Mountaintop Removal Coal Mining Contaminates Snowpack across a Broad Region.

Mountaintop removal coal mining is a source of downstream pollution. Here, we show that mountaintop removal coal mining also pollutes ecosystems downwind. We sampled regional snowpack near the end of winter along a transect of sites located 3-60 km downwind of coal mining in the Elk River valley of British Columbia, Canada. Vast quantities of polycyclic aromatic compounds (PACs), a toxic class of organic contaminants, are emitted and transported atmospherically far from emission sources. Summed PAC (ΣPAC) snowpack concentrations ranged from 29-94,866 ng/L. Snowpack ΣPAC loads, which account for variable snowpack depth, ranged from <10 µg/m2 at sites >50 km southeast of the mines to >1000 µg/m2 at sites in the Elk River valley near mining operations, with one site >15,000 µg/m2. Outside of the Elk River valley, snowpack ΣPAC loads exhibited a clear spatial pattern decreasing away from the mines. The compositional fingerprint of this PAC pollution matches closely with Elk River valley coal. Beyond our study region, modeling results suggest a depositional footprint extending across western Canada and the northwestern United States. These findings carry important implications for receiving ecosystems and for communities located close to mountaintop removal coal mines exposed to air pollution elevated in PACs.

Legacy coal mining impacts downstream ecosystems for decades in the Canadian Rockies.

Mountaintop removal coal mining leaves a legacy of disturbed landscapes and abandoned infrastructure with clear impacts on water resources; however, the intensity and persistence of this water pollution remains poorly characterized. Here we examined the downstream impacts of over a century of coal mining in the Crowsnest Pass (Alberta, Canada). Water samples were collected downstream of two historical coal mines: Tent Mountain and Grassy Mountain. Tent Mountain hosts a partially reclaimed surface mine that closed in 1983. Selenium concentrations downstream of Tent Mountain reached 185 µg/L in a lake below the mine spoil pile, and up to 23 µg/L in Crowsnest Creek, which drains the lake and the mine property. Further downstream, a well-dated sediment core from Crowsnest Lake records increases in sediment, selenium, lead, carbon, nitrogen, and polycyclic aromatic compounds that closely tracked the history of mining at Tent Mountain. In contrast, episodic discharge of mine water from abandoned underground adits at Grassy Mountain drive periodic (but short-term) increases in iron, various metals, and suspended sediment. These results underscore the lasting downstream impacts of abandoned and even reclaimed coal mines.

Glacial Erosion Drives High Summer Mercury Exports from the Yukon River, Canada.

Mercury concentrations and yields in the Yukon River are the highest of the world's six largest panarctic drainages. Permafrost thaw has been implicated as the main driver of these high values. Alternative sources include mercury released from glacial melt and erosion, atmospheric mercury pollution, or surface mining. To determine the summer source and speciation of mercury across the Yukon River basin within Canada, we sampled water from 12 tributaries and the mainstem during July 2021. The total (unfiltered) mercury concentration in the glacier-fed White River was 57 ng/L, >10 times higher than all other sampled tributaries. The White River's high total mercury concentrations were driven by suspended sediment and persisted ∼300 km downstream of glacierized headwaters. Total mercury concentrations were lowest (typically <2 ng/L) in tributaries downstream of still-water landscape features (e.g., lakes and settling ponds), suggesting these features are effective sinks for sediment-bound mercury. Low total mercury concentrations (∼2 ng/L) were also observed in five tributaries across diverse thawing permafrost landscapes. These results suggest that glacial erosion and meltwater transport, not permafrost, drive enhanced exports of mercury with suspended sediment. Mercury exports may decline as glacial watersheds pass peak water. Other factors, including mercury released from permafrost thaw, are minor components at present.

Dissolved polycyclic aromatic compounds in Canada's Athabasca River in relation to Oil Sands from 2013 through 2019.

