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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. Finally, 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. Khalifa Univ. of Science and Technology, Abu Dhabi (United Arab Emirates); New York Univ., Abu Dhabi (United Arab Emirates)
  2. Khalifa Univ. of Science and Technology, Abu Dhabi (United Arab Emirates); TITAN Cement Company, Athens (Greece)
  3. Khalifa Univ. of Science and Technology, Abu Dhabi (United Arab Emirates)
  4. Khalifa Univ. of Science and Technology, Abu Dhabi (United Arab Emirates); Romanian Academy, Bucharest (Romania)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  6. Vanderbilt Univ., Nashville, TN (United States)
  7. Khalifa Univ. of Science and Technology, Abu Dhabi (United Arab Emirates); Univ. Politehnica of Bucharest, 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; thiophenes; catalysts; carbon nanotubes; order; materials

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:https://doi.org/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. Tue . "Cobalt-Molybdenum Single-Layered Nanocatalysts Decorated on Carbon Nanotubes and the Influence of Preparation Conditions on Their Hydrodesulfurization Catalytic Activity". United States. doi:https://doi.org/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. Finally, 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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Works referencing / citing this record:

Sacrificial carbonaceous coating over alumina supported Ni–MoS 2 catalyst for hydrodesulfurization
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