請用此 Handle URI 來引用此文件:
http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/42585
完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 張慶源 | |
dc.contributor.author | Pei-Tao Hung | en |
dc.contributor.author | 洪培堯 | zh_TW |
dc.date.accessioned | 2021-06-15T01:16:58Z | - |
dc.date.available | 2010-07-28 | |
dc.date.copyright | 2009-07-28 | |
dc.date.issued | 2009 | |
dc.date.submitted | 2009-07-28 | |
dc.identifier.citation | Bhasin, M. M., W. J. Bartlev, P. C. Ellqen, T. P. Wilson, Synthesis gas conversion over supported rhodium and rhodium-iron catalysts, J. Catal, 54(2), 120-128(2008).
Bowker, M., On the mechanism of ethanol synthesis on rhodium, Catal. Today, 15(1), 77-100 (1992). Chuang, S. C., J. G. Goodwin and I. Wender, The effect of alkali promotion on CO hydrogenation over Rh/TiO2, J. Catal., 95(2), 435-446 (1985). Clausen, E. C. and J. L. Gaddy, Biological conversion of synthesis gas, Prepr. Pap.–Am. Chem. Soc., Div. Fuel Chem., 38, 855-861(1993). Forzatti. P., E. Tronconi and I. Pasquon, Higher alcohol synthesis, Cataly Rev., 33(1&2), 109-168 (1991). Hamada, H, Y. Kuwahara, Y. Kintaichi, T. Ito, K. Wakabayashi, H. Iijima and K. Sano, Construction of the C46-C55 fragment of ciguatoxin, Chem. Lett., 23(9), 1611-1612 (1984). Hoffert, M. I., K. Caldeira, G. Benford, D. R. Criswell, C. Green, H. Herzog, A. K. Jain, H. S. Kheshgi, K. S. Lackner, J. S. Lewis, H. D. Lightfoot, W. Manheimer, J. C. Mankins, M. E. Mauel, L. J. Perkins, M. E. Schlesinger, T. Volk and T. M. L. Wigley, Advanced technology paths to global climate stability: Energy for a greenhouse planet, Science, 298(5595), 981-987 (2002). IEA (International Energy Agency), Work energy outlook (2006). IEA, Coal Industry Advisory Board (CIAB), 2006 Workshop Report. http://www.iea.org/Textbase/work/2006/ciab_nov/workshopreport.pdf (November, 2006). Iranmahboob, J., H. Toghiani and D. O. Hill, Dispersion of alkali on the surface of Co-MoS2/clay catalyst: a comparison of K and Cs as a promoter for synthesis of alcohol, Appl Catal A-Gen, 247(2), 207-218(2003). Iranmahboob, J., H. Toghiani and D. O. Hill, K2CO3/Co-MoS2/clay catalyst for synthesis of alcohol: influence of potassium and cob, Appl Catal A-Gen, 231(1-2), 99-108(2002). Jun, K. W., H. S. Roh., K. S. Kim., J. S. Ryu and K. W. Lee., Catalytic investigation for Fischer–Tropsch synthesis from bio-mass derived syngas, Appl. Catal. A-Gen., 259(2), 221-226 (2004). Kintaichi, Y., Y. Kuwahara, H. Hamada, T. Ito and K. Wakabayashi, Selective synthesis of C2-oxygenates by CO hydrogenation over silica-supported Co-Ir catalyst, Chem. Lett., 14(9), 1305-1306 (1985). Koizumi, N., K. Murai, T. Ozaki and M. Yamada, Development of sulfur tolerant catalysts for the synthesis of high quality transportation fuels, Catal. Today, 89(4), 465-478 (2004). Li, D., C. Yang, N. Zhao, H. Qi, W. Li, Y. Sun and B. Zhong. The