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Light-Driven, Proton-Controlled, Catalytic Aerobic C-H Oxidation Mediated by a Mn(III) Porphyrinoid Complex

Title
Light-Driven, Proton-Controlled, Catalytic Aerobic C-H Oxidation Mediated by a Mn(III) Porphyrinoid Complex
Authors
Neu, Heather M.Jung, JieunBaglia, Regina A.Siegler, Maxime A.Ohkubo, KeiFukuzumi, ShunichiGoldberg, David P.
Ewha Authors
Shunichi Fukuzumi
SCOPUS Author ID
Shunichi Fukuzumiscopus
Issue Date
2015
Journal Title
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN
0002-7863JCR Link
Citation
vol. 137, no. 14, pp. 4614 - 4617
Publisher
AMER CHEMICAL SOC
Indexed
SCI; SCIE; SCOPUS WOS scopus
Abstract
The visible light-driven, catalytic aerobic oxidation of benzylic C-H bonds was mediated by a Mn-III corrolazine complex. To achieve catalytic turnovers, a strict selective requirement for the addition of protons was established. The resting state of the catalyst was unambiguously characterized by X-ray diffraction as [Mn-III((HO)-O-2)(TBP(8)Cz(H))](+), in which a single, remote site on the ligand is protonated. If two remote sites are protonated, however, reactivity with O-2 is shut down. Spectroscopic methods revealed that the related Mn-V(O) complex is also protonated at the same remote site at -60 degrees C, but undergoes valence tautomerization upon warming.
DOI
10.1021/jacs.5b00816
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자연과학대학 > 화학·나노과학전공 > Journal papers
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