Effect of Metal-support Interaction on Catalytic Performance of Pd/ZrO_x in CO₂ Hydrogenation to Formate

Abstract

Pd-based catalysts have been widely used in CO₂ hydrogenation to formic acid/formate and their catalytic performance is strongly related to the metal-support interaction, which determines the geometric and electronic structure of Pd sites. Herein, the interaction of Pd species with ZrO₂ support is effectively regulated by altering the synthesis method. Pd_0.4/ZrO_x(SG) prepared by the sol-gel (SG) method shows higher catalytic activity than Pd_0.4/ZrO_x(IM) prepared by the impregnation method (IM) in CO₂ hydrogenation to formate. This is due to the strong metal-support interaction that hinders the agglomeration of Pd species at high temperatures, thus, exposing more active sites. However, further improvement of the interaction of Pd with the support by decreasing Pd loading on ZrO_x(SG) leads to a considerable decrease of both formate formation rate and TON. This is because of the suppression of the reduction of PdO_x species that decreases H₂ dissociation and subsequent hydrogenation activity.

Keywords

CO₂ hydrogenation / Formate / Metal-support interaction / Pd/ZrO_x catalyst / Reaction mechanism

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Jilin University, The Editorial Department of Chemical Research in Chinese Universities and Springer-Verlag GmbH