地下水被石油碳氫化合物所污染是一個愈趨普遍且嚴重的問題，此碳氫化合物包括汽油添加劑-甲基第三丁基醚(methyl tertiary-butyl ether, MTBE)、苯、甲苯、乙苯及二甲苯[BTEX (benzene, toluene, ethylbenzene和xylenes)]及三甲基苯[TMB (1,2,4-trimethylbnezene及1,3,5-trimethylbenzene)]均會對人體造成危害；而MTBE具有水溶性高、在地下水環境擴散容易及生物分解性較低之特性，苯在厭氧環境中較甲苯、二甲苯及乙苯不易被分解，且已被公告為致癌性物質。此外，含氯有機溶劑[如三氯乙烯(trichloroethylene, TCE)]為地下水中最常見之重質非水相溶液污染物，其對脂類有高溶解力，並且具有低可燃、易爆、低沸點及高蒸氣壓等特性，故大量的被使用於工業製程中。由於不當之管理與處置，含氯有機溶劑成為國內外土壤及地下水污染之主要污染來源之一。
被動式透水性整治牆(passive permeable reactive barrier)由於具有經濟性及環境友善性，目前已是受到矚目的整治選項。本研究目的則分別設計化學及生物透水性整治牆，並發展一種可緩慢持續釋放氧化劑(如過硫酸鹽)或基質之緩釋物質，分別進行石油碳氫化合物及含氯溶劑之處理成效評估。第一部分研究主要為發展釋氧化劑整治牆(in-situ oxidant-releasing wall)處理現地受石油碳氫化合物污染之下水水，(甲基第三丁基醚及苯為本研究目標污染物)污染之地下水。研究主要工作包含設計可緩慢持續釋放過硫酸鹽之氧化劑物質並研究其組成及釋放效率，瞭解長期釋放之特性。此外，並以管柱試驗評估利用釋氧化劑物質現地整治受甲基第三丁基醚及苯污染地下水之可行性。在緩釋氧化劑物質製備實驗之結果顯示，配比為1/1.1/0.24/0.7(過硫酸鈉/水泥/砂/水)之平均釋放速率為7.26 mg/S2O82-/d/g。管柱試驗中，甲基第三丁基醚及苯在操作前期(48 PV前)去除率分別為86-92%及95-99%；操作後期之甲基第三丁基醚及苯去除率分別降至40-56%及85-93%。甲基第三丁基醚之降解副產物-丙酮，於實驗期間被測得。添加二價鐵離子可促進活化過硫酸鹽氧化反應，但過量的二價鐵離子可能會與污染物競爭過硫酸鹽，造成氧化速率降低。第二部分研究之目的為設計生物透水性整治牆，並發展一種可緩慢釋放碳源、氫源及營養物質之基質，以加速三氯乙烯之生物降解。生物透水性整治牆合成之基質結合蔬菜油及生物可分解界面活性劑[simple green, (SG)和卵磷脂]，使蔬菜油乳化為較易擴散之緩釋型聚合膠體基質(slow-releasing polycolloid substrate)，此結果長期提供微生物厭氧還原脫氯所需之碳源或氫源。研究中50%乳化油為基準，當卵磷脂及SG濃度分別為71mg/L及72 mg/L時，其乳化程度可達100%，顯示該配方為乳化最佳比例。乳化油合成方式則以卵磷脂及SG混合乳化油在乳化均質機攪拌30分鐘所生成之粒徑最小，且界達電位為負值，有利於土壤孔隙間傳輸。若假設透水性反應牆注入之乳化油寬度約3 m，且含水層中無任何微生物反應，則上游三氯乙烯污染物需0.28年方能穿透反應牆。綜合上述結果，發現聚合膠體基質確實可有效促進厭氧生物還原脫氯反應，並消耗硝酸鹽及硫酸鹽。由以上結果顯示緩釋型聚合膠體基質建立之生物透水性整治牆具有下列機制：(1)蔬菜油對於三氯乙烯具吸附性及(2)緩慢釋出氫氣及醋酸鹽促進厭氧還原脫氯作用，並有效攔阻及降解三氯乙烯及其降解副產物，在溶氧消耗促使反應環境處於還原狀態下，加速厭氧脫氯菌群之增長。選用緩釋型物質做為透水性整治牆之填充材可避免持續灌注之高操作費用，在考量成本及效能上，緩釋型化學或生物透水性整治牆極具競爭力，但目前仍缺乏實際應用案例，而本研究結果應可提供將朝模場或實場應用所需之操作參數。

