Effects of support and promoter on Ru catalyst activity in microwave-assisted ammonia synthesis
Abstract
Microwave-assisted ammonia synthesis is a promising alternative to the energy-intensive Haber-Bosch process, specially at small- and medium-scale with renewable H2 as resource. Here, we report that Cs promoted Ru/CeO2 catalyst exhibits considerable activity at 533 K and ambient pressure. In this work, the combined theoretical and experimental approaches are adopted to optimize the electronic and geometric structures of Ru on the catalysts. Both DFT modeling work and structural characterization show that the strong interaction between Ru and CeO2 results in the formation of highly dispersed Ru particles favoring ammonia synthesis. The higher electron donating ability of CeO2 and lower electronegativity of Cs promoter result in higher electron density on Ru reducing the N≡N dissociation barrier. Finally, the work demonstrates the potential of microwave-assisted catalytic process in activating stable molecules for ammonia synthesis.
- Authors:
-
- West Virginia Univ., Morgantown, WV (United States)
- National Energy Technology Laboratory (NETL), Morgantown, WV (United States); Leidos, Morgantown, WV (United States)
- West Virginia Univ., Morgantown, WV (United States); Council of Scientific & Industrial Research (CSIR), Dehradun (India). Indian Inst. of Petroleum
- National Energy Technology Laboratory (NETL), Morgantown, WV (United States)
- Marshall Univ., Huntington, WV (United States)
- Publication Date:
- Research Org.:
- National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
- Sponsoring Org.:
- USDOE Office of Fossil Energy (FE); USDOE Advanced Research Projects Agency - Energy (ARPA-E)
- OSTI Identifier:
- 1871013
- Alternate Identifier(s):
- OSTI ID: 1786404
- Report Number(s):
- DOE/NETL-2021/2838
Journal ID: ISSN 1385-8947
- Grant/Contract Number:
- AR0000807
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemical Engineering Journal
- Additional Journal Information:
- Journal Volume: 425; Journal Issue: 2021; Journal ID: ISSN 1385-8947
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ammonia synthesis; microwave; Ru catalyst; density functional theory; promoters
Citation Formats
Wang, Yuxin, Wildfire, Christina, Khan, Tuhin S., Shekhawat, Dushyant, Hu, Jianli, Tavadze, Pedram, Quiñones-Fernández, Rosalynn, and Moreno, Sara. Effects of support and promoter on Ru catalyst activity in microwave-assisted ammonia synthesis. United States: N. p., 2021.
Web. doi:10.1016/j.cej.2021.130546.
Wang, Yuxin, Wildfire, Christina, Khan, Tuhin S., Shekhawat, Dushyant, Hu, Jianli, Tavadze, Pedram, Quiñones-Fernández, Rosalynn, & Moreno, Sara. Effects of support and promoter on Ru catalyst activity in microwave-assisted ammonia synthesis. United States. https://doi.org/10.1016/j.cej.2021.130546
Wang, Yuxin, Wildfire, Christina, Khan, Tuhin S., Shekhawat, Dushyant, Hu, Jianli, Tavadze, Pedram, Quiñones-Fernández, Rosalynn, and Moreno, Sara. Tue .
"Effects of support and promoter on Ru catalyst activity in microwave-assisted ammonia synthesis". United States. https://doi.org/10.1016/j.cej.2021.130546. https://www.osti.gov/servlets/purl/1871013.
@article{osti_1871013,
title = {Effects of support and promoter on Ru catalyst activity in microwave-assisted ammonia synthesis},
author = {Wang, Yuxin and Wildfire, Christina and Khan, Tuhin S. and Shekhawat, Dushyant and Hu, Jianli and Tavadze, Pedram and Quiñones-Fernández, Rosalynn and Moreno, Sara},
abstractNote = {Microwave-assisted ammonia synthesis is a promising alternative to the energy-intensive Haber-Bosch process, specially at small- and medium-scale with renewable H2 as resource. Here, we report that Cs promoted Ru/CeO2 catalyst exhibits considerable activity at 533 K and ambient pressure. In this work, the combined theoretical and experimental approaches are adopted to optimize the electronic and geometric structures of Ru on the catalysts. Both DFT modeling work and structural characterization show that the strong interaction between Ru and CeO2 results in the formation of highly dispersed Ru particles favoring ammonia synthesis. The higher electron donating ability of CeO2 and lower electronegativity of Cs promoter result in higher electron density on Ru reducing the N≡N dissociation barrier. Finally, the work demonstrates the potential of microwave-assisted catalytic process in activating stable molecules for ammonia synthesis.},
doi = {10.1016/j.cej.2021.130546},
journal = {Chemical Engineering Journal},
number = 2021,
volume = 425,
place = {United States},
year = {Tue Jun 01 00:00:00 EDT 2021},
month = {Tue Jun 01 00:00:00 EDT 2021}
}
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