4.8 Article

Crystal plane induced metal-support interaction in Pd/Pr-CeO2 catalyst boosts H2O-assisted CO oxidation

期刊

JOURNAL OF CATALYSIS
卷 417, 期 -, 页码 60-73

出版社

ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2022.11.026

关键词

Metal-support interaction; CO oxidation; Highly dispersed Pd; Oxygen vacancy; H2O tolerance

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The efficiency of CO oxidation catalysts can be improved under wet conditions by controlling the metal-support interaction of Pd/Pr-CeO2 catalysts.
Catalytic oxidation is an effective method to remove CO in exhaust gas, yet it is challenging to enhance the H2O tolerance of catalysts at low temperature due to the strong competitive adsorption between H2O and reactants (CO and O-2). Here, we report that the precise control of the metal-support interaction by regulating the support crystal plane of Pd/Pr-CeO2 catalysts leads to highly efficient CO oxidation cata-lysts under wet conditions. The addition of H2O inhibits the CO oxidation activity of Pr-CeO2 nano-cube and octahedron supported highly dispersed Pd catalysts, but enhances the CO oxidation activity over Pr-CeO2 nanorod supported highly dispersed Pd catalysts. After introduction of H2O in feed gas, the T99 (Temperature to achieve 99 % conversion of CO) decreases from 157 degrees C to 115 degrees C for Pd/Pr-CeO2-NRs (Nanorods) catalyst at a gas hourly space velocity of 70, 000 h-1 and remains stable for more than 2000 min in the presence of H2O. Systematic characterization reveals that the (110) crystal plane of Pr-CeO2 nanorod enhance the interaction between Pd species and support, resulting in the formation of abundant high dispersed Pd-oxygen vacancy (Ov) active sites. The kinetics study and in-situ DRIFTS char-acterization confirmed that CO oxidation Pd/Pr-CeO2-NRs mainly follows the H2O-mediated Langmuir-Hinshelwood mechanism in the presence of H2O. H2O promote the formation of active OH groups and accelerate CO oxidation through formate pathway at low temperature. In contrast, the CO oxidation fol-low traditional MvK mechanism in the absence of H2O.

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