On the Structure-Activity Relationship for NO-SCR with NH3 Catalyzed by Cu-exchanged Natural Chabazite and SSZ-13
DOI:
https://doi.org/10.29356/jmcs.v65i1.1267Keywords:
Selective catalytic reduction of NO, Cu-CHA, natural chabazite, SSZ-13, UV-VisAbstract
Abstract. In spite of their similar structures, the catalytic properties of natural and synthetic (SSZ-13) Chabazite during the selective reduction of NO with NH3 have a different dependence on the Cu exchange level when tested under conditions equivalent to those found in Diesel vehicles. At low (1-2 wt.%) and high copper loadings (6-14 wt.%), their activities differ, because there are variations in the different species of Cu (Cu+, Cu2+, Cu-O-Cu) detected by UV-Vis. At intermediate Cu loadings (2-3 wt.%) they have similar high activities, reaching 100 % conversion. High deNOx activity per Cu site appears to correlate with the predominance of charge compensation Cu2+ species over CuOx moieties. There are changes in the distribution of Cu moieties during operation of both catalysts, evidenced by DR-UV-Vis.
Resumen. A pesar de sus estructuras similares, las propiedades catalíticas de Chabazita natural y sintética (SSZ-13) durante la reducción selectiva de NO con NH3 dependen de manera diferente frente al nivel de intercambio con Cu cuando se prueban bajo condiciones equivalentes a las de vehículos Diesel. A bajos (1-2 % p/p) y altos contenidos de Cu (6-14 % p/p) la reducción de NO es diferente debido a variaciones en las distintas especies de Cu (Cu+, Cu2+, Cu-O-Cu) observadas por UV-Vis. Por su parte, los catalizadores intercambiados con 2-3 % p/p de Cu tuvieron alta actividad por sitio de Cu, alcanzando 100 % de conversión de NO, lo que parece deberse a la predominancia de especies de Cu2+ sobre especies CuOx de acuerdo con el análisis por DR-UV-Vis, el que también muestra la existencia de variaciones en la distribución de especies de Cu debido a la reacción.
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References
Qi, G.; Yang, R. T.; Chang, R. App. Catal., B 2004, 51, 93–106.
Si, Z.; Weng, D.; Wu, X.; Li, J.; Li, G. J. Catal. 2010, 271, 43–51.
Sjövall, H.; Blint, R.J.; Olsson, L. App. Catal., B 2009, 92, 138–153.
Kwak, J.H.; Tran, D.; Szanyi, J.; Peden, C.H.F.; Lee, J.H. Catal. Lett. 2012, 142, 295–301.
Fickel, D.W.; D’Addio, E.; Lauterbach, J.A.; Lobo, R.F. App. Catal., B 2011, 102, 441–448.
Stacey I. Zones, U S Patent 1985, 4, 544, 538.
Komatsu, T.; Nunokawa, M.; Moon, I.S.; Takahara, T.; Namba, S.; Yashima, T. J. Catal. 1994, 148, 427–437.
Kieger, S.; Delahay, G.; Coq, B. App. Catal., B 2000, 25, 1–9.
Kefirov, R.; Penkova, A.; Hadjiivanov, K.; Dzwigaj, S.; Che, M. Microporous Mesoporous Mater. 2008, 116, 180–187.
Bull, I.; Xue, W.M.; Burk, P.; Boorse, R.S.; Jaglowski, W.M.; Koermer, G.S.; Moini, A.; Patchett, J.A.; Dettling, J.C.; Caudle, M.T.; Llc, B.C. Patent 2008, US 7,601,662 B2, BASF Catalysts LLC.
Kwak, J.H.; Tonkyn, R.G.; Kim, D.H.; Szanyi, J.; Peden, C.H.F. J. Catal. 2010, 275, 187–190.
Pham, T.D.; Liu, Q.; Lobo, R.F. Langmuir 2013, 29, 832–839.
Anunziata, O.A.; Beltramone, A.R.; Juric, Z.; Pierella, L.B.; Requejo, F.G. App. Catal., A 2004, 264, 93–101.
Gelves, J.F.; Dorkis, L.; Márquez, M.A.; Álvarez, A.C.; González, L.M.; Villa, A.L. Catal. Today 2019, 320, 112–122.
Martín, N.; Paris, C.; Vennestrøm, P.N.R.; Thøgersen, J.R.; Moliner, M.; Corma, A. App. Catal., B 2017, 217, 125–136.
Thommes, T.; Kaneko, K.; Neimark, A.V.; Olivier, J.P.; Rodriguez-Reinoso, F.; Rouquerol, J.; Sing, K.S.W. Pure App. Chem. 2015, 87, 1051–1069.
Negri, C.; Signorile, M.; Porcaro, N.G.; Borfecchia, E.; Berlier, G.; Janssens, T.V.W.; Bordiga, S. App. Catal., A 2019, 578, 1–9.
Ipek, B.; Wulfers, M.J.; Kim, H.; Göltl, F.; Hermans, I.; Smith, J.P.; Booksh, K.S.; Brown, C.M.; Lobo, R.F.; ACS Catal. 2017, 7, 4291–4303.
Gang, L.; van Grondelle, J.; Anderson, B.G.; van Santen, R.A. J. Catal. 1999, 186, 100–109.
Pestryakov, A.N.; Petranovskii, V.P.; Kryazhov, A.; Ozhereliev, O.; Pfänder, N.; Knop-Gericke, A. Chem. Phys. Lett. 2004, 385, 173–176.
Gao, F.; Walter, E.D.; Washton, N.M.; Szanyi, J.; Peden, C.H.F. App. Catal., B 2015, 162, 501–514.
Wang, L.; Gaudet, J.R.; Li, W.; Weng, D. J. Catal. 2013, 306, 68–77.
Giordanino, F.; Vennestrøm, P.N.R.; Lundegaard, L.F.; Stappen, F.N.; Mossin, S.; Beato, P.; Bordiga, S.; Lamberti, C. Dalton Trans. 2013, 42, 12741–12761.
Wang, D.; Zhang, L.; Li, J.; Kamasamudram, K.; Epling, W.S. Catal.Today 2014, 231, 64–74.
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