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Selective Oxidation of Acetaldehyde to Acetic Acid on Pd-Au Bimetallic Model Catalysts

Author:
Han, Sungmin  Shin, Kihyun  Henkelman, Graeme  Mullins, C. Buddie  


Journal:
ACS CATALYSIS


Issue Date:
2019


Abstract(summary):

Acetic acid is a widely employed reactant in the chemical industry, and it is also used as a food ingredient. Here, we report a catalytic reaction pathway for the gas-phase selective oxidation of acetaldehyde to acetic acid on a Pd-Au(111) heterogeneous model catalyst. On an oxygen precovered Pd-Au surface, acetaldehyde is selectively oxidized to acetic acid from 250 to 340 K. Using FT-IR, the formation of acetate species is detected from 160 to 260 K on this surface, which is a widely known adsorbate derived from acetic acid on metal surfaces. With higher Pd coverages, the acetaldehyde is less selectively oxidized to acetic acid, and near 375 K, CO2, H2O, CH4, and H-2 are evolved, evidence for the decarboxylation of acetate. In our density functional theory calculations, we confirm that the relative energy difference decreases as Pd ensemble size increases. between the acetate state and the decarboxylated state decrease as pd ensemble size increases.


Page:
4360---4368


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