自民國89年「土壤及地下水污染整治法」公佈後，行政院環保署即陸續針對不明廢棄物非法棄置場址、全國各加油站、大型油槽設施等場址進行土壤及地下水污染調查工作，並對超出土壤或地下水污染管制標準之場址，依法公告為控制場址或整治場址，要求污染行為人進行污染改善、控制及整治工作。有鑑於有機污染場址之數量有逐年增加之趨勢，且其整治工作有時必須採用「多種整治技術同時施工」，或需以「分時程、分階段增加整治單元」之方式進行，並隨個案場址狀況不同而異，故有關有機污染場址之整治技術，近年來已逐漸為各界所重視。
在眾多污染事件中，受NAPL (non-aqueous phase liquid, 非水相溶液)污染場址之整治具有相當高之困難度，而傳統之整治方式(例如抽取處理法及空氣灌入法)僅針對溶解相之有機污染物進行處理，並無法有效移除NAPL造成之污染源，導致整治時程之延長及整治經費之提高。本研究所研發之三階段整治列車系統(treatment train system)，可有效同時移除DNAPL(dense-non-aqueous phase liquid)與LNAPL(light non-aqueous phase liquid)污染源並處理溶解相之有機污染物，而此整治列車系統之研究成果將可作為規劃設計NAPL污染場址整治系統之重要參考依據。研究中，我們以三氯乙烯(trichloroethylene, TCE)及燃料油(total petroleum hydrocarbon, TPH)為目標污染物，而論文所提出之三階段整治方式包括第一階段地下水及生物可分解之界面活性劑沖排(surfactant flushing)，第二階段之化學氧化(高錳酸鉀及Fenton-like氧化)及第三階段之加強式生物處理。當第一階段之處理效率降低後，即進行第二階段之化學氧化處理，以氧化殘留於土壤及地下水中污染物，而剩餘之污染物將應用加強式生物處理之方式進行降解去除。
實驗結果顯示，所使用之兩種非離子型界面活性劑Tween 80與Triton X-100之沖洗效率略優於第三種界面活性劑Simple GreenTM(簡稱SG)，但在環保(SG有較佳之生物分解性)與成本雙重考量下，本研究使用SG(成本為其他二種界面活性劑之1/3至1/4)進行後續之整治列車系統處理受TCE與燃料油污染之地下水與土壤。在高錳酸鉀氧化批次試驗方面，經過假一階反應動力參數推算後發現，當有添加1 g L-1 of SG於高錳酸鉀氧化TCE之系統時，其反應速率常數皆高於未添加SG之系統。因此添加SG對於高錳酸鉀氧化地下水中之TCE有正面效果，主要原因為SG可增進高錳酸鹽傳輸及提昇氧化速率之功能。結果也顯示，在96 mg L-1高錳酸鉀處理5 mg L-1 TCE之系統中，高錳酸鉀耗損速率常數及氯離子產生量可佐證添加SG確實有助於提昇高錳酸鉀脫氯降解TCE之效率。我們以較佳之整治列車系統組合進行管柱試驗，發現第一階段地下水及SG(1 g L-1)沖排可達到87.6%之TCE (初始濃度為40 mg/L)去除率；而第二階段注入96 mg L-1高錳酸鉀(第一階段殘留1 g L-1 of SG)氧化可再去除10.7%之TCE，殘留之TCE(1.7%)將可由第三階段之加強式生物處理去除，使TCE污染之介質達到完全整治之目標。
本研究也應用整治列車系統，以連續串聯的方式進行燃料油污染土壤之改善及復育。其中，以SG及地下水沖排、Fenton-like氧化技術與加強式生物處理串聯成整治列車系統處理受燃料油污染之土壤。結果顯示，第一階段SG及地下水沖排可達到80.3%之TPH去除率；而第二階段之Fenton-like氧化可再去除15.0%之TPH，殘留之TPH(4.7%)可由第三階段之加強式生物處理(利用第二階段殘留過氧化氫提供氧氣)去除。經三階段處理後，TPH濃度可由50,000 mg/kg降至ND值，達到完全去除之目標。總而言之，在複雜的地下環境中，整治列車概念系統可借重單一整治技術之優點，而彌補彼此間之缺點，對於受NAPL污染之地下水與土壤，極具應用發展潛力，未來更可應用於其他難分解污染物污染之土壤或地下水場址之整治。

