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Potential Emissions and Exposures of Toxic Organics from Storage Tanks for Chemical Additions in Hydraulic Fracturing: a Modeling Approach

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Potential Emissions and Exposures of Toxic Organics from Storage Tanks for Chemical Additions in Hydraulic Fracturing: a Modeling Approach University of Tennessee, Knoxville TRACE: Tennessee Research and Creative Exchange Doctoral Dissertations Graduate School 12-2016 Potential Emissions and Exposures of Toxic Organics from Storage Tanks for Chemical Additions in Hydraulic Fracturing: A Modeling Approach Huan Chen University of Tennessee, Knoxville, [email protected] Follow this and additional works at: https://trace.tennessee.edu/utk_graddiss Part of the Environmental Engineering Commons Recommended Citation Chen, Huan, "Potential Emissions and Exposures of Toxic Organics from Storage Tanks for Chemical Additions in Hydraulic Fracturing: A Modeling Approach. " PhD diss., University of Tennessee, 2016. https://trace.tennessee.edu/utk_graddiss/4088 This Dissertation is brought to you for free and open access by the Graduate School at TRACE: Tennessee Research and Creative Exchange. It has been accepted for inclusion in Doctoral Dissertations by an authorized administrator of TRACE: Tennessee Research and Creative Exchange. For more information, please contact [email protected]. To the Graduate Council: I am submitting herewith a dissertation written by Huan Chen entitled "Potential Emissions and Exposures of Toxic Organics from Storage Tanks for Chemical Additions in Hydraulic Fracturing: A Modeling Approach." I have examined the final electronic copy of this dissertation for form and content and recommend that it be accepted in partial fulfillment of the equirr ements for the degree of Doctor of Philosophy, with a major in Civil Engineering. Kimberly E. Carter, Major Professor We have read this dissertation and recommend its acceptance: Joshua S. Fu, Qiang He, Paul D. Terry, Wenjun Zhou Accepted for the Council: Carolyn R. Hodges Vice Provost and Dean of the Graduate School (Original signatures are on file with official studentecor r ds.) Potential Emissions and Exposures of Toxic Organics from Storage Tanks for Chemical Additions in Hydraulic Fracturing: A Modeling Approach A Dissertation Presented for the Doctor of Philosophy Degree The University of Tennessee, Knoxville Huan Chen December 2016 Copyright © 2016 by Huan Chen All rights reserved. ii DEDICATION This dissertation is dedicated to my advisor (Dr. Kimberly E. Carter), my committee members (Dr. Joshua S. Fu, Dr. Qiang He, Dr. Paul D. Terry, and Dr. Wenjun Zhou), and my family (Qilin Chen, Ming’e Zhang, and Jianxiong Chen). iii ACKNOWLEDGEMENTS The moonlight is sprinkling on the window, and I am sitting in my apartment to write the part of acknowledgements in the dissertation, which is for my Ph.D. degree from the University of Tennessee, Knoxville, a university in the United States (U.S.). Time flies, and I cannot remember how many nights I spent and how many weekends it costs me to arrive at this final step. I guess I cannot make it without my industrious and assiduous attempts, and moreover without all merciful and graceful favors from the surrounding people. Thanks to my parents and my younger sister, they helped me making the tough decision of resigning my job and coming here for the Ph.D. degree which I had dreamed for several years. Acknowledgements to my advisor - Dr. Kimberly E. Carter, for the opportunity she offered to work together with her three years ago and for her continuously advising on my research during those three years. If I have any improvements on my academic career, it is because of her enduring training and cultivations. Thanks to my group members, Laura W. Matzek and Katherine E. Manz, for their company which makes me feeling I am not the only one who was suffering and struggling with the academic research and dissertation. Thanks to my friends living in the U.S. and China, their comforts and encouragements are the oases, without which I cannot survive when going through the desert. Thanks to my committee members (Dr. Joshua S. Fu, Dr. Qiang He, Dr. Paul D. Terry, and Dr. Wenjun Zhou), for willingly serving on my committee and providing the critical reviews and suggestions which improve my dissertation significantly. I am deeply aware that I cannot enjoy my academic life in the palace of science and engineering without their assistances. Hope all of them having a good and enjoyable life. Huan Chen June 3, 2016 Knoxville, TN iv ABSTRACT Hydraulic fracturing has promoted the exploitation of natural gas in the United States (U.S.). However, the storing and emptying of chemical additives in hydraulic fracturing wells may pose adverse effects through inhalation exposures. Based on the information about hydraulic fracturing fluids, this study investigated: 1) water volumes used to mix chemical additives