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Conventional polycrystalline NMCs, however, suffer from severe cracking along the grain boundaries of primary particles and capacity loss under high charge and\/or discharge rates, hindering their implementation in fast\u2010charging electric vehicular (EV) batteries. Single\u2010crystal (SC) NMCs are attractive alternatives as they eliminate intergranular cracking and allow for grain\u2010level surface optimization for fast Li transport. In the present study, the authors report synthetic approaches to produce SC LiNi<jats:sub>0.8<\/jats:sub>Co<jats:sub>0.1<\/jats:sub>Mn<jats:sub>0.1<\/jats:sub>O<jats:sub>2<\/jats:sub> (NMC811) samples with different morphologies: Oct\u2010SC811 with predominating (012)\u2010family surface and Poly\u2010SC811 with predominating (104)\u2010family surface. Poly\u2010SC811, representing the first experimentally synthesized NMC811 single crystals with (104) surface, delivers superior performance even at the ultra\u2010high rate of 6 C. Through detailed X\u2010ray analysis and electron microscopy characterization, it is shown that the enhanced performance originates from better chemical and structural stabilities, faster Li<jats:sup>+<\/jats:sup> diffusion kinetics, suppressed side reactions with electrolyte, and excellent cracking resistance. These insights provide important design guidelines in the future development of fast\u2010charging NMC\u2010type cathode materials.<\/jats:p>","DOI":"10.1002\/smll.202105833","type":"journal-article","created":{"date-parts":[[2022,1,21]],"date-time":"2022-01-21T10:00:51Z","timestamp":1642759251000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":70,"title":["Single\u2010Crystal LiNi<i><sub>x<\/sub><\/i>Mn<i><sub>y<\/sub><\/i>Co<sub>1\u2212<\/sub><i><sub>x<\/sub><\/i><sub>\u2212<\/sub><i><sub>y<\/sub><\/i>O<sub>2<\/sub> Cathodes for Extreme Fast Charging"],"prefix":"10.1002","volume":"18","author":[{"given":"Yanying","family":"Lu","sequence":"first","affiliation":[{"name":"Energy Storage and Distributed Resources Division Lawrence Berkeley National Laboratory  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tianyu","family":"Zhu","sequence":"additional","affiliation":[{"name":"Energy 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