Use of Solvents for Pahs Extraction and Enhancement of the Pahs Bioremediation in Coal- Tar-Contaminated Soils Pak-Hing Lee Iowa State University
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Iowa State University Capstones, Theses and Retrospective Theses and Dissertations Dissertations 2000 Use of solvents for PAHs extraction and enhancement of the PAHs bioremediation in coal- tar-contaminated soils Pak-Hing Lee Iowa State University Follow this and additional works at: https://lib.dr.iastate.edu/rtd Part of the Environmental Engineering Commons Recommended Citation Lee, Pak-Hing, "Use of solvents for PAHs extraction and enhancement of the PAHs bioremediation in coal-tar-contaminated soils " (2000). Retrospective Theses and Dissertations. 13912. https://lib.dr.iastate.edu/rtd/13912 This Dissertation is brought to you for free and open access by the Iowa State University Capstones, Theses and Dissertations at Iowa State University Digital Repository. It has been accepted for inclusion in Retrospective Theses and Dissertations by an authorized administrator of Iowa State University Digital Repository. For more information, please contact [email protected]. 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Photographs included in the original manuscript have been reproduced xerographically in this copy. Higher quality 6' x 9' black and white photographic prints are available for any photographs or illustrations appearing in this copy for an additional charge. Contact UMI directly to order. Bell & Howell Information and Learning 300 North Zeeb Road. Ann Arbor, Ml 48106-1346 USA UMJ' 800-521-0600 Use of solvents for PAHs extraction and enhancement of the PAHs bioremediation in coal-tar-contaminated soils by Pak-Hing Lee A dissertation submitted to the graduate faculty in partial fulfillment of the requirement for the degree of DOCTOR OF PHILOSOPHY Major: Civil Engineering (Environmental Engineering) Major Professor: Say Kee Ong Iowa State University Ames, Iowa 2000 UMl Number 9962828 UMl ® UMl Microfomi9962828 Copyright 2000 by Bell & Howell Infomiation and Learning Company. All rights reserved. This microfomn edition is protected against unauthorized copying under Title 17, United States Code. Bell & Howell Information and Learning Company 300 North Zeeb Road P.O. 80x1346 Ann Arbor, Ml 48106-1346 ii Graduate College Iowa State University This is to certify that the doctoral dissertation of Pak-Hing Lee has met the dissertation requirements of Iowa State University Signature was redacted for privacy. Committee Member Signature was redacted for privacy. Committee Member Signature was redacted for privacy. Committefe Member Signature was redacted for privacy. Comm' ttee VIember Signature was redacted for privacy. Commi ttee ^^ber Signature was redacted for privacy. fajor pressor Signature was redacted for privacy. For tfi^ Ms^r Program Signature was redacted for privacy. For the^Qsrauate College iii TABLE OF CONTENTS LIST OF FIGURES vi LIST OF TABLES ix ABSTRACT xii CHAPTER 1. INTRODUCTION AND OBJECTIVES 1 Introduction 1 Dissertation Objectives 2 Dissertation Organization 3 CHAPTER 2. LITERATURE REVIEW 4 Background 4 Polycyclic Aromatic Hydrocarbons 6 Bioremediation 12 Environmental Factors Affecting Bioremediation 12 Microbial Degradation of PAHs 17 Acclimatization, Adaptation and Bioaugmentation 19 Biochemical Pathways 20 Cometabolic Biodegradation 23 Bioavailability 25 Enhancement of Bioavailability 27 Field-scale Bioremediation Technologies for Coal-Tar-Contaminated Soils 30 Summary 34 References 34 CHAPTER 3. EXTRACTION METHOD FOR ANALYSIS OF PAHS IN COAL-TAR-CONTAMINATED SOILS 50 Abstract 50 Introduction 51 Materials and Methods 54 Direct Extraction Method 54 Screening of Different Solvents 55 Coal-Tar-Contaminated Soils 55 Results and Discussion 57 Solvent Screening Test 57 Comparison of Extracted Concentrations for Four Coal-Tar-Contaminated Soils 59 Comparison of Different Solvents Using a Certified Soil 61 Comparison of the Direct Extraction Method with Other Extraction Methods 62 iv Conclusions 67 Acknowledgments 68 References 68 CHAPTER 4. ESTIMATION OF POTENTIAL PAHS BIODEGRADATION FOR COAL-TAR-CONTAMINATED SOILS 70 Abstract 70 Introduction 71 Materials and Methods 73 Soil Characteristics 73 Solvent Extraction Study 74 Soil Slurry Biodegradation Studies 77 Results and Discussion 78 Solvent-Water Extraction Experiments 78 Extent of PAH