The industrial solvent trichloroethylene (TCE) and petroleum hydrocarbons (e.g., fuel oil) are among the most ubiquitous organic compounds found in subsurface contaminated environment. The developed treatment train system included the first stage of groundwater and surfactant flushing followed by the second stage of chemical oxidation such as potassium permanganate (KMnO4) and Fenton-like treatment. The third stage was the application of enhanced bioremediation for the further removal of residual contaminants after the first two treatment processes. The objectives of this study were to (1) assess the applicability of treatment train system for the remediation of organic compounds contaminated subsurface environment, (2) determine the optimal operational conditions of the three-stage treatment system, and (3) evaluate the effects of residual surfactant Simple GreenTM (SG) and hydrogen peroxide (H2O2) after chemical oxidation stage on the efficiency of bioremediation process. In this study, three different surfactants [SG, Triton X-100, and Tween 80] were evaluated in batch experiments for their feasibility on contaminants removal. Results from the surfactant biodegradation and microbial enumeration study indicate that SG was more biodegradable and was able to enhance the microbial activity of the intrinsic microorganisms. Thus, SG was applied in the following batch or column experiments of the treatment train system. Results from this study indicate that approximately 87.6% of TCE in the system (with initial concentration of 40 mg L-1) could be removed from the simulated dense non-aqueous-phase liquids (DNAPLs) system after groundwater flushing followed by biodegradable surfactant (1 g L-1 of SG) flushing, while the TCE concentrations dropped from 40 to 4.96 mg L-1 at the end of the flushing experiment. Moreover, approximately 10.7% of the remaining TCE could be removed from the system after the oxidation process using KMnO4 as the oxidant. Results from the oxidation process show that TCE was reduced from 4.96 to 0.69 mg L-1, and chloride concentation was increased from ND to 0.88 mg L-1 with the presence of 1 g L-1 of SG. The residual 1.7% of the TCE could be further remediated via the enhanced bioremediation stage, and the TCE concentrations dropped from 0.69 mg L-1 to below detection limit at the end of the bioremediation experiment. Results also indicate that the remaining KMnO4 had no significant inhibition on bacterial growth and TCE biodegradation. Thus, SG flushing and KMnO4 oxidation would not cause adverse effect on subsequent bioremediation process using intrinsic bacteria. Thus, complete TCE remediation was observed in this study using the three-stage treatment scheme. Results from the column experiment reveal that a complete TPH removal could be obtained after the application of three consecutive treatment processes. Results show that TPH concentration could be reduced from 50,000 mg kg-1 to below detection limit. This indicates that the treatment train system is a promising technology to remediate fuel-oil contaminated soils. Results from the column study indicate that approximate 80.3% of initial TPH in the soil could be removed after the SG [50 pore volumes (PVs)] followed by groundwater (30 PVs) flushing. The Fenton-like oxidation (with 6% of H2O2 addition) was able to remove another 15.0% of TPH. The observed first-order reaction rate constant of TPH oxidation was 2.74×10-2 min-1, and the half-life was 25.3 min during the first 40 min of reaction. The residual 4.7% of the TPH could be further remediated via the aerobic bioremediation process. Thus, complete TPH removal was obtained in this study using the three-stage treatment scheme. The proposed treatment train system would be expected to provide a more efficient and cost-effective alternative to remediate chlorinated solvent and petroleum hydrocarbons contaminated sites.

List of Contents
Page
謝誌 Ⅰ
中文摘要 III
Abstract V
List of Contents …...........................................................................VIII
List of Tables .................................................................................... XII
List of Figures.................................................................................. XIII

Chapter 1 Introduction 1
1.1 Background of the Study 2
1.2 Objectives of Research 2

