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A Mononuclear Non-heme Manganese(III)-Aqua Complex as a New Active Oxidant in Hydrogen Atom Transfer Reactions

Title
A Mononuclear Non-heme Manganese(III)-Aqua Complex as a New Active Oxidant in Hydrogen Atom Transfer Reactions
Authors
Sankaralingam, MuniyandiLee, Yong-MinKarmalkar, Deepika G.Nam, WonwooFukuzumi, Shunichi
Ewha Authors
남원우Shunichi Fukuzumi
SCOPUS Author ID
남원우scopus; Shunichi Fukuzumiscopus
Issue Date
2018
Journal Title
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN
0002-7863JCR Link
Citation
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY vol. 140, no. 40, pp. 12695 - 12699
Publisher
AMER CHEMICAL SOC
Indexed
SCIE; SCOPUS WOS scopus
Document Type
Article
Abstract
A mononuclear non-heme Mn(III)-aqua complex, [(dpaq)Mn-III(OH2)](2+) (1, dpaq = 2-[bis-(pyridin-2-ylmethyl)]amino-N-quinolin-8-yl-acetamidate), is capable of conducting hydrogen atom transfer (HAT) reactions much more efficiently than the corresponding Mn(III)-hydroxo complex, [(dpaq)Mn-III(OH)](+) (2); the high reactivity of 1 results from the positive one-electron reduction potential of 1 (E-red vs SCE = 1.03 V), compared to that of 2 (E-red vs SCE = -0.1 V). The HAT mechanism of 1 varies between electron transfer followed by proton transfer and one-step concerted proton-coupled electron transfer, depending on the one-electron oxidation potentials of substrates. To the best of our knowledge, this is the first example showing that metal(III)-aqua complex can be an effective H-atom abstraction reagent.
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DOI
10.1021/jacs.8b07772
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자연과학대학 > 화학·나노과학전공 > Journal papers
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