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A study on structural features of bimetallic Pd-M/C (M: Zn, Ga, Ag) catalysts for liquid-phase selective hydrogenation of acetylene
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2018-06-27 , DOI: 10.1016/j.apcata.2018.06.029
Daria V. Glyzdova , Aleksey A. Vedyagin , Anna M. Tsapina , Vasily V. Kaichev , Alexander L. Trigub , Mikhail V. Trenikhin , Dmitry A. Shlyapin , Pavel G. Tsyrulnikov , Alexander V. Lavrenov

The present work is devoted to the study of doping effects of zinc, gallium and silver on the structure of active sites and catalytic properties of carbon-supported 0.5 wt% Pd catalysts in the liquid-phase selective hydrogenation of acetylene to ethylene. Carbonaceous graphite-like material Sibunit was used as a support. The reaction was performed in a medium of N-methyl-2-pyrrolidone at 55 °C. It was shown that the bimetallic Pd-Zn/C, Pd-Ga/C and Pd-Ag/C catalysts exhibit better activity and selectivity towards target product if compare with the monometallic Pd/C catalyst. The ethylene yield increases in a row as follows: Pd/C (19%) < Pd-Ag/C (34%) < Pd-Ga/C (42%) < Pd-Zn/C (53%). Using X-ray absorption spectroscopy and transmission electron microscopy it was found that an improvement of the selectivity is stipulated by the formation of bimetallic PdZn, PdxGay and PdAg nanophases. In the case of Pd-Zn/C and Pd-Ag/C systems, an increased distance between neighboring Pd atoms (2.82–2.89 Å) in relation with monometallic Pd/C, where this distance is 2.72 Å, was observed. The higher activity of modified bimetallic systems is connected with increased number of active sites due to enhanced dispersity of supported palladium doped with second metal.



中文翻译:

乙炔液相选择性加氢的双金属Pd-M / C(M:Zn,Ga,Ag)催化剂的结构特征研究

目前的工作致力于锌,镓和银对乙炔液相选择性加氢制乙烯反应中活性部位的结构和碳负载的0.5 wt%Pd催化剂的催化性能的掺杂作用的研究。碳质石墨状材料Sibunit用作载体。反应在N的介质中进行-甲基-2-吡咯烷酮在55℃。结果表明,与单金属Pd / C催化剂相比,双金属Pd-Zn / C,Pd-Ga / C和Pd-Ag / C催化剂表现出更好的活性和对目标产物的选择性。乙烯收率连续增加如下:Pd / C(19%)<Pd-Ag / C(34%)<Pd-Ga / C(42%)<Pd-Zn / C(53%)。使用X射线吸收光谱法和透射电子显微镜发现,通过形成双金属PdZn,Pd x Ga y可以提高选择性。和PdAg纳米相。在Pd-Zn / C和Pd-Ag / C系统的情况下,观察到相邻Pd原子之间的距离(2.82-2.89Å)相对于单金属Pd / C而言增加了,该距离为2.72Å。改性双金属体系的较高活性与活性位点数目的增加有关,这归因于掺杂有第二种金属的负载钯的分散性增强。

更新日期:2018-06-27
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