| 研究生: |
楊家明 Chia-Ming Yang |
|---|---|
| 論文名稱: |
以離子交換法製備矽-鋁二元氧化物擔體鎳觸媒之研究 Preparation of RHA-Al2O3 Binary Oxide Supported Nickel Catalyst by Ion Exchange |
| 指導教授: |
張奉文
Feg-Wen Chang |
| 口試委員: | |
| 學位類別: |
碩士 Master |
| 系所名稱: |
工學院 - 化學工程與材料工程學系 Department of Chemical & Materials Engineering |
| 畢業學年度: | 88 |
| 語文別: | 中文 |
| 論文頁數: | 106 |
| 中文關鍵詞: | 二氧化碳甲烷化 、鎳觸媒 、矽-鋁二元氧化物擔體 、稻殼灰分 、離子交換法 |
| 外文關鍵詞: | CO2 methanation, nickel catalyst, RHA-Al2O3 binary oxide support, rice husk ash, ion exchange |
| 相關次數: | 點閱:8 下載:0 |
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本研究以稻殼灰分為主原料,利用離子交換法製備矽-鋁二元氧化物擔體鎳觸媒,並於一大氣壓、573K ~ 923K下進行二氧化碳甲烷化反應活性測試,結果顯示矽-鋁二元氧化物擔體鎳觸媒於高溫下的熱穩定性能使甲烷化反應有高甲烷選擇率。
於觸媒製備方面,實驗結果發現:金屬載量愈低,則金屬分散度愈高;而適當的鍛燒程序,能夠控制觸媒表面金屬晶粒的大小及分佈,使其有較佳的催化活性。因此,欲使矽-鋁二元氧化物擔體鎳觸媒發揮最佳的催化效率,4.44 wt%的金屬載量、773K下4小時的鍛燒,由室溫升溫至773K的還原程序及923K下的甲烷化反應,將是最佳的製備及操作條件。且經由TPR及TPD技術的分析證實,以稻殼灰分製備而成的矽-鋁二元氧化物擔體﹙RHA-Al2O3﹚,其特殊的擔體表面性質有利於鎳金屬分散,乃是一種兼具高促進效果及經濟效益的甲烷化觸媒擔體。
RHA-Al2O3 binary oxide supported nickel catalyst prepared by ion exchange was examined in methanation of CO2 at 573 ~ 923K and high selectivity for CH4 formation was found at high reaction temperature due to its thermal stability.
During the investigations of preparation conditions, effects of nickel loading, calcination temperature, calcination time, reaction time and reaction temperature on catalytic behavior were presented and discussed. The results indicate that the metal dispersion increases with decreasing of nickel loading; the CH4 selectivity depends on calcination conditions; the activity of nickel catalyst achieves a maximum value with a nickel loading of 4.44 wt% , calcined at 773K for 4h and reduced at 773K in CO2 hydrogenation at 973K.
Moreover, by using TPR and H2-TPD techniques, RHA-Al2O3 is good for the dispersion of nickel and is a preferable and economic support.
Aguinaga. A. ,J. C. De La Cal, J. M. Asua, and M. Montes, “Effect of the Preparation on the Activity and Selectivtiy of Supported Nickel Catalysts”, Appl. Catal. A. , 51,1(1989).
Amick, J. A. ,“Purification of Rice Hulls As a Source of Solar Grade Silicon for Solar-Cells”, J. Electrochem. Soc. , 129(4),864(1982).
Anderson, J. H. , J. Catal. , 26,277(1972).
Benenek, S. ,E. Fedorynska, and P. Winiarek, ”Investigation of the Acidity of Ni/Al2O3 and Ni/SiO2-Al2O3 Catalysts”, React. Kinet. Catal. Lett. , 51,89(1993).
Boar, P. L. and L. K. Ingram , “The Comprehensive Analysis of Coal Ash and Silicate Rocks by Atomic-Absorption Spectrophotometry by a fusion Technique” , Analyst. , 95,124(1970).
Bonneviot, L. , O. Clause , M. Che , and H. Dexpert , Catal. Today , 6,39(1989).
Burton, R. S. ,R. C. Richard, and S. Alpert, “Municipal Solid Waste Prolysis” , AIChE System , 70(141),116(1974).
Burwell, R. , G. Pearson , G. Haller , and S. Chock , Inorganic Chemistry , 4,1123(1965).
Carter, J. L. ,J. A. Cusumano, and J. H. Sinfelt, “Catalysis Over Supported Metal. V. The Effect of Crystallite Size on the Catalystic Activity of Nickel”, J. Phy. Chem. , 70,2257(1966).
Chakraverty, A. ,P. Mishra, and H. D. Banerjee, “Investigation of Thermal Decomposition of Rice Husk”, Thermochimica Acta , 94,267(1985).
Chakraverty, A. ,P. Mishra, and H. D. Banerjee, “Investigation of Production of Pure Amorphous White Silica”, J. Master. Sci. , 23,21(1988).
Chang, F. W. ,Hsiao T. J. ,Chang S. W. ,Lo J. J. , “Nickel Supported on Rice Husk Ash-Activity and Selectivity in CO2 Methanation”, Appl. Catal. A. , 164,225(1997).
Chang, F. W. ,T. J. Hsiao, and J. D. Shih, “Hydrogenation of CO2 over a Rice Husk Ash Supported Nickel Catalyst by Deposition-Precipitation”, Ind. Eng. Chem. Res. , 37(10),3838(1998).
Clause, O. ,L. Bonneviot, and M. Che, “Nickel(II) Ion-Support Interactions as a Function of Preparation Method of Silica-Supported Nickel Materials”, J. Amer. Chem. Soc. , 114,4709(1992).
