Abstract

Modification of a 1wt% Pd/CeO2 catalyst by Atomic Layer Deposition of thin ZrO2 films was studied. Calcination of the unmodified Pd/CeO2, prepared by precipitation of aqueous Ce(NO3)3 solutions, with Pd added by impregnation, caused a large decrease in surface area and an increase in crystallite size between 673K and 1073K; however, catalysts modified by 0.4nm ZrO2 films showed no change in either surface area or CeO2 crystallite size upon calcination to 1073K. Methane-oxidation rates in 0.5% CH4 and 5% O2 were slightly lower on the ZrO2-covered catalyst when both materials were calcined at 673K but the activity of the ZrO2-modified catalyst did not decrease with catalyst calcination temperature. Both catalysts showed good activity for the water–gas-shift reaction but the ZrO2 film improved sulfur tolerance by preventing formation of cerium sulfates.

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