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Title: Effect of high-temperature on the swellable organically-modified silica (SOMS) and its application to gas-phase hydrodechlorination of trichloroethylene

Abstract

Pd catalysts supported on swellable organically-modified silica (SOMS) and high-temperature-treated swellable organically-modified silica (H-SOMS) were characterized and tested for gas-phase hydrodechlorination (HDC) of trichloroethylene (TCE) conditions. The high-temperature treatment on SOMS resulted in an increase in surface area and pore diameter as well as significant improvement of Pd dispersion on H-SOMS with smaller Pd particle sizes compared to the Pd/SOMS catalyst. Although the high-temperature treatment led to some alteration of the SOMS polysiloxane network, the hydrophobicity and organic vapor adsorption characteristics of SOMS were preserved. The reduction and oxidation characteristics of Pd on SOMS and HSOMS were investigated in situ using XANES technique. It was found that the Pd sites in the pores of SOMS was accessible to small molecules such as H 2, facilitating the reduction of PdO x, whereas oxidation of metallic Pd was limited even at higher temperatures when O 2 was used. This effect was only observed over Pd/SOMS catalyst. For Pd/H-SOMS, because the pores were more widely open than Pd/SOMS, both reduction and oxidation of Pd were observed. Finally, the catalytic activity of Pd/H-SOMS for gas-phase HDC of TCE was significantly better than Pd/SOMS. When water was added to the reactant stream (TCE + Hmore » 2O), both Pd/SOMS and Pd/H-SOMS maintained its catalytic performances due to hydrophobic property of the supports.« less

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
National Science Foundation (NSF)
OSTI Identifier:
1373768
Resource Type:
Journal Article
Resource Relation:
Journal Name: Applied Catalysis. B, Environmental; Journal Volume: 209; Journal Issue: C
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sohn, Hyuntae, Celik, Gokhan, Gunduz, Seval, Majumdar, Sreshtha Sinha, Dean, Stacey L., Edmiston, Paul L., and Ozkan, Umit S.. Effect of high-temperature on the swellable organically-modified silica (SOMS) and its application to gas-phase hydrodechlorination of trichloroethylene. United States: N. p., 2017. Web. doi:10.1016/j.apcatb.2017.02.056.
Sohn, Hyuntae, Celik, Gokhan, Gunduz, Seval, Majumdar, Sreshtha Sinha, Dean, Stacey L., Edmiston, Paul L., & Ozkan, Umit S.. Effect of high-temperature on the swellable organically-modified silica (SOMS) and its application to gas-phase hydrodechlorination of trichloroethylene. United States. doi:10.1016/j.apcatb.2017.02.056.
Sohn, Hyuntae, Celik, Gokhan, Gunduz, Seval, Majumdar, Sreshtha Sinha, Dean, Stacey L., Edmiston, Paul L., and Ozkan, Umit S.. Sat . "Effect of high-temperature on the swellable organically-modified silica (SOMS) and its application to gas-phase hydrodechlorination of trichloroethylene". United States. doi:10.1016/j.apcatb.2017.02.056.
@article{osti_1373768,
title = {Effect of high-temperature on the swellable organically-modified silica (SOMS) and its application to gas-phase hydrodechlorination of trichloroethylene},
author = {Sohn, Hyuntae and Celik, Gokhan and Gunduz, Seval and Majumdar, Sreshtha Sinha and Dean, Stacey L. and Edmiston, Paul L. and Ozkan, Umit S.},
abstractNote = {Pd catalysts supported on swellable organically-modified silica (SOMS) and high-temperature-treated swellable organically-modified silica (H-SOMS) were characterized and tested for gas-phase hydrodechlorination (HDC) of trichloroethylene (TCE) conditions. The high-temperature treatment on SOMS resulted in an increase in surface area and pore diameter as well as significant improvement of Pd dispersion on H-SOMS with smaller Pd particle sizes compared to the Pd/SOMS catalyst. Although the high-temperature treatment led to some alteration of the SOMS polysiloxane network, the hydrophobicity and organic vapor adsorption characteristics of SOMS were preserved. The reduction and oxidation characteristics of Pd on SOMS and HSOMS were investigated in situ using XANES technique. It was found that the Pd sites in the pores of SOMS was accessible to small molecules such as H2, facilitating the reduction of PdOx, whereas oxidation of metallic Pd was limited even at higher temperatures when O2 was used. This effect was only observed over Pd/SOMS catalyst. For Pd/H-SOMS, because the pores were more widely open than Pd/SOMS, both reduction and oxidation of Pd were observed. Finally, the catalytic activity of Pd/H-SOMS for gas-phase HDC of TCE was significantly better than Pd/SOMS. When water was added to the reactant stream (TCE + H2O), both Pd/SOMS and Pd/H-SOMS maintained its catalytic performances due to hydrophobic property of the supports.},
doi = {10.1016/j.apcatb.2017.02.056},
journal = {Applied Catalysis. B, Environmental},
number = C,
volume = 209,
place = {United States},
year = {Sat Jul 01 00:00:00 EDT 2017},
month = {Sat Jul 01 00:00:00 EDT 2017}
}