Propyne Hydrogenation over a Pd/Cu(111) Single-Atom Alloy Studied using Ambient Pressure Infrared Spectroscopy

被引:24
作者
Abdel-Rahman, Mohammed K. [1 ]
Trenary, Michael [1 ]
机构
[1] Univ Illinois, Dept Chem, Chicago, IL 60607 USA
基金
美国国家科学基金会;
关键词
propyne; methylacetylene; selective hydrogenation; kinetics; single-atom alloy; RAIRS; Cu(111); turnover frequency; SELECTIVE HYDROGENATION; PALLADIUM; METHYLACETYLENE; ADSORPTION; PLATINUM; CU(111); COPPER; PROPYLENE; CATALYSTS;
D O I
10.1021/acscatal.0c02475
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
The hydrogenation of propyne (C3H4) to propene (C3H6) using a Pd/Cu(111) single-atom alloy (SAA) has been studied using polarization-dependent reflection absorption infrared spectroscopy. This method allows for simultaneous monitoring of reactants and products in the gas phase and species adsorbed on the surface during the reaction. The results were compared with the hydrogenation of propyne using Pd-free Cu(111) as well as with previous studies on Pd/Cu SAA catalysts supported on alumina. Propene production occurs at temperatures of 383 K and above as indicated by the appearance of an infrared peak at 912 cm(-1), which is a unique characteristic feature of gas phase propene. Propyne was found to adsorb on the surface at 300 K in the presence of gas phase propyne to form a di-s/di-p structure, as the spectrum was identical to that reported in the literature for propyne adsorbed on Cu(111) at 150 K in ultrahigh vacuum. The presence of a carbonaceous layer on the surface is indicated by a dramatic increase in the intensity of a peak at 2968 cm(-1) at temperatures above 400 K. The progression of gas phase peaks at 912 and 3322 cm-1 was used to calculate the rate of production of propene and the rate of consumption of propyne, respectively. This reaction rate was used to determine a turnover frequency of 25.4 s(-1) at 383 K for the reaction on the Pd/Cu(111) SAA surface. The reaction was not impeded by the presence of the carbonaceous layer, even for a layer so thick that only carbon was detectable on the surface with Auger electron spectroscopy.
引用
收藏
页码:9716 / 9724
页数:9
相关论文
共 33 条
  • [1] Submonolayer growth of Pd on Cu(111) studied by scanning tunneling microscopy
    Aaen, AB
    Laegsgaard, E
    Ruban, AV
    Stensgaard, I
    [J]. SURFACE SCIENCE, 1998, 408 (1-3) : 43 - 56
  • [2] Permanent alkene selectivity enhancement in copper-catalyzed propyne hydrogenation by temporary CO supply
    Bridier, Blaise
    Hevia, Miguel A. G.
    Lopez, Nuria
    Perez-Ramirez, Javier
    [J]. JOURNAL OF CATALYSIS, 2011, 278 (01) : 167 - 172
  • [3] Partial hydrogenation of propyne over copper-based catalysts and comparison with nickel-based analogues
    Bridier, Blaise
    Lopez, Nuria
    Perez-Ramirez, Javier
    [J]. JOURNAL OF CATALYSIS, 2010, 269 (01) : 80 - 92
  • [4] A FOURIER-TRANSFORM REFLECTION-ABSORPTION INFRARED SPECTROSCOPIC STUDY OF ALKYNE ADSORPTION ON CU(111)
    CHESTERS, MA
    MCCASH, EM
    [J]. JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA, 1987, 44 : 99 - 108
  • [5] A theoretical study of catalytic coupling of propyne on Cu{111}
    Clotet, A
    Ricart, JM
    Illas, F
    Pacchioni, G
    Lambert, RM
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2000, 122 (31) : 7573 - 7578
  • [6] Lonely Atoms with Special Gifts: Breaking Linear Scaling Relationships in Heterogeneous Catalysis with Single-Atom Alloys
    Darby, Matthew T.
    Stamatakis, Michail
    Michaelides, Angelos
    Sykes, E. Charles H.
    [J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2018, 9 (18): : 5636 - 5646
  • [7] SYMMETRY AND THE SURFACE INFRARED SELECTION RULE FOR THE DETERMINATION OF THE STRUCTURE OF MOLECULES ON METAL-SURFACES
    FAN, JF
    TRENARY, M
    [J]. LANGMUIR, 1994, 10 (10) : 3649 - 3657
  • [8] Interplay between carbon monoxide, hydrides, and carbides in selective alkyne hydrogenation on palladium
    Garcia-Mota, Monica
    Bridier, Blaise
    Perez-Ramirez, Javier
    Lopez, Nuria
    [J]. JOURNAL OF CATALYSIS, 2010, 273 (02) : 92 - 102
  • [9] Propene adsorption on Ag(111): a TPD and RAIRS study
    Huang, WX
    White, JM
    [J]. SURFACE SCIENCE, 2002, 513 (02) : 399 - 404
  • [10] HYDROGENATION OF PROPYNE OVER PALLADIUM CATALYSTS
    JACKSON, SD
    CASEY, NJ
    [J]. JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1995, 91 (18): : 3269 - 3274