臺灣博碩士論文加值系統

本研究旨在探討操作條件對活性碳再生效率及脫附產物之影響，所選用之吸附質為苯環類碳氫化合物(C6H6及C7H8)，吸附劑為球狀活性碳，本研究所探討之操作條件包括:攜行氣體(氮氣及空氣)、攜行氣體流量(2~10 l/min)、微波功率(350~700 W)、再生時間(0~5 min)等。本研究將吸附飽和之活性碳置於微波產生器(2,450 MHz、700 W)中予以脫附再生。研究結果顯示，當使用下列操作條件時，微波脫附後活性碳之物理性質破壞情形較為嚴重:(1)使用空氣為攜行氣體，(2)攜行氣體流量較小，(3)接受微波能量愈大。操作條件對活性碳再生效率之影響，與活性碳物理性質變化之影響的實驗結果相似，即上述三項因素會因活性碳孔隙結構之破壞，影響再生後活性碳之吸附能力，因而使得活性碳再生效率降低。本研究發現，當吸附質為苯及甲苯時，微波脫附之反應產物包括C6H6、C7H8、CH4、CO及CO2等。其中大部分均是脫附出的吸附質(C6H6及C7H8)，其它產物(CH4、CO及CO2)則來自吸附質與吸附劑因於高溫環境下產生所貢獻。此外，研究結果顯示，於溫度較高之操作環境(氧含量較高之攜行氣體、流量較小之攜行氣體或微波所提供之能量較高者)中，吸附質因為高溫之破壞，造成其脫附量有下降之現象，而其它產物之生成量則呈現增加之趨勢。

The objective of this study was to investigate the regeneration of activated carbon by microwave heating process. The multi-component adsorption of both benzene and toluene by spherical activated carbon (SAC) was tested in the research. The regeneration efficiencies of SAC under different experimental parameters included different types of carrier gases (air and nitrogen), carrier flow rates (2.0-10.0 l/min), microwave output power (350-700 W), and regeneration times (0-5 mins). The compositions of flue gas during regeneration were also identified and quantified in the investigation. Experimental results indicated that the decrease in regeneration efficiencies for SAC was detected in the experimental conditions of lower carrier gas flow rates, higher microwave output power, and air as carrier gas. The experimental results were also showed that the SAC pore size was increased and specific surface area was decreased after heating with microwave, which also resulted in the regeneration efficiencies less than 100%. The identified compositions in the flue gas included benzene, toluene, CH4, CO, and CO2. Both benzene and toluene were two major reaction products among these compounds, and the rest compounds mainly resulted from the decomposition of benzene or toluene and oxidation of carbon. The carbon balance for the investigation can be reached up to 90%. Higher concentrations of CH4, CO, and CO2 were observed in the experimental conditions of higher oxygen content in the carrier gas, lower carrier gas flow rates, and greater provided microwave energy. This research provided an innovative process for carbon regeneration.

第一章 緒論…………………………………………………………1-1
1-1 研究緣起……………………………………………………1-1
1-2 研究範圍……………………………………………………1-2
1-3 研究目的……………………………………………………1-3
第二章 文獻回顧……………………………………………………2-1
2-1 活性碳的種類及應用………………………………………2-1
2-2 活性碳脫附再生方法………………………………………2-3
2-2-1 熱脫附再生法……………………………………… 2-7
2-2-2 化學處理再生法…………………………………… 2-9
2-2-3 溶液萃取再生法…………………………………… 2-11
2-2-4 生物處理再生法…………………………………… 2-13
2-2-5 超臨界流體萃取再生法…………………………… 2-14
2-3 微波電能原理、應用及特性…………………………… 2-15
2-3-1 微波電能應用之源起……………………………… 2-15
2-3-2 微波電能加熱之基本原理………………………… 2-16
2-3-3 微波電能技術之應用……………………………… 2-20
2-4 微波脫附再生之優點………………………………………2-30
2-5 影響微波脫附之操作條件………………………………… 2-32
2-5-1 吸附劑及吸附質特性……………………………… 2-33
