臺灣博碩士論文加值系統

　　甲基第三丁基醚 (methy1 tert-buty1 ether，MTBE) 是目前全世界廣泛使用的汽油添加劑，以提高油品之辛烷值與燃燒效率，減低臭氧和一氧化碳之排放。由於MTBE具有高度水溶解度、低亨利係數值、不易被土壤及含水層物質吸附及生物難以分解等特性，一旦洩漏在環境系統中，將隨著地下水流在地下環境中擴散流動，污染地下水，造成極大的危害。吸附劑材質透水性反應牆 (adsorbent-based PRBs) 由於整合吸附技術之快速、便利、高去除率，和現地處理 (in-situ treatment) 之低成本、沒有廢水排放問題之優點，對於處理難分解污染物，例如MTBE，具有很大發展潛力。

　　為瞭解吸附劑材質透水性反應牆，處理受MTBE污染地下水之效能，研究針對不同吸附劑在不同類型之天然水中，進行平衡、動力吸附及管柱實驗。研究使用三種不同類型之吸附劑，包括活性碳 (F600、F400、F300、Unicarb)、樹脂 (Ambersorb 572、Ambersorb 563) 及沸石 (mordenite、HiSiv 1000)。天然水部份，包括台灣三條崙地下水、鳳山水庫原水和東港溪河水；德國卡爾斯魯 (Karlsruhe) 地下水、萊茵河 (Rhine) 河水。實驗結果顯示，活性碳和樹脂吸附劑在天然水中之MTBE平衡吸附量，會由於天然有機物質 (NOM) 之競爭吸附，低於吸附劑在去離子水中之MTBE吸附量。由於NOM之競爭吸附效應，會進一步導致活性碳和樹脂在天然水之吸附等溫線，隨著污染物之初始濃度高低而變化。天然水吸附系統中，較低污染物初始濃度之等溫吸附線，會比高初始濃度之等溫吸附線，有較大程度之NOM吸附競爭，導致較大程度之吸附量降低。另一方面，吸附劑特性和NOM的分子量分布，也會影響MTBE之吸附效能和NOM競爭程度。較高分子量之NOM和適當孔徑之吸附劑，可以藉由分子篩效應 (molecular sieve effect)，減輕NOM之競爭吸附。例如在mordenite/天然水和Ambersorb 563/三條崙地下水吸附系統中，沒有明顯之競爭吸附發生。由於NOM之競爭吸附行為，本研究提出SCAM-EBC 模式，以描述及預測MTBE和NOM在不同吸附劑、初始濃度條件下之平衡吸附行為，作為後續吸附劑材質之PRBs設計基準參考。SCAM-EBC模式係結合等背景化合物 (EBC) 和簡化競爭吸附模式 (SCAM) 所產生。藉由所獲得之EBC參數值，SCAM-EBC 模式成功地預測不同類型活性碳及樹脂，在不同天然水之不同初始濃度MTBE等溫吸附線。此外，SCAM-EBC模式也可以應用在不同種類之污染物，例如高吸附強度污染物 (TCP、atrazine、chloroform) 和土臭味化合物 (MIB、geosmin)。另一方面，SCAM-EBC模式也可以描述粉狀活性碳 (PAC) 處理系統中常見之等溫吸附線彎曲效應 (isotherm curvature)。結果顯示，當relative adsorptivity大於critical relative adsorptivity 時，會有明顯之彎曲效應產生。

　　動力實驗結果顯示，表面擴散 (SDM) 和孔隙擴散 (PDM) 結合SCAM-EBC平衡模式，皆可以模擬不同實驗條件下，MTBE在吸附劑活性碳、樹脂和沸石顆粒之傳輸行為。模式所獲得之表面或是孔隙擴散係數值，與MTBE之初始濃度和吸附劑添加劑量無關。活性碳和樹脂兩種吸附劑，在去離子水和天然水中之表面或是孔隙擴散係數幾乎相同，顯示NOM對於MTBE傳輸沒有顯著之妨礙或是曲折效應。然而，mordenite 沸石卻具有明顯緩慢之動力傳輸結果。

