CO Adsorption on Au Nanoparticles Grown on Hexagonal Boron Nitride/Rh(111)
Abstract
CO adsorption on size-controlled Au nanoparticles grown on an $$h$$-BN/Rh(111) nanomesh surface has been examined to probe their potential catalytic properties. A combination of high-resolution electron energy loss spectroscopy (HREELS), temperature-programmed desorption (TPD), and density functional theory (DFT) calculations demonstrate that the CO adsorption strength depends heavily on the Au deposition coverage and particle morphology. Particles resulting from low Au coverages deposited at the liquid nitrogen temperature exhibit significantly enhanced CO binding relative to bulk crystalline Au. The resulting CO TPD spectra, and the significantly red-shifted C–O stretching frequency and negative charging of the Au nanoparticles as evidenced by HREELS and DFT, all correspond to those reported for catalytically active Au nanoparticles grown on reactive metal oxides, even though the h-BN/Rh(111) surface is free of carbon, oxygen, or defects. DFT modeling further suggests that the enhanced CO adsorption occurs at highly undercoordinated Au atoms on the perimeters of the nanoparticles. As the Au coverage is increased, the CO adsorption energy and C–O stretching frequency converge toward values associated with bulk Au. Annealing to 600 K results in bulk-like CO adsorption characteristics at any Au coverage. These results suggest that the $$h$$-BN/Rh(111) surface represents a potential platform for evaluating the role of Au vs support in low-temperature CO oxidation.
- Authors:
-
- Louisiana State Univ., Baton Rouge, LA (United States)
- Texas A & M Univ., College Station, TX (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Atomic-Level Catalyst Design (CALCD)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1369695
- Grant/Contract Number:
- SC0001058
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 120; Journal Issue: 20; Related Information: CALCD partners with Louisiana State University (lead); Clemson University; University of Florida; Georgia Institute of Technology; Grambling State University; Oak Ridge National Laboratory; Ohio State University; Pennsylvania State; Texas A&M University; Vienna University of Technology, Austria; University of Utrecht, Netherlands; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Desorption; Metal nanoparticles; Adsorption; Gold; Metal clusters
Citation Formats
McKee, W. C., Patterson, M. C., Huang, D., Frick, J. R., Kurtz, R. L., Sprunger, P. T., Liu, L., and Xu, Y. CO Adsorption on Au Nanoparticles Grown on Hexagonal Boron Nitride/Rh(111). United States: N. p., 2016.
Web. doi:10.1021/acs.jpcc.6b01645.
McKee, W. C., Patterson, M. C., Huang, D., Frick, J. R., Kurtz, R. L., Sprunger, P. T., Liu, L., & Xu, Y. CO Adsorption on Au Nanoparticles Grown on Hexagonal Boron Nitride/Rh(111). United States. https://doi.org/10.1021/acs.jpcc.6b01645
McKee, W. C., Patterson, M. C., Huang, D., Frick, J. R., Kurtz, R. L., Sprunger, P. T., Liu, L., and Xu, Y. Mon .
"CO Adsorption on Au Nanoparticles Grown on Hexagonal Boron Nitride/Rh(111)". United States. https://doi.org/10.1021/acs.jpcc.6b01645. https://www.osti.gov/servlets/purl/1369695.
@article{osti_1369695,
title = {CO Adsorption on Au Nanoparticles Grown on Hexagonal Boron Nitride/Rh(111)},
author = {McKee, W. C. and Patterson, M. C. and Huang, D. and Frick, J. R. and Kurtz, R. L. and Sprunger, P. T. and Liu, L. and Xu, Y.},
abstractNote = {CO adsorption on size-controlled Au nanoparticles grown on an $h$-BN/Rh(111) nanomesh surface has been examined to probe their potential catalytic properties. A combination of high-resolution electron energy loss spectroscopy (HREELS), temperature-programmed desorption (TPD), and density functional theory (DFT) calculations demonstrate that the CO adsorption strength depends heavily on the Au deposition coverage and particle morphology. Particles resulting from low Au coverages deposited at the liquid nitrogen temperature exhibit significantly enhanced CO binding relative to bulk crystalline Au. The resulting CO TPD spectra, and the significantly red-shifted C–O stretching frequency and negative charging of the Au nanoparticles as evidenced by HREELS and DFT, all correspond to those reported for catalytically active Au nanoparticles grown on reactive metal oxides, even though the h-BN/Rh(111) surface is free of carbon, oxygen, or defects. DFT modeling further suggests that the enhanced CO adsorption occurs at highly undercoordinated Au atoms on the perimeters of the nanoparticles. As the Au coverage is increased, the CO adsorption energy and C–O stretching frequency converge toward values associated with bulk Au. Annealing to 600 K results in bulk-like CO adsorption characteristics at any Au coverage. These results suggest that the $h$-BN/Rh(111) surface represents a potential platform for evaluating the role of Au vs support in low-temperature CO oxidation.},
doi = {10.1021/acs.jpcc.6b01645},
journal = {Journal of Physical Chemistry. C},
number = 20,
volume = 120,
place = {United States},
year = {Mon May 02 00:00:00 EDT 2016},
month = {Mon May 02 00:00:00 EDT 2016}
}
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Works referencing / citing this record:
Growth and stability of Pt nanoclusters from 1 to 50 atoms on h-BN/Rh(111)
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