2-5-2 影響活性碳再生之操作條件……………………… 2-36
2-6 微波脫附後之產物分析………………………………… 2-38
第三章 實驗方法…………………………………………………… 3-1
3-1 實驗設計與流程…………………………………………… 3-1
3-2 實驗設備…………………………………………………… 3-2
3-2-1 恆溫吸附系統……………………………………… 3-2
3-2-2 微波脫附系統……………………………………… 3-4
3-2-3 分析系統…………………………………………… 3-4
3-3 實驗材料及製備方法……… …………………………… 3-7
3-3-1 實驗材料…………………………………………… 3-7
3-3-2 活性碳製備方法…………………………………… 3-8
3-4 實驗方法……………………………………………………3-9
3-4-1 操作條件及範圍…………………………………… 3-9
3-4-2 操作條件對活性碳特性之影響……………………3-10
3-4-3 操作條件對活性碳再生效率及反應產物之影響…3-11
3-5 分析方法………………………………………………… 3-12
3-6 分析方法之品保與品管………………………………… 3-15
3-6-1 標準品之比對………………………………………3-15
3-6-2 檢量線繪製…………………………………………3-16
3-6-3 準確度、精密度及方法偵測極限…………………3-19
第四章 結果與討論………………………………………………… 4-1
4-1 操作條件對活性碳物理性質之影響………………………4-1
4-1-1 活性碳質量之影響………………………………… 4-2
4-1-2 噴流床溫度之影響………………………………… 4-6
4-1-3 活性碳比表面積及平均孔隙半徑之影響………… 4-12
4-1-4 活性碳外觀之影響………………………………… 4-17
4-2 微波脫附反應產物種類……………………………………4-21
4-3 攜行氣體對活性碳再生效率及反應產物之影響…………4-22
4-3-1 攜行氣體對活性碳再生效率之影響……………… 4-24
4-3-2 攜行氣體對反應產物之影響……………………… 4-28
4-4 攜行氣體流量對活性碳再生效率及反應產物之影響… 4-30
4-4-1 攜行氣體流量對活性碳再生效率之影響………… 4-33
4-4-2 攜行氣體對反應產物之影響……………………… 4-37
4-5 微波能量對活性碳再生效率及反應產物之影響…………4-43
4-5-1 微波能量對活性碳再生效率之影響……………… 4-44
4-5-2 微波能量對反應產物之影響……………………… 4-48
4-6 再生時間對產物分佈之影響………………………………4-52
第五章 結論與建議………………………………………………… 5-1
5-1 結論…………………………………………………………5-1
5-2 建議…………………………………………………………5-3
參考文獻……………………………………………………………… 6-1
附錄A GC/FID層析圖例…………………………………………… A-1
附錄B 微波脫附反應結果一覽表………………………………… B-1
附錄C 檢量線……………………………………………………… C-1

1. 蔣本基,張璞,"有機溶劑蒸氣之吸附及脫附研究",工業污染防治 第58期(Apr.1996).
2. Chen-Chia Huang,Tzyy-Ling Hwu,and Yen-Sheng Hsia,"Regeneration of a Fixed Bed of Activated Carbon Adsorbed Organic Vapor by Using Hot Nitrogen Purge,"Separation Science and Technology,28,pp.2431-2447,1993.
3. B.M. Van Vliet and L. Venter,"Infrared Thermal Regeneration of Spent Activated Carbon from Water Reclamation," Wat.Sci.Tech. Vol.17,Amsterdam,pp.1029-1042.
4. Chen-Chia Huang,Tzyy-Ling Hwu,and Yen-Sheng Hsia."Recovery of Acetone Vapor by a Thermal Swing Adsorber with Activated Carbon".Journal of Chemical Engineering of Japan.Vol.26 NO.1,1993.
5. C.Moreno-Castilla,"Thermal Regeneration of an Activated Carbon Exhausted with Different Substituted Phenols," Carbon Vol.33,NO.10,pp.1417-1423,1995.
6. Dennis Clifford,Philip Chu and Albert Lau,"Thermal Regeneration of Powered Activated Carbon(PAC) and PAC-Biological Sludge Mixtures," Water Res. Vol.17 NO.9,pp.1125-1138.1983.
7. Kunio Kato,Kenji Matsuura,Yoshinori Sawamura,and Tamotsu Hanzawa,"The Thermal Regeneration of Spent Activated Carbon".Journal of Chemical Engineering of Japan. Vol.13, NO.3,1980.
8. P.C.Chiang and J.S.Wu,"Evaluation of Chemical and Thermal Regenaration of Activated Carbon," Wat. Sci. Tech. Vol.21, Brightton,pp.1697-1700,1989.
9. R.J.Martin abd W.J.Ng,"The Repeated Exhaustion and Chemical Regeneration of Activated Carbon," Wat. Res. Vol.21, No.8, pp.961-965,1987.
