Elucidation of the Active Sites in Single-Atom Pd1/CeO2 Catalysts for Low-Temperature CO Oxidation
Abstract
Supported precious metals with atomic dispersion are of great interest in catalysis due to their potentials in achieving maximum atom efficiency and unique reactivities. Herein, the active sites for low-temperature CO oxidation are elucidated over single-atom Pd1/CeO2 catalysts prepared via high-temperature atom trapping (AT). The increased oxygen vacancies on CeO2 surface induced by 800 °C air calcination result in decreased Pd–CeO2 coordinations, i.e., the coordination-unsaturated Pd2+ on CeO2. Light-off and light-out measurements coupled with CO-DRIFTS and X-ray absorption characterization confirm that these coordination-unsaturated Pd2+ on CeO2 are much more reactive than the fully coordinated counterpart, evidenced by a decrease of T90 (temperature to achieve 90% conversion) by ~100 °C in CO oxidation at a gas hourly space velocity of 300 L g–1 h–1.
- Authors:
-
[1];
[1];
[3];
[1];
[4]
- Washington State Univ., Pullman, WA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
- Washington State Univ., Pullman, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1726231
- Report Number(s):
- PNNL-SA-155490
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- AC05-76RL01830; FG02-05ER15712; AC02-06CH11357; AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 19; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; palladium; colloids; catalysts; oxidation; reactivity; active site; CO oxidation; single-atom catalyst; atom trapping
Citation Formats
Jiang, Dong, Wan, Gang, García-Vargas, Carlos E., Li, Linze, Pereira-Hernández, Xavier Isidro, Wang, Chongmin, and Wang, Yong. Elucidation of the Active Sites in Single-Atom Pd1/CeO2 Catalysts for Low-Temperature CO Oxidation. United States: N. p., 2020.
Web. doi:10.1021/acscatal.0c02480.
Jiang, Dong, Wan, Gang, García-Vargas, Carlos E., Li, Linze, Pereira-Hernández, Xavier Isidro, Wang, Chongmin, & Wang, Yong. Elucidation of the Active Sites in Single-Atom Pd1/CeO2 Catalysts for Low-Temperature CO Oxidation. United States. https://doi.org/10.1021/acscatal.0c02480
Jiang, Dong, Wan, Gang, García-Vargas, Carlos E., Li, Linze, Pereira-Hernández, Xavier Isidro, Wang, Chongmin, and Wang, Yong. Thu .
"Elucidation of the Active Sites in Single-Atom Pd1/CeO2 Catalysts for Low-Temperature CO Oxidation". United States. https://doi.org/10.1021/acscatal.0c02480. https://www.osti.gov/servlets/purl/1726231.
@article{osti_1726231,
title = {Elucidation of the Active Sites in Single-Atom Pd1/CeO2 Catalysts for Low-Temperature CO Oxidation},
author = {Jiang, Dong and Wan, Gang and García-Vargas, Carlos E. and Li, Linze and Pereira-Hernández, Xavier Isidro and Wang, Chongmin and Wang, Yong},
abstractNote = {Supported precious metals with atomic dispersion are of great interest in catalysis due to their potentials in achieving maximum atom efficiency and unique reactivities. Herein, the active sites for low-temperature CO oxidation are elucidated over single-atom Pd1/CeO2 catalysts prepared via high-temperature atom trapping (AT). The increased oxygen vacancies on CeO2 surface induced by 800 °C air calcination result in decreased Pd–CeO2 coordinations, i.e., the coordination-unsaturated Pd2+ on CeO2. Light-off and light-out measurements coupled with CO-DRIFTS and X-ray absorption characterization confirm that these coordination-unsaturated Pd2+ on CeO2 are much more reactive than the fully coordinated counterpart, evidenced by a decrease of T90 (temperature to achieve 90% conversion) by ~100 °C in CO oxidation at a gas hourly space velocity of 300 L g–1 h–1.},
doi = {10.1021/acscatal.0c02480},
journal = {ACS Catalysis},
number = 19,
volume = 10,
place = {United States},
year = {Thu Aug 20 00:00:00 EDT 2020},
month = {Thu Aug 20 00:00:00 EDT 2020}
}
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