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Occurrence and behavior of uranium and thorium series radionuclides in the Permian shale hydraulic fracturing wastes

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Abstract

Over the last decade, there has been a rapid growth in the use of hydraulic fracturing (fracking) to recover unconventional oil and gas in the Permian Basin of southeastern New Mexico (NM) and western Texas. Fracking generates enormous quantities of wastes that contain technologically enhanced naturally occurring radioactive materials (TENORM), which poses risks to human health and the environment because of the relatively high doses of radioactivity. However, very little is known about the chemical composition and radioactivity levels of Permian Basin fracking wastes. Here, we report chemical as well as radiochemical compositions of hydraulic fracking wastes from the Permian Basin. Radium, the major TENORM of interest in unconventional drilling wastes, varied from 19.1 ± 1.2 to 35.9 ± 3.2 Bq/L for 226Ra, 10.3 ± 0.5 to 21.5 ± 1.2 Bq/L for 228Ra, and 2.0 ± 0.05 to 3.7 ± 0.07 Bq/L for 224Ra. In addition to elevated concentrations of radium, these wastewaters also contain elevated concentrations of dissolved salts and divalent cations such as Na+ (31,856–43,000 mg/L), Ca2+ (668–4123 mg/L), Mg2+ (202–2430 mg/L), K+ (148–780 mg/L), Sr2+ (101–260 mg/L), Cl (5160–66,700 mg/L), SO42− (291–1980 mg/L), Br (315–596 mg/L), SiO2 (20–32 mg/L), and high total dissolved solid (TDS) of 5000–173,000 mg/L compared to background waters. These elevated levels are of radiological significance and represent a major source of Ra in the environment. The recent discovery of large deposits of recoverable oil and gas in the Permian Basin will lead to more fracking, TENORM generation, and radium releases to the environment. This paper evaluates the potential radiation risks associated with TENORM wastes generated by the oil and gas recovery industry in the Permian Basin.

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References

  • Al-Masri MS (2006)  Spatial and monthly variations of radium isotopes in produced water during oil production monthly variations of radium isotopes in produced water during oil production. Appl Radiat Isot 64:615–623

  • Ali K (2017) Radiological hazard Assessment Due to Natural Occurring Radioactive Materials (NORM) in Oil and Gas Production Industry East Baghdad Oil Field. Iraqi J Sci 58:115–126

  • API (2000) Overview of exploration and production waste volumes and waste management practices in the United States, prepared by ICF Consulting for the American Petroleum Institute. DC, May, Washington

    Google Scholar 

  • ASER (2016) Waste isolation pilot plant annual site environmental report for 2016. DOE/WIPP-17–3591. www.wipp.energy.gov/library/aser/DOE. Accessed May 2021

  • ATWIR - Annual Transuranic Waste Inventory Report (2020) DOE/TRU-20–3425 Revision 0 November 2020. U.S. Department of Energy Carlsbad Field Office

  • Avwiri GO, Esi E, Agbalagba EO (2013) Gamma spectroscopy analysis of produced water from selected flow stations in Delta State, Nigeria. Int J Environ Monit Anal 1:167–174

    CAS  Google Scholar 

  • Barbot E, Vidic NS, Gregory KB, Vidic RD (2013) Spatial and temporal correlation of water quality parameters of produced waters from Devonian-Age shale following hydraulic Fracturing. Environ Sci Technol 47:2562–2569

    Article  CAS  Google Scholar 

  • Botezatu E, Grecea C (2004) Radiological impact assessment on behalf of oil/gas industry. J Prev Med 12:16–21

    Google Scholar 

  • CEMRC- Carlsbad Environmental Monitoring and Research Center 1998 Report Carlsbad, NM. Accessed April 2021

  • CEMRC- Carlsbad Environmental Monitoring and Research Center Annual Report 1999–2018. http://www.cemrc.org/annualreport. Accessed June 2021

  • Center for Wearwern Priorities New Mexico Oil and gas Spill tracker. http://westernpriorities.org. Accessed October 2021

  • Chapman JB (1988). Chemical and radiochemical characteristics of groundwater in the culebra dolomite, Southeastern New Mexico. Environmental Evaluation Group, EEG Report 39. DOE/AL/10752–39.