The Canada-Alberta Oil Sands Monitoring (OSM) Program began long-term surface water quality monitoring on the lower Athabasca River in 2012. Sampling of low level, bio-accumulative polycyclic aromatic compounds (PACs) targeted a suite of parent and alkylated compounds in the Athabasca River (AR) mainstem using semi-permeable membrane devices (SPMDs). Samples were collected along a gradient from upstream reference near Athabasca, Alberta, through exposure to the Athabasca oil sands deposit (AOSD), various tributary inflows, and mining activities within the OSMA, to downstream recovery near Wood Buffalo National Park (WBNP) and reference on the Slave River. The program adapted over the years, shifting in response to program review and environmental events. The AOSD chemical fingerprint was present in samples collected within the AOSD, through the oil sands mineable area (OSMA), downstream to recovery from 2013 to 2019. PACs were dominated by alkylated phenanthrenes/anthracenes (PAs) and dibenzothiophenes (Ds), with elevated levels of alkylated fluorenes (Fs), naphthalenes (Ns), fluoranthenes/pyrenes (FlPys) and benzo[a]anthracenes/chrysenes (BaACs), increasing in concentration from C1 < C2 < C3 < C4. Concentrations of these petrogenic PACs were at their highest within the OSMA and downstream of tributaries. The AOSD fingerprint was absent from sites located outside of the influence of the AOSD and downstream of the Peace-Athabasca Delta on the Slave River. PAC concentrations in the AR increased with mainstem discharge and loadings from tributaries, were moderated by the PAD, and diluted by the Peace River. This work bolsters the baseline PAC information previously reported for the Athabasca River and waters downstream, reporting 7 years of data, from all sites within the mainstem monitoring program, and exploring potential regional and hydrological drivers of these between sites and over time.

Paleolimnological evaluation of metal(loid) enrichment from oil sands and gold mining operations in northwestern Canada.

Abundant reserves of metals and oil have spurred large-scale mining developments across northwestern Canada during the past 80 years. Historically, the associated emissions footprint of hazardous metal(loid)s has been difficult to identify, in part, because monitoring records are too short and sparse to have characterized their natural concentrations before mining began. Stratigraphic analysis of lake sediment cores has been employed where concerns of pollution exist to determine pre-disturbance metal(loid) concentrations and quantify the degree of enrichment since mining began. Here, we synthesize the current state of knowledge via systematic re-analysis of temporal variation in sediment metal(loid) concentrations from 51 lakes across four key regions spanning 670 km from bitumen mining in the Alberta Oil Sands Region (AOSR) to gold mining (Giant and Con mines) at Yellowknife in central Northwest Territories. Our compilation includes upland and floodplain lakes at varying distances from the mines to evaluate dispersal of pollution-indicator metal(loid)s from bitumen (vanadium and nickel) and gold mining (arsenic and antimony) via atmospheric and fluvial pathways. Results demonstrate 'severe' enrichment of vanadium and nickel at near-field sites (≤20 km) within the AOSR and 'severe' (near-field; ≤ 40 km) to 'considerable' (far-field; 40-80 km) enrichment of arsenic and antimony due to gold mining at Yellowknife via atmospheric pathways, but no evidence of enrichment of vanadium or nickel via atmospheric or fluvial pathways at the Peace-Athabasca Delta and Slave River Delta. Findings can be used by decision makers to evaluate risks associated with contaminant dispersal by the large-scale mining activities. In addition, we reflect upon methodological approaches to be considered when evaluating paleolimnological data for evidence of anthropogenic contributions to metal(loid) deposition and advocate for proactive inclusion of paleolimnology in the early design stage of environmental contaminant monitoring programs.

Polycyclic Aromatic Compounds in Rivers Dominated by Petrogenic Sources after a Boreal Megafire.

Polycyclic aromatic compounds (PACs) threaten the health of aquatic ecosystems. In northeastern Alberta, Canada, decades of oil sands mining and upgrading activities have increased PAC delivery into freshwaters. This PAC pollution adds to natural inputs from river erosion of bitumen-bearing McMurray Formation outcrops and wildfire inputs. Quantifying these petrogenic and pyrogenic PAC inputs, which is key for understanding industrial impacts, remains a challenge. To distinguish petrogenic from pyrogenic inputs, we characterized river water PACs before and after the 2016 Fort McMurray wildfire, one of the largest natural disasters in Canadian history. Samples of wildfire ash and outcropping bitumen allow us to distinguish between these important PAC sources. River PAC concentrations ranged over multiple orders of magnitude (10s-10 000s ng/L). Petrogenic PACs dominated most of the postfire period with only short-term episodes of pyrogenic signatures in burned watersheds due to the wash-in of ash from the watershed. Wildfire PAC inputs during these events resulted in exceptional increases in concentrations that met or exceeded high (petrogenic) background concentrations, driven by the natural erosion of outcropping bitumen. Our dataset offers the first quantification of these two important PAC sources in this industrialized region and provides new insight into the impacts of increasing wildfire frequency and severity across the Boreal Forest.

Interhemispheric antiphasing of neotropical precipitation during the past millennium.

