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대한화학회 제124회 학술발표회 및 총회 Photodriven Water Oxidation by p-Benzoquinone Derivatives with an Iron Catalyst as a functional model of Photosystem II

2019년 8월 15일 19시 49분 35초
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목 09시 : 30분
Inorganic Chemistry - Oral Presentation of Young Inorganic Chemistry
저자 및
Young Hyun Hong, Yong-Min Lee1, Wonwoo Nam*, Shunichi Fukuzumi2,*
Department of Chemistry and Nano Science, Ewha Womans University, Korea
1Research Institute for Basic Sciences, Ewha Womans University, Korea
2Osaka University, Japan
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승인 1건
Photoirradiation of a solution containing p-benzoquinone derivatives (X-Q) as plastoquinone analogs, a nonheme iron(II) complex, [(N4Py)FeII]2+ (N4Py = N,N-bis(2-pyridylmethyl)-N-bis(2-pyridyl)methylamine), and H2O afforded the O2 evolution and the formation of the corresponding hydroquinone derivatives (X-QH2) quantitatively. During the photodriven water oxidation by X-Q, [(N4Py)FeII]2+ was oxidized by the excited state of X-Q (3X-Q*) to produce the iron(IV)-oxo complex, [(N4Py)FeIV(O)]2+, quantitatively. The concentration of [(N4Py)FeIV(O)]2+ remained virtually the same during the repeated cycles of photodriven water oxidation by X-Q. [(N4Py)FeIV(O)]2+ was further oxidized by 3X-Q* to [(N4Py)FeV(O)]3+, which is proposed as an active oxidant that affects the water oxidation. The photocatalytic mechanism of the water oxidation by X-Q with [(N4Py)FeII]2+ was clarified by detecting intermediates using various spectroscopic techniques, such as transient absorption and electron paramagnetic resonance measurements. The present study reports the first example of a functional model of Photosystem II (PSII) using X-Q as plastoquinone analogs in the photocatalytic water oxidation.