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研究生:陳鴻偉
研究生(外文):Hong-Wei Chen
論文名稱:應用乳化液進行底泥中鄰苯二甲酸酯類去除及生物降解模場實驗
論文名稱(外文):Emulsion-enabled direct removal and biodegradation of phthalates in river sediment
指導教授:張書奇張書奇引用關係
指導教授(外文):Shu-Chi Chang
口試委員:盧至人蔡利局余光昌
口試委員(外文):Chih-Jen LuLi-Chu TsaiKuan-Chung Yu
口試日期:2015-07-20
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:2015
畢業學年度:103
語文別:中文
論文頁數:147
中文關鍵詞:鄰苯二甲酸酯底泥乳化液去除生物降解模場試驗
外文關鍵詞:phthalatessedimentEmulsion-enabledremovalbiodegradation
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河川底泥在生態系中扮演重要功能,因為人類活動,使得河川底泥遭受污染,污染物循食物鏈造成生態系之破壞,人體健康也因此受到危害。鄰苯二甲酸酯類化合物(phthalate esters, PAEs)為新興污染物中內分泌干擾物質的一種。在日常生活中使用之聚氯乙烯(poly vinyl chloride, PVC)材質之塑膠中即會有高量之PAEs。台灣室內空氣塵粒中之塑化劑濃度為全球最高,土壤與底泥中之鄰苯二甲酸二(2-乙基己基)酯(di(2-ethylhexyl)phthalate, DEHP )濃度與世界各國比較也偏高。PAEs因其為疏水性物質極易蓄積於底泥中,但目前PAEs整治技術大多針對廢水處理,其處理方式有物化處理及生物處理,無法適用於河川底泥整治,如添加藥劑可能使底泥環境遭受二次破壞,而生物處理則因為廢水處理使用之菌株,可因操作之條件不同而提高處理效果,但對於本研究主要處理目標為現地整治直接整治,並無法調整一適合菌株降解PAEs之所需環境。然而目前國際間廣泛使用之河川底泥整治方法,因台灣地勢陡峭且河流湍急,並不完全適用於台灣污染場址。
本研究以大豆油製成之不穩定乳化液,藉由乳化液之油相與土顆粒相對較高之比表面積,在高速有效碰撞下,將底泥中之PAEs重新分布至油相且總油水分層回收而去除,並且利用殘餘之乳化液加強其生物降解。本研究除了針對乳化液之除污處理成效外,亦同時探討自然回復、厭氧分解、好氧分解以及厭氧-好氧分解之不同處理方法進行模場測試PAEs整治復育之效果。其結果為乳化液添加量與底泥乾重比為1:0.84,破乳化之碳酸鈉最終濃度0.78M進行回收去除,最佳操作條件為使用每分鐘4 L之曝氣流量、曝氣時間30分鐘、靜置時間12小時進行乳化液回收試驗。依據模場試驗結果顯示乳化液去除之部分:針對額外新添加之PAEs之污染物去除率為60-70%,但對於底泥中風化之污染回收僅BBP去除率77%較佳外,其他三種去除率為3-25%;生物降解之部分,有添加乳化液之組別的確有增強生物降解之情況,結果顯示添加乳化液除了有去除污染效果,也有助於PAEs之降解。

