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Photocatalytic hydrogen evolution from carbon-neutral oxalate with 2-phenyl-4-(1-naphthyl)quinolinium ion and metal nanoparticles

Title
Photocatalytic hydrogen evolution from carbon-neutral oxalate with 2-phenyl-4-(1-naphthyl)quinolinium ion and metal nanoparticles
Authors
Yamada Y.Miyahigashi T.Ohkubo K.Fukuzumi S.
Ewha Authors
Shunichi Fukuzumi
SCOPUS Author ID
Shunichi Fukuzumiscopus
Issue Date
2012
Journal Title
Physical Chemistry Chemical Physics
ISSN
1463-9076JCR Link
Citation
vol. 14, no. 30, pp. 10564 - 10571
Indexed
SCI; SCIE; SCOPUS WOS scopus
Abstract
Photocatalytic hydrogen evolution has been made possible by using oxalate as a carbon-neutral electron source, metal nanoparticles as hydrogen-evolution catalysts and the 2-phenyl-4-(1-naphthyl)quinolinium ion (QuPh +-NA), which forms the long-lived electron-transfer state upon photoexcitation, as a photocatalyst. The hydrogen evolution was conducted in a deaerated mixed solution of an aqueous buffer and acetonitrile (MeCN) [1:1 (v/v)] by photoirradiation (λ > 340 nm). The gas evolved during the photocatalytic reaction contained H 2 and CO 2 in a molar ratio of 1:2, indicating that oxalate acts as a two-electron donor. The hydrogen yield based on the amount of oxalate reached more than 80% under pH conditions higher than 6. Ni and Ru nanoparticles as well as Pt nanoparticles act as efficient hydrogen-evolution catalysts in the photocatalytic hydrogen evolution. The photocatalyst for hydrogen evolution can be used several times without significant deactivation of the catalytic activity. Nanosecond laser flash photolysis measurements have revealed that electron transfer from oxalate to the photogenerated QuPh-NA +, which forms a π-dimer radical cation with QuPh +-NA [(QuPh-NA +)(QuPh +-NA)], occurs followed by subsequent electron transfer from QuPh-NA to the hydrogen-evolution catalyst in the photocatalytic hydrogen evolution. Oxalate acts as an efficient electron source under a wide range of reaction conditions. © 2012 the Owner Societies.
DOI
10.1039/c2cp41906h
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자연과학대학 > 화학·나노과학전공 > Journal papers
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