Operando real-space imaging of a structural phase transformation in the high-voltage electrode LixNi0.5Mn1.5O4

Yifei Sun, Sunny Hy, Nelson Hua, James Wingert, Ross Harder, Ying Shirley Meng, Oleg Shpyrko and Andrej Singer ()
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Yifei Sun: Cornell University
Sunny Hy: University of California San Diego
Nelson Hua: University of California San Diego
James Wingert: University of California San Diego
Ross Harder: Argonne National Laboratory
Ying Shirley Meng: University of California San Diego
Oleg Shpyrko: University of California San Diego
Andrej Singer: Cornell University

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract Discontinuous solid-solid phase transformations play a pivotal role in determining the properties of rechargeable battery electrodes. By leveraging operando Bragg Coherent Diffractive Imaging (BCDI), we investigate the discontinuous phase transformation in LixNi0.5Mn1.5O4 within an operational Li metal coin cell. Throughout Li-intercalation, we directly observe the nucleation and growth of the Li-rich phase within the initially charged Li-poor phase in a 500 nm particle. Supported by the microelasticity model, the operando imaging unveils an evolution from a curved coherent to a planar semi-coherent interface driven by dislocation dynamics. Our data indicates negligible kinetic limitations from interface propagation impacting the transformation kinetics, even at a discharge rate of C/2 (80 mA/g). This study highlights BCDI’s capability to decode complex operando diffraction data, offering exciting opportunities to study nanoscale phase transformations with various stimuli.

Date: 2024
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DOI: 10.1038/s41467-024-55010-6

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