臺灣博碩士論文加值系統

本研究係以氧氣做為奈米氣泡(Nanobubbles, NBs)產生源，開發新穎現地好氧生物整治技術；以NBs顆粒小、持久性高之特性，使其能擴散至傳統現地曝氣方式較難抵達之土壤孔隙中，營造適合地下好氧微生物生存之環境，促進降解污染物之效率。由模場試驗觀察現地環境微生物菌群變化及污染物降解率，評估技術可行性。
實驗室試驗利用玻璃管柱填入石英砂介質，模擬高溶氧水於地下環境觀察時間推移溶氧(Dissolved oxygen, DO)的變化量；根據管柱試驗結果顯示高溶氧水滯留於介質中24小時便下降至原溶氧濃度之33 %－37 %，而後衰退量趨緩。砂箱試驗以一長方箱體模擬地下環境，結果發現NBs因傳輸過程中撞擊介質而消散，能夠得知在介質中溶氧濃度受距離及滯留時間所影響。
模場試驗建置於一石化業場址，共設置2口監測井(MW1、MW2)及3口灌注井(GW1、GW2、GW3)，於每週進行一次水質參數監測，每個月進行一次採樣分析目標污染物(苯、甲苯、乙苯、苯乙烯)，灌注初期微生物菌群半年分析一次，爾後每月一次。高溶氧水灌注頻率試驗分別為8 hr/day、12 hr/day及24 hr/day，每個頻率執行約一個月，溶氧提升效果以24 hr/day較佳，平均能使監測井溶氧濃度上升至12.6 mg/L－14.2 mg/L，其次則為12 hr/day及8 hr/day，其中，溶氧提升效果主要取決灌注高溶氧水之體積及監測井與灌注井之間的距離。但研究過程發現24 hr/day灌注頻率可能稀釋或干擾微生物生長、設備所需電力及氧氣成本提高，根據實驗室試驗中高溶氧水在24小時後溶氧濃度才會大幅下降，故後續油品分解菌添加試驗使用12 hr/day之頻率灌注，以維持地下好氧環境。執行高溶氧水灌注試驗後，各口井之微生物種類數均呈上升趨勢，其中Pseudomonas、Cloacibacterium、Sphingobium、Enterobacter、Magnetospirillum之菌屬，根據前人文獻資料顯示在上述模場中所鑑別出來的菌屬皆有降解油品能力，故灌注高溶氧水能顯著改變地下環境，促進好氧微生物菌群生長。比對背景調查及灌注一年後採樣分析結果顯示，土壤苯之去除率為59.2 %－99.9 %，乙苯為77.4 %－99.8 %；地下水苯之去除率為93.9 %－100 %，乙苯為84.5 %－99.9 %，其濃度大幅下降，顯現灌注高溶氧水的成效。