  • DOE/WIPP-92-037 (1992) Statistical summary of the radiological baseline for the waste isolation pilot plant. Waste Isolation Pilot Plant, Carlsbad NM

  • Eriksen DO, Sidhu R, Stralberg E (2006) Radionuclides in produced water from Norwegian oil and gas installations-concentrations and bioavailability. Czechoslovak J Phys 56:D43–D48

    Article  CAS  Google Scholar 

  • Fisher RS (1998) Geologic and geochemical controls on naturally occurring radioactive materials (NORM) in produced water from oil, gas, and geothermal operations. Environ Geosci 5:139–150

    Article  Google Scholar 

  • Fleischer RL (1980) Isotopic disequilibrium of uranium: ALPHA-recoil damage and preferential solution effects. Science 207:979–981

    Article  CAS  Google Scholar 

  • Frazier JR (2015) Characterization of naturally occurring radioactive materials and radiological conditions in the oil and gas field. Marcellus Shale Coalition Pittsburgh, Pennsylvania 15241. from geochemical and isotopic tracers. Appl Geochem 38:161–175

    Google Scholar 

  • Gadeken LL (1989) Radioactive well logging method, Patent EP 89304075-A

  • Gaswirth SB, French KL, Pitman JK, Marra KR, Mercier TJ, Leathers-Miller HM, Schenk CJ, Tennyson ME, Woodall CA, Brownfield ME, Finn TM, Le PA (2018) Assessment of undiscovered continuous oil and gas resources in the Wolfcamp Shale and Bone Spring Formation of the Delaware Basin, Permian Basin Province, New Mexico and Texas, 2018: U.S. Geological Survey Fact Sheet 2018–3073, 4 p., https://doi.org/10.3133/fs20183073.

  • Guerin (2014). Permian Basin: America’s newest fracking boom where there's not much water. High Country News.

  • Hajer H-E- B, Baccouche S (2013) Evaluation of radiological impacts of TENORM in the Tunisian petroleum industry. J Environ Radioact 115:107–113

    Article  Google Scholar 

  • Hamilton LD, Meinhold AF, Nagy J (1991) Produced water radionuclide hazard/risk assessment -phase I Report, prepared for the American Petroleum Institute, Washington, D.C. Brookhaven National Laboratory, BNL 47403

  • Hancock GJ, Murray AS (1996) Source and distribution of dissolved radium in the Bega River estuary, southeastern Australia. Earth Planet Sci Lett 138:45–155

    Article  Google Scholar 

  • Herczeg AL, Simpson JH, Anderson RF, Trier RM, Gathieu GG, Deck BL (1988) Uranium and radium mobility in groundwaters and brines within the delaware basin, Southeastern New Mexico, USA. Chem Geol 72:181–196

  • Hrichi H, Baccouche S, Belgaied (2013) Evaluation of radiological impacts of TENORM in the Tunisian petroleum industry. 115:107–113

  • Inn K, Hall E, Woodward J, Stewart B, Pollanen R, Selvig L, Turner S, Outola I, Nour S, Kurosaki H, Larosa J, Schultz M, Lin Z, Yu Z, McMahon C (2008) Use of thin collodion films to prevent recoil-ion contamination of alpha-spectrometry detectors. J. Radioanal. Nucl. Chem. 276:385–390

    Article  CAS  Google Scholar 

  • Jodłowski CNDP, Macuda J, Nowak J (2017) Radioactivity in wastes generated from shale gas exploration and production North Eastern Poland. J Environ Radioact 175(176):34–38

    Article  Google Scholar 

  • Jonkers G, Hartog FA, Knaepen WAI, Lancée PFJ (1997) Characterization of NORM in oil & gas production (E&P) industry. In: International Symposium on Radiological Problems with Natural Radioactivity in the Non-nuclear Industry, Amsterdam, The Netherlands, September.

  • Kondash AJ, Albright E, Vengosh A (2017) Quantity of flowback and produced waters from unconventional oil and gas exploration. Sci Tot Environ 574:314–321

    Article  CAS  Google Scholar 

  • Kondash AJ, Lauer NE, Vengosh A (2018) The intensification of the water footprint of hydraulic fracturing. Sci Adv 4:5982

    Article  Google Scholar 

  • Kpeglo DO, Mantero J, Darko EO, Emi-Reynolds G, Faanu A, Manjon G, Vioque I, Akaho EHK, Garcia-Tenorio R (2016) Radiochemical characterization of produced water from twoproduction offshore oilfield In Ghana. J Environ Radioact 152:35–45

    Article  CAS  Google Scholar 

  • Kraemer TF, Reid DF (1984) The occurrence and behaviour of radium in saline formation water of the U.S. Gulf Coast Region. Isot Geosci 2:153–174

    CAS  Google Scholar 

  • Lagera L, Hart A, Graham B (1999) Radionuclides in oil and gas operational discharges and environmental samples associated with offshore oil and gas production facilities. I: Continental Shelf Associates, Inc. Radionuclides, metals, and hydrocarbons in oil and gas operational discharges and environmental samples associated with offshore production facilities on the Texas/Louisiana continental shelf with an environmental assessment of metals and hydrocarbons. Prepared for U.S. Department of Energy. (DOE/MT/92001–23). Tulsa, OK (US): National Petroleum Technology Office, chapter 6.