10. R.J.Martin abd W.J.Ng,"Chemical Regeneration of Ehausted Activated Carbon-Ⅱ," Wat.Res. Vol.19, No.12, pp.1527-1535, 1985.
11. R.J.Martin abd W.J.Ng,"Chemical Regeneration of Ehausted Activated Carbon-Ⅰ," Wat.Res. Vol.18, No.1, pp.59-73, 1984.
12. M.Angeles Ferro-Garcia,Jose Rivera-Utrilla,"Chemical and thermal regeneration of an Activated Carbin Saturated with Chlorophenols," J.Chem.Tech.Biotechnol. Vol,67, pp183-189.
13. Chi-Cheng Leng and Neville G.Pinto,"An Investigation of the Mechanism of Chemical Regeneration of Activated Carbon", Ind. Eng. Chem. Res. Vol.35, 2024-2031.
14. David O.Cooney,Andrew Nagerl and Anthony L.Hines,"Solvent Regeneration of Activated Carbon," Water Res. Vol.17, NO.4, pp.403-410,1983.
15. Hajime Tamon,Takashi Saito,Masaaki Kishimura,Morio Okazaki and Ryozo Toei,"Solvent Regeneration of Spent Activated Carbon in Wastewater Treatment," Journal of Chemical Engineering of Japan",Vol.23, No.4, 1990.
16. Dichard J.Posey,Byung R.Kim,"Solvent Regeneration of Dye-Laden Activated Carbon," Journal WPCF, Vol.59, NO.1, Jan.1987.
17. David H.Hutchinson and Campbell W.Robinson,"A Microbial Regeneration Process for Granular Activated Carbon-Ⅰ Process Modelling," Wat.Res. Vol.24, No.10, pp.1209-1215, 1990.
18. 談駿嵩,"超臨界流體中之吸附與脫附",化工 ,第41卷 ,第4期, 1994.
19. Chung-Sung Tan and Din-Chung Liou,"Supercritical Regeneration of Activated Carbon Loaded with Benzene and Toluene",Ind. Eng. Chem. Res. Vol.28, 1222-1226.
20. Kazuyuki Chihara,Kanji Oomori,Takao Oono and Yosuke Mochizuki,"Supercritical CO2 Regeneration of Activated Carbon with Organic Adsorbates," Wat. Sci. Tech. Vol.15, No.7, pp.261-268, 1997.
21. Girridhar Madras, Can Erkey ,and Aydin Akgerman , "Supercritical Fluid Regeneration of Activated Carbon Loaded with Heavy Molecular Weight Organics," Ind. Eng. Chem. Res. Vol.32, pp.1163-1168.
22. C.S.Fang ,Bruce K.L. Chang,and Peter M.C. Lai, "Microwave Regeneration of Spent Activated Carbon," presented at AIChE annual meeting,Nov. pp.15-17,1987,New York,NY.
23. C.S.Fang and Lai,Peter M.C., "Regeneration of Spent Power Activated Carbon by Microwave Radiation," presented at AIChE annual Meeting,April 15 1991.
24. 楊英傑,"以球狀活性碳吸附水溶液中甲苯及其脫附方法之研究",成大化工所碩土士論文,1992.
25. 林勳佑,"在噴流床中應用微波技術再生活性碳之可行性研究", 中山環工所碩士論文,1996.
26. C.S.Fang, Bruce K. L. Chang and Peter M.C. Lai,"Microwave Demulsification",Chem.Eng.Comm., Vol.73, pp.227-239,1988
27. Fang C.S. Bruce K. L. Chang and Peter M.C. Lai,"Oil Recovery and Waste reduction by Microwave Radiation," Environmental Progress , Vol.8, No.4 Nov., 1989.
28. Battelle Institute e.V.,"Separating Oil-Water Emulsions by Electrocoagulation May be Far Cheaper," Chem. Eng. ,Jan. 1989, pp.19.
29. S.Shelley, "Microwaves Surge in the CPI--Uses Range From Processing to Waste Treatment", Chem. Eng., pp.44A-44I, April 1991.
30. C.E.George and G.R.Lightsey,"PVC Waste Recovery Utilizing Electromagnetic Energy," Presented at AIChE Annual Meeting, April 1989.
