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Mechanistic dichotomies in redox reactions of mononuclear metal-oxygen intermediates

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dc.contributor.authorFukuzumi, Shunichi-
dc.contributor.authorCho, Kyung-Bin-
dc.contributor.authorLee, Yong-Min-
dc.contributor.authorHong, Seungwoo-
dc.contributor.authorNam, Wonwoo-
dc.date.available2021-02-22T04:57:21Z-
dc.date.issued2020-12-
dc.identifier.issn0306-0012-
dc.identifier.issn1460-4744-
dc.identifier.urihttps://scholarworks.sookmyung.ac.kr/handle/2020.sw.sookmyung/1008-
dc.description.abstractThere are mechanistic dichotomies with regard to the formation, electronic structures and reaction mechanisms of metal-oxygen intermediates, since these metal-oxygen species could be composed of different resonance structures or canonical structures of the oxidation states of metals and ligands, which may undergo different reaction pathways. Even the same metal-oxygen intermediates, such as metal-oxo species, may undergo an electron-transfer pathway or a direct hydrogen or oxygen atom transfer pathway depending on the one-electron redox potentials of metal-oxo species and substrates. Electron-transfer pathways are also classified into two mechanisms, such as outer-sphere and inner-sphere pathways. The one-electron redox potentials of metal-oxygen species and substrates are also shifted because of the binding of acids, which can result from either hydrogen bonding or protonation. There are a rebound pathway and a non-rebound pathway following the initial electron transfer or hydrogen atom transfer step to produce hydroxylated products, depending on the one-electron redox potentials of metal-oxo species and substrates. Nucleophilic reactions can be switched to electrophilic pathways, depending on reaction conditions such as reaction temperature. Spin states of metal-oxygen intermediates are also an important factor that controls the redox reactivity of oxidants in oxidation reactions. Here, we review such various mechanistic dichotomies in redox reactions of metal-oxygen intermediates with the emphasis on understanding and controlling the redox reactivity of metal-oxygen intermediates from experimental and theoretical points of view.-
dc.format.extent40-
dc.language영어-
dc.language.isoENG-
dc.publisherROYAL SOC CHEMISTRY-
dc.titleMechanistic dichotomies in redox reactions of mononuclear metal-oxygen intermediates-
dc.typeArticle-
dc.publisher.location영국-
dc.identifier.doi10.1039/d0cs01251c-
dc.identifier.scopusid2-s2.0-85097888440-
dc.identifier.wosid000598713800005-
dc.identifier.bibliographicCitationCHEMICAL SOCIETY REVIEWS, v.49, no.24, pp 8988 - 9027-
dc.citation.titleCHEMICAL SOCIETY REVIEWS-
dc.citation.volume49-
dc.citation.number24-
dc.citation.startPage8988-
dc.citation.endPage9027-
dc.type.docTypeReview-
dc.description.isOpenAccessN-
dc.description.journalRegisteredClassscie-
dc.description.journalRegisteredClassscopus-
dc.relation.journalResearchAreaChemistry-
dc.relation.journalWebOfScienceCategoryChemistry, Multidisciplinary-
dc.subject.keywordPlusO-O BOND-
dc.subject.keywordPlusCOUPLED ELECTRON-TRANSFER-
dc.subject.keywordPlusC-H ACTIVATION-
dc.subject.keywordPlusHIGH-VALENT IRON-
dc.subject.keywordPlusNONHEME IRON(IV)-OXO COMPLEX-
dc.subject.keywordPlusALPHA-HYDROXYLATING MONOOXYGENASE-
dc.subject.keywordPlusHIGH-SPIN IRON(III)-ALKYLPEROXO-
dc.subject.keywordPlusOXIDATIVE ADDITION-REACTION-
dc.subject.keywordPlusCOPPER-DIOXYGEN ADDUCT-
dc.subject.keywordPlusHYDROGEN-ATOM TRANSFER-
dc.identifier.urlhttps://pubs.rsc.org/en/content/articlelanding/2020/CS/D0CS01251C#!divAbstract-
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