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A suite of road sediment and soil samples from a post-industrial city (Detroit, MI) were collected and analyzed for atmospherically-delivered Pb, Po, Be along with Ra and Cs in the bulk and size-fractionated solid samples. From the measured atmospheric depositional fluxes of Be, Po, and Pb, the initial Po/Pb activity ratio was quantified. In all samples, there is disequilibrium between Po and Pb, with a Po/Pb activity ratio (AR) of <1.0, which is reported for the first time. Using the measured Po/Pb AR, the average 'apparent age' of road sediment was found to be 146 ± 62 days. Using numerical modeling, it is predicted that the (Po/Pb) excess activity ratio will reach a 'dynamic equilibrium' value of ~0.59 over a period of >1 year. Results from a subset of samples that were sequentially extracted for exchangeable, carbonate, Fe-Mn oxide, organic and residual phases indicate the Fe-Mn oxide fraction was found to contain the largest fraction of Be and Pb; however, the largest fraction of Pb was associated with the residual phase and is attributed to complexation of Pb with recalcitrant organic matter. This study shows that the natural tagging of Be and Po-Pb pair via precipitation provides insights on the time scale of their mobility and adds a new dimension of time information on the pollutant-laden road sediment.
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| http://dx.doi.org/10.1016/j.scitotenv.2023.164738 | DOI Listing |
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