Chapter 2 Literature Review 4
2.1 Groundwater Pollution of Chlorinated Solvents 5
2.2 Soils Pollution of Petroleum Hydrocarbons 6
2.3 Treatment Trains System 7
2.4 Surfactant Flushing 9
2.5 In-Situ Chemical Oxidation Technology……………………………10
2.5.1 Fenton-like in Soils Remediation 12
2.5.2 Potassium Permanganate in Groundwater Remediation 13
2.6 Enhanced Bioremediation 15
Chapter 3 Materials and Methods 16
3.1 Soil and Groundwater Characterization 17
3.1.1 Site A 17
3.1.2 Site B 17
3.2 Surface Tension Test 18
3.3 Treatment Train System Development of TCE in Groundwater 19
3.3.1 Surfactant Selection Study 19
3.3.1.1 Surfactant Solubilization of TCE………………………….20
3.3.1.2 TCE Biodegradation Experiment………………………….20
3.3.1.3 Surfactant Flushing Experiment..………………………….22
3.3.2 Batch Experiments of Surfactant Enhanced Permanganate
Oxidation of Trichloroethylene in Groundwater…….....………..22
3.3.3 Column Experiments of Surfactant Enhanced Permanganate
Oxidation of Trichloroethylene in Groundwater….……………..23
3.3.4 Effect of Surfactant on Contaminant Biodegradation..………….25
3.3.5 Remediation of TCE-Contaminated Groundwater by Treatment
Train System…………………………………………………….26
3.3.5.1 Stage 1 - Groundwater and Surfactant Flushing...…………26
3.3.5.2 Stage 2 - Potassium Permanganate Oxidation…………..…26
3.3.5.3 Stage 3 - Enhanced Bioremediation……..…………………27
3.4 Treatment Train System Development of Fuel-oil in Soil 28
3.4.1 Surfactant Selection Study………………………………………28
3.4.1.1 TPH Biodegradation Experiment………………………….28
3.4.1.2 Surfactant Flushing Experiment..………………………….29
3.4.2 Remediation of Fuel-Oil Contaminated Soils by Treatment Train
System…………………………………………………………...30
3.4.2.1 Stage 1 - Surfactant and Groundwater Flushing ..………...30
3.4.2.2 Stage 2 - Fenton-like Oxidation…………….…….….....…32
3.4.2.3 Stage 3 - Enhanced Bioremediation …....…………………32

Chapter 4 Results and Discussion 34
4.1 Surface Tension Test 35
4.2 Treatment Train System Development of Chlorinated Solvents in Groundwater 35
4.2.1 Surfactant Selection Study 35
4.2.1.1 Surfactant Solubilization of TCE………………………….35
4.2.1.2 TCE Biodegradation Experiment………………………….37
4.2.1.3 Surfactant Flushing Experiment..………………………….40
4.2.2 Batch Experiments of Surfactant Enhanced Permanganate
Oxidation of Trichloroethylene in Groundwater…….....………..42
4.2.3 Column Experiments of Surfactant Enhanced Permanganate
Oxidation of Trichloroethylene in Groundwater….……………..50
4.2.4 Effect of Surfactant on Contaminant Biodegradation..………….54
4.2.5 Remediation of TCE-Contaminated Groundwater by Treatment
Train System…………………………………………………….57
4.2.5.1 Stage 1 - Groundwater and Surfactant Flushing …………..57
4.2.5.2 Stage 2 - Potassium Permanganate Oxidation…………..…59
4.2.5.3 Stage 3 - Enhanced Bioremediation…….…………………62
4.2.5.4 Removal Efficiency of Treatment Train System..…………63

4.3 Treatment Train System Development of Petroleum Hydrocarbons in Soil 64
4.3.1 Surfactant Selection Study 64
4.3.1.1 TPH Biodegradation Experiment………………….………64
4.3.1.2 Surfactant Flushing Experiment..………………………….68
4.3.2 Remediation of Fuel-Oil Contaminated Soils by Treatment Train
System…………………………………………………………...70
4.3.2.1 Stage 1 - Surfactant and Groundwater Flushing ..………...70
4.3.2.2 Stage 2 - Fenton-like Oxidation…………….…….….....…71
4.3.2.3 Stage 3 - Enhanced Bioremediation …....…………………74
4.3.2.4 Removal Efficiency of Treatment Train System..…………75

Chapter 5 Conclusions and Recommendations 76
Chapter 6 References 80




List of Tables
Page
Table 2-1 The properties of chlorinated solvents……………... 6
Table 2-2 Properties of chemical oxidants……………………. 11
Table 3-1 Chemical and physical properties of selected commercial surfactants……………………………..
20
Table 4-1 The degradation rates, reaction rate constants, and half-life values of TCE oxidation employed various KMnO4 and surfactant SG concentrations………….

45
Table 4-2 The concentrations of TCE degradition by-products, chloride generation, oxidatnt KMnO4 monitiored at the column outlet during two oxidation stages……..

52
Table 4-3 Removal efficiencyies of three different treatment processes…………………………………………….
64
Table 4-4 Calculated percentage of total TPH removal after the application of the three-stage treatment train system.........................................................................

75











List of Figures
Page
Figure 2-1 Superfund remedial actions: treatment trains with innovative treatment technologies………………......
8
Figure 3-1 Schematic of the column apparatus………………… 24
Figure 3-2 Schematic diagram of the column experiment……... 31
Figure 4-1 Properties of surfactant SG solution as surface tension analyses…………………………………......
35
Figure 4-2 The solubilization of 40 mg L-1 of TCE in different solutions (groundwater, 1 g L-1 of Tween 80, 1 g L-1 of Triton X-100, and 1 g L-1 of SG)………………...

