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Catalytic mechanisms of hydrogen evolution with homogeneous and heterogeneous catalysts

Title
Catalytic mechanisms of hydrogen evolution with homogeneous and heterogeneous catalysts
Authors
Fukuzumi S.Yamada Y.Suenobu T.Ohkubo K.Kotani H.
Ewha Authors
Shunichi Fukuzumi
SCOPUS Author ID
Shunichi Fukuzumiscopus
Issue Date
2011
Journal Title
Energy and Environmental Science
ISSN
1754-5692JCR Link
Citation
vol. 4, no. 8, pp. 2754 - 2766
Indexed
SCI; SCIE; SCOPUS WOS scopus
Abstract
This perspective focuses on reaction mechanisms of hydrogen (H 2) evolution with homogeneous and heterogeneous catalysts. First, photocatalytic H 2 evolution systems with homogeneous catalysts are discussed from the viewpoint of how to increase the efficiency of the two-electron process for the H 2 evolution via photoinduced electron-transfer reactions of metal complexes. Two molecules of the one-electron reduced species of [Rh III(Cp*)(bpy)(H 2O)](SO 4) (bpy = 2,2′-bipyridine) and [Ir III(Cp*)(H 2O)(bpm) Ru II(bpy) 2](SO 4) 2 (bpm = 2,2′-bipyrimidine) produced by photoinduced electron-transfer reactions are converted to the two-electron reduced complexes suitable for H 2 generation by disproportionation. The photocatalytic mechanism of H 2 evolution using Pt nanoparticles as a catalyst is also discussed based on the kinetic analysis of the electron-transfer rates from a photogenerated electron donor to Pt nanoparticles, which are comparable to the overall H 2 evolution rates. The electron-transfer rates become faster with increasing proton concentrations with an inverse kinetic isotope effect, when H + is replaced by D +. The size and shape effects of Pt nanoparticles on the rates of hydrogen evolution and the electron-transfer reaction are examined to optimize the catalytic efficiency. Finally, catalytic H 2 evolution systems from H 2 storage molecules are described including shape dependent catalytic activity of Co 3O 4 particles for ammonia borane hydrolysis and a large tunneling effect observed in decomposition of formic acid with [Ir III(Cp*)(H 2O)(bpm)Ru II(bpy) 2](SO 4) 2. © 2011 The Royal Society of Chemistry.
DOI
10.1039/c1ee01551f
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자연과학대학 > 화학·나노과학전공 > Journal papers
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