Biodegradation in Different Soils 81 Correlation between Percent Extracted and Biodegradation 87 Conclusions 105 Acknowledgments 106 References 106 CHAPTER 5. USE OF SOLVENT TO ENHANCE PAHs BIODEGRADATION OF COAL-TAR- CONTAMINATED SOILS 110 Abstract 110 Introduction 111 Materials and Methods 112 Coal-Tar-Contaminated Soils 112 Solvent Pretreatment 113 Soil Slurry Biodegradation Studies 113 Analysis of Soil PAH Concentrations 116 Results and Discussion 116 Total PAH Degradation 116 Degradation of 3-ring PAH 118 Degradation of 4-ring PAH 120 Degradation of 5-ring PAH 123 Effects of Properties of Soil and PAHs on Solvent Enhancement 123 Conclusions 128 Acknowledgments 129 References 129 V CHAPTER 6. EFFECTS OF LOW MOLECULAR WEIGHT PAHS ON THE BIODEGRADATION OF BENZO(a)PYRENE IN AQUEOUS PHASE AND FOR VARIOUS PAH-CONTAMINATED SOILS 133 Abstract 133 Introduction 134 Materials and Methods 136 Chemicals 136 BaP Degradation in Liquid Phase Treatment 136 BaP Degradation in Solid Phase Treatment 138 Results 141 BaP Degradation in Liquid Phase Treatment 141 BaP Degradation in Solid Phase Treatment 144 Discussion 1 SO Acknowledgments 152 References 152 CHAPTER 7. GENERAL CONCLUSIONS AND FUTURE STUDIES 156 APPENDIX RAW DATA 158 ACKNOWLEDGMENTS 172 vi LIST OF nCURES Figure 2-1. Chemical structures of 16 polycyclic aromatic hydrocarbons 8 Figure 2-2. Influence of PAH physical and chemical characteristics on environmental fate mechanisms (Smith et al., 1999) 10 Figure 2-3. Proposed pathway for the degradation of naphthalene by bacteria (Gibson and Subramanian, 1994) 21 Figure 2-4. Pathway of fungal transformation of benzo(a)pyrene adapted from Cemiglia and Heitkamp (1989) 22 Figiu-e 4-1. Extraction of PAHs using different acetone-water mixtures for five different soils 79 Figure 4-2. Extraction of PAHs using different ethanol-water mixtures for five different soils 80 Figure 4-3. Biodegradation of PAHs for Vandalia (LTU) soil in soil slurry reactor 82 Figure 4-4. Biodegradation of PAHs for Charles City soil in soil slurry reactor 83 Figure 4-5. Biodegradation of PAHs for Vandalia (EXC) soil in soil slurry reactor 84 Figure 4-6. Biodegradation of PAHs for Hampton soil in soil slurry reactor 85 Figure 4-7. Biodegradation of PAHs for Independence soils in soil slurry reactor 86 Figure 4-8. Degradation of Total PAHs for five different soils in soil slurry reactor 89 Figure 4-9. Plot of percent PAH extracted and percent biodegraded for Hampton soil using different ethanol-water mixtures 90 Figure 4-10. Plot of percent PAH extracted and biodegradation rate constant (k) for Hampton soil using different acetone-water mixtures 91 Figure 4-11. Plot of vs. acetone-water volume flection for five different soils. is for percent PAH extracted and percent biodegraded 94 vii Figure 4-12. Plot of vs. acetone-water volume fraction for five different soils. is for percent extracted and percent biodegraded 95 Figure 4-13. Plot of percent PAH extracted vs. percent biodegraded for four different soils using 0.6 volume fraction of acetone in acetone-water mixture 96 Figure 4-14. Plot of percent PAH extracted vs. biodegraded rate constant (k) for four different soils using 0.6 volume fraction of acetone in acetone-water mixture 97 Figure 4-15. Plot of percent PAH extracted (modified with Kow) vs. percent biodegraded (modified with Mw) for all five soils using 0.6 volume fraction of acetone (Mw = molecular weight, nap = naphthalene, i = particular PAH) 99 Figure 4-16. Plot of slopes of regression line (percent biodegraded vs. percent extracted using 0.6 acetone-water mixture) and organic carbon content for four different soils 101 Figure 4-17. Plot of intercepts of regression line (percent biodegraded vs. percent extracted using 0.6 acetone-water mixture) and percent clay plus silt fi^ction for four different soils 102 Figure 4-18. Comparison of experimental and calculated percent biodegraded of 16 PAHs by using acetone-water mixture (0.6 volume fraction) for Independence soil 104 Figure 5-1. Comparison of Total PAHs removal for Vandalia (EXC) soil with and without solvent pretreatment 117 Figure 5-2. Phenanthrene degradation for different solvent pretreatments and different MGP soils 119 Figure 5-3. Chrysene degradation for different solvent pretreatments and different MGP soils 121 Figure 5-4. Benzo(a)pyrene degradation for different solvent pretreatments and different MGP soils 124 Figure 5-5. Correlation