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研究生:周立杰
研究生(外文):Li-Jay Chou
論文名稱:聚乙烯亞胺改質多壁奈米碳管吸附水中硝酸根離子之研究
論文名稱(外文):A Study on the Sorption of Nitrate from Water with Polyethylenimine Modified Multiwalled Carbon Nanotubes
指導教授:盧重興盧重興引用關係
指導教授(外文):Chung-Sying Lu
口試委員:林明瑞黃思蓴
口試委員(外文):Min-Ray LinSz-Chwun Hwang
口試日期:2016-05-31
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:2016
畢業學年度:104
語文別:中文
論文頁數:78
中文關鍵詞:多壁奈米碳管硝酸根離子聚乙烯亞胺吸附脫附
外文關鍵詞:Multi-walled carbon nanotubesnitratePolyethyleneimineadsorptiondesorption
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本研究以多壁奈米碳管(Multiwalled carbon nanotubes, MWCNTs)為吸附劑經由聚乙烯亞胺(Polyethyleneimine, PEI)改質後吸附水中硝酸根離子(NO3-)。研究結果顯示,MWCNTs經由PEI改質後,碳管表面正電荷增加,顯著提升對NO3-的吸附量。在水溫25°C下,以Langmuir模式求取飽和吸附量發現,MWCNTs(PEI)重量比為0.5之吸附劑其飽和吸附量為133.3 mg/g,大於改質粒狀活性碳(101.6 mg/g)以及改質分子篩(103.0 mg/g)。而將PEI/MWCNTs重量比由(0.5:1)提高至(2:1),飽和吸附量將由133.3提升至203.1 mg/g。在吸附動力學探討,其吸附動力符合擬二階動力模式(pseudo-second order kinetic model)。
MWCNTs(PEI)吸附NO3-之平衡吸附量隨溶液離子強度及pH上升而減少,隨溶液溫度及震盪頻率上升而增加。熱力學探討結果顯示,吸附過程屬於自發性之吸熱反應,吸附過程以胺官能基結合為主。經由初始濃度200 mg/L之NO3-溶液吸附飽和後之碳管,以0.05M氯化鈉溶液在25°C下進行脫附再生,結果發現MWCNTs(PEI)經10次脫附再生實驗後, MWCNTs(PEI)約有79.1%再生效率,大於GAC(PEI)之70.7%,顯示改MWCNTs(PEI)在脫附再生效能上有很好的表現。綜合以上述研究結果,MWCNTs(PEI)對於處理水中硝酸根離子具有良好的應用潛力。

Multi-walled carbon nanotubes(MWCNT) were modified by polyethyleneimine(PEI) and employed as adsorbents to study adsorption characteristics of NO3− from aqueous solution. The result shows that the surface charge of MWCNT become more positive as well as the NO3− adsorption capacity had greatly improved after the modification. At solution temperature 25°C, the equilibrium NO3− adsorption capacity of MWCNTs(PEI) with 0.5 solid/liquid ratio is 133.3 mg/L from Langmuir model fitting. It is better than GAC(PEI) (101.6 mg/L) and 13X(PEI) (103.0 mg/L).When PEI/MWCNTs ratio(in weight) change from (0.5:1) to (2:1), the equilibrium NO3− adsorption capacity of MWCNTs(PEI) change from 133.3 to 203.1 mg/L from Langmuir model fitting. The adsorption dynamics study revealed that the NO3− adsorption by MWCNTs(PEI) fits pseudo-second-order equation.
The NO3− adsorption capacity by MWCNTs(PEI) decreased with the increasing ionic strength and pH of the solution, but increased with increasing solution temperature and agitation speed. The thermodynamic analysis revealed that the reaction of NO3− adsorption on MWCNTs(PEI) is endothermic and spontaneous. The adsorption mechanism is the combination of NO3− with functional groups on the surface of MWCNTs(PEI). The regeneration study showed that NO3− could be desorbed easily by a 0.05 M NaCl solution and the adsorption capacity was maintained at 79.1% after 10 times of cyclic adsorption/desorption process. The regeneration efficiency is greater than GAC(PEI) (70.7%). In conclusion, MWCNTs(PEI) has highly potential applications on NO3− removal from aqueous solution.

