Preparation and structure-property relationships of supported trimetallic PdAuAg catalysts for the selective hydrogenation of acetylene

被引:53
|
作者
Feng, Junting [1 ]
Liu, Yanan [1 ]
Yin, Min [1 ]
He, Yufei [1 ]
Zhao, Jiaying [1 ]
Sun, Jianhua [2 ]
Li, Dianqing [1 ]
机构
[1] Beijing Univ Chem Technol, State Key Lab Chem Engn, Beijing 100029, Peoples R China
[2] Guangxi Univ, Guangxi Key Lab Petrochem Resource Proc & Proc In, Nanning 530004, Peoples R China
关键词
Selective hydrogenation; PdAuAg trimetallic catalyst; Synergetic effect; Mesocrystals; Defect sites; DENSITY-FUNCTIONAL THEORY; ALKYNE HYDROGENATION; PD CATALYST; SURFACE CHARACTERIZATION; PD/GAMMA-AL2O3; CATALYST; BIMETALLIC CATALYSTS; SUBSURFACE CARBON; LOW-TEMPERATURE; WO3; NANORODS; NANOPARTICLES;
D O I
10.1016/j.jcat.2016.08.003
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
To simultaneously achieve thorough purification of acetylene and maximum ethene increment, a sea urchinlike trimetallic PdAuAg mesocrystal catalyst as targeting sample and cuboctahedral trimetallic PdAuAg and bimetallic catalyst as control samples were prepared by a co-reduction method, immobilized on MgAl hydrotalcite. Compared with bimetallic PdAu and PdAg catalysts, trimetallic PdAuAgx catalyst gave prior selectivity due to the positive synergetic effect. Significantly, PdAuAg2 mesocrystal catalyst exhibited a turnover frequency of 0.063 s(-1), 46.5% higher than that of cuboctahedral PdAuAg2 catalyst. A 76.2% ethene selectivity was achieved for the thorough purification of acetylene over PdAuAg mesocrystal catalyst with H-2:C2H2 of 2:1. Further improving H-2:C2H2 to 3, 76.5% yield can be maintained at 140 degrees C. Enhanced activity of the mesocrystal catalyst could be attributed to a high concentration of defect sites and a low activation barrier. Improved ethene selectivity could be ascribed to the increase in the (111)/(100) facets ratio and the formation of a Pd-C phase. (C) 2016 Elsevier Inc. All rights reserved.
引用
收藏
页码:854 / 864
页数:11
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