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Study of Steam Enhanced Dry Reforming of Methane Using Bimetallic Catalysts
|關鍵字:||合成氣;沼氣重組;雙金屬觸媒;轉化率;產率;熱穩定性;syngas;dry reforming of biogas;bimetallic catalyst;conversion;yield;thermal stability||引用:|| 2017年中華民國國家溫室氣體排放清冊報告，行政院環保署，2017。  中油2017永續報告書，台灣中油股份有限公司，2017。  2016年能源產業技術白皮書，經濟部能源局，2016。  105年經濟部能源局年報，經濟部能源局，2017。  P. Weiland, Biogas production: current state and perspectives, Applied Microbiology and Biotechnology 2010; 85:849–860.  沼氣利用技術與實例，現代養豬，2009。  S. S. Itkulova, G. D. Zakumbaeva, Y. Y. Nurmakanov, A. A. Mukazhanova, and A. K. Yermaganbetova, Syngas production by bireforming of methane over Co-based alumina-supported catalysts, Catalysis Today 2014; 228:194–198.  D. Park, C. Lee, D. J. Moon, and T. Kim, Design, analysis, and performance evaluation of steam-CO2 reforming reactor for syngas production in GTL process, International Journal of Hydrogen Energy 2015; 40:11785–11790.  T. Stroud, T. J. Smith, E. Le Saché, J. L. Santos, M. A. Centeno, H. Arellano-Garcia, J. A. Odriozola, and T. R. 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本研究以甲烷乾重組反應為基礎，探討反應溫度 (600~800℃)、進料CH4/CO2比 (1/0.25~1/1) 以及添加水蒸汽對沼氣重組產製合成氣的影響。採用含浸法製備Ni/Al2O3、Pt/Al2O3和Pt-Ni/Al2O3觸媒，並以氮氣物理吸附 (BET)、氫氣程序升溫還原 (H2-TPR) 與X-ray繞射試驗 (XRD) 分析觸媒表徵。由於甲烷乾重組為吸熱反應，因此提升反應溫度可獲得較高CH4和CO2轉化率以及H2和CO產率。實驗結果顯示，3wt%Pt-10wt%Ni/Al2O3雙金屬觸媒表現出較佳的觸媒性能。當進料中含有較多的CO2時，會獲得較高的CH4轉化率和H2產率，但CO2轉化率和CO產率會較低。在進料中添加水蒸汽後，由於甲烷蒸汽重組反應的影響，可獲得較高的CH4轉化率、H2產率以及高於1的H2/CO比。而受到水煤氣轉化反應的影響，會獲得較低的CO2轉化率，甚至出現負值。從穩定性測試發現，Pt-Ni/Al2O3雙金屬觸媒比Ni/Al2O3單金屬觸媒具有更好的熱穩定性。
In this study, syngas production from catalytic dry reforming of biogas was experimentally studied. The Ni/Al2O3, Pt/Al2O3, and Pt-Ni/Al2O3 were used as the catalysts, prepared by wet impregnation method, and characterized by N2 physisorption (BET), hydrogen temperature programmed reduction (H2-TPR), and X-ray diffraction (XRD). A continuous flow tubular reactor was built to perform the catalytic reaction tests, and the following reaction variables were analyzed: reaction temperature (600~800°C) and CH4/CO2 ratio (1/0.25~1/1). Due to endothermic reaction, increasing the reaction temperature led to higher conversions of CH4 and CO2 and yields of H2 and CO. From the measured results, it was found that the bimetallic 3wt%Pt-10wt% Ni/Al2O3 catalyst has the best performance among the catalysts prepared. It was also found that CH4 conversion and H2 yield can be enhanced when biogas contained more CO2. However, CO2 conversion and CO yield decreased. With the addition of steam in the reaction, it was found that CH4 conversion and H2 yield can be enhanced due to the dominance of steam reforming of methane. The H2/CO ratio higher than one can be obtained. However, low or even negative CO2 conversion was resulted due to the enhancement of water-gas shift reaction. From stability test, it was found that Pt-Ni/Al2O3 has better thermal stability than Ni/Al2O3 catalyst.
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