　　最後，進行迷你管柱試驗 (RSSCTs) 模擬透水性反應牆在現地場址之處理效能。結果顯示，和去離子水之吸附系統相比，天然水中所獲得之貫穿曲線 (BTCs) 較為陡峭，且具有較低之吸附容量。推測其原因，與批次平衡實驗相同，皆為NOM和MTBE競爭吸附所導致。管柱進流MTBE濃度高低，對於管柱之MTBE吸附容量和BTCs形狀分佈有一定程度之影響。愈低進流MTBE濃度，會造成較大程度之NOM競爭吸附，導致吸附容量變小及較寬胖形狀之BTCs。固定床之表面擴散模式結合SCAM-EBC，成功地預測不同空床接觸時間 (EBCTs) 時，不同進流MTBE濃度與天然水之RSSCTs管柱MTBE吸附容量與BCTs。SDM-SCAM-EBC模式之輸入參數，是由批次平衡/動力實驗和質量傳輸經驗式所獲得，並沒有調整任何參數，顯示模式之可預測性。基於平衡、動力和管柱實驗與模式分析成果顯示，研究所提出之SDM-SCAM-EBC模式，可以藉由一組等溫吸附線和動力實驗，獲得EBC參數值，合理預測不同實驗條件下之PRBs操作效能，以估算現地處理之PRB使用年限及處理效能評估。

　Methyl tert-butyl ether (MTBE) is the most common oxygenated fuel additive used to increase the octane rating and to enhance the combustion efficiency of gasoline. As a consequence of widespread use of MTBE, it has been found to be a ubiquitous and recalcitrant contaminant in groundwater and surface water due to its physicochemical properties. To remediate MTBE-contaminated groundwater, the passive in-situ permeable reactive barriers (PRBs) with different types of adsorbing media including granular activated carbon (GAC), carbonaceous resin and zeolite were used in this study. Although this research focuses mainly on simplified natural and engineering environmental systems, the results may provide useful information and insights for more complex large-scale experimental systems and for field applications.

　To evaluate the performances of the adsorbent-based PRBs for treating MTBE-contaminated groundwater, equilibrium and kinetic adsorption of MTBE onto the adsorbent pellets of activated carbons (F600, F400, F300, Unicarb and WPH), carbonaceous resins (Ambersorb 563 and 572) and zeolites (mordenite and HiSiv 1000) in different natural waters located in Taiwan and Germany were first explored. The experimental results revealed that adsorption isotherms of MTBE for the activated carbons and carbonaceous resins in natural waters were different than those in deionized water. It was suggested that natural organic matter (NOM) competed with MTBE for the adsorption sites of the adsorbents tested. The initial concentration of MTBE has great influence on the equilibrium capacity for the activated carbons and resins in the presence of NOM. The lower the applied initial concentration, the higher the extent of competition was founded. Additionally, the NOM fraction of low-molecular weight and adsorbent properties, such as pore size distribution, aperture size and the SiO2/Al2O3 ratio for zeolite, have considerable influences on the equilibrium capacity of MTBE for the adsorbents tested in different water matrix. No competitive adsorption of NOM and MTBE was observed for mordenite whose aperture size is highly uniform and concentrated due to molecular sieve effect.

　A predictive method, called the SCAM-EBC approach, based on the well-known equivalent background compound (EBC) and simplified competitive adsorption model (SCAM) was developed to describe the competitive adsorption of NOM. The results revealed that the SCAM-EBC approach has excellent predictive ability of the isotherms at different initial concentrations for all the activated carbons/carbonaceous resins/natural water systems. Besides MTBE, several other pollutants, including strongly adsorbing compounds (TCP, atrazine, and chloroform) and two taste and odor causing compounds (MIB and geosmin) onto different activated carbons in natural and artificial groundwaters, were tested to verify the SCAM-EBC approach. Moreover, the relative adsorptivity based on the SCAM-EBC approach was proposed to quantify and predict the extent of isotherm curvature occurred at lower applying absorbent dosage. The marked isotherm curvature was found when the relative adsorptivity is larger than 2.0 to 4.0, called critical relative adsorptivity, for all the systems tested.

　The transport of MTBE onto those three types of adsorbent pellets in different water matrixes was simulated by intraparticle surface diffusion model (SDM) and pore diffusion model (PDM) combined with either the SCAM-EBC approach or IAST-EBC model. Both the intraparticle diffusion models fit the experimental kinetic data fairly well and successfully predicted the transport of MTBE within all of the adsorbents under different experimental conditions. The intraparticle surface and pore diffusivities showed different in deionized water and natural water systems and were attributed to the hindering effect and tortuous pathways. The results indicated that NOM seems to have no obvious impact on the transport of MTBE onto the activated carbons and resins. For mordenite, NOM may, however, block the surface opening aperture and hinder the diffusional paths of MTBE, causing slower adsorption kinetics.

