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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 張慶源 | |
| dc.contributor.author | Shih-Yun Chen | en |
| dc.contributor.author | 陳詩韻 | zh_TW |
| dc.date.accessioned | 2021-06-14T16:45:15Z | - |
| dc.date.available | 2013-08-04 | |
| dc.date.copyright | 2008-08-04 | |
| dc.date.issued | 2008 | |
| dc.date.submitted | 2008-07-31 | |
| dc.identifier.citation | 1. Bauer, M., R. Herrmann, A. Martin and H. Zellmann, Chemodynamics, transport behaviour and treatment of phthalic acid esters in municipal landfill leachates. Water Sci. Technol., 38(2), 185–192 (1998).
2. Bond, G.C., Heterogous Catalysis Principle and Application. 12nd ed., Oxford Science Publication, Oxford University Press, Oxford UK (1987). 3. Carlsson, P.A., L. Österlund, P. Thormählen, A. Palmqvist, E. Fridell, J. Jansson and M. Skoglundh, A transient in situ FTIR and XANES study of CO oxidation over Pt/Al2O3 catalysts. J. Catal., 226(2), 422–434 (2004). 4. Charest, F. and E. Chornet, Wet oxidation of active carbon. Can. J. Chem. Eng., 54(6), 190 (1976). 5. Chang, B.V., C.M. Yang, C.H. Cheng and S.Y. Yuan, Biodegradation of phthalate esters by two bacteria strains.Chemosphere, 55(4), 533–538 (2004) 6. Cheng, H.F., S.Y. Chen and J.G. Lin, Hazardous organic matters in municipal sewage sludge in Taiwan. Water Sci. Technol., 44(10), 65-70 (2001). 7. Day, D.C., R.R. Hudgins and P.L. Silveston, Oxidation of propionic acid solutions. Can. J. Chem. Eng., 51(6), 733 (1973). 8. Debellefontaine, H., M. Chakchouk, J.N. Foussard, D. Tissot and P. Striolo., Treatment of organic aqueous wastes: wet air oxidation and peroxide oxidation. Environ. Pollut., 92(2), 155-164 (1996). 9. Debellefontaine, H. and J.N. Foussard, Wet air oxidation for the treatment of industrial wastes, Chemical aspects, reactor design and industrial applications in Europe. Waste Manage., 20(1), 15-25 (2000). 10. Ding, Z.Y., M.A. Frisch, L. Li and E.F. Gloyna, Catalytic oxidation in supercritical water. Ind. Eng. Chem. Res., 35(10), 3257-3279 (1996). 11. Ejlertsson, J., E. Johansson, A. Karlsson, U. Meyerson and B.H. Svensson, Anaerobic degradation of xenobiotics by orgainsams for municipal solid waste under landfills conditions. Antonie Van Leewenhoek, 69(1), 67-74 (1996). 12. Ejlertsson, J. and Svensson, B.H. Degradation of bio(2-ethylhexyl)phthalate constituents under methanogenic conditions. Biodegradation, 7(6), 501-506 (1997). 13. Ernst, M., F. Lurot and J.C. Schrotter, Catalytic ozonation of refractory organic model compounds in aqueous solution by aluminum oxide. Appl. Catal. B-Environ., 47(1), 15-25 (2004). 14. Fang, H.H.P., D. Liang and T. Zhang, Aerobic degradation of diethyl phthalate by Shingomonas sp. Bioresours Technol., 98(3), 717–720 (2007) 15. Frish, M.A., L. Li and E.F. Gloyna, Catalyst Evaluation: Supercritical water oxidation process. Proceedings of the 49th Annual Purdue University Industrial Wastewaters Conference, Purdue, IN, USA(1994). 