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Effects of divalent metal ions of hydrotalcites on catalytic behavior of supported gold nanocatalysts for chemoselective hydrogenation of 3-nitrostyrene
Journal of Catalysis ( IF 6.5 ) Pub Date : 2018-06-06 , DOI: 10.1016/j.jcat.2018.05.007
Yuan Tan , Xiao Yan Liu , Lin Li , Leilei Kang , Aiqin Wang , Tao Zhang

The effect of the divalent metal ions on the hydrotalcite (HT) (MAl-HT; M = Mg, Zn, Ni)-supported thiolated Au25 nanoclusters (NCs) as the precatalysts for the chemoselective hydrogenation of 3-nitrostyrene to 3-vinylaniline was investigated. The highest chemoselectivity was obtained over the Au25/ZnAl-HT-300 (calcined at 300 °C) catalyst, with a maintained selectivity of desired product above 98%. The Au25/NiAl-HT-300 catalyst exhibited the highest activity, although the particle size of gold (3.2 nm) was greater than those of the Au25/MgAl-HT-300 (2.2 nm) and Au25/ZnAl-HT-300 (1.7 nm) catalysts. The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results of CO adsorption revealed that Ni interacting intimately with gold could be reduced easily, which affected the catalytic behavior of the Au25/NiAl-HT-300 catalyst. Furthermore, the results of the in situ DRIFTS of the adsorption of nitrostyrene at 10 bar of hydrogen suggested that, besides the condensation route, it also followed the direct route to produce aniline on Au25/NiAl-HT-300, which was different from the other two catalysts. This work provides new insight into the support effect over the gold catalysts for selective hydrogenation reactions.



中文翻译:

水滑石的二价金属离子对负载型金纳米催化剂催化3-硝基苯乙烯化学选择加氢反应的影响

二价金属离子对水滑石(HT)(MAl-HT; M = Mg,Zn,Ni)负载的巯基化Au 25纳米团簇(NCs)的催化作用,该催化剂为3-硝基苯乙烯化学选择性加氢为3-乙烯基苯胺的前催化剂被调查了。在Au 25 / ZnAl-HT-300(在300°C下煅烧)催化剂上获得了最高的化学选择性,所需产物的选择性保持在98%以上。尽管金(3.2 nm)的粒径大于Au 25 / MgAl-HT-300(2.2 nm)和Au 25的粒径,Au 25 / NiAl-HT-300催化剂表现出最高的活性/ ZnAl-HT-300(1.7 nm)催化剂。CO吸附的原位漫反射红外傅里叶变换光谱(DRIFTS)结果表明,与金发生紧密相互作用的Ni容易被还原,从而影响了Au 25 / NiAl-HT-300催化剂的催化性能。此外,原位DRIFTS在10 bar氢气下吸附硝基苯乙烯的结果表明,除缩合路线外,它还遵循直接路线在Au 25 / NiAl-HT-300上生产苯胺,这与其他两种催化剂。这项工作为选择性加氢反应对金催化剂的支持作用提供了新的见解。

更新日期:2018-06-06
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