Uncertainty about the influence of anthropogenic radiative forcing on the position and strength of convective rainfall in the Intertropical Convergence Zone (ITCZ) inhibits our ability to project future tropical hydroclimate change in a warmer world. Paleoclimatic and modeling data inform on the timescales and mechanisms of ITCZ variability; yet a comprehensive, long-term perspective remains elusive. Here, we quantify the evolution of neotropical hydroclimate over the preindustrial past millennium (850 to 1850 CE) using a synthesis of 48 paleo-records, accounting for uncertainties in paleo-archive age models. We show that an interhemispheric pattern of precipitation antiphasing occurred on multicentury timescales in response to changes in natural radiative forcing. The conventionally defined "Little Ice Age" (1450 to 1850 CE) was marked by a clear shift toward wetter conditions in the southern neotropics and a less distinct and spatiotemporally complex transition toward drier conditions in the northern neotropics. This pattern of hydroclimatic change is consistent with results from climate model simulations indicating that a relative cooling of the Northern Hemisphere caused a southward shift in the thermal equator across the Atlantic basin and a southerly displacement of the ITCZ in the tropical Americas, with volcanic forcing as the principal driver. These findings are at odds with proxy-based reconstructions of ITCZ behavior in the western Pacific basin, where changes in ITCZ width and intensity, rather than mean position, appear to have driven hydroclimate transitions over the last millennium. This reinforces the idea that ITCZ responses to external forcing are region specific, complicating projections of the tropical precipitation response to global warming.

Caribbean Lead and Mercury Pollution Archived in a Crater Lake.

Lead and mercury have long histories of anthropogenic use and release to the environment extending into preindustrial times. Yet, the timing, magnitude, and persistence of preindustrial emissions remain enigmatic, especially for mercury. Here, we quantify tropical lead and mercury deposition over the past ∼3000 years using a well-dated sediment core from a small crater lake (Lake Antoine, Grenada). Preindustrial increases in lead and mercury concentrations can be explained by varying inputs of watershed mineral and organic matter, which in turn reflect climate-driven changes in the lake level. We find no evidence that preindustrial lead and mercury use raised deposition rates in this remote ecosystem, and our results underscore the need to carefully evaluate common normalization approaches for changing lithogenic inputs and sedimentation rates. Industrial-era lead and mercury accumulation rates in Lake Antoine have been accelerated by land use and land cover change within the crater rim, yet global industrial pollution remains evident. After correcting for watershed inputs, we find that recent atmospheric lead and mercury deposition rates averaged 2925 and 24 µg/m2/y, respectively, which are in close agreement with monitoring data. Our results challenge recent assessments suggesting preindustrial mercury use raised atmospheric deposition rates globally, highlighting the unique nature of 20th Century industrial pollution.

Tracking historical sources of polycyclic aromatic compounds (PACs) in dated lake sediment cores near in-situ bitumen operations of Cold Lake, Alberta.

Most bitumen in the Alberta oil sands (Canada) is extracted by thermal in-situ recovery. Despite the widespread use of in-situ bitumen extraction, little information is available on the release of petroleum hydrocarbons by this method to adjacent land and water. Here we analyzed the composition and abundance of parent and alkylated polycyclic aromatic compounds (PACs) in 11 radiometrically-dated lake sediment cores collected near in-situ operations at Cold Lake Alberta to assess potential petroleum contamination sources to surrounding lakes over the past century. Like open-pit mining areas, alkylated PACs in Cold Lake sediments were elevated compared to unsubstituted parent PACs and increased coeval with the onset of bitumen extraction in the area. Diagnostic ratios and pyrogenic indices showed that PAC sources to these lake sediments were dominantly pyrogenic, likely from historic forest fires, however they shifted to more petrogenic sources coeval with expanding oil sands extraction at Cold Lake. PACs in sediment from regional lakes are weakly correlated to their proximity to in-situ oil wells, once corrected for lake area. These results suggest that in-situ operations, via diesel-fueled vehicular emissions and the combustion of natural gas for steam generation, are a source of PACs to nearby lakes, but PACs did not exceed Canadian sediment quality guidelines for the protection of aquatic life.

Quantification of Spatial and Temporal Trends in Atmospheric Mercury Deposition across Canada over the Past 30 Years.

