TY - JOUR
T1 - Steady-state kinetic modeling of NH3-SCR by monolithic Cu-CHA catalysts
AU - Shibata, Gen
AU - Shibayama, Naoki
AU - Araki, Keita
AU - Kobashi, Yoshimitsu
AU - Ogawa, Hideyuki
AU - Nakasaka, Yuta
AU - Shimizu, Ken ichi
N1 - Funding Information:
The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Gen Shibata reports financial support was provided by The Research association of Automotive Internal Combustion Engines. Gen Shibata reports a relationship with The Research association of Automotive Internal Combustion Engines that includes: funding grants.
Publisher Copyright:
© 2022 Elsevier B.V.
PY - 2022
Y1 - 2022
N2 - The kinetic modeling of NH3-SCR with a Cu-ion-exchanged chabazite (Cu-CHA) catalyst in steady-state reactions was investigated by a combination of flow reactor experiments and kinetic modeling with an in-house computational code. Here H-CHA and Cu-CHA monolith cylindrical catalyst specimens were used to identify the reactions at both Brønsted (H+) acid sites and Cu sites. Based on the proposals in the literature for NH3-SCR mechanism, a scheme for SCR and side reactions incorporating 17 reactions is proposed, and some of the reactions were verified by the experimental results here for the adsorption/desorption of NH3, unsteady-state reactions of the adsorbed NH3 with NO2 over the Cu-CHA and H-CHA, and NH3 oxidation over Cu-CHA. The Arrhenius parameters for Standard, Fast, and Slow SCR reactions, NH3 oxidation, NO oxidation to NO2, NO2 decomposition to NO, and NH3 desorption were obtained by kinetic experiments. This report develops a quantitative simulation model for SCR and side reactions, and the model was validated by experimental data for adsorption/desorption of NH3 and NO2, steady-state SCR reactions (Standard, Fast, and Slow SCR), and side reactions (NH3 and NO oxidation). The simulation model developed in this study can predict the steady-state SCR data and adsorption/desorption of NH3 and NO2 under unsteady-state.
AB - The kinetic modeling of NH3-SCR with a Cu-ion-exchanged chabazite (Cu-CHA) catalyst in steady-state reactions was investigated by a combination of flow reactor experiments and kinetic modeling with an in-house computational code. Here H-CHA and Cu-CHA monolith cylindrical catalyst specimens were used to identify the reactions at both Brønsted (H+) acid sites and Cu sites. Based on the proposals in the literature for NH3-SCR mechanism, a scheme for SCR and side reactions incorporating 17 reactions is proposed, and some of the reactions were verified by the experimental results here for the adsorption/desorption of NH3, unsteady-state reactions of the adsorbed NH3 with NO2 over the Cu-CHA and H-CHA, and NH3 oxidation over Cu-CHA. The Arrhenius parameters for Standard, Fast, and Slow SCR reactions, NH3 oxidation, NO oxidation to NO2, NO2 decomposition to NO, and NH3 desorption were obtained by kinetic experiments. This report develops a quantitative simulation model for SCR and side reactions, and the model was validated by experimental data for adsorption/desorption of NH3 and NO2, steady-state SCR reactions (Standard, Fast, and Slow SCR), and side reactions (NH3 and NO oxidation). The simulation model developed in this study can predict the steady-state SCR data and adsorption/desorption of NH3 and NO2 under unsteady-state.
KW - Cu-CHA
KW - Heat-transfer
KW - Kinetic modeling
KW - Mass-transfer
KW - NH-SCR
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U2 - 10.1016/j.cattod.2022.06.012
DO - 10.1016/j.cattod.2022.06.012
M3 - Article
AN - SCOPUS:85132923016
SN - 0920-5861
JO - Catalysis Today
JF - Catalysis Today
ER -