臺灣博碩士論文加值系統

本研究應用非均相臭氧程序(Heterogeneous Catalytic Ozonation)處理油品洩漏至地下水之污染情形，實驗方法是取地下水配製不同濃度之油品成份(包括汽油、柴油等烷羥類化合物、BTEX(包括Benzene、Toluene、Ethylbenzene、p-Xylene)及MTBE(Methyl tert-butyl ether)等)，利用臭氧反應槽添加TiO2觸媒，探討臭氧化及催化臭氧程序分解汽油成份之動力反應及預估可能之反應機制。
研究結果顯示，針對汽油中烷羥類化合物在單獨使用臭氧條件下，去除率約80%，另由各烷羥類化合物組成份在臭氧化過程之變動情形，高碳數者(C5-C12)在氧化過程如臭氧施加量不足，有大部份將裂解成低碳數者(C3-C4)。另外，針對高碳數柴油組成份，在低臭氧量下其分解效率不佳。另添加200 mg/L TiO2條件之臭氧反應結果，可提升去除率至95%。
再者，針對BTEX四種汽油成份以臭氧及催化臭氧分解情形，發現以Benzene被氧化分解效率最低，Xylene最高，主因是前者未鍵結官能基，結構穩定，單獨藉由臭氧之分解率僅有約40%，然針對催化臭氧程序，在200mg/L TiO2添加量，相同臭氧條件，Benzene之分解率可提升至85%以上。

This study is using heterogeneous catalytic ozonation to treat oil pollutants in groundwater, the background water were collected from deeped groundwater, then added various concentration of oils (the oil in this study included alkane hydroxyl compound、BTEX (Bezene、Toluene、Ethylbenzene、p-Xylene、m-Xylene) and MTBE (Methyl tert-butyl ether), such as gasoline and diesel).The reaction was employed ozone combine TiO2 catalyst to decompose oil components. The kinetic of decompose gasoline with ozone process and catalytic ozonation was estimated in this stuidy.
The results show, removal of alkane hydroxyl during ozone processes, the removal rate were approach 80%. The components of alkane hydroxyl compounds variety after ozonation was found, that compounds with large amount of carbon ( C5-C12 ). were degraded by ozone when the ozone dosages under the experimental required.
On the other hand, the degradation rate of low carbon ( C3-C4 ) composited oils, was low during the ozonation diesel oil with large carbon components. Further more, the ozone combine with 200 mg/L TiO2 could increased the removal rate to 95%.
The results of ozonation of BTEX composition in gasoline was found, the benzene has the lowest degraded rate, and most of Xylene can be degraded by ozone, due to the stable structure of benzene, which no bonding functional groups. There are only 40% degradation rate during ozonation. However, the degradation rate can be increased to 85% in same ozone dosages during catalytic ozonation processes.