for making up the hydraulic fracturing fluids; 2) chemical species, concentrations and their degradability in the hydraulic fracturing fluids; 3) emissions of organics from chemical storage tanks; and 4) the occupational inhalation exposures by toxic and organic vapors. Results shows for 80,047 wells fractured between 2008 and 2014 and located in the 14 states studied, the highest total amount of water was consumed in Texas with 457.42 Mm3 of water used to fracture 40,521 wells; followed by Pennsylvania with 108.67 Mm3 of water used to treat 5,127 wells. For 5,071 wells completed in 2008 through July 2014 and located in the Marcellus Shale Formation, there were totally 517 chemicals introduced into the hydraulic fracturing fluids. Although most of the added chemicals can be removed with the appropriate treatments, the degradation of some chemicals would produce more toxic and persistent degradation produces. For 72,023 out of 80,047 wells, the median daily emission values were 0.221 kg d-1 per well. Those emissions were primarily contributed by the non-methane volatile organic compounds (NMVOCs). Furthermore, 95.14% of emissions caused by all NMVOCs were due to 60 NMVOCs which belong to the 847 candidate substances for the Priority List of Hazardous Substances defined by Agency for Toxic Substances & Disease Registry (ATSDR) in 2011. Results shows there were 2,893, 8, 4,415, and 2,992 out of 60,644 wells with the possibilities of the acute exposure for non-cancer risks, the chronic exposure for non-cancer risks, the acute exposure for cancer risks, and the chronic exposure for cancer risks on workers. Methanol was the major organic causing the acute exposure for non-cancer risks in hydraulic fracturing. Formaldehyde was the dominant contributor to both the acute and chronic exposures for cancer risks. v TABLE OF CONTENTS Chapter 1 Introduction ............................................................................................................................... 1 1.1. Background ................................................................................................................................ 2 1.2. Objectives, Hypothesis and Studies ......................................................................................... 7 1.3. Data Source .............................................................................................................................. 11 Chapter 2 Water usage for natural gas production through hydraulic fracturing in the United States from 2008 to 2014 ...................................................................................................................................... 12 2.1. Abstract .................................................................................................................................... 13 2.2. Introduction ............................................................................................................................. 14 2.2.1. Background ..................................................................................................................... 14 2.2.2. Motivations and hypothesis ............................................................................................ 16 2.2.3. Summary.......................................................................................................................... 16 2.3. Database and Tools .................................................................................................................. 18 2.4. Results and Discussion ............................................................................................................ 21 2.4.1. Volume of Water Use and Vertical Depth in Hydraulic Fracturing .......................... 21 2.4.2. Components of Water Use in Hydraulic Fracturing ................................................... 28 2.5. Conclusions and Future works ............................................................................................... 34 Chapter 3 Characterization of the Chemicals Used Hydraulic Fracturing Fluids for Wells Located in the Marcellus Shale Play .......................................................................................................................... 36 3.1. Abstract .................................................................................................................................... 37 3.2. Introduction ............................................................................................................................. 38 3.2.1. Background ..................................................................................................................... 38 3.2.2. Motivations and hypothesis ............................................................................................ 39 3.2.3. Summary.........................................................................................................................
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