三氯乙烯(trichloroethylene, TCE)和四氯乙烯(perchloroethylene, PCE)為常見之地下水污染物，而且由於常以重質非水相型式存在，故往往難以整治。本研究之目的為發展一種可緩慢釋放碳源及營養物質之基質，用以加速TCE之生物降解。本研究中所設計合成之基質以結合蔬菜油、台糖二級砂糖及生物可分解界面活性劑(Simple Green和卵磷脂)，使蔬菜油乳化為較易擴散之乳化型基質，以期能長期提供微生物好氧共代謝或厭氧還原脫氯所需之碳源。本研究項目包括好氧及厭氧微生物批次試驗(好氧組包含單純地下水、乳化型基質、生物可分解界面活性劑及營養基質；厭氧組包含單純乳化型基質、富硝酸鹽及富硫酸鹽組)及利用基因分析法與菌相鑑定評估生物整治之處理成效。卵磷脂、Simple Green、台糖二級砂糖、綜合維他命及乳化型基質可在氧氣存在下，進行共代謝作用，當氧氣耗盡後，可加強厭氧降解。然而綜合維他命雖可促進微生物生長，但無法有效提升微生物活性，因此無法單獨作為好氧共代謝TCE之碳源。另外，卵磷脂及砂糖經微生物代謝後易產生有機酸，造成pH值下降，當環境之pH值偏酸性時，會抑制微生物生長，因而造成TCE降解發生延遲。現地地下水(無基質)、卵磷脂、Simple Green、綜合維他命、台糖二級砂糖及乳化型基質之好氧降解比率依大小之分可得Simple Green>台糖二級砂糖>卵磷脂>綜合維他命>乳化型基質>現地地下水(無基質)。由厭氧批次試驗得知，乳化型基質可有效促進還原脫氯反應產生，使TCE降解。當環境中硝酸鹽濃度過高時，可能會延緩乳化型基質產氫，進而延遲TCE還原脫氯作用；反應環境若處於富硫酸鹽狀態時，亦能持續產氫刺激脫氯菌進行還原脫氯作用。解比率依大小之分可得乳化型基質組>富硫酸鹽組>富硝酸鹽組>現地地下水(無基質)。由基因評估法得知，於卵磷脂組、Simple Green組、台糖二級砂糖組及乳化型基質組可測得phenol monooxygenase、toluene monooxygenase及toluene dioxygenase之基因，因此可有效針對微生物進行誘發酵素降解TCE的潛能。乳化型基質在單純乳化型基質及乳化型基質於富硝酸鹽和富硫酸鹽下皆可有效刺激Dehalococcoides菌群誘發生成tceA、bvcA及vcrA等還原脫氯酵素。

Trichloroethene (TCE) and tetrachloroethene (PCE) are among the most commonly detected groundwater contaminants, and are often difficult to remediate due to their presence as dense non-aqueous phase liquids (DNAPLs) in the subsurface. The objective of this study was to assess the potential of using a passive in situ carbon/hydrogen releasing barrier system to bioremediate TCE-contaminated groundwater. The slow carbon/hydrogen releasing material would cause the aerobic cometabolism and reductive dechlorination of TCE in aquifer. The carbon/hydrogen releasing materials would release carbon when contacts with groundwater and release hydrogen after the anaerobic biodegradation of released carbon, thus cause the reductive dechlorination of TCE. Results from the microcosm study indicate that the addition of emulsified substrate, cane molasses, Simple GreenTM (a biodegradable surfactant), or lecithin would enhance the biodegradation rate of TCE under anaerobic conditions. However, addition of multivitamin would increase the bacterial population in the media but would not be able to enhance the TCE degradation rate. Results show that a significant pH drop was observed due to the production of organic acids after the aerobic biodegradation process of cane molasses and lecithin. This also caused the inhibition of microbial growth in microcosms. Results reveal that higher TCE removal efficiency was observed in microcosms with Simple GreenTM addition followed by the addition of cane molasses, lecithin, multivitamin, emulsified substrate, groundwater (without substrate addition). Results from the microcosm study indicate that the addition of emulsified substrate would enhance the biodegradation rate of TCE under anaerobic conditions. However, appearance of high nitrate concentration would inhibit the TCE degradation process due to the occurrence of denitrification. Compared with nitrate, high sulfate concentration would not have significant impact on the reductive dechlorination of TCE. Results reveal that higher TCE removal efficiency was observed in microcosms with emulsified substrate addition followed by the addition of high sulfate concentration, high nitriate concentration, groundwater (without substrate addition). Results from the gene analysis show that phenol monooxygenase, toluene monooxygenase, and toluene dioxygenase were observed in the microcosms with lecithin, cane molasses, Simple GreenTM, and emulsified substrate. This indicates that the addition of substrates would induce the potential of TCE-degrading enzyme. Addition of emulsified substrate and emulsified substrate in nitrate or sulfate-rich media would stimulate Dehalococcoides sp. to induce tceA, bvcA, and vcrA, enzymes for TCE reductive dechlorination.

謝誌 I
摘要 III
Abstract V
表目錄 IX
圖目錄 XI
第一章 前言 1
1.1 研究緣起 1
1.2 研究目的 2
第二章 文獻回顧 3
2.1 含氯有機物之相關特性 3
2.1.1 地下水氯化乙烯類化合物污染的來源 3
2.1.2 TCE之性質、用途及對人體的危害 5
2.1.3 TCE之傳輸行為 11
2.2 地下水污染整治技術之種類 13
2.2.1 綠色整治技術 13
2.2.2 現地生物復育技術 14
2.3 利用乳化油進行現地生物復育之類似場址回顧 33
第三章 實驗與方法 35
3.1 研究流程 35
3.2乳化型基質的合成 37
3.3 微生物批次試驗 40
3.3.1 好氧共代謝降解TCE實驗 40
3.3.2 還原脫氯降解TCE實驗 43
3.4 實驗設備與材料 49
3.4.1 實驗材料 49
3.4.2 實驗設備 50
3.5 分析方法 50
3.5.1 污染物分析 50
3.5.2 水質分析 51
3.5.3 生物性分析 53
第四章 結果與討論 63
4.1 油/水對TCE分配係數 63
4.2 微生物好氧批次試驗 65
4.2.1 現地地下水組 67
4.2.2 界面活性劑組 69
4.2.3 營養基質組 74
4.2.4 乳化型基質組 78
4.2.5 各基質好氧共代謝降解比較 80
4.3 微生物厭氧批次試驗 82
4.3.1 現地地下水組 83
4.3.2 乳化型基質組 85
4.3.3 富硝酸鹽組 89
4.3.4 富硫酸鹽組 92
4.3.5 各基質厭氧共代謝降解比較 97
4.4 好氧/厭氧菌群及酵素評估 99
第五章 結論與建議 117
5.1 結論 117
5.2 建議 119
參考文獻 121

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