Nanobubble (NBs)technologies have drawn great attention due to their wide applications in watertreatment, biomedical engineering, and nanomaterials in recent years. Use ofoxygen saturated NBs would have great potential implication in soil andgroundwater remediation due to their extremely high bioactivity and masstransfer efficiency. The objective of this study is to develop the use of NBsin petroleum hydrocarbon contaminated site to enhance bioremediation. 
Laboratory experimentswere conducted to investigate flow of discrete microbubbles through awater-saturated porous medium by column and sand box experiments in this study.NBs was release from a diffuser, move upward through a column filled withpacked soil. Outflowing bubbles were collected for flux measurements. Theresults of column experiments indicated that loss of dissolved oxygen (DO) inair-saturated water was about 1 mg/L after 72 hours. After 120 hour ofretention time in the packed column, loss of DO in air-saturated water wasabout 1.90 mg/L. Vertical columns tended to retain oxygen for longer time thanthe horizontal setting. Dissolved oxygen was measured to be 40.9 mg/L afternano-scale oxygen bubble was produced for 30 min. Longer exposure time did notsignificantly increase the level of DO. Dramatic depletion of DO from 27 mg/Lto 10 mg/L was observed in the first 24 hours of the column experiment. Afterthe time period, the depletion was slow down. After 120 hours, DO wasmaintained higher than saturated water of room temperature. Forty percent of DOdepletion was observed after 96 hours in the sand box experiment. However, thedepletion tended to be slower between 4 to 16 days. 
Test zone with injectionand extraction wells were designed and employed in a petroleum hydrocarboncontaminated site in Kaohsiung. Injection of NBs was conducted in the test zonewith three injection wells and two monitoring wells. Injection of oxygen-supersaturatedwater was 8 hours per day in the first month. It was increased to 12 hours perday in the second months. Finally, continuous injection of 24 hours wasperformed. After the long term practice, injection of oxygen-supersaturatedwater of 12 hours was recommended because the whole day injection of oxygen-supersaturatedwater may potentially dilute the dissolved phase contaminants and dilute thepopulations of microorganisms in the subsurface environment. 
Groundwater monitoringof pH, dissolved oxygen, nutrients and change of population/diversity ofmicroorganisms was performed. Retention time of NBs, concentration of dissolvedoxygen, and change of petroleum degrading bacteria species was observedmonthly. 
After the one yearinjection practice of oxygen-supersaturated water, the apparent concentrationsof target contaminants were declined. Benzene was reduced from 198 to 266 mg/Lto not detectable to 15.1 mg/L. Though concentration of ethylbenzene ingroundwater decreased from 5398 mg/L to 1.25 639 mg/L, it remained the majorcontaminant. The degradation mechanism is unclear due to potential impact ofdilution of groundwater by injection or high rate of biodegradation. 
It was anticipated thatfunctions of enhanced bioremediation can be achieved through injection andcirculation of NBs by field practices. The results of microorganism diversityindicated that bacteria species tended to increase with long term injection of oxygen-supersaturatedwater. Petroleum-degrading bacteria (Enterobactertabaci) was applied in the site for enhanced bioremediation. Theconcentrations of target contaminants were decreased. This study served forfuture investigations to employ nanobubbles in the field of soil andgroundwater remediation.

第一章前言1
1.1 研究動機1
1.2 研究目的3
第二章文獻回顧4
2.1 目標污染物於地下環境中之特性4
2.2 生物整治技術7
2.2.1 整治方法介紹7
2.2.2 影響生物整治之環境因子10
2.3 微生物降解油品碳氫化合物之途徑12
2.4 奈米氣泡14
2.4.1 奈米氣泡之特性14
2.4.2 奈米氣泡之產生原理14
2.4.3 奈米氣泡之應用16
第三章材料方法18
3.1 研究架構18
3.2 實驗材料19
3.2.1 供試藥品19
3.2.2 試驗添加菌種20
3.3 實驗設備及分析方法21
3.3.1 高溶氧水製造設備21
3.3.2 水質參數量測22
3.3.3 目標污染物分析22
3.3.4 營養鹽分析23
3.3.5 微生物菌群分析23
3.3.6 地下水採樣方法24
3.3.7 土壤採樣方法24
3.4 實驗品保/品管25
3.5 實驗室試驗27
3.5.1 管柱試驗27
3.5.2 砂箱試驗27
3.6 場址介紹及模場規劃30
3.6.1 場址現況及環境特性30
3.6.2 場址水文資訊30
3.6.3 場址地質資訊31
3.6.4 模場試驗33
3.6.5 高溶氧水頻率灌注試驗34
3.6.6 油品分解菌添加試驗34
3.6.7 地下水水質監測及土壤地下水採樣頻率35
3.7 土壤地下水背景資料建立36
第四章結果與討論43
4.1 溶氧水之管柱試驗43
4.1.1 飽和溶氧水之溶氧變化43
4.1.2 高溶氧水之溶氧變化45
4.2 高溶氧水之砂箱試驗47
4.3 模場試驗之高溶氧水灌注頻率試驗50
4.3.1 地下水溶氧濃度及氧化還原電位變化50
4.3.2 地下水pH值變化53
4.3.3 地下水導電度變化55
4.3.4 地下水營養鹽濃度變化56
4.3.5 地下水目標污染物濃度變化58
4.3.6 地下水微生物菌群變化62
4.4 油品分解菌添加試驗65
4.4.1 地下水微生物菌群變化65
4.4.2 地下水溶氧濃度及氧化還原電位變化72
4.4.3 地下水pH值變化74
4.4.4 地下水導電度變化75
4.4.5 地下水營養鹽濃度變化76
4.4.6 地下水目標污染物濃度變化78
4.5 土壤目標污染物濃度變化82
4.6 高溶氧水成效評估85
4.6.1 實驗室試驗85
4.6.2 高溶氧水灌注頻率試驗85
4.6.3 油品分解菌添加試驗86
第五章結論與建議87
5.1 結論87
5.2 建議88
參考文獻89


