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Formation of carbonaceous deposits on Pd-based hydrodechlorination catalysts: Vibrational spectroscopy investigations over Pd/Al2O3 and Pd/SOMS
Date
2019-02-15
Author
Çelik, Gökhan
Ailawar, Saurabh A.
Gunduz, Seval
Edmiston, Paul L.
Ozkan, Umit S.
Metadata
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The widespread utilization and commercialization of hydrodechlorination (HDC) over Pd-based catalysts as a remediation technique has been impeded because of catalyst deactivation problems such as formation of carbonaceous deposits under the reductive environment of HDC. In this study, we investigated the use of a novel animated material, swellable organically-modified silica (SOMS), as a catalyst scaffold for HDC of trichloroethylene (TCE) to develop a catalytic system resistant to carbon formation. The state of aggregation of adsorbed TCE on Pd/SOMS was characterized. It was found that the unique nature of SOMS scaffold caused condensation of adsorbents in the SOMS matrix. This is of particular importance considering the fact that the increase of local concentration of reactants due to condensation may enhance the kinetics of catalytic reactions. To determine the resistance to the formation of carbonaceous materials under reaction conditions, in-situ vibrational spectroscopy experiments (diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and laser Raman spectroscopy) were undertaken over Pd-incorporated SOMS in the absence and presence of water vapor in the reactant stream. The commonly used HDC catalyst Pd/Al2O3 was also studied for comparison purposes. Formation of carbonaceous deposits of different nature were observed over Pd/Al2O3 whereas no detectable carbon formation was observed over Pd/SOMS. It was confirmed that surface hydroxyl groups which are in basic character act as coking agents. The carbon formation resistant behavior of Pd/SOMS is closely related to the nature and low concentration of surface hydroxyl groups.
Subject Keywords
Hydrodechlorination
,
Trichloroethylene
,
Swellable organically-modified silica (SOMS)
,
Palladium
,
DRIFTS
,
Pd/Al2O3
,
Carbonaceous materials
,
Coke
,
Groundwater remediation
,
FTIR
,
Laser Raman spectroscopy
URI
https://hdl.handle.net/11511/41585
Journal
Catalysis Today
DOI
https://doi.org/10.1016/j.cattod.2018.05.001
Collections
Department of Chemical Engineering, Article
Citation Formats
IEEE
ACM
APA
CHICAGO
MLA
BibTeX
G. Çelik, S. A. Ailawar, S. Gunduz, P. L. Edmiston, and U. S. Ozkan, “Formation of carbonaceous deposits on Pd-based hydrodechlorination catalysts: Vibrational spectroscopy investigations over Pd/Al2O3 and Pd/SOMS,”
Catalysis Today
, vol. 323, pp. 129–140, 2019, Accessed: 00, 2020. [Online]. Available: https://hdl.handle.net/11511/41585.