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The prevailing O<jats:sub>3<\/jats:sub> phase LiCoO<jats:sub>2<\/jats:sub> adopts the ABCABC (A, B, and C stand for lattice sites in the close\u2010packed plane) stacking modes of close\u2010packed oxygen atoms. Currently, the focus of LiCoO<jats:sub>2<\/jats:sub> development is application at high voltage (&gt;4.55\u2009V versus Li<jats:sup>+<\/jats:sup>\/Li) to achieve a high specific capacity (&gt;190\u2009mAh\u2009g<jats:sup>\u22121<\/jats:sup>). However, cycled with a high cutoff voltage, O<jats:sub>3<\/jats:sub>\u2013LiCoO<jats:sub>2<\/jats:sub> suffers from rapid capacity decay. The causes of failure are mostly attributed to the irreversible transitions to H1\u20103\/O<jats:sub>1<\/jats:sub> phase after deep delithiation and severe interfacial reactions with electrolytes. In addition to O<jats:sub>3<\/jats:sub>, LiCoO<jats:sub>2<\/jats:sub> is also known to crystalize in an O<jats:sub>2<\/jats:sub> phase with ABAC stacking. Since its discovery, little is known about the high\u2010voltage behavior of O<jats:sub>2<\/jats:sub>\u2013LiCoO<jats:sub>2<\/jats:sub>. Herein, through systematic comparison between electrochemical performances of O<jats:sub>3<\/jats:sub> and O<jats:sub>2<\/jats:sub> LiCoO<jats:sub>2<\/jats:sub> at high voltage, the significantly better stability of O<jats:sub>2<\/jats:sub>\u2013LiCoO<jats:sub>2<\/jats:sub> (&gt;4.5\u2009V) than that of O<jats:sub>3<\/jats:sub>\u2013LiCoO<jats:sub>2<\/jats:sub> in the same micro\u2010sized particle morphology is revealed. Combining various characterization techniques and multiscale simulation, the outstanding high\u2010voltage stability of O<jats:sub>2<\/jats:sub>\u2013LiCoO<jats:sub>2<\/jats:sub> is attributed to the high Li diffusivity and ideal mechanical properties. Uniform Li<jats:sup>+<\/jats:sup> distribution and balanced internal stress loading may hold the key to improving the high\u2010voltage performance of LiCoO<jats:sub>2<\/jats:sub>.<\/jats:p>","DOI":"10.1002\/smsc.202400162","type":"journal-article","created":{"date-parts":[[2024,8,2]],"date-time":"2024-08-02T06:55:05Z","timestamp":1722581705000},"source":"Crossref","is-referenced-by-count":23,"title":["On the Much\u2010Improved High\u2010Voltage Cycling Performance of LiCoO<sub>2<\/sub> by Phase Alteration from O<sub>3<\/sub> to O<sub>2<\/sub> Structure"],"prefix":"10.1002","author":[{"given":"Mingwei","family":"Zan","sequence":"first","affiliation":[{"name":"Beijing Frontier Research Center on Clean Energy Institute of Physics Chinese Academy of Sciences  Beijing 100190 China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing 100049 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