Effects of divalent metal ions of hydrotalcites on catalytic behavior of supported gold nanocatalysts for chemoselective hydrogenation of 3-nitrostyrene
Effects of divalent metal ions of hydrotalcites on catalytic behavior of supported gold nanocatalysts for chemoselective hydrogenation of 3-nitrostyrene
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水滑石二价金属离子对负载金纳米催化剂化学选择性加氢3-硝基苯乙烯催化行为的影响
DOI：
10.1016/j.jcat.2018.05.007
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发表时间：
2018-08
影响因子：
7.3
通讯作者：
Zhang Tao
中科院分区：
文献类型：
--
作者：
Tan Yuan;Liu Xiao Yan;Li Lin;Karig Leilei;Wang Aiqin;Zhang Tao
研究了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（NC）作为3-硝基苯乙烯化学选择性加氢合成3-乙烯基苯胺的预催化剂的影响。在Au 25/ZnAl-HT-300（在300 °C下煅烧）催化剂上获得最高的化学选择性，其中所需产物的选择性保持在98%以上。Au 25/NiAl-HT-300催化剂表现出最高的活性，尽管金的颗粒尺寸（3.2 nm）大于Au 25/MgAl-HT-300（2.2 nm）和Au 25/ZnAl-HT-300（1.7 nm）催化剂。原位漫反射红外光谱（DRIFTS）结果表明，Au 25/NiAl-HT-300催化剂中与Au相互作用密切的Ni容易被还原，从而影响催化剂的催化性能。原位DRIFTS结果表明，在Au 25/NiAl-HT-300催化剂上，苯胺的生成除了缩合途径外，还遵循直接途径，这与其它两种催化剂不同。这项工作提供了新的见解，支持在选择性加氢反应的金催化剂的效果。
The effect of the divalent metal ions on the hydrotalcite (HT) (MAl-HT; M = Mg, Zn, Ni)-supported thiolated Au25nanoclusters (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.
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影响因子：
15
作者：
Praneeth Reddy Nimmala;A. Dass
通讯作者：
Praneeth Reddy Nimmala;A. Dass
影响因子：
4.9
作者：
Jagadeesh, Rajenahally V.;Wienhoefer, Gerrit;Beller, Matthias
通讯作者：
Beller, Matthias
影响因子：
5.2
作者：
Takasaki, Mikihiro;Motoyama, Yukihiro;Nagashima, Hideo
通讯作者：
Nagashima, Hideo
影响因子：
6.2
作者：
Duval, Antoine;Lange, Heiko;Crestini, Claudia
通讯作者：
Crestini, Claudia
影响因子：
4.7
作者：
Petri A. Rautanen;J. Aittamaa;A. Krause
通讯作者：
Petri A. Rautanen;J. Aittamaa;A. Krause