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Title: Hydrodechlorination of 1,2-Dichloroethane Catalyzedby Dendrimer-Derived Pt-Cu/SiO2 Catalysts

Abstract

Dendrimer-metal-nanocomposites (DMNs) were used as precursors to prepare SiO2 supported monometallic Pt, Cu and bimetallic Pt-Cu catalysts with Pt/Cu atomic ratios of 1:1 (Pt50Cu50) and 1:3 (Pt25Cu75). After impregnation of these DMNs onto the support, the catalysts were thermally treated and activated following an optimized protocol. Scanning transmission electron microscopy (STEM) shows that the metal nanoparticles in dendrimer-derived SiO2-supported catalysts are smaller and have a more narrow size distribution than those in conventional catalysts prepared using corresponding metal salts via the wet impregnation method. Slow deactivation was observed for hydrodechlorination of 1,2-dichloroethane over monometallic Cu catalysts, which showed an activity about one to two orders of magnitude lower than that of the Pt-containing catalysts. Hydrodechlorination of 1,2-dichloroethane over Pt and Pt50Cu50 catalysts mainly produces ethane and the selectivity towards ethane increases with temperature. For Pt25Cu75 catalyst, the selectivity towards ethane decreases in favor of ethylene. The overall activity decreases with increasing Cu loading in the catalysts. Activity based on surface Pt sites suggests the formation of bi-functional surfaces in Pt25Cu75 catalyst favoring C-Cl bond scission on Cu sites and hydrogenation of intermediate .CH2CH2. on Pt sites. Furthermore, kinetic analyses suggest different reaction mechanisms for hydrodechlorination of 1,2-dichloroethane over Pt andmore » Cu-enriched surfaces in the Pt-Cu bimetallic catalysts.« less

Authors:
 [1];  [1];  [1];  [2];  [3];  [3]
  1. ORNL
  2. University of South Carolina, Columbia
  3. University of South Carolina
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
979088
DOE Contract Number:  
DE-AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 259; Journal Issue: 1; Journal ID: ISSN 0021-9517
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CHLORINATED ALIPHATIC HYDROCARBONS; DECHLORINATION; HYDROGENATION; CATALYTIC EFFECTS; PLATINUM; COPPER; CATALYST SUPPORTS; SILICON OXIDES; CHEMICAL PREPARATION; CATALYSTS; CHEMICAL REACTION KINETICS; ETHANE; ETHYLENE

Citation Formats

Xie, Hong, Howe, Jane Y, Schwartz, Viviane, Monnier, J. R., Williams, Christopher T., and Ploehn, Harry J. Hydrodechlorination of 1,2-Dichloroethane Catalyzedby Dendrimer-Derived Pt-Cu/SiO2 Catalysts. United States: N. p., 2008. Web. doi:10.1016/j.jcat.2008.07.018.
Xie, Hong, Howe, Jane Y, Schwartz, Viviane, Monnier, J. R., Williams, Christopher T., & Ploehn, Harry J. Hydrodechlorination of 1,2-Dichloroethane Catalyzedby Dendrimer-Derived Pt-Cu/SiO2 Catalysts. United States. https://doi.org/10.1016/j.jcat.2008.07.018
Xie, Hong, Howe, Jane Y, Schwartz, Viviane, Monnier, J. R., Williams, Christopher T., and Ploehn, Harry J. 2008. "Hydrodechlorination of 1,2-Dichloroethane Catalyzedby Dendrimer-Derived Pt-Cu/SiO2 Catalysts". United States. https://doi.org/10.1016/j.jcat.2008.07.018.
@article{osti_979088,
title = {Hydrodechlorination of 1,2-Dichloroethane Catalyzedby Dendrimer-Derived Pt-Cu/SiO2 Catalysts},
author = {Xie, Hong and Howe, Jane Y and Schwartz, Viviane and Monnier, J. R. and Williams, Christopher T. and Ploehn, Harry J.},
abstractNote = {Dendrimer-metal-nanocomposites (DMNs) were used as precursors to prepare SiO2 supported monometallic Pt, Cu and bimetallic Pt-Cu catalysts with Pt/Cu atomic ratios of 1:1 (Pt50Cu50) and 1:3 (Pt25Cu75). After impregnation of these DMNs onto the support, the catalysts were thermally treated and activated following an optimized protocol. Scanning transmission electron microscopy (STEM) shows that the metal nanoparticles in dendrimer-derived SiO2-supported catalysts are smaller and have a more narrow size distribution than those in conventional catalysts prepared using corresponding metal salts via the wet impregnation method. Slow deactivation was observed for hydrodechlorination of 1,2-dichloroethane over monometallic Cu catalysts, which showed an activity about one to two orders of magnitude lower than that of the Pt-containing catalysts. Hydrodechlorination of 1,2-dichloroethane over Pt and Pt50Cu50 catalysts mainly produces ethane and the selectivity towards ethane increases with temperature. For Pt25Cu75 catalyst, the selectivity towards ethane decreases in favor of ethylene. The overall activity decreases with increasing Cu loading in the catalysts. Activity based on surface Pt sites suggests the formation of bi-functional surfaces in Pt25Cu75 catalyst favoring C-Cl bond scission on Cu sites and hydrogenation of intermediate .CH2CH2. on Pt sites. Furthermore, kinetic analyses suggest different reaction mechanisms for hydrodechlorination of 1,2-dichloroethane over Pt and Cu-enriched surfaces in the Pt-Cu bimetallic catalysts.},
doi = {10.1016/j.jcat.2008.07.018},
url = {https://www.osti.gov/biblio/979088}, journal = {Journal of Catalysis},
issn = {0021-9517},
number = 1,
volume = 259,
place = {United States},
year = {Tue Jan 01 00:00:00 EST 2008},
month = {Tue Jan 01 00:00:00 EST 2008}
}