Nonlinear estimation of weathering rate parameters for uranium in surface soil near a nuclear facility

Abstract

A dynamic mass-balance model has been calibrated by a nonlinear parameter estimation method, using time-series measurements of uranium in surface soil near the former Feed Materials Production Center (FMPC) near Fernald, Ohio, USA. The time-series data, taken at six locations near the site boundary since 1971, show a statistically significant downtrend of above-background uranium concentration in surface soil for all six locations. The dynamic model is based on first-order kinetics in a surface-soil compartment 10 cm in depth. Median estimates of weathering rate coefficients for insoluble uranium in this soil compartment range from about 0.065–0.14 year -1, corresponding to mean transit times of about 7–15 years, depending on the location sampled. The model, calibrated by methods similar to those discussed in this paper, has been used to simulate surface soil kinetics of uranium for a dose reconstruction study. It was also applied, along with other data, to make confirmatory estimates of airborne releases of uranium from the FMPC between 1951 and 1988. Two soil-column models (one diffusive and one advective, the latter similar to a catenary first-order kinetic box model) were calibrated to profile data taken at one of the six locations in 1976. The temporal predictions of the advective model approximate the trend of the time series data for that location.