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Photocatalytic hydrogen evolution from formate and aldehyde over molecular iridium complexes stabilized by bipyridine-bridging organosilica nanotubes
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2018-05-20 , DOI: 10.1016/j.apcatb.2018.05.058
Shengbo Zhang , Mei Li , Qilong Wu , Hongchen Yang , Jinyu Han , Hua Wang , Xiao Liu

An efficient heterogeneous photocatalytic system for high-purity hydrogen evolution from formate or aldehyde-water solution were developed using IrCp*Cl (Cp* = η5-pentamethylcyclopentadienyl) complex anchored onto the robust bipyridine-based organosilica nanotubes as a solid catalyst. This system can be conducted at the room temperature with a visible light (λ > 420 nm) illumination. The heterogeneous molecular photocatalyst displayed much improved catalytic activity and recyclability compared to the analogous homogeneous catalyst, benefiting from the isolated photoactive sites as well as the efficient transport of substrates and products in the nanotube channels. A detailed characterization for the solid catalyst after the reactions by UV/vis, XPS and 13C CP MAS NMR testified the molecular nature of the active species. This work provides an easy method to construct the heterogeneous molecular photocatalysts for the high-purity hydrogen generation under mild conditions.



中文翻译:

联吡啶桥联有机硅纳米管稳定的分子铱络合物上甲酸和醛的光催化氢释放

利用锚固在坚固的联吡啶基有机硅纳米管上的IrCp * Cl(Cp * =η5-甲基五环戊二烯基)络合物作为固体催化剂,开发了一种高效的多相光催化体系,用于从甲酸盐或醛水溶液中高纯度制氢。该系统可以在室温下用可见光(λ> 420 nm)照明进行。与类似的均相催化剂相比,非均相分子光催化剂显示出大大改善的催化活性和可回收性,这得益于分离的光活性位以及纳米管通道中底物和产物的有效运输。UV / vis,XPS和13反应后的固体催化剂的详细表征C CP MAS NMR证明了活性物质的分子性质。这项工作为构建温和条件下高纯度氢生成的非均相分子光催化剂提供了一种简便的方法。

更新日期:2018-05-20
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