Partial Hydrogenation of 2-Methyl-3-butyn-2-ol over Pd/ZnO: Effect of Reduction Temperature on Alloy Formation and Catalytic Response

Alberto Gonzalez Fernandez, Chiara Pischetola, Lioubov Kiwi-Minsker, Fernando Cardenas-Lizana

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Abstract

We have investigated the catalytic effect of the β-phase PdZn alloy on selective gas-phase hydrogenation of 2-methyl-3-butyn-2-ol over Pd/ZnO using Pd/Al2O3 as a benchmark. Activation (in H2) of Pd/ZnO to 973 K generated a β-phase PdZn alloy (from X-ray diffraction). Five intermediate samples with a modified surface PdZn/Pdδ− mole ratio (based on X-ray photoelectron spectroscopy) but similar metal nanoparticle size (mean size = 6 nm from high-resolution scanning electron microscopy/scanning transmission electron microscopy) were generated by changing the final activation temperature between 403 and 973 K. Activation over the same temperature range increased metal nanoparticle size (6 → 10 nm) and lowered the surface Pdδ− content in the Pd/Al2O3 samples. In each case, regardless of the activation temperature, greater selectivity to target 2-methyl-3-buten-2-ol (MBE) was observed over Pd/ZnO relative to Pd/Al2O3. Both catalysts delivered a similar activity/selectivity trend characterized by enhanced MBE selectivity and lower activity over the systems activated at a higher temperature. We associate this response with the formation of β-PdZn alloy and metal encapsulation that impacts on surface Pdδ− in Pd/ZnO. Pd/ZnO outperformed an industrial Lindlar catalyst, Pd/CuO, and Au/Al2O3 in terms of selective transformation to MBE. Our results establish the beneficial effect of the PdZn alloy phase to promote the continuous production of commercially important alkenols.

Original languageEnglish
Pages (from-to)3681–3691
Number of pages11
JournalJournal of Physical Chemistry C
Volume124
Issue number6
Early online date19 Jan 2020
DOIs
Publication statusPublished - 13 Feb 2020

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