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Title: Exploring the activity of a novel Au/TiC(001) model catalyst towards CO and CO2 hydrogenation

Small metallic nanoparticles supported on transition metal carbides exhibit an unexpected high activity towards a series of chemical reactions. In particular, the Au/TiC system has proven to be an excellent catalyst for SO2 decomposition, thiophene hydrodesulfurization, O2 and H2 dissociation and the water gas shift reaction. Recent studies have shown that Au/TiC is a very good catalyst for the reverse water–gas shift (CO2 + H2 → CO + H2O) and CO2 hydrogenation to methanol. The present work further expands the range of applicability of this novel type of systems by exploring the catalytic activity of Au/TiC towards the hydrogenation of CO or CO2 with periodic density functional theory (DFT) calculations on model systems. Hydrogen dissociates easily on Au/TiC but direct hydrogenation of CO to methanol is hindered by very high activation barriers implying that, on this model catalyst, methanol production from CO2 involves the hydrogenation of a HOCO-like intermediate. Thus, when dealing with mixtures of syngas (CO/CO2/H2/H2O), CO could be transformed into CO2 through the water gas shift reaction with subsequent hydrogenation of CO2 to methanol.
Authors:
 [1] ;  [2] ;  [3] ;  [4]
  1. Univ. Rovira i Virgili C/Marcel-li Domingo, Tarragona (Spain); Univ. de Barcelona, Barcelona (Spain)
  2. Univ. Rovira i Virgili C/Marcel-li Domingo, Tarragona (Spain)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Univ. de Barcelona, Barcelona (Spain)
Publication Date:
OSTI Identifier:
1224763
Report Number(s):
BNL--108473-2015-JA
Journal ID: ISSN 0039-6028; R&D Project: CO009; KC0302010
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
Surface Science
Additional Journal Information:
Journal Volume: 640; Journal Issue: C; Journal ID: ISSN 0039-6028
Publisher:
Elsevier
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY syngas; methanol synthesis; CO; CO2; Au/TiC; DFT