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A.R. Flegal

Publications and source records attributed to A.R. Flegal.

9 recordsLinked to original sources

Mercury contamination from historic mining in water and sediment, Guadalupe River and San Francisco Bay, California

The New Almaden mercury mines in California (USA), which collectively represent the largest historic producers of mercury in North America, are a persistent source of mercury contamination to the San Francisco Bay estuary. An estimate based on total mercury concentration (HgTOT) and provisional stream flow data measured at a gauging station in the Guadalupe River during base flow conditions yields a base flow flux of 30 g of mercury for the month of October 2000. In contrast to this base flow estimate, one 2-day rain event in October 2000 resulted in a flux of 22 g of mercury past this site. An estimate of mercury transport from the entire Guadalupe River watershed based on a sediment transport model and our measured suspended particulate HgTOT (0.5-4 ??g g-1) results in a total of 4-30 kg year-1 transported to the southern reach of the estuary. Sediments in the southern reach have lower HgTOT (most ??? 0.4 ??g g-1 dry wt) and monomethyl-mercury (MMHg, c. 1 ng g-1 dry wt) concentrations than those in the Guadalupe River (HgTOT, 0.41-33 ??g g-1 dry wt; MMHg, 1-10 ng g-1 dry wt). Because the most elevated methylmercury concentrations (8-12 ng g-1 dry wt) were found in sediments deposited immediately upstream of hydraulic structures (e.g. diversion dams and weirs) within the river, it is proposed that such physical structures may represent important zones of MMHg production and fluxes to San Francisco Bay.

Geochemistry: Exploration, Environment, Analysis↗

Mercury speciation and transport via submarine groundwater discharge at a southern California coastal lagoon system

We measured total mercury (HgT) and monomethylmercury (MMHg) concentrations in coastal groundwater and seawater over a range of tidal conditions near Malibu Lagoon, California, and used 222Rn-derived estimates of submarine groundwater discharge (SGD) to assess the flux of mercury species to nearshore seawater. We infer a groundwater-seawater mixing scenario based on salinity and temperature trends and suggest that increased groundwater discharge to the ocean during low tide transported mercury offshore. Unfiltered HgT (U-HgT) concentrations in groundwater (2.2–5.9 pM) and seawater (3.3–5.2 pM) decreased during a falling tide, with groundwater U-HgT concentrations typically lower than seawater concentrations. Despite the low HgT in groundwater, bioaccumulative MMHg was produced in onshore sediment as evidenced by elevated MMHg concentrations in groundwater (0.2–1 pM) relative to seawater (∼0.1 pM) throughout most of the tidal cycle. During low tide, groundwater appeared to transport MMHg to the coast, resulting in a 5-fold increase in seawater MMHg (from 0.1 to 0.5 pM). Similarly, filtered HgT (F-HgT) concentrations in seawater increased approximately 7-fold during low tide (from 0.5 to 3.6 pM). These elevated seawater F-HgT concentrations exceeded those in filtered and unfiltered groundwater during low tide, but were similar to seawater U-HgT concentrations, suggesting that enhanced SGD altered mercury partitioning and/or solubilization dynamics in coastal waters. Finally, we estimate that the SGD HgT and MMHg fluxes to seawater were 0.41 and 0.15 nmol m–2 d–1, respectively – comparable in magnitude to atmospheric and benthic fluxes in similar environments.

