Operando real-space imaging of a structural phase transformation in the high-voltage electrode Li<sub>x</sub>Ni<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub>.

Sun, Yifei; Hy, Sunny; Hua, Nelson; Wingert, James; Harder, Ross; Meng, Ying Shirley; Shpyrko, Oleg; Singer, Andrej · Nat Commun · 2024

basic_science · Level V

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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 Li<sub>x</sub>Ni<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> 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.