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研究生:黃威翔
研究生(外文):Wei-Hsiang Huang
論文名稱:以加強式硫酸鹽還原法處理受石油碳氫化合物污染之地下水
論文名稱(外文):Application of Enhanced Sulfate Reduction Method to Remediate Petroleum-hydrocarbon Contaminated Groundwater
指導教授:高志明高志明引用關係
指導教授(外文):Chin-Ming Kao
學位類別:博士
校院名稱:國立中山大學
系所名稱:環境工程研究所
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:140
中文關鍵詞:緩釋合成物石油碳氫化合物加強式生物復育地下水污染硫酸鹽還原
外文關鍵詞:groundwater contaminationsulfate reductionpetroleum hydrocarbonreleasing materialsenhanced bioremediation
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由於石油碳氫化合物被廣泛運用,造成土壤地下水受油污染是一個普遍且嚴重的問題,其污染物以非水相溶液(non-aqueous phase liquids, NAPLs)存在地下水中,對地下水之水質可能造成長期的危害,廣泛於汽油中添加劑甲基第三丁基醚(methyl tertiary-butyl ether, MTBE)及汽油中主要成分苯(benzene)及甲苯(toluene),以上三種化合物在石油碳氫化合物中水溶性相對較高,因此當受油品污染該些物質於地下水中溶於水傳輸性較佳,在加上benzene具致癌性及MTBE具有對動物致癌性,當意外洩漏時對人類健康及環境具有嚴重危害。本研究以MTBE、benzene及toluene作為目標污染物,並發展主動及被動加強式硫酸鹽還原方法,以有效處理石油碳氫化合物污染之地下水。本研究針對緩釋合成物進行配比設計及釋放實驗瞭解釋放效果;微生物批次及管柱實驗瞭解微生物降解能力,並結合變性膠體電泳(denaturing gradient gel electrophoresis, DGGE)及定序技術進行菌種鑑定以瞭解其功能及特性。研究結果顯示微生物批次實驗結果自然衰減組初期會消耗溶氧進行好氧反應,當還原電位低於-150 mV會啟動硫酸鹽還原作用。硫酸鹽還原基質組確實可刺激微生物生長,對Toluene、Benzene及MTBE降解效率分別為90%、63%及8%,但隨基質的消耗及硫化物生成,會產生抑制現象。硫酸鹽還原基質添加二價金屬組,Toluene及Copper,降解效率分別99及100%,二價銅與硫化物產生硫化物銅生物沉澱,並能降低硫化物對微生物之毒性。緩釋合成物實驗結果澱粉組S-B1(-1.46×10-2)、稻殼組R-B3(-2.18×10-2),釋放總量超過70%,釋放時間較長,且釋放速率穩定。管柱實驗現地土壤對污染物吸附作用為Toluene>Benzene>MTBE。主動加強式管柱實驗降解效率Toluene、Benzene及MTBE第一階段(92%、65%及45%),衰減率分別為(34.24、1.75及1 d-1)第二階段(64%、52%及40%),衰減率分別為(1.34、1.14及0.95 d-1),隨著二價鐵的消耗,及硫化物大量的生成累積,造成為生物受到抑制,因而降低對污染物去除效率,定序鑑定出39種菌株,包含具有降解芳香烴及以硫酸鹽還原方式降解石油碳氫化合物之功能。被動加強式管柱實驗Toluene、Benzene及MTBE第一階段(96%、69%及36%),衰減率分別為(5.74、2.08及0.78),第二階段(90%、61%及22%),衰減率分別為(4.05、1.70及0.43),緩釋合成物主要為聚乳酸及稻殼粉組成其具有吸附作用能於初期聚集污染物,隨著硫酸鹽濃度的減少微生物對污染物的降解會有減緩或停滯。在硫酸鹽還原條件下,Toluene是較Benzene及MTBE更易被生物降解。案例設計目標廠址Toluene污染總量為59.8 kg,,其共需提供86.4 kg硫酸鹽,依攔阻日通量計算0.52 kg/ day,每日硫酸鹽投藥量為2.46 kg,共需花費36天進行整治。以最佳釋出效率之組別R-B3 (2.8 mg of SO4/day/g material)共需提供 879 kg 之緩釋硫酸鹽合成物於9口井。結果顯示硫酸鹽還原方法為一個環境和經濟上可接受的修復技術。整治方案預計將提供一個更具成本效益的替代修復受石油烴污染之地下水。從這項研究中獲得的知識將有助於規劃硫酸鹽還原系統現場整治。
Groundwater at many existing or former industrial areas and underground storage tank sites is contaminated by petroleum hydrocarbons. The purpose of this study was to develop a passive enhanced sulfate reduction system to treat the methyl tertiary-butyl ether (MTBE), benzene, and toluene contaminated groundwater. A sulfate-releasing material was developed for long-term sulfate releasing for sulfate supplement. Microcosm study was performed to evaluate the contaminants (e.g., MTBE, benzene, toluene) removal efficiency under sulfate reducing conditions. A column experiment was applied to evaluate the effectiveness and mechanisms of sulfate reduction processes on the bioremediation of benzene, toluene, and MTBE contaminated groundwater. The denaturing gradient gel electrophoresis (DGGE) and DNA sequencing methods were also applied to determine the microbial diversity and dominant bacteria under sulfate reducing conditions. Results from the microcosm study show that the ORP dropped to below -150 mv after initial oxygen consumption. Sulfate reduction was activated when the oxidation-reduction stage reached anaerobic conditions. Results show that the removal efficiencies for toluene, benzene, and MTBE were 90, 63, and 8%, respectively. The sulfate reduction process was inhibited after the sulfate was consumed. The production of sulfide also caused the inhibition of the sulfate