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Electron Transfer in Dye-Sensitised Semiconductors Modified with Molecular Cobalt Catalysts: Photoreduction of Aqueous Protons.
MedLine Citation:
PMID:  23033059     Owner:  NLM     Status:  Publisher    
Abstract/OtherAbstract:
A visible-light driven H(2) evolution system comprising of a Ru(II) dye (RuP) and Co(III) proton reduction catalysts (CoP) immobilised on TiO(2) nanoparticles and mesoporous films is presented. The heterogeneous system evolves H(2) efficiently during visible-light irradiation in a pH-neutral aqueous solution at 25 °C in the presence of a hole scavenger. Photodegradation of the self-assembled system occurs at the ligand framework of CoP, which can be readily repaired by addition of fresh ligand, resulting in turnover numbers above 300 mol H(2) (mol CoP)(-1) and above 200,000 mol H(2) (mol TiO(2) nanoparticles)(-1) in water. Our studies support that a molecular Co species, rather than metallic Co or a Co-oxide precipitate, is responsible for H(2) formation on TiO(2) . Electron transfer in this system was studied by transient absorption spectroscopy and time-correlated single photon counting techniques. Essentially quantitative electron injection takes place from RuP into TiO(2) in approximately 180 ps. Thereby, upon dye regeneration by the sacrificial electron donor, a long-lived TiO(2) conduction band electron is formed with a half-lifetime of approximately 0.8 s. Electron transfer from the TiO(2) conduction band to the CoP catalysts occurs quantitatively on a 10 μs timescale and is about a hundred times faster than charge-recombination with the oxidised RuP. This study provides a benchmark for future investigations in photocatalytic fuel generation with molecular catalysts integrated in semiconductors.
Authors:
Fezile Lakadamyali; Anna Reynal; Masaru Kato; James R Durrant; Erwin Reisner
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Publication Detail:
Type:  JOURNAL ARTICLE     Date:  2012-10-2
Journal Detail:
Title:  Chemistry (Weinheim an der Bergstrasse, Germany)     Volume:  -     ISSN:  1521-3765     ISO Abbreviation:  Chemistry     Publication Date:  2012 Oct 
Date Detail:
Created Date:  2012-10-3     Completed Date:  -     Revised Date:  -    
Medline Journal Info:
Nlm Unique ID:  9513783     Medline TA:  Chemistry     Country:  -    
Other Details:
Languages:  ENG     Pagination:  -     Citation Subset:  -    
Copyright Information:
Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Affiliation:
Christian Doppler Laboratory for Sustainable SynGas Chemistry, Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW (UK).
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