  • Langmuir D, Herman JS (1980) The mobility of thorium in natural waters at low temperatures. Geochim Cosmochim Acta 44:1753–1766

    Article  CAS  Google Scholar 

  • Lauer NE, Harkness JS, JS, Vengosh A, (2016) Brine spills associated with unconventional oil development in North Dakota. Environ, Sci Technol 50:5389–5397

    Article  CAS  Google Scholar 

  • Luisa Torres L, Yadav OP, Khan E (2018) Risk assessment of human exposure to Ra-226 in oil produced water from the Bakken Shale. Sci Total Environ 626:867–874

    Article  Google Scholar 

  • McMahon PB, Kulongoski JT, Vengosh A, Cozzarelli IM, Matthew K, Landon MK, Kharaka YK, Gillespie JM, Davis TA (2018) Regional patterns in the geochemistry of oil-field water, southern San Joaquin Valley, California, USA. Appl Geochem. 98:127–140

    Article  CAS  Google Scholar 

  • Melson NH, Haliena BP, Kaplan DI, Barnett MO (2012) Adsorption of tetravalent thorium by geomedia. Radiochim Acta 100:827–832

    Article  CAS  Google Scholar 

  • Moater F, Shadizadeh SR, Karbassi AR, Ardalani E, Akbari Derakhshi R, Asadi M (2010) Determination of naturally occurring radioactive materials (NORM) in formation water during oil exploration. J Radioanal Nucl Chem 283:3–7

    Article  CAS  Google Scholar 

  • Nabhani Khalid AL, Khan F, Yang M (2016) Technologically enhanced naturally occurring radioactive materials in oil and gas production: a silent killer. Process Saf Environ 99:237–247

    Article  Google Scholar 

  • National Research Council (1996) The Waste Isolation Pilot Plant: A Potential Solution for the Disposal of Transuranic Waste. The National Academies Press, Washington, DC. https://doi.org/10.17226/5269

    Book  Google Scholar 

  • National Research Council (2006) Health Risks from Exposure to Low Levels of Ionizing Radiation: BEIR VII Phase 2. The National Academies Press, Washington, DC. https://doi.org/10.17226/11340

    Book  Google Scholar 

  • Neff JM, Foster K (1997) Composition, Fates, and effects of Produced Water Discharges to Offshore Waters of the Java Sea, Indonesia. Report to Pertimena/Maxus, Jakarta, Indonesia

  • Nelson AW, May D, Knight AW, Eitrheim ES, Mehrhoff M, Shannon R, Litman R, Schultz MK (2014) Matrix complications in the determination of radium levels in hydraulic fracturing flowback water from Marcellus Shale. Environ Sci Technol Lett 1:204–208

    Article  CAS  Google Scholar 

  • Nelson AW, Eitrheim ES, Knight AW, May D, Mehrhoff MA, Shannon R, Litman R, Burnett WC, Forbes TZ, Schultz MK (2016) Understanding the radioactive ingrowth and decay of naturally occurring radioactive materials in the environment: an analysis of produced fluids from the Marcellus Shale Environ. Health Perspectives 123:689–696

    Article  Google Scholar 

  • NRPA (Norwegian Radiation Protection Authority) (2004) Natural radioactivity in produced water from the Norwegian oil and gas industry in 2003. Stråralevern Rapport 2005:2

    Google Scholar 

  • Osmond JK, Cowart JB, Ivanovich M (1983) Uranium isotopic dis-equilibrium in ground water as an indicator of anomalies. Int J Appl Radiat Isot 34:283–308

    Article  CAS  Google Scholar 

  • Plyatsuk LD, Burla OA, Yu AI, Hurets LL, Roy IO (2017) Investigation of produced waters radioactivity of oil and gas deposits in the Dnieper-Donets province. J Eng Sci 4:G17–G21

    Article  Google Scholar 

  • Rowan EL, Engle MA, Kirby CS, Kraemer TF (2011). Radium content of oil- and gas-field produced waters in the Northern Appalachian Basin (USA): summary and discussion of data. Scientific Investigations Report 2011–5135. Available: http://pubs.usgs.gov/sir/2011/5135/pdf/sir2011–5135.pdf

  • Schmidt HW, Kurz K (1906) Natural radioactive substances in thermal brines. Phys Z 7:213–224

    Google Scholar 

  • Scott III GL (1995) US Patent No. US5441110: System and method for monitoring fracture growth during hydraulic fracture treatment. US Patent Publications

  • Scott III GL (1997) US Patent No. 5635712: Method for monitoring the hydraulic fracturing of a subterranean formation. US Patent Publications

  • Shawky S, Amer H, Nada AA, El-Maksoud TMA, Ibrahiem NM (2001) Characteristics of NORM in the oil industry from eastern and western deserts of Egypt. Appl Radiat Isot 55:135–139

