二氧化碳減量是目前全世界的共識，利用二氧化碳甲烷重組可以將溫室氣體減量並且達到二氧化碳再利用的效果，但由於此重組反應需在高溫下反應且會吸收大量熱量，故本研究使用多孔性介質增進熱傳效益，輔助二氧化碳甲烷重組反應進行。研究方向主要分成三個部分，第一部分探討多孔性介質對重組器內部溫度場分佈的影響，並打入不同流率氮氣，觀察未反應氣體的加熱成效，第二部分探討二氧化碳甲烷重組，給予不同環境溫度與使用不同觸媒，找出較佳的重組成效，第三部分探討多孔性介質的構成段溫度場分佈的改變，及對重組的影響。從實驗結果發現於管內放置多孔性介質能使加熱成效更好，且氣體在到達觸媒反應前會被加熱到最高溫度，適合打入的氣體流率為10 LPM~20 LPM；而二氧化碳甲烷重組反應在越高的環境溫度，其重組效果越好，使用的三種觸媒中，以Rh-Ni/ Al2O3- CeO2有最好重組成效，在觸媒前後反應溫度為650℃與550℃時，二氧化碳轉化率約為30%，甲烷轉化率約為20%；使用的多孔性介質構成有三個部分，分別為蜂巢陶瓷、上游段碳化矽與下游段碳化矽，有無使用蜂巢陶瓷與下游段碳化矽並不會對重組結果有明顯影響，但上游段碳化矽使用的長度，會影響重組效果。

The carbon dioxide reforming of methane takes place at high temperatures and is an endothermic reaction. Thus, porous medium is used in this study to accelerate the reaction of carbon dioxide reforming of methane by improving the heat transfer. This work can be divided into three parts. First, effects of the porous medium and nitrogen flow rate on the temperature profile are studied. Second, the effects of the heating temperature and the catalyst on the performance of carbon dioxide reforming of methane are studied to find a better operational condition. Third, the effects of porous medium formations on the temperature profile and that on the reforming performance are studied.
Results showed that the porous medium improved the heating performance, and the highest temperature of the reactive gases occurred prior to entering the catalyst, at the suitable flow ranged from 10 LPM to 20 LPM. In addition, increasing the heating temperature resulted in an increase of the efficiency of the carbon dioxide reforming of methane. Among the three kinds of catalyst, the Rh-Ni/ Al2O3-CeO2 provide the best reforming performance, the rate of the carbon dioxide conversion rate was about 30 %, and the rate of the methane conversion was about 20 %. The honeycomb, the upstream SiC and the downstream SiC are three major stages in this study. The honeycomb and the downstream SiC did not affect the carbon dioxide reforming of methane, however the length of upstream SiC did affected significantly.

[1] Intergovernmental Panel On Climate Change(IPCC), “Climate Change 2007:Synthesis Report, ” 2007
[2] International Energy Agency, “Key World Energy Statistics,” 2009
[3] International Energy Agency, “World Energy Outlook,” 2009
[4] Chunshan Song, “Global Challenges and Strategies for Control, Conversion and Utilization of CO2 for Sustainable Development Involving Energy, Catalysis, Adsorption and Chemical Processing,” Catalysis Today, 115, 2–32, 2006
[5] http://www.zeep.com/zeep-technology/gasification-vs-combustion.php
[6] Shaobin Wang, G. Q. Lu, Graeme J. Millar, “Carbon Dioxide Reforming of Methane to Produce Synthesis Gas over Metal-supported Catalysts: State of the Art,” Energy & Fuels, 10, 896–904, 1996
[7] J. A. Peter. ARL Technical Report 88-008, the Pennsylvania University
[8] V. R. Choudhary, B. S. Uphade, A. S. Mamman, “Simultaneous Steam and CO2 Reforming of Methane to Syngas over NiO/MgO/SA-5205 in Presence and Absence of Oxygen,” Applied Catalysis A: General, 168, 33–46, 1998
