Activating Edge Sites on Pd Catalysts for Selective Hydrogenation of Acetylene via Selective Ga2O3 Decoration

被引:106
作者
Ding, Liangbing [1 ,2 ,3 ]
Yi, Hong [2 ,3 ]
Zhang, Wenhua [2 ,4 ]
You, Rui [1 ,2 ,3 ]
Cao, Tian [1 ,2 ,3 ]
Yang, Jinlong [1 ,3 ]
Lu, Junling [2 ,3 ]
Huang, Weixin [1 ,2 ,3 ]
机构
[1] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Jinzhai Rd 96, Hefei 230026, Peoples R China
[2] Univ Sci & Technol China, CAS Key Lab Mat Energy Convers, Jinzhai Rd 96, Hefei 230026, Peoples R China
[3] Univ Sci & Technol China, Dept Chem Phys, Jinzhai Rd 96, Hefei 230026, Peoples R China
[4] Univ Sci & Technol China, Dept Mat Sci & Engn, Jinzhai Rd 96, Hefei 230026, Peoples R China
来源
ACS CATALYSIS | 2016年 / 6卷 / 06期
基金
中国国家自然科学基金;
关键词
atomic layer deposition; activity; selectivity; stability; subsurface carbon; density functional theory; ATOMIC LAYER DEPOSITION; ETHENE-RICH STREAMS; PALLADIUM CATALYSTS; SUBSURFACE CARBON; KINETICS; ETHYLENE; NANOPARTICLES; SURFACES; ETHYNE; SPECTROSCOPY;
D O I
10.1021/acscatal.6b00702
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
Pd catalysts are industrially used in the selective hydrogenation of acetylene to ethylene. Terrace Pd atoms of the closely packed {111} facets on supported Pd particles are generally considered to be the catalytically active sites. We herein report that deposition of an appropriate amount of Ga203 adlayers on Pd particles supported on alumina by the atomic layer deposition (ALD) technique substantially enhanced the catalytic activity, selectivity, and stability in the selective hydrogenation of acetylene to ethylene. Structural characterization results demonstrate that Ga203 is preferentially deposited at the edges and open facets of Pd particles with the ALD technique. This transforms the poisoning edge sites of the {111} facets into the catalytically active terrace -like sites, leading to an increase in the number of active sites and subsequently the enhancement of the catalytic activity; this also suppresses the formation of poisoning carbonaceous deposits on the open facets and blocks the migration of carbonaceous deposits from the open facets to the neighboring active {111} facets, leading to a significant improvement in catalytic stability. These results demonstrate a concept of selective oxide decoration to comprehensively improve the performance of supported metal catalysts and provide a practical strategy.
引用
收藏
页码:3700 / 3707
页数:8
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