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Photodriven Oxidation of Water by Plastoquinone Analogs with a Nonheme Iron Catalyst
- Title
- Photodriven Oxidation of Water by Plastoquinone Analogs with a Nonheme Iron Catalyst
- Authors
- Hon, Young Hyun; Jung, Jieun; Awa, Tatsuo Naka; Sharma, Namita; Lee, Yong-Min; Nam, Wonwoo; Fukuzumi, Shunichi
- Ewha Authors
- 남원우; 이용민; Shunichi Fukuzumi; 정지은
- SCOPUS Author ID
- 남원우; Shunichi Fukuzumi; 정지은
- Issue Date
- 2019
- Journal Title
- JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
- ISSN
- 0002-7863
- Citation
- JOURNAL OF THE AMERICAN CHEMICAL SOCIETY vol. 141, no. 16, pp. 6748 - 6754
- Publisher
- AMER CHEMICAL SOC
- Indexed
- SCIE; SCOPUS
- Document Type
- Article
- Abstract
- Photoirradiation of an acetonitrile solution containing p-benzoquinone derivatives (X-Q) as plastoquinone analogs, a nonheme iron(II) complex, [(N4Py)Fe-II](2+) (N4Py = N,N-bis(2-pyridylmethyl)-N-bis(2-pyridyl)-methylamine), and H2O afforded the evolution of O-2 and the formation of the corresponding hydroquinone derivatives (X-QH(2)) quantitatively. During the photodriven oxidation of water by X-Q, [(N4Py)Fe-II](2+) was oxidized by the excited state of X-Q to produce the iron(IV)-oxo complex([(N4Py)-Fe-IV(O)](2+)) quantitatively. The concentration of [(N4Py)-Fe-IV(O)](2+) remained virtually the same during the repeated cycles of photodriven oxidation of water by X-Q. [(N4Py)Fe-IV(O)](2+) was the excited state of X-Q to [(N4Py)Fe-V(O)](3+); this Fe-V-oxo species is proposed as an active oxidant that affects the water oxidation. The photocatalytic mechanism of the water oxidation by X-Q with [(N4Py)Fe-II](2+) was clarified by detecting intermediates using various spectroscopic techniques, such as transient absorption and electron paramagnetic resonance measurements. To the best of our knowledge, the present study reports the first example of a functional model of Photosystem II (PSII) using X-Q as plastoquinone analogs in the photocatalytic oxidation of water.
- DOI
- 10.1021/jacs.9b02517
- Appears in Collections:
- 자연과학대학 > 화학·나노과학전공 > Journal papers
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