Volume 136, Issue 6 e202316790
Forschungsartikel

Manipulated Fluoro-Ether Derived Nucleophilic Decomposition Products for Mitigating Polarization-Induced Capacity Loss in Li-Rich Layered Cathode

Baodan Zhang

Baodan Zhang

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

Fujian Science & Technology Innovation Laboratory for Energy Materials of China (Tan Kah Kee Innovation Laboratory), Xiamen, 361005 P. R. China

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Haitang Zhang

Haitang Zhang

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

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Haiyan Luo

Haiyan Luo

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

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Haiming Hua

Haiming Hua

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

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Xiaohong Wu

Xiaohong Wu

Fujian Provincial Key Laboratory of Functional Materials and Applications, Institute of Advanced Energy Materials, School of Materials Science and Engineering, Xiamen University of Technology, Xiamen, 361024 P. R. China

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Yilong Chen

Yilong Chen

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

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Shiyuan Zhou

Shiyuan Zhou

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

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Jianhua Yin

Jianhua Yin

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

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Kang Zhang

Kang Zhang

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

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Hong-Gang Liao

Hong-Gang Liao

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

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Qingsong Wang

Qingsong Wang

Bavarian Center for Battery Technology (BayBatt), Department of Chemistry, University of Bayreuth, 95447 Bayreuth, Germany

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Yeguo Zou

Corresponding Author

Yeguo Zou

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

Fujian Science & Technology Innovation Laboratory for Energy Materials of China (Tan Kah Kee Innovation Laboratory), Xiamen, 361005 P. R. China

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Yu Qiao

Corresponding Author

Yu Qiao

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

Fujian Science & Technology Innovation Laboratory for Energy Materials of China (Tan Kah Kee Innovation Laboratory), Xiamen, 361005 P. R. China

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Shi-Gang Sun

Shi-Gang Sun

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 P. R. China

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First published: 20 December 2023

Abstract

Electrolyte engineering is a fascinating choice to improve the performance of Li-rich layered oxide cathodes (LRLO) for high-energy lithium-ion batteries. However, many existing electrolyte designs and adjustment principles tend to overlook the unique challenges posed by LRLO, particularly the nucleophilic attack. Here, we introduce an electrolyte modification by locally replacing carbonate solvents in traditional electrolytes with a fluoro-ether. By benefit of the decomposition of fluoro-ether under nucleophilic O-related attacks, which delivers an excellent passivation layer with LiF and polymers, possessing rigidity and flexibility on the LRLO surface. More importantly, the fluoro-ether acts as “sutures”, ensuring the integrity and stability of both interfacial and bulk structures, which contributed to suppressing severe polarization and enhancing the cycling capacity retention from 39 % to 78 % after 300 cycles for the 4.8 V-class LRLO. This key electrolyte strategy with comprehensive analysis, provides new insights into addressing nucleophilic challenge for high-energy anionic redox related cathode systems.

Conflict of interest

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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