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It is shown that this is not necessary for Mn\u2010rich DRX\u2010cathodes demonstrated by Li<jats:sub>1.05<\/jats:sub>Mn<jats:sub>0.90<\/jats:sub>Nb<jats:sub>0.05<\/jats:sub>O<jats:sub>2<\/jats:sub> and Li<jats:sub>1.20<\/jats:sub>Mn<jats:sub>0.60<\/jats:sub>Nb<jats:sub>0.20<\/jats:sub>O<jats:sub>2<\/jats:sub>, which both deliver high capacity (&gt;250 mAh g<jats:sup>\u22121<\/jats:sup>) regardless of their Li\u2010excess level. By contextualizing this finding within the broader space of DRX chemistries and confirming with first\u2010principles calculations, it is revealed that the percolation effect is not crucial at the nanoparticle scale. Instead, Li\u2010excess is necessary to lower the charging voltage (through the formation of condensed oxygen species upon oxygen oxidation) of certain DRX cathodes, which otherwise would experience difficulties in charging due to their very high TM\u2010redox potential. The findings reveal the dual roles of Li\u2010excess \u2013 modifying the cathode voltage in addition to promoting Li diffusion through percolation \u2013 that must be simultaneously considered to determine the criticality of Li\u2010excess for high\u2010capacity DRX cathodes.<\/jats:p>","DOI":"10.1002\/aenm.202100204","type":"journal-article","created":{"date-parts":[[2021,5,5]],"date-time":"2021-05-05T13:59:08Z","timestamp":1620223148000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":71,"title":["Determining the Criticality of Li\u2010Excess for Disordered\u2010Rocksalt Li\u2010Ion Battery Cathodes"],"prefix":"10.1002","volume":"11","author":[{"given":"Jinhyuk","family":"Lee","sequence":"first","affiliation":[{"name":"Department of Nuclear Science and Engineering Massachusetts Institute of Technology  Cambridge MA 02139 USA"},{"name":"Department of Mining and Materials Engineering McGill University  Montreal QC H3A 0C5 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