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Effect of Ceria Crystal Plane on the Physicochemical and Catalytic Properties of Pd/Ceria for CO and Propane Oxidation

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Key Laboratory for Advanced Materials and Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
*E-mail: [email protected] (Y. Guo).
*Fax: +86-21-64252923. E-mail: [email protected] (G. Z. Lu).
Cite this: ACS Catal. 2016, 6, 4, 2265–2279
Publication Date (Web):February 23, 2016
https://doi.org/10.1021/acscatal.5b02617
Copyright © 2016 American Chemical Society
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Abstract

Ceria nanocrystallites with different morphologies and crystal planes were hydrothermally prepared, and the effects of ceria supports on the physicochemical and catalytic properties of Pd/CeO2 for the CO and propane oxidation were examined. The results showed that the structure and chemical state of Pd on ceria were affected by ceria crystal planes. The Pd species on CeO2-R (rods) and CeO2-C (cubes) mainly formed PdxCe1–xO2−σ solid solution with −Pd2+–O2––Ce4+– linkage. In addition, the PdOx nanoparticles were dominated on the surface of Pd/CeO2-O (octahedrons). For the CO oxidation, the Pd/CeO2-R catalyst showed the highest catalytic activity among three catalysts, its reaction rate reached 2.07 × 10–4 mol gPd–1 s–1 at 50 °C, in which CeO2-R mainly exposed the (110) and (100) facets with low oxygen vacancy formation energy, strong reducibility, and high surface oxygen mobility. TOF of Pd/CeO2-R (3.78 × 10–2 s–1) was much higher than that of Pd/CeO2-C (6.40 × 10–3 s–1) and Pd/CeO2-O (1.24 × 10–3 s–1) at 50 °C, and its activation energy (Ea) was 40.4 kJ/mol. For propane oxidation, the highest reaction rate (8.08 × 10–5 mol gPd–1 s–1 at 300 °C) was obtained over the Pd/CeO2-O catalyst, in which CeO2-O mainly exposed the (111) facet. There are strong surface Ce–O bonds on the ceria (111) facet, which favors the existence of PdO particles and propane activation. The turnover frequency (TOF) of the Pd/CeO2-O catalyst was highest (3.52 × 10–2 s–1) at 300 °C and its Ea value was 49.1 kJ/mol. These results demonstrate the inverse facet sensitivity of ceria for the CO and propane oxidation over Pd/ceria.

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  • The Pd particle size calculated by CO chemisorption, the catalytic stabilities of Pd/CeO2 samples for CO and propane oxidation (Figure S1); TEM images of 1.0% Pd/CeO2–O and its Pd particle distribution (Figure S2); and C3H8-TPSR curves on CeO2 samples (Figure S3) (PDF)

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