Abstract
Catalysts with highly dispersed palladium on alumina, alumina doped with 20 wt% ceria and ceria have been prepared, characterized and examined for net-lean methane oxidation. In particular, the activity and selectivity were investigated during rich/lean cycling of the feed. The ceria content is found to influence both the general and the instantaneous activity responses. The results indicate that the active phase of palladium changes between reduced and oxidised Pd during the rich/lean cycling, and that the process is influenced by the presence of ceria.
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References
Ciuparu D, Lyubovsky MR, Altman E, Pfefferle LD, Datye A (2002) Catalytic combustion of methane over palladium-based catalysts. Catal Rev 44(4):593–649. doi:10.1081/cr-120015482
Carstens JN, Su SC, Bell AT (1998) Factors affecting the catalytic activity of Pd/ZrO2 for the combustion of methane. J Catal 176(1):136–142
Carlsson P-A, Fridell E, Skoglundh M (2007) Metahne oxidation over Pt/Al2O3 and Pd/Al2O3 catalysts under transient conditions. Catal Lett 115(1):1–7. doi:10.1007/s10562-007-9057-1
Trovarelli A, de Leitenburg C, Boaro M, Dolcetti G (1999) The utilization of ceria in industrial catalysis. Catal Today 50(2):353–367
Haneda M, Mizushima T, Kakuta N (1998) Synergistic effect between Pd and nonstoichiometric cerium oxide for oxygen activation in methane oxidation. J Phys Chem B 102(34):6579–6587. doi:10.1021/jp9819285
Becker E, Carlsson P-A, Skoglundh M (2009) Methane oxidation over alumina and ceria supported platinum. Top Catal 52(13):1957–1961. doi:10.1007/s11244-009-9379-x
Dawody J, Eurenius L, Abdulhamid H, Skoglundh M, Olsson E, Fridell E (2005) Platinum dispersion measurements for Pt/BaO/Al2O3, NOx storage catalysts. Appl Catal A 296(2):157–168
Lundgren S, Keck KE, Kasemo B (1994) A flow reactor system for catalytic reaction studies, allowing time- and space-resolved measurements of gas composition and temperature around the catalyst. Rev Sci Instrum 65(8):2696–2703
Wang-Hansen C, Kamp CJ, Skoglundh M, Andersson B, Carlsson P-A (2011) Experimental method for kinetic studies of gas–solid reactions: oxidation of carbonaceous matter. J Phys Chem C 115(32):16098–16108. doi:10.1021/jp204539g
Faria WLS, Perez CAC, Cesar DV, LdC Dieguez, Schmal M (2009) In situ characterizations of Pd/Al2O3 and Pd/CeO2/Al2O3 catalysts for oxidative steam reforming of propane. Appl Catal B 92(1–2):217–224
Ramírez-López R, Elizalde-Martinez I, Balderas-Tapia L (2010) Complete catalytic oxidation of methane over Pd/CeO2-Al2O3: the influence of different ceria loading. Catal Today 150(3–4):358–362
Santos ACSF, Damyanova S, Teixeira GNR, Mattos LV, Noronha FB, Passos FB, Bueno JMC (2005) The effect of ceria content on the performance of Pt/CeO2/Al2O3 catalysts in the partial oxidation of methane. Appl Catal A 290(1–2):123–132
Anderson JRPK, Pratt KC (1985) Introduction to characterization and testing of catalysts. Academic Press, Orlando
Kašpar J, Fornasiero P, Graziani M (1999) Use of CeO2-based oxides in the three-way catalysis. Catal Today 50(2):285–298
Barbier J Jr, Duprez D (1994) Steam effects in three-way catalysis. Appl Catal B 4(2–3):105–140
Matam SK, Aguirre MH, Weidenkaff A, Ferri D (2010) Revisiting the problem of active sites for methane combustion on Pd/Al2O3 by operando XANES in a lab-scale fixed-bed reactor. J Phys Chem C 114(20):9439–9443. doi:10.1021/jp1019697
Santhosh Kumar M, Eyssler A, Hug P, van Vegten N, Baiker A, Weidenkaff A, Ferri D (2010) Elucidation of structure, activity relationships of model three way catalysts for the combustion of methane. Appl Catal B 94(1–2):77–84
Hicks RF, Qi H, Young ML, Lee RG (1990) Structure sensitivity of methane oxidation over platinum and palladium. J Catal 122(2):280–294
