Thermal durability of Cu-CHA NH3-SCR catalysts for diesel NOx reduction

• Published in: Catalysis today 2012-04, Vol.184 (1), p.252-261
• Main Authors: Schmieg, Steven J., Oh, Se H., Kim, Chang H., Brown, David B., Lee, Jong H., Peden, Charles H.F., Kim, Do Heui
• Format: Article
• Language: English
• Subjects: AGGLOMERATION; AGING; CAPACITY; CATALYSTS; catalytic activity; Cu-chabazite; Deactivation; durability; Environmental Molecular Sciences Laboratory; INDUCTION; INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; Laboratory aging; NH3-SCR; NITROGEN OXIDES; NUCLEAR MAGNETIC RESONANCE; nuclear magnetic resonance spectroscopy; OXIDATION; prediction; Selective catalytic reduction; SPECTROSCOPY; STORAGE; temperature; TRANSMISSION ELECTRON MICROSCOPY; Vehicle aging; X-radiation; X-RAY DIFFRACTION; ZEOLITES
• ISSN: 0920-5861; 1873-4308
• DOI: 10.1016/j.cattod.2011.10.034

[Display omitted] ► Commercial Cu-CHA catalysts were aged both in the laboratory and the vehicle. ► Reactor-aged catalyst deactivates due to Cu agglomeration and destruction of zeolite structure. ► Vehicle-aged catalyst poisoned by S, Ca, Zn and Pt decreases DeNOx activity. ► Vehicle-aged Cu-CHA SCR catalyst showed equivalent NOx conversion to 800°C 16h reactor-aged Cu-CHA. Multiple catalytic functions (NOx conversion, NO and NH3 oxidation, NH3 storage) of a commercial Cu-chabazite (CHA) urea/NH3-SCR catalyst were assessed in a laboratory fixed-bed flow reactor system after differing degrees of hydrothermal aging. Catalysts were characterized by using X-ray diffraction (XRD), 27Al solid state nuclear magnetic resonance (NMR) and transmission electron microscopy (TEM)/energy dispersive X-ray (EDX) spectroscopy to develop an understanding of degradation mechanisms during catalyst aging. The catalytic reaction measurements of laboratory-aged catalysts were performed, which allows us to obtain a universal curve for predicting the degree of catalyst performance deterioration as a function of time at each aging temperature. Results show that as the aging temperature becomes higher, the zeolite structure collapses in a shorter period of time after an induction period. The decrease in SCR performance was explained by zeolite structure destruction and/or Cu agglomeration, as detected by XRD/27Al NMR and by TEM/EDX, respectively. Destruction of the zeolite structure and agglomeration of the active phase also results in a decrease in NO/NH3 oxidation activity and NH3 storage capacity of the catalyst. Laboratory aging conditions (16h at 800°C) compare well with a 135,000mile vehicle-aged catalyst, except for the chemically poisoned inlet section of the vehicle-aged catalyst.