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Title: An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation

Abstract

Single-atom catalysts have attracted great attention in recent years due to their high efficiencies and cost savings. However, there is debate concerning the nature of the active site, interaction with the support, and mechanism by which single-atom catalysts operate. Here, using a combined surface science and theory approach, we designed a model system in which we unambiguously show that individual Pt atoms on a well-defined Cu 2O film are able to perform CO oxidation at low temperatures. Isotopic labelling studies reveal that oxygen is supplied by the support. Density functional theory rationalizes the reaction mechanism and confirms X-ray photoelectron spectroscopy measurements of the neutral charge state of Pt. Scanning tunneling microscopy enables visualization of the active site as the reaction progresses, and infrared measurements of the CO stretch frequency are consistent with atomically dispersed Pt atoms. These results serve as a benchmark for characterizing, understanding and designing other single-atom catalysts.

Authors:
; ORCiD logo; ; ORCiD logo; ; ; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1491735
Report Number(s):
PNNL-SA-135489
Journal ID: ISSN 2520-1158
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Nature Catalysis
Additional Journal Information:
Journal Volume: 1; Journal Issue: 3; Journal ID: ISSN 2520-1158
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English

Citation Formats

Therrien, Andrew J., Hensley, Alyssa J. R., Marcinkowski, Matthew D., Zhang, Renqin, Lucci, Felicia R., Coughlin, Benjamin, Schilling, Alex C., McEwen, Jean-Sabin, and Sykes, E. Charles H. An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation. United States: N. p., 2018. Web. doi:10.1038/s41929-018-0028-2.
Therrien, Andrew J., Hensley, Alyssa J. R., Marcinkowski, Matthew D., Zhang, Renqin, Lucci, Felicia R., Coughlin, Benjamin, Schilling, Alex C., McEwen, Jean-Sabin, & Sykes, E. Charles H. An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation. United States. doi:10.1038/s41929-018-0028-2.
Therrien, Andrew J., Hensley, Alyssa J. R., Marcinkowski, Matthew D., Zhang, Renqin, Lucci, Felicia R., Coughlin, Benjamin, Schilling, Alex C., McEwen, Jean-Sabin, and Sykes, E. Charles H. Thu . "An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation". United States. doi:10.1038/s41929-018-0028-2.
@article{osti_1491735,
title = {An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation},
author = {Therrien, Andrew J. and Hensley, Alyssa J. R. and Marcinkowski, Matthew D. and Zhang, Renqin and Lucci, Felicia R. and Coughlin, Benjamin and Schilling, Alex C. and McEwen, Jean-Sabin and Sykes, E. Charles H.},
abstractNote = {Single-atom catalysts have attracted great attention in recent years due to their high efficiencies and cost savings. However, there is debate concerning the nature of the active site, interaction with the support, and mechanism by which single-atom catalysts operate. Here, using a combined surface science and theory approach, we designed a model system in which we unambiguously show that individual Pt atoms on a well-defined Cu2O film are able to perform CO oxidation at low temperatures. Isotopic labelling studies reveal that oxygen is supplied by the support. Density functional theory rationalizes the reaction mechanism and confirms X-ray photoelectron spectroscopy measurements of the neutral charge state of Pt. Scanning tunneling microscopy enables visualization of the active site as the reaction progresses, and infrared measurements of the CO stretch frequency are consistent with atomically dispersed Pt atoms. These results serve as a benchmark for characterizing, understanding and designing other single-atom catalysts.},
doi = {10.1038/s41929-018-0028-2},
journal = {Nature Catalysis},
issn = {2520-1158},
number = 3,
volume = 1,
place = {United States},
year = {2018},
month = {3}
}