the lack of valid quantization approaches have resulted in knowledge gap, which hinders the formulation of new electrolytes. Herein, we construct a standard curve based on representative solvation structures to quantify the oxidation stability of ether-based electrolytes, which reveals the linear correlation between the oxidation potential and the atomic charge of the least oxidation-resistant solvent. Dictated by the regularity between solvation composition and oxidation potential, a (Trifluoromethyl)cyclohexane-based localized high-concentration electrolyte dominated by anion-less solvation structures was designed to optimize the cycling performance of 4.5 V 30 μm-Li||3.8 mAh cm−2-LiCoO2 batteries, which maintained 80 % capacity retention even after 440 cycles. The consistency of experimental and computational results validates the proposed principles, offering a fundamental guideline to evaluate and design aggressive electrochemical systems.

Conflict of interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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