Elucidation of the Active Sites in Single-Atom Pd1/CeO2 Catalysts for Low-Temperature CO Oxidation

被引:130
|
作者
Jiang, Dong [1 ]
Wan, Gang [2 ]
Garcia-Vargas, Carlos E. [1 ]
Li, Linze [3 ]
Pereira-Hernandez, Xavier Isidro [1 ]
Wang, Chongmin [3 ]
Wang, Yong [1 ,4 ]
机构
[1] Washington State Univ, Gene & Linda Voiland Sch Chem Engn & Bioengn, Pullman, WA 99164 USA
[2] Stanford Univ, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA
[3] Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA
[4] Pacific Northwest Natl Lab, Inst Integrated Catalysis, Richland, WA 99354 USA
关键词
active site; CO oxidation; single-atom catalyst; palladium; atom trapping; PROBING DEFECT SITES; WATER-GAS SHIFT; PD/CEO2; CATALYSTS; CARBON-MONOXIDE; METHANE COMBUSTION; OXYGEN VACANCIES; LOCAL-STRUCTURE; CH4; OXIDATION; CERIA; PD;
D O I
10.1021/acscatal.0c02480
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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).
引用
收藏
页码:11356 / 11364
页数:9
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