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Issue 17, 2017
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Formation and stability of an active PdZn nanoparticle catalyst on a hydrotalcite-based support for ethanol dehydrogenation

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Abstract

A hydrotalcite-based PdZn nanoparticle catalyst, PdZn/Mg(Al)(Pd)(Zn)Ox has been synthesized via a one-pot procedure. The activation comprising H2 and air treatment(s) allows tuning the nanoparticle formation and, hence, the catalyst performance. Based on an elaborate set of characterization data from EXAFS, in situ XRD, STEM and CO chemisorption, it is concluded that single reduction leads to the formation of Pd-rich alloy nanoparticles, i.e., a PdZn shell with a Pd core. Cycled reduction, i.e., 3 subsequent hydrogen and air treatments, ensures the formation of more homogeneously mixed PdZn nanoparticles. Compared with a PdZn/ZnO reference catalyst, the nanoparticles obtained after cycled reduction exhibit a higher initial average turnover frequency in ethanol dehydrogenation, i.e., 7.0 molEtOH (molPd s)−1 rather than 3.2 molEtOH (molPd s)−1. An activity loss is observed during the first hours on stream. It is attributed to coking of the Pd sites which are also deemed responsible for acetaldehyde decomposition. Hence, the acetaldehyde selectivity steadily increases during the first hours on stream. Subsequently, the acetaldehyde space time yield and selectivity stabilize at 0.7 × 10−4 mol s−1 kg−1Pd and 98%, respectively.

Graphical abstract: Formation and stability of an active PdZn nanoparticle catalyst on a hydrotalcite-based support for ethanol dehydrogenation

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Publication details

The article was received on 02 Jun 2017, accepted on 09 Jul 2017 and first published on 11 Jul 2017


Article type: Paper
DOI: 10.1039/C7CY01105A
Citation: Catal. Sci. Technol., 2017,7, 3715-3727
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    Formation and stability of an active PdZn nanoparticle catalyst on a hydrotalcite-based support for ethanol dehydrogenation

    J. De Waele, V. V. Galvita, H. Poelman, C. Detavernier and J. W. Thybaut, Catal. Sci. Technol., 2017, 7, 3715
    DOI: 10.1039/C7CY01105A

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