誌謝...........................................................................................................I
摘要........................................................................................................III
Abstract...................................................................................................IV
目錄..........................................................................................................V
表目錄.....................................................................................................IX
圖目錄.....................................................................................................XI
附錄目錄.................................................................................XVII
1 前言…………………………………………….…………………………..1
2 文獻回顧............................................................................................3
2-1 油品污染物在環境中之來源及傳輸途徑......................................3
2-1-1 歷年油污染事件彙整........................................................4
2-1-2 油品特性與分析................................................................7
2-1-3 汽油的組成及物化特性....................................................8
2-1-4 柴油的組成及物化性質..................................................12
2-2 油品中主要有害污染物..............................................................14
2-2-1 BTEX & MTBE對人體之危害.......................................17
2-2-2 BTEX & MTBE之去除技術............................................22
2-2-2-1 抽出處理法(Pump And Treat)………………………22
2-2-2-2 自然衰減法(Natural Attenuation)……………………23
2-2-2-3 化學氧化法(Chemical Oxidation)…………………….23
2-2-2-4 空氣注入法( Air Sparging)……………………………23
2-2-2-5 生物復育法(Bioremediation)………………………….24
2-3 臭氧的特性及應用......................................................................25
2-3-1 臭氧的介紹.....................................................................25
2-3-2 臭氧的物化特性..............................................................25
2-3-3 臭氧在水相與污染物反應途徑.......................................28
2-3-3-1 環加成反應(cycle addition)…………………………28
2-3-3-2 親電子反應(electrophilic reaction)………………….30
2-3-3-3 親核反應(nucleophilic reaction)………………………30
2-3-4 臭氧在水處理中的應用..................................................32
2-3-4-1 消毒..........................................................................33
2-3-4-2 鐵及錳之金屬氧化....................................................34
2-3-4-3 臭味物質氧化...........................................................35
2-3-4-4 消毒副產物的控制....................................................35
2-3-4-5 增加有機物的生物分解............................................36
2-3-4-6 混凝及過濾的改善....................................................36
2-3-5 結合臭氧之高級氧化程序...............................................37
2-3-5-1 臭氧/H2O2程序..........................................................37
2-3-5-2 UV/TiO2程序............................................................38
2-3-5-3 均相催化臭氧程序....................................................39
2-3-5-4 非均相催化臭氧程序................................................40
2-3-5-5 臭氧結合光催化程序................................................41
3 實驗設備與方法................................................................................42
3-1 實驗流程....................................................................................42
3-2 設備與材料................................................................................43
3-2-1 實驗設備........................................................................43
3-2-1-1 臭氧產生機..............................................................43
3-2-1-2 半批式錐型反應槽..................................................45
3-2-1-3 連續流臭氧程序反應槽...........................................47
3-2-2 實驗藥品.......................................................................49
3-2-2-1 汽油........................................................................49
3-2-2-2 柴油........................................................................49
3-2-2-3 粉末二氧化鈦(Titanium Dioxide, TiO2)……………50
3-3 分析方法...................................................................................54
3-3-1 液相中汽油分析方法.....................................................54
3-3-2 液相中柴油分析方法......................................................56
3-3-3 BTEX分析方法..............................................................57
3-3-4 氣相臭氧濃度分析.........................................................61
3-3-5 液相臭氧濃度分析.........................................................62
4 結果與討論.......................................................................................63
4-1 國內汽、柴油油品成份分析......................................................63
4-2 半批式臭氧反應槽分解汽油、柴油之去除效率分析................69
4-3 半批式臭氧反應槽對BTEX之去除效率分析.......................81
4-4 臭氧及催化臭氧對BTEX之氧化分解動力分析.......................88
4-5 連續流臭氧反應槽對汽油之處理效率..................................103
4-6 汽油組成份臭氧化過程之變動............................................109
5 結論..............................................................................................114
6 參考文獻...........................................................................116
7 附錄............................................................................122

表目錄
表2-1-1 水源地遭油污染事件整理..........................................................5
表2-1-2國內市售無鉛汽油之物化性質...................................................9
表2-1-3 國內市售無鉛汽油之組成份.....................................................10
表2-1-4環保署公告之毒性化學物質表..................................................11
表2-1-5國內市售柴油之物化性質..........................................................13
表2-2-1 BTEX & MTBE物化性質基本性質............................................15
表2-2-2 BTEX 相關法規標準................................................................16
表2-3-1臭氧物理化學性質......................................................................26
表2-3-2 臭氧與各鹵素系物種之氧化-還原電位....................................27
表3-2-1 二氧化鈦種類............................................................................51
表3-2-2 此為本實驗所使用之二氧化鈦性……………..……………….51
表3-3-1 汽油分析方法之Purge&Trap條件..........................................55
表3-3-2 汽油分析方法之GC/MS條件..................................................55
表 3-3-4 柴油分析方法之GC/MS條件...................................................56
表3-3-5 BTEX分析方法之Purge&Trap條件.................................58
表3-3-6 BTEX分析方法之GC/MS條件………………………………….59
表4-1-1 汽油GC-MS質譜鑑定之化合物…………………………………65
表4-1-2 柴油GC-MS質譜鑑定之化合物…………………………………68
表4-2-1 不同的臭氧濃度與反應時間對汽油去除效率…………………74
表4-2-2 柴油在不同的臭氧濃度與反應時間的去除效率………………77
表4-2-3 汽油各組成份在臭氧反應後之去除率………………………….78
表4-2-4 柴油各組成份在臭氧反應後之去除率………………………….80
表4-4-1 單純臭氧程序對BTEX各原水濃度之擬一階速率常數(k, min-1)之比較………………………………………………………………………96
表4-4-2 添加TiO2催化臭氧程序對BTEX各原水初始濃度之擬一階速率常數(k, min-1)之比較………………………………………………………96
表4-4-3 BTEX在單純臭氧及TiO2催化臭氧程序之動力速率常數(kh)與吸附平衡常數(KH)比較……………………………………………………….97
表4-5-1 汽油在不同初始濃度之擬一階速率常數(k, min-1)之比較.....108


