PdZn Intermetallic Nanostructure with Pd-Zn-Pd Ensembles for Highly Active and Chemoselective Semi-Hydrogenation of Acetylene

doi:10.1021/acscatal.5b01933

	PdZn Intermetallic Nanostructure with Pd-Zn-Pd Ensembles for Highly Active and Chemoselective Semi-Hydrogenation of Acetylene
	Zhou, Huiran 1,3; Yang, Xiaofeng 1; Li, Lin 1; Liu, Xiaoyan 1; Huang, Yanqiang 1; Pan, Xiaoli 1; Wang, Aiqin 1; Li, Jun 2; Zhang, Tao 1
刊名	ACS CATALYSIS
	2016-02-01
卷号	6 期号:2 页码:1054-1061
关键词	Pd-zn-pd Ensembles Pdzn Chemoselectivity Acetylene Semihydrogenation Microcalorimetry Density Functional Theory
ISSN号	2155-5435
DOI	10.1021/acscatal.5b01933
文献子类	Article
英文摘要	Intermetallic alloying of one active metal to another inert metal provides not only the improved dispersion of active centers but also a unique and homogeneous ensemble of active sites, thus offering new opportunities in a variety of reactions. Herein, we report that PdZn intermetallic nanostructure with Pd-Zn-Pd ensembles are both highly active and selective for the semihydrogenation of acetylene to ethylene, which is usually inaccessible due to the sequential hydrogenation to ethane. Microcalorimetric measurements and density functional theory calculations demonstrate that the appropriate spatial arrangement of Pd sites in the Pd-Zn-Pd ensembles of the PdZn alloy leads to the moderate sigma-bonding mode for acetylene with two neighboring Pd sites while the weak pi-bonding pattern of ethylene adsorption on the single Pd site, which facilitates the chemisorption toward acetylene and promotes the desorption of ethylene from the catalyst surface. As a result, it leads to the kinetic favor of the selective conversion of acetylene to ethylene.
WOS关键词	SINGLE-ATOM CATALYSTS ; GAS SHIFT REACTION ; SELECTIVE HYDROGENATION CATALYST ; PALLADIUM CATALYSTS ; ALLOY CATALYSTS ; UNSATURATED-HYDROCARBONS ; HETEROGENEOUS CATALYSIS ; ALKYNE HYDROGENATION ; SURFACE-STRUCTURES ; SUBSURFACE CARBON
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000369774900065
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/171160]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Wang, Aiqin; Zhang, Tao
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, iChEM Collaborat Innovat Ctr Chem Energy Mat, Dalian 116023, Peoples R China 2.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Zhou, Huiran,Yang, Xiaofeng,Li, Lin,et al. PdZn Intermetallic Nanostructure with Pd-Zn-Pd Ensembles for Highly Active and Chemoselective Semi-Hydrogenation of Acetylene[J]. ACS CATALYSIS,2016,6(2):1054-1061.
APA	Zhou, Huiran.,Yang, Xiaofeng.,Li, Lin.,Liu, Xiaoyan.,Huang, Yanqiang.,...&Zhang, Tao.(2016).PdZn Intermetallic Nanostructure with Pd-Zn-Pd Ensembles for Highly Active and Chemoselective Semi-Hydrogenation of Acetylene.ACS CATALYSIS,6(2),1054-1061.
MLA	Zhou, Huiran,et al."PdZn Intermetallic Nanostructure with Pd-Zn-Pd Ensembles for Highly Active and Chemoselective Semi-Hydrogenation of Acetylene".ACS CATALYSIS 6.2(2016):1054-1061.