36
Figure 4-3 Removal efficiency of TCE (1 mg L-1) in microcosms containing various surfactants…………
39
Figure 4-4 The microbial growth patterns of the total viable bacterial count in the reactors using surfactants (1 g L-1) of SG, Tween 80, and Triton X-100…………….

39
Figure 4-5 Variations in TCE (initial TCE concentration = 40 mg L-1) removal efficiency versus flushed pore volumes in batch experiment using groundwater and different surfactant solutions (Tween 80, Triton X-100, and SG) with (a) initial surfactant concentration = 1 g L-1; (b) initial surfactant concentration = 0.5 g L-1…………………………....





41
Figure 4-6 Effect of [KMnO4] on the oxidation of TCE: (a) different KMnO4 and surfactant SG concentrations; (b) 12 mg L-1 KMnO4 + different surfactant SG concentrations; (c) 48 mg L-1 KMnO4 + different surfactant SG concentrations………………..……...



44
Figure 4-7 The effect of surfactant SG addition on the KMnO4 consumption rates as the initial KMnO4 concentration was 96 mg L-1 and TCE concentration was 38.1 μM: (a) KMnO4 consumption concentration; (b) Pseudo-first-order rate constants analyses………….…………………………………..




48
Figure 4-8 The amounts of chloride generated and TCE degraded under the oxidation reaction with 96 mg L-1 KMnO4 in the absence and presence of 1 g L-1 SG: (a) amounts of chloride generated; (b) concentration of TCE in groundwater………..……..



49
Figure 4-9 The concentrations of chloride generation and by-products under the degradation of TCE in column experiment…………………..……………...

53
Figure 4-10 Pseudo-first-order rate constant kobs for KMnO4 consumption rate under both oxidation stages……...
53
Figure 4-11 The ratio of [TCE]/[MnO4-] and TCE degradation during two oxidation testing stages…………………
54
Figure 4-12 TCE degradation under aerobic microcosm experiments with sludge and surfactant SG (0.1 g L-1 and 1 g L-1) addition……………………………..

57
Figure 4-13 Percentage of TCE removal versus the pore volumes of groundwater and 1 g L-1 of SG used……………..
58
Figure 4-14 Amounts of produced chloride and degraded TCE during the oxidation reaction with 96 mg L-1 of KMnO4 in the absence or presence of 1 g L-1 of SG...

60
Figure 4-15 Ratio of [TCE]/[MnO4-] and KMnO4 consumption during the oxidation stage…………………………..
60
Figure 4-16 Amounts of MnO2 produced during the oxidation reaction with 96 mg L-1 of KMnO4 in the absence or presence of 1 g L-1 of SG……………………………

61
Figure 4-17 Reaction of permanganate and TCE in the presence (left) and absence (right) of 1 g L-1 of SG…………..
61
Figure 4-18 Disappearance of 0.69 mg L-1 of TCE and the growth pattern of culturable bacterial counts………
63
Figure 4-19(a) Biodegradation of 1,000 mg kg-1 of TPH in microcosms using surfactants (1 g L-1) of SG, Tween 80, and Triton X-100………………………………..
67
Figure 4-19(b) The microbial growth patterns of the culturable bacterial counts in the soil using surfactants (1 g L-1) with SG, Tween 80, and Triton X-100………………
67
Figure 4-20(a) Variations in TPH removal efficiency versus flushed pore volumes in batch experiment using different surfactant solutions (10 g L-1 of SG, 10 g L-1 of Triton X-100, and 10 g L-1 of Tween 80) with initial fuel oil concentration of 10,000 mg kg-1…………… 69
Figure 4-20(b) Variations in TPH removal efficiency versus flushed pore volumes in batch experiment using different surfactant solutions (10 g L-1 of SG, 10 g L-1 of Triton X-100, and 10 g L-1 of Tween 80) with initial fuel oil concentration of 50,000 mg kg-1……………



69
Figure 4-21 Percentage of TPH removal versus the pore volumes of SG (10 g L-1) and groundwater used……………..
71
Figure 4-22 Variations in TPH concentrations, temperature, H2O2 concentrations, and ORP versus the oxidation time………………………………………………….

73
Figure 4-23 Disappearance of 2,354 mg of TPH/kg and the growth pattern of culturable bacterial counts……….
74

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