performances of higher alcohol synthesis over nickel modified K2CO3/MoS2 catalyst, Fuel Process Technol, 88(2), 125-127(2007). Li, D., N. Zhao, H. Qi, W. Li and Y.H. Sun, Ultrasonic preparation of Ni modified K2CO3/MoS2 catalyst for higher alcohols synthesis, Catal Commun, 6(10), 674-678(2005). Li, Z, Effect of rhodium modification on structures of sulfided Rh-Mo-K/Al2O3 catalysts studied by XAFS, J Synchrotron Radiat, 6(3), 462(1999). Olson, E. S., R. K. Sharma and T. R. Aulich., Higher-alcohols biorefinery, Appl. Biochem. Biotech., 115(1-3), 913-932 (2004). Pijolat, M., Synthesis of alcohols from CO and H2 on a Fe/Al2O3 catalyst at 8-30 bars pressure, Appl CataL B-Environ., 13(2), 321(1985). Riley, C., Conversion of Mixtures of Methane and Ethylene or Acetylene into Liquids, AIChE Spring Meeting, New Orleans, Louisiana (2002). Stevens, R. R., Process for producing alcohols from synthesis gas, U.S. Patent No. 4,882,360 (1989). Slaa, J. C., J. G. van Ommen and J. R. H. Ross., The synthesis of higher alcohols using modified Cu/ZnO/Al2O3 catalysts, Catal. Today, 15(1), 129-148 (1992). Spath, P. L. and D. C. Dayton, Preliminary Screening – Technical and Economic Assessment of Synthesis gas to Fuels and Chemicals with Emphasis on the potential for Biomass-Derived Syngas NREL/TP-510-34929, National Renewable Energy Laboratory, Golden, CO (2003). Spivey, J. J. and A. Egbebi, Heterogeneous catalytic synthesis of ethanol from biomass-derived syngas, Chem. Soc. Rev., 36(9), 1514-1528 (2007). Sugier, A., E. Freund, Process for manufacturing alcohols, particularly linear saturated primary alcohols, from synthesis gas, U.S-.Patent No. 4122110(1978). Tien-Thao, N., M. H. Zahedi-Niaki, H. Alamdan and S. Kaliaguine, Effect of alkali additives over nanocrystalline Co–Cu-based perovskites as catalysts for higher-alcohol synthesis, J Catal, 245(2), 348-357(2007). Tyson, K. S., J. Bozell, R. Wallace, E. Petersen and L. Moens, Biomass Oil Analysis: Research Needs and Recommendations NREL/TP-510-34796, National Renewable Energy Lab, Golden, CO (2004). Wang, M., C. Seracks, and D. Santini, Near Future Cases for E-10 Use, ANL/ESD-38, Argonne National Lab, Argonne, IL (1999). Winter, C. L., Make ethanol via syngas. Hydrocarb Process., 65(4), 71-73 (1986). Woo, H. C., T. Y. Park, Y. G. Kim, I. S. Nam, J. S. Lee and J. S.Chung, Alkali-promoted MoS2 catalysts for alcohol synthesis: The effect of alkali promotiom and preparation condition on activity and selectivity, Stud. Surf. Sci. Catal., 75(3), 2749-2752 (1993). Xiang, M., D. Li, W. Li, B. Zhong and Y. Sun, Potassium and nickel doped β-Mo2C catalysts for mixed alcohols synthesis via syngas, Catal Commun, 8(3), 513-518(2007). Xiang, M., D. Li, W. Li, B. Zhong and Y. Sun, K/Fe/β-Mo2C: A novel catalyst for mixed alcohols synthesis from carbon monoxide hydrogenation, Catal Commun, 8(1), 88-90(2007). Zimmerman, W. H., C. N. Campbell and J. L. Kuester, Catalytic conversion of biomass derived synthesis gas to diesel fuel in a slurry reactor, Prepr. Pap.