Alpha Recoil Flux of Radon in Groundwater and its Experimental Measurement

Groundwater Radon (Rn222) activity is primarily controlled by alpha recoil process (radioactive decay), however, evaluating the rate and extent of this process, and its impact on porewater radioactivity, remains uncertain. Numerous factors contribute to this uncertainty, including the spatial distribution of parent radionuclides (e.g. U238, Th232 , Ra226 and Ra228) within native materials, differences in nuclide recoil length in host matrix and the physical structure of the rock strata (pore size distribution and porosity). Here, we experimentally measure Radon activities within porewater contributed through alpha recoil, and analyze its variations as a function of pore structure and parent nuclide distribution within host matrices, including Marcellus shale rock and Serrie-Copper Pegmatite. The shale cores originate from the Marcellus formation in Mckean, Pennsylvania collected at depths ranging from 1000-7000 feet, and the U-Th-rich Pegmatite is obtained from South Platte District, Colorado. Columns are packed with granulated rock of varying surface area (30,000-60,000 cm2/g) and subjected to low salinity sodium chloride solution in a close loop configuration. The activity of Radon (Rn222) and radium (Ra226) in the saline fluid is measured over time to determine recoil supply rates. Mineralogical and trace element data for rock specimens are characterized using XRD and XRF, and detailed geochemical profiles are constructed through total dissolution and analysis using ICP-MS and ICP-OES. Naturally occurring Radium nuclides and its daughters are quantified using a low-energy Germanium detector. The parent nuclide (U238 and Th232) distribution in the host rock is studied using X-Ray Absorption Spectroscopy (XAS). Our study elucidates the contribution of alpha recoil on the appearance and distribution of Radon (Rn222) within porewater of representative rock matrices. Further, we illustrate the effects of chemical and physical heterogeneity on the rate of this process, which may inform models predicting the fate and transport of radionuclides in subsurface environments.