Single Pd Atoms on θ-Al2O3 (010) Surface do not Catalyze NO Oxidation
Abstract
New convenient wet chemistry synthetic routes have made it possible to explore catalytic activities of a variety of single supported atoms. The majority of single supported atoms have been synthesized on active supports which participate in oxidation reactions. The single supported atoms on inert substrates (e.g. alumina) are limited to Pt adatoms and Pd cations, and are generally active toward CO oxidation. In this manuscript, we show that single Pd atoms on -alumina show high CO oxidation activity; however, they exhibit no detectable NO oxidation under our experimental conditions. This led us to employ first principles modeling to explore multiple Langmuir-Hinshelwood-type pathways to explain high CO oxidation activity but lack of NO oxidation activity. For completeness, we have also examined Eley-Riedel pathways. We find that a pathway that involves carbonate or nitrate as an intermediate can explain the experimental results of CO and NO oxidation on single alumina supported Pd cations.
- Authors:
-
[1];
[2];
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy & Transportation Science Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1349596
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Narula, Chaitanya K., Allard, Lawrence F., Moses-DeBusk, Melanie, Stocks, G. Malcom, and Wu, Zili. Single Pd Atoms on θ-Al2O3 (010) Surface do not Catalyze NO Oxidation. United States: N. p., 2017.
Web. doi:10.1038/s41598-017-00577-y.
Narula, Chaitanya K., Allard, Lawrence F., Moses-DeBusk, Melanie, Stocks, G. Malcom, & Wu, Zili. Single Pd Atoms on θ-Al2O3 (010) Surface do not Catalyze NO Oxidation. United States. https://doi.org/10.1038/s41598-017-00577-y
Narula, Chaitanya K., Allard, Lawrence F., Moses-DeBusk, Melanie, Stocks, G. Malcom, and Wu, Zili. Mon .
"Single Pd Atoms on θ-Al2O3 (010) Surface do not Catalyze NO Oxidation". United States. https://doi.org/10.1038/s41598-017-00577-y. https://www.osti.gov/servlets/purl/1349596.
@article{osti_1349596,
title = {Single Pd Atoms on θ-Al2O3 (010) Surface do not Catalyze NO Oxidation},
author = {Narula, Chaitanya K. and Allard, Lawrence F. and Moses-DeBusk, Melanie and Stocks, G. Malcom and Wu, Zili},
abstractNote = {New convenient wet chemistry synthetic routes have made it possible to explore catalytic activities of a variety of single supported atoms. The majority of single supported atoms have been synthesized on active supports which participate in oxidation reactions. The single supported atoms on inert substrates (e.g. alumina) are limited to Pt adatoms and Pd cations, and are generally active toward CO oxidation. In this manuscript, we show that single Pd atoms on -alumina show high CO oxidation activity; however, they exhibit no detectable NO oxidation under our experimental conditions. This led us to employ first principles modeling to explore multiple Langmuir-Hinshelwood-type pathways to explain high CO oxidation activity but lack of NO oxidation activity. For completeness, we have also examined Eley-Riedel pathways. We find that a pathway that involves carbonate or nitrate as an intermediate can explain the experimental results of CO and NO oxidation on single alumina supported Pd cations.},
doi = {10.1038/s41598-017-00577-y},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {Mon Apr 03 00:00:00 EDT 2017},
month = {Mon Apr 03 00:00:00 EDT 2017}
}
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Works referencing / citing this record:
Ab Initio Density Functional Calculations and Infra-Red Study of CO Interaction with Pd Atoms on θ-Al2O3 (010) Surface
journal, July 2017
- Narula, Chaitanya K.; Allard, Lawrence F.; Wu, Zili
- Scientific Reports, Vol. 7, Issue 1