Early View e202400501
Research Article

Acid Etching-Driven Self-Assembly of Mn-Shell Inducing Rock-Salt Phase for Enhanced Single-Crystal Ni-Rich Cathodes

Xiaotu Ma

Xiaotu Ma

Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA, 01609 USA

Contribution: Conceptualization (equal), Data curation (lead), Formal analysis (lead), ​Investigation (lead), Methodology (equal), Writing - original draft (lead), Writing - review & editing (supporting)

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Zifei Meng

Zifei Meng

Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA, 01609 USA

Contribution: Formal analysis (supporting), ​Investigation (supporting), Methodology (supporting), Writing - review & editing (supporting)

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Jiahui Hou

Jiahui Hou

Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA, 01609 USA

Contribution: Formal analysis (supporting), ​Investigation (supporting), Methodology (supporting), Writing - review & editing (supporting)

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Zeyi Yao

Zeyi Yao

Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA, 01609 USA

Contribution: ​Investigation (supporting), Methodology (supporting), Writing - review & editing (supporting)

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Zexin Wang

Zexin Wang

Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA, 01609 USA

Contribution: ​Investigation (supporting), Methodology (supporting), Writing - review & editing (supporting)

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Fulya Dogan

Fulya Dogan

Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S Cass Ave, Lemont, IL, 60439 USA

Contribution: ​Investigation (supporting), Methodology (supporting), Writing - review & editing (supporting)

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Zhenzhen Yang

Zhenzhen Yang

Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S Cass Ave, Lemont, IL, 60439 USA

Contribution: ​Investigation (supporting), Methodology (supporting), Writing - review & editing (supporting)

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Maksim Sultanov

Maksim Sultanov

Center for Nanoscale Materials, Argonne National Laboratory, 9700 S Cass Ave, Lemont, IL, 60439 USA

Northern Illinois University, Department of Physics, 1425 W. Lincoln Hwy, DeKalb, IL 60115

Contribution: ​Investigation (supporting), Methodology (supporting), Writing - review & editing (supporting)

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Guanhui Gao

Guanhui Gao

Department of Materials Science and Nanoengineering, Rice University, 6100 Main St, Houston, TX, 77005 USA

Contribution: ​Investigation (supporting), Methodology (supporting), Writing - review & editing (supporting)

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Hua Guo

Hua Guo

Department of Materials Science and Nanoengineering, Rice University, 6100 Main St, Houston, TX, 77005 USA

Contribution: ​Investigation (supporting), Methodology (supporting), Writing - review & editing (supporting)

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Yimo Han

Yimo Han

Department of Materials Science and Nanoengineering, Rice University, 6100 Main St, Houston, TX, 77005 USA

Contribution: ​Investigation (supporting), Methodology (supporting), Writing - review & editing (supporting)

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Jianguo Wen

Jianguo Wen

Center for Nanoscale Materials, Argonne National Laboratory, 9700 S Cass Ave, Lemont, IL, 60439 USA

Contribution: Formal analysis (supporting)

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Yan Wang

Corresponding Author

Yan Wang

Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA, 01609 USA

Contribution: Conceptualization (equal), Formal analysis (supporting), Funding acquisition (lead), ​Investigation (supporting), Methodology (equal), Project administration (lead), Resources (lead), Supervision (lead), Validation (lead), Writing - review & editing (equal)

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First published: 28 September 2024

Graphical Abstract

Single crystal 83Ni with a manganese-rich shell, achieved through the etching of polycrystalline particles, demonstrates significantly enhanced electrochemical properties when compared to various other counterparts. This advancement is expected to substantially drive progress in the development and manufacturing of cathodes, offering improved performance and efficiency in battery technologies.

Abstract

With the wide adoption of Li-ion batteries, Ni-rich cathode is considered as one of the most promising candidates of cathodes due to its high energy density and low cost. However, stability decreased with increasing Ni content in the Ni-rich cathode. To solve this bottleneck, many strategies, such as coating, doping, surface modification, and special morphologies, have been developed. Herein, we introduce a groundbreaking approach for enhancing Ni-rich cathode through an innovative acid etching process that promotes Mn shell self-assembly, inducing a rock-salt phase on the surface. This method not only simplifies the Ni-rich cathode modification process, but also significantly improves the structural stability and electrochemical performance of Ni-rich cathode. Our findings demonstrate that developed single-crystal Ni-rich cathode shows 3–34 % better stability compared to both commercial modified Ni-rich cathode and unmodified counterparts. The unique Mn shell effectively mitigates reversible phase shifts during cycling, contributing to a remarkable enhancement in cycling stability. This novel fabrication technique paves the way for cost-effective production of high-performance cathode materials, offering substantial benefits for lithium-ion battery technology. And this study proves the potential of this method in advancing the design and development of durable, high-capacity cathode materials for next-generation batteries.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available on request from the corresponding author. The data are not publicly available due to privacy or ethical restrictions.