California↗

Mercury concentrations and loads in a large river system tributary to San Francisco Bay, California, USA

In order to estimate total mercury (Hg T ) loads entering San Francisco Bay, USA, via the Sacramento-San Joaquin River system, unfiltered water samples were collected between January 2002 and January 2006 during high flow events and analyzed for Hg T . Unfiltered Hg T concentrations ranged from 3.2 to 75 ng/L and showed a strong correlation (r 2 = 0.8, p < 0.001, n = 78) to suspended sediment concentrations (SSC). During infrequent large floods, Hg T concentrations relative to SSC were approximately twice as high as observed during smaller floods. This difference indicates the transport of more Hg-contaminated particles during high discharge events. Daily Hg T loads in the Sacramento-San Joaquin River at Mallard Island ranged from below the limit of detection to 35 kg. Annual Hg T loads varied from 61 ?? 22 kg (n = 5) in water year (WY) 2002 to 470 ?? 170 kg (n = 25) in WY 2006. The data collected will assist in understanding the long-term recovery of San Francisco Bay from Hg contamination and in implementing the Hg total maximum daily load, the long-term cleanup plan for Hg in the Bay. ?? 2009 SETAC.

Environmental Toxicology and Chemistry↗

The persistence of lead from past gasoline emissions and mining drainage in a large riparian system: Evidence from lead isotopes in the Sacramento River, California

Lead concentrations and isotope ratios measured in river water colloids and streambed sediment samples along 426 km of the Sacramento River, California reveal that the influence of lead from the historical mining of massive sulfide deposits in the West Shasta Cu-mining district (at the headwaters of the Sacramento River) is confined to a 60 km stretch of river immediately downstream of that mining region, whereas inputs from past leaded gasoline emissions and historical hydraulic Au-mining in the Sierra Nevadan foothills are the dominant lead sources in the remaining 370 km of the river. Binary mixing calculations suggest that more than 50% of the lead in the Sacramento River outside of the region of influence of the West Shasta Cu-mining district is derived from past depositions of leaded gasoline emissions. This predominance is the first direct documentation of the geographic extent of gasoline lead persistence throughout a large riparian system (>160,000 km 2 ) and corroborates previous observations based on samples taken at the mouth of the Sacramento River. In addition, new analyses of sediment samples from the hydraulic gold mines of the Sierra Nevada foothills confirm the present-day fluxes into the Sacramento River of contaminant metals derived from historical hydraulic Au-mining that occurred during the latter half of the 19th and early part of the 20th centuries. These fluxes occur predominantly during periods of elevated river discharge associated with heavy winter precipitation in northern California. In the broadest context, the study demonstrates the potential for altered precipitation patterns resulting from climate change to affect the mobility and transport of soil-bound contaminants in the surface environment.

Geochimica et Cosmochimica Acta↗

Spatial and temporal variations in silver contamination and toxicity in San Francisco Bay

Although San Francisco Bay has a "Golden Gate", it may be argued that it is the "Silver Estuary". For at one time the Bay was reported to have the highest levels of silver in its sediments and biota, along with the only accurately measured values of silver in solution, of any estuarine system. Since then others have argued that silver contamination is higher elsewhere (e.g., New York Bight, Florida Bay, Galveston Bay) in a peculiar form of pollution machismo, while silver contamination has measurably declined in sediments, biota, and surface waters of the Bay over the past two to three decades. Documentation of those systemic temporal declines has been possible because of long-term, ongoing monitoring programs, using rigorous trace metal clean sampling and analytical techniques, of the United States Geological Survey and San Francisco Bay Regional Monitoring Program that are summarized in this report. However, recent toxicity studies with macro-invertebrates in the Bay have indicated that silver may still be adversely affecting the health of the estuarine system, and other studies have indicated that silver concentrations in the Bay may be increasing due to new industrial inputs and/or the diagenetic remobilization of silver from historically contaminated sediments being re-exposed to overlying surface waters and benthos. Consequently, the Bay may not be ready to relinquish its title as the "Silver Estuary".

California↗

Diagnostic modeling of trace metal partitioning in south San Francisco Bay

The two-dimensional numerical model ELAmet was used to investigate the effect of adsorption kinetics on the apparent distribution coefficients of Cu, Cd, and Zn in south San Francisco Bay, California. The numerical experiments were designed to determine whether adsorption kinetics can control the basin-scale variability of the observed partitioning and to define the conditions under which adsorption kinetics could account for strong interannual variability in partitioning. The numerical results indicate that aqueous speciation will control basin-scale spatial variations in the apparent distribution coefficient, K d a , if the system is close to equilibrium. However, basin-scale spatial variations in K d a are determined by the location of the sources of metal and the suspended solids concentration of the receiving water if the system is far from equilibrium. The overall spatial variability in K d a also increases as the system moves away from equilibrium.

