在過去受重金屬污染之六價鉻整治場址調查中發現，含水層中鉻污染主要源自工業廢水及有害廢棄物不當棄置所造成，六價鉻具有致癌性且因其所帶電荷性質與土壤相同，進而造成其在含水層之高移動性，而六價鉻污染物具有強氧化性，因此容易影響地下水含水層中之還原區間，故在整治工程上較不容易處理。近年來許多國內外學者致力於相關研究，利用微生物還原代謝之機制將污染物還原降解，且透過微生物分解土壤或地下水中之污染物，對於場址破壞性較小，可經由添加基質來增加其碳源濃度，透過提高碳源刺激微生物菌群生長進而加強生物整治成效，因此可透過現地加強式厭氧生物整治技術，針對長期受六價鉻污染地下水，推動生物還原且符合經濟之綠色整治技術。國內受地形(河流沖積扇及山勢)影響，使部分地區地下水含水層中呈現流速較快之情形，造成整治時所投入之整治藥劑因傳輸性高較易流失而提高整治成本，因此提高整體整治困難；本研究目的為研發綠色變性膠體緩釋材，其特性在於灌注後複合型膠體能形成一個介於固體與液體之間的特殊形態，膠體於含水層土壤孔隙中形成膠凝顆粒，增加此材料滯留與接觸污染物面積，可利用凝膠基質表面之官能基進行吸附及釋放碳源供微生物利用，同時凝膠基質所形成之三維立體網狀結構，亦可提供微生物附著提升整治效益。本研究先針對綠色變性膠體緩釋材進行基本特性分析，接著進行前導試驗及流通性測試，評估適用於土壤地下水之最佳化膠體緩釋材配比，另一方面，本研究利用凝膠基質組、凝膠結合糖蜜組及直接添加糖蜜組分別進行管柱實驗，模擬各組基質在含水層中各項水質參數、六價鉻還原去除、總鉻變化與分布之情形進行探討，最後通過次世代定序(next generation sequencing, NGS)分析技術結合即時定量聚合酶連鎖反應(real-time polymerase chain reaction, real-time PCR)於管柱實驗中進行菌相分析瞭解特徵基因和優勢菌之變化，以利後續現地整治應用。本研究之凝膠基質各配比經強度測試之結果顯示，當明膠濃度維持在3%且瓊脂濃度為0.5%時具有較佳之效果，當藥劑注入時可順利於土壤孔隙間形成膠羽顆粒增加地下水污染物與藥劑接觸面積。由管柱實驗結果顯示，凝膠基質於注入後pH範圍為pH 7.4至pH 7.5之間呈現中性，得知管柱內透過凝膠基質可緩衝受六價鉻污染水體pH值酸化及實驗後期基質發酵產生有機酸而抑制微生物生長問題；管柱實驗在凝膠基質添加後，實驗第四至五天內六價鉻濃度及呈現明顯下降趨勢，在實驗第十天後平均濃度低於0.1 mg/L，在此同時溶液中總鉻亦呈現明顯下降趨勢，其在管柱實驗後期平均濃度低於0.1 mg/L皆低於地下水污染管制標準。透過次世代定序分析管柱內土壤菌相結果得知，於初始組別中具功能性微生物比例為34.65%，而透過糖蜜基質添加後促進管柱內功能性微生物比例提升至89.38%，透過糖蜜基質添加之管柱組別，主要優勢菌種為Sporolactobacillus，通過代謝後可產生乳酸鹽，能提供其它微生物利用，並促進六價鉻生物整治還原之成效。結合上述結果得知，本研究所研發之綠色變性緩釋膠體，除了能夠有效控制pH值、穩定持續提供碳源供微生物利用、濃縮六價鉻於膠體成膠區及固定糖蜜基質於目標污染區域，延長糖蜜於灌注區之滯留時間，因此以綠色變性膠體緩釋材生物整治受六價鉻污染地下水具備創新研發、環境友善、與土水整治技術發展潛能。

