English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT
 
 
DownloadE-Mail
  Origin of different deactivation of Pd/SnO2 and Pd/GeO2 catalysts in methanol dehydrogenation and reforming: A comparative study

Lorenz, H., Zhao, Q., Turner, S., Lebedev, O. I., Van Tendeloo, G., Klötzer, B., et al. (2010). Origin of different deactivation of Pd/SnO2 and Pd/GeO2 catalysts in methanol dehydrogenation and reforming: A comparative study. Applied Catalysis A: General, 381(1-2), 242-252. Retrieved from http://dx.doi.org/10.1016/j.apcata.2010.04.015.

Item is

Files

show Files
hide Files
:
494410.pdf (Preprint), 936KB
Name:
494410.pdf
Description:
-
OA-Status:
Visibility:
Public
MIME-Type / Checksum:
application/pdf / [MD5]
Technical Metadata:
Copyright Date:
2010
Copyright Info:
Elsevier
License:
-
:
735575.pdf (Correspondence), 189KB
 
File Permalink:
-
Name:
735575.pdf
Description:
-
OA-Status:
Visibility:
Private
MIME-Type / Checksum:
application/pdf
Technical Metadata:
Copyright Date:
-
Copyright Info:
-
License:
-

Locators

show

Creators

show
hide
 Creators:
Lorenz, Harald, Author
Zhao, Qian, Author
Turner, Stuart, Author
Lebedev, Oleg I., Author
Van Tendeloo, Gustaaf, Author
Klötzer, Bernhard, Author
Rameshan, Christoph1, Author           
Pfaller, Kristian, Author
Konzett, Jürgen, Author
Penner, Simon, Author
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              

Content

show
hide
Free keywords: Electron microscopy; Pd3Sn2; Pd2Ge; Metal–support interaction; Methanol conversion; Selected area electron diffraction; Pd2Sn; PdSn Research Context: Paladium catalyst
 Abstract: Pd particles supported on SnO2 and GeO2 have been structurally investigated by X-ray diffraction, (High-Resolution) transmission and scanning electron microscopy after different reductive treatments to monitor the eventual formation of bimetallic phases and catalytically tested in methanol dehydrogenation/reforming. For both oxides this included a thin film sample with well-defined Pd particles and a powder catalyst prepared by incipient wetness impregnation. The hexagonal and the tetragonal polymorph were studied for powder GeO2. Pd2Ge formation was observed on all GeO2-supported catalysts, strongly depending on the specific sample used. Reduction of the thin film at 573 K resulted in full transformation into the bimetallic state. The partial solubility of hexagonal GeO2 in water and its thermal structural instability yielded Pd2Ge formation at 473 K, at the cost of a structurally inhomogeneous support and Ge metal formation at higher reduction temperatures. Pd on tetragonal GeO2 entered a state of strong metal–support interaction after reduction at 573–673 K, resulting in coalescing Pd2Ge particles on a sintered and re-crystallized support, apparently partially covering the bimetallic particles and decreasing the catalytic activity. Pd2Ge on amorphous thin film and hexagonal GeO2 converted methanol primarily via dehydrogenation to CO and H2.

At 573 K, formation of Pd2Sn and also PdSn occurred on the Pd/SnO2 thin film. Pd3Sn2 (and to some extent Pd2Sn) were predominantly obtained on the respective powder catalyst. Strong deactivation with increasing reduction temperature was observed, likely not based on the classical strong metal–support interaction effect, but rather on a combination of missing active structural ensembles on Sn-enriched bimetallic phases and the formation of metallic β-Sn. Correlations to Pd and its bimetallics supported on ZnO, Ga2O3 and In2O3 were also discussed.

Details

show
hide
Language(s): eng - English
 Dates: 2010-06-15
 Publication Status: Issued
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: eDoc: 494410
URI: http://dx.doi.org/10.1016/j.apcata.2010.04.015
 Degree: -

Event

show

Legal Case

show

Project information

show

Source 1

show
hide
Title: Applied Catalysis A: General
Source Genre: Journal
 Creator(s):
Affiliations:
Publ. Info: Amsterdam : Elsevier
Pages: - Volume / Issue: 381 (1-2) Sequence Number: - Start / End Page: 242 - 252 Identifier: ISSN: 0926-860X
CoNE: https://pure.mpg.de/cone/journals/resource/954925567761_1