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Research Article

Structural self-reconstruction strategy empowering Ni-rich layered cathodes with low-strain for superior cyclabilities

Zhouliang Tan1,2, Yunjiao Li1,2 ( ), Xiaoming Xi3, Shijie Jiang1,2, Xiaohui Li1,2, Xingjie Shen1,2, Panpan Zhang4, Zhenjiang He1,2
School of Metallurgy and Environment, Central South University, Changsha 410083, China
Engineering Research Center of the Ministry of Education for Advanced Battery Materials, Central South University, Changsha 410083, China
Changsha Research Institute of Mining and Metallurgy, Changsha 410083, China
Office of Laboratory and Equipment Management, Xinjiang University, Urumqi 830000, China
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Graphical Abstract

A perovskite Li0.35La0.55TiO3 (LLTO) layer is built on Ni-rich cathodes crystal to induce layered@spinel@perovskite heterostructure, which could effectively suppress the mechanical strain, cation mixing, and electrolyte corrosion. This work provides a new perspective of surface interface engineering for layered cathode materials.

Abstract

The key to hindering the commercial application of Ni-rich layered cathode is its severe structural and interface degradation during the undesired phase transition (hexagonal to hexagonal (H2 → H3)), degenerating from the build-up of mechanical strain and undesired parasitic reactions. Herein, a perovskite Li0.35La0.55TiO3 (LLTO) layer is built onto Ni-rich cathodes crystal to induce layered@spinel@perovskite heterostructure to solve the root cause of capacity fade. Intensive exploration based on structure characterizations, in situ X-ray diffraction techniques, and first-principles calculations demonstrate that such a unique heterostructure not only can improve the ability of the host structure to withstand the mechanical strain but also provides fast diffusion channels for lithium ions as well as provides a protective barrier against electrolyte corrosion. Impressively, the LLTO modified LiNi0.9Co0.05Mn0.05O2 cathode manifests an unexpected cyclability with an extremely high-capacity retention of ≈ 94.6% after 100 cycles, which is superior to the pristine LiNi0.9Co0.05Mn0.05O2 (79.8%). Furthermore, this modified electrode also shows significantly enhanced cycling stability even withstanding a high cut-off voltage of 4.6 V. This surface self-reconstruction strategy provides deep insight into the structure/interface engineering to synergistically stabilize structure stability and regulate the physicochemical properties of Ni-rich cathodes, which will also unlock a new perspective of surface interface engineering for layered cathode materials.

Keywords

Ni-rich layered oxides cathodestructural self-reconstructionphase transitionmechanical strainfirst-principal calculation

Electronic Supplementary Material

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Nano Research
Volume 16 Issue 4,
April 2023
Pages 4950-4960
DOI: 10.1007/s12274-022-5161-1
Cite this article:
Tan Z, Li Y, Xi X, et al. Structural self-reconstruction strategy empowering Ni-rich layered cathodes with low-strain for superior cyclabilities. Nano Research, 2023, 16(4): 4950-4960. https://doi.org/10.1007/s12274-022-5161-1
Topics:
Lithium batteries

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Received: 27 August 2022
Revised: 21 September 2022
Accepted: 06 October 2022
Published: 29 November 2022
© Tsinghua University Press 2022
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