–Am. Chem. Soc., Div. Fuel Chem., 31(3), 116-123 (1986). 左峻德、蘇美惠、方俊德,「國產酒精料源生產力與能源及經濟性指標研析計畫」期末報告,農委會農糧署,2008。 台灣經濟部能源局 (Bureau of Energy, Ministry of Economic Affairs) http://www.moeaec.gov.tw/Promote/regeneration/PrRegMain.aspx?PageId=pr_reg_list01 ,2007。 | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/42585 | - |
dc.description.abstract | 本研究開發合成氣重組製造燃料及化學品之相關應用技術,以協助解決國內有機或生質廢棄物所造成之環境問題,並將其轉化為能源燃料,期能提供國內分散式能源供應的技術能量。
本研究使用高溫高壓液化設備將合成氣(CO及H2)轉化成液體產物,比較添加Pt/γ-Al2O3及MoS2/γ-Al2O3觸媒催化以增進醇類生成選擇率之結果。由實驗結果顯示,比較乾式無添加觸媒(dry syngas liquefaction, DSL)、白金觸媒(Pt/γ-Al2O3 dry catalytic syngas liquefaction, DCSL-Pt)及二硫化鉬(MoS2/γ-Al2O3 dry catalytic syngas liquefaction, DCSL-Mo)三程序,當進料之CO及H2分別為4.77及0.68 g時,比較473、523、573及593 K反應溫度,反應時間一小時之結果顯示DSL於T = 593 K可得235 μg CH4為最佳值;DCSL-Pt於T = 573 K可得68.3 μg CH3OH為最佳值;DCSL-Mo於T = 573 K可得208 μg C2H5OH為最佳值。並添加水分以增加氫氧來源下,其對醇類生成及收集之影響,於水式(hydro-)合成氣液化HSL、HCSL-Pt及HCSL-Mo三程序中,結果顯示HCSL-Pt於T = 593 K可得2,575 μg CH3OH為最佳值;HCSL-Mo於T = 593 K可得128 μg CH4 及6,590 μg C2H5OH為最佳值、於T = 573及523 K時分別得808 μg C3H7OH及11,874 μg other HC-MOH皆為最佳值。並比較乾式及水式各程序,結果顯示於系統中添加水份除可助收集醇類外,水份之添加可明顯減少CH4之產生,有效增進CH3OH、C2H5OH甚至更高碳數之碳氫化合物之產生。 增加添加水量時,除了可以抑制甲烷產生進而增加醇類產物生成以外,更由產物組成比例之變化,可得知水亦可扮演增進其產物選擇性之角色,大幅增進觸媒催化效用。對於CH3OH產率而言,HCSL-Pt程序中添加6 mL H2O催化液化,於T = 573 K時可得6,204 μg為最佳值,相當於同條件下DCSL-Pt程序產生68.3 μg之90倍。對於C2H5OH產率而言,HCSL-Mo程序中添加6 mL H2O催化液化,於T = 573 K時可得8,139 μg之為最佳值,相當於同條件下DCSL-Mo程序產生208 μg之39倍。 | zh_TW |
dc.description.abstract | Bio-energy is now accepted as having a potential to provide a significant portion of the projected renewable energy provisions of the future. Therefore, biomass waste is one of the bio-energy sources and can be reused as a fuel or as a raw material to produce chemical feedstocks.
This study examined the feasibility and operation performance of reaction and liquefaction of syngas (CO and H2) (denoted as SL process), and the enhancement effects of addition of MoS2/γ-Al2O3 and Pt/γ-Al2O3 catalysts (noted as CSL-Mo and CSL-Pt processes, respectively) to increase the yields and selectivities of alcohols generated. For the cases at 473, 523, 573 and 593 K for 1 hr with feeding gas consisting of CO and H2 of 4.77 and 0.68 g, respectively, the DSL process operated at 593 K yields the highest production of CH4 of 235 μg, the DCSL-Pt process at 573 K gives the highest production of CH3OH of 68.3 μg and the DCSL-Mo process at 573 K offers the highest production of C2H5OH of 208 μg. The presence of H2O (called as hydro-process or H-process) assists the generation and collection of alcohols. The results show that the use of Pt/γ-Al2O3 catalyst in the HSL process noted as HCSL-Pt process enhances the formation of CH3OH, giving the highest production