[9] Jin Xuan, Michael K. H. Leung, Dennis Y. C. Leung, Meng Ni, “A Review of Biomass-derived Fuel Processors for Fuel Cell Systems,” Renewable and Sustainable Energy Reviews, 13, 1301–1313, 2009
[10] Julian R. H. Ross, “Natural Gas Reforming and CO2 Mitigation,” Catalysis Today, 100, 151–158, 2005
[11] Patrick O. Graf, Barbara L. Mojet, Jan G. van Ommen, Leon Lefferts, “Comparative Study of Steam Reforming of Methane, Ethane and Ethylene on Pt, Rh and Pd Supported on Yttrium-stabilized Zirconia, ” Applied Catalysis A: General, 332, 310–317, 2007
[12] Zhaoyin Hou, Ping Chen, Heliang Fang, Xiaoming Zheng, TatsuakiYashima, “Production of Synthesis Gas Via Methane Reforming with CO2 on Noble Metals and Small Amount of Noble-(Rh-)promoted Ni Catalysts,” International Journal of Hydrogen Energy, 31, 555–561, 2006
[13] Chan Zen Chen, Hung Shan Weng, “A Comparative Study on Methane Reforming of Carbon Dioxide over Some Ni-based Catalysts, ” 2007
[14] Vasant R. Choudhary, Kartick C. Mondal, Ajit S. Mamman, “High-temperature Stable and Highly Active/Selective SupportedNiCoMgCeOx Catalyst Suitable for Autothermal Reforming of Methaneto Syngas,” Journal of Catalysis, 233, 36–40, 2005
[15] Vasant R. Choudhary, Kartick C. Mondal, “CO2 Reforming of Methane Combined with Steam Reforming or Partial Oxidation of Methane to Syngas over NdCoO3 Perovskite-type Mixed Metal-oxide Catalyst,” Applied Energy, 83, 1024–1032, 2006
[16] Kartick C. Mondal , Vasant R. Choudhary, Upendra A. Joshi, “CO2 Reforming of Methane to Syngas over Highly Active and Stable Supported CoOx (Accompanied with MgO, ZrO2 or CeO2) Catalysts,” Applied Catalysis A: General, 316, 47–52, 2007
[17] Eli Ruckenstein, Yun Hang Hu, “Carbon Dioxide Reforming of Methane over Nickel/Alkaline Earth Metal Oxide Catalysts,” Applied Catalysis A: General, 133, 149–161, 1995
[18] Eli Ruckenstein, Yun Hang Hu, “Role of Support in CO2 Reforming of CH4 to Syngas over Ni Catalysts,” Journal of Catalysis, 162, 230–238, 1996
[19] S. Damyanova, J. M. C. Bueno, “Effect of CeO2 Loading on The Surface and Catalytic Behaviors of CeO2-Al2O3-supported Pt Catalysts,” Applied Catalysis A: General, 253, 135–150, 2003
[20] S. Damyanova, B. Pawelec, K. Arishtirova, M.V. Martinez Huerta, J. L. G. Fierro, “The Effect of CeO2 on The Surface and Catalytic Properties of Pt/CeO2–ZrO2 Catalysts for Methane Dry Reforming,” Applied Catalysis B:Environmental, 89, 149–159, 2009
[21] L. V. Mattos, E. Rodino, D. E. Resasco, F. B. Passos, F. B. Noronha, “Partial Oxidation and CO2 Reforming of Methane on Pt/Al2O3, Pt/ZrO2, and Pt/Ce–ZrO2 Catalysts,” Fuel Processing Technology, 83, 147–161, 2003
[22] 陳彥廷, 陳吟足, 廖炳傑, “CH4/CO2 於CeO2 氧化物與CexZr1-xO2 共氧化物負載式Pt 觸媒之重組反應研究,” 2003
[23] Chunshan Song, Wei Pan, “Tri-reforming of Methane: a Novel Concept for Catalytic Production of Industrially Useful Synthesis Gas with Desired H2/CO Ratios,” Catalysis Today, 98, 463–484, 2004
[24] A. C. S. F. Santos, S. Damyanova, G. N. R. Teixeira, L.V. Mattos, F.B. Noronha, F.B. Passos, J.M.C. Bueno, “The Effect of Ceria Content on The Performance of Pt/CeO2/Al2O3 Catalysts in The Partial Oxidation of Methane,” Applied Catalysis A: General, 290, 123–132, 2005
