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High-entropy oxides (HEOs) are a new class of emerging materials with fascinating properties (such as structural stability, tensile strength, and corrosion resistance). High-entropy oxide coated Ni-rich cathode materials have great potential to improve the electrochemical performance. Here, we present a facile self-ball milling method to obtain (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 (HEO) coated LiNi0.8Co0.1Mn0.1O2 (NCM811). The HEO coating endows NCM811 with a stable surface, reduces the contact with the external environment (air and electrolyte), and inhibits side reactions between cathode and electrolyte. These favorable effects, especially when the coating amount is 5 wt%, result in a significant reduction of the battery polarization and an increase in the capacity retention from 57.3% (NCM811) to 74.2% (5HEO-NCM811) after 300 cycles at 1 C (1 C = 200 mA·h·g-1). Moreover, the morphology and spectroscopy analysis after the cycles confirmed the inhibitory effect of the HEO coating on electrolyte decomposition, which is important for the cycle life. Surprisingly, HEO coating reduces the viscosity of slurry by 37%-38% and significantly improves the flowability of the slurry with high solid content. This strategy confirms the feasibility of HEO-modified Ni-rich cathode materials and provides a new idea for the design of high-performance cathode materials for Li-ion batteries.


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Self-ball milling strategy to construct high-entropy oxide coated LiNi0.8Co0.1Mn0.1O2 with enhanced electrochemical performance

Show Author's information Kai YUANaTianzhe TUbChao SHENa,c( )Lin ZHOUbJixuan LIUb( )Jing LIdKeyu XIEa,cGuojun ZHANGb
State Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi’an 710072, China
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Institute of Functional Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China
Research & Development Institute of Northwestern Polytechnical University in Shenzhen, Northwestern Polytechnical University, Shenzhen 518057, China
State Key Laboratory of Environment-friendly Energy Materials, School of Materials Science and Engineering, Southwest University of Science and Technology, Mianyang 621010, China

Abstract

High-entropy oxides (HEOs) are a new class of emerging materials with fascinating properties (such as structural stability, tensile strength, and corrosion resistance). High-entropy oxide coated Ni-rich cathode materials have great potential to improve the electrochemical performance. Here, we present a facile self-ball milling method to obtain (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 (HEO) coated LiNi0.8Co0.1Mn0.1O2 (NCM811). The HEO coating endows NCM811 with a stable surface, reduces the contact with the external environment (air and electrolyte), and inhibits side reactions between cathode and electrolyte. These favorable effects, especially when the coating amount is 5 wt%, result in a significant reduction of the battery polarization and an increase in the capacity retention from 57.3% (NCM811) to 74.2% (5HEO-NCM811) after 300 cycles at 1 C (1 C = 200 mA·h·g-1). Moreover, the morphology and spectroscopy analysis after the cycles confirmed the inhibitory effect of the HEO coating on electrolyte decomposition, which is important for the cycle life. Surprisingly, HEO coating reduces the viscosity of slurry by 37%-38% and significantly improves the flowability of the slurry with high solid content. This strategy confirms the feasibility of HEO-modified Ni-rich cathode materials and provides a new idea for the design of high-performance cathode materials for Li-ion batteries.

Keywords: high-entropy oxides (HEOs), Li-ion battery (LIB), Ni-rich cathode, coating modification

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Publication history

Received: 25 November 2021
Revised: 26 January 2022
Accepted: 19 February 2022
Published: 11 May 2022
Issue date: June 2022

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© The Author(s) 2022.

Acknowledgements

The authors acknowledge the financial support provided by the Science, Technology, and Innovation Commission of Shenzhen Municipality (JCYJ20180508151856806), the Key R&D Program of Shaanxi (2019ZDLGY04-05), the National Natural Science Foundation of Shaanxi Province (2019JLZ-01), and the Fundamental Research Funds for the Central Universities (19GH020302, 3102019JC005, 3102021ZD0401, and 3102021TS0406).

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