Please use this identifier to cite or link to this item: https://doi.org/10.1016/j.mcat.2019.110461
Title: Zirconia phase effect in Pd/ZrO2 catalyzed CO2 hydrogenation into formate
Authors: Zhang, Zhenhua 
Zhang, Liyuan
Hulsey, Max J
Yan, Ning 
Keywords: CO2
Support effect
Hydrogenation
Formic acid
Pd
Issue Date: 1-Oct-2019
Publisher: Elsevier B.V.
Citation: Zhang, Zhenhua, Zhang, Liyuan, Hulsey, Max J, Yan, Ning (2019-10-01). Zirconia phase effect in Pd/ZrO2 catalyzed CO2 hydrogenation into formate. MOLECULAR CATALYSIS 475. ScholarBank@NUS Repository. https://doi.org/10.1016/j.mcat.2019.110461
Abstract: © 2019 Elsevier B.V. In heterogeneous catalysis, transformation of CO2 into formate largely relies on supported palladium catalyst, in which the support and in particular the support basicity plays a critical role. In this study, we prepared a series of Pd catalysts loaded on ZrO2 bearing three different crystal phases, namely the tetragonal phase (ZrO2-T), the monoclinic phase (ZrO2-M), and the hybrid tetragonal and monoclinic phase (ZrO2-M&T). With the same metal loading, ZrO2-T supported Pd catalyst exhibited considerably higher intrinsic activity in CO2 hydrogenation into formate compared with the other two catalysts. Pd/ZrO2-T with 2 wt% Pd was the most active one in the series, affording a TOF of 2817 h−1 at 373 K. In situ DRIFTS spectroscopy, kinetic study and CO2-TPD analysis provided evidence that all Pd/ZrO2 catalysts follow a similar catalytic mechanism, and the origin of the superior activity for Pd/ZrO2-T is the higher density of weak basic sites on ZrO2-T, which facilitates the transformation of CO2 into the desirable surface adsorbed bicarbonate as the precursor for formate. This work highlights the importance of crystal-phase engineering of the support in tuning the catalytic activity of Pd based catalysts for CO2 hydrogenation.
Source Title: MOLECULAR CATALYSIS
URI: https://scholarbank.nus.edu.sg/handle/10635/168914
ISSN: 24688231
DOI: 10.1016/j.mcat.2019.110461
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