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The role of heterogeneous catalysts in the plasma-catalytic ammonia synthesis
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Patil, Bhaskar S., Cherkasov, Nikolay, Srinath, Nadadur Veeraraghavan, Lang, Juergen, Ibhadon, Alex O., Wang, Qi and Hessel, Volker (2021) The role of heterogeneous catalysts in the plasma-catalytic ammonia synthesis. Catalysis Today, 362 . pp. 2-10. doi:10.1016/j.cattod.2020.06.074 ISSN 0920-5861.
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WRAP-Role-heterogeneous-catalysis-plasma-ammonia-synthesis-Cherkasov-2020.pdf - Accepted Version - Requires a PDF viewer. Available under License Creative Commons Attribution Non-commercial No Derivatives 4.0. Download (2211Kb) | Preview |
Official URL: https://doi.org/10.1016/j.cattod.2020.06.074
Abstract
Ammonia, being the second largest produced industrial chemical, is used as a raw material for many chemicals. Besides, there is a growing interest in the applications of ammonia as electrical energy storage chemical, as fuel, and in selective catalytic reduction of NOx. These applications demand on-site distributed ammonia production under mild process conditions. In this paper, we investigated 16 different transition metal and oxide catalysts supported on γ-Al2O3 for plasma-catalytic ammonia production in a dielectric barrier discharge (DBD) reactor. This paper discusses the influence of the feed ratio (N2/H2), specific energy input, reaction temperature, metal loading, and gas flow rates on the yield and energy efficiency of ammonia production. The optimum N2/H2 feed flow ratio was either 1 or 2 depending on the catalyst – substantially above ammonia stoichiometry of 0.33. The concentration of ammonia formed was proportional to the specific energy input. Increasing the reaction temperature or decreasing gas flow rates resulted in a lower specific production due to ammonia decomposition. The most efficient catalysts were found to be 2 wt% Rh/Al2O3 among platinum-group metals and 5 wt% Ni/Al2O3 among transitional metals. With the 2 wt% Rh catalyst, 1.43 vol% ammonia was produced with an energy efficiency of 0.94 g kWh−1. The observed behaviour was explained by a combination of gas-phase and catalytic ammonia formation reactions with plasma-activated nitrogen species. Plasma catalysts provide a synergetic effect by activation of hydrogen on the surface requiring lower-energy nitrogen species.
Item Type: | Journal Article | ||||||||
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Subjects: | Q Science > QD Chemistry | ||||||||
Divisions: | Faculty of Science, Engineering and Medicine > Engineering > Engineering | ||||||||
SWORD Depositor: | Library Publications Router | ||||||||
Library of Congress Subject Headings (LCSH): | Plasma chemistry, Catalysis, Ammonia , Ammonia -- Synthesis, Transition metal oxides , Chemical kinetics | ||||||||
Journal or Publication Title: | Catalysis Today | ||||||||
Publisher: | Elsevier | ||||||||
ISSN: | 0920-5861 | ||||||||
Official Date: | 15 February 2021 | ||||||||
Dates: |
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Volume: | 362 | ||||||||
Page Range: | pp. 2-10 | ||||||||
DOI: | 10.1016/j.cattod.2020.06.074 | ||||||||
Status: | Peer Reviewed | ||||||||
Publication Status: | Published | ||||||||
Access rights to Published version: | Restricted or Subscription Access | ||||||||
Date of first compliant deposit: | 14 August 2020 | ||||||||
Date of first compliant Open Access: | 25 July 2021 | ||||||||
RIOXX Funder/Project Grant: |
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