abstract
DFT based calculations were employed in the study of the dissociation of the water molecule onto copper and nickel (110) and (111) surface models, incorporating two additional metallic elements, because it was found previously that metal alloying leads to strong synergic effects in the catalysis of this reaction. The dissociation reaction was studied on the Pt/Ru/Ni, Pt/Ru/Cu, Rh/Ru/Cu, Ni/Ru/Cu and Al/Zn/Cu combinations, in a total of 25 trimetallic surfaces. Very low activation energy barriers for the dissociation of water were calculated on several of the surface models, suggesting that multimetallic surfaces can be interesting alternatives for catalyzing the dissociation of the water molecule, which is a crucial elementary step in the water gas shift reaction. Encouragingly, the calculations predict a facile dissociation of the water molecule onto the (AlZn) Cu(111) catalyst model which is in agreement with recent experimental studies where it was found that a Cu0.5Zn0.5Al2O4 spinel oxide catalyst holds improved activity for the water gas shift reaction. (C) 2017 Elsevier B.V. All rights reserved.
keywords
TRANSITION-METAL SURFACES; GAS SHIFT REACTION; GENERALIZED GRADIENT APPROXIMATION; TOTAL-ENERGY CALCULATIONS; AUGMENTED-WAVE METHOD; BASIS-SET; HYDROGEN; REACTIVITY; DESCRIPTORS; ACTIVATION
subject category
Chemistry; Engineering
authors
Fajin, JLC; Cordeiro, MNDS; Gomes, JRB
our authors
José R. B. Gomes
Principal Researcheracknowledgements
This work was developed within the scope of the projects CICECO-Aveiro Institute of Materials, POCI-01-0145-FEDER-007679 (FCT UID/CTM/50011/2013), LAQV@REQUIMTE, POCI/01/0145/FEDER/007265, (FCT UID/QUI/50006/2013 and NORTE-01-0145-FEDER-000011), financed by national funds through the FCT/MEC and when appropriate co-financed by FEDER under the PT2020 Partnership Agreement. J.L.C.F. and J.R.B.G. acknowledge FCT for the grant SFRH/BPD/105650/2015, cofinanced by the Programa Operacional Potential Humano (POPH)/Fundo Social Europeu (FSE) and Quadro de Referenda Estrategico Nacional 2009-2013 do Governo da Republica Portuguesa, and for the Programme Investigador FCT, respectively. M.N.D.S.C. also acknowledges FCT/MEC for Grant SFRH/BSAB/127789/2016.