Mercury (Hg) is a pollutant of concern across Canada and transboundary anthropogenic Hg sources presently account for over 95% of national anthropogenic Hg deposition. This study applies novel statistical analyses of 82 high-resolution dated lake sediment cores collected from 19 regions across Canada, including nearby point sources and in remote regions and spanning a full west-east geographical range of ∼4900 km (south of 60°N and between 132 and 64°W) to quantify the recent (1990-2018) spatial and temporal trends in anthropogenic atmospheric Hg deposition. Temporal trend analysis shows significant synchronous decreasing trends in post-1990 anthropogenic Hg fluxes in western Canada in contrast to increasing trends in the east, with spatial patterns largely driven by longitude and proximity to known point source(s). Recent sediment-derived Hg fluxes agreed well with the available wet deposition monitoring. Sediment-derived atmospheric Hg deposition rates also compared well to the modeled values derived from the Hg model, when lake sites located nearby (<100 km) point sources were omitted due to difficulties in comparison between the sediment-derived and modeled values at deposition "hot spots". This highlights the applicability of multi-core approaches to quantify spatio-temporal changes in Hg deposition over broad geographic ranges and assess the effectiveness of regional and global Hg emission reductions to address global Hg pollution concerns.

Isotopic Analyses Fingerprint Sources of Polycyclic Aromatic Compound-Bearing Dust in Athabasca Oil Sands Region Snowpack.

Fugitive dust associated with surface mining activities is one of the principal vectors for transport of airborne contaminants in Canada's Athabasca oil sands region (AOSR). Effective environmental management requires quantitative identification of the sources of this dust. Using natural abundance radiocarbon (Δ14C) and dual (δ13C, δ2H) compound-specific isotope analysis (CSIA), this study investigated the sources of dust and particulate-bound polycyclic aromatic compounds (PACs) deposited in AOSR lake snowpack. Lower Δ14C values, higher particulate and PAC loadings, and lower δ13C values for phenanthrene and C1-alkylated phenanthrenes/anthracenes (C1-Phen) at sites closer to the mining operations indicated unprocessed oil sand and/or petroleum coke (petcoke-a byproduct of bitumen upgrading) as major sources of anthropogenic fugitive dust. However, a Bayesian isotopic mixing model that incorporated both δ13C and δ2H could discriminate petcoke from oil sand, and determined that petcoke comprised between 44 and 95% (95% credibility intervals) of a C1-Phen isomer at lakes <25 km from the heart of the mining operations, making it by far the most abundant source. This study is the first to demonstrate the potential of CSIA to provide accurate PAC source apportionment in snowpack and reveals that petcoke rather than oil sand is the main source of mining-related particulate PACs deposited directly to AOSR lakes.

Structural equation modeling of long-term controls on mercury and bromine accumulation in Pinheiro mire (Minas Gerais, Brazil).

The application of statistical modeling is still infrequent in mercury research in peat, despite the ongoing debate on the weight of the diverse factors (climate, peat decomposition, vegetation changes, etc.) that may affect mercury accumulation. One of the few exceptions is the Hg record of Pinheiro mire (souheast Brazil). Previous studies on this mire modeled mercury using principal components regression and partial least squares. These methods assume independence between factors, which is seldom the case in natural systems, thus hampering the identification of mediating effects and interactions. To overcome these limitations, in this reserach we use structural equation modeling (PLS-SEM) to model mercury and bromine peat records - bromine has been used in some investigations to normalize mercury accumuation. The mercury model explained 83% of the variance and suggested a complex control: increased peat decomposition, dust deposition and humid climates enhanced mercury accumulation, while increased mineral fluxes resulted in a decrease in mercury accumulation. The bromine model explained 90% of the variation in concentrations: increased dust deposition and peat decomposition promoted bromine accumulation, while time (i.e. peat age) promoted bromine depletion. Thus, although mercury and bromine are both organically bound elements with relevant atmospheric cycles the weights of the factors involved in their accumulation differed significantly. Our results suggest caution when using bromine to normalize mercury accumulation. PLS-SEM results indicate a large time dependence of peat decomposition, catchment mineral fluxes, long-term climate change, and atmospheric deposition; while atmospheric dust, mineral fluxes and peat decomposition showed high to moderate climate dependency. In particular, they also point to a relevant role of autogenic processes (i.e. the build up and expansion of the mire within the catchment), which controlled local mineral fluxes; an aspect that has seldom been considered.

Biological Factors Moderate Trace Element Accumulation in Fish along an Environmental Concentration Gradient.

