Atomic-scale probing of short-range order and its impact on electrochemical properties in cation-disordered oxide cathodes

Li, Linze; Ouyang, Bin; Lun, Zhengyan; Huo, Haoyan; Chen, Dongchang; Yue, Yuan; Ophus, Colin; Tong, Wei; Chen, Guoying; Ceder, Gerbrand; Wang, Chongmin

doi:10.1038/s41467-023-43356-2

Title: Atomic-scale probing of short-range order and its impact on electrochemical properties in cation-disordered oxide cathodes

Journal Article · 17 November 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-43356-2 · OSTI ID:2216968

Li, Linze;

;

; Chen, Dongchang; Yue, Yuan;

;

; Ceder, Gerbrand;

Abstract Chemical short-range-order has been widely noticed to dictate the electrochemical properties of Li-excess cation-disordered rocksalt oxides, a class of cathode based on earth abundant elements for next-generation high-energy-density batteries. Existence of short-range-order is normally evidenced by a diffused intensity pattern in reciprocal space, however, derivation of local atomic arrangements of short-range-order in real space is hardly possible. Here, by a combination of aberration-corrected scanning transmission electron microscopy, electron diffraction, and cluster-expansion Monte Carlo simulations, we reveal the short-range-order is a convolution of three basic types: tetrahedron, octahedron, and cube. We discover that short-range-order directly correlates with Li percolation channels, which correspondingly affects Li transport behavior. We further demonstrate that short-range-order can be effectively manipulated by anion doping or post-synthesis thermal treatment, creating new avenues for tailoring the electrochemical properties. Our results provide fundamental insights for decoding the complex relationship between local chemical ordering and properties of crystalline compounds.

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Sponsoring Organization:: USDOE

OSTI ID:: 2216968

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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