The legacy of mercury cycling from mining sources in an aquatic ecosystem: from ore to organism.

Clear Lake is the site of an abandoned mercury (Hg) mine (active intermittently from 1873 to 1957), now a U.S. Environmental Protection Agency Superfund Site. Mining activities, including bulldozing waste rock and tailings into the lake, resulted in approximately 100 Mg of Hg entering the lake's ecosystem. This series of papers represents the culmination of approximately 15 years of Hg-related studies on this ecosystem, following Hg from the ore body to the highest trophic levels. A series of physical, chemical, biological, and limnological studies elucidate how ongoing Hg loading to the lake is influenced by acid mine drainage and how wind-driven currents and baroclinic circulation patterns redistribute Hg throughout the lake. Methylmercury (MeHg) production in this system is controlled by both sulfate-reducing bacteria as well as newly identified iron-reducing bacteria. Sediment cores (dated with dichlorodiphenyldichlorethane [DDD], 210pb, and 14C) to approximately 250 cm depth (representing up to approximately 3000 years before present) elucidate a record of total Hg (TotHg) loading to the lake from natural sources and mining and demonstrate how MeHg remains stable at depth within the sediment column for decades to millenia. Core data also identify other stresses that have influenced the Clear Lake Basin especially over the past 150 years. Although Clear Lake is one of the most Hg-contaminated lakes in the world, biota do not exhibit MeHg concentrations as high as would be predicted based on the gross level of Hg loading. We compare Clear Lake's TotHg and MeHg concentrations with other sites worldwide and suggest several hypotheses to explain why this discrepancy exists. Based on our data, together with state and federal water and sediment quality criteria, we predict potential resulting environmental and human health effects and provide data that can assist remediation efforts.

Clear Lake sediments: anthropogenic changes in physical sedimentology and magnetic response.

We analyzed the sedimentological characteristics and magnetic properties of cores from the three basins of Clear Lake, California, USA, to assess the depositional response to a series of land use changes that occurred in the watershed over the 20th century. Results indicate that distinct and abrupt shifts in particle size, magnetic concentration/mineralogy, and redox conditions occur concurrently with a variety of ecological and chemical changes in lake bed sediments. This coincidence of events occurred around 1927, a datum determined by an abrupt increase in total mercury (Hg) in Clear Lake cores and the known initiation of open-pit Hg mining at the Sulphur Bank Mercury Mine, confirmed by 210Pb dating. Ages below the 1927 horizon were determined by accelerator mass spectrometry on 14C of coarse organic debris. Calculated sedimentation rates below the 1927 datum are approximately 1 mm/yr, whereas rates from 1927 to 2000 are up to an order of magnitude higher, with averages of approximately 3.5-19 mm/yr. In both the Oaks and Upper Arms, the post-1927 co-occurrence of abrupt shifts in magnetic signatures with color differences indicative of changing redox conditions is interpreted to reflect a more oxygenated diagenetic regime and rapid burial of sediment below the depth of sulfate diffusion. Post-1927 in the Oaks Arm, grain size exhibits a gradual coarsening-upward pattern that we attribute to the input of mechanically deposited waste rock related to open-pit mining activities at the mine. In contrast, grain size in the Upper Arm exhibits a gradational fining-upward after 1927 that we interpret as human-induced erosion of fine-grained soils and chemically weathered rocks of the Franciscan Assemblage by heavy earthmoving equipment associated with a road- and home-building boom, exacerbated by stream channel mining and wetlands destruction. The flux of fine-grained sediment into the Upper Arm increased the nutrient load to the lake, and that in turn catalyzed profuse cyanobacterial blooms through the 20th century. The resulting organic biomass, in combination with the increased inorganic sediment supply, contributed to the abrupt increase in sedimentation rate after 1927.

Anthropogenic stressors and changes in the Clear Lake ecosystem as recorded in sediment cores.

Sediment cores were collected to investigate multiple stresses on Clear Lake, California, USA, through the period of European occupation to the present day. Earlier workers suggested the hypothesis that the use of mechanized earthmoving equipment, starting in the 1920s and 1930s, was responsible for erosion, mercury (Hg) contamination, and habitat loss stresses. Cores (approximately 2.5 m in depth) were collected in 1996 and 2000 from each of the three arms of the lake. Carbon-14 dating suggests that these cores represent as much as 3000 years of the lake's history, beginning long before European settlement. Total mercury (TotHg) and methylmercury (MeHg), dry matter, water, carbon, nitrogen, phosphorus, sulfur, and the stable isotopes 13C and 15N were measured at 5-cm intervals. Nearly all parameters show major changes at depths of 58-135 cm, beginning at ca. 1927 (dated with 210Pb). Accepting this date for concomitant major changes in seven cores yields an estimated 8.6 mm/yr average sedimentation rate after 1927. Pre-1927 sedimentation rates were approximately 1 mm/yr. Total mercury and MeHg, dry matter, phosphorus, and 15N increase significantly, whereas nitrogen, sulfur, carbon, and water content decrease significantly above the 1927 horizon. Both TotHg and MeHg show extremely large increases (roughly 10-fold) above the 1927 horizon. A peak in inorganic deposition rate and minimum values for percentage of water is present at depths corresponding to ca. 1970. Interestingly, the first 75 years of European settlement in the Clear Lake basin (including the most productive years of the Sulphur Bank Mercury Mine) appeared to have had undetectable effects on lake cores. Changes since 1927 were dramatic. The large increase in Hg beginning about 1927 corresponds to the use of heavy equipment to exploit the ore deposit at the mine using open-pit methods. Increases in sediment deposition from increased earthmoving in the basin and sulfate loading from the mine are the most likely explanations for the dramatic changes seen in the post-1927 sections of the cores.