of 2,575 μg at 593 K for 1 hr. For the case via the hydro MoS2/γ-Al2O3 process (denoted as HCSL-Mo), it yields the highest productions of 128 μg of CH4 and 6,590 μg of C2H5OH at 593 K. Thus, the addition of H2O enhances the production of alcohols by reducing the generation of CH4. Further, the increase of the addition of H2O in H-process also plays a role to promote the selectivity and enhance the catalytic effectiveness of catalysts, changing the composition of products. Regarding the production of CH3OH, the HCSL-Pt process with 6 mL H2O gives the highest production of 6,204 μg at 573 K, which is about 90 times of that via the DCSL-Pt process. Aiming at C2H5OH, the HCSL-Mo process with 6 mL H2O yields the highest production of 8,139 μg at 573K, which is 39 times of that via the DCSL-Mo process. | en |
dc.description.provenance | Made available in DSpace on 2021-06-15T01:16:58Z (GMT). No. of bitstreams: 1 ntu-98-R96541125-1.pdf: 6625589 bytes, checksum: 2ee335b55c0d5780ea4c37be0a171c53 (MD5) Previous issue date: 2009 | en |
dc.description.tableofcontents | 摘要 I
Abstract III 目錄 V 圖目錄 IX 表目錄 XIII Nomenclature XVII 壹、前言 1 1.1研究緣起 1 1.2研究內容 2 1.3 研究目標 2 貳、文獻回顧 3 2.1合成氣合成液體燃料與化學品技術 3 2.2合成乙醇之化學路徑 4 2.3 合成乙醇之條件 6 2.4合成乙醇之觸媒 10 2.5合成乙醇之選擇率及產率 10 2.6液體燃料產製技術之商業應用 19 2.7生質酒精之經濟利益 20 参、研究方法 23 3.1 實驗設計流程 24 3.2 原料與觸媒來源 24 3.3分析方法與設備 25 3.3.1 氣相層析儀 熱傳導偵測器 25 3.3.2 氣相層析儀 火焰離子偵測器 26 3.3.3 溫度計 28 3.3.4壓力計 29 3.4標準品配置 29 3.4.1氣體標準品 29 3.4.2 液體標準品 29 3.4.3 檢量線之製作 30 3.5 高溫高壓反應設備 31 3.6 實驗步驟 31 3.6.1觸媒製備 31 3.6.2合成氣之反應與液化實驗 32 3.6.3合成氣之催化反應與液化試驗 32 肆、結果與討論 37 4.1觸媒製備及其特性分析 37 4.2乾式合成氣液化程序 38 4.2.1 反應溫度之影響 38 4.2.2觸媒種類之影響 41 4.2.3壓力之變化 45 4.3水式合成氣液化程序 48 4.3.1反應溫度之影響 48 4.3.2觸媒種類之影響 53 4.3.3 壓力之變化 57 4.4綜合討論 61 4.5不同水量於HCSL、HCSL-MO及HCSL-PT 67 4.5.1水量之影響 67 4.5.2觸媒之影響 70 4.5.3 壓力之變化 75 伍、結論與建議 79 5.1結論 79 5.2建議 80 陸、參考文獻 81 附錄A. 不同溫度下乾式合成氣催化反應實驗數據 A-1 附錄B.水式合成氣催化反應實驗數據 B-1 附錄C. 碳氫化合物產率及CO碳轉化率 C-1 附錄D. 不同溫度乾式合成氣液化催化反應實驗壓力變化 D-1 附錄E. 水式合成氣液化催化反應實驗壓力變化 E-1 附錄F. 有機產物碳當量組成比例 F-1 附錄G. 連續採樣式合成氣液化程序 G-1 G.1實驗步驟 G-1 G-2溫度之影響 G-2 G-2反應時間之影響 G-2 G-3合成氣組成之影響 G-2 附錄H.水式合成氣催化反應實驗GC分析圖譜 H-1 附錄I.合成氣擴散特性說明 I-2 附錄J.發表於WORLD RENEWABLE ENERGY CONGRESS 2009 – ASIA之論文 J-1 | |
dc.language.iso | zh-TW | |
dc.title | 合成氣重組製造甲醇及乙醇之研究 | zh_TW |
dc.title | Synthesis of Methanol and Ethanol from Syngas | en |
dc.type | Thesis | |
dc.date.schoolyear | 97-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 謝哲隆,曾錦清 | |
dc.subject.keyword | 合成氣,液化,MoS2/γ-Al2O3,Pt/γ-Al2O3,水式, | zh_TW |
dc.subject.keyword | Syngas,liquefaction,MoS2/γ-Al2O3,Pt/γ-Al2O3, | en |
dc.relation.page | 84 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2009-07-28 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 環境工程學研究所 | zh_TW |
顯示於系所單位: | 環境工程學研究所 |
文件中的檔案:
檔案 | 大小 | 格式 | |
---|---|---|---|
ntu-98-1.pdf 目前未授權公開取用 | 6.47 MB | Adobe PDF |
系統中的文件,除了特別指名其著作權條款之外,均受到著作權保護,並且保留所有的權利。