4.7 Article

Fundamental understanding of high-capacity lithium-excess cathodes with disordered rock salt structure

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JOURNAL MATER SCI TECHNOL
DOI: 10.1016/j.jmst.2020.07.041

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Salt-rock structure; Hard/soft XAS; In-situ DSC; Structural evolution

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The study focuses on a high capacity cation-disordered positive electrode Li1.2Ni0.4Nb0.4O2 to investigate the intrinsic reaction mechanism, kinetics, thermal stability, and structural evolution of disordered rock-salt cathodes. By utilizing various techniques including XAS, XPS, DSC, GITT, CV, and XRD, comprehensive insights into the disordered rock-salt cathode are provided for designing new positive electrodes.
As a new class of lithium rich cathodes, disordered rock-salt cathodes have been of primary interest, because of their ability to deliver a promisingly high capacity up to 300 mA h/g. Nevertheless, some fundamental issues are yet to be fully understood and a comprehensive mastering of their solid-state chemistry, kinetics and thermal stability is required. Here, we select a high capacity cation-disordered positive electrode-Li1.2Ni0.4Nb0.4O2 as a model compound to study intrinsic reaction mechanism, including charge compensation mechanism, kinetics, thermal stability, and structural evolution. By combining soft and hard X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS) with operando and exsitu differential scanning calorimetry (DSC), galvanostatic intermittent titration technique (GITT), cyclic voltammetry (CV), and X-ray diffraction (XRD), we present holistic information on disordered rock-salt cathode. This work provides beneficial insights into designing and tailoring new positive electrodes with disordered rock-salt structure. (C) 2021 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.

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