[25] L. S. F. Feio a, C. E. Hori b, L. V. Mattos c, D. Zanchet d, F. B. Noronha c, J. M. C. Bueno, “Partial Oxidation and Auto thermal Reforming of Methane on Pd/CeO2–Al2O3 Catalysts,” Applied Catalysis A: General, 348, 183–192, 2008
[26] Jing Gao, Zhaoyin Hou, Jianzhong Guo, Yinghong Zhu, Xiaoming Zheng, “Catalytic Conversion of Methane and CO2 to Synthesis Gas over a La2O3-modified SiO2 Supported Ni Catalyst in Fluidized-bed Reactor,” Catalysis Today, 131, 278–284, 2008
[27] Jing Gao, Jianzhong Guo, Dan Liang, Zhaoyin Hou, Jinhua Fei, Xiaoming Zheng, “Production of Syngas Via Autothermal Reforming of Methane in a Fluidized-bed Reactor over The Combined CeO2–ZrO2/SiO2 Supported Ni Catalysts,” International Journal of Hydrogen Energy, 33, 5493–5500, 2008
[28] Jianzhong Guo, Zhaoyin Hou, Jing Gao, Xiaoming Zheng, “Syngas Production via Combined Oxy-CO2 Reforming of Methane over Gd2O3-modified Ni/SiO2 Catalysts in a Fluidized-bed Reactor,” Fuel, 87, 1348–1354, 2008
[29] Sufang He, Hongmiao Wu, Wanjin Yu, Liuye Mo, Hui Lou, Xiaoming Zheng, “Combination of CO2 Reforming and Partial Oxidation of Methane to Produce Syngas over Ni/SiO2 and Ni–Al2O3/SiO2 Catalysts with Different Precursors,” International Journal of Hydrogen Energy, 34, 839–843, 2009
[30] Yan Li, Xiaoxing Wang, Chao Xie, Chunshan Song, “Influence of Ceria and Nickel Addition to Alumina-supported Rh Catalyst for Propane Steam Reforming at Low Temperatures,” Applied Catalysis A: General, 357, 213–222, 2009
[31] Aisling M. O'Connor, Julian R. H. Ross, “The Effect of O2 Addition on The Carbon Dioxide Reforming of Methane over Pt/ZrO2 Catalysts,” Catalysis Today, 46, 203–210, 1998
[32] Jiang Hong Tao, Li Hui Quan, Zhang Yi, “Tri-reforming of Methane to Syngas over Ni/Al2O3–Thermal Distribution in The Catalyst Bed,” Journal of Fuel Chemistry and Technology, 35(1), 72–78, 2007
[33] T. Wurzel, S. Malcus, L. Mleczko, “Reaction Engineering Investigations of CO2 Reforming in A Fluidized-bed Reactor,” Chemical Engineering Science, 55, 3955–3966, 2000
[34] J. Zhu, M. S. M. Mujeebur Rahuman, J. G. van Ommen, L. Lefferts, “Dual Catalyst Bed Concept for Catalytic Partial Oxidation of Methane to Synthesis Gas,” Applied Catalysis A: General, 259, 95–100, 2004
[35] Qiangshan Jing, Hui Lou, Liuye Mo, Xiaoming Zheng, “Comparative Study Between Fluidized Bed and Fixed Bed Reactors in Methane Reforming with CO2 and O2 to Produce Syngas,” Energy Conversion and Management, 47, 459–469, 2006
[36] Susie Wood, Andrew T. Harris, “Porous Burners for Lean-burn Applications,” Progress in Energy and Combustion Science, 34, 667–684, 2008
[37] T. Tomimura, K. Hamano, Y. Honda, R. Echigo, “Experimental Study on Multi-layered Type of Gas-to-gas Heat Exchanger Using Porous Media,” International Journal of Heat and Mass Transfer, 47, 4615–4623, 2004
[38] Amanda J. Barra, Janet L. Ellzey, “Heat Recirculation and Heat Transfer in Porous Burners,” Combustion and Flame, 137, 230–241, 2004
[39] Pei Xue Jiang, Xiao Chen Lu, “Numerical Simulation and Theoretical Analysis of Thermal Boundary Characteristics of Convection Heat Transfer in Porous Media,” International Journal of Heat and Fluid Flow, 28, 1144–1156, 2007
