ArticleInorganic chemistry2013
Hydrogen-bonding effects on the reactivity of [X-Fe(III)-O-Fe(IV)═O] (X = OH, F) complexes toward C-H bond cleavage.
Article in Inorganic chemistry, 2013. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 17 papers.
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17 citing papers in PubMed.
- Enhanced Reactivities of Iron(IV)-Oxo Porphyrin Species in Oxidation Reactions Promoted by Intramolecular Hydrogen-Bonding.Advanced science (Weinheim, Baden-Wurttemberg, Germany) · 2024Article
- Electronic structure analysis of electrochemical COChemical science · 2022Article
- Electronic Structure and Reactivity of Dioxygen-Derived Aliphatic Thiolate-Ligated Fe-Peroxo and Fe(IV) Oxo Compounds.Journal of the American Chemical Society · 2022Article
- Explorations of the nonheme high-valent iron-oxo landscape: crystal structure of a synthetic complex with an [FeIV2(μ-O)Faraday discussions · 2022Article
- Peptidic Scaffolds Enable Rapid and Multivariate Secondary Sphere Evolution for an Abiotic Metallocatalyst.Inorganic chemistry · 2022Article
- Opening the CoJournal of the American Chemical Society · 2020Article
- Deciphering the origin of million-fold reactivity observed for the open core diiron [HO-FeChemical science · 2020Article
- Structure of a Ferryl Mimic in the Archetypal Iron(II)- and 2-(Oxo)-glutarate-Dependent Dioxygenase, TauD.Biochemistry · 2019Article
- Dioxygen Activation by Nonheme Diiron Enzymes: Diverse Dioxygen Adducts, High-Valent Intermediates, and Related Model Complexes.Chemical reviews · 2018Review
- Acid-facilitated product release from a Mo(IV) center: relevance to oxygen atom transfer reactivity of molybdenum oxotransferases.Journal of biological inorganic chemistry : JBIC : a publication of the Society of Biological Inorganic Chemistry · 2018Article
- X-ray absorption spectroscopic characterization of the diferric-peroxo intermediate of human deoxyhypusine hydroxylase in the presence of its substrate eIF5a.Journal of biological inorganic chemistry : JBIC : a publication of the Society of Biological Inorganic Chemistry · 2016Article
- Toward the synthesis of more reactive S = 2 non-heme oxoiron(IV) complexes.Accounts of chemical research · 2015Article
- [CuO](+) and [CuOH](2+) complexes: intermediates in oxidation catalysis?Accounts of chemical research · 2015Review
- Magnetic circular dichroism and computational study of mononuclear and dinuclear iron(IV) complexes.Chemical science · 2015Article
- Spectroscopic and theoretical investigation of a complex with an [O═Fe(IV)-O-Fe(IV)═O] core related to methane monooxygenase intermediate Q.Journal of the American Chemical Society · 2014Article
- Isolation and characterization of a dihydroxo-bridged iron(III,III)(μ-OH)2 diamond core derived from dioxygen.Inorganic chemistry · 2013Article
- High-Valent Nonheme Iron Oxidants in Biology: Lessons from Synthetic FeBulletin of Japan Society of Coordination Chemistry · 2013Article
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Abstract
Complexes 1-OH and 1-F are related complexes that share similar [X-Fe(III)-O-Fe(IV)═O](3+) core structures with a total spin S of ½, which arises from antiferromagnetic coupling of an S = 5/2 Fe(III)-X site and an S = 2 Fe(IV)═O site. EXAFS analysis shows that 1-F has a nearly linear Fe(III)-O-Fe(IV) core compared to that of 1-OH, which has an Fe-O-Fe angle of ~130° due to the presence of a hydrogen bond between the hydroxo and oxo groups. Both complexes are at least 1000-fold more reactive at C-H bond cleavage than 2, a related complex with a [OH-Fe(IV)-O-Fe(IV)═O](4+) core having individual S = 1 Fe(IV) units. Interestingly, 1-F is 10-fold more reactive than 1-OH. This raises an interesting question about what gives rise to the reactivity difference. DFT calculations comparing 1-OH and 1-F strongly suggest that the H-bond in 1-OH does not significantly change the electrophilicity of the reactive Fe(IV)═O unit and that the lower reactivity of 1-OH arises from the additional activation barrier required to break its H-bond in the course of H-atom transfer by the oxoiron(IV) moiety.
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