Time-integrated, Flux-based Monitoring Using Semipermeable Membrane Devices to Estimate the Contribution of Industrial Facilities to Regional Polychlorinated Biphenyl Budgets

Passive monitoring of polychlorinated biphenyls (PCB) using semipermeable membrane devices (SPMD) was employed to evaluate the contribution of point and nonpoint sources to the flux of PCB in a drainage system encompassing three U.S. Department of Energy (U.S. DOE) industrial and research facilities in eastern Tennessee, USA. Polychlorinated biphenyls concentrations were highest at outfalls containing process waste from the DOE industrial facilities. The significance of these releases was evaluated by calculating the PCB flux (mass per unit time) at different monitoring locations. The flux was calculated from the timeintegrated estimates of the aqueous concentrations of PCB and estimates of the volumetric flow rates of discharges and receiving streams during the deployment period. The DOE discharges accounted for most of the flux of PCB entering the Clinch River from the DOE drainage areas, but these sources constituted only 10% of the flux in the Clinch River about the DOE sources. Principal components analysis was helpful in attributing sources of PCB. In a stream receiving multiple inputs of PCB, congener profiles from upstream sources and discrete discharges were consistent with a mixture of those congener profiles in the downstream receiving water. In another stream with a single upstream source of PCB, changes in PCB flux and congener profiles suggested an apparent steady-state distribution between dissolved PCB and PCB adsorbed to organic matter on the streambed. The flux of dissolved PCB along different stream reaches reflected changes in the sediment organic content. Subtle alterations in congener profiles moving downstream suggested preferential desorption of less chlorinated congeners and sorption of more highly chlorinated congeners to sediment. Time-integrated, flux-based monitoring can be useful across a range of spatial scales for evaluating the significance of point and nonpoint contaminant sources and can help identify and prioritize feasible remedial alternatives. Keywords—Semipermeable membrane devices Polychlorinated biphenyls Principle components analysis Surface water Budget