Heavy metal hexavalent chromium remediation of contaminated sites survey found that in the past, the main aquifer chromium contamination from industrial waste and hazardous waste caused by improper disposal, hexavalent chromium is carcinogenic and its electric charge and the nature of the soil same. This in turn results in high mobility in the aquifer. And hexavalent chromium having strong oxidizing contaminants, and therefore susceptible to the reduction in the aquifer interval, it is more difficult to handle on a renovation project. In recent years, many scholars dedicated to research, the use of microbial metabolic reduction mechanism of the reduction of pollutant degradation and decomposition of contaminants in the soil or groundwater through microbes, for sites less destructive, it can be increased by the addition of substrate concentration of carbon source, by raising the carbon source to stimulate the growth of microbial flora thereby strengthening the effectiveness of bioremediation. Therefore enhance anaerobic bioremediation technology through to now, for the long-term by hexavalent chromium contaminated groundwater, promote bio-economy in line with the reduction and green remediation technologies. Domestic terrain (mountains and river alluvial fan) affect the parts of the aquifer in the case showed faster the flow rate, resulting in improvement of the drug into the time of remediation due to high transmission losses and improve remediation costs more easily, thus improving the overall Remediation difficulties. Purpose of this study for the development of green denatured colloidal release material, wherein the perfusion characteristics thereof capable of forming a complex colloidal special form interposed between the solid and the liquid. Colloidal particles form a gel in soil pore water layer, this increased area of exposure to contaminants and material retention may be utilized functional groups of the surface of the substrate gel adsorption and release of carbon sources by microorganisms, while the gel matrix formed of three-dimensional a mesh structure, may also be provided to enhance microbial adhesion remediation efficiency. In this study, the basic characteristics of the green modified colloidal release material were first analyzed, followed by the lead test and the flow test to evaluate the optimal colloidal release material ratio suitable for soil groundwater. On the other hand, the study used the gel matrix. The tube-column experiments were carried out in the group, the gel-bound molasses group and the directly added molasses group. The water quality parameters, hexavalent chromium reduction and total chromium change and distribution of the matrix in each group were simulated. Finally, in column experiments with bacteria analyzed to understand the characteristics and advantages of the bacteria by the next generation of gene sequencing (next generation sequencing, NGS) for real time binding analysis by quantitative polymerase chain reaction (real-time polymerase chain reaction, real-time PCR) the changes to facilitate subsequent current remediation applications. The results of the strength tests of the gel matrix of the present study showed that the gelatin concentration was maintained at 3% and the agar concentration was 0.5%. When the pharmaceutical injection can be smoothly formed floc particles and an agent to increase the groundwater contaminants to the contact area between the soil pore. The results shown by the column, the gel matrix after injection to render a neutral pH range between pH 7.4 to pH 7.5, hexavalent chromium contaminated water that was acidified and pH of the gel matrix may be post-experimental buffer through the column by matrix organic acid fermentation inhibiting the growth of microbiological The development of this study denaturation green colloid release, in addition to effectively control the pH value, providing a carbon source for microbial stable for use, and concentrated to hexavalent chromium and colloidal gel-forming region is fixed to the target matrix molasses contaminated area, the extension region perfusion molasses the residence time, so green colloid degeneration slow-release material bioremediation of groundwater contaminated by hexavalent chromium with innovative research and development, environment-friendly, water and soil remediation technology development potential.

目錄
論文審定書 i
論文公開授權書 ii
謝誌 iii
摘要 iv
Abstract vi
目錄 ix
圖目錄 xii
表目錄 xiii
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 4
2.1地下水受鉻污染之概況 4
2.2六價鉻污染物的物化特性 6
2.3鉻污染對人體的危害 10
2.4重金屬的物理整治技術 11
2.5重金屬的化學整治技術 17
2.6重金屬的生物整治方法 19
2.6.1六價鉻生物還原 19
2.6.2常見的鉻酸鹽還原菌 20
2.7六價鉻經還原後化合物介紹 25
2.8阻斷型緩釋膠體基質載體之特性介紹 27
2.9次世代定序(NGS)分析技術與總體基因體學(Metagenomics)發展與應用 34
第三章 實驗材料與方法 37
3.1研究流程 37
3.2實驗材料 39
3.2.1實驗藥品 39
3.3實驗儀器與設備 39
3.4實驗設計 40
3.4.1膠體基質配比前導試驗 40
3.4.2 凝膠材料緩釋/阻隔六價鉻實驗 41
3.4.3微生物管柱實驗 41
3.5實驗基質材料分析 42
3.6基本水質分析 43
3.7次世代定序(NGS)分析 46
第四章 結果與討論 48
4.1膠體基質強度配比測試 48
4.2微生物管柱實驗 50
4.3管柱實驗組別DO、pH and ORP 50
4.4管柱內水樣總有機碳分析 56
4.5管柱內六價鉻及總鉻分析 58
4.6管柱內水樣-總鐵、亞鐵、硫酸鹽、硫化物分析 60
4.7管柱內氨氮.亞硝酸鹽.硝酸鹽變化 62
4.8管柱內甲烷及氫氣濃度變化 63
4.9菌相分析結果 66
第五章 結論與建議 68
5.1結論 68
5.2建議 69
參考文獻 70

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