圖目錄
圖2-1-1 油品經洩漏之傳播途徑..............................................................3
圖2-1-2 石門水庫油污染點與水場取水口之相關位置............................5
圖2-3-1 臭氧反應路徑...........................................................................28
圖2-3-2臭氧環加成反應(cycle addition)…………………………………..29
圖2-3-3環加成反應機構改變圖……………………………………………29
圖2-3-4親電子反應...............................................................................31
圖2-3-5 光催化機制圖...........................................................................38
圖3-1-1本研究之實驗流程圖.................................................................42
圖3-2-1臭氧產生機示意圖及實體圖......................................................43
圖3-2-2 臭氧產率與電壓之關係圖........................................................44
圖3-2-3半批式反應槽試驗示意圖…………………………………………46
圖3-2-4 臭氧程序連續流反應槽模廠配置圖..........................................48
圖3-2-5 粉末二氧化鈦顆粒之FE-SEM圖……………...………………….52
圖3-2-6 粉末二氧化鈦顆粒之EDS圖…………………………………...…52
圖3-2-7 粉末二氧化鈦顆粒之SAXS圖……………………………………53
圖3-3-1 BTEX之標準品層析圖……………………………………………60
圖4-1-1 中油95無鉛汽油之氣相層析質譜儀分析圖譜………………...64
圖4-1-2 中油高級柴油之氣相層析質譜儀分析圖譜………….…………67
圖4-2-1 含汽油試驗原水之GC-MS層析圖………………………………72
圖4-2-2 汽油原水經0.8 mg/L之臭氧反應5分鐘之GC-MS層析圖….72
圖4-2-3 汽油原水經0.8 mg/L之臭氧反應10分鐘之GC-MS層析圖…73
圖4-2-4 汽油原水經8.0 mg/L之臭氧反應5分鐘之GC-MS層析圖….73
圖4-2-5 汽油原水經8.0 mg/L之臭氧反應10分鐘之GC-MS層析圖....74
圖4-2-6含柴油試驗原水之GC-MS層析圖………………………………75
圖4-2-7 柴油原水經0.8 mg/L之臭氧反應5分鐘之GC-MS層析圖….75
圖4-2-8 柴油原水經0.8 mg/L之臭氧反應10分鐘之GC-MS層析圖…76
圖4-2-9 柴油原水經8 .0 mg/L之臭氧反應5分鐘之GC-MS層析圖….76
圖4-2-10 柴油原水經8.0 mg/L之臭氧反應10分鐘之GC-MS層析圖..77
圖4-3-1 臭氧對m-Xylene之去除效率…………………………………..83
圖4-3-2 臭氧對p-Xylene之去除效率........................................83
圖4-3-3 臭氧對Ethylbenzene之去除效率………………………………84
圖4-3-4 臭氧對Toluene之去除效率……………………………………..84
圖4-3-5 臭氧對Benzene之去除效率…………………………………….85
圖4-3-6 催化臭氧對m-Xylene之去除效率……………………………..85
圖4-3-7 催化臭氧對p-Xylene之去除效率……………………………..86
圖4-3-8 催化臭氧對Ethylbenzene之去除效率…………………………86
圖4-3-9 催化臭氧對Toluene之去除效率……………………………….87
圖4-3-10 催化臭氧對Benzene之去除效率……………………………..87
圖4-4-1 臭氧(1.0 mg/L)反應對Benzene各初始濃度(C0)之擬一階反應速率常數....................................................................................................91
圖4-4-2 臭氧(1.0 mg/L)反應對Toluene各初始濃度(C0)之擬一階反應速率常數....................................................................................................91
圖4-4-3 臭氧(1.0 mg/L)反應對Ethylbenzene各初始濃度(C0)之擬一階反應速率常數............................................................................................92
圖4-4-4 臭氧(1.0 mg/L)反應對p-Xylene各初始濃度(C0)之擬一階反應速率常數.....................................................................................................92
圖4-4-5 臭氧(1.0 mg/L)反應對m-Xylene各初始濃度(C0)之擬一階反應速率常數.................................................................................................93
圖4-4-6添加TiO2(200 mg/L)催化臭氧(1.0 mg/L)反應對Benzene各初始濃度(C0)之擬一階反應速率常數.........................................................93
圖4-4-7添加TiO2(200 mg/L)催化臭氧(1.0 mg/L)反應對Toluene各初始濃度(C0)之擬一階反應速率常數............................................................94
圖4-4-8添加TiO2(200 mg/L)催化臭氧(1.0 mg/L)反應對Ethylbenzene各初始濃度(C0)之擬一階反應速率常數.....................................................94
圖4-4-9添加TiO2(200 mg/L)催化臭氧(1.0 mg/L)反應對p-Xylene各初始濃度(C0)之擬一階反應速率常數........................................................95
圖4-4-10添加TiO2(200 mg/L)催化臭氧(1.0 mg/L)反應對m-Xylene各初始濃度(C0)之擬一階反應速率常數.......................................................95
