Passive NOx adsorption on Pd/H-ZSM-5: Experiments and modeling

[Display omitted] •NO and NO2 uptake and release on Pd/H-ZSM-5 conducted.•Passive NOx adsorption Pd/H-ZSM-5 model developed.•Two Pd redox microkinetic schemes tuned and validated.•Model predicts multiple NO sorption sites and NO2 generation.•Model captures subtle trends for range of operating condit...

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Bibliographic Details
Published in:Applied catalysis. B, Environmental Environmental, 2020-07, Vol.269 (C), p.118802, Article 118802
Main Authors: Ambast, Mugdha, Karinshak, Kyle, Rahman, Bhuiyan Md. Mushfikur, Grabow, Lars C., Harold, Michael P.
Format: Article
Language:English
Subjects:
Binding sites
Density functional theory
Emission control
ENGINEERING
Infrared spectroscopy
Material properties
Mathematical models
Microkinetics
Modelling
Nitrogen dioxide
Parameters
Passive NOx adsorption
ZSM-5
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Summary:[Display omitted] •NO and NO2 uptake and release on Pd/H-ZSM-5 conducted.•Passive NOx adsorption Pd/H-ZSM-5 model developed.•Two Pd redox microkinetic schemes tuned and validated.•Model predicts multiple NO sorption sites and NO2 generation.•Model captures subtle trends for range of operating conditions and Pd loadings. A combined experimental and modeling study of the passive NOx adsorber (PNA) is presented that advances the understanding and prediction of the effects of various operating parameters and material properties of H-ZSM-5 and Pd/H-ZSM-5. Experiments reveal the NOx uptake process to be kinetically limited. Two microkinetic schemes are developed to explain the NOx uptake and release and NO2 generation data. Both schemes are incorporated into a 1 + 1 D monolith model to predict and validate NOx uptake and temperature programmed desorption (TPD) data. Scheme I involves Z-[PdOH]+, Z-Pd2+Z-and Z-Pd+ with Z-Pd+ as the strongest NO binding site. Scheme II involves reduction of PdO2 to PdO and nitrate formation. Model tuning utilizes a combination of infrared spectroscopy measurements and density functional theory (DFT) estimates of energy barriers. The model is validated at different conditions including feed parameters and Pd loading.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2020.118802