Combining STM, RAIRS and TPD to Decipher the Dispersion and Interactions Between Active Sites in RhCu Single-Atom Alloys
Abstract
Single-atom alloys are a new class of heterogeneous catalyst in which trace amounts of metal dopants exist as individual, isolated sites in a host metal. In this study, we examine RhCu, a new single-atom alloy with a combination of scanning tunneling microscopy, reflectance absorption infrared spectroscopy, and temperature programed desorption to understand the atomic structure of the alloy and correlate this with the behavior of CO, a common probe molecule. We find that Rh alloys into Cu(111) preferentially from step edges. As such, step density plays an important role in the vibrational structure of CO on isolated Rh sites. We find that atomically dispersed Rh sites can be close enough together to have dipole-dipole coupling interactions. Together, this combined experimental approach enables us to understand the alloying mechanism of Rh with Cu and yields important signatures of the atomic sites that are useful in benchmarking CO vibrational data.
- Authors:
-
[1]
- Tufts Univ., Medford, MA (United States)
- Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.; Imperial College, London (United Kingdom)
- Publication Date:
- Research Org.:
- Tufts Univ., Medford, MA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1595290
- Alternate Identifier(s):
- OSTI ID: 1573523; OSTI ID: 1773871
- Grant/Contract Number:
- SC0004738; FG02-10ER16170
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 2; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Single-atom alloy; surface science; catalysis; microscopy; IR-spectroscopy
Citation Formats
Hannagan, Ryan T., Patel, Dipna A., Cramer, Laura A., Schilling, Alex C., Ryan, Paul T. P., Larson, Amanda M., Çınar, Volkan, Wang, Yicheng, Balema, Tedros A., and Sykes, E. Charles H. Combining STM, RAIRS and TPD to Decipher the Dispersion and Interactions Between Active Sites in RhCu Single-Atom Alloys. United States: N. p., 2019.
Web. doi:10.1002/cctc.201901488.
Hannagan, Ryan T., Patel, Dipna A., Cramer, Laura A., Schilling, Alex C., Ryan, Paul T. P., Larson, Amanda M., Çınar, Volkan, Wang, Yicheng, Balema, Tedros A., & Sykes, E. Charles H. Combining STM, RAIRS and TPD to Decipher the Dispersion and Interactions Between Active Sites in RhCu Single-Atom Alloys. United States. https://doi.org/10.1002/cctc.201901488
Hannagan, Ryan T., Patel, Dipna A., Cramer, Laura A., Schilling, Alex C., Ryan, Paul T. P., Larson, Amanda M., Çınar, Volkan, Wang, Yicheng, Balema, Tedros A., and Sykes, E. Charles H. Tue .
"Combining STM, RAIRS and TPD to Decipher the Dispersion and Interactions Between Active Sites in RhCu Single-Atom Alloys". United States. https://doi.org/10.1002/cctc.201901488. https://www.osti.gov/servlets/purl/1595290.
@article{osti_1595290,
title = {Combining STM, RAIRS and TPD to Decipher the Dispersion and Interactions Between Active Sites in RhCu Single-Atom Alloys},
author = {Hannagan, Ryan T. and Patel, Dipna A. and Cramer, Laura A. and Schilling, Alex C. and Ryan, Paul T. P. and Larson, Amanda M. and Çınar, Volkan and Wang, Yicheng and Balema, Tedros A. and Sykes, E. Charles H.},
abstractNote = {Single-atom alloys are a new class of heterogeneous catalyst in which trace amounts of metal dopants exist as individual, isolated sites in a host metal. In this study, we examine RhCu, a new single-atom alloy with a combination of scanning tunneling microscopy, reflectance absorption infrared spectroscopy, and temperature programed desorption to understand the atomic structure of the alloy and correlate this with the behavior of CO, a common probe molecule. We find that Rh alloys into Cu(111) preferentially from step edges. As such, step density plays an important role in the vibrational structure of CO on isolated Rh sites. We find that atomically dispersed Rh sites can be close enough together to have dipole-dipole coupling interactions. Together, this combined experimental approach enables us to understand the alloying mechanism of Rh with Cu and yields important signatures of the atomic sites that are useful in benchmarking CO vibrational data.},
doi = {10.1002/cctc.201901488},
journal = {ChemCatChem},
number = 2,
volume = 12,
place = {United States},
year = {Tue Sep 24 00:00:00 EDT 2019},
month = {Tue Sep 24 00:00:00 EDT 2019}
}
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