Trace elements can accumulate in aquatic food webs, becoming potentially hazardous to wildlife and human health. Whereas many studies have examined mercury dynamics in freshwater environments, evidence for the bioaccumulative potential of other trace elements (e.g., arsenic) is conflicting. Trace element concentrations found in surface water of the Red Deer River, Alberta, Canada, have raised concern for potential accumulation in aquatic biota. We investigated fish from this river to better understand the influence of biological and environmental factors in trace element bioaccumulation. We analyzed 20 trace elements, and stable nitrogen (δ15 N) and carbon (δ13 C) isotopes, in the muscle tissue of 8 species. Zinc, selenium, arsenic, chromium, and nickel were detected in the majority of fish at low concentrations. However, mercury was detected in all fish and often exceeded criteria for the protection of consumers. Body size was often positively correlated with trace element concentrations. In addition, δ15 N and δ13 C were correlated to mercury and arsenic concentrations, indicating that mercury biomagnifies whereas arsenic biodiminishes. Spatial patterns of fish trace element concentrations did not reflect differences in surface water concentrations. These findings indicate that fish trace element concentrations are primarily moderated by biological factors, such as trophic position and body size, and are not locally restricted to areas of relatively high environmental concentrations in the Red Deer River. Environ Toxicol Chem 2021;40:422-434. © 2020 SETAC.

Mercury bioaccumulation in stream fish from an agriculturally-dominated watershed.

Bioaccumulation of mercury in freshwater fish is a complex process driven by environmental and biological factors. In this study, we assessed mercury in fish from four tributaries to the Red Deer River, Alberta, Canada, which are characterized by high surface water mercury concentrations. We used carbon (δ13C) and nitrogen (δ15N) stable isotopes to examine relationships between fish total mercury (THg) concentrations, food web dynamics and patterns in unfiltered THg and methylmercury (MeHg) concentrations. We found that THg concentrations exceeded the tissue residue quality guideline for the protection of wildlife consumers in 99.7% of fish sampled. However, while the surface water THg concentration was highest in Michichi Creek and the MeHg concentration was consistent across streams, patterns of fish THg concentrations varied depending on species. Furthermore, body size and trophic level were only correlated with THg concentrations in white sucker (Catostomus commersoni) and Prussian carp (Carrasius gibelio). The results of this study suggest that mercury poses a risk to the health of piscivorous wildlife in the Red Deer River watershed. Despite high THg concentrations in these streams, mercury bioaccumulation is not driven by environmental inorganic mercury concentrations. Additionally, commonly cited factors associated with mercury concentrations in fish, such as body size and trophic level, may not strongly influence bioaccumulation in these stream ecosystems.

Severe western Canadian wildfire affects water quality even at large basin scales.

Wildfires can have severe and lasting impacts on the water quality of aquatic ecosystems. However, our understanding of these impacts is founded primarily from studies of small watersheds with well-connected runoff regimes. Despite the predominance of large, low-relief rivers across the fire-prone Boreal forest, it is unclear to what extent and duration wildfire-related material (e.g., ash) can be observed within these systems that typically buffer upstream disturbance signals. Following the devastating 2016 Fort McMurray wildfire in western Canada, we initiated a multi-faceted water quality monitoring program that suggested brief (hours to days) wildfire signatures could be detected in several large river systems, particularly following rainfall events greater than 10 mm. Continuous monitoring of flow and water quality showed distinct, precipitation-associated signatures of ash transport in rivers draining expansive (800-100,000 km2) and partially-burned (<1-22 percent burned) watersheds, which were not evident in nearby unburned regions. Yields of suspended sediment, nutrients (nitrogen, phosphorus) and metals (lead, others) from impacted rivers were 1.2-10 times greater than from those draining unburned regions. Post-fire suspended sediment concentrations in impacted rivers were often larger than pre-fire 95% prediction intervals based on several years of water sampling. These multiple lines of evidence indicate that low-relief landscapes can mobilize wildfire-related material to rivers similarly, though less-intensively and over shorter durations, than headwater regions. We propose that uneven mixing of heavily-impacted tributaries with high-order rivers may partially explain detection of wildfire signals in these large systems that may impact downstream water users.

Environmental archives of atmospheric Hg deposition - A review.

