耐酸鹼改性β-殼聚醣吸附劑對反應性染料的等溫吸附性質之研究

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研究生：	吳明宗 Wu-Ming-Tsung
論文名稱：	耐酸鹼改性β-殼聚醣吸附劑對反應性染料的等溫吸附性質之研究 Isothermal Adsorption Properties of Reactive Blue 221 Dye from Aqueous Solutions by Modified β-Chitosan as Acid–Alkali Resistance Adsorbent
指導教授：	邱智瑋 Chih-Wei Chiu
口試委員:	游進陽 Chin-Yang Yu 邱智瑋 Chih-Wei Chiu 邱顯堂 Shen-Tarng Chiou 鄭智嘉 Chih-Chia Cheng 劉定宇 Ting-Yu Liu 鄭如忠 Ru-Jong Jeng 蔡燕鈴 Yen-Ling Tsai
學位類別：	博士 Doctor
系所名稱：	工程學院 - 材料科學與工程系 Department of Materials Science and Engineering
論文出版年：	2020
畢業學年度：	108
語文別：	中文
論文頁數：	149
中文關鍵詞：	殼聚醣、氧化石墨烯、吸附、活性藍221 、染料、耐酸鹼性能、廢水處理
外文關鍵詞：	chitosan, graphene oxide, adsorption, reactive blue 221, dye, acid–alkali resistance property, wastewater treatment
相關次數：	點閱：432 下載：0
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摘要    I
Abstract    III
誌謝    V
目錄    VI
圖目錄    X
表目錄    XIII
第一章    緒論    1
1.1 前言    1
1.2 研究動機及目的    4
第二章    文獻回顧    5
2.1 染整工業簡介    5
2.1.1 染整製程    7
2.1.2 染料簡介    9
2.1.3 染料廢水危害    18
2.1.4 染整廢水特點    20
2.1.5 台灣染整業放流水管制標準    22
2.2 染料廢水處理技術概述    24
2.3 吸附技術理論    25
2.3.1 吸附現象的定義    25
2.3.2 吸附作用力    26
2.3.3 吸附劑移除能力計算    31
2.3.4等溫吸附模型    32
2.3.4.1 Langmuir 等溫吸附模型    32
2.3.4.2 Freundlich 等溫吸附模型    33
2.3.4.3 Temkin  等溫吸附模型    34
2.3.5吸附熱力學    35
2.3.6吸附動力學    35
2.3.6.1 吸附的質傳過程    35
2.3.6.2 擬一級反應動力學模型    36
2.3.6.3 擬二級反應動力學模型    37
2.3.6.4 Elovich 模型    37
2.3.6.5 Weber-Morris模型(顆粒內擴散方程式)    37
2.4 殼聚醣(Chitosan)簡介    38
2.4.1殼聚醣結構    39
2.4.2殼聚醣制備    40
2.4.3殼聚醣對染料吸附機制概述    42
2.5 石墨烯(Graphene)及氧化石墨烯(Graphene oxide )簡介    43
2.5.1氧化石墨烯結構[81]    45
2.5.2氧化石墨烯制備    47
2.5.3氧化石墨烯對染料吸附機制概述    50
第三章    實驗方法    52
3.1 實驗藥品與實驗儀器    52
3.1.1藥品    52
3.1.2實驗儀器及操作方法    53
3.2實驗步驟    55
3.2.1β–chitosan改質吸附劑合成    55
3.2.1.1交聯改質β–chitosan吸附劑製備    55
交聯改質β–chitosan吸附劑製備流程[92]:    55
3.2.1.2 β–chitosan/graphene oxide 混摻改質吸附劑製備    57
3.2.2 β–chitosan改質吸附劑對反應性染料吸附能力測試    59
3.2.2.1 pH值變化對不同吸附劑吸附能力的影響    59
3.2.2.2吸附溫度及吸附時間變化對不同吸附劑吸附能力的影響    59
3.2.2.3初始染料濃度變化對不同吸附劑吸附能力的影響    60
3.3.3β–chitosan/graphene oxide 混摻改質吸附劑對反應性染料吸附能力測試    60
3.3.3.1 pH值變化對不同吸附劑吸附能力的影響    60
3.3.3.2吸附溫度及吸附時間變化對不同吸附劑吸附能力的影響    61
3.3.3.3初始染料濃度變化對不同吸附劑吸附能力的影響    61
第四章 交聯改質β–chitosan吸附劑對反應性染料吸附能力測試    62
4.1交聯改質β–chitosan吸附劑結構分析    62
4.1.1 傅立葉紅外線光譜儀分析    62
4.1.2固態核磁共振光譜儀分析    64
4.2 pH值變化對不同吸附劑吸附能力的影響    65
4.3 等溫吸附模型    67
4.4 吸附熱力學    72
4.5 吸附動力學    75
4.6 BCCT對Reactive Blue 221染料的吸附機制    80
4.6.1氫鍵作用力    80
4.6.2傅立葉紅外線光譜儀分析    82
4.6.3元素分析    83
4.6.4 Zeta Potential Analyzer    84
4.6.5 吸附劑吸附染料前後外觀變化對照    85
第五章  β–chitosan/氧化石墨烯混摻吸附劑對反應性染料吸附能力測試    87
5.1β–chitosan/graphene接枝改質吸附劑結構分析    87
5.1.1傅立葉紅外線光譜儀分析    87
5.1.2拉曼光譜儀分析    88
5.1.3元素分析儀分析    89
5.1.4 TEM分析GO and TFGO結構    90
5.2 pH值變化對不同吸附劑吸附能力的影響    92
5.3等溫吸附模型    94
5.4吸附熱力學    99
5.6 BCCT對Reactive Blue 221染料的吸附機制    109
5.6.1氫鍵作用力    109
5.6.2傅立葉紅外線光譜儀分析    110
5.6.3元素分析    112
5.6.4 吸附劑吸染料前後外觀變化對照    112
第六章  總結    115
6.1 交聯改質β–chitosan吸附劑對反應性染料吸附能力測試    115
6.2 β–chitosan/氧化石墨烯混摻吸附劑對反應性染料吸附能力測試    116
參考文獻    118
附錄    130

