| Hydrophilicity Control of Visible-Light Hydrogen Evolution and Dynamics of the Charge-Separated State in Dye/TiO(2) /Pt Hybrid Systems. | |
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MedLine Citation:
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PMID: 23042083 Owner: NLM Status: Publisher |
Abstract/OtherAbstract:
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Visible-light-driven H(2) evolution based on Dye/TiO(2) /Pt hybrid photocatalysts was investigated for a series of (E)-3-(5'-{4-[bis(4-R(1) -phenyl)amino]phenyl}-4,4'-(R(2) )(2) -2,2'-bithiophen-5-yl)-2-cyanoacrylic acid dyes. Efficiencies of hydrogen evolution from aqueous suspensions in the presence of ethylenediaminetetraacetic acid as electron donor under illumination at λ>420 nm were found to considerably depend on the hydrophilic character of R(1) , varying in the order MOD (R(1) =CH(3) OCH(2) , R(2) =H)≈MO4D (R(1) =R(2) =CH(3) OCH(2) )>HD (R(1) =R(2) =H)>PD (R(1) =C(3) H(7) , R(2) =H). In the case of MOD/TiO(2) /Pt, the apparent quantum yield for photocatalyzed H(2) generation at 436 nm was 0.27±0.03. Transient absorption measurements for MOD- or PD-grafted transparent films of TiO(2) nanoparticles dipped into water at pH 3 commonly revealed ultrafast formation (<100 fs) of the dye radical cation (Dye(.) (+) ) followed by multicomponent decays, which involve minor fast decays (<5 ps) almost independent of R(1) and major slower decays with significant differences between the two samples: 1) the early decay of the major components for MOD is about 2.5 times slower than that for PD and 2) a redshift of the spectrum occurred for MOD with a time constant of 17 ps, but not for PD. The substituent effects on H(2) generation as well as on transient behavior have been discussed in terms substituent-dependent charge recombination (CR) of Dye(.) (+) with electrons in bulk, inner-trap, and/or interstitial-trap states, arising from different solvent reorganization. |
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Authors:
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Won-Sik Han; Kyung-Ryang Wee; Hyun-Young Kim; Chyongjin Pac; Yu Nabetani; Daisuke Yamamoto; Tetsuya Shimada; Haruo Inoue; Heesung Choi; Kyeongjae Cho; Sang Ook Kang |
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Publication Detail:
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Type: JOURNAL ARTICLE Date: 2012-10-5 |
Journal Detail:
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Title: Chemistry (Weinheim an der Bergstrasse, Germany) Volume: - ISSN: 1521-3765 ISO Abbreviation: Chemistry Publication Date: 2012 Oct |
Date Detail:
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Created Date: 2012-10-8 Completed Date: - Revised Date: - |
Medline Journal Info:
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Nlm Unique ID: 9513783 Medline TA: Chemistry Country: - |
Other Details:
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Languages: ENG Pagination: - Citation Subset: - |
Copyright Information:
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Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. |
Affiliation:
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Department of Advanced Materials Chemistry, Sejong, Korea University, 208 Seochang, Chochiwon, Chung-nam 339-700 (Korea), Fax: (+82) 44-867-5396. |
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From MEDLINE®/PubMed®, a database of the U.S. National Library of Medicine
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