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Title: HDS and deep HDS activity of Co/Mo/S-mesostructured synthetic clays.

Abstract

The goal of this work is to identify more promising supports from synthetic clay materials to advance hydrotreating catalyst development. Silica sol can be used as the silicon-containing starting material when creating nanoporous layered silicate catalysts with a certain portion of unreacted sol particles incorporated into the final matrix. The resulting structure then has mesoporosity and a unique morphology. Hectorite-based clays have been prepared using different silica sols in order to ascertain the importance of sol characteristics on the final matrix. Several techniques have been applied to characterize the materials, including XRD, TGA, N2 porosimetry, and TEM. For hydrodesulfurization (HDS), the conversion of dibenzothiophene (DBT) to biphenyl was examined at 400 degrees C using CoMoS-loaded mesostructured clay supports. No hydrogenation or hydrocracking was observed with any of the clay supports. The most active clay was derived from Ludox silica sol AS-30 with an activity of 65% DBT conversion and 100% selectivity to biphenyl (BP). For comparison, a reference commercial catalyst displayed 94% BP selectivity. For deep HDS, the conversion of 4,6-dimethyldibenzothiophene was tested at 325 and 350 degrees C. At 325 degrees C, conversions are 92% of commercial catalysts for a CoMoS-loaded mesostructured clay derived from Ludox AM-30 silica sol.more » A commercially available synthetic hectorite called laponite has very low activity, indicating that the unique morphology of the mesostructured clays is important. Hydrogenolysis vs. hydrogenation pathways are compared for the deep HDS reaction. HR-TEM of the most active deep HDS catalyst revealed a multilayered MoS2 morphology.« less

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
982017
Report Number(s):
ANL/CHM/CP-114858
TRN: US201013%%869
DOE Contract Number:  
DE-AC02-06CH11357
Resource Type:
Conference
Resource Relation:
Journal Name: Catal. Today; Journal Volume: 116; Journal Issue: 4 ; 2006; Conference: 229th American Chemical Society National Meeting; Mar. 13, 2005 - Mar. 17, 2005; San Diego, CA
Country of Publication:
United States
Language:
ENGLISH
Subject:
36 MATERIALS SCIENCE; BIPHENYL; CATALYSTS; CLAYS; CONVERSION; HYDROCRACKING; HYDROGENATION; MATERIALS; MEETINGS; MONTMORILLONITE; MORPHOLOGY; PARTICLES; SILICA; SILICATES; SOLS; SUPPORTS; WORK; X-RAY DIFFRACTION

Citation Formats

Carrado, K. A., Song, C., Kim, J. H., Castagnola, N., Fernandez-Saavedra, R., Marshall, C. L., Schwartz, M. M., Penn State Univ., and ICMM-CSIC. HDS and deep HDS activity of Co/Mo/S-mesostructured synthetic clays.. United States: N. p., 2006. Web. doi:10.1016/j.cattod.2006.06.033.
Carrado, K. A., Song, C., Kim, J. H., Castagnola, N., Fernandez-Saavedra, R., Marshall, C. L., Schwartz, M. M., Penn State Univ., & ICMM-CSIC. HDS and deep HDS activity of Co/Mo/S-mesostructured synthetic clays.. United States. doi:10.1016/j.cattod.2006.06.033.
Carrado, K. A., Song, C., Kim, J. H., Castagnola, N., Fernandez-Saavedra, R., Marshall, C. L., Schwartz, M. M., Penn State Univ., and ICMM-CSIC. Sun . "HDS and deep HDS activity of Co/Mo/S-mesostructured synthetic clays.". United States. doi:10.1016/j.cattod.2006.06.033.
@article{osti_982017,
title = {HDS and deep HDS activity of Co/Mo/S-mesostructured synthetic clays.},
author = {Carrado, K. A. and Song, C. and Kim, J. H. and Castagnola, N. and Fernandez-Saavedra, R. and Marshall, C. L. and Schwartz, M. M. and Penn State Univ. and ICMM-CSIC},
abstractNote = {The goal of this work is to identify more promising supports from synthetic clay materials to advance hydrotreating catalyst development. Silica sol can be used as the silicon-containing starting material when creating nanoporous layered silicate catalysts with a certain portion of unreacted sol particles incorporated into the final matrix. The resulting structure then has mesoporosity and a unique morphology. Hectorite-based clays have been prepared using different silica sols in order to ascertain the importance of sol characteristics on the final matrix. Several techniques have been applied to characterize the materials, including XRD, TGA, N2 porosimetry, and TEM. For hydrodesulfurization (HDS), the conversion of dibenzothiophene (DBT) to biphenyl was examined at 400 degrees C using CoMoS-loaded mesostructured clay supports. No hydrogenation or hydrocracking was observed with any of the clay supports. The most active clay was derived from Ludox silica sol AS-30 with an activity of 65% DBT conversion and 100% selectivity to biphenyl (BP). For comparison, a reference commercial catalyst displayed 94% BP selectivity. For deep HDS, the conversion of 4,6-dimethyldibenzothiophene was tested at 325 and 350 degrees C. At 325 degrees C, conversions are 92% of commercial catalysts for a CoMoS-loaded mesostructured clay derived from Ludox AM-30 silica sol. A commercially available synthetic hectorite called laponite has very low activity, indicating that the unique morphology of the mesostructured clays is important. Hydrogenolysis vs. hydrogenation pathways are compared for the deep HDS reaction. HR-TEM of the most active deep HDS catalyst revealed a multilayered MoS2 morphology.},
doi = {10.1016/j.cattod.2006.06.033},
journal = {Catal. Today},
number = 4 ; 2006,
volume = 116,
place = {United States},
year = {Sun Jan 01 00:00:00 EST 2006},
month = {Sun Jan 01 00:00:00 EST 2006}
}

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