    Article  CAS  Google Scholar 

  • Sill C (1974) Purification of radioactive tracers for use in high sensitivity alpha spectrometry. Anal Chem 46:1426–1431

    Article  CAS  Google Scholar 

  • Strand T, Lysebo I, Kristensen D, Birovljev A (1997) Deposits of naturally occuring radioactivity in production of oil and natural gas. NRPA report 1997:1. Østerås, Norwegian Radiation Protection Authority, 1997

  • Thakur P, Ward AL (2019) Sources and distribution of 241Am in the vicinity of a deep geologic repository. Environ Sci Pollut Res 26:2328–2344

    Article  CAS  Google Scholar 

  • Thakur P, Ward AL (2020) 210Po in the environment: insight into the naturally occurring polonium isotope. J Radioanal Nucl Chem 323:27–49

  • Tufail M (2012) Radium equivalent activity in the light of UNSCEAR report. Environ Monit Assess 184:5663–5667

    Article  CAS  Google Scholar 

  • UNSCEAR (2000) Sources and effects of ionizing radiation. United Nations Scientific Committee on the Effects of Atomic Radiation. Report to the General Assembly, with scientific annexes. New York: United Nations.

  • USDOE-U. S. Department of Energy (2011) Available online: http://www.statista.com/statistics/250408/flowback-water-salinity-from-different-us-shales-by-tds-concentration/

  • USNRC (2010) U.S. nuclear regulatory commission. “CFR – code of federal regulations title 4249 10 part 20 standards for protection against radiation.” https://www.nrc.gov/reading-rm/doc-collections/cfr/. Accessed 27 April 2021. (U.S. Government Printing Office, 4251 Washington, DC)

  • USNRC (2018) Consolidated guidance about materials licenses: program-specific guidance about well logging, tracer, and field flood study licenses (NUREG-1556, Volume 14, Revision 1). Office of Nuclear Material Safety and Safeguards U.S. Nuclear Regulatory Commission Washington, DC 20555–0001

  • US Environmental Protection Agency (2000) National Water Quality Inventory Report to Congress, Washington DC 20460

  • Vegueria JSF, Godoy JM, Miekeley N (2002) Environmental impact studies of barium and radium discharges by produced waters from the “Bacia de Campos” oil field offshore platforms, Brazil. J Environ Radioact 62:23–38

    Google Scholar 

  • Vengosh A, Hirschfeld D, Vinson D, Dwyer G, Raanan H, Rimawi O, Al-Zoubi A, Akkawi E, Marie A, Haquin G, Zaarur S, Ganor J (2009) High naturally occurring radioactivity in fossil groundwater from the Middle East. Environ Sci Technol 43:1769–1775

    Article  CAS  Google Scholar 

  • Vinson DS, Tagma T, Bouchaou L, Dwyer GS, Warner NR, Vengosh A (2013) Occurrence and mobilization of radium in fresh to saline coastal groundwater inferred radioactive material at US Geological Survey research site B. Appl Geochem 22:2125–2137

    Google Scholar 

  • Walter GR, Benke RR, Pickett DA (2012) Effect of biogas generation on radon emissions from landfills receiving radium-bearing waste from shale gas development. J Air Waste Manage Assoc 62:1040–1049

    Article  CAS  Google Scholar 

  • Waste Isolation Pilot Plant (WIPP)- Site Enviromental Report for the calender year 1995. DOE/WIPP 96–2182

  • Zhang T, Bain D, Hammack R, Vidic RD (2015) Analysis of radium-226 in high salinity wastewater from unconventional gas extraction by inductively coupled plasma-mass spectrometry. Environ Sci Technol 49:2969–2976

    Article  CAS  Google Scholar 

  • Zhang T (2015) Origin and fate of radium in flowback and produced water from Marcellus shale gas exploration. PhD thesis , University of Pittsburgh.

  • Zielinski RA, Budahn JR (2007) Mode of occurrence and environmental mobility of oil-field radioactive material at US Geological Survey research site B. Appl Geochem 22:2125–2137

    Article  CAS  Google Scholar 

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Acknowledgements

This research is supported by a grant from the US Department of Energy, Carlsbad Field Office of DOE through Grant No. DE-EM 0005159. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the sponsors.

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The project is funded by the US Department of Energy (USDOE) through a grant.

US-DOE, Grant No. DE-EM 0005159

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All authors contributed to the study’s conception and design. Punam Thakur: investigation, method development, writing, and data curation; Anderson L Ward: writing, article review, and graphics; Tanner M. Schaub: sample collection and article review.

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Correspondence to Punam Thakur.

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Thakur, P., Ward, A. & Schaub, T. Occurrence and behavior of uranium and thorium series radionuclides in the Permian shale hydraulic fracturing wastes. Environ Sci Pollut Res 29, 43058–43071 (2022). https://doi.org/10.1007/s11356-021-18022-z

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