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dc.contributor.authorYu, Yang
dc.contributor.authorKarayaylali, Pinar
dc.contributor.authorSokaras, Dimosthenis
dc.contributor.authorGiordano, Livia
dc.contributor.authorKou, Ronghui
dc.contributor.authorSun, Cheng-Jun
dc.contributor.authorMaglia, Filippo
dc.contributor.authorJung, Roland
dc.contributor.authorGittleson, Forrest S.
dc.contributor.authorShao-Horn, Yang
dc.date.accessioned2021-09-29T17:26:59Z
dc.date.available2021-09-29T17:26:59Z
dc.date.issued2021-02
dc.date.submitted2020-12
dc.identifier.issn1754-5692
dc.identifier.issn1754-5706
dc.identifier.urihttps://hdl.handle.net/1721.1/132661
dc.description.abstractAnionic redox in positive electrode materials in Li-ion batteries provides an additional redox couple besides conventional metal redox, which can be harvested to further boost the energy density of current Li-ion batteries. However, the requirement for the reversible anionic redox activity remains under debate, hindering the rational design of new materials with reversible anionic redox. In this work, we employed differential electrochemical mass spectrometry (DEMS) to monitor the release of oxygen and to quantify the reversibility of the anionic redox of Li[subscript 2]Ru[subscript 0.75]M[subscript 0.25]O[subscript 3](M = Ti, Cr, Mn, Fe, Ru, Sn, Pt, Ir) upon first charge. X-ray absorption spectroscopy, coupled with density functional theory (DFT) calculations, show that various substituents have a minimal effect on the nominal metal redox, yet more ionic substituents and reduced metal–oxygen covalency introduce irreversible oxygen redox, accompanied with easier distortion of the M–O octahedron and a smaller barrier for forming an oxygen dimer within the octahedron. Therefore, a strong metal–oxygen covalency is needed to enhance the reversible oxygen redox. We proposed an electron–phonon-coupled descriptor for the reversibility of oxygen redox, laying the foundation for high-throughput screening of novel materials that enable reversible anionic redox activity.en_US
dc.publisherRoyal Society of Chemistry (RSC)en_US
dc.relation.isversionofhttp://dx.doi.org/10.1039/d0ee03765fen_US
dc.rightsCreative Commons Attribution Noncommercial 3.0 unported licenseen_US
dc.rights.urihttps://creativecommons.org/licenses/by-nc/3.0/en_US
dc.sourceRoyal Society of Chemistry (RSC)en_US
dc.titleTowards controlling the reversibility of anionic redox in transition metal oxides for high-energy Li-ion positive electrodesen_US
dc.typeArticleen_US
dc.identifier.citationYu, Yang et al. "Towards controlling the reversibility of anionic redox in transition metal oxides for high-energy Li-ion positive electrodes." Energy & Environmental Science 14, 4 (February 2021): 2322-2334. © 2021 The Royal Society of Chemistryen_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Materials Science and Engineeringen_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Mechanical Engineeringen_US
dc.contributor.departmentMassachusetts Institute of Technology. Research Laboratory of Electronicsen_US
dc.relation.journalEnergy & Environmental Scienceen_US
dc.type.urihttp://purl.org/eprint/type/JournalArticleen_US
eprint.statushttp://purl.org/eprint/status/PeerRevieweden_US
dspace.date.submission2021-04-09T12:03:27Z
mit.journal.volume14en_US
mit.journal.issue4en_US
mit.licensePUBLISHER_CC
mit.metadata.statusCompleteen_US


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