Journal
CHEMICAL ENGINEERING JOURNAL
Volume 451, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.138865
Keywords
CH4 oxidation pathways; O2-dithering; Three-way catalyst; Pd; Operando XAS
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This study investigates the effects of O2 pulsing on the activity of Pd/Al2O3 catalyst through experiments and calculations, and reveals some regularities. It is necessary to accurately evaluate the concentration and conversion of NO in order to calculate the concentration of O2 in the reaction feed accurately.
Under periodic lean/rich operation generated by repeated O2 pulses (O2-dithering), the abatement of CH4 and NO is enhanced compared to static operation. However, it is not well understood how the dithering parameters (pulse amplitude and frequency) affect CH4 conversion, making it difficult to anticipate the impact of such pulses on the catalytic performance. Here, we show that the effect of O2-dithering on the activity of Pd/Al2O3 can be reliably assessed as a function of dithering parameters, temperature, and exhaust gas composition. Operando Xray absorption spectroscopy was used to support the conclusions based on considerations of the Pd oxidation state. Our work relies on explicit calculations of the O2 concentration present in the reactive feed, which is based on the amount of O2 pulsed to the system and the pollutants' conversion. Since NO contributes to the amount of oxygen available during reaction, its concentration and conversion need to be correctly evaluated.
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