 
圖目錄

圖2.1 紡織產業上、中、下游各產業之關聯圖    6
圖2.2染整製程單元分類彙整圖    7
圖2. 3吸附過程示意圖    26
圖2. 4表面氫鍵吸附模型    30
圖2. 5 表面烴基團接受π軌域電子    31
圖2. 6苯環與四氰基乙烯之間的供體 - 受體相互作用    31
圖2. 7吸附劑吸附過程中的質傳過程    36
圖2. 8 a.幾丁質與b.殼聚醣分子結構    40
圖2. 9幾丁質及殼聚醣提取方法    41
圖2. 10 殼聚醣吸附機理圖    42
圖2. 11碳的同素異形體示意圖    44
圖2. 12石墨烯的製備方法    45
圖2. 13早期所提出的氧化石墨烯結構模型    46
圖2. 14 Lerf及Klinowskin所建構氧化石墨烯結構模型    47
圖2. 15天然石墨結構圖    48
圖2. 16氧化石墨烯製備方法    49
圖2. 17氧化石墨烯吸附染料機制    51
圖3. 1改質Β-殼聚醣衍生產物及其中間體產物的合成示意圖….…57
圖3. 2 β-殼聚醣/多胺氧化石墨烯混掺吸附劑製備示意圖    58

圖4. 1交聯改質β - chitosan及其中間產物的FTIR分析圖    63
圖4. 2殼聚醣改質前後13C 固態NMR CP/MAS 圖譜    64
圖 4. 3 pH值對吸附劑吸附能力變化趨勢    67
圖 4. 4不同溫度下吸附材( ■ α - chitosan  ●b-chitosan  ▲ BCCT )之等溫吸附模型    70
圖4. 5 ( ■ α - chitosan  ●b-chitosan  ▲ BCCT )Van’t Hoff 圖    73
圖4. 6不同溫度下吸附材( ■ α - chitosan  ●β - chitosan  ▲ BCCT )之吸附動力模型    78
圖4. 7不同溫度下吸附材( ■ α - chitosan  ●β-chitosan  ▲ BCCT )之時間變化吸附趨勢    80
圖4. 8 UV/VIS電子吸收光譜圖    81
圖4. 9 BCCT吸附RB221前後紅外線光譜變化    82
圖4. 10 BCCT RB221 600ppm    84
圖4. 11吸附劑吸附染料前後對照圖    85
圖4. 12吸附劑對RB221吸附機制圖    86

圖5. 1 GO and TFGO 傅立葉紅外線分析圖    87
圖5. 2 GO and TFGO拉曼光譜分析圖    89
圖5. 3 TEM analysis on the GO and TFGO    91
圖5. 4 pH值變化對吸附劑吸附能力影響趨勢。    94
圖5. 5不同溫度下兩種吸附材料 ( ■ β-chitosan , ● CSGO )之等溫吸附模型    98
圖5. 6( ■ β-chitosan, ●CSGO ) Van’t Hoff 圖    101
圖5. 7不同溫度下對各種吸附材料之吸附動力模型    106
圖5. 8不同pH值及溫度下對吸附材料吸附量的時間變化趨勢影響    108
圖5. 9 UV-VIS電子吸收光譜圖    110
圖5. 10 CSGO吸附RB221染料的前後紅外線光譜的變化。    111
圖5. 11不同吸附材料吸附RB221染料水溶液前後之照片:    113
圖5. 12吸附劑CSGO吸附RB221的吸附機制。    114

 
表目錄

表2. 1染整製程工序概述表    8
表2. 2著色劑種類對比表    9
表2. 3染料分類及適用材料表    18
表2. 4台灣染整業放流水管制標準    23
表2. 5物理吸附和化學吸附的差異性    28

表4. 1 在不同溫度下及吸附材對Reactive Blue 221等溫線模型和參數    71
表4. 2 Reactive Blue 221對不同吸附劑吸附的熱力學參數    74
表4. 3吸附材對Reactive Blue 221吸附的不同動力學模型    79
表4. 4吸附劑吸附前後及RB 2221紅外線光譜官能基定性    83
表4. 5吸附前後之元素分析    84

表5. 1紅外線光譜分析GO改質的前後官能基表徵。    88
表5. 2 Elemental Analysis on the GO and TFGO    90
表5. 3 Elemental Analysis on the β-chitosan and CSGO    90
表5. 4在不同溫度及各種吸附材料對Reactive Blue 221等溫線模型和參數    99
表5. 5不同吸附劑對REACTIVE BLUE 221的吸附熱力學參數    101
表5. 6吸附劑對REACTIVE BLUE 221吸附的不同動力學模型    107
表5. 7紅外線光譜分析吸附劑吸附RB 2221的前後官能基表徵    111
表5. 8吸附劑對RB221染料吸附前後之元素分析。    112

 

                                

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