Accelerated Oxygen Atom Transfer and C-H Bond Oxygenation by Remote Redox Changes in Fe3Mn-Iodosobenzene Adducts

de Ruiter, Graham; Carsch, Kurtis M.; Gul, Sheraz; Chatterjee, Ruchira; Thompson, Niklas B.; Takase, Michael K.; Yano, Junko; Agapie, Theodor

doi:10.1002/anie.201701319

Title: Accelerated Oxygen Atom Transfer and C-H Bond Oxygenation by Remote Redox Changes in Fe₃Mn-Iodosobenzene Adducts

Journal Article · 24 March 2017 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.201701319 · OSTI ID:1379810

de Ruiter, Graham ^[1]; Carsch, Kurtis M. ^[1]; Gul, Sheraz ^[2]; Chatterjee, Ruchira ^[2]; Thompson, Niklas B. ^[1]; Takase, Michael K. ^[1]; Yano, Junko ^[2];

^[1]

California Inst. of Technology (CalTech), Pasadena, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Abstract We report the synthesis, characterization, and reactivity of [LFe ₃ (PhPz) ₃ OMn( ^s PhIO)][OTf] _x ( 3 : x =2; 4 : x =3), where 4 is one of very few examples of iodosobenzene–metal adducts characterized by X‐ray crystallography. Access to these rare heterometallic clusters enabled differentiation of the metal centers involved in oxygen atom transfer (Mn) or redox modulation (Fe). Specifically, ⁵⁷ Fe Mössbauer and X‐ray absorption spectroscopy provided unique insights into how changes in oxidation state ( Fe ^III ₂ Fe ^II Mn ^II vs. Fe ^III ₃ Mn ^II ) influence oxygen atom transfer in tetranuclear Fe ₃ Mn clusters. In particular, a one‐electron redox change at a distal metal site leads to a change in oxygen atom transfer reactivity by ca. two orders of magnitude.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Inst. of Health (NIH) (United States)

Grant/Contract Number:: AC02-05CH11231; R01-GM102687B; DEAC02- 05CH11231

OSTI ID:: 1379810

Alternate ID(s):: OSTI ID: 1401528

Journal Information:: Angewandte Chemie (International Edition), Vol. 56, Issue 17; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
C-H bond oxygenation
clusters
iodosobenzene adduct
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CCDC 1536076: Experimental Crystal Structure Determination: MANJIX : (μ-oxo)-(μ-1,3,5-tris(2-(bis(2-pyridyl)oxymethyl)phenyl)benzene)-tris(μ-3-phenylpyrazolato)-tri-iron-manganese bis(trifluoromethanesulfonate) acetonitrile diethyl ether solvate de Ruiter, Graham; Carsch, Kurtis; Gul, Sheraz https://doi.org/10.5517/ccdc.csd.cc1nkdvg The current record is supplemented by this dataset	dataset	March 2017
CCDC 1536080: Experimental Crystal Structure Determination: MANKEU : (μ-oxo)-(μ-1,3,5-tris(2-(bis(2-pyridyl)oxymethyl)phenyl)benzene)-tris(μ-3-phenylpyrazolato)-acetonitrile-tri-iron-manganese tris(trifluoromethanesulfonate) acetonitrile solvate De Ruiter, Graham; Carsch, Kurtis M.; Gul, Sheraz https://doi.org/10.5517/ccdc.csd.cc1nkdzl The current record is supplemented by this dataset	dataset	March 2017
CCDC 1536077: Experimental Crystal Structure Determination: MANJOD : (μ-oxo)-(μ-1,3,5-tris(2-(oxybis(2-pyridyl)methyl)phenyl)benzene)-(μ-3-(2-oxyphenyl)pyrazolato)-bis(μ-3-phenylpyrazolato)-tri-iron-manganese bis(trifluoromethanesulfonate) acetonitrile solvate de Ruiter, Graham; Carsch, Kurtis; Gul, Sheraz https://doi.org/10.5517/ccdc.csd.cc1nkdwh The current record is supplemented by this dataset	dataset	March 2017
CCDC 1536078: Experimental Crystal Structure Determination: MANJUJ : (μ-oxo)-(μ-1,3,5-tris(2-(bis(2-pyridyl)oxymethyl)phenyl)benzene)-tris(μ-3-phenylpyrazolato)-acetonitrile-tri-iron-manganese tris(trifluoromethanesulfonate) acetonitrile diethyl ether solvate de Ruiter, Graham; Carsch, Kurtis; Gul, Sheraz https://doi.org/10.5517/ccdc.csd.cc1nkdxj The current record is supplemented by this dataset	dataset	March 2017
CCDC 1536079: Experimental Crystal Structure Determination: MANKAQ : (μ-oxo)-(μ-1,3,5-tris(2-(bis(2-pyridyl)oxymethyl)phenyl)benzene)-tris(μ-3-phenylpyrazolato)-(2-t-butylsulfonylphenyliodoxo)-tri-iron-manganese tris(trifluoromethanesulfonate) dichloromethane toluene solvate de Ruiter, Graham; Carsch, Kurtis; Gul, Sheraz https://doi.org/10.5517/ccdc.csd.cc1nkdyk The current record is supplemented by this dataset	dataset	March 2017

Title: Accelerated Oxygen Atom Transfer and C-H Bond Oxygenation by Remote Redox Changes in Fe3Mn-Iodosobenzene Adducts

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