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Effects of Ce-promoted Nickel Catalysts and O2-enhanced on Dry Reforming of Methane
|關鍵字:||合成氣;甲烷乾重組;積碳;氧化鈰改性觸媒;氧氣添加;dry Syngas;Dry reforming of methane (DRM);Carbon deposition;CeO2-modified catalyst;O2 addition||引用:|| 溫室氣體排放統計，行政院環境保護署，2017。  我國2015年燃料燃燒二氧化碳排放統計與分析，經濟部能源局，2017。  S. Aghamohammadi, M. Haghighi, M. Maleki, and N. Rahemi, Sequential impregnation vs. sol-gel synthesized Ni/Al2O3-CeO2 nanocatalyst for dry reforming of methane： Effect of synthesis method and support promotion, Molecular Catalysis, vol. 431, pp. 39-48, 2017.  C. E. Daza, A. Kiennemann, S. Moreno, and R. Molina, Dry reforming of methane using Ni–Ce catalysts supported on a modified mineral clay, Applied Catalysis A： General, vol. 364, pp. 65-74, 2009.  W. Chen, G. Zhao, Q. Xue, L. Chen, and Y. Lu, High carbon-resistance Ni/CeAlO3-Al2O3 catalyst for CH4/CO2 reforming, Applied Catalysis B： Environmental, vol. 136-137, pp. 260-268, 2013.  S. Khajeh Talkhoncheh, M. Haghighi, N. Jodeiri, and S. Aghamohammadi, Hydrogen production over ternary supported Ni/Al2O3-clinoptilolite-CeO2 nanocatalyst via CH4/CO2 reforming： Influence of support composition, Journal of Natural Gas Science and Engineering, vol. 46, pp. 699-709, 2017.  I. Luisetto, S. Tuti, C. Battocchio, S. Lo Mastro, and A. Sodo, 'Ni/CeO2–Al2O3 catalysts for the dry reforming of methane： The effect of CeAlO3 content and nickel crystallite size on catalytic activity and coke resistance, Applied Catalysis A： General, vol. 500, pp. 12-22, 2015.  S. K. Chawl, M. George, F. Patel, and S. Patel, Production of Synthesis Gas by Carbon Dioxide Reforming of Methane over Nickel based and Perovskite Catalysts, Procedia Engineering, vol. 51, pp. 461-466, 2013.  S. J. Hassani Rad, M. Haghighi, A. Alizadeh Eslami, F. Rahmani, and N. Rahemi, Sol–gel vs. impregnation preparation of MgO and CeO2 doped Ni/Al2O3 nanocatalysts used in dry reforming of methane： Effect of process conditions, synthesis method and support composition, International Journal of Hydrogen Energy, vol. 41, pp. 5335-5350, 2016.  S. Damyanova, B. Pawelec, R. Palcheva, Y. Karakirova, M. C. C. Sanchez, G. Tyuliev, et al., Structure and surface properties of ceria-modified Ni-based catalysts for hydrogen production, Applied Catalysis B： Environmental, vol. 225, pp. 340-353, 2018.  H. R. Gurav, S. Dama, V. Samuel, and S. Chilukuri, Influence of preparation method on activity and stability of Ni catalysts supported on Gd doped ceria in dry reforming of methane, Journal of CO2 Utilization, vol. 20, pp. 357-367, 2017.  L. Smoláková, M. Kout, L. Čapek, A. Rodriguez-Gomez, V. M. Gonzalez-Delacruz, L. Hromádko, et al., Nickel catalyst with outstanding activity in the DRM reaction prepared by high temperature calcination treatment, International Journal of Hydrogen Energy, vol. 41, pp. 8459-8469, 2016.  L. Yao, M. E. Galvez, C. Hu, and P. Da Costa, Mo-promoted Ni/Al2O3 catalyst for dry reforming of methane, International Journal of Hydrogen Energy, vol. 42, pp. 23500-23507, 2017.  J. Han, Y. Zhan, J. Street, F. To, and F. Yu, Natural gas reforming of carbon dioxide for syngas over Ni–Ce–Al catalysts, International Journal of Hydrogen Energy, vol. 42, pp. 18364-18374, 2017.  C. A. Schwengber, F. A. da Silva, R. A. Schaffner, N. R. C. Fernandes-Machado, R. J. Ferracin, V. R. Bach, et al, Methane dry reforming using Ni/Al2O3 catalysts： Evaluation of the effects of temperature, space velocity and reaction time, Journal of Environmental Chemical Engineering, vol. 4, pp. 3688-3695, 2016.  X. Chen, J. Jiang, K. Li, S. Tian, and F. Yan, Energy-efficient biogas reforming process to produce syngas： The enhanced methane conversion by O2, Applied Energy, vol. 185, pp. 687-697, 2017.  A. S. A. Al-Fatesh and A. H. Fakeeha, Effects of calcination and activation temperature on dry reforming catalysts, Journal of Saudi Chemical Society, vol. 16, pp. 55-61, 2012.  S. Wang, G. Q. Lu, and G. J. Millar, Carbon Dioxide Reforming of Methane To Produce Synthesis Gas over Metal-Supported Catalysts： State of the Art, Energy & Fuels, vol. 10, pp. 896-904, 1996.  S. Praserthdam and P. B. Balbuena, Evaluation of dry reforming reaction catalysts via computational screening, Catalysis Today, vol. 312, pp. 23-34, 2018.  N. Kumar, M Shojaee, and J. J. Spivey, Catalytic bi-reforming of methane: from greehouse gases to syngas, Current Opinion in Chemical Engineering, vol. 9, pp. 8-15, 2015.  王誌謙，觸媒對二氧化碳甲烷化之影響，國立中興大學機械工程學系碩士論文，2017。  B. Abdullah, N. A. Abd Ghani, and D.-V. N. Vo, Recent advances in dry reforming of methane over Ni-based catalysts, Journal of Cleaner Production, vol. 162, pp. 170-185, 2017.  M. K. Nikoo and N. A. S. Amin, Thermodynamic analysis of carbon dioxide reforming of methane in view of solid carbon formation, Fuel Processing Technology, vol. 92, pp. 678-691, 2011.||摘要:||
In this study, syngas production via dry reforming of methane (DRM) with CO2 was experimentally investigated using Ni-based catalysts. In order to suppress the carbon deposition for enhancing the catalyst activity, Ni/Al2O3 modified with CeO2 addition and O2 addition in the reactant were employed in this study. Due to the formation of CeAlO3 that enhancing the carbon-resistance ability, it was found that DRM performance can be enhanced by using CeO2 modified Ni/Al2O3 catalyst. Due to decrease in specific surface area as CeO2 amount increased, there appeared an optimum CeO2 loading for obtaining the best DRM performance. With O2 addition in the fed reactant, it was found that CH4 conversion can be enhanced by O2 addition. However, decrease in CO2 conversion due to CO2 formation from methane oxidation was resulted. It was also found that exothermic partial oxidation of methane was dominant when reaction temperature was low. This led to the results of higher yields of H2 and CO. The TGA test results showed that the CeO2 modified Ni/Al2O3 catalyst would have the lowest amount of carbon deposition when O2 was introduced in the reaction as compared with unmodified Ni/Al2O3 catalyst.
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