Journal
INORGANIC CHEMISTRY
Volume 55, Issue 16, Pages 8153-8159Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.6b01267
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Funding
- Natural Science Foundation of China [21421005, 21531001]
- Natural Science Foundation of Jiangsu Province [BK20140234]
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The design of a new photocatalytic system and integrating the essential components in a structurally controlled manner to create artificially photosynthetic systems is high desirable. By incorporating a photoactive triphenylamine moiety to assemble a Gd-based metal-organic framework as a heterogeneous photosensitizer, new artificial systems were constructed for the proton and carbon dioxide reduction under irradiation. The assembled MOFs exhibited a one-dimensional metal-oxygen pillar that was connected together by the depronated TCA(3-) ligands to form a three-dimensional non interpenetrating porous framework. The combining of proton reduction and/or the carbon dioxide reduction catalysts, i.e., the Fe-Fe hydrogenase active site models and the Ni(Cyclam) complexes, initiated a photoinduced single electron transfer from its excited state to the substrate. The system exhibited an initial TOF of 320 h(-1) of hydrogen per catalyst and an overall quantum yield of about 0.21% and,is able to reduce carbon dioxide under irradiation. The deposit of the photoactive Gd-TCA into the film of an alpha-Al2O3 plate provided a platform for the practical applications through prolonging the lifetime of the artifical system and allowed the easily operated devices being recyclable as a promising photocatalytic system.
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