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嵌入有机硅纳米管用于水氧化的铱联吡啶配合物的耐久性增强

Enhanced durability of an iridium-bipyridine complex embedded into organosilica nanotubes for water oxidation.

作者信息

Zhang Shengbo, Wang Hua, Li Mei, Han Jinyu, Inagaki Shinji, Liu Xiao

机构信息

Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China.

Toyota Central R&D Laboratories., Inc., Nagakute, Aichi 480-1192, Japan.

出版信息

Dalton Trans. 2017 Jul 25;46(29):9369-9374. doi: 10.1039/c7dt02026k.

Abstract

Heterogeneous metal complex catalysts for the water oxidation reaction have ever been desired for the development of devices simulating photosynthesis. This paper describes the design of highly active and robust heterogeneous iridium complex catalysts for chemical water oxidation. The heterogeneous catalyst (Ir-BPy-NT) was prepared by the post-synthetic metalation of bipyridine-containing mesoporous organosilica nanotubes (BPy-NT) with an [IrCpCl(μ-Cl)] (Cp = η-pentamethylcyclopentadienyl) complex. The as-prepared Ir-BPy-NT catalyst showed enhanced durability with high reaction activity compared to the analogous homogeneous and the conventional heterogeneous ones, due to the stable nanotube structures as well as the isolated active sites. The unique one-dimensional nanotubes with large pore diameters can also reduce the diffusion limitation and facilitate the transport of reactants and products during reactions.

摘要

用于水氧化反应的多相金属络合物催化剂一直是模拟光合作用设备发展所需要的。本文描述了用于化学水氧化的高活性和稳健的多相铱络合物催化剂的设计。多相催化剂(Ir-BPy-NT)是通过含联吡啶的介孔有机硅纳米管(BPy-NT)与[IrCpCl(μ-Cl)](Cp = η-五甲基环戊二烯基)络合物进行合成后金属化制备的。与类似的均相和传统多相催化剂相比,所制备的Ir-BPy-NT催化剂由于稳定的纳米管结构以及孤立的活性位点,表现出更高的耐久性和高反应活性。具有大孔径的独特一维纳米管还可以减少扩散限制,并在反应过程中促进反应物和产物的传输。

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