Photodriven Oxidation of Water by Plastoquinone Analogs with a Nonheme Iron Catalyst
- 주제(기타) Chemistry, Multidisciplinary
- 설명문(일반) [Hon, Young Hyun; Jung, Jieun; Sharma, Namita; Lee, Yong-Min; Nam, Wonwoo; Fukuzumi, Shunichi] Ewha Womans Univ, Dept Chem & Nano Sci, Seoul 03760, South Korea; [Jung, Jieun] Nagoya Univ, Grad Sch Sci, Dept Chem, Chikusa Ku, Nagoya, Aichi 4648602, Japan; [Awa, Tatsuo Naka] Unisoku Co Ltd, SENTAN, Japan Sci & Technol Agcy JST, Hirakata, Osaka 5730131, Japan; [Nam, Wonwoo] Chinese Acad Sci, LICP, Suzhou Res Inst, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Gansu, Peoples R China; [Fukuzumi, Shunichi] Meijo Univ, SENTAN, Japan Sci & Technol Agcy JST, Fac Sci & Engn, Nagoya, Aichi 4680073, Japan
- 등재 SCIE, SCOPUS
- 발행기관 AMER CHEMICAL SOC
- 발행년도 2019
- URI http://www.dcollection.net/handler/ewha/000000159689
- 본문언어 영어
- Published As http://dx.doi.org/10.1021/jacs.9b02517
- PubMed https://pubmed.ncbi.nlm.nih.gov/30943724
초록/요약
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.
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