臺灣博碩士論文加值系統

三氯乙烯具脂溶性、高蒸氣壓、高密度及低沸點等特性，常用於金屬脫脂、衣物乾洗等用途，並因長期使用而導致其累積於土壤及地下水中。微生物復育是處理地下水三氯乙烯污染方法之一。惟地下水三氯乙烯具一定毒性、會下滲、地下水環境微生物營養源及移動性受限，因此如何有效且可及地創造微生物復育環境，是快速處理地下水中三氯乙烯污染的關鍵議題。本研究將依需要開發浮/沉式生物粒料，定位地下水中三氯乙烯位置進行處理，並藉由保持顆粒結構完整，以利長期釋放營養源及馴化微生物，創造適宜生物復育環境，加速處理效率，研究目的包括：(1)評估三氯乙烯及其中間產物在地下水中流布、(2)確認生物粒料營養成分含量、微生物數量及是否調整其密度、(3)測試生物粒料處理地下水中三氯乙烯效率等。研究首先以小型模槽利用GC-FID分析三氯乙烯於模擬地下水中的流布，再利用所製造生物粒料處理地下水中三氯乙烯，最後利用GC-MS分析其中間產物流布情形。研究結果包括:(1)三氯乙烯分布需等待4個月達到平衡且各深度間無明顯濃度差異，而三氯乙烯的回收率約為51 ± 3%。後續分析生物粒料處理TCE期間中間產物分布，發現二氯乙烯(DCE)在管柱中與三氯乙烯有相同的濃度分布現象。(2)在馴養微生物階段反應速率常數最高達0.33 Day -1，且有發現二氯乙烯(DCE)及氯乙烯(VC)等中間產物。在活性測試方面則在植入高OD菌液濃度(VSS= 1.02 ± 0.03 mg/mL)有較佳的TCE去除率，期間最高反應速率常數為0.62 Day -1。(3) 生物粒料所使用的環保酵素每克含有410.4 ± 29.7 mg-TOC、9.1 ± 0.2 mg-TN、20.5 ± 0.7 mg-TP及K、Ca、Fe、Mg等金屬成分(不含重金屬)。而生物粒料可於水中維持約74天，其營養物質及金屬成分約74小時後達到平衡。(4)在管柱運行期間，使用含有馴化後TCE降解菌生物粒料在水面下10, 30及50 cm處其降解率比空白組多約63.5%。同上，在第74天發現有43.5%的TCE(1480 mg)揮發，沒有植種的TCE降解率最低，約為5%；而有植種的TCE降解率約為34%。

Trichloroethylene (TCE), characterized as lipid soluble, high vapor pressure and density, and low boiling point, is commonly used in metal cleaning and washing dry clothes, leading to soil and groundwater accumulation. Although bioremediation is an effective way in removing TCE, yet TCE’s toxicity, downward movement, and scarce growth nutrients limit the treatment efficiency of TCE in the groundwater. In this study, pellets, made with adjustable density for easy locating the TCE, allow long-term release of nutrients and acclimated TCE degraders, which creates a suitable remedial environment to speed up the TCE degradation. The objectives of this study include: (1) to assess the distributions of TCE and its degrading intermediates in groundwater, (2) to manufacture the TCE-degrading bio-pellets embedded with acclimated microbes and nutrients at controlled density if needed, and (3) to confirm the TCE removal efficiency of the groundwater using the multifunctional bio-pellets. Columns mimicking the groundwater were set up for monitoring the TCE distribution, bio-pellets were made, and TCE and its intermediates were analyzed over time using a GC-MS. The results showed that (1) It took about four months to reach a stable TCE distribution in columns with a recovery rate of 51 ± 3%, and the presence of bio-pellets resulting the observation of dichloroethylene in the liquid, (2) during the acclimation of TCE degraders, its degradation coefficient reached 0.33 day -1 with the presence of mono and dichloroethylenes, and the packed TCE degraders at VSS= 1.02 ± 0.03 mg/mL had highest degradation of coefficient at 0.62 day -1, (3) the self-made bio-pellet could stay in its pellet type for 74 days, and each gram of a bio-pellet contained 410.4 ± 29.7 mg-TOC, 9.1 ± 0.2 mg-TN, 20.5 ± 0.7 mg-TP, and some metals like potassium, calcium, iron, and magnesium. K、Ca、Fe、Mg, and (4) In the column runs, pellets with TCE degraders removed around 63.5% more TCE than the blank runs in depths of 10, 30, and 50 cm. On day 74, 43.5% of the spiked TCE (1480 mg in total) was volatilized, the control had minimal TCE degradation of around 5%, and the seeded one had about 34% of TCE degraded.