圖4-4-11 Benzene於單純臭氧程序之Langmuir-Hinshelwood Kinetic模式線性迴歸........................................................................................98
圖4-4-12 Toluene於單純臭氧程序之Langmuir-Hinshelwood Kinetic模式線性迴歸.....................................................................................98
圖4-4-13 Ethylbenzene於單純臭氧程序之Langmuir-Hinshelwood Kinetic模式線性迴歸..................................................................................99
圖4-4-14 p-Xylene於單純臭氧程序之Langmuir-Hinshelwood Kinetic模式線性迴歸.........................................................................................99
圖4-4-15 m-Xylene於單純臭氧程序之Langmuir-Hinshelwood Kinetic模式線性迴歸.........................................................................................100
圖4-4-16 Benzene於添加TiO2催化臭氧程序之Langmuir-Hinshelwood Kinetic模式線性迴歸........................................................................100
圖4-4-17 Toluene於添加TiO2催化臭氧程序之Langmuir-Hinshelwood Kinetic模式線性迴歸...........................................................................101
圖4-4-18 Ethylbenzene於添加TiO2催化臭氧程序之Langmuir-Hinshelwood Kinetic模式線性迴歸......................................101
圖4-4-19 p-Xylene於添加TiO2催化臭氧程序之Langmuir-Hinshelwood Kinetic模式線性迴歸...........................................................................102
圖4-4-20 m-Xylene於添加TiO2催化臭氧程序之Langmuir-Hinshelwood Kinetic模式線性迴歸........................................................................102
圖4-5-1 臭氧(2.0 mg/L)對汽油原水(汽油濃度：C4至C12總合為0.5 mg/L)之去除效率..........................................................................................105
圖4-5-2 臭氧(0.8 mg/L)對汽油原水(汽油濃度：C4至C12總合為0.5 mg/L)之去除效率.......................................................................................105
圖4-5-3 臭氧(0.2 mg/L)對汽油原水(汽油濃度：C4至C12總合為0.5 mg/L)之去除效率.....................................................................................106
圖4-5-4 臭氧(0 mg/L)對汽油原水(汽油濃度：C4至C12總合為0.5 mg/L)之去除效率..........................................................................................106
圖4-5-5 臭氧(2.0 mg/L)/TiO2(200 mg/L)對汽油原水(汽油濃度：C4至C12總合為0.5 mg/L)之去除效率..............................................................107
圖4-5-6汽油在臭氧反應下各臭氧初始濃度及添加TiO2參與反應之擬一階反應速率常數..........................................................................................................107
圖4-5-7 汽油於不同臭氧濃度程序之Langmuir-Hinshelwood Kinetic模式線性迴歸圖...........................................................................................108
圖4-6-1 臭氧劑量為0.2 mg/L時低碳數(C3)與高碳數(C4~C12)在時間上的比較.......................................................................................................111
圖4-6-2 臭氧劑量為0.8 mg/L時低碳數(C3)與高碳數(C4~C12)在時間上的比較..................................................................................................112
圖4-6-3 臭氧劑量為2.0 mg/L時低碳數(C3)與高碳數(C4~C12)在時間上的比較................................................................................................113

附錄目錄
圖3-1 Benzene之標準品之質譜圖……………………………………….122
圖3-2 Toluene之標準品之質譜圖…………….………………………….122
圖3-3 Ethylbenzene之標準品之質譜圖……………………………..…...123
圖3-4 p-Xylene之標準品之質譜圖………………………………………123
圖4-1 中油98無鉛汽油之氣相層析質譜儀分析圖譜………………...124
圖4-2 中油92無鉛汽油之氣相層析質譜儀分析圖譜………………...124
圖4-3 台塑98無鉛汽油之氣相層析質譜儀分析圖譜…………………125
圖4-4 台塑95無鉛汽油之氣相層析質譜儀分析圖譜…………………125
圖4-5 台塑92無鉛汽油之氣相層析質譜儀分析圖譜…………………126
圖4-6 台塑高級柴油之氣相層析質譜儀分析圖譜………….…………126

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