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Research Article

In-situ construction of a thermodynamically stabilized interface on the surface of single crystalline Ni-rich cathode materials via a one-step molten-salt route

Huiya Yang, Xiangbang Kong, Jiyang Li, Pengpeng Dai, Jing Zeng, Yang Yang( ), Jinbao Zhao( )
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Centre of Chemistry for Energy Materials, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, Engineering Research Center of Electrochemical Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
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A thermodynamically stabilized interface is constructed on the surface of single-crystalline Ni-rich cathode materials (SC811@RS) to suppress the generation of microcracks and interfacial parasitic side reactions simultaneously. Such a thermodynamically stable protective layer can not only prevent the direct contact between highly reactive LiNixCoyMn1−x−yO2 and electrolyte, but also mitigate deformation of structure caused by stress thus strengthening the mechanical properties.

Abstract

Nickel rich LiNixCoyMn1−x−yO2 cathode materials have been studied extensively to increase the energy density of lithium-ion batteries (LIBs) due to their advantages of high capacity and low cost. However, the anisotropic crystal expansion and contraction inside the secondary particles would cause detrimental micro-cracks and severe parasitic reactions at the electrode/electrolyte interface during cycling, which severely decreases the stability of crystalline structure and cathode-electrolyte interphase and ultimately affects the calendar life of batteries. Herein, a thermodynamically stabilized interface is constructed on the surface of single-crystalline Ni-rich cathode materials (SC811@RS) via a facile molten-salt route to suppress the generation of microcracks and interfacial parasitic side reactions simultaneously. Density functional theory calculations show that the formation energy of interface layer (−1.958 eV) is more negative than that of bulk layered structure (−1.421 eV). Such a thermodynamically stable protective layer can not only prevent the direct contact between highly reactive LiNixCoyMn1−x−yO2 and electrolyte, but also mitigate deformation of structure caused by stress thus strengthening the mechanical properties. Raman spectra further confirm the excellent structural reversibility and reaction homogeneity of SC811@RS at particle, electrode, and time scales. Consequently, SC811@RS cathode material delivers significantly improved cycling stability (high capacity retention of 92% after 200 cycles at 0.5 C) compared with polycrystalline LiNi0.8Co0.1Mn0.1O2 (82%).

Keywords

LiNixCoyMn1−x−yO2single crystallinepolycrystallinecathodelithium-ion battery

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Nano Research
Volume 16 Issue 5,
May 2023
Pages 6771-6779
DOI: 10.1007/s12274-022-4768-6
Cite this article:
Yang H, Kong X, Li J, et al. In-situ construction of a thermodynamically stabilized interface on the surface of single crystalline Ni-rich cathode materials via a one-step molten-salt route. Nano Research, 2023, 16(5): 6771-6779. https://doi.org/10.1007/s12274-022-4768-6
Topics:
Lithium batteries

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Received: 10 May 2022
Revised: 15 June 2022
Accepted: 13 July 2022
Published: 20 August 2022
© Tsinghua University Press 2022
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