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Model for NOx storage/reduction in the presence of CO2 on a Pt–Ba/γ-Al2O3 catalyst
Affiliation:1. Universidad Autónoma de Nuevo León, UANL, Facultad de Ciencias Químicas, Av. Universidad S/N, San Nicolás de los Garza, Ciudad Universitaria, C.P. 66451 N.L, Mexico;2. Universidad Autónoma Metropolitana-Iztapalapa, Área de Ingeniería Química, A.P. 55-534, 09340 México, D.F., Mexico;2. Univ Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON, F-69626, Villeurbanne, France;1. Enhanced Oil Recovery (EOR) Research Center, School of Chemical and Petroleum Engineering, Shiraz University, Shiraz, Iran;2. Department of Chemical Engineering, School of Chemical and Petroleum Engineering, Curtin University, Kent Street, Bentley, WA, Australia;3. Department of Chemical and Petroleum Engineering, Sharif University of Technology, Tehran, Iran;1. Chemical Engineering Faculty, Sahand University of Technology, P.O.Box 51335-1996, Sahand New Town, Tabriz, Iran;2. Reactor and Catalysis Research Center (RCRC), Sahand University of Technology, P.O.Box 51335-1996, Sahand New Town, Tabriz, Iran;1. Key Lab of Applied Chemistry of Zhejiang Province, Department of Chemistry, Zhejiang University, Hangzhou, 310007, China;2. College of Biological, Chemical Sciences and Engineering, Jiaxing University, Jiaxing, 314001, China;3. School of Material, Sun Yat-Sen University, Guangdong, 510006, China;4. State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310007, China
Abstract:We have constructed a global reaction kinetic model to better understand and describe the NOx storage/reduction process in the presence of CO2. Experiments were performed in a packed-bed reactor with a Pt–Ba/γ-Al2O3 powder catalyst (1 wt% Pt and 30 wt% Ba) with different lean/rich cycle timings. The model is based on a multiple storage sites mechanism and considers that fast NOx storage occurs at surface barium sites, as determined by the reaction kinetics. Slow NOx storage occurs at the semi-bulk and bulk barium sites, where diffusion plays a major role. It is assumed that surface, bulk, and semi-bulk sites differ not only in physical appearance, but also in chemical reactivity. The distribution of these sites is obtained from 9-h lean-phase and 15-h rich-phase cycling experiments and thermogravimetric analysis of fresh catalyst. The model adequately describes the NO and NO2 breakthrough profiles during 9 h of lean exposure, as well as the subsequent release and reduction of the stored NOx. Furthermore, the model is also capable of simulating transient reactor experiments with 240-s lean-cycle and 60-s rich-cycle timings.
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