　Finally, laboratory column experiments of the GACs, the rapid small scale column tests (RSSCTs), were conducted to simulate the transport of MTBE through the PRBs. Steeper breakthrough curves (BTCs) and smaller integrated column capacities of the RSSCTs for F600 and F300 GACs in groundwaters and river waters were found compared with those in deionized water. Like the batch adsorption systems for the activated carbons and resins used, both initial concentration effect and competitive adsorption between NOM and MTBE were found in the RSSCT column studies. The influent MTBE concentrations have great influences on the integrated column capacities as well as the spreading of BTCs for the RSSCTs under different empty bed contact times (EBCTs). A fixed-bed model based on a combination of the SDM and the SCAM-EBC approach was employed to simulate the experimental BTCs. The model predictions were compared with the BTCs of RSSCTs under different conditions. No adjustable parameters were required in modeling the fixed-bed BTCs. All the model input parameters were either extracted from the batch equilibrium and kinetic experiments or calculated from empirical correlations. The models successfully predicted the experimental BTCs at different EBCTs and influent concentrations of MTBE. Although the conditions tested in this study are simplified, the elucidation of clean up mechanisms and interactions taking place between the adsorbent media and MTBE plumes in this study should be informative enough to give a useful perspective when attempting to remediate MTBE-contaminated groundwater using adsorbent-based permeable reactive barriers (PRBs).

Abstract (In Chinese) i
Abstract iv
Dedication viii
Acknowledgments (In Chinese) ix
Table of Contents x
Table of Figures xiii
Table of Tables xvi

Chapter I. Introduction 1
Background 1
Usage of Methyl tert-Butyl Ether 1
Contamination of Methyl tert-Butyl Ether in Groundwater 2
Transport and Treatment of Methyl tert-Butyl Ether 3
In-Situ Permeable Reactive Barriers 4
Scope And Objectives 5
Dissertation Overview 6

Chapter II. Predicting Adsorption Capacity and Isotherm Curvature of Organic Compounds onto Activated Carbons in Natural Waters 13
Abstract 13
Introduction 14
Materials And Methods 17
Results And Discussion 19
Adsorption Isotherms of MTBE 19
Development of the SCAM-EBC Approach 20
Predictions of the SCAM-EBC Approach 23
Analysis of Relative Adsorptivity 25
Isotherm Curvature Analysis 27
Summary 31

Chapter III. Competitive and Hindering Effects of Natural Organic Matter on the Adsorption of MTBE onto Activated Carbons and Zeolites 43
Abstract 43
Introduction 44
Materials And Methods 45
Results And Discussion 48
Adsorption Isotherms in Deionized Water 48
Adsorption Isotherms of Activated Carbons in Natural Water 50
Adsorption Isotherms of Zeolite 52
Adsorption Kinetics of Activated Carbon and Zeolite 53
Summary 56

Chapter IV. Adsorption of MTBE from Contaminated Water by Carbonaceous Resins and Mordenite Zeolite 69
Abstract 69
Introduction 70
Materials And Methods 72
Results And Discussion 75
Adsorption Isotherms in Deionized Water 75
Adsorption Isotherms of Resins in Natural Waters 75
Modeling the Adsorption Isotherms of Resins in Natural Waters 77
Adsorption Isotherms of Mordenite in Natural Waters 79
Adsorption Kinetics and Tortuosity 80
Summary 83

Chapter V. Performance of Laboratory Adsorbent-based Permeable Reactive Barrier for Treating MTBE-contaminated Groundwater 95
Abstract 95
Introduction 96
Theory 97
The Dispersed Flow, Pore and Surface Diffusion Model (DFPSDM) 97
Rapid Small Scale Column Tests (RSSCTs) 99
Materials And Methods 102
Results And Discussion 103
BTCs in Deionized Water and Groundwater 103
Impact of Influent Concentrations on RSSCT Performances 105
Impact of EBCTs on RSSCT Performances 106
Comparison of RSSCTs and Large Column Studies 107
Modeling the PRB Performances 108
Applications 110
Summary 112

Chapter VI. Conclusions 127
Summary 127
Implications And Future Research Directions 130
Closing Remark 133
References 135
Appendix A: IASTM Program 145
Appendix B: Batch Kinetic Program 153
VITA 160

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