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

Jolien De Waele (UGent) , Vladimir Galvita (UGent) , Hilde Poelman (UGent) , Christophe Detavernier (UGent) and Joris Thybaut (UGent)
(2017) CATALYSIS SCIENCE & TECHNOLOGY. 7(17). p.3715-3727
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Abstract
A hydrotalcite-based PdZn nanoparticle catalyst, PdZn/Mg(Al)(Pd)(Zn)O-x has been synthesized via a one-pot procedure. The activation comprising H-2 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 (mol(Pd) s)(-1) rather than 3.2 molEtOH (mol(Pd) 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 x 10(-4) mol s(-1) kg(Pd)(-1) and 98%, respectively.
Keywords
ATOMIC LAYER DEPOSITION, PROPANE DEHYDROGENATION, COPPER-CATALYSTS, ETHYL-ACETATE, HETEROGENEOUS CATALYSIS, SYNERGISTIC CATALYSIS, REFORMING, CATALYSTS, REACTION-KINETICS, LIQUID-PHASE, METHANOL

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Chicago
De Waele, Jolien, Vladimir Galvita, Hilde Poelman, Christophe Detavernier, and Joris Thybaut. 2017. “Formation and Stability of an Active PdZn Nanoparticle Catalyst on a Hydrotalcite-based Support for Ethanol Dehydrogenation.” Catalysis Science & Technology 7 (17): 3715–3727.
APA
De Waele, Jolien, Galvita, V., Poelman, H., Detavernier, C., & Thybaut, J. (2017). Formation and stability of an active PdZn nanoparticle catalyst on a hydrotalcite-based support for ethanol dehydrogenation. CATALYSIS SCIENCE & TECHNOLOGY, 7(17), 3715–3727.
Vancouver
1.
De Waele J, Galvita V, Poelman H, Detavernier C, Thybaut J. Formation and stability of an active PdZn nanoparticle catalyst on a hydrotalcite-based support for ethanol dehydrogenation. CATALYSIS SCIENCE & TECHNOLOGY. Cambridge: Royal Soc Chemistry; 2017;7(17):3715–27.
MLA
De Waele, Jolien, Vladimir Galvita, Hilde Poelman, et al. “Formation and Stability of an Active PdZn Nanoparticle Catalyst on a Hydrotalcite-based Support for Ethanol Dehydrogenation.” CATALYSIS SCIENCE & TECHNOLOGY 7.17 (2017): 3715–3727. Print.
@article{8536176,
  abstract     = {A hydrotalcite-based PdZn nanoparticle catalyst, PdZn/Mg(Al)(Pd)(Zn)O-x has been synthesized via a one-pot procedure. The activation comprising H-2 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 (mol(Pd) s)(-1) rather than 3.2 molEtOH (mol(Pd) 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 x 10(-4) mol s(-1) kg(Pd)(-1) and 98\%, respectively.},
  author       = {De Waele, Jolien and Galvita, Vladimir and Poelman, Hilde and Detavernier, Christophe and Thybaut, Joris},
  issn         = {2044-4753},
  journal      = {CATALYSIS SCIENCE \& TECHNOLOGY},
  keyword      = {ATOMIC LAYER DEPOSITION,PROPANE DEHYDROGENATION,COPPER-CATALYSTS,ETHYL-ACETATE,HETEROGENEOUS CATALYSIS,SYNERGISTIC CATALYSIS,REFORMING,CATALYSTS,REACTION-KINETICS,LIQUID-PHASE,METHANOL},
  language     = {eng},
  number       = {17},
  pages        = {3715--3727},
  publisher    = {Royal Soc Chemistry},
  title        = {Formation and stability of an active PdZn nanoparticle catalyst on a hydrotalcite-based support for ethanol dehydrogenation},
  url          = {http://dx.doi.org/10.1039/c7cy01105a},
  volume       = {7},
  year         = {2017},
}

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