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Physical and Chemical Interactions Affecting U and V Transport from Mine Wastes Sumant Avasarala

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Physical and Chemical Interactions Affecting U and V Transport from Mine Wastes Sumant Avasarala University of New Mexico UNM Digital Repository Civil Engineering ETDs Engineering ETDs Spring 3-2-2018 Physical and Chemical Interactions Affecting U and V Transport from Mine Wastes Sumant Avasarala Follow this and additional works at: https://digitalrepository.unm.edu/ce_etds Part of the Environmental Engineering Commons Recommended Citation Avasarala, Sumant. "Physical and Chemical Interactions Affecting U and V Transport from Mine Wastes." (2018). https://digitalrepository.unm.edu/ce_etds/205 This Dissertation is brought to you for free and open access by the Engineering ETDs at UNM Digital Repository. It has been accepted for inclusion in Civil Engineering ETDs by an authorized administrator of UNM Digital Repository. For more information, please contact [email protected]. Sumant Avasarala Candidate Civil Engineering Department This dissertation is approved, and it is acceptable in quality and form for publication: Approved by the Dissertation Committee: Dr. Jose M. Cerrato , Chairperson Dr. Ricardo Gonzalez Pinzon Dr. Bruce Thomson Dr. Adrian Brearley Dr. Mehdi Ali i Sumant Avasarala B.S., Chemical Engineering, Anna University 2009, India M.S., Chemical Engineering, Wayne State University, 2012, U.S. DISSERTATION Submitted in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy Engineering The University of New Mexico Albuquerque, New Mexico May 2018 ii Dedication I would like to dedicate my PhD to my parents (Seshargiri Rao and Radha), my brother (Ashwin Avsasarala), my friends, and my grandfathers (V.V. Rao and Late Chalapathi Rao) without whose blessings, prayers, and support this journey would have never been possible. Special dedication to my best friend, Dr. Sriraam Ramanathan Chandrasekaran, who guided me and supported me through my rough times. I couldn’t think of a better way to indicate your role in my life than dedicating my biggest achievement to you! Thank you for always being there! iii Acknowledgement I never will have enough words to express my gratitude and gratefulness towards my advisor, Dr. José Cerrato, who offered me a PhD position despite many red flags on the way. His exceptional support, advisement, and love for his students (in this case, me) has always kept me driven and motivated—so motivated that it has finally allowed me to see light towards the end of a long, cheerful, fun, and challenging PhD tunnel. Thank you very much, José, for transforming me from a naïve graduate student to an eligible independent researcher. I really appreciate it! I am forever in your debt! Of course next on my list is Dr. Mehdi Ali for his continuous “It’s working, it’s not.” There is not a day when I have not felt I could talk to you about any challenge that I ran into. You have always comforted, guided, and supported me in both on a professional and personal level. I have relished all moments spent with you from the weekend brunches (green Chile cheese omelets) to all the laughs we shared. Thank you very much, Dr. Ali, for making my journey a lot more memorable and fun. I am also very thankful to my committee members Dr. Ricardo Gonzalez, Dr. Adrian Brearley, and Dr. Bruce Thomson for all their help, guidance, and support during my PhD research. I am also very thankful to all my co-authors without whose efforts reaching this point would have been extremely difficult. Special thanks to Dr. Brearley for his patience towards my constant harassment for data. Finally, my acknowledgement would be incomplete without my friends and lab mates. I consider myself extremely lucky to have had the opportunity to pursue a PhD alongside such smart, supportive, and loving friends. You have always been there to cheer, hold, and encourage me during my difficult times. I have learned so much from all of you, and I wish the best for you all. Thank you. I have learned so much from each and every one of you that I am forever in your debt. I hope someday I can return the favor. iv Sumant Avasarala B.S., Chemical Engineering, Anna University 2009, India M.S., Chemical Engineering, Wayne State University, U.S. Abstract. This research investigates the physical and chemical interactions that affect the transport of uranium (U) and vanadium (V) from uranium mine waste sites by integrating laboratory experiments and reactive transport modelling with various spectroscopy, microscopy, and diffraction techniques. The document consists of results from three related studies. In the first study (Chapter 3), the reactive transport of U and V was investigated by sequentially reacting mine wastes collected from Blue Gap/Tachee Claim-28 mine site, AZ with 10mM NaHCO3 (7.9) and 10mM CH3COOH (3.4) during