摘要 i
Abstrate ii
目錄 iii
圖目錄 vi
表目錄 viii
第一章 緒論 1
1.1 研究緣起與動機 1
1.2 研究目的 1
1.3 研究內容 2
第二章 文獻回顧 3
2.1. 硝酸鹽其來源及危害性 3
2.2. 聚乙烯亞胺(Polyethylenimine,PEI)簡介 4
2.3. 奈米碳管簡介 4
2.4. 吸附模式理論 5
2.4.1. 等溫吸附模式 5
2.4.2. 動力吸附模式 8
2.5. 吸附機制 9
第三章 實驗設備與方法 11
3.1. 研究流程 11
3.2. 實驗材料 12
3.2.1. 實驗試藥與器材 12
3.2.1. 吸附材材料及製備方法 12
3.3. 儀器設備 13
3.4. 吸附材表面特性分析方法 13
3.4.1. 比表面積分析儀(BET) 13
3.4.2. 傅立葉轉換紅外光譜儀(FT-IR) 14
3.4.3. 界達電位分析儀 15
3.4.4. 熱重量分析儀(TGA) 15
3.4.5. 表面含氧官能基定量分析 16
3.4.6. 拉曼光譜(Raman) 17
3.4.7. X射線光電子能譜(XPS) 17
3.5. 樣品硝酸鹽(NO3-)分析方法與設備 17
3.6. 實驗方法 18
3.6.1. 奈米碳管改質實驗 18
3.6.2. 奈米碳管劑量及震盪頻率影響之實驗 18
3.6.3. 吸附動力實驗 19
3.6.4. 等溫吸附平衡實驗 20
3.6.5. 離子強度影響與不同pH 值之吸附平衡實驗 20
3.6.6. 不同溫度之吸附動力實驗及等溫吸附實驗 21
3.6.7. 脫附再生實驗 22
第四章 結果與討論 23
4.1. 奈米碳管改質實驗及表面含氧官能基定量分析 23
4.2. 奈米碳管改質前後物化特性分析 25
4.2.1. 比表面積分析儀與孔洞分佈分析 25
4.2.2. 熱重量分析 28
4.2.3. 界達電位分析 30
4.2.4. 傅立葉轉換紅外光譜分析 31
4.2.5. 拉曼光譜分析 32
4.2.6. X射線光電子能譜分析 33
4.3. 奈米碳管吸附硝酸鹽批次實驗 34
4.3.1. 奈米碳管固液比及震盪頻率影響之吸附實驗 34
4.3.2. 吸附動力實驗 36
4.3.3. 等溫吸附平衡實驗 37
4.3.4. 離子強度影響與不同pH值之吸附平衡實驗 39
4.3.5. 不同溫度下動力吸附實驗 42
4.3.6. 吸附動力學之探討 43
4.3.7. 不同溫度下之等溫吸附平衡實驗 45
4.3.8. 吸附熱力學之探討 48
4.4. 化學性吸附機制 50
4.5. 不同吸附材吸附效能比較 52
4.5.1. 表面含氧官能基定量分析 52
4.5.2. 等溫吸附平衡實驗 53
4.5.3. 不同溫度下之等溫吸附平衡實驗 55
4.5.4. 吸附熱力學之探討 59
4.6. 脫附再生實驗 60
4.6.1. 脫附再生液濃度對再生效率影響 61
4.6.2. 脫附時間對再生效率影響 62
4.6.3. 多次脫附再生實驗之探討 63
4.6.4. 經濟效益評估 66
4.7. 文獻比較 68
第五章 結論與建議 69
5.1. 結論 69
5.2. 建議 71
參考文獻 73

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