Abstract
Nickel-calcium phosphate/hydroxyapatite catalysts have recently been reported to exhibit high activity and selectivity in partial oxidation of methane (POM). In this work the optimum composition was determined. The optimum mole ratio of Ca/PO4 was around 10/6 and that of Ni/PO4 was in a range from 1.0/6 to 3.0/6 with the optimum Ca/PO4, and the activity could be related with the amount of metallic nickel. In a temperature range from ca. 400 to 700 K, an apparent autothermal reaction was observed to occur in some cases. This is due to the fact that the actual catalyst temperature is higher than the measured temperature, which comes from the exothermic nature of the reaction. The mixing sequence of the precursors during the catalyst preparation does little affect the catalyst activity and characteristics. Deactivation of the catalyst occurred slowly, but the catalyst could easily be regenerated. Moreover, the nickel-calcium phosphate/hydroxyapatite catalyst showed higher activity than the nickel-strontium phosphate catalyst.
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Au, C. T. and Wang, H.Y., “Mechanistic Studies of Methane Partial Oxidation to Syngas over SiO2-supported Rhodium Catalysts,”J. Catal.,167, 337 (1997).
Chen, Y., Hu, C., Gong, M., Chen, Y. and Tian, A., “Partial Oxidation and Chemisorption of Methane over Ni/Al2O3 Catalysts,”Stud. Surf. Sci. Catal.,130, 2543 (2000).
Choudhary, V. R., Uphade, B. S. and Mamman, A. S., “Oxidative Conversion of Methane to Syngas over Nickel Supported on Commercial Low Surface Area Porous Catalyst Precoated with Alkaline and Rare Earth Oxides,”J. Catal.,172, 281 (1997).
Diskin, A. M. and Ormerod, R.M., “Partial Oxidation of Methane over Supported Nickel Catalysts,”Stud. Surf. Sci. Catal.,130, 3519 (2000).
Dissanayake, D., Rosynek, M. P., Kharas, K. C. C. and Lunsford, J. H., “Partial Oxidation of Methane to Carbon Monoxide and Hydrogen over a Ni/Al2O3 Catalyst,”J. Catal.,132, 117 (1991).
Dissanayake, D., Rosynek, M. P. and Lunsford, J. H., “Are the Equilibrium Concentrations of CO and H2 Exceeded during the Oxidation of CH4 over a Ni/Yb2O3 Catalyst?”J. Phys. Chem.,97, 3644 (1993).
Hayakawa, T., Harihara, H., Anderson, A.G., Suzuki, K., Yasuda, H., Tsunoda, T., Hamakawa, S., York, A. P. E., Yoon, Y. S., Shimizu, M. and Takehira, K., “ Sustainable Ni/Ca1-xSrxTiO3 Catalyst Prepared in Situ for the Partial Oxidation of Methane to Synthesis Gas,”Appl. Catal. A,149, 391 (1997).
Hydrocarbon Processing, “Gas Processes 2002,” 103 (May, 2002).
Jun, J.H., Lee, S. J., Lee, S.-H., Lee, T.-J., Kong, S. J., Lim, T.H., Nam, S.-W., Hong, S.-A. and Yoon, K. J., “Characterization of a Nickel-Strontium Phosphate Catalyst for Partial Oxidation of Methane,”Korean J. Chem. Eng., 20(5), 829 (2003).
Jun, J.H., Lee, T.-J., Lim, T.H., Nam, S.-W., Hong, S.-A. and Yoon, K. J., “Nickel-Calcium Phosphate/Hydroxyapatite Catalysts for Partial Oxidation of Methane to Syngas: Characterization and Activation,”J. Catal, 221(1), 178 (2004).
Lee, S.-H. and Yoon, K. J., “Oxidative Coupling of Methane over Transition-Metal-Substituted Strontium Hydroxyapatite,”Korean J. Chem. Eng.,18, 228 (2001).
Lee, S. J., Jun, J.H., Lee, S.-H., Yoon, K. J., Lim, T.H., Nam, S.-W. and Hong, S.-A., “Partial Oxidation of Methane over Nickel-Added Strontium Phosphate,”Appl. Catal. A,230, 61 (2002).
Liu, S., Xiong, G., Dong, H., Yang, W., Sheng, S., Chu, W. and Yu, Z., “Sustainable Ni Catalyst for Partial Oxidation of CH4 to Syngas at High Temperature,”Stud. Surf. Sci. Catal.,130, 3567 (2000).
Liu, Z. -W., Jun, K. -W., Roh, H. -S., Park, S. -E. and Oh, Y. -S., “ Partial Oxidation of Methane over Nickel Catalysts Supported on Various Aluminas, ”Korean J. Chem. Eng.,19, 735 (2002a).
Liu, Z. -W., Roh, H. -S., Jun, K. -W., Park, S. -E. and Song, T. -Y., “ Partial Oxidation of Methane over Ni/Ce-ZrO2/ θ-Al2O3, ”Korean J. Chem. Eng.,19, 742 (2002b).
Takehira, K., Shishido, T., Kondo, M., Furukawa, R., Tanabe, E., Ito, K., Hamakawa, S. and Hayakawa, T., “Partial Oxidation of CH4 into Synthesis Gas on Ni/Perovskite Catalysts Prepared SPC Method,”Stud. Surf. Sci. Catal.,130, 3525 (2000).
Takehira, K., “ Highly Dispersed and Stable Supported Metal Catalysts Prepared by Solid Phase Crystallization Method,”Catal. Surv. Jpn.,6, 19 (2002).
Torniainen, P. M., Chu, X. and Schmidt, L.D., “Comparison of Monolith-Supported Metals for the Direct Oxidation of Methane to Syngas,”J. Catal.,146, 1 (1994).
van Looij, F., Geus, J.W., “Nature of Active Phase of a Nickel Catalyst during the Partial Oxidation of Methane to Synthesis Gas,”J. Catal.,168, 154 (1997).
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This paper is dedicated to Professor Hyun-Ku Rhee on the occasion of his retirement from Seoul National University.
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Jun, J.H., Jeong, K.S., Lee, TJ. et al. Nickel-calcium phosphate/hydroxyapatite catalysts for partial oxidation of methane to syngas: Effect of composition. Korean J. Chem. Eng. 21, 140–146 (2004). https://doi.org/10.1007/BF02705392
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DOI: https://doi.org/10.1007/BF02705392