Abstract
Perovskite-related mixed-oxides based on La Ni Nb and La Sr Ni Nb were synthesized by the auto combustion method to use as precursors materials for the catalytic reforming of methane at 700 ºC, atmospheric pressure, CH4:CO2 = 1:1. LaNiO3 and LaNbO4 were used as reference. XRD analysis show that the synthesis method produce a new series of precursor family formed by a mixture of oxides where Ni crystallized as part of a perovskite and Ruddlesden–Popper structure while Nb formed lanthanum orthoniobate LaNbO4, a scheelite-type structure alternating with oxide layers, with phase distribution depending on niobium content. For Nb (x ≤ 0.3) Ni crystallizes as LaNiO3 perovskite-type oxide while for Nb (x ≥ 0.7) it forms mainly the orthoniobate phase LaNbO4 a scheelite-type structure. At higher calcined temperatures (~1100 °C) La2Ni0.8Nb0.2O4 was formed with a Ruddlesden–Popper structure consisting of three perovskite type layers along the c-axis alternating with a layer of the rock salt type phase. TEM analysis showed the presence of cubic particles with sizes varying between 5 and 60 nm depending on the extent of substitution of Ni by Nb. Reduction of the perovskite-related precursor oxides produced a series of Ni0/La2O3–NbOx oxides with high metallic dispersion which favors the activity and stability of the catalysts. Introduction of doping quantities of Sr into LaNi0.8Nb0.2O3±λ structure produced a mixture of oxides with Sr dissolved in the lanthanum orthoniobate LaNbO4 scheelite-type structure due to the similarity of ionic radii of La and Sr. Under the reaction conditions conversions near the thermodynamic equilibrium were attained which remains for long periods of time assessing the stability of the synthesized catalysts.
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References
Somorjai GA, McCrea K (2001) Appl Catal A Gen 222:3–18
Lira E, Lopez CM, Oropeza F, Bartolini M, Alvarez J, Goldwasser MR, Lopez Linares F, Lamonier Jean-François, Josefina Perez Zurita M (2008) J Mol Catal A Chem 281:146–153
Nagaoka K, Jentys A, Lercher JA (2005) J Catal 229:185–196
Basini L (2005) Catal Today 106:34–40
Rivas ME, Fierro JLG, Guil-López R, Peña MA, La Parola V, Goldwasser MR (2008) Catal Today 133–135:367–373
Rivas ME, Fierro JLG, Goldwasser MR, Pietri E, Perez Zurita MJ, Griboval-Constant A, Leclercq G (2008) Appl Catal A Gen 344:10–19
Hori C, Rivas ME, Fierro JLG, Goldwasser MR, Griboval A (2008) J Power Source 184:265–275
Erdohelyi A, Fodor K, Szailer T (2004) Appl Catal B Environ 53:153–160
Goldwasser MR, Rivas ME, Pietri E, Pérez Zurita MJ, Cubeiro ML, Griboval-Constant A, Leclercq G (2005) J Mol Catal A Chem 228:325–331
Goldwasser MR, Dorantes V, Pérez-Zurita MJ, Sojo PR, Cubeiro ML, Pietri E, González-Jiménez F, Lee Ng, Moronta D (2003) J Mol Catal A Chem 193:227–236
Martinez R, Romero E, Guimon C, Bilbao R (2004) Appl Catal A Gen 274:139–149
Batiot-Dupeyrat C, Valderrama G, Meneses A, Martínez F, Barrault J, Tatibouët JM (2003) Appl Catal A Gen 248:143–151
Goldwasser MR, Rivas ME, Pietri E, Pérez Zurita MJ, Cubeiro ML, Griboval-Constant A, Leclercq L, Leclercq G (2003) Appl Catal A Gen 225:45–57
Pereira MM, Pereira EB, Lam YL, dos Santos T, Schmal M (2000) Stud Surf Sci Catal 130:2339–2344
Tanabe K (2003) Catal Today 78:65–77
Parlinski K, Hashi Y, Tsunekawa S, Kawazoe Y (1997) J Mater Res 12(9):2428–2437
Amow G, Davidson IJ, Skinner SJ (2006) Solid State Ionics 177:1205–1210
Valderrama G, Goldwasser MR, de Navarro C Urbina, Tatibouët JM, Barrault J, Batiot-Dupeyrat C, Martinez F (2005) Catal Today 107–108:785–791
Valderrama G, Kiennemann A, Goldwasser MR (2010) J Power Sources 195:1765–1771
Goldwasser MR, Rivas ME, Lugo ML, Pietri E, Pérez-Zurita J, Cubeiro ML, Griboval-Constant A, Leclercq G (2005) Catal Today 107–108:106–113
Rivas I, Álvarez J, Pietri E, Pérez Zurita MJ, Goldwasser MR (2010) Catal Today 149(3–4):388–393
Sleight AW (1977) In: Burton JJ, Garten RL (eds) Advanced materials in catalysis. Academic Press, San Diego, p 181
Maschio S, Bachiorrini A, Di Monte R, Montanaro L (1995) J Mater Sci 30:5433–5437
Weng X, Boldrin P, Abrahams I, Skinner SJ, Kellici S, Wenga Xiaole, Darr JA (2008) J Solid State Chem 181:1123–2123
Mogni L, Prado F, Ascolani H, Abbate M, Moreno M, Manthiram A, Caneiro A (2005) J Solid State Chem 178:1559–1568
Xiancai Li, Min Wu, Zhihua Lai, Fei He (2005) Appl Catal A Gen 290:81–86
Acknowledgements
The authors thank Brazilian Metallurgy and Mineral Company CBMM, Araxá, MG-Brazil, for the Niobium samples supplied and the Council of Scientific and Humanistic Development of Venezuelan Central University (UCV-CDCH) and the Draft Law on Science and Technology (LOCTI), through projects PG-03-00-6504-2006 and LOCTI-2008-2009 respectively, for financial support.
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Alvarez, J., Valderrama, G., Pietri, E. et al. Ni–Nb-Based Mixed Oxides Precursors for the Dry Reforming of Methane. Top Catal 54, 170–178 (2011). https://doi.org/10.1007/s11244-011-9636-7
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DOI: https://doi.org/10.1007/s11244-011-9636-7