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研究生:胡舒剴
研究生(外文):Suh-Kai Hu
論文名稱:改質奈米碳管吸附水中BTEX之研究
論文名稱(外文):A Study on the sorption of BTEX from water with purified carbon nanotubes
指導教授:盧重興盧重興引用關係
學位類別:碩士
校院名稱:國立中興大學
系所名稱:環境工程學系所
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2008
畢業學年度:96
語文別:中文
論文頁數:112
中文關鍵詞:奈米碳管吸附甲苯乙苯二甲苯
外文關鍵詞:Carbon nanotubesAdsorptionBenzeneEthylbenzeneToluenep-Xylene
相關次數:
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本研究藉由不同化學藥劑(HCl, H2SO4, HNO3及NaOCl)改質自備奈米碳管(carbon nanotubes,CNTs)吸附水中芳香環類有機溶劑苯(Benzene)、甲苯(Toluene)、乙苯(Ethylbenzene)、二甲苯(p-Xylene),合稱(BTEX)。奈米碳管經改質處理後,顯示其金屬催化劑與觸媒載體被移除,提高奈米碳管的開口率、增加表面活性位址,產生有利於吸附之官能基。其吸附結果顯示對BTEX吸附量分別為NaOCl>HNO3>H2SO4>HCl。經由改質後,CNTs表面的官能基增加且表面羧基(carboxylic groups)可促使BTEX上的π鍵有電子轉移現象增加之吸附機制。由批次吸附實驗顯示次氯酸鈉改質自備奈米碳管CNT(NaOCl)吸附BTEX之吸附量隨著溫度降低、離子強度上升而有增加的趨勢而pH影響不大。以Langmuir等溫吸附模式求出經由次氯酸鈉改質其最大吸附量為苯(118.49mg/g)、甲苯(140.73mg/g)、乙苯(357.28mg/g)、二甲苯(515.51mg/g)比未改質CNTs高出三倍,也高於粒狀活性碳(GAC)。
根據熱力學及動力學參數,求得次氯酸鈉改質自備奈米碳管符合一階動力且吸附量隨溫度下降而增加,屬於放熱反應。由再生吸脫附實驗結果顯示次氯酸鈉較硝酸有更好脫附效果,次氯酸鈉改質自備奈米碳管在吸附容量與脫附再生特性上均較次氯酸鈉改質商用奈米碳管及商用活性碳有較佳之表現。綜合以上研究結果,次氯酸鈉改質後之奈米碳管對於處理廢水中BTEX具有良好的應用潛力。
Carbon nanotubes (CNTs) were fabricated by the catalytic chemical vapor deposition method and oxidized by HCl, H2SO4, HNO3 and NaOCl solutions for enhancing benzene, toluene, ethylbenzene and p-xylene (BTEX) adsorption in an aqueous solution. The NaOCl-oxidized CNTs show the greatest enhancement in BTEX adsorption, followed by the HNO3-oxidized CNTs, and then the H2SO4-oxidized CNTs. The adsorption mechanism of BTEX via CNTs is mainly attributed to the π-π electron-donor-acceptor interaction between the aromatic ring of BTEX and the surface carboxylic groups of CNTs. The equilibrium amount of BTEX adsorbed on CNTs(NaOCl)(qe) increased with agitation speed, contact time, initial BTEX concentration and solution ionic strength but appeared no remarkable change with solution pH.The maximum adsorbed amounts of BTEX onto heated CNT(NaOCl) calculated by the Langmuir model at 25oC were (B:118.49mg/g, T:40.73mg/g, E:357.28mg/g, X:515.51mg/g) respectively,which were much higher than that onto commercially available granular activated carbon.
The thermodynamic analysis, the adsorption of BTEX onto CNTs(NaOCl) is an exothermic and spontaneous process. A comparative study on the adsorption of BTEX among CNTs, CNT(NaOCl) and GAC showed that under the same conditions the CNT(NaOCl) possess superior adsorption capacities for of BTEX than the CNTs and GAC. The adsorption/desorption study indicated that the CNT(NaOCl) have better reversible adsorption performance than the commercially available CNT(NaOCl) and GAC. This suggests that the as-prepared oxidized CNTs are promising BTEX adsorbents and have good potential for BTEX removal in wastewater treatment.
