Structure sensitivity and its effect on methane turnover and carbon co-product selectivity in thermocatalytic decomposition of methane over supported Ni catalysts
Abstract
We explore how thermocatalytic decomposition of methane (TCD) is a promising approach for producing CO2-free hydrogen and solid carbon co-product. In this study, a series of Al2O3- and MgAl2O4-based Ni catalysts, prepared with varying synthesis and pretreatment methods, were evaluated for methane TCD performance at 650°C and characterized before and after reaction to elucidate activity-structure relationships. We found that methane TCD turnover increases with Ni particle size. Further, large Ni particle sizes (i.e., >20 nm) are selective toward the formation of carbon nanotubes (CNTs), while small Ni particle sizes (i.e., <10 nm) are selective toward the formation of graphitic carbon layers. The formation of graphitic carbon layers block access to Ni active sites, thus rendering the catalyst inactive more quickly than when CNTs are produced. Additionally, the catalyst deactivation observed with time-on-stream is due to the fragmentation of Ni particles into smaller Ni particles followed by their encapsulation with graphitic carbon layers.
- Authors:
-
[1];
[1];
[1];
[1]
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- West Virginia Univ., Morgantown, WV (United States)
- (John) [West Virginia Univ., Morgantown, WV (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1755019
- Alternate Identifier(s):
- OSTI ID: 1778323
- Report Number(s):
- PNNL-SA-158733
Journal ID: ISSN 0926-860X
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Catalysis. A, General
- Additional Journal Information:
- Journal Volume: 611; Journal ID: ISSN 0926-860X
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Thermocatalytic decomposition; Ni catalysts; Carbon nanotubes; Structure sensitivity; Ni particle size
Citation Formats
Xu, Mengze, Lopez-Ruiz, Juan A., Kovarik, Libor, Bowden, Mark E., Davidson, Stephen D., Weber, Robert S., Wang, I-Wen, Hu, Jianli, and Dagle, Robert A. Structure sensitivity and its effect on methane turnover and carbon co-product selectivity in thermocatalytic decomposition of methane over supported Ni catalysts. United States: N. p., 2021.
Web. doi:10.1016/j.apcata.2020.117967.
Xu, Mengze, Lopez-Ruiz, Juan A., Kovarik, Libor, Bowden, Mark E., Davidson, Stephen D., Weber, Robert S., Wang, I-Wen, Hu, Jianli, & Dagle, Robert A. Structure sensitivity and its effect on methane turnover and carbon co-product selectivity in thermocatalytic decomposition of methane over supported Ni catalysts. United States. https://doi.org/10.1016/j.apcata.2020.117967
Xu, Mengze, Lopez-Ruiz, Juan A., Kovarik, Libor, Bowden, Mark E., Davidson, Stephen D., Weber, Robert S., Wang, I-Wen, Hu, Jianli, and Dagle, Robert A. Mon .
"Structure sensitivity and its effect on methane turnover and carbon co-product selectivity in thermocatalytic decomposition of methane over supported Ni catalysts". United States. https://doi.org/10.1016/j.apcata.2020.117967. https://www.osti.gov/servlets/purl/1755019.
@article{osti_1755019,
title = {Structure sensitivity and its effect on methane turnover and carbon co-product selectivity in thermocatalytic decomposition of methane over supported Ni catalysts},
author = {Xu, Mengze and Lopez-Ruiz, Juan A. and Kovarik, Libor and Bowden, Mark E. and Davidson, Stephen D. and Weber, Robert S. and Wang, I-Wen and Hu, Jianli and Dagle, Robert A.},
abstractNote = {We explore how thermocatalytic decomposition of methane (TCD) is a promising approach for producing CO2-free hydrogen and solid carbon co-product. In this study, a series of Al2O3- and MgAl2O4-based Ni catalysts, prepared with varying synthesis and pretreatment methods, were evaluated for methane TCD performance at 650°C and characterized before and after reaction to elucidate activity-structure relationships. We found that methane TCD turnover increases with Ni particle size. Further, large Ni particle sizes (i.e., >20 nm) are selective toward the formation of carbon nanotubes (CNTs), while small Ni particle sizes (i.e., <10 nm) are selective toward the formation of graphitic carbon layers. The formation of graphitic carbon layers block access to Ni active sites, thus rendering the catalyst inactive more quickly than when CNTs are produced. Additionally, the catalyst deactivation observed with time-on-stream is due to the fragmentation of Ni particles into smaller Ni particles followed by their encapsulation with graphitic carbon layers.},
doi = {10.1016/j.apcata.2020.117967},
journal = {Applied Catalysis. A, General},
number = ,
volume = 611,
place = {United States},
year = {Mon Feb 01 00:00:00 EST 2021},
month = {Mon Feb 01 00:00:00 EST 2021}
}
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