16. Foussard, J.N., “Study on Aqueous Phase Oxidation at Elevated Temperatures and Pressures,” PhD Diss., National Institute of Applied Science, Toulouse, France (1983). 17. Foussard, J.N., H. Debellefontaine and J. Besombes-Vailhe, “Efficient Elimination of Organic Liquid Wastes: Wet Air Oxidation,”J. Enuiron. Eng., 115(2), 367 (1989). 18. Garcia, J., H.T. Gomes, P. Serp, P. Kalck, J.L. Figueiredo and J.L. Faria, Platinum catalysts supported on MWNT for catalytic wet airoxidation of nitrogen containing compounds. Catal. Today, 102-103(1), 101-109 (2005). 19. Gavala, H.N., A.M. Felipe, I. Reza and K.A. Birgitte, Biodegradation of phthalate esters during the mesophilic anaerobic digestion of sludge. Chemosphere, 52(4), 673-682 (2003). 20. Gomes, H.T., J.L. Figueiredo and J.L. Faria, Catalytic wet air oxidation of low molecular weight carboxylic acids using a carbon supported platinum catalyst. Appl. Catal. B-Environ., 27(4), L217–L223 (2000). 21. Gomes H.T., P.V. Samanta, P. Serp, P. Kalckc, J.L. Figueiredoa and J.L. Faria, Carbon nanotubes and xerogels as supports of well-dispersed Pt catalysts for environmental applications. Appl. Catal. B-Environ., 54(3), 175–182(2004). 22. Imamura, S., I. Fukuda and S. Ishido, Wet oxidation catalyzed by ruthenium supported on Cerium(IV) Oxides. Ind. Eng. Chem. Res, 27(4), 718-721 (1988). 23. Joglekar, H. S., S. D. Samant, and J. B. Joshi, “Kinc:tics of Wet Air Oxidation of Phenol and Substituted Phenols,” Wht. Res., 25(2),135 (1991). 24. Joshi, J.B., V.S. Mishra and V.V. Mahajani, Wet Air Oxidation. Ind. Eng. Chem. Res., 34(1), 2-48 (1995). 25. Howard, P.H., Handbook of environmental degradation rates, Lewis Publisher Inc., Chelsea, MI, 725(1991). 26. Kacar, Y., E. Alpay and V.K. Ceylan, Pretreatment of Afyon alcaloide factory’s wastewater by wet air oxidation (WAO). Water Res. 37(5), 1170–1176(2003). 27. Klinghoffer, A.A., R.L. Cerro and M.A. Abraham, Catalytic wet oxidation of acetic acid using Platinum on alumina monolith catalyst. Catal. Today, 40(1), 59-71(1998). 28. Lei, L., X. Hu, H.P. Chu, G. Chen and P.L. Yue, Catalytic wet air oxidation of dying and printing wastewater. Water Sci. Technol., 35(4), 311-319 (1997). 29. Li, L., P.S. Chen and E.F. Gloyna, Generalized kinetic model for wet oxidation of organic compounds. AIChE J., 37(11), 1687-1697 (1991). 30. Liang, D.W., T. Zhang and H.P. Herbert Fang, Anaerobic degradation of dimethyl phthalate in wastewater in a UASB reactor. Water Res., 41(13), 2879-2884 (2007). 31. Lin, S.H., S.J. Ho and C.L. Wu, Kinetic and performance characteristics of wet air oxidation of high-concentration wastewater. Ind. Eng. Chem. Res., 35(1), 307-314 (1996). 32. Lin, S.H. and S.J. Ho, Treatment of high-strength industrial wastewater by wet air oxidation- a case study. Waste Manage.,17(1), 71-78(1997). 