River sediments play a vital role in an ecosystem, such as self-purification, habitats for benthic organisms and planktons, fish reproduction and feeding place, and feeding ground for wading birds. However, due to human activities, sediments are polluted. Thus, human health in turn is under threats. Phthalate esters (PAEs) are one of the endocrine disrupting compounds in the so-called emerging contaminants and are usually used as industrial plasticizers to increase the flexibility and softness of plastics. Commonly used poly vinyl chloride (PVC) plastics have high level of PAEs. The concentrations of PAEs on the dusts of indoor air in Taiwan are the highest in the world. The concentration of one type of PAEs, di(2-ethylhexyl)phthalate (DEHP) in soil and sediment Taiwan is also ranked at the front of all countries in the world. Due to their hydrophobicity, they tend to accumulate in sediments. However, most treatment methods for PAEs are aimed at wastewater treatment instead of sediment contamination. These methods include physicochemical and biological methods and cannot be directly applied to sediment remediation. Moreover, currently widely applied technologies on sediment remediation cannot be employed in Taiwan because the steep landscape of Taiwan resulting high flow velocity of river water in Taiwan.
In this study, an instable soy bean oil emulsion is used to recover PAEs from contaminated sediment through frequent high speed collision between oil droplets and sediment granules resulting re-partitioning of PAEs between sediments and soybean oil. Afterwards, the emulsion is broken by increasing ionic strength and the extracted PAEs are removed with separated soybean oil. The residual soybean oil and surfactants elevated the biodegradation rates of PAEs. In this pilot study, both weathered and fresh PAEs in sediment were tested and several different biological treatment schemes were tested, i.e., natural attenuation, anaerobic remediation, aerobic remediation, and sequential aerobic-anaerobic remediation. The optimum emulsion removal parameters are as follows: the ratio of emulsion to sediment (dry weight) at 1:0.84, the final concentration of sodium carbonate as emulsion breaker at 0.78 M, aeration rate at 4.0 L/min, aeration time at 30 min, and left-undisturbed period at 12 hours. Emulsion removal of fresh PAEs ranged from 60% to 70% while that of weathered PAEs ranged from 3% to 25% with an exception of benzyl-butyl phthalate at 77%. For the biological treatment, emulsion did enhance the biodegradation of PAEs.

第一章 緒論 1
1.1 研究起源 1
1.2 研究目的 2
第二章 文獻回顧 4
2.1塑化劑 4
2.1.1鄰苯二甲酸酯類(phthalate esters,PAEs) 4
2.2鄰苯二甲酸酯類使用情形 7
2.3鄰苯二甲酸酯類之暴露途徑與毒性 9
2.3.1鄰苯二甲酸酯類暴露途徑 9
2.3.2鄰苯二甲酸酯類濃度規範 11
2.3.3鄰苯二甲酸酯類毒性 14
2.4鄰苯二甲酸酯類之環境流布與宿命 17
2.4.1鄰苯二甲酸酯類之環境流布 17
2.4.2 鄰苯二甲酸酯類之宿命 24
2.5 鄰苯二甲酸酯類之處理技術 26
2.5.1 物理/化學處理與高級氧化法技術 26
2.5.2生物處理技術 29
2.6 底泥整治技術 33
2.6.1浚渫法 33
2.6.2水域掩埋 34
2.6.3水下掩埋 35
2.6.4現址加蓋處理 36
2.6.5自然回復 39
2.6.6深海棄置 40
2.7乳化液成分與製備介紹 42
2.7.1界面活性劑之介紹 43
2.7.2 HLB值(Hydrophilic-lipophilic balance) 48
2.7.3乳化液製備方式 50
2.7.4以乳化液回收底泥中有機物之整治技術 52
第三章 研究方法 54
3.1實驗設備 54
3.2實驗藥品 56
3.3實驗架構 58
3.4實驗方法 58
3.5模場試驗 59
3.5.1模場位置及設置 59
3.5.2模場組別及操作說明 60
3.5.3採樣方法 61
3.6高油量乳化液製備與操作 62
3.6.1乳化液製備 62
3.6.2破乳劑 63
3.6.3試驗操作條件之方法 64
3.6.4乳化液操作方式 65
3.7.1去活化中性氧化鋁配製 65
3.7.2去活化矽酸鎂配製 65
3.7.3 PAEs分析方法 66
3.8總菌數分析方法及藥品製備 67
3.8.1緩衝溶液製備 67
3.8.3總菌數分析方法 67
第四章 結果與討論 68
4.1整治復育材料與操作之最佳條件 68
4.1.1曝氣流量影響沉降速率與浮油回收速率 69
4.1.2曝氣時間影響沉降速率與浮油回收速率 71
4.1.3整治操作與微生物之影響 73
4.2模場試驗結果 75
4.2.1現場量測 75
4.2.2微生物生長情況 81
4.2.3污染物下降之情況 84
4.2.4污染物降解之成效 92
4.2.4乳化液污染物去除成效 95
4.2.6工程干預研析探討 105
第五章 結論與建議 110
5.1結論 110
5.2建議 112
參考文獻 113
附錄 133


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