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Title: Cobalt-Molybdenum Single-Layered Nanocatalysts Decorated on Carbon Nanotubes and the Influence of Preparation Conditions on Their Hydrodesulfurization Catalytic Activity

Abstract

Hydrodesulfurization (HDS) of crude oil plays a vital role in the refining of petroleum products. With ever-increasing regulations restricting the allowable concentrations of sulfur in fuel, further research is required to produce more efficient and effective catalysts. Herein, we have synthesized carbon nanotube (CNT)-supported cobalt-molybdenum (CoMo) catalysts for HDS of dibenzothiophene (DBT) via Co-first and Mo-first sequential impregnation as well as co-impregnation. Spectroscopic analysis shows the formation of a CoMo catalyst with no free sulfided Co phase present. Additionally, CoMo catalysts are found to be predominantly single-layered nanocatalysts layered on the CNT support. Temperature-programmed reduction (TPR) measurements show differences in reducing temperature of the sulfided CoMo catalysts prepared by the different methods, but catalyst activities for HDS of DBT did not fully align with the TPR-predicted order. Thus, provided the reaction temperature is high enough, reducibility may not always be an adequate gauge of catalytic activity. Conversion of DBT was highest in Mo-first sequential impregnation (81.5%), followed by co-impregnation (64%) and Co-first sequential impregnation (60%) on a CNT support. While these results contrast with some others regarding the order of impregnation, we propose that the preferred impregnation order is actually support-dependent, rather than an absolute quality.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [3];  [3];  [4];  [5];  [6];  [3];  [7]; ORCiD logo [3]
  1. Department of Chemical Engineering, The Petroleum Institute, Khalifa University of Science and Technology, P.O. Box 127788, Abu Dhabi, United Arab Emirates; Chemistry Program, Division of Science, New York University Abu Dhabi, P.O. Box 129188, Abu Dhabi, United Arab Emirates
  2. Department of Chemical Engineering, The Petroleum Institute, Khalifa University of Science and Technology, P.O. Box 127788, Abu Dhabi, United Arab Emirates; TITAN Cement Company, 22Α Ηalkidos Str., P.O. 111 43, Αthens, Greece
  3. Department of Chemical Engineering, The Petroleum Institute, Khalifa University of Science and Technology, P.O. Box 127788, Abu Dhabi, United Arab Emirates
  4. Department of Chemical Engineering, The Petroleum Institute, Khalifa University of Science and Technology, P.O. Box 127788, Abu Dhabi, United Arab Emirates; Centre for Organic Chemistry “C.D. Nenitescu”, Romanian Academy, 202B Spl Independentei, 060023 Bucharest, Romania
  5. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  6. Department of Physics and Astronomy and Department of Electrical Engineering and Computer Science, Vanderbilt University, Nashville, Tennessee 37235, United States
  7. Department of Chemical Engineering, The Petroleum Institute, Khalifa University of Science and Technology, P.O. Box 127788, Abu Dhabi, United Arab Emirates; Department of Chemical and Biochemical Engineering, University Politehnica of Bucharest, 313 Spl. Independentei, sector 6, 060042 Bucharest, Romania
Publication Date:
Research Org.:
Vanderbilt Univ., Nashville, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1597897
Grant/Contract Number:  
[FG02-09ER46554]
Resource Type:
Accepted Manuscript
Journal Name:
Energy and Fuels
Additional Journal Information:
[ Journal Volume: 32; Journal Issue: 7]; Journal ID: ISSN 0887-0624
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Whelan, Jamie, Katsiotis, Marios S., Stephen, Samuel, Luckachan, Gisha E., Tharalekshmy, Anjana, Banu, Nicoleta Doriana, Idrobo, Juan-Carlos, Pantelides, Sokrates T., Vladea, Radu V., Banu, Ionut, and Alhassan, Saeed M. Cobalt-Molybdenum Single-Layered Nanocatalysts Decorated on Carbon Nanotubes and the Influence of Preparation Conditions on Their Hydrodesulfurization Catalytic Activity. United States: N. p., 2018. Web. doi:10.1021/acs.energyfuels.8b01571.
Whelan, Jamie, Katsiotis, Marios S., Stephen, Samuel, Luckachan, Gisha E., Tharalekshmy, Anjana, Banu, Nicoleta Doriana, Idrobo, Juan-Carlos, Pantelides, Sokrates T., Vladea, Radu V., Banu, Ionut, & Alhassan, Saeed M. Cobalt-Molybdenum Single-Layered Nanocatalysts Decorated on Carbon Nanotubes and the Influence of Preparation Conditions on Their Hydrodesulfurization Catalytic Activity. United States. doi:10.1021/acs.energyfuels.8b01571.
Whelan, Jamie, Katsiotis, Marios S., Stephen, Samuel, Luckachan, Gisha E., Tharalekshmy, Anjana, Banu, Nicoleta Doriana, Idrobo, Juan-Carlos, Pantelides, Sokrates T., Vladea, Radu V., Banu, Ionut, and Alhassan, Saeed M. Fri . "Cobalt-Molybdenum Single-Layered Nanocatalysts Decorated on Carbon Nanotubes and the Influence of Preparation Conditions on Their Hydrodesulfurization Catalytic Activity". United States. doi:10.1021/acs.energyfuels.8b01571. https://www.osti.gov/servlets/purl/1597897.
@article{osti_1597897,
title = {Cobalt-Molybdenum Single-Layered Nanocatalysts Decorated on Carbon Nanotubes and the Influence of Preparation Conditions on Their Hydrodesulfurization Catalytic Activity},
author = {Whelan, Jamie and Katsiotis, Marios S. and Stephen, Samuel and Luckachan, Gisha E. and Tharalekshmy, Anjana and Banu, Nicoleta Doriana and Idrobo, Juan-Carlos and Pantelides, Sokrates T. and Vladea, Radu V. and Banu, Ionut and Alhassan, Saeed M.},
abstractNote = {Hydrodesulfurization (HDS) of crude oil plays a vital role in the refining of petroleum products. With ever-increasing regulations restricting the allowable concentrations of sulfur in fuel, further research is required to produce more efficient and effective catalysts. Herein, we have synthesized carbon nanotube (CNT)-supported cobalt-molybdenum (CoMo) catalysts for HDS of dibenzothiophene (DBT) via Co-first and Mo-first sequential impregnation as well as co-impregnation. Spectroscopic analysis shows the formation of a CoMo catalyst with no free sulfided Co phase present. Additionally, CoMo catalysts are found to be predominantly single-layered nanocatalysts layered on the CNT support. Temperature-programmed reduction (TPR) measurements show differences in reducing temperature of the sulfided CoMo catalysts prepared by the different methods, but catalyst activities for HDS of DBT did not fully align with the TPR-predicted order. Thus, provided the reaction temperature is high enough, reducibility may not always be an adequate gauge of catalytic activity. Conversion of DBT was highest in Mo-first sequential impregnation (81.5%), followed by co-impregnation (64%) and Co-first sequential impregnation (60%) on a CNT support. While these results contrast with some others regarding the order of impregnation, we propose that the preferred impregnation order is actually support-dependent, rather than an absolute quality.},
doi = {10.1021/acs.energyfuels.8b01571},
journal = {Energy and Fuels},
number = [7],
volume = [32],
place = {United States},
year = {2018},
month = {6}
}

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