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Reconstructing Early Industrial Contributions to Legacy Trace Metal Contamination in Southwestern Pennsylvania Robert James Rossi, Daniel J. Bain, Aubrey L. Hillman, David P. Pompeani, Matthew S Finkenbinder, and Mark B. Abbott Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.6b03372 • Publication Date (Web): 31 Mar 2017 Downloaded from http://pubs.acs.org on April 2, 2017
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Reconstructing Early Industrial Contributions to Legacy Trace Metal Contamination in Southwestern Pennsylvania
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Robert J. Rossi*,1, Daniel J. Bain1, Aubrey L. Hillman,2, David P. Pompeani1, Matthew S. Finkenbinder1,3, Mark B. Abbott1,
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Department of Geology and Environmental Science, University of Pittsburgh, Pittsburgh, PA 15260 School of Geosciences, University of Louisiana at Lafayette, Lafayette, LA 70503 3 Department of Environmental Engineering & Earth Sciences, Wilkes University, Wilkes-Barre, PA 18766 2
TOC/Abstract Art
Abstract: Early industrial trace metal loadings are poorly characterized, but potentially substantial sources of trace metals to the landscape. The magnitude of legacy contamination in Southwestern Pennsylvania, the cradle of North American fossil fuel industrialization, is reconstructed from trace metal concentrations in a sediment core with proxies including major and trace metal chemistry, bulk density, and magnetic susceptibility. Trace metal chemistry in this sediment record reflects 19th and 20th century land use and industry. In particular, early 19th century arsenic loadings to the lake are elevated from pesticides used by early European settlers at a lakeside tannery. Later, sediment barium concentrations rise, likely reflecting the onset of acidic mine drainage from coal operations. Twentieth century zinc, cadmium, and lead concentrations are dominated by emissions from the nearby, infamous, Donora Zinc Works, yet record both the opening of a nearby coal-fired power plant and amendments to the Clean Air Act. The impact of early industry is substantial and rivals more recent metal fluxes, resulting in a significant potential source of contaminated sediments. Thus, modern assessments of trace metal contamination cannot ignore early industrial inputs as the potential remobilization of legacy contamination would impact ecosystem and human health.
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Introduction Human activities have increased trace metal inputs to the environment, primarily via modern
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vehicular and industrial emissions.1,2 In particular, trace metal loadings from metallurgical facilities3–5 are
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relatively well characterized. However, trace metal loadings from early and pre-industrial activities,
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though also potential sources of trace metal inputs, are poorly characterized. Specifically, while the use
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of trace metals in early human activities is noted (e.g., arsenic use in historical leather tanning),6 the
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magnitude and distribution of contamination associated with these activities is often unknown.
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Furthermore, the sequential input of trace metal contamination from multiple industries (e.g., leather
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tanneries, metallurgical facilities, coal-fired power stations) accumulates. Consequently, elevated trace
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metal loadings often stretch beyond the lifespan of a single pollution source and can result in a
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significant amount of trace metal contamination that is challenging to detect.
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Alluvial and lacustrine sediments can accumulate trace metals,7–9 and by extension, record
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periods of significant trace metal contamination.10–13 However, the accumulation of trace metals in
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alluvial systems results in a reservoir of contamination with a strong potential for mobilization as alluvial
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processes continue.10,14–17 Moreover, potential changes in global precipitation patterns will likely
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increase the probability of extreme precipitation events18 and increase rates of alluvial processes such as
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bank erosion.19 Thus, changing climate can increase mobilization of contaminated sediments and
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therefore characterization of legacy trace metal contamination will inform adaptive catchment water
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quality protection frameworks.
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This study reconstructs substantial trace metal contamination from early industrial activities
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using a lake sediment record from an oxbow lake in Southwestern Pennsylvania, USA. Specifically, we
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characterize trends in trace metal loadings from changes in land use and industry in the 19th and 20th
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centuries by examining major and trace metal chemistry, bulk density, and magnetic susceptibility in an
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approximately 210 year lake sediment record (169 cm). Additionally, we combine historical
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documentation and elemental molar ratios to identify principal sources of trace metal content. This
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reconstruction also documents modern trace metal contamination from the Donora Zinc Works, a
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notorious environmental polluter.20 More importantly, this study highlights the potential for
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accumulation of complicated mixes of trace metal contaminants in alluvial sediments. As industry and
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industrial hygiene have evolved, waste materials have also evolved.
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Study Location and Methods
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In September 2014, three adjacent sediment cores (C14, D14, E14) were collected from an
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unnamed oxbow lake hereafter referred to as Markle Lake (Figure S1). Water depth at the coring sites
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was 1.06 m (Figure S1b, circle). Because sites C14, D14, and E14 are separated by