33. Luck, F., Wet air oxidation: past, present and future. Catal. Today, 53(1), 81–91 (1999). 34. Lin, J., A. Kawai and T. Nakajima, Effective catalysts for decomposition of aqueous ozone, Appl. Catal. B-Environ., 39(2), 157-165 (2002). 35. Main, K.M., G.K. Mortensen , M.M. Kaleva, K.A. Boisen, I.N. Damgaard and M. Chellakooty, Human breastmilk contaminationwith phthalates and alterations of endogenous reproductive hormones in infants three months of age. Environ. Health. Persp., 114(2), 270–276 (2006). 36. Morteani, G, P. Möller, A. Fuganti and T. Paces, Input and fate of anthropogenic estrogens and gadoliniumin surface water and sewage, plants in the hydrological basin of Prague (Czech Republic). Environ. Geochem. Health., 28(3), 257–64 (2006). 37. Niazi, J.H., D.T. Prasad and T.B. Karegoudar, Initial degradation of Dimethyl phthalate by esterases from Bacillus species. FEMS Microbiol. Lett., 196, 201–205 (2001). 38. Okitsu, K.; Higasi, K.; Nagata, Y.; Dohmaru, T.; Takenaka, N.;Bandow, H.; Maeda, Y. Decomposition of p-Chlorophenol by Wet Oxidation in the Presence of Supported Noble Metal Catalysts. Chem. Abstr., 122, 22180 (1995). 39. Ovejero, G., J.L. Sotelo, A. Rodrı′guez, C. Dı′az, R. Sanz and J. Garcı′a, Platinum catalyst on multiwalled carbon nanotubes for the catalytic wet air oxidation of Phenol. Ind. Eng. Chem. Res., 46, 6449-6455 (2007). 40. Perkas, N., D.P. Minh, P. Gallezot, A. Gedanken and M. Besson, Platinum and ruthenium catalysts on mesoporous titanium and zirconium oxides for the catalytic wet air oxidationof model compounds. Appli. Catal. B-Environ, 59(3-4), 121–130 (2005). 41. Seiler, G.S., Passaic Valley Sewerage Commissioners. Annual Report 1996, Sludge Manage., Series 17, 100 (1987). 42. Schwarzenbach, R.P., B.I. Escher, K. Fenner, T.B. Hofstetter, C.A. Johnson, U. Von Gunten and B. Wehrli, The challenge of micropollutants in aquatic systems. Science, 313(5790), 1072–1077 (2006). 43. Shie, J.L., C.Y. Chang, J.H. Chen, W.T. Tsai, Y.H. Chen, C.S. Chiou and C.F. Chang, Catalytic oxidation of naphthalene using a Pt/Al2O3 catalyst. Appli. Catal. B-Environ., 58(3-4), 289-297 (2005). 44. Staples, C.A., R.D. Peterson, T.F. Parkerton and J.A. William, The environmental fat of phthalate esters. Chemosphere, 35(4), 667-749 (1997). 45. Suarez-Ojeda, M. E., Guisasola A, J.A. Baeza, A. Fabregat, F. Stuber, A. Fortuny , J. Font and J. Carrera, Integrated catalytic wet air oxidation and aerobic biological treatment in a municipal WWTP of a high-strength o-cresol wastewater. Chemosphere, 66(11), 2096-2105 (2007). 46. Tang, W.W., X. Zeng, J. Zhao, G. Gu, Y. Li and Y. Ni, The study on the wet air oxidation of highly concentrated emulsified wastewater and its kinetics. Sep. Puri. Technol., 31(1), 77-82 (2003). 