reduction process. In the experiment with Cu(II) addition, the removal efficiencies for toluene and Cu(II) were 99 and 100%, respectively. Results also show that the formation of Cu precipitate was observed due to the reaction of Cu and sulfide. This would result in the reduction of toxicity effect caused by the sulfide. In the sulfate releasing experiment, the sulfate release rates were -1.46×10-2 and -2.18×10-2 in starch and rice husk groups, respectively. The total amount of sulfate release reached 70%. In the column experiment with sulfate addition, simulated anaerobic groundwater containing benzene, toluene, and MTBE (average concentration = 20 mg/L) was pumped into the system at a flow rate of 0.36 mL/min. Sulfate (used as the electron acceptor) was injected into the system to activate the sulfate reducing process. Anaerobic sludge collected from an anaerobic basin of an industrial wastewater treatment plant was inoculated into the system to enhance the sulfate reduction rate. Up to 92, 65, and 45% of toluene, benzene, and MTBE removal efficiencies were observed with the first-order decay rate of 34, 1.8, and 1 1/d, respectively. Results indicate that toluene is more biodegradable under sulfate reducing conditions compared to benzene and MTBE, and 0.7 g/L of sulfate consumption was observed during the biodegradation process. The occurrence of sulfate reduction can be confirmed by the increased sulfide (increased from 7 - 9 to 340 - 520 mg/L) and ferrous iron (increased from <0.1 to 52 mg/L then dropped to 0.14 mg/L due to the formation of iron sulfide) concentrations. In the latter part of this study, accumulation of hydrogen sulfide caused the microbial inhibition, and thus, decreased contaminant removal efficiencies were observed. The microbial communities were characterized by 16S rRNA-based DGGE profiling for soils in the system. Results show that sulfate addition could result in the enhancement of sulfate reducer growth, and thus, sulfate reduction became the dominant biodegradation process. A total of 39 different petroleum-hydrocarbon degrading bacteria were observed under the sulfate-reducing conditions. Results indicate that the sulfate reduction has the potential to be developed into a practically and economically acceptable technology to remediate petroleum-hydrocarbon contaminated groundwater.
謝誌.. i
中文摘要 ii
Abstract iv
目錄.. vi
圖目錄 ix
表目錄 xi
一、 前言 1
1.1 研究緣起 1
1.2 研究目的 3
1.3 研究內容 4
二、 文獻回顧 5
2.1 土壤地下水油品污染概況 5
2.1.1 MTBE特性與危害 5
2.1.2 BTEX特性與危害 6
2.2 土壤及地下水整治技術 8
2.2.1 整治技術發展 8
2.2.2 綠色整治技術 9
2.2.3 生物降解 10
2.3 硫酸鹽還原理論 12
2.3.1 自然生物復育中的硫酸鹽還原 18
2.3.2 加強式硫酸鹽還原方法 18
2.3.3 硫酸鹽還原相關案例 20
2.3.4 使用硫酸鹽加強生物復育技術之優勢 23
2.4 透水性反應牆 25
2.4.1 控制釋放技術的發展 27
2.4.2 生物可分解之高分子材料的發展 28
2.5 分子生物在地下水生物復育之應用 29
2.5.1 以16S rDNA為基礎之分子生物技術 31
2.5.2 生物指標(microbial biomarker) 32
三、 實驗設備與方法 34
3.1 材料與方法 34
3.2.1 實驗藥品及材料 34
3.2.2 實驗器材 34
3.2.3 實驗用水 34
3.2.4 供試土壤來源 35
3.2.5 供試地下水來源 37
3.2.6 緩釋控制釋放物質 37
3.2 實驗方法 40
3.3.1 微環境實驗 (microcosm) 40
3.3.2 管柱試驗 41
3.3.3 實驗分析方法 44
四、 結果與討論 51
4.1 微生物批次試驗 51
4.1.1 自然衰減組 52
4.1.2 硫酸鹽還原基質組 55
4.1.3 硫酸鹽還原基質添加二價金屬組 59
4.1.4 批次實驗生物沉澱分析 62
4.1.5 菌相分析結果 64
4.2 緩釋合成物 65
4.2.1 緩釋合成物配比設計 65
4.2.2 緩釋物質批次試驗 66
4.3 主動加強式管柱實驗 80
4.3.1 管柱土壤污染物濃度累積試驗 80
4.3.2 管柱水質基本性質分析 82
4.3.3 管柱污染物分析 88
4.3.4 管柱菌相分析 92
4.4 被動加強式管柱實驗 98
4.4.1 管柱水質基本性質分析 98
4.4.2 管柱污染物分析 102
4.5 案例設計規劃與緩釋硫酸鹽合成物添加量估算 105
五、 結論與建議 108
5.1 結論 108
5.2 建議 110
參考文獻 111
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