Light-driven hydrogen evolution system with glutamic-acid-modified zinc porphyrin as photosensitizer and [FeFe]-hydrogenase model as catalyst : Pure and Applied Chemistry

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Pure and Applied Chemistry

The Scientific Journal of IUPAC

Ed. by Burrows, Hugh / Weir, Ron / Stohner, Jürgen


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Light-driven hydrogen evolution system with glutamic-acid-modified zinc porphyrin as photosensitizer and [FeFe]-hydrogenase model as catalyst

Shan Yu1 / Feng Wang1 / Jing-Jing Wang1 / Hong-Yan Wang1 / Bin Chen1 / Ke Feng1 / Chen-Ho Tung1 / Li-Zhu Wu1

1Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, the Chinese Academy of Sciences, Beijing 100190, China

Conference

IUPAC Symposium on Photochemistry, International Symposium on Photochemistry, PHOTO, Photochemistry, XXIVth, Coimbra, Portugal, 2012-07-15–2012-07-20

Citation Information: Pure and Applied Chemistry. Volume 85, Issue 7, Pages 1405–1413, ISSN (Online) 1365-3075, ISSN (Print) 0033-4545, DOI: 10.1351/PAC-CON-12-08-05, January 2013

Publication History

Published Online:
2013-01-19

An intermolecular light-driven hydrogen evolution system with free glutamic-acid-modified zinc tetra(p-phenyl) porphyrin (Glu-ZnP) as a photosensitizer and [Fe2(CO)6(μ-adt)C6H5] [μ-adt = N(CH2S)2] (Badt) as a catalyst has been constructed. Using phenylmercaptan (BSH) as electron donor and acetic acid (HOAc) as proton source, hydrogen was obtained after irradiation with visible light for 2 h; the efficiency is comparable to that of the similar intramolecular dyad. Steady-state and time-resolved spectroscopy and cyclic voltammetry show that both the first and the second electron transfer from singlet 1*Glu-ZnP to Badt and reduced Badt are thermodynamically feasible. However, the competition of electron transfer from singlet 1*Glu-ZnP to Badt with intersystem crossing from singlet 1*Glu-ZnP to triplet 3*Glu-ZnP, inefficient electron transfer from triplet 3*Glu-ZnP to Badt, and the lower energy of triplet 3*Glu-ZnP and possible 3*Badt to that of yielded charge-separated state of Glu-ZnP+·-Badt−· were believed to be the obstacles for efficient hydrogen evolution.

Keywords: [2Fe2S] model; back electron transfer; energy transfer; [FeFe]-hydrogenase; intersystem crossing; light-driven hydrogen evolution; photoinduced electron transfer; zinc porphyrin

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[1]
Shang Gao, Shuai Huang, Qian Duan, Jianhua Hou, Dayong Jiang, Qingcheng Liang, and Jianxun Zhao
International Journal of Hydrogen Energy, 2014, Volume 39, Number 20, Page 10434

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