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Open AccessArticle

An Aging Model of NH3 Storage Sites for Predicting Kinetics of NH3 Adsorption, Desorption and Oxidation over Hydrothermally Aged Cu-Chabazite

1
Department of Chemical and Biological Engineering, Koç University, Sarıyer, 34450 Istanbul, Turkey
2
Ford Otosan R&D Center, Sancaktepe, 34885 Istanbul, Turkey
*
Author to whom correspondence should be addressed.
Catalysts 2020, 10(4), 411; https://doi.org/10.3390/catal10040411
Received: 31 January 2020 / Revised: 14 February 2020 / Accepted: 16 February 2020 / Published: 8 April 2020
A unified transient kinetic model which can predict the adsorption, desorption and oxidation kinetics of NH3 over hydrothermally aged Cu-chabazite was developed. The model takes into account the variation of fractional coverages of NH3 storage sites due to hydrothermal aging. In order to determine the fractional coverage of these sites, the catalyst was aged for various times at a certain temperature followed by NH3 adsorption, desorption and temperature-programmed desorption (TPD) experiments. TPD profiles were deconvoluted mainly into three peaks with centres at 317, 456 and 526 °C, respectively. Hydrothermal aging resulted in the progressive increase in the intensity of the peak at 317 °C and decrease in the intensity of the peaks at 456 and 526 °C, along with decreased NH3 oxidation at high temperatures. A model for hydrothermal aging kinetics of the fractional coverage of storage sites was developed using three reactions with appropriate rate expressions with parameters regressed from experimental data. The model was then incorporated into a multi-site kinetic model for the degreened Cu-Chabazite by the addition of aging reactions on each storage site. The effects of both aging time and temperature on the kinetics NH3 adsorption, desorption and oxidation were successfully predicted in the 155-540 °C range. This study is the first step towards the development of a hydrothermal aging-unified kinetic model of NH3-Selective Catalytic Reduction over Cu-chabazite. View Full-Text
Keywords: kinetic model; hydrothermal aging; NH3-TPD; Cu-Chabazite; Cu-SSZ-13; adsorption; desorption; oxidation; NH3-SCR kinetic model; hydrothermal aging; NH3-TPD; Cu-Chabazite; Cu-SSZ-13; adsorption; desorption; oxidation; NH3-SCR
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MDPI and ACS Style

Bozbag, S.E.; Şanlı, D.; Özener, B.; Hisar, G.; Erkey, C. An Aging Model of NH3 Storage Sites for Predicting Kinetics of NH3 Adsorption, Desorption and Oxidation over Hydrothermally Aged Cu-Chabazite. Catalysts 2020, 10, 411.

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