Journal
ACS CATALYSIS
Volume 10, Issue 19, Pages 11356-11364Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c02480
Keywords
active site; CO oxidation; single-atom catalyst; palladium; atom trapping
Categories
Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-FG02-05ER15712, DE-AC02-06CH11357, DE-AC02-76SF00515]
- DOE Office of Energy Efficiency and Renewable Energy (EERE)'s Vehicle Technologies Office
- Office of Biological and Environmental Research [grid.436923.9]
- Canadian Light Source
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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 Pd-1/CeO2 catalysts prepared via high-temperature atom trapping (AT). The increased oxygen vacancies on CeO2 surface induced by 800 degrees 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 T-90 (temperature to achieve 90% conversion) by similar to 100 degrees C in CO oxidation at a gas hourly space velocity of 300 L g(-1) h(-1).
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