圖 2 1 生物通氣法示意圖8
圖 2 2 土耕法示意圖9
圖 2 3 生物堆法示意圖9
圖 2 4 苯環降解途徑示意圖13
圖 2 5 氣泡、微米氣泡及奈米氣泡於水體環境中之變化15
圖 2 6 溶氧提升能力比較16
圖 3 1 實驗架構圖18
圖 3 2 菌種鑑定報告20
圖 3 3 高濃度氣體溶解裝置21
圖 3 4 管柱試驗示意圖29
圖 3 5 砂箱示意圖29
圖 3 6 場址平面圖31
圖 3 7 場址壤心剖面圖32
圖 3 8 模場試驗井場示意圖33
圖 3 9 Group A與Group B地下水中菌種同異之文氏圖40
圖 3 10 土壤背景調查採樣佈點位置(第一次土壤採樣)41
圖 4 1 溶氧在滯留管柱中不同時間之變化44
圖 4 2 溶氧在滯留管柱中不同時間之變化46
圖 4 3 高溶氧水傳輸於砂箱中濃度變化及衰退率48
圖 4 4 溶氧在砂箱中濃度變化48
圖 4 5 高溶氧水滯留於砂箱中溶氧濃度之衰退率49
圖 4 6 灌注頻率試驗期間之模場地下水溶氧濃度及氧化還原電位變化52
圖 4 7 灌注頻率試驗期間之模場地下水pH值變化54
圖 4 8 灌注頻率試驗期間之模場地下水導電度變化55
圖 4 9 灌注頻率試驗期間之模場地下水營養鹽及氧化還原電位變化57
圖 4 10 灌注頻率試驗期間之模場地下水苯濃度變化60
圖 4 11 灌注頻率試驗期間之模場地下水甲苯濃度變化60
圖 4 12 灌注頻率試驗期間之模場地下水乙苯濃度變化61
圖 4 13 灌注頻率試驗期間之模場地下水苯乙烯濃度變化61
圖 4 14 油品分解菌添加試驗期間之模場地下水溶氧濃度及氧化還原電位變化73
圖 4 15 油品分解菌添加試驗期間之模場地下水pH值變化74
圖 4 16 油品分解菌添加試驗期間之模場地下水導電度變化75
圖 4 17 油品分解菌添加試驗期間之模場地下水位變化及日降雨量76
圖 4 18 油品分解菌添加試驗期間之模場地下水營養鹽及氧化還原電位變化77
圖 4 19 油品分解菌添加試驗期間之模場地下水苯濃度變化79
圖 4 20 油品分解菌添加試驗期間之模場地下水甲苯濃度變化80
圖 4 21 油品分解菌添加試驗期間之模場地下水乙苯濃度變化80
圖 4 22 油品分解菌添加試驗期間之模場地下水苯乙烯濃度變化81
圖 4 23 第一次及第二次土壤採樣佈點位置83


表 2 1 國內土壤及地下水污染監測及管制標準值5
表 2 2 目標化合物之物化特性6
表 3 1 灌注井及監測井基本資料34
表 3 2 地下水背景調查資料37
表 3 3 模場地下水微生物菌群背景調查資料38
表 3 4 土壤背景調查資料42
表 4 1 灌注頻率試驗期間之模場地下水微生物菌群分析資料64
表 4 2 油品分解菌添加試驗期間之模場地下水微生物菌群分析資料67
表 4 3 第二次土壤採樣目標污染物分析結果84

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