California↗

Past leaded gasoline emissions as a nonpoint source tracer in riparian systems: A study of river inputs to San Francisco Bay

Variations in the isotopic composition of lead in 1995-1998 river waters flowing into San Francisco Bay trace the washout of lead deposited in the drainage basin from leaded gasoline combustion. At the confluence of the Sacramento and San Joaquin rivers where they enter the Bay, the isotopic compositions of lead in the waters define a linear trend away from the measured historical compositions of leaded gas in California. The river waters are shifted away from leaded gasoline values and toward an isotopic composition similar to Sierra Nevadan inputs which became the predominant source of sedimentation in San Francisco Bay following the onset of hydraulic gold mining in 1853. Using lead isotopic compositions of hydraulic mine sediments and average leaded gasoline as mixing end members, we calculate that more than 50% of the lead in the present river water originated from leaded gasoline combustion. The strong adsorption of lead (log K(d) > 7.4) to particulates appears to limit the flushing of gasoline lead from the drainage basin, and the removal of that lead from the system may have reached an asymptotic limit. Consequently, gasoline lead isotopes should prove to be a useful nonpoint source tracer of the environmental distribution of particle- reactive anthropogenic metals in freshwater systems.

Environmental Science & Technology↗

Stable lead isotopic analyses of historic and contemporary lead contamination of San Francisco Bay estuary

Variations in stable lead isotopic composition (240Pb, 206Pb, 207Pb, 208Pb) in three sediment cores from the San Francisco Bay estuary document temporal changes in sources of lead during the past two centuries. Sediment, with lead from natural geologic sources, and relatively homogeneous lead isotopic compositions are overlain by sediments whose isotopic compositions indicate change in the sources of lead associated with anthropogenic modification of the estuary. The first perturbations of lead isotopic composition in the cores occur in the late 1800s concordant with the beginning of industrialization around the estuary. Large isotopic shifts, toward lower 206Pb/207Pb, occur after the turn of the century in both Richardson and San Pablo Bays. A similar relationship among lead isotopic compositions and lead concentrations in both Bays suggest contamination from the same source (a lead smelter). The uppermost sediments (post 1980) of all cores also have a relatively homogenous lead isotopic composition distinct from pre-anthropogenic and recent aerosol signatures. Lead isotopic compositions of leachates from fourteen surface sediments and five marsh samples from the estuary were also analyzed. These analyses suggest that the lead isotopic signature identified in the upper horizons of the cores is spatially homogeneous among recently deposited sediments throughout the estuary. Current aerosol lead isotopic compositions [Smith, D.R., Niemeyer, S., Flegal, A.R., 1992. Lead sources to California sea otters: industrial inputs circumvent natural lead biodepletion mechanisms. Environmental Research 57, 163-175] are distinct from the isotopic compositions of the surface sediments, suggesting that the major source of lead is cycling of historically contaminated sediments back through the water column. Both the upper core sediments and surface sediments apparently derive their lead predominantly from sources internal to the estuary. These results support the idea that geochemical cycling of lead between sediments and water accounts for persistently elevated lead concentrations in the water column despite 10-fold reduction of external source inputs to San Francisco Bay [Flegal, A.R., Rivera-Duarte, I., Ritson, P.I., Scelfo, G., Smith, G.J., Gordon, M., Sanudo-Wilhelmy, S.A., 1996. Metal contamination in San Francisco Waters: historic perturbations, contemporary concentrations, and future considerations in San Francisco Bay. In: Hollobaugh, J.T. (Ed.), The Ecosystem. AAAS, pp. 173-188].

California↗