47. Williams, P.E. L., D.C. Day, R.R. Hudgins and P.L. Silveston, Wet air oxidation of low molecular weight organic acids, Water Pollut. Res. in Can., 8, 224 (1973). 48. Yurii, I. Matatov-Meytal and M. Sheintuch, Catalytic abatement of water pollutants. Ind. Eng. Chem. Res., 37(2), 309-326 (1998). 49. Zimmermann, F.J., Waste disposal. US Patent No. 2 665 249., U.S. Patent Office, 6(10), 630-1 (1954). 50. Zhou Y.R., W.P. Zhu, F.D. Liu, J.B. Wang and S.X. Yang, Catalytic activity of Ru/Al2O3 for ozonation of dimethyl phthalate in aqueous solution. Chemosphere, 66(1), 145-150 (2007). 51. 王建龍、吳立波、施漢昌、錢易，馴化活性污染降解鄰本二甲酸酯類化合物的 研究，Environmental science (China), 19(1), 18-20 (1998)。 52. 杭州大學化學系分析化學教室，「化學分析手冊」，化學工業出版社出版，第二版，北京 (1997)。 53. 陳俊揚，「以Cu/La/Ce混合金屬塗覆陶瓷處理氨水溶液之研究」國立中山大學環境工程研究所碩士論文，高雄 (2003)。 54. 黃名儀，「有機酸催化濕式氧化反應之研究」元智大學化學工程系研究所碩士論文，桃園 (2003)。 55. 閻子峰，「奈米催化技術」， 五南圖書出版社出版，第一版，臺北 (2004)。 56. 盧至人、李季眉、蔡岳訓、陳淑貞、黃明智，「多重碳源對水中低濃度有機化合物生物分解的影響」, 行政院國家科學委員會專題研究計畫成果報告,國立中興大學環境工程研究所，臺中 (1991)。 57. 盧德笙，「應用磁性吸附劑吸附環境荷爾蒙-以鄰苯二甲酸二甲酯為例」國立台灣大學環境工程學研究所碩士論文，臺北(2006)。 58. 行政院環保署毒性化學物質災害防救查詢系統，http://61.30.108.131/Chm_/Chm_Index.aspx?vp=MSDS (May, 2008)。 | |
| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/40341 | - |
| dc.description.abstract | 本研究以濕式氧化法(wet air oxidation, WAO)處理鄰苯二甲酸二甲酯(dimethyl phthalate, DMP)。除研究濕式氧化分解DMP之最適化操作參數外，並添加不同種類之觸媒－Pt/Al2O3及γ-Al2O3以濕式催化分解DMP。
研究結果顯示WAO分解DMP之反應速率效率受到轉速(Nr)、反應溫度(T)、系統壓力(PT)等不同參數影響，其中溫度為主要參數。反應溫度愈高，對DMP降解效果愈明顯。其主要分解程序可分為兩階段式反應: (1)自室溫升溫達反應溫度之期間為DMP之無氧熱解反應，DMP降解為中間產物；(2)氧氣的加入後進行濕式氧化反應，中間產物氧化產生低分子量之羰酸，羰酸再經由氧化分解成CO2及H2O。 添加觸媒進行濕式催化分解反應結果可知，於不同工作氣體環境反應有不同之反應機制，DMP在有氧的環境下(工作氣體為氧、空氣)反應時，觸媒表面活性位置幾乎被O2佔據，此時DMP進行催化濕式氧化分解，升溫至473 K時後其DMP可完全去除，但TOC分解率僅達20%。 若工作氣體僅為N2時，DMP之降解機制主要以無氧裂解及吸附為主。DMP於觸媒催化下無氧裂解形成中間產物吸附於觸媒上之活性位置，並進一步分解。將濕式催化反應後之觸媒進行熱重分析發現，以N2為工作氣體反應後之觸媒之有機物吸附量較以O2為工作氣體多，而γ-Al2O3之吸附量又較Pt/Al2O3為多，Pt/Al2O3能將吸附於觸媒表面之有機物更進一步分解。不論使用何種觸媒皆可有效提升DMP之濕式分解效率。 | zh_TW |
| dc.description.abstract | This study investigated the treatment of dimethyl phthalate (DMP) via wet air oxidation (WAO) and catalytic decomposition processes. The Pt/Al2O3 and γ- Al2O3 was used as catalyst to enhance the DMP and total organic compound (TOC) decomposition efficiency (ηDMP and ηTOC).
The result shows the ηDMP and ηTOC of WAO process are related to rotating speed (Nr), temperature (T) and pressure (PT). The temperature is the key factor of organic compound oxidation via WAO process. To increasing reaction temperature can promote the DMP decomposition. The DMP decomposition via WAO process can divide into two steps: (1) at the temperature rising stage (298 to 483 K), the DMP was pyrolysis without O2, (2) oxidation at 483 K for 3 h, DMP was decomposition into acid intermediates (such as formic acid), CO2 and H2O. The adding of catalyst makes different pathway for the decomposition of DMP. The working gas plays an important role in wet catalytic decomposition. In aerobic catalytic decomposition (working