Chemical Research in Chinese Universities ›› 2025, Vol. 41 ›› Issue (3): 529-538.doi: 10.1007/s40242-025-4217-7

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

LI Mengwei1,2, WANG Sen1, DONG Mei1, WANG Jianguo1, FAN Weibin1   

  1. 1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, P. R. China;
    2. University of the Chinese Academy of Sciences, Beijing 100049, P. R. China
  • Received:2024-10-30 Revised:2024-12-30 Online:2025-06-01 Published:2025-05-27
  • Contact: WANG Sen,E-mail:wangsen@sxicc.ac.cn;FAN Weibin,E-mail:fanwb@sxicc.ac.cn E-mail:wangsen@sxicc.ac.cn;fanwb@sxicc.ac.cn
  • Supported by:
    This work was supported by the National Key R&D Program of China (No. 2023YFB4103700), the National Natural Science Foundation of China (Nos. U1910203, 21991090, 21991092, 22322208, 22272195, U22A20431), the Natural Science Foundation of Shanxi Province of China (No. 202203021224009), the Innovation Foundation of the Institute of Coal Chemistry, Chinese Academy of Sciences (No. SCJC-DT-2023-06), and the Project of the Youth Innovation Promotion Association CAS (No. 2021172).

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. 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.

Key words: CO2 hydrogenation, Formate, Metal-support interaction, Pd/ZrOx catalyst, Reaction mechanism