An Experimental Observation of the Thermal Effects and NO Emissions during Dissociation and Oxidation of Ammonia in the Presence of a Bundle of Thermocouples in a Vertical Flow Reactor
Ammonia (NH3) dissociation and
oxidation in a cylindrical quartz reactor has been experimentally studied for
various inlet NH3 concentrations (5%, 10%, and 15%) and reactor
temperatures between 700K and 1000K. The thermal effects
during both NH3 dissociation (endothermic) and oxidation (exothermic) were observed using a bundle of
thermocouples positioned along the central axis of the quartz reactor,
while the corresponding NH3 conversions and nitrogen oxides
emissions were determined by analysing the gas composition of the reactor exit
stream. A stronger endothermic effect, as indicated by a greater temperature
drop during NH3 dissociation, was observed as the NH3 feed concentration and reactor temperature increased. During NH3 oxidation, a predominantly greater exothermic effect with increasing NH3 feed concentration and reactor temperature was also evident; however, it was apparent that NH3 dissociation occurred near
the reactor inlet, preceding the downstream NH3 and H2 oxidation. For both NH
References
[1]
Riahi, K. and Roehrl, R.A. (2000) Energy Technology Strategies for Carbon Dioxide Mitigation and Sustainable Development. Environmental Economics and Policy Studies, 3, 89-123. https://doi.org/10.1007/BF03354032
[2]
Hignett, T.P. (1985) Transportation and Storage of Ammonia. In: Hignett, T.P., Eds., Fertilizer Manual, Springer, Dordrecht, 73-82. https://doi.org/10.1007/978-94-017-1538-6_7
[3]
Ullman, F. (2000) Ullmann’s Encyclopedia of Industrial Chemistry. Wiley-VCH, Weinheim.
[4]
Valera-Medina, A., Xiao, H., Owen-Jones, M., David, W.I.F. and Bowen, P.J. (2018) Ammonia for Power. Progress in Energy and Combustion Science, 69, 63-102. https://doi.org/10.1016/j.pecs.2018.07.001
[5]
Zamfirescu, C. and Dincer, I. (2009) Ammonia as a Green Fuel and Hydrogen Source for Vehicular Applications. Fuel Processing Technology, 90, 729-737. https://doi.org/10.1016/j.fuproc.2009.02.004
[6]
Appl, M. (1999) Ammonia: Principles and Industrial Practice. Wiley-VCH, Weinheim. https://doi.org/10.1002/9783527613885
[7]
Flank, W.H., Abraham, M.A. and Matthews, M.A. (2009) Innovations in Industrial and Engineering Chemistry: A Century of Achievements and Prospects for the New Millennium. American Chemical Society, Washington DC. https://doi.org/10.1021/bk-2009-1000
[8]
Modak, J.M. (2011) Haber Process for Ammonia Synthesis. Resonance, 16, 1159-1167. https://doi.org/10.1007/s12045-011-0130-0
[9]
Smith, C., Hill, A.K. and Torrente-Murciano, L. (2020) Current and Future Role of Haber–Bosch Ammonia in a Carbon-Free Energy Landscape. Energy & Environmental Science, 13, 331-344. https://doi.org/10.1039/C9EE02873K
[10]
Zhang, R., Wang, J., Zhang, Y., Cheng, F., Liu, Y., Gao, J., Holden, S.R. and Zhang, D. (2022) An Experimental Study of Ammonia Dissociation in a Fixed-Bed Reactor Packed with Quartz Particles. Clearwater Clean Energy Conference, Clearwater, 1-4 August 2022, 1-8.
