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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
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.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
keyword
ATOMIC LAYER DEPOSITION, PROPANE DEHYDROGENATION, COPPER-CATALYSTS, ETHYL-ACETATE, HETEROGENEOUS CATALYSIS, SYNERGISTIC CATALYSIS, REFORMING, CATALYSTS, REACTION-KINETICS, LIQUID-PHASE, METHANOL
journal title
CATALYSIS SCIENCE & TECHNOLOGY
Catal. Sci. Technol.
volume
7
issue
17
pages
13 pages
publisher
Royal Soc Chemistry
place of publication
Cambridge
Web of Science type
Article
Web of Science id
000408678500007
ISSN
2044-4753
2044-4761
DOI
10.1039/c7cy01105a
language
English
UGent publication?
yes
classification
A1
copyright statement
I don't know the status of the copyright for this publication
id
8536176
handle
http://hdl.handle.net/1854/LU-8536176
date created
2017-11-03 11:52:44
date last changed
2017-11-06 08:59:48
@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},
}

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.