Alumina-Supported Palladium-Silver Bimetallic Catalysts with Single-Atom Pd1 Sites in the Liquid-Phase Hydrogenation of Substituted Alkynes

被引:16
作者
Rassolov, A., V [1 ]
Bragina, G. O. [1 ]
Baeva, G. N. [1 ]
Mashkovsky, I. S. [1 ]
Stakheev, A. Yu [1 ]
机构
[1] Russian Acad Sci, Zelinsky Inst Organ Chem, Moscow 119991, Russia
基金
俄罗斯科学基金会;
关键词
single-atom alloy catalysts; isolated Pd-1 sites; bimetallic catalysts; Pd– Ag; heterogeneous catalysts; liquid-phase hydrogenation; diphenylacetylene; 1-phenyl-1-propyne; SELECTIVE HYDROGENATION; SURFACE SEGREGATION; CU/AL2O3; CATALYSTS; ACETYLENE; AG; PHENYLACETYLENE; SEMIHYDROGENATION; METAL; MECHANISM; ETHYLENE;
D O I
10.1134/S0023158420060129
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
The catalytic characteristics of Pd-Ag/Al2O3 bimetallic catalysts with an Ag/Pd atomic ratio of 0.03-3.0 have been studied in the selective liquid-phase hydrogenation of diphenylacetylene and 1-phenyl-1-propyne. It has been found that an increase in the Ag/Pd ratio leads to a significant increase in selectivity, which, however, is accompanied by a decrease in the catalyst activity. Comparison with data of an earlier structural study suggests that an increase in selectivity observed with an increase in the Ag/Pd ratio to 0.5-1.0 is attributed to the following two factors: (1) the suppression of the formation of palladium hydride and (2) an increase in the fraction of "single-atom" Pd-1 sites isolated from each other by Ag atoms on the surface of the Pd-Ag nanoparticles. An increase in the Ag/Pd value to 2.0-3.0 leads to a further increase in the selectivity, which exceeds the selectivity of a commercial Lindlar catalyst (Pd-Pb/CaCO3). In this case, the most probable cause of the high selectivity is the formation of the single-atom Pd-1 sites on the surface of the Pd-Ag alloy and an increase in the stability of the structure.
引用
收藏
页码:869 / 878
页数:10
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