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

Linze Li, Bin Ouyang (), Zhengyan Lun, Haoyan Huo, Dongchang Chen, Yuan Yue, Colin Ophus, Wei Tong, Guoying Chen, Gerbrand Ceder () and Chongmin Wang ()
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Linze Li: Pacific Northwest National Laboratory
Bin Ouyang: University of California – Berkeley
Zhengyan Lun: University of California – Berkeley
Haoyan Huo: University of California – Berkeley
Dongchang Chen: Lawrence Berkeley National Laboratory
Yuan Yue: Lawrence Berkeley National Laboratory
Colin Ophus: Molecular Foundry, Lawrence Berkeley National Laboratory
Wei Tong: Lawrence Berkeley National Laboratory
Guoying Chen: Lawrence Berkeley National Laboratory
Gerbrand Ceder: University of California – Berkeley
Chongmin Wang: Pacific Northwest National Laboratory

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-43356-2

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