Soil and groundwater at many existing and former industrial areas and disposal sites is contaminated by organic solvent compounds that were released into the environment. Organic solvent compounds are heavier than water. When they are released into the subsurface, they tend to adsorb onto the soils and cause the appearance of LNAPL (light nonaqueous phase liquid) and DNAPL (dense nonaqueous phase liquid) pool. The industrial petroleum hydrocarbons (e.g., methyl tertiary-butyl ether, MTBE and benzene) and chlorinated solvent (e.g., trichloroethylene, TCE) are among the most ubiquitous organic compounds found in subsurface contaminated environment. One cost-effective approach for the remediation of the chlorinated solvent and petroleum products contaminated aquifers is the installation of permeable reactive zones or barriers within aquifers. As contaminated groundwater moves through the emplaced reactive zones, the contaminants are removed, and uncontaminated groundwater emerges from the downgradient side of the reactive zones.
The objectives of this study were developed to evaluate the feasibility of applying in-situ chemical oxidation (ISCO) barrier and in-situ slow polycolloid-releasing substrate (SPRS) biobarrier system on the control of petroleum hydrocarbons and chlorinated solvent plume in aquifer. In the ISCO barrier system, it contained oxidant-releasing materials, to release oxidants (e.g., persulfate) contacting with water for oxidating contaminants existed in groundwater. In this study, laboratory-scale fill-and-draw experiments were conducted to determine the compositions ratios of the oxidant-releasing materials and evaluate the persulfate release rates. Results indicate that the average persulfate-releasing rate of 7.26 mg S2O82-/d/g was obtained when the mass ratio of sodium persulfate/cement/sand/water was 1/1.4/0.24/0.7. The column study was conducted to evaluate the efficiency of in situ application of the developed ISCO barrier system on MTBE and benzene oxidation. Results from the column study indicate that approximately 86-92% of MTBE and 95-99% of benzene could be removed during the early persulfate-releasing stage (before 48 pore volumes of groundwater pumping). The removal efficiencies for MTBE and benzene dropped to approximately 40-56% and 85-93%, respectively, during the latter part of the releasing period due to the decreased persulfate-releasing rate. Results reveal that acetone, byproduct of MTBE, was observed and then further oxidized completely. Results suggest that the addition of ferrous ion would activate the persulfate oxidation. However, excess ferrous ion would compete with organic contaminants for persulfate, causing the decrease in contaminant oxidation rates. In the SPRS biobarrier system, the food preparation industry has tremendous experiences in producing stable oil-in-water (W/O, 50/50) emulsions with a uniformly small droplet size. Surfactant mixture (71 mg/L of SL and 72 /L of SG) blending with water could yield a stable and the optimal emulsion was considered the best. The small absolute value of the emulsion zeta potential reduces inter-particle repulsion, causing the emulsion droplets to stick to each other when they collided. Overtime, large masses of flocculated droplets can form which then clog the sediment pores. The results can be used to predict abiotic interactions and distribution of contaminant mass expected after SPRS injection, and thus provides a more accurate estimate of the mass of TCE removed due to enhanced biodegradation. The effect of TCE partitioning to the vegetable oil on contaminant migration rates can be approximated using a retardation factor approach, where 0.28 years through a 3 m barrier. In anaerobic microcosm experiments, result show that SPRS can be fermented to hydrogen and acetate could be used as a substrate to simulate reductive dehalorination. The apparent complete removal of nitrate and sulfate by SPRS addition was likely a major factor that promoted the complete reduction of TCE at later stages of this study. Results from the column experiment indicate that occurrence of anaerobic reductive dechlorination in the biobarrier system can be verified by: (1) the oil: water partition coefficients of dissolved TCE into vegetable oil were be used to predict abiotic interactions and distribution of contaminant mass expected after SPRS injection. (2) The SPRS can ferment to hydrogen and acetate could be used as a substrate to simulate reductive dechlorination. The proposed treatment scheme would be expected to provide a more cost-effective alternative to remediate other petroleum hydrocarbons and chlorinated solvents-contaminated aquifers. Experiments and operational parameters obtained from this study provide an example to design a passive barriers system for in-site remediation.

謝誌 I
中文摘要 III
Abstract V
List of Contents IX
List of Tables XI
List of Figures XIII
CHAPTER 1 1
Introduction 1
1.1 Background 3
1.2 Objectives 3
CHAPTER 2 Literature Review 5
2.1 Groundwater contamination 7
2.2 Nonaqueous phase liquid 8
2.3 Groundwater remediation technologies 12
2.3.1 Physical processes 13
2.3.2 Chemical processes 16
2.3.2.1 Chemical oxidation overview 16
2.3.2.2 In-situ chemical oxidation of contaminated soil and groundwater using persulftae 22
2.3.3 Bioremediation 25
2.3.3.1 Bioremediation overview 25
2.3.3.2 Reductive dechlorination 28
2.4 Passive permeable reactive barrier system 30
2.4.1 Passive permeable reactive barrier system overview 30
2.4.2 Biobarrier system 34
2.4.3 Biobarrier systems for chlorinated-hydrocarbon contaminated groundwater remediation 38
CHAPTER 3 Materials and Methods 45
3.1 In-situ chemical oxidation (ISCO) barrier system 47
3.1.1 Materials 47
3.1.2 Design of oxidant-releasing materials 47
3.1.3 Evaluation of the released persulfate on groundwater remediation 48
3.1.4 Performance evaluation and sample analysis 50
3.2 In-situ slow polycolloid-releasing substrate (SPRS) biobarrier system 53
3.2.1 Materials 53
3.2.2 Emulsion preparation 53
3.2.3 The experiments of NAPL oil and emulsion inject 55
3.2.4 Batch experiments on TCE sorption to vegetable oil 56
3.2.5 Anaerobic microcosm experiment 57
CHAPTER 4 Results and Discussion 59
4.1 ISCO barrier system 61
4.1.1 Design of oxidant-releasing materials 61
4.1.2 Evaluation of the released persulfate on groundwater remediation 63
4.2 SPRS biobarrier system 77
4.2.1 Emulsion preparation 77
4.2.2 The experiments of NAPL oil and emulsion inject 82
4.2.3 Partitioning of dissolved TCE into vegetable oil 85
4.2.4. Anaerobic microcosm study 87
CHAPTER 5 Conclusions and Recommendations 93
5.1 Conclusions 95
5.1.1 ISCO barrier system 95
5.1.2 SPRS biobarrier system 96
5.2 Recommendations 97
Chapter 6 References 99

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