Highly Active and Stable Single Atom Rh1/CeO2 Catalyst for CO Oxidation during Redox Cycling

被引:5
作者
Garcia-Vargas, Carlos E. [1 ,2 ]
Pereira-Hernandez, Xavier Isidro [1 ]
Jiang, Dong [1 ]
Alcala, Ryan [3 ,4 ]
DeLaRiva, Andrew T. [3 ,4 ]
Datye, Abhaya [3 ,4 ]
Wang, Yong [1 ,5 ]
机构
[1] Washington State Univ, Gene & Linda Voiland Sch Chem Engn & Bioengn, Pullman, WA 99164 USA
[2] Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA
[3] Univ New Mexico, Dept Chem & Biol Engn, Albuquerque, NM 87131 USA
[4] Univ New Mexico, Ctr Microengn Mat, Albuquerque, NM 87131 USA
[5] Pacific Northwest Natl Lab, Inst Integrated Catalysis, Richland, WA 99354 USA
关键词
Rh single atom; Rh; CeO2; CO Oxidation; REDOX cycling; TWC; INFRARED-SPECTRA; CHEMISORBED CO; RHODIUM; RH; DECOMPOSITION; AL2O3; N2O; DEACTIVATION; SPECTROSCOPY; ADSORPTION;
D O I
10.1002/cctc.202201210
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
We report a single atom Rh-1/CeO2 catalyst prepared by the high temperature (800 degrees C) atom trapping (AT) method which is stable under both oxidative and reductive conditions. Infrared spectroscopic and electron microscopy characterization revealed the presence of exclusively ionic Rh species. These ionic Rh species are stable even under reducing conditions (CO at 300 degrees C) due to the strong interaction between Rh and CeO2 achieved by the AT method, leading to high and reproducible CO oxidation activity regardless of whether the catalyst is reduced or oxidized. In contrast, ionic Rh species in catalysts synthesized by a conventional impregnation approach (e. g., calcined at 350 degrees C) can be readily reduced to form Rh nanoclusters/nanoparticles, which are easily oxidized under oxidative conditions, leading to loss of catalytic performance. The single atom Rh-1/CeO2 catalysts synthesized by the AT method do not exhibit changes during redox cycling hence are promising catalysts for emission control where redox cycling is encountered, and severe oxidation (fuel cut) leads to loss of performance.
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页数:6
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