[11]
Huo, Y., Zhang, R., Zhu, S., Gao, J., Holden, S.R., Zhu, M., Zhang, Z. and Zhang, D. (2022) A Preliminary Experimental Investigation into Ammonia Oxidation in a Fixed-Bed. International Journal of Energy for a Clean Environment, 23, 23-37. https://doi.org/10.1615/InterJEnerCleanEnv.2022039811
[12]
Benés, M., Pozo, G., Abián, M., Millera, Á., Bilbao, R. and Alzueta, M.U. (2021) Experimental Study of the Pyrolysis of NH3 under Flow Reactor Conditions. Energy & fuels, 35, 7193-7200. https://doi.org/10.1021/acs.energyfuels.0c03387
[13]
Manna, M.V., Sabia, P., Ragucci, R. and de Joannon, M. (2020) Oxidation and Pyrolysis of Ammonia Mixtures in Model Reactors. Fuel, 264, Article ID: 116768. https://doi.org/10.1016/j.fuel.2019.116768
[14]
Gómez-García, M.A., Pitchon, V. and Kiennemann, A. (2005) Pollution by Nitrogen Oxides: An Approach to NOX Abatement by Using Sorbing Catalytic Materials. Environment International, 31, 445-467. https://doi.org/10.1016/j.envint.2004.09.006
[15]
Husnain, N., Wang, E., Li, K., Anwar, M.T., Mehmood, A., Gul, M., Li, D. and Mao, J. (2019) Iron Oxide-Based Catalysts for Low-Temperature Selective Catalytic Reduction of NOX with NH3. Reviews in Chemical Engineering, 35, 239-264. https://doi.org/10.1515/revce-2017-0064
[16]
Li, Z., Chen, G., Shao, Z., Zhang, H. and Guo, X. (2022) The Effect of Iron Content on the Ammonia Selective Catalytic Reduction Reaction (NH3-SCR) Catalytic Performance of FeOX/SAPO-34. International Journal of Environmental Research and Public Health, 19, Article 14749. https://doi.org/10.3390/ijerph192214749
[17]
Javed, M.T., Ahmed, Z., Ibrahim, M.A. and Irfan, N. (2008) A Comparative Kinetic Study of SNCR Process Using Ammonia. Brazilian Journal of Chemical Engineering, 25, 109-117. https://doi.org/10.1590/S0104-66322008000100012
[18]
Locci, C., Vervisch, L., Farcy, B., Domingo, P. and Perret, N. (2018) Selective Non-Catalytic Reduction (SNCR) of Nitrogen Oxide Emissions: A Perspective from Numerical Modeling. Flow, Turbulence and Combustion, 100, 301-340. https://doi.org/10.1007/s10494-017-9842-x
[19]
Sorrels, J.L., Randall, D.D., Fry, C.R. and Schaffner, K.S. (2019) Selective Noncatalytic Reduction. U.S. Environmental Protection Agency.
[20]
Nakamura, H., Hasegawa, S. and Tezuka, T. (2017) Kinetic Modeling of Ammonia/Air Weak Flames in a Micro Flow Reactor with a Controlled Temperature Profile. Combustion and Flame, 185, 16-27. https://doi.org/10.1016/j.combustflame.2017.06.021
[21]
Stagni, A., Cavallotti, C., Arunthanayothin, S., Song, Y., Herbinet, O., Battin-Leclerc, F. and Faravelli, T. (2020) An Experimental, Theoretical and Kinetic-Modeling Study of the Gas-Phase Oxidation of Ammonia. Reaction Chemistry & Engineering, 5, 696-711. https://doi.org/10.1039/C9RE00429G
[22]
Feng, P., Lee, M., Wang, D. and Suzuki, Y. (2023) Ammonia Thermal Decomposition on Quartz and Stainless Steel Walls. International Journal of Hydrogen Energy. https://doi.org/10.1016/j.ijhydene.2023.04.106
[23]
Jennings, J.R. (1991) Catalytic Ammonia Synthesis, Fundamentals and Practice. Plenum Press, New York. https://doi.org/10.1007/978-1-4757-9592-9
[24]
Liu, H. (2013) Ammonia Synthesis Catalysts: Innovation and Practice. World Scientific Publishing Co. Pte. Ltd and Chemical Industry Press, Singapore and Beijing.
[25]
Liu, H. (2014) Ammonia Synthesis Catalyst 100 Years: Practice, Enlightenment and Challenge. Chinese Journal of Catalysis, 35, 1619-1640. https://doi.org/10.1016/S1872-2067(14)60118-2
[26]
Arabczyk, W. and Zamłynny, J. (1999) Study of the Ammonia Decomposition over Iron Catalysts. Catalysis Letters, 60, 167-171. https://doi.org/10.1023/A:1019007024041
[27]
Pelka, R., Moszyńska, I. and Arabczyk, W. (2009) Catalytic Ammonia Decomposition Over Fe/Fe4N. Catalysis Letters, 128, 72-76. https://doi.org/10.1007/s10562-008-9758-0
[28]
Lucentini, I., Garcia, X., Vendrell, X. and Llorca, J. (2021) Review of the Decomposition of Ammonia to Generate Hydrogen. Industrial & Engineering Chemistry Research, 60, 18560-18611. https://doi.org/10.1021/acs.iecr.1c00843