Pd-Au bimetallic catalysts supported on ZnO for selective 1,3-butadiene hydrogenation

被引:24
作者
Bachiller-Baeza, Belen [1 ]
Iglesias-Juez, Ana [1 ]
Agostini, Giovanni [2 ]
Castillejos-Lopez, Eva [3 ]
机构
[1] CSIC, Inst Catalisis & Petroleoquim, C Marie Curie 2, Madrid 28049, Spain
[2] European Synchrotron, ESRF, 71 Ave Martyrs, Grenoble 38000, France
[3] UNED, Fac Ciencias, Dept Quim Inorgan & Tecn, C Senda Rey 9, Madrid 28040, Spain
关键词
PD/ZNO CATALYSTS; SURFACE SITES; NANOPARTICLES; MORPHOLOGY; ALLOY; METAL; NANOSTRUCTURES; SPECTROSCOPY; ADSORPTION; BUTADIENE;
D O I
10.1039/c9cy02395j
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Bimetallic Pd-Au catalysts were synthesized using two differently shaped ZnO supports, ZnO-t (tetrapods) and ZnO-n (needles). These catalysts were tested in the partial hydrogenation of 1,3-butadiene and the results were compared to those for the corresponding monometallic catalysts of Pd. The structural and electronic properties of the catalysts were analysed by transmission electron microscopy and scanning transmission electron microscopy (TEM-STEM), Fourier transform infrared spectroscopy analysis of adsorbed CO (CO-FTIR), X-ray photoelectron spectroscopy (XPS) and in situ X-ray absorption spectroscopy (XAS) measurements combined with in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). On both catalysts, gold diffusion on the Pd(111) faces and formation of small Pd-rich particles and big Au-rich core/Pd-rich shell like structures were confirmed. Besides, both Pd-Au bimetallic samples gave similar conversion and selectivity values in the hydrogenation reaction. The product distribution resembled that for monometalic Pd on ZnO-t, except for the selectivity to 1-butene among the butenes which was slightly higher. The best catalyst in terms of selectivity to the butenes is Pd-ZnO-n. The differences found in the catalytic performance were analysed based on electronic and ensemble effects. In contrast to that found for the monometallic catalysts, the support morphology does not seem to be a determinant for the properties in the case of the Pd-Au bimetallic samples.
引用
收藏
页码:2503 / 2512
页数:10
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