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Naturally-occurring radioactive materials (NORM) associated with unconventional drilling produced fluids from the Marcellus Shale have raised environmental concerns. However, few investigations into the fundamental chemistry of NORM in Marcellus Shale produced fluids have been performed. Thus, we performed radiochemical experiments with Marcellus Shale produced fluids to understand the partitioning behavior of major radioelements of environmental health concern (uranium (U), thorium (Th), radium (Ra), lead (Pb), and polonium (Po)). We applied a novel radiotracer, (203)Pb, to understand the behavior of trace-levels of (210)Pb in these fluids. Ultrafiltration experiments indicated U, Th, and Po are particle reactive in Marcellus Shale produced fluids and Ra and Pb are soluble. Sediment partitioning experiments revealed that >99% of Ra does not adsorb to sediments in the presence of Marcellus Shale produced fluids. Further experiments indicated that although Ra adsorption is related to ionic strength, the concentrations of heavier alkaline earth metals (Ba, Sr) are stronger predictors of Ra solubility.

BACKGROUND: The economic value of unconventional natural gas resources has stimulated rapid globalization of horizontal drilling and hydraulic fracturing. However, natural radioactivity found in the large volumes of "produced fluids" generated by these technologies is emerging as an international environmental health concern. Current assessments of the radioactivity concentration in liquid wastes focus on a single element--radium. However, the use of radium alone to predict radioactivity concentrations can greatly underestimate total levels. OBJECTIVE: We investigated the contribution to radioactivity concentrations from naturally occurring radioactive materials (NORM), including uranium, thorium, actinium, radium, lead, bismuth, and polonium isotopes, to the total radioactivity of hydraulic fracturing wastes. METHODS: For this study we used established methods and developed new methods designed to quantitate NORM of public health concern that may be enriched in complex brines from hydraulic fracturing wastes. Specifically, we examined the use of high-purity germanium gamma spectrometry and isotope dilution alpha spectrometry to quantitate NORM. RESULTS: We observed that radium decay products were initially absent from produced fluids due to differences in solubility. However, in systems closed to the release of gaseous radon, our model predicted that decay products will begin to ingrow immediately and (under these closed-system conditions) can contribute to an increase in the total radioactivity for more than 100 years. CONCLUSIONS: Accurate predictions of radioactivity concentrations are critical for estimating doses to potentially exposed individuals and the surrounding environment. These predictions must include an understanding of the geochemistry, decay properties, and ingrowth kinetics of radium and its decay product radionuclides. [ABSTRACT FROM AUTHOR]