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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.
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页码:854 / 864
页数:11
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