Abstract
A series of mixed oxides Ce1 − x Fe x O2 was prepared by a hydrothermal method. XRD and Raman spectra were measured to study the structure of the prepared materials. The temperature-programmed reduction was undertaken to estimate reducibility of the oxides. Syngas generation from methane using these materials as oxygen carriers/catalysts via a chemical-looping procedure was investigated in detail. This procedure includes catalytic oxidation and decomposition of methane to produce H2-rich gas at the first step followed by the production of the CO-rich gas by oxidizing the carbon deposited on deactivated catalysts. The results showed that all iron ions were incorporated into the ceria lattice with the formation of oxygen vacancies in the Ce0.9Fe0.1O2 sample, while isolated Fe2O3 particles were distributed on the surface of the Ce0.8Fe0.2O2 sample. TPR measurements and the analysis of the two-step chemical-looping reactions indicated a strong interaction between the Ce and Fe species which accounts for an increased activity of the mixed oxides in the syngas generation compared to that of individual oxides. Among the several samples, the Ce0.8Fe0.2O2 catalyst showed the highest activity for methane partial oxidation due to the synergetic effects caused by the interaction of surface iron entities and Ce-Fe solid solution. In addition, selective oxidation of carbon by oxygen to CO can also be found over this material since gaseous products are formed at the carbon oxidation step with the selectivity to CO reaching 91.2%. Evidence is presented that syngas can be feasibly produced from methane with high selectivity via the chemical-looping procedure over the CeO2-Fe2O3 mixed oxides.
Similar content being viewed by others
References
Otsuka, K., Wang, Y., Sunada, E., and Yamanaka, I., J. Catal., 1998, vol. 175, p. 152.
Greish, A.A., Glukhov, L.M., Finashina, E.D., Kustov, L.M., Sung, J.S., Choo, K.Y., and Kim, T.H., Mendeleev Commun., 2010, vol. 20, p. 28.
Fathi, M., Bjorgum, E., Viig, T., and Rokstad, O.A., Catal. Today, 2000, vol. 63, p. 489.
Li, K.Z., Wang, H., Wei, Y.G., and Liu, M.C., J. Chin. Rare Earth Soc., 2008, vol. 26, p. 129.
Li, K.Z., Wang, H., Wei, Y.G., and Yan, D.X., J. Phys. Chem. C, 2009, vol. 113, p. 15288.
Takenaka, S., Ogihara, H., and Otsuka, K., J. Catal., 2002, vol. 208, p. 54.
Takenaka, S., Tomikubo, Y., Kato, E., and Otsuka, K., Fuel, 2004, vol. 83, p. 47.
Zhang, T.J. and Amiridis, M.D., Appl. Catal., A, 1998, vol. 167, p. 161.
Aiello, R., Fiscus, J.E., zur Loye, H.C., and Amiridis, M.D., Appl. Catal., A, 2000, vol. 192, p. 227.
Otsuka, K., Takenaka, S., and Ohtsuki, H., Appl. Catal., A, 2004, vol. 273, p. 113.
Li, J. and Smith, K., Appl. Catal., A, 2008, vol. 349, p. 116.
Odier, E., Schuurman, Y., and Mirodatos, C., Catal. Today, 2007, vol. 127, p. 230.
Li, K.Z., Wang, H., Wei, Y.G., and Yan, D.X., Chem. Eng. J., 2010, vol. 156, p. 512.
Li, K.Z., Wang, H., Wei, Y.G., and Yan, D.X., Appl. Catal., B, 2010, vol. 97, p. 361.
Li, K.Z., Wang, H., Wei, Y.G., and Yan, D.X., Int. J. Hydrogen Energy, 2011, vol. 36, p. 3471.
Li, K.Z., Wang, H., Wei, Y.G., and Yan, D.X., Chem. Eng. J., 2011, vol. 173, p. 574.
Otsuka, K., Wang, Y., and Nakamura, M., Appl. Catal., A, 1999, vol. 183, p. 317.
Magnacca, G., Cerrato, G., Morterra, C., Signoretto, M., Somma, F., and Pinna, F., Chem. Mater., 2003, vol. 15, p. 675.
Laguna, O.H., Centeno, M.A., Boutonnet, M., and Odriozola, J.A., Appl. Catal., B, 2011, vol. 106, p. 621.
Hernandez, W.Y., Centeno, M.A., Romero-Sarria, F., and Odriozola, J.A., J. Phys. Chem. C, 2009, vol. 113, p. 5629.
Bao, H.Z., Chen, X., Fang, J., Jiang, Z.Q., and Huang, W.X., Catal. Lett., 2008, vol. 125, p. 160.
Ilieva, L., Pantaleo, G., Sobczakc, J.W., Ivanov, I., Venezia, A.M., and Andreeva, D., Appl. Catal., B, 2007, vol. 76, p. 107.
Li, G.S., Smith, R.L., and Inomata, H., J. Am. Chem. Soc., 2001, vol. 123, p. 11091.
Atribak, I., Bueno-Lopez, A., and Garcia-Garcia, A., J. Catal., 2008, vol. 259, p. 123.
Qiao, D.S., Lu, G.Z., Liu, X.H., Guo, Y., Wang, Y.Q., and Guo, Y.L., J. Mater. Sci., 2011, vol. 46, p. 3500.
Takenaka, S., Serizawa, M., and Otsuka, K., J. Catal., 2004, vol. 222, p. 520.
Kaspar, J., Fornasiero, P., and Graziani, M., Catal. Today, 1999, vol. 50, p. 285.
Millet, C.N., Menegazzi, P., Martin, B., and Colas, H., Oil Gas Sci. Technol. Rev., 2003, vol. 58, p. 151.
Hofstad, K.H., Hoebink, J.H.B.J., Holmen, A., and Marin, G.B., Catal. Today, 1998, vol. 40, p. 157.
Campbell, C.T. and Peden, C.H.F., Science, 2005, vol. 309, p. 713.
Author information
Authors and Affiliations
Corresponding author
Additional information
The article is published in the original.
Rights and permissions
About this article
Cite this article
Gu, Z., Li, K., Wang, H. et al. Syngas production from methane over CeO2-Fe2O3 mixed oxides using a chemical-looping method. Kinet Catal 54, 326–333 (2013). https://doi.org/10.1134/S002315841303004X
Received:
Published:
Issue Date:
DOI: https://doi.org/10.1134/S002315841303004X