Abstract
In this study, NH3 adsorption isotherms for a commercial vanadium-based SCR catalyst coated on a monolith substrate were obtained using a gas flow reactor over a wide range of parameters which have not been performed before in a single study. The isotherms were obtained under different conditions, where adsorption temperature, NH3 concentration, water concentration, washcoat loading, and catalyst oxidation state were varied. For this purpose, a systematic data processing method was developed, which characterizes the dispersion and delay effects in the experimental setup using a residence time distribution model, and artifacts such as NH3 adsorbed in the experimental setup and uncertainties in the washcoat loading were removed. As a result, data from different catalyst samples were integrated, and adsorption isotherms with low data spread and well-defined regions were obtained. This allows the identification of the complex nature of the catalyst and dynamics, where multiple types of adsorption sites are present. For instance, the oxidized catalyst has 50% higher NH3 storage capacity compared to the reduced state of the sample. Moreover, water reduces the NH3 storage capacity at high concentrations (5.0%), whereas at low concentration (0.5%), water increases the NH3 adsorption capacity for an oxidized catalyst. The proposed data processing method can be extended for the analysis of further phenomena in catalysts studied using gas flow reactors, complementing current methods and providing information for models with extended validity and lower parameter correlations.
Highlights
The emission after-treatment system of an internal combustion engine plays an important role in reducing the environmental impact of the combustion technology.[1]
The present work aimed at characterizing the adsorption of NH3 on a vanadium-based selective catalytic reduction (SCR) catalyst over a wide range of conditions using the transient data obtained from a gas flow reactor
NH3 adsorption isotherms were obtained for a vanadium-based SCR catalyst coated on a monolith substrate over a wide experimental region, where variables such as temperature, NH3 concentration, water concentration, and catalyst oxidation state were analyzed
Summary
The emission after-treatment system of an internal combustion engine plays an important role in reducing the environmental impact of the combustion technology.[1]. The development of after-treatment systems that fulfill current and future environmental regulations requires detailed experimental data over a wide parameter range, which in consequence calls for the development and improvement of experimental and theoretical techniques for understanding the nature of a catalyst.[4,5] Among the main experimental setups used for catalyst studies, gas flow reactors provide the flexibility to emulate conditions relevant for industrial applications, at a small but geometrically and structurally similar scale.[6,7]
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