Clause, O. ,L. Bonneviot, and M. Che, “Effect of the Preparation Method on the Thermal Stability of Silica-Supported Nickel Oxide as Studied by EXAFS and TPR Techniques”, J. Catal. , 138,195(1992).
Gil. A. ,A. Diaz. ,L. M. Gandia, and M. Montes, “Influence of the Preparation Method and the Nature of the Support on the Stability of Nickel Catalysts”, Appl. Catal. A:General , 109,167(1994).
Hamad, M. A. , “Thermal Characteristic of Rice Hulls”, J. Chem. Tech. Biotechnol. , 31,624(1981).
Hindustan Lever Ltd. , Indian Patent , No.147090(1979).
Houston, D. F. ,“Rice Hulls”, Rice Chemistry and technology , Chapter 12 , Houston, D. F. ,Eds. ,American of Association of Cereal Chemistry, St. Paul. Minnessota(1972).
Klbag, S. S. ,P. K. Basu, and N. V. Bringi, Indian Patent,No.146570(1979).
Liou, T. H. and F. W. Chang, “The Nitridation Kinetics of Pyrolyzed Rice Husk”, Ind. Eng. Chem. Res. , 35(10),3375(1996).
Liou, T. H. ,F. W. Chang, and J. J. Lo, “Pyrolysis Kinetics of Acid-Leached Rice Husk” , Ind. Eng. Chem. Res. , 36(3),568(1997).
Longgaback, J. R. and F. Banner, Industrial and Laboratory Pyrolyusis , Chap.27,476(1976).
Loosdrecht, J. van de, A. M. van der Kraan, A. J. van Dillen, and J. W. Geus,“Metal-Support Interaction:Titania-Supported and Silica-Supported Nickel Catalysts”, J. Catal. , 170,217(1997).
Medsford. S. , J. Chem. Soc. , 123,1452(1923).
Michael C. J. Bradford, M. Albert Vannice, ”Catalytic Reforming of Methane with Carbon Dioxide Over Nickel Catalysts. I. Catalyst Characterization and Activity”, App. Catal. A:General , 142,73(1996).
Mile, B. D. Stirling, M. A. Zammitt, A. Lovell, and M. Webb, “The Location of Nickel Oxide and Nickel in Silica-Supported Catalysts:Two Forms of “NiO” and the assignment of Temperature Programmed Reduction Profiles”, J. Catal. , 114,217(1988).
Mills, G. A. and F. W. Steffgen, “Mechaism of CO2 Methanation”, Catal. Rev. , 8,159(1974).
Patel, M. , A. Karera, and P. Prasanna, “Effect of Thermal and Chemical Treatment on Carbon and Silica Contents in Rice Husk”, J. Master. Sci. , 20,4387(1987).
Pichler H. , Brennst.-Chem. , 24,39(1943).
Richardson, J. T. and R. J. Dubus, “Crystallite Size Distributions of Sintered Nickel Catalysts”, J. Catal. , 57,417(1979).
Riverors, H. and C. Garz, “Rice Husks as a Source of High Purity Silica”, J.Master. Sci. , 22,4665(1987).
Russell, W. W. and G. H. Miller, J. Amer. Vhem. Soc. , 72,2446(1950).
Schlesinger, M. D. ,W. S. Sianner, and D. E. Wolfson, “Processing Agrricultural and Municipal Wastes”, AVI Press Chap.9 , 93(1972).
Scokart., P. O. ,F. D. Declerck, R. E. Sempels, and P. G. Rouxhet, J. Chem. Soc., Faraday Trans.I , 73,359(1977).
Sealock, L. J. , Bisource Digest , 2,(1980).
Sermon, P. A. and J. Sivalingam, ”Mechanisms of Preparation of Silica Supported”, Colloids and Surfaces , 63,59(1992).
Stanislaus. A. ,M. Absi-Halab, and K. Al-Dolama, “Effect of Nickel on the Surface-Acidity of Gamma-Alumina and Alumina-Supported Nickel-Molybdenum Hydrotreating Catalysts”, Appl. Catal. A. , 50,237(1989).
Tanabe. K., “Solid Acids and Bases”, Kodansha, Tokyo, and Academic Press, New York (1970).
Tauster, S. J. ,S. C. Fung, and R. L. Garten, J. Amer. Chem. Soc. , 100,170(1978).
Tsay, M. T. and F. W. Chang, “Characterization of Rice Husk Ash-Supported Nickel Catalysts Prepared by Ion Exchange” , Appl. Catal. A (in press,2000).
Vannice, M. A., “The Catalytic Synthesis of Hydrocarbon from H2/CO Mixture over the Group VIII Metals”, J. Catal. , 37,449(1975).
Vlasenko. V. M. and G. E. Yuzefovich, “Mechanism of the Catalytic Hydrogenation of Oxides of Carbon to Methane”, Russian Chem. Rev. , 38(9)(1969).
Yoshida, S. and K. Kitagishi, “Chemical Forms, Mobility and Depostion of Silicon in Rice Plant”, Soil Science and Plant Nutrition , 8,15(1962).
黃豐智, ”氧化矽載體無電鍍鎳觸媒之研究”, 私立逢甲大學化學工程研究所碩士論文(1994).
劉宗宏, ”二氧化矽/碳粉和稻殼灰分氮化反應動力學之研究”, 國立中央大學化學工程研究所博士論文(1995).
梁世平, ”以稻殼灰分離子交換製備擔體鎳觸媒之研究”, 國立中央大學化學工程研究所碩士論文(1996).
歐迪政, ”以含浸法製備矽-鋁二元氧化物擔體鎳觸媒之研究”, 國立中央大學化學工程研究所碩士論文(1997).