gas as O2, air and mixing gas), the oxygen molecule adsorb on the active site of the catalyst surface and be excited as O* which is active. The DMP and intermediates reacted with O* and decomposed into CO2 and H2O. With the O2 content working gas, the DMP destroyed totally at 473K and removed 20% of TOC. The mechanism of anaerobic wet catalytic decomposition (working gas as N2) is quite different as aerobic processes. The intermediate of pyrolysis can be absorbed by both Pt/Al2O3 and γ-Al2O3 where the ηTOC are 80 and 20%. It indicated that Pt on the γ-Al2O3 surface not only can absorb the pyrolysis intermediate but also further catalyzed the organic decomposition. | en |
| dc.description.provenance | Made available in DSpace on 2021-06-14T16:45:15Z (GMT). No. of bitstreams: 1 ntu-97-R95541134-1.pdf: 3374020 bytes, checksum: 92b57d017dd19afe89e3b5697826960e (MD5) Previous issue date: 2008 | en |
| dc.description.tableofcontents | 中文摘要 i
Abstract iii 目錄 v 圖目錄 vii 符號說明 x 第一章 緒論 1 1.1 研究背景 1 1.2 研究方法 3 1.3 研究目的 3 第二章 文獻回顧 5 2.1濕式氧化 5 2.1.1濕式氧化法發展 5 2.1.2 濕式氧化法原理 6 2.1.4濕式氧化反應機制 8 2.1.5氣相在濕式氧化中的傳輸與溶解度 9 2.1.6 濕式氧化法之動力學 11 2.2 影響濕式氧化法之因素 14 2.2.1 攪拌速度 14 2.2.2 溫度 14 2.2.3 壓力 14 2.2.4觸媒濕式氧化法 15 2.3 液相氧化觸媒 16 2.3.1 觸媒的特性 16 2.3.3 觸媒擔體 20 2.3.4 Pt觸媒於CWAO上之應用 20 2.3.5 Pt/γAl2O3觸媒之物理特性 21 2.4鄰苯二甲酸二甲酯 21 2.4.1 鄰苯二甲酸酯類之來源與應用 21 2.4.2 鄰苯二甲酸酯類之特性與環境流布 23 2.4.3 鄰苯二甲酸酯類之主要分解作用 25 2.4.4 鄰苯二甲酸二甲酯相關處理文獻 25 第三章 研究方法 28 3.1 實驗裝置 28 3.1.1 反應系統 28 3.2實驗藥品與設備 31 3.3 實驗步驟 32 3.3.1 實驗流程 32 3.3.2 樣品配置 33 3.3.3 觸媒前處理 33 3.4 實驗內容 33 3.4.1 WAO實驗 33 3.4.2 觸媒濕式催化分解實驗 34 3.5分析項目及方法 37 第四章 結果與討論 40 4.1濕式氧化分解DMP 40 4.1.1攪拌速度之影響 40 4.1.2反應溫度之影響 42 4.1.3反應壓力對濕式氧化分解DMP的影響 44 4.1.4 濕式氧化分解DMP之結論 49 4.2.1 觸媒吸附試驗 50 4.2.2 不同觸媒之WAO催化 53 4.2.5 DMP濕式催化分解機制之探討 72 第五章 結論與建議 81 5.1 結論 81 5.2 建議 82 附錄A. DMP及TOC之檢量線 A-1 附錄B. 實驗數據 B-1 | |
| dc.language.iso | zh-TW | |
| dc.subject | 氧化鋁 | zh_TW |
| dc.subject | 濕式氧化 | zh_TW |
| dc.subject | 濕式催化分解 | zh_TW |
| dc.subject | 觸媒 | zh_TW |
| dc.subject | 鄰苯二甲酸二甲酯 | zh_TW |
| dc.subject | 白金觸媒 | zh_TW |
| dc.subject | dimethyl phthalate (DMP) | en |
| dc.subject | wet catalytic decomposition | en |
| dc.subject | wet oxidation (WO) | en |
| dc.subject | Pt/Al2O3、γ-Al2O3 | en |
| dc.subject | catalyst | en |
| dc.title | 觸媒濕式催化分解DMP之研究 | zh_TW |
| dc.title | Catalytic Wet Air Decomposition of Dimethyl Phthalate | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 96-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 李公哲,邱浚祐,商能洲 | |
| dc.subject.keyword | 濕式氧化,濕式催化分解,觸媒,鄰苯二甲酸二甲酯,白金觸媒,氧化鋁, | zh_TW |
| dc.subject.keyword | catalyst,Pt/Al2O3、γ-Al2O3,wet oxidation (WO),wet catalytic decomposition,dimethyl phthalate (DMP), | en |
| dc.relation.page | 97 | |
| dc.rights.note | 有償授權 | |
| dc.date.accepted | 2008-08-01 | |
| 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 | |
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