摘 要......................................i
ABSTRACT....................................ii
目錄........................................iii
圖目錄......................................vi
表目錄......................................viii
第一章 前言.................................1
1-1 研究緣起................................1
1-2研究目的.................................2
1-3研究內容.................................3
第二章 文獻回顧.............................5
2-1 BTEX的來源..............................5
2-1-1 BTEX物化特性及其危害..................5
2-1-2 BTEX之去除技術........................9
2-2奈米碳管的介紹...........................11
2-2-1奈米碳管的發展及應用...................11
2-2-2奈米碳管的結構.........................12
2-2-3 奈米碳管的製備與合成..................13
2-2-4 奈米碳管之純化方法....................15
2-2-5 奈米碳管於環境污染防制之應用..........18
2-3 吸附理論................................21
2-3-1 物理吸附..............................21
2-3-2 化學吸附..............................22
2-3-3 特定吸附..............................23
2-3-4 非特定吸附............................24
2-3-5 吸附技術之應用........................24
2-3-6 影響吸附能力因素......................25
2-3-7 動力吸附模式..........................27
2-3-8 等溫吸附模式..........................28
第三章 實驗方法與設備.......................31
3-1吸附材料及特性分析.......................31
3-1-1 吸附材料..............................31
3-1-2 吸附材料特性分析......................31
3-2 BTEX分析方法與設備......................39
3-3 批次吸附實驗方法........................41
3-3-1 實驗試藥與材料........................43
3-3-2 實驗裝置..............................44
3-3-3 奈米碳管製備..........................45
3-3-4 奈米碳管改質實驗......................46
3-3-5 批次吸附實驗..........................48
3-3-6 奈米碳管劑量及震盪頻率影響之實驗......48
3-3-7 不同接觸時間之實驗....................49
3-3-8 離子強度影響之吸附平衡實驗............50
3-3-9不同pH值之吸附平衡實驗.................50
3-3-10等溫吸附平衡實驗......................51
3-3-11 BTEX之競爭性吸附評估.................52
3-3-12 不同溫度之動力吸附實驗及熱力吸附實驗.52
3-3-13 脫附再生實驗.........................53
第四章 結果與討論...........................55
4-1 奈米碳管純化實驗........................55
4-1-1 不同改質方法實驗......................55
4-2 改質前後特性分析........................57
4-2-1 穿透式電子顯微鏡(TEM).................57
4-2-2 比表面積分析(BET).....................59
4-2-3 熱重量分析(TGA).......................62
4-2-4 傅立葉轉換紅外線光譜分析(FTIR)........63
4-2-5 X光繞射分析(XRD)......................65
4-2-6 拉曼光譜分析(Raman spectroscopy)......66
4-2-7 界達電位(Zeta potential)..............67
4-2-8 表面官能基定量分析(Boehm titration)...68
4-3 奈米碳管吸附BTEX批次實驗................70
4-3-1 吸附劑劑量之影響......................70
4-3-2 震盪頻率影響 ..........................72
4-3-3 不同接觸時間之影響....................73
4-3-4 水中離子強度之影響....................74
4-3-5 水中pH值之影響........................75
4-3-6 等溫吸附..............................76
4-3-7 競爭吸附..............................79
4-3-8 動力學之探討..........................80
4-3-9 活化能................................85
4-3-10 不同溫度下之平衡吸附.................86
4-3-11 熱力學之探討.........................88
4-4 脫附再生實驗............................90
4-4-1 脫附再生濃度對再生效率之影響..........91
4-4-2 脫附時間對再生效率之影響..............92
4-4-3 多次脫附再生實驗之探討................94
4-4-4 經濟效益評估..........................97
第五章 結論與建議...........................99
5-1 結論....................................99
5-2 建議....................................101
參考文獻....................................102
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