[40] Vijaisri Nagarajana, Valery Ponyavin, Yitung Chen, Milton E.Vernon, Paul Pickard, Anthony E. Hechanova, “Numerical Study of Sulfur Trioxide Decomposition in Bayonet Type Heat Exchanger and Chemical Decomposer with Porous Media Zone and Different Packed Bed Designs, ” International Joural of Hydrogen Energy, 33, 6445–6455, 2008
[41] Bogdan I. Pavel, Abdulmajeed A. Mohamad, “An Experimental and Numerical Study on Heat Transfer Enhancement for Gas Heat Exchangers Fitted with Porous Media,” International Journal of Heat and Mass Transfer, 47, 4939–4952, 2004
[42] R.Bradean, D. B. Inghan, “The Unsteady Penetration of Free Convection Flows Caused by Heating and Cooling Flat Surfaces in Porous Media,” International Journal Heat Mass Transfer, 40, 665–687, 1997
[43] Z. Al-Hamamre, A. Al-Zoubi, “The Use of Inert Porous Media Based Reactors for Hydrogen Production,” International Journal of Hydrogen Energy, 35, 1971–1986, 2010
[44] H. Pedersen-Mjaanes, L. Chan, E. Mastorakos, “Hydrogen Production from Rich Combustion in Porous Media,” International Journal of Hydrogen Energy, 30, 579–592, 2005
[45] S. Afsharvahid, P. J. Ashman, B. B. Dally, “Investigation of NOx Conversion Characteristics in A Porous Medium,” Combustion and Flame, 152, 604–615, 2008
[46] Z. Al-Hamamrea, S. Voß, D. Trimis, “Hydrogen Production by Thermal Partial Oxidation of Hydrocarbon Fuels in Porous Media Based Reformer,” International Journal of Hydrogen Energy, 34, 827–832, 2009
[47] Marc Steen, Luigi Ranzani, “Potential of SiC as A Heat Exchanger Material in Combined Cycle Plant,” Ceramics International, 26, 849–854, 2000
[48] T. L. Marbach, A. K. Agrawal, “Experimental Study of Surface and Interior Combustion Using Composite Porous Inert Media,” Journal of Engineering for Gas Turbines and Power, 127, 307–313, 2005
[49] S. K. Alavandi, A. K. Agrawal, “Experimental Study of Combustion of Hydrogen–Syngas/Methane Fuel Mixtures in A Porous Burner,” International Journal of Hydrogen Energy, 33, 1407–1415, 2008
[50] Wei Hsiang Lai, Yan Charng Luan, “Solid Oxide Fuel Cell System –Sequential Burner Design and Optimization,” 2009 Taiwan SOFC International Symposium, Hosted by Institute of Nuclear Energy Research (INER), Tau-Yuan, Aug.11-13, pp.492-502, 2009
[51] Raviraj S. Dhamrat, Janet L. Ellzey, “Numerical and Experimental Study of The Conversion of Methane to Hydrogen in a Porous Media Reactor,” Combustion and Flame, 144, 698–709, 2006
[52] M. J. Dixon, I. Schoegl, C. B. Hull, J. L. Ellzey, “Experimental and Numerical Conversion of Liquid Heptane to Syngas Through Combustion in Porous Media,” Combustion and Flame, 154, 217–231, 2008
[53] I. Schoegl, S. R. Newcomb, J. L. Ellzey, “Ultra-rich Combustion in Parallel Channels to Produce Hydrogen-rich Syngas from Propane,” International Journal of Hydrogen Energy, 34, 5152–5163, 2009
[54] Mario Toledo, Valeri Bubnovich, Alexei Saveliev, Lawrence Kennedy, “Hydrogen Production in Ultra-rich Combustion of Hydrocarbon Fuels in Porous Media,” International Journal of Hydrogen Energy, 34, 1818–1827, 2009