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Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/91309
標題: Kinetic Developments for Ultrahigh Temperature Water-Gas Shift Reaction Catalyst Using Coal-Derived Syngases
煤基合成氣之超高溫水氣轉化反應觸媒動力開發
作者: 林志彥
Jhih-Yan Lin
關鍵字: Ultrahigh temperature;water-gas shift reaction (WGSR);syngas;CO conversion;chemical reaction kinetics;超高溫;水氣轉化反應;合成氣;CO轉化率;反應動力
引用: 2007年能源科技研究發展白皮書,經濟部能源局。 Linga P, Kumar R, Englezos P. The clathrate hydrate process for post and pre-combustion capture of carbon dioxide. Journal of Hazardous Materials 2007;149:625–629. Schematic of Polygeneration Plant. U.S. Department of Energy (DOE). Haryanto A, Fernando SD, Filip To SD, Steele PH, Pordesimo L, Adhikari S. Hydrogen Production through the Water-Gas Shift Reaction: Thermodynamic Equilibrium versus Experimental Results over Supported Ni Catalysts. Energy & Fuels 2009;23:097–3102. Haryanto A, Fernando S, Adhikari S. Ultrahigh temperature water gas shift catalysts to increase hydrogen yield from biomass gasification. Catalysis Today 2007;129:269–274. Panagiotopoulou P, Kondarides DI. A comparative study of the water-gas shift activity of Pt catalysts supported on single (MO_x) and composite (MO_x/Al_2 O_3, MO_x/TiO_2) metal oxide carriers. Catalysis Today 2007;127:319–329. 林筵翔，超高溫水氣轉化反應觸媒與膜反應器合成氣產氫之實驗探討，中興大學機械工程研究所，台中市，中華民國，2013。 Murgia S, Cau G, Mura G. Experimental investigation and CFD numerical simulation of WGSR for hydrogen enrichment of high CO2 content syngas from an air-blown updraft coal gasifier. Fuel 2012;101:139–147. Hla SS, Morpeth LD, Sun Y, Duffy GJ, Ilyushechkin AY, Roberts DG, Edwards JH. A CeO_2-La_2 O_3- based Cu catalyst for the processing of coal-derived syngases via high-temperature water–gas shift reaction. Fuel 2013;114:178–186. Hla SS, Park D, Duffy GJ, Edwards JH, Roberts DG, Ilyushechkin A, Morpeth LD, Nguyen T. Kinetics of high-temperature water-gas shift reaction over two iron-based commercial catalysts using simulated coal-derived syngases. Chemi -cal Engineering Journal 2009;146:148–154. Sun Y, Hla SS, Duffy GJ, Cousins AJ, French D, Morpeth LD, Edwards JH, Roberts DG. High temperature water–gas shift Cu catalysts supported on Ce–Al containing materials for the production of hydrogen using simulated coal-derived syngas. Catalysis Communications 2010;12:304–309. Jiang L, Zhu H, Razzaq R, Zhu M, Li C, Li Z. Effect of zirconium addition on the structure and properties of CuO/CeO_2 catalysts for high-temperature water-gas shift in an IGCC system. International Journal of Hydrogen Energy 2012;37:15914-15924. Chayakul K, Srithanratana T, Hengrasmee S. Catalytic activities of Re–Ni/CeO_2 bimetallic catalysts for water gas shift reaction. Catalysis Today 2011;175:420–429. Qi X, Flytzani-Stephanopoulos M. Activity and Stability of Cu-CeO_2 Catalysts in High-Temperature Water-Gas Shift for Fuel-Cell Applications. Ind. Eng. Chem. Res. 2004;43:3055-3062. Valsamakis I, Flytzani-Stephanopoulos M. Sulfur-tolerant lanthanide oxysulfide catalysts for the high-temperature water–gas shift reaction. Applied Catalysis B: Environmental 2011;106:255– 263. Manrique YA, Miguel CV, Mendes D, Mendes A, Madeira LM. Modeling and simulation of a packed-bed reactor for carrying out the water-gas shift reaction. Int. J. Chemical Reactor Engineering 2012;10:A84. Laidler KJ and Meiser JM. Physical Chemistry. Benjamin/Cummings 1982:18 -19. Chang LP, Xie ZL, Xie KC. Study on the Formation of NH_3 and HCN during the Gasification of Brown Coal in Steam. Trans IChemE 2006;84(B6):446–452. Zhong C, Shuai Y, Qinfeng L, Fuchen W, Zunhong Y. Distribution of HCN, NH3, NO and N2 in an entrained flow gasifier. Chemical Engineering Journal 2009;148:312–318. Ming-yan X, Yin-ping C, Ling-li Q, Li-ping C, Ke-chang X. Key factors Influen -cing the release and formation of HCN during pyrolysis of iron-containing coal. J Fuel Chem Technol 2007;35(1):5?9. McKenzie LJ, Fu-Jun T, Xin G, Chun-Zhu L. NH3 and HCN formation during the gasification of three rank-ordered coals in steam and oxygen. Fuel 2008;87 :1102–1107.