摘要 iv
Abstract vi
誌謝 viii
目錄 ix
表目錄 xii
圖目錄 xiv
符號對照表 xvii
第一章 研究緣起及目的 1
第二章 文獻回顧 3
2-1三氯乙烯及污染現況 3
2-1-1氯乙烯類化合物用途及其污染物來源 3
2-1-2氯乙烯類化合物暴露及毒性 5
2-1-3三氯乙烯基本特性 7
2-1-4國內外三氯乙烯地下水污染現況 10
2-2地下水三氯乙烯復育技術 15
2-2-1常用物化與生物復育技術介紹與選擇 15
2-2-2 微生物復育技術種類與選擇 28
2-2-3 影響造粒技術要素 33
2-3造粒技術與策略 35
2-3-1微生物的來源及馴化 35
2-3-2包埋材料的選擇 37
2-3-3粒料內容 39
2-3-4造粒目的與測試流程 40
第三章 實驗材料與方法 41
3-1研究架構與流程 41
3-2實驗藥品、材料及器材 43
3-2-1模擬地下水三氯乙烯污染及分析藥品 43
3-2-2 菌種培養的培養基配置 45
3-2-3 碳氮磷及重金屬分析藥品 47
3-2-4 生物粒料製作所需材料、藥品及流程(楊敦勝 2019) 49
3-2-5 實驗器材 51
3-3實驗相關儀器及設備 52
3-3-1氣相層析質譜儀(GC-MS) 52
3-3-2氣相層析儀-火焰離子偵檢器(GC-FID) 54
3-3-3總有機碳分析儀(TOC) 56
3-3-4紫外/可見光分光光譜儀 57
3-3-5感應耦合電漿原子發射光譜儀(ICP-AES) 58
3-3-6桌上型高速冷凍離心機 60
3-3-7造粒機 61
3-4 分析方法 62
3-4-1 地下水中三氯乙烯分析方法—頂空法及內標法 62
3-4-2生物粒料金屬檢測-王水消化法 63
3-4-3菌體細胞密度(OD)及營養鹽及分析方法 64
3-4-4 pH值測定 65
3-4-5 溶氧值測定 66
3-4-6三成分分析 67
3-5生物粒料碳氮磷釋放速率測試 68
3-6生物粒料菌體活性測試 68
3-7利用粒料處理地下水三氯乙烯污染 70
3-7實驗數據之QA/QC管制 71
3-7-1檢量線建立 71
3-7-2三重複數據 77
第四章 結果與討論 78
4-1管柱內三氯乙烯分布結果 78
4-1-1管柱內純三氯乙烯溶劑濃度分布分析 78
4-1-2管柱內三氯乙烯溶液(溶劑：乙醇)濃度分布分析 80
4-2 三氯乙烯降解菌馴化 83
4-2-1菌種培養第一階段馴化 83
4-2-2菌種培養第二階段馴化 85
4-3製造後生物粒料測試 89
4-3-1生物粒料於水中持續時間、營養鹽及金屬成分含量 89
4-3-2生物粒料於水中C/N/P及金屬離子釋放速率測試 90
4-3-3生物粒料於水中去除三氯乙烯活性測試 92
4-4利用生物粒料處理地下水三氯乙烯污染 97
4-4-1生物粒料處理三氯乙烯濃度變化 97
4-4-2生物粒料處理三氯乙烯期間中間產物濃度變化 100
4-4-3生物粒料處理三氯乙烯期間OD濃度、pH及DO變化 102
4-4-4生物粒料處理三氯乙烯期間C/N/P濃度變化 108
第五章 結論與建議 111
5-1結論 111
5-2建議 113
第六章 工程應用性 114
參考文獻 115
附錄A 原始數據 118
附錄B 口試委員提問及建議 142

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