期刊
CHEMSUSCHEM
卷 11, 期 15, 页码 2517-2528出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201801255
关键词
hydrogen production; photocatalysis; photosensitizer; transient absorption; Zn-II porphyrin
资金
- Hong Kong Research Grants Council [PolyU 123021/17P]
- National Natural Science Foundation of China [21504074]
- Science, Technology and Innovation Committee of Shenzhen Municipality [JCYJ20160531193836532]
- Hong Kong Polytechnic University [1-BE0Q]
- U.S. National Science Foundation's Chemical Catalysis division [CHE- 1566080]
Three molecular photosensitizers (PSs) with carboxylic acid anchors for attachment to platinized titanium dioxide nanoparticles were studied for light-driven hydrogen production from a fully aqueous medium with ascorbic acid (AA) as the sacrificial electron donor. Two zinc(II) porphyrin (ZnP)-based PSs were used to examine the effect of panchromatic sensitization on the photocatalytic H-2 generation. A dyad molecular design was used to construct a difluoro boron-dipyrromethene (bodipy)-conjugated ZnP PS (ZnP-dyad), whereas the other one featured an electron-donating diarylamino moiety (YD2-o-C8). To probe the use of the ZnP scaffold in this particular energy conversion process, an organic PS without the ZnP moiety (Bodipy-dye) was also synthesized for comparison. Ultrafast transient absorption spectroscopy was adopted to map out the energy transfer processes occurring in the dyad and to establish the bodipy-based antenna effect. In particular, the systems with YD2-o-C8 and ZnP-dyad achieved a remarkable initial activity for the production of H-2 with an initial turnover frequency (TOFi) higher than 300 h(-1) under white light irradiation. The use of ZnP PSs in dye-sensitized photocatalysis for the H-2 evolution reaction in this study indicated the importance of the panchromatic sensitization capability for the development of light absorbing PSs.
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