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Title: CO 2 hydrogenation on Pt, Pt/SiO 2 and Pt/TiO 2: Importance of synergy between Pt and oxide support

In this paper we combined density functional theory (DFT), kinetic Monte Carlo (KMC) simulations and experimental measurements to gain insight into the mechanisms of CO 2 conversion by hydrogen on the Pt nanoparticle (NP). The results show that in spite of the presence of active, low-coordinated sites, Pt NP alone is not able to catalyze the reaction due to the weak CO 2 binding on the catalyst. Once CO 2 is stabilized, the hydrogenation of CO 2 to CO via the reverse-water–gas shift (RWGS) reaction is promoted; in contrast, the enhancement for further *CO hydrogenation to CH 4 is less significant and no CH 3OH is observed. The selectivity to CO is mainly determined by CO binding energy and the energetics of *CO hydrogenation to *HCO, while that for CH 4 and CH 3OH is determined by the competition between hydrogenation and C–O bond scission reactions of the *H 2COH species. Using SiO 2 and TiO 2 as the support, Pt NP is able to promote the overall CO 2 conversion, while the impact on the selectivity is rather small. The theoretically predicted trend in activity and selectivity is in good agreement with the experimental results. Finally, the enhanced activitymore » of Pt/oxide over Pt is originated from the sites at the Pt–oxide interface, where the synergy between Pt and oxide plays an important role.« less
 [1] ;  [2] ;  [3] ;  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.; Tsinghua Univ., Beijing (China). Dept. of Chemical Engineering
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.; Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
Publication Date:
Report Number(s):
Journal ID: ISSN 0021-9517; R&D Project: CO035; KC0302010
Grant/Contract Number:
SC0012704; AC02-05CH11231; AC05-00OR22725
Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 343; Journal ID: ISSN 0021-9517
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Orgs:
Tsinghua Univ., Beijing (China); Columbia Univ., New York, NY (United States)
Country of Publication:
United States
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 activation; Selectivity; Activity; Kinetics; DFT; Platinum
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1398838