Structure Sensitivity of Acrolein Hydrogenation by Platinum Nanoparticles on Ba x Sr 1− x TiO 3 Nanocuboids
Abstract
Abstract The structure sensitivity of Pt nanoparticles (Pt N ) for gas‐phase acrolein (AC) hydrogenation was probed for Pt N on Ba x Sr 1− x TiO 3 nanocuboid supports with (0 0 1) facets in a combined theoretical and experimental study. The in situ selectivity for allyl alcohol increased with the increase of the Sr concentration in the support, which corresponds to modifications in the stable Winterbottom shape and lattice strain of the Pt nanoparticles as a result of the interfacial energy between Pt and the Ba x Sr 1− x TiO 3 supports. “Local model” nanofacets of the Pt surface, edge, and corner morphologies were developed as compact representations of adsorption and reaction sites. DFT was used as the primary modeling tool for the equilibrium adsorption states. We argue that adsorption on edge sites is critically important for the overall allyl alcohol selectivity of Pt N catalysts. A simple model was developed to represent Pt N strain effects caused by its interaction with the substrate. Bader topological atom, spherical volume averaging charge, and modified bond valence sum analyses were used to understand the bonding structure. Density of states analysis was performed for themore »
- Authors:
-
[2];
- Applied Physics Program Northwestern University Evanston IL 60208 USA
- Department of Chemistry Northwestern University Evanston IL 60208 USA
- Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL USA
- Department of Chemistry Northwestern University Evanston IL 60208 USA, Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL USA
- Applied Physics Program Northwestern University Evanston IL 60208 USA, Department of Chemistry Northwestern University Evanston IL 60208 USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1464548
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Name: ChemCatChem Journal Volume: 10 Journal Issue: 3; Journal ID: ISSN 1867-3880
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Engelhardt, Christopher M., Kennedy, Robert M., Enterkin, James A., Poeppelmeier, Kenneth R., Ellis, Donald E., Marshall, Christopher L., and Stair, Peter C. Structure Sensitivity of Acrolein Hydrogenation by Platinum Nanoparticles on Ba x Sr 1− x TiO 3 Nanocuboids. Germany: N. p., 2018.
Web. doi:10.1002/cctc.201701505.
Engelhardt, Christopher M., Kennedy, Robert M., Enterkin, James A., Poeppelmeier, Kenneth R., Ellis, Donald E., Marshall, Christopher L., & Stair, Peter C. Structure Sensitivity of Acrolein Hydrogenation by Platinum Nanoparticles on Ba x Sr 1− x TiO 3 Nanocuboids. Germany. https://doi.org/10.1002/cctc.201701505
Engelhardt, Christopher M., Kennedy, Robert M., Enterkin, James A., Poeppelmeier, Kenneth R., Ellis, Donald E., Marshall, Christopher L., and Stair, Peter C. Fri .
"Structure Sensitivity of Acrolein Hydrogenation by Platinum Nanoparticles on Ba x Sr 1− x TiO 3 Nanocuboids". Germany. https://doi.org/10.1002/cctc.201701505.
@article{osti_1464548,
title = {Structure Sensitivity of Acrolein Hydrogenation by Platinum Nanoparticles on Ba x Sr 1− x TiO 3 Nanocuboids},
author = {Engelhardt, Christopher M. and Kennedy, Robert M. and Enterkin, James A. and Poeppelmeier, Kenneth R. and Ellis, Donald E. and Marshall, Christopher L. and Stair, Peter C.},
abstractNote = {Abstract The structure sensitivity of Pt nanoparticles (Pt N ) for gas‐phase acrolein (AC) hydrogenation was probed for Pt N on Ba x Sr 1− x TiO 3 nanocuboid supports with (0 0 1) facets in a combined theoretical and experimental study. The in situ selectivity for allyl alcohol increased with the increase of the Sr concentration in the support, which corresponds to modifications in the stable Winterbottom shape and lattice strain of the Pt nanoparticles as a result of the interfacial energy between Pt and the Ba x Sr 1− x TiO 3 supports. “Local model” nanofacets of the Pt surface, edge, and corner morphologies were developed as compact representations of adsorption and reaction sites. DFT was used as the primary modeling tool for the equilibrium adsorption states. We argue that adsorption on edge sites is critically important for the overall allyl alcohol selectivity of Pt N catalysts. A simple model was developed to represent Pt N strain effects caused by its interaction with the substrate. Bader topological atom, spherical volume averaging charge, and modified bond valence sum analyses were used to understand the bonding structure. Density of states analysis was performed for the structures of Pt N , adsorbed AC, and intermediate products to examine adsorbate–particle interactions. The simulated hydrogenation of AC on Pt N nanofacets was compared to the in situ hydrogenation of AC by Pt N on Ba x Sr 1− x TiO 3 to examine the effects of facet, edge, and corner sites on the overall selectivity.},
doi = {10.1002/cctc.201701505},
journal = {ChemCatChem},
number = 3,
volume = 10,
place = {Germany},
year = {Fri Jan 05 00:00:00 EST 2018},
month = {Fri Jan 05 00:00:00 EST 2018}
}
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