<p>Pd-based catalysts have been widely used in CO<sub>2</sub> 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 ZrO<sub>2</sub> support is effectively regulated by altering the synthesis method. Pd<sub>0.4</sub>/ZrO<sub><i>x</i></sub>(SG) prepared by the sol-gel (SG) method shows higher catalytic activity than Pd<sub>0.4</sub>/ZrO<sub><i>x</i></sub>(IM) prepared by the impregnation method (IM) in CO<sub>2</sub> 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<sub><i>x</i></sub>(SG) leads to a considerable decrease of both formate formation rate and TON. This is because of the suppression of the reduction of PdO<sub><i>x</i></sub> species that decreases H<sub>2</sub> dissociation and subsequent hydrogenation activity.</p>

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

  • Mengwei Li,
  • Sen Wang,
  • Mei Dong,
  • Jianguo Wang,
  • Weibin Fan

摘要

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. Pd0.4/ZrOx(SG) prepared by the sol-gel (SG) method shows higher catalytic activity than Pd0.4/ZrOx(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 ZrOx(SG) leads to a considerable decrease of both formate formation rate and TON. This is because of the suppression of the reduction of PdOx species that decreases H2 dissociation and subsequent hydrogenation activity.