Radium Sorption to Iron (Hydr)oxides, Pyrite, and Montmorillonite: Implications for Mobility

摘要

Radium (Ra) is a radioactive element commonly found within soils, sediments, and natural waters. Elevated Ra activities arising through natural and anthropogenic processes pose a threat to groundwater resources and human health, and Ra isotope ratios are used to decipher groundwater movement, estimate submarine discharge flux, and fingerprint contamination associated with hydraulic fracturing operations. Although adsorption to metal (hydr)oxides and certain clay minerals is well established as a dominant mechanism controlling Ra transport and retention, the extent of Ra sorption to other minerals and under variable environmental conditions (e.g., pH and salinity) is limited. Accordingly, we present results of sorption studies and surface complexation modeling (SCM) of Ra to ferrihydrite, goethite, montmorillonite, and pyrite, for a range of pH values and common background cations. Ra sorption to all substrates is observed under geochemical conditions considered, but varies according to mineral, solution pH and specific competing cations. Literature derived SCMs for Ra sorption were fitted to match either sorption impacts due to pH or different background cations, but were not able to predict the impacts of different geochemical conditions. Despite this, the use of SCMs provided a more mechanistic understanding of Ra sorption as compared to commonly used distribution coefficients.