摘要: 
In this study, catalyst performance of water-gas shift reaction (WGSR) operated in ultrahigh temperature region (750~850°C) was examined experimentally. The bimetallic Pt-Ni supported on Al2O3 spheres was prepared and used as the catalyst for the WGSR. The thermal stability of the bimetallic catalyst was examined first. Using pure CO mixed with steam to carbon ratio (S/C) of 5 as feedstock, good thermal stability of the catalyst was resulted after 72 hours operation. Using the synthetic gas (syngas) with various compositions and S/C ratios as feedstock, the chemical reaction kinetics of WGSR using 2.5wt%Pt-2.5wt%Ni/5wt%CeO2/Al2O3 as catalyst can be established. Based on the experimental data and simple power law, the chemical reaction kinetics can be expressed as,
Reaction temperature = 750°C,
R_co=1.81×?10?^(-9) P_co^0.8932 P_(H_2 O)^1.7329 P_(co_2)^(-0.2561) P_(H_2)^0.1072 (1-1/k_eq (P_(co_2 ) P_(H_2 ))/(P_co P_(H_2 O) ))
Reaction temperature = 800°C,
R_co=1.41×?10?^(-9) P_co^0.7892 P_(H_2 O)^1.8886 P_(co_2)^(-0.2111) P_(H_2)^(-0.0062) (1-1/k_eq (P_(co_2 ) P_(H_2 ))/(P_co P_(H_2 O) ))
Reaction temperature = 850°C,
R_co=4.33×?10?^(-10) P_co^0.9613 P_(H_2 O)^1.9865 P_(co_2)^(-0.2161) P_(H_2)^0.1259 (1-1/k_eq (P_(co_2 ) P_(H_2 ))/(P_co P_(H_2 O) ))

本研究開發適用於超高溫水氣轉化反應之觸媒，首先使用1wt%Pt-2.5wt%Ni/5wt%CeO2/Al2O3觸媒、進料氣體為CO與水蒸汽於反應溫度750℃及水碳莫耳比為5進行長時間72hr實驗，測試觸媒之熱穩定性。實驗結果顯示，觸媒在72hr反應後，熱穩定性仍佳。第二部分使用2.5wt%Pt-2.5wt%Ni/5wt%CeO2/Al2O3觸媒於反應溫度750~850℃、進料氣體為合成氣進行反應，探討合成氣濃度變化對觸媒效能之影響，並依據測得之CO轉化率、CO反應率、H_2產率及H_2產量等數據，求取反應動力。以簡單指數型式來表示，化學反應動力可表為
反應溫度為750℃時，
R_co=1.81×?10?^(-9) P_co^0.8932 P_(H_2 O)^1.7329 P_(co_2)^(-0.2561) P_(H_2)^0.1072 (1-1/k_eq (P_(co_2 ) P_(H_2 ))/(P_co P_(H_2 O) ))
反應溫度為在800℃時，
R_co=1.41×?10?^(-9) P_co^0.7892 P_(H_2 O)^1.8886 P_(co_2)^(-0.2111) P_(H_2)^(-0.0062) (1-1/k_eq (P_(co_2 ) P_(H_2 ))/(P_co P_(H_2 O) ))
反應溫度為在850℃時，
R_co=4.33×?10?^(-10) P_co^0.9613 P_(H_2 O)^1.9865 P_(co_2)^(-0.2161) P_(H_2)^0.1259 (1-1/k_eq (P_(co_2 ) P_(H_2 ))/(P_co P_(H_2 O) ))
URI: http://hdl.handle.net/11455/91309
Rights: 同意授權瀏覽/列印電子全文服務，2016-08-31起公開。
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