Ca-Modified Pd/CeO2-ZrO2-Al2O3 Catalysts for Methanol Decomposition

doi:10.3724/SP.J.1088.2011.10703

Abstract

Abstract: CeO₂-ZrO₂-Al₂O₃ and CeO₂-ZrO₂-Al₂O₃-CaOsupports were prepared by the coprecipitation method and were loaded with Pd by impregnation to form Pd/CeO₂-ZrO₂-Al₂O₃(Pd/CZA) and Pd/CeO₂-ZrO₂-Al₂O₃-CaO (Pd/CZACa) catalysts. The catalysts were characterized by X-ray diffraction, low temperature N₂ adsorption-desorption, oxygen storage capacity, CO chemisorption, NH₃ temperature-programmed desorption (NH₃-TPD), CO₂ temperature-programmed desorption (CO₂-TPD), H₂ temperature-programmed reduction (H₂-TPR), and X-ray photoelectron spectroscopy (XPS). The catalyst activity for methanol decomposition showed that the Ca modification improved the low-temperature activity of the catalyst, which lowered the complete conversion temperature on 34 ^oC. NH₃-TPD and CO₂-TPD showed that the addition of Ca poisoned the acid sites of the support or increased the number of weak basic sites and therefore changed the adsorption-desorption equilibria of the adsorbed species. It also enhanced the metal-support interaction and increased the electronic surroundings of Pd sites, which maintained Pd in a partly oxidized (Pd^δ⁺) state and consequently increased the activity for methanol decomposition according to H₂-TPR and XPS measurements.

Key words: palladium, calcium, methanol decomposition, ceria, zirconia, alumina

LI Xue, WANG Xiao-Wen, ZHAO Ming, LIU Jian-Ying, GONG Mao-Chu, CHEN Yao-Qiang. Ca-Modified Pd/CeO₂-ZrO₂-Al₂O₃ Catalysts for Methanol Decomposition[J]. Chinese Journal of Catalysis, 2011, 32(11): 1739-1746.

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Ca-Modified Pd/CeO₂-ZrO₂-Al₂O₃ Catalysts for Methanol Decomposition

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