K-i Fujimoto, Ribeiro FH, Avalos-Borja M, Iglesia E (1998) Structure and reactivity of PdOx/ZrO2 catalysts for methane oxidation at low temperatures. J Catal 179(2):431–442
Su SC, Carstens JN, Bell AT (1998) A study of the dynamics of Pd oxidation and PdO reduction by H2 and CH4. J Catal 176(1):125–135
Burch R, Urbano FJ (1995) Investigation of the active state of supported palladium catalysts in the combustion of methane. Appl Catal A 124(1):121–138
Choudhary TV, Banerjee S, Choudhary VR (2005) Influence of PdO content and pathway of its formation on methane combustion activity. Catal Commun 6(2):97–100
Hellman A, Resta A, Martin NM, Gustafson J, Trinchero A, Carlsson PA, Balmes O, Felici R, van Rijn R, Frenken JWM, Andersen JN, Lundgren E, Grönbeck H (2012) The active phase of palladium during methane oxidation. J Phys Chem Lett 3(6):678–682. doi:10.1021/jz300069s
Kinnunen NM, Hirvi JT, Suvanto M, Pakkanen TA (2011) Role of the interface between Pd and PdO in methane dissociation. J Phys Chem C 115(39):19197–19202. doi:10.1021/jp204360c
Kinnunen NM, Hirvi JT, Venalainen T, Suvanto M, Pakkanen TA (2011) Procedure to tailor activity of methane combustion catalyst: relation between Pd/PdOx active sites and methane oxidation activity. Appl Catal A Gen 397(1–2):54–61
Thevenin PO, Pocoroba E, Pettersson LJ, Karhu H, Väyrynen IJ, Järås SG (2002) Characterization and activity of supported palladium combustion catalysts. J Catal 207(1):139–149
Yazawa Y, Yoshida H, Takagi N, S-i Komai, Satsuma A, Hattori T (1998) Oxidation state of palladium as a factor controlling catalytic activity of Pd/SiO2–Al2O3 in propane combustion. Appl Catal B 19(3–4):261–266
Schwartz WR, Pfefferle LD (2012) Combustion of methane over palladium-based catalysts: support interactions. J Phys Chem C 116(15):8571–8578. doi:10.1021/jp2119668
Ciuparu D, Bozon-Verduraz F, Pfefferle L (2002) Oxygen exchange between palladium and oxide supports in combustion catalysts. J Phys Chem B 106(13):3434–3442. doi:10.1021/jp013577r
Burch R, Urbano FJ, Loader PK (1995) Methane combustion over palladium catalysts: the effect of carbon dioxide and water on activity. Appl Catal A 123(1):173–184
Card RJ, Schmitt JL, Simpson JM (1983) Palladium-carbon hydrogenolysis catalysts: the effect of preparation variables on catalytic activity. J Catal 79(1):13–20
Cullis CF, Nevell TG, Trimm DL (1972) Role of the catalyst support in the oxidation of methane over palladium. J Chem Soc Faraday Trans 1 Phys Chem Condens Phases 68:1406–1412
Ciuparu D, Pfefferle L (2001) Support and water effects on palladium based methane combustion catalysts. Appl Catal A 209(1–2):415–428
Carlsson P-A, Skoglundh M (2011) Low-temperature oxidation of carbon monoxide and methane over alumina and ceria supported platinum catalysts. Appl Catal B 101(3–4):669–675
Acknowledgments
This study has been performed at the Competence Centre for Catalysis, which is hosted by Chalmers University of Technology and financially supported by the Swedish Energy Agency and the member companies AB Volvo, Volvo Car Corporation, Scania CV AB, Haldor Topsøe A/S, and ECAPS AB. The authors acknowledge support by the DAAD (Deutscher Akademischer Austauschdienst) and by the COST Action CM1104. J.L. and St.S. acknowledge additional financial support by the Deutsche Forschungsgemeinschaft, including the Excellence Cluster “Engineering of Advanced Materials” in the framework of the excellence initiative. St.S. gratefully acknowledges a PhD grant of the “Fonds der Chemischen Industrie”.
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Fouladvand, S., Schernich, S., Libuda, J. et al. Methane Oxidation Over Pd Supported on Ceria–Alumina Under Rich/Lean Cycling Conditions. Top Catal 56, 410–415 (2013). https://doi.org/10.1007/s11244-013-9988-2
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DOI: https://doi.org/10.1007/s11244-013-9988-2