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Ultrasound Induced Destruction of Emerging Contaminants ULTRASOUND INDUCED DESTRUCTION OF EMERGING CONTAMINANTS A Dissertation Submitted to the Temple University Graduate Board In Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy By Gangadhar Andaluri JANUARY 2011 Examining Committee Members: Rominder Suri, Advisory Chair, Civil and Environmental Engineering Saroj Biswas, Electrical Engineering Benoit Van Aken, Civil and Environmental Engineering Tony Singh, Civil and Environmental Engineering Svetlana Neretina, Mechanical Engineering © by Gangadhar Andaluri 2010 All Rights Reserved i ABSTRACT There are many reports indicating the presence of emerging contaminants such as: estrogen hormones, 1,4-dioxane and perfluoro-octanoic acids in the natural environment. Estrogen hormones are considered important emerging class of contaminants due to their endocrine disrupting effects. These compounds are invariably found in the environment originating mostly from natural sources. Trace concentrations of estrogen hormones (low µg/L concentrations) have been detected in municipal wastewater treatment plants and observed in receiving water bodies. 1,4-Dioxane (C4H8O2) is used as an organic solvent and solvent stabilizer numerous in chemical processes. The United States Environmental Protection Agency (US-EPA) has recognized 1,4-dioxane as a toxic chemical and a possible human carcinogen. 1,4-dioxane has been detected as a contaminant in the natural environment, drinking water supplies, superfund sites, public groundwater sources in the United States, Canada and Japan at concentrations greater than the permissible standards. Perfluorinated chemicals such as perfluoro-octanoic acid (PFOA) and perfluorooctane-sulfonate (PFOS) have been manufactured for use in a variety of industrial and consumer applications. Due to their environmental persistence, PFOAs have been detected in surface waters at a number of locations at concentrations ranging from pg/L to ng/L. Elevated concentrations of PFOAs have been measured in surface and ground waters near specific point sources. Through this project, successful attempts have been made for the destruction of emerging contaminants using ultrasound. This study deals with the optimization of various process parameters for the destruction of estrogen hormones. The influence of process parameters such as power density, reactor geometry, power intensity, ultrasound amplitude, and external mixing was investigated. Artificial neural network (ANN) approach was used to describe the interactions between optimized parameters. The important findings obtained in the present work for the optimized estrogen degradation can help tackle the challenges of scale up such as operational optimization and energy consumption. The effect of process conditions such as pH and presence of oxidizing agents on the ultrasonic destruction of 1,4-dioxane and PFOA was studied. Acidic conditions favored the destruction of both the compounds. The presence of activated sulfate radicals enhanced the reaction rate kinetics. An innovative technology using electric potential and ultrasound for the removal organic contaminants was developed. The existence of organic contaminants in ionic form under certain process conditions has led to the development of this technology. Applying a low electric potential across the ii probe enhances the mass transfer of the contaminants into effective reaction zone, thereby enhancing the total destruction. A two-fold increase in the reaction rates was observed. This study shows ultrasound as an efficient and effective treatment technology for the destruction of emerging contaminants. Part of this thesis work is submitted for publication in journals: Gangadhar Andaluri, Rominder Suri and Kuldip Kumar, “Occurrence of Estrogen Hormones in Biosolids, Animal Manure and Mushroom Compost”, submitted to Environmental Monitoring and Assessment, 2010 Gangadhar Andaluri, Rominder Suri and Ekatrina Rokhina, “Optimization of Sonochemical Reactor for Removal of Estrogen Hormones: Combined Theoretical (ANN modeling) and Experimental Approach”, manuscript under preparation, (2010) Gangadhar Andaluri and Rominder Suri, “Effect of process conditions on ultrasound induced destruction of 1,4 dioxane”, manuscript under preparation (2010) iii ACKNOWLEDGEMENTS I would like to express my sincere and deep gratitude to Dr. Rominder Suri for his continuous guidance and wisdom over the duration of my doctoral program. As a research and academic advisor he helped me improve my knowledge and ability to understand the concepts of environmental engineering. Without his help and guidance none of this would have been possible and I appreciate that very much. I would also like to thank Water and Environmental Technology Center and Civil Engineering Department at Temple University for the continuous support. I would also like to thank Dr. Biswas, Dr. Van Aken, Dr. Tony Singh and Dr. Svetlana for accepting to be on my dissertation committee. I would also like to thank Wyeth Pharmaceuticals for funding the project. I would also like to thank to Dr. Ekaterina for help in neural network modeling and Dr. Weiyue for helping me in the analytical lab. Special thanks to my colleagues Shashi, Deepthi, Mohan, Uthappa, Sagar, Bikash, Dan, Marianne, Candice, Rupam, Amruta, Tugba, Thida, Niki and Gurwinder for their support in the lab. Special thanks to Elenie for administrative assistance. Finally I would like to dedicate this dissertation to my dad, mom and brother for their continuous support and encouragement during the past few years. iv TABLE OF CONTENTS ABSTRACT.....................................................................................................................................................ii ACKNOWLEDGEMENTS .........................................................................................................................iv LIST OF TABLES.........................................................................................................................................ix LIST OF FIGURES....................................................................................................................................xiii CHAPTER 1 EMERGING CONTAMINANTS: BACKGROUND AND PROJECT OBJECTIVES..................................................................................................................................................1 1.1 Introduction ....................................................................................................................................................1 1.2 Estrogen Hormones .....................................................................................................................................2 1.2 1,4-Dioxane................................................................................................................................................... 12 1.3 Perfluoro-Octanoic Acid.......................................................................................................................... 20 1.4 Project Objectives ...................................................................................................................................... 21 1.4.1 Specific objectives of the project................................................................................................ 22 CHAPTER 2 ULTRASOUND TECHNOLOGY ..................................................................................23 2.1 Theory of Cavitation ................................................................................................................................. 25 2.1.1. Micro-discharGe theory................................................................................................................. 25 2.1.2. Hot-Spot theory ................................................................................................................................ 26 2.2 Ultrasound Reactors................................................................................................................................. 29 2.3 Sonication of ECs........................................................................................................................................ 37 CHAPTER 3 EXPERIMENTAL METHODS.....................................................................................41 3.1 Steroid Hormone Analysis ..................................................................................................................... 41 v 3.1.1 Chemical and reaGents.................................................................................................................... 41 3.1.2 Glassware preparation ................................................................................................................... 41 3.1.3 Calibration standards...................................................................................................................... 42 3.1.4 Solid phase extraction (SPE)........................................................................................................ 43 3.1.5 Derivatization..................................................................................................................................... 43 3.1.6 Estrogen extraction from solid waste matrices................................................................... 44 3.1.7 Desorption experiments ................................................................................................................ 45 3.1.8 Gas chromatography – mass spectrometry (GC/MS) analysis.....................................
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