continuous flow through column experiments. Under both of these conditions (pH 3.4 and 7.9), dissolution of U-V bearing minerals predominant at the site were identified as a key mechanism affecting the reactive transport of U and V. The equilibrium (Keq) and reaction rate constants (km) for U-V bearing mineral dissolution were estimated to be Keq -44.81 -13 -2 -1 -38.65 = 10 and km = 4.8x10 mol cm sec at circumneutral conditions, and Keq = 10 -13 -2 -1 and km = 3.2x10 mol cm sec under acidic conditions. These results, coupled with electron microscopy data, suggest that the release of U and V is affected by difference in v solution pH and crystalline structure of U-V bearing minerals. Identifying the crystal chemistry of these U-V bearing minerals was the task in the second study (Chapter 4) of the dissertation. Using various diffraction and microscopy tools, the U-V bearing minerals were identified as hydrated carnotite. Finally, the mobility of U from co-occurring submicron U(IV) and U(VI) mineral phases in mine wastes from the Jackpile mine in Laguna Pueblo, NM was investigated under oxidizing conditions. Co-occurrence of U(VI) and U(IV) at a 19:1 ratio mostly as coffinite (USiO4) and U-phosphate was observed in these mine waste solids. The highest U release from these mine wastes was observed during batch reactions with 10 mM NaHCO3 solution containing ambient dissolved oxygen concentrations. Results from these investigations provide an improved understanding on the role of thermodynamics, crystallinity, stoichiometry, and solution chemistry in the reactive transport of U and V from mine wastes that affect the water quality of surface and ground water resources. vi Physical and Chemical Interactions Affecting U and V Transport from Mine Wastes ....... i Physical and Chemical Interactions Affecting U and V Transport from Mine Wastes .......v 1 Table of Contents....................................................................................................... vii 2 List of Figures ...............................................................................................................x 3 List of Tables ........................................................................................................... xvii 1 Introduction ..................................................................................................................1 2 Literature Review .........................................................................................................4 Background and Significance................................................................................4 Study Areas: Blue Gap Tachee Claim-28, AZ and Jackpile-Paguate Mine, NM .6 State of the Knowledge about Processes Affecting U and V Transport from Mine Wastes .....................................................................................................................8 2.3.1 PFLOTRAN and Its Applications. ...............................................................10 2.3.2 Effect of Crystallinity on Metal Mobility. ...................................................11 Research Gap and Objectives ..............................................................................12 3 Reactive Transport of U and V from Abandoned Uranium Mine Wastes .................14 Abstract ...............................................................................................................14 Introduction .........................................................................................................15 Materials and Methods ........................................................................................18 3.3.1 Materials. .....................................................................................................19 3.3.2 Batch Experiments. ......................................................................................19 3.3.3 Continuous Flow Through Column Experiments. .......................................20 3.3.4 Aqueous Chemical Analyses. ......................................................................21 3.3.5 Reactive Transport Modelling. ....................................................................21 3.3.6 Solids Characterization. ...............................................................................23 Results and Discussion ........................................................................................24 3.4.1 Mine Waste Reactivity in Columns Using 18 MΩ Water (pH 5.4). ............24 3.4.2 Reactive Transport of U and V at Circumneutral pH. .................................25 3.4.3 Reactive transport of U and V at Acidic pH. ...............................................28 Environmental Implications. ...............................................................................32 4 Crystal chemistry of Uranyl Vanadates (Carnotite) in Mine Wastes .........................39
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