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Pure and Applied Chemistry

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Volume 85, Issue 7 (Jan 2013)

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

Shan Yu
  • Corresponding author
  • Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, the Chinese Academy of Sciences, Beijing 100190, China
/ Feng Wang
  • Corresponding author
  • Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, the Chinese Academy of Sciences, Beijing 100190, China
/ Jing-Jing Wang
  • Corresponding author
  • Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, the Chinese Academy of Sciences, Beijing 100190, China
/ Hong-Yan Wang
  • Corresponding author
  • Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, the Chinese Academy of Sciences, Beijing 100190, China
/ Bin Chen
  • Corresponding author
  • Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, the Chinese Academy of Sciences, Beijing 100190, China
/ Ke Feng
  • Corresponding author
  • Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, the Chinese Academy of Sciences, Beijing 100190, China
/ Chen-Ho Tung
  • Corresponding author
  • Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, the Chinese Academy of Sciences, Beijing 100190, China
/ Li-Zhu Wu
  • Corresponding author
  • Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, the Chinese Academy of Sciences, Beijing 100190, China
Published Online: 2013-01-19 | DOI: https://doi.org/10.1351/PAC-CON-12-08-05

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

Conference

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

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About the article

Published Online: 2013-01-19

Published in Print: 2013-01-19



Citation Information: Pure and Applied Chemistry, ISSN (Online) 1365-3075, ISSN (Print) 0033-4545, DOI: https://doi.org/10.1351/PAC-CON-12-08-05. Export Citation

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