Physicochemical heterogeneity controls on uranium bioreduction rates at the field scale.

It has been demonstrated in laboratory systems that U(VI) can be reduced to immobile U(IV) by bacteria in natural environments. The ultimate efficacy of bioreduction at the field scale, however, is often challenging to quantify and depends on site characteristics. In this work, uranium bioreduction rates at the field scale are quantified, for the first time, using an integrated approach. The approach combines field data, inverse and forward hydrological and reactive transport modeling, and quantification of reduction rates at different spatial scales. The approach is used to explore the impact of local scale (tens of centimeters) parameters and processes on field scale (tens of meters) system responses to biostimulation treatments and the controls of physicochemical heterogeneity on bioreduction rates. Using the biostimulation experiments at the Department of Energy Old Rifle site, our results show that the spatial distribution of hydraulic conductivity and solid phase mineral (Fe(III)) play a critical role in determining the field-scale bioreduction rates. Due to the dependence on Fe-reducing bacteria, field-scale U(VI) bioreduction rates were found to be largely controlled by the abundance of Fe(III) minerals at the vicinity of the injection wells and by the presence of preferential flow paths connecting injection wells to down gradient Fe(III) abundant areas.