31. IIT Research Institute,"Decontaminatimg Hazardous Wastes in Soils with Radio Waves," Chem. Eng. pp.23. Aug.15, 1988.
32. New Jersey Institute of Technology, "Microwaves Can Steam Distill and Destroy Toxic Wastes in Soils," Chem. Eng. , pp.23. Sept., 1988.
33. 林基興,"化學化工辭典",曉園出版社,1989.
34. 行政院環保署,"危害性化學物質災害緊急處理手冊",1992.
35. Kinoshita Kim, "Carbon-Electrochemical and Physicochemical Properties," John Wiley ＆ Sons. 1987.
36. Dubinin,M.M.,"Adsorption Properties and Microporous Structure of Carbonaceous Adsorbents", Carbon, Vol.25 , NO.5 ,pp.593-589, 1987.
37. 趙承琛，"界面科學基礎"，7th ,復文書局，1985。
38. Peter Harriott and Alan Tat-Yan Chang, "kinetics of Spent Activated Carbon Regeneration ," AIChE Journal Vol. 34, NO.10, Oct. 1988.
39. T.J. Fabish and D.E. Schleifer, "Surface Chemistry and the Carbon Black Work Function" ,Carbon , Vol.22, NO.1 ,pp.19-38, 1984.
40. Kazuyuki Chihara and J.M.Smith and Motoyuki Suzuki, "Regeneration of Powdered Ativated Carbon" ,AIChE Journal , Vol.27 ,NO.2 , March, 1981.
41. Tadashi Umehara, Peter Harriott and J.M. Smith, "Regeneration of Activated Carbon" ,AIChE Journal , Vol.29,NO.5, September , 1983.
42. 蔣本基, "活性碳物理化學特性對VOCs吸附之影響" ,工業污染防治 第58期 (Apr.1996)
43. Rollor, Michael Allan, "Organic Solvent Regeneration of Granular activated Carbon" ,Georgia Institute of Technology, Sep. 1982.
44. J. M. Osepchuk, "A History of Microwave Heating Applications," IEEE Transactions on Microwave Theory and Techniques, Vol. MTT-32, NO.9, Sep.1984.
45. M.A.Stuchly,Ph.D.,and S.S.Stuchly, Ph.D. "Industrial, Scientific, Medical and Domestic Applications of Microwaves," IEE Proceeding. Vol.130, pt.A, No.8, Nov 1983.
46. Harry E. Thomas, "微波原理與應用" ,1985.
47. 孫又予,"微波電路學" ,國立編譯館，1988.
48. Jerl Walker, "The Secret of a Microwave Oven''s Rapid Cooking Action is Disclosed," Scientific American,Vol.256, Feb.1987, pp.134-138.
49. Rober V. Decareau, "Microwave Food Processing Equipment Through the World," ,Food Technology, June 1986.
50. 賴敏中, "微波電能技術-奇妙的能量傳送於工業上之應用" ,化工, 第40卷 第一期(1993).
51. Nicholas P. Chironis, "Microwaves Dry Fine Coal," Coal Age, Dec,1986.
52. Shute,R.A., "Industrial Microwave Systems For the Rubber Industry," J. of Microwave Power,pp.193-205, Mar.1971.
53. Commonwealth Scientific and Industrial Organization (CSIRO), "Microwave Factory Speeds Synthesis of Chemical Compounds", Chem.Eng, , pp.17. Nov.1989.
54. Goerz D. J. Jr. and Leonard, B. H. Jr.,"Microwave irradiation of Sewage and Sewage Sludge, "U.S. Patent, July 1968.
55. Worman, C. H. Jr.,"Removal of Vinyl Chloride From PVC Resins Using Microwave Radiation," U.S. Patent, June 1976.
56. Suzuki, M., "Adsorption Engineering," Elsevier, New York, NY 1990.
57. Urano, K., and E. Yamamoto, "A Treatment Process of Waste Gas Containing Tolylenediisocyanate by Adsorption with Activated Carbon," Ind.Eng. Chem. Process Des. Ev., 23, 665 ,1984.
58. Dubinin, M.M., "Chemistry and Physics of Carbon," (Edited by P.L. Walker) Vol.2, Marcel Dekker ,New York, NY ,1969.
59. Smithson N., "Carbon Adsorption Handbook," ANN ARBOR Science Publishers, Inc. 1978.
60. 尤建華、江鴻龍、蔣本基, "苯化合物熱解過程中PAHs與碳煙粒狀物的生成探討" ,第十屆空氣污染控制技術研討會論文集, 民國82年12月.