Natural attenuation of dissolved petroleum fuel constituents in a fractured Chalk aquifer: Contaminant mass balance with probabilistic analysis

A plume-scale mass balance is developed to assess the natural attenuation (NA) of dissolved organic contaminants in fractured, dual porosity aquifers. This methodology can be used to evaluate contaminant distribution within the aquifer, plume source term, contaminant biodegradation and plume status. The approach is illustrated for a site on the UK Upper Chalk aquifer impacted by petroleum fuel containing MTBE and TAME. Variability in site investigation data and uncertainty in the mass balance was assessed using probabilistic analysis. The analysis shows that BTEX compounds are biodegraded primarily by denitrification and sulphate reduction in the aquifer, with an equivalent plume-scale first-order biodegradation rate of 0.49 year-1. Other biodegradation processes are less important. Sorption contributes to hydrocarbon attenuation in the aquifer but is less important for MTBE and TAME. Uncertainty in the plume source term and site hydrogeological parameters had the greatest effect on the mass balance. The probabilistic analysis enabled the most likely long-term composition of the plume source term to be deduced and provided a site-specific estimate of contaminant mass flux for the prediction of plume development. The mass balance methodology provides a novel approach to improve NA assessments for petroleum hydrocarbons and other organic contaminants in these aquifer settings.