Role of the surface-subsurface interlayer interaction in enhancing oxygen hydrogenation to water in Pd3Co alloy catalysts

被引:10
|
作者
Manogaran, Dhivya [1 ]
Hwang, Gyeong S. [2 ]
机构
[1] Univ Texas Austin, Dept Chem & Biochem, Austin, TX 78712 USA
[2] Univ Texas Austin, Dept Chem Engn, Austin, TX 78712 USA
关键词
REDUCTION REACTION; ELECTROCATALYSTS; NANOPARTICLES; STABILITY; PLATINUM; PT(111); FE;
D O I
10.1039/c3cp50618e
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
Based on density functional theory calculations, we present mechanisms underlying the improvement in the catalytic performance of Pd-based alloys for oxygen hydrogenation to water. As a model case, we consider the Pd/Pd3Co system where one or two Pd overlayers are located on top of the bimetallic substrate. Our calculations clearly demonstrate that the subsurface Co atoms assist in facilitating the oxygen reduction reaction by lowering the activation barriers for O/OH hydrogenation with a slight increase in the O-2 scission barrier; however, we also find that the Co atoms lying below the subsurface have no significant contribution in altering the surface reactivity towards oxygen hydrogenation. The analysis of intra- and interlayer orbital interactions in the near-surface region elucidates the synergetic interplay between the surface electronic structure modification due to the underlying Co atoms (interlayer ligand effect) and the compressive strain caused by the Pd3Co substrate. This result also brings to light the significant contribution of the out of plane (d(xz) and d(yz)) states in altering the surface reactivity towards O hydrogenation.
引用
收藏
页码:12118 / 12123
页数:6
相关论文
共 29 条
  • [1] Preparation and Characterization of Carbon-Titania Nanocomposite-Supported Pd3Co Alloy Nanoparticles for Oxygen Reduction
    Lim, Y.
    Bae, S. J.
    Kim, S.
    Lim, Y.
    Choi, J.
    Nahm, K. S.
    Kim, P.
    JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY, 2013, 13 (08) : 5698 - 5701
  • [2] Hydrogen Interaction (Electrosorption and Evolution) Characteristics of Pd and Pd3Co Alloy Nanoparticles: An In-situ Investigation with Electrochemical Impedance Spectroscopy
    Singh, Ramesh Kumar
    Ramesh, Rahul
    Devivaraprasad, Ruttala
    Chakraborty, Arup
    Neergat, Manoj
    ELECTROCHIMICA ACTA, 2016, 194 : 199 - 210
  • [3] CO ADSORPTION AND ITS INTERACTION WITH OXYGEN ON PD-CATALYSTS, CO-CATALYSTS AND PD-CO/AL2O3-CATALYSTS
    SAVELEVA, GA
    SASS, AS
    VOZDVIZHENSKII, VF
    TUNGATAROVA, SA
    POPOVA, NM
    ZHURNAL FIZICHESKOI KHIMII, 1988, 62 (04): : 1021 - 1025
  • [4] Role of the Various Surface Sites and Species in CO Hydrogenation Over Alumina-supported Co-Pd Catalysts
    Shopska, Maya G.
    Shtereva, Iskra Z.
    Kolev, Hristo G.
    Tenchev, Krasimir K.
    Todorova, Silviya Z.
    Kadinov, Georgi B.
    CROATICA CHEMICA ACTA, 2020, 93 (02) : 121 - 131
  • [5] Mechanistic Understanding of Alloy Effect and Water Promotion for Pd-Cu Bimetallic Catalysts in CO2 Hydrogenation to Methanol
    Nie, Xiaowa
    Jiang, Xiao
    Wang, Haozhi
    Luo, Wenjia
    Janik, Michael J.
    Chen, Yonggang
    Guo, Xinwen
    Song, Chunshan
    ACS CATALYSIS, 2018, 8 (06): : 4873 - 4892
  • [6] The role of subsurface oxygen in oscillatory behaviour of CO+O2 reaction over Pd metal catalysts:: Monte Carlo model
    Latkin, EI
    Elokhin, VI
    Matveev, AV
    Gorodetskii, VV
    JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2000, 158 (01) : 161 - 166
  • [7] AuPd alloy formation in Au-Pd/Al2O3 catalysts and its role on aromatics hydrogenation
    Pawelec, B
    Venezia, AM
    La Parola, V
    Cano-Serrano, E
    Campos-Martin, JM
    Fierro, JLG
    APPLIED SURFACE SCIENCE, 2005, 242 (3-4) : 380 - 391
  • [8] Co3O4/rGO Catalysts for Oxygen Electrocatalysis: On the Role of the Oxide/Carbon Interaction
    Abidat, I.
    Cazayus, E.
    Loupias, L.
    Morais, C.
    Comminges, C.
    Napporn, T. W.
    Portehault, D.
    Durupthy, O.
    Mamede, A-S.
    Chaneac, C.
    Lamonier, J. -F.
    Habrioux, A.
    Kokoh, K. B.
    JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2019, 166 (04) : H94 - H102
  • [9] Role of Surface Iron in Enhanced Activity for the Oxygen Reduction Reaction on a Pd3Fe(111) Single-Crystal Alloy
    Yang, Xiaofang
    Hu, Jun
    Fu, Jie
    Wu, Ruqian
    Koel, Bruce E.
    ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (43) : 10182 - 10185
  • [10] Infrared studies of CO oxidation by oxygen and by water over Pt/Al2O3 and Pd/Al2O3 catalysts
    Busca, Guido
    Finocchio, Elisabetta
    Sanchez Escribano, Vicente
    APPLIED CATALYSIS B-ENVIRONMENTAL, 2012, 113 : 172 - 179