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向MoO载体中掺杂氢以调节金属-载体相互作用并实现铱纳米催化剂上糠醛的高效氢化反应

Hydrogen Doping into MoO Supports toward Modulated Metal-Support Interactions and Efficient Furfural Hydrogenation on Iridium Nanocatalysts.

作者信息

Xie Lifang, Chen Ting, Chan Hang Cheong, Shu Yijin, Gao Qingsheng

机构信息

Department of Chemistry, College of Chemistry and Materials Science, Jinan University, No. 601 Huangpu Avenue West, 510632, Guangzhou, P.R. China.

出版信息

Chem Asian J. 2018 Mar 16;13(6):641-647. doi: 10.1002/asia.201701661. Epub 2018 Feb 1.

Abstract

As promising supports, reducible metal oxides afford strong metal-support interactions to achieve efficient catalysis, which relies on their band states and surface stoichiometry. In this study, in situ and controlled hydrogen doping (H doping) by means of H spillover was employed to engineer the metal-support interactions in hydrogenated MoO -supported Ir (Ir/H-MoO ) catalysts and thus promote furfural hydrogenation to furfuryl alcohol. By easily varying the reduction temperature, the resulting H doping in a controlled manner tailors low-valence Mo species (Mo and Mo ) on H-MoO supports, thereby promoting charge redistribution on Ir and H-MoO interfaces. This further leads to clear differences in H chemisorption on Ir, which illustrates its potential for catalytic hydrogenation. As expected, the optimal Ir/H-MoO with controlled H doping afforded high activity (turnover frequency: 4.62 min ) and selectivity (>99 %) in furfural hydrogenation under mild conditions (T=30 °C, PH2 =2 MPa), which means it performs among the best of current catalysts.

摘要

作为有前景的载体,可还原金属氧化物能提供强大的金属-载体相互作用以实现高效催化,这依赖于它们的能带状态和表面化学计量比。在本研究中,通过氢溢流原位且可控地进行氢掺杂(H掺杂),以调控负载于氢化MoO上的Ir(Ir/H-MoO)催化剂中的金属-载体相互作用,从而促进糠醛加氢制糠醇。通过轻松改变还原温度,以可控方式进行的H掺杂可调控H-MoO载体上的低价Mo物种(Mo和Mo),进而促进Ir与H-MoO界面上的电荷重新分布。这进一步导致Ir上H化学吸附的明显差异,这表明其在催化加氢方面的潜力。正如预期的那样,具有可控H掺杂的最佳Ir/H-MoO在温和条件下(T = 30°C,PH2 = 2 MPa)的糠醛加氢反应中具有高活性(周转频率:4.62 min)和选择性(>99%),这意味着它在当前催化剂中表现优异。

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