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Title: CO2 hydrogenation on Pt, Pt/SiO2 and Pt/TiO2: Importance of synergy between Pt and oxide support

Abstract

In this paper we combined density functional theory (DFT), kinetic Monte Carlo (KMC) simulations and experimental measurements to gain insight into the mechanisms of CO2 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 CO2 binding on the catalyst. Once CO2 is stabilized, the hydrogenation of CO2 to CO via the reverse-water–gas shift (RWGS) reaction is promoted; in contrast, the enhancement for further *CO hydrogenation to CH4 is less significant and no CH3OH is observed. The selectivity to CO is mainly determined by CO binding energy and the energetics of *CO hydrogenation to *HCO, while that for CH4 and CH3OH is determined by the competition between hydrogenation and C–O bond scission reactions of the *H2COH species. Using SiO2 and TiO2 as the support, Pt NP is able to promote the overall CO2 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 activity of Pt/oxide over Pt is originated from the sites at the Pt–oxidemore » interface, where the synergy between Pt and oxide plays an important role.« less

Authors:
 [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:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Contributing Org.:
Tsinghua Univ., Beijing (China); Columbia Univ., New York, NY (United States)
OSTI Identifier:
1341672
Alternate Identifier(s):
OSTI ID: 1398838
Report Number(s):
BNL-113400-2017-JA
Journal ID: ISSN 0021-9517; R&D Project: CO035; KC0302010
Grant/Contract Number:  
SC0012704; AC02-05CH11231; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 343; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 activation; Selectivity; Activity; Kinetics; DFT; Platinum

Citation Formats

Kattel, Shyam, Yan, Binhang, Chen, Jingguang G., and Liu, Ping. CO2 hydrogenation on Pt, Pt/SiO2 and Pt/TiO2: Importance of synergy between Pt and oxide support. United States: N. p., 2016. Web. https://doi.org/10.1016/j.jcat.2015.12.019.
Kattel, Shyam, Yan, Binhang, Chen, Jingguang G., & Liu, Ping. CO2 hydrogenation on Pt, Pt/SiO2 and Pt/TiO2: Importance of synergy between Pt and oxide support. United States. https://doi.org/10.1016/j.jcat.2015.12.019
Kattel, Shyam, Yan, Binhang, Chen, Jingguang G., and Liu, Ping. Wed . "CO2 hydrogenation on Pt, Pt/SiO2 and Pt/TiO2: Importance of synergy between Pt and oxide support". United States. https://doi.org/10.1016/j.jcat.2015.12.019. https://www.osti.gov/servlets/purl/1341672.
@article{osti_1341672,
title = {CO2 hydrogenation on Pt, Pt/SiO2 and Pt/TiO2: Importance of synergy between Pt and oxide support},
author = {Kattel, Shyam and Yan, Binhang and Chen, Jingguang G. and Liu, Ping},
abstractNote = {In this paper we combined density functional theory (DFT), kinetic Monte Carlo (KMC) simulations and experimental measurements to gain insight into the mechanisms of CO2 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 CO2 binding on the catalyst. Once CO2 is stabilized, the hydrogenation of CO2 to CO via the reverse-water–gas shift (RWGS) reaction is promoted; in contrast, the enhancement for further *CO hydrogenation to CH4 is less significant and no CH3OH is observed. The selectivity to CO is mainly determined by CO binding energy and the energetics of *CO hydrogenation to *HCO, while that for CH4 and CH3OH is determined by the competition between hydrogenation and C–O bond scission reactions of the *H2COH species. Using SiO2 and TiO2 as the support, Pt NP is able to promote the overall CO2 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 activity 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.},
doi = {10.1016/j.jcat.2015.12.019},
journal = {Journal of Catalysis},
number = ,
volume = 343,
place = {United States},
year = {2016},
month = {1}
}

Journal Article:

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Cited by: 11 works
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