Performance of Cu-Alloyed Pd Single-Atom Catalyst for Semihydrogenation of Acetylene under Simulated Front-End Conditions

doi:10.1021/acscatal.6b03293

	Performance of Cu-Alloyed Pd Single-Atom Catalyst for Semihydrogenation of Acetylene under Simulated Front-End Conditions
	Zhang, Tao 1; Liu, Xiao Yan 1; Yang, Xiaofeng 1; Zhang, Leilei 1; Wang, Aiqin 1; Pei, Guang Xian 1,2; Li, Lin 1; Wang, Hua 1; Wang, Xiaodong 1
刊名	ACS CATALYSIS
	2017-02-01
卷号	7 期号:2 页码:1491-1500
关键词	Cu Pd Single Atom Xas Acetylene Hydrogenation Excess Ethylene Microcalorimetry H-2 Adsorption Ib Metal
ISSN号	2155-5435
DOI	10.1021/acscatal.6b03293
文献子类	Article
英文摘要	Selective hydrogenation of acetylene to ethylene is an industrially important reaction. Pd-based catalysts have been proved to be efficient for the acetylene conversion, while enhancing the selectivity to ethylene is challenging. Here, we chose Cu as the partner of Pd, fabricated an alloyed Pd single-atom catalyst (SAC), and investigated its catalytic performance for the selective hydrogenation of acetylene to ethylene under a simulated front-end hydrogenation process in industry: that is, with a high concentration of hydrogen and ethylene. The Cu-alloyed Pd SAC showed similar to 85% selectivity to ethylene and 100% acetylene elimination. In comparison with the Au- or Ag-alloyed Pd SAC, the Cu-alloyed analogue exceeded both of them in conversion, while the selectivity rivaled that of the Ag-alloyed Pd SAC and surpassed that of the Au-alloyed Pd SAC. As Cu is a low-cost metal, Cu-alloyed Pd SAC would minimize the noble-metal usage and possess high utilization potential for industry. The Cu-alloyed Pd SAC was verified by EXAFS, with the Pd/Cu atomic ratio lowered to 0.006, corresponding to the loading of Pd at 494 ppm. The microcalorimetric measurement results demonstrated that the adsorption of C2H4 over the Cu-alloyed Pd SAC was weaker than that over the catalyst with large Pd ensembles; thus, the selectivity to ethylene was greatly enhanced. At the same time, the adsorption of H-2 was stronger than that over the corresponding monometallic Cu catalyst; thus, the activation of H-2 was obviously promoted. On the basis of the above results, a possible reaction path over the Cu-alloyed Pd SAC was proposed. Furthermore, by systematic comparison of the IB-metal-alloyed Pd SACs, we found that the apparent activation energies of the IB-metal-alloyed Pd SACs were close to each other, indicating similar active sites and/or catalytic mechanisms over the three catalysts. The isolation of the Pd atoms by the IB metal distinctly contributed to both the conversion and the selectivity. Further DFT calculation results suggested that electron transfer between the IB metal and Pd might be responsible for their different selectivities to ethylene.
WOS关键词	AUGMENTED-WAVE METHOD ; GAS SHIFT REACTION ; SELECTIVE HYDROGENATION ; BIMETALLIC CATALYSTS ; EXCESS ETHYLENE ; HETEROGENEOUS CATALYSIS ; PD/SIO2 CATALYSTS ; C2H4 ADSORPTION ; PARTICLE-SIZE ; AG
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000393539200066
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/169642]
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	Zhang, Tao; Liu, Xiao Yan
作者单位	1.Chinese Acad Sci, State Key Lab Catalysis, iChEM Collaborat Innovat Ctr Chem Energy Mat, Dalian Inst Chem Phys, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Tao,Liu, Xiao Yan,Yang, Xiaofeng,et al. Performance of Cu-Alloyed Pd Single-Atom Catalyst for Semihydrogenation of Acetylene under Simulated Front-End Conditions[J]. ACS CATALYSIS,2017,7(2):1491-1500.
APA	Zhang, Tao.,Liu, Xiao Yan.,Yang, Xiaofeng.,Zhang, Leilei.,Wang, Aiqin.,...&Wang, Xiaodong.(2017).Performance of Cu-Alloyed Pd Single-Atom Catalyst for Semihydrogenation of Acetylene under Simulated Front-End Conditions.ACS CATALYSIS,7(2),1491-1500.
MLA	Zhang, Tao,et al."Performance of Cu-Alloyed Pd Single-Atom Catalyst for Semihydrogenation of Acetylene under Simulated Front-End Conditions".ACS CATALYSIS 7.2(2017):1491-1500.