Journal
CHEMICAL ENGINEERING JOURNAL
Volume 445, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136681
Keywords
Acetylene semi-hydrogenation; Pd catalysts; Al2O3 microrods; Acidic properties; Kinetics descriptor
Categories
Funding
- Natural Science Foundation of China [21922803, 22122807, 22008067, 22008072]
- Innovation Program of Shanghai Municipal Education Commission
- Program of Shanghai Academic/Technology Research Leader [21XD1421000]
- China Postdoctoral Science Foundation [2020M681202, 2021T140204, 2020M671025, 2019TQ0093]
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The acidic properties of the support have a remarkable effect on the kinetics behavior and selectivity of acetylene hydrogenation, with different electronic structures of Pd as the underlying origin.
The acidic properties of the support show remarkable effects on Pd-catalyzed reactions including the semi-hydrogenation of acetylene. Herein, Al2O3 microrods with distinct acidic properties are synthesized as the supports for Pd catalysts to address the acidic properties dominated kinetics behavior of acetylene hydrogenation. The acidic properties of Al2O3 microrods decrease with the calcination temperature, in the order of Al2O3-1400 < Al2O3-1200 < Al2O3-800, in which the numbers denote the temperature for calcination process. Catalytic performance show that the hydrogenation activities of the corresponding Pd catalysts increase by Pd/Al2O3-1400 < Pd/Al2O3-800 < Pd/Al2O3-1200, while the selectivities to the target ethylene decrease by Pd/Al2O3-1400 > Pd/Al2O3-1200 > Pd/Al2O3-800. A quantitative analysis combined with structure characterizations are further performed to elucidate the underlying origin of such acidic-property dependent performances. It is demonstrated that the different electronic structures of Pd caused by the acidic properties contribute to distinct adsorption properties for the reactant and the target products, which can be quantitatively described by the entropy of activation (Delta S*).
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