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Photochemical hydrogen production with molecular devices comprising a zinc porphyrin and a cobaloxime catalyst
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2012 (English)In: Science China Chemistry, ISSN 1674-7291, Vol. 55, no 7, 1274-1282 p.Article in journal (Refereed) Published
Abstract [en]

Two new noble-metal-free molecular devices, [{Co(dmgH)(2)Cl}{Zn(PyTPP)}] (1, dmgH = dimethyloxime, PyTPP = 5-(4-pyridyl)-10,15,20-triphenylporphyrin) and [{Co(dmgH)(2)Cl}{Zn(apPyTPP)}] (2, apPyTPP = 5-[4-(isonicotinamidyl)phenyl]-10,15,20-triphenylporphyrin), for light-driven hydrogen generation were prepared and spectroscopically characterized. The zinc porphyrin photosensitizer and the Co-III-based catalyst unit are linked by axial coordination of a pyridyl group in the periphery of zinc-porphyrin to the cobalt centre of catalyst with different lengths of bridges. The apparent fluorescence quenching and lifetime decays of 1 and 2 were observed in comparison with their reference chromophores, Zn(PyTPP) (3) and Zn(apPyTPP) (4), suggesting a possibility for an intramolecular electron transfer from the singlet excited state of zinc porphyrin unit to the cobalt centre in the molecular devices. Photochemical H-2-evolving studies show that complexes 1 and 2 are efficient molecular photocatalysts for visible light-driven H-2 generation from water with triethylamine as a sacrificial electron donor in THF/H2O, with turnover numbers up to 46 and 35 for 1 and 2, respectively. In contrast to these molecular devices, the multicomponent catalyst of zinc porphyrin and [Co(dmgH)(2)PyCl] did not show any fluorescence quenching and as a consequence, no H-2 gas was detected by GC analysis in the presence of triethylamine with irradiation of visible light. The plausible mechanism for the photochemical H-2 generation with these molecular devices is discussed.

Place, publisher, year, edition, pages
2012. Vol. 55, no 7, 1274-1282 p.
Keyword [en]
cobaloxime, hydrogen production, molecular device, photocatalysis, zinc porphyrin
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-99411DOI: 10.1007/s11426-012-4514-0ISI: 000306070500011Scopus ID: 2-s2.0-84866069331OAI: oai:DiVA.org:kth-99411DiVA: diva2:542300
Funder
Swedish Research CouncilKnut and Alice Wallenberg Foundation
Note
QC 20120731Available from: 2012-07-31 Created: 2012-07-30 Last updated: 2012-07-31Bibliographically approved

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Sun, LiCheng

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