Photoactive Metal–Organic Framework and Its Film for Light-Driven Hydrogen Production and Carbon Dioxide Reduction

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• 作者：Pengyan Wu ; Xiangyang Guo ; Linjuan Cheng ; Cheng He ; Jian Wang ; Chunying Duan
• 刊名：Inorganic Chemistry
• 出版年：2016
• 出版时间：August 15, 2016
• 年：2016
• 卷：55
• 期：16
• 页码：8153-8159
• 全文大小：487K
• 年卷期：0
• ISSN：1520-510X

文摘

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 noninterpenetrating 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 α-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.