Environmental archives offer an opportunity to reconstruct temporal trends in atmospheric Hg deposition at various timescales. Lake sediment and peat have been the most widely used archives; however, new records from ice, tree rings, and the measurement of Hg stable isotopes, are offering new insights into past Hg cycling. Preindustrial Hg deposition has been studied over decadal to millennial timescales extending as far back as the late Pleistocene. Exploitation of mercury deposits (mainly cinnabar) first began during the mid to late Holocene in South America, Europe, and Asia, but increased dramatically during the Colonial era (1532-1900) for silver production. However, evidence for preindustrial Hg pollution is restricted to regions directly downwind or downstream of cinnabar or precious metal mining centers. Excluding these areas, there has been an approximately four-fold increase in atmospheric deposition globally over the industrial era (i.e., since 1800-1850), though regional differences exist, especially during the early 20th Century. Lake sediments, peat, ice, and tree rings are all influenced by (and integrate) a range of processes. For example, lake sediments are influenced by atmospheric deposition, sediment focusing, and the input of allochthonous material from the watershed, peat records reflect atmospheric deposition and biotic uptake, ice cores are a record of Hg scrubbed during precipitation, and tree rings record atmospheric concentrations. No archive represents an absolute record of past Hg deposition or concentrations, and post-depositional transformation of Hg profiles remains an important topic of research. However, natural archives continue to provide important insight into atmospheric Hg cycling over various timescales.

Accumulating Mercury and Methylmercury Burdens in Watersheds Impacted by Oil Sands Pollution.

Bitumen mining and upgrading in northeastern Alberta, Canada, releases toxic pollutants into the atmosphere, including mercury (Hg) and methylmercury (MeHg). This Hg and MeHg is then deposited to the surrounding landscape; however, the fate of these contaminants remains unknown. Here, we compare snowpack chemistry to high-frequency measurements of river water quality across six watersheds (five impacted by oil sands development and one unimpacted). Catchment scale snowpack Hg and MeHg loads normalized to watershed area were highest near oil sands operations. River water Hg concentrations and loads tracked discharge and tended to be higher downstream of mining operations, while MeHg concentrations and loads increased through the summer, reflecting peak summer MeHg production rates. Except in the reference watershed, snowpack Hg and MeHg loads equaled or exceeded the amount of Hg and MeHg exported during freshet and, in some cases, the entire hydrologic year. This suggests landscapes across the oil sands region, which are dominated by low-relief wetlands and other shallow-water systems, are accumulating Hg and MeHg. Importantly, during years of high discharge, these low-relief systems appear to become better connected and flush MeHg (and Hg) from the watershed. Thus, these watersheds may act as temporary, rather than as permanent, natural repositories of oil sands contaminants.

Total Mercury and Methylmercury in Lake Water of Canada's Oil Sands Region.

Increased delivery of mercury to ecosystems is a common consequence of industrialization, including in the Athabasca Oil Sands Region (AOSR) of Canada. Atmospheric mercury deposition has been studied previously in the AOSR; however, less is known about the impact of regional industry on toxic methylmercury (MeHg) concentrations in lake ecosystems. We measured total mercury (THg) and MeHg concentrations for five years from 50 lakes throughout the AOSR. Mean lake water concentrations of THg (0.4-5.3 ng L-1) and MeHg (0.01-0.34 ng L-1) were similar to those of other boreal lakes and <5% of all samples exceeded Provincial water quality guidelines. Lakes with the highest THg concentrations were found >100 km northwest of oil sands mines and received runoff from geological formations high in metals concentrations. MeHg concentrations were highest in those lakes, and in smaller productive lakes closer to oil sands mines. Simulated annual average direct deposition of THg to sampled lakes using an atmospheric chemical transport model showed <2% of all mercury deposited to sampled lakes was emitted from oil sands activities. Consequently, spatial patterns of mercury in AOSR lakes were likely most influenced by watershed and lake conditions, though mercury concentrations in these lakes may be perturbed with future development and climatic change.

Climate, Fire, and Vegetation Mediate Mercury Delivery to Midlatitude Lakes over the Holocene.

The rise in mercury concentrations in lake sediment deposited over the last ∼150 years is widely recognized to have resulted from human activity. However, few studies in the Great Lakes region have used lake sediment to reconstruct atmospheric mercury deposition on millennial time scales. Here we present a 9000-year mercury record from sediment in Copper Falls; a small closed-basin lake on the Keweenaw Peninsula. Prior to abrupt increases in the 19th and 20th centuries, mercury remains at relatively low concentrations for the last 9000 years. Higher mercury fluxes in the early Holocene (3.4 ± 1.1 µg m-2 yr-1) are attributed to drier conditions and greater forest fire occurrence. The gradual decline in mercury flux over the middle to late Holocene (1.9 ± 0.2 µg m-2 yr-1) is interpreted to reflect a transition to wetter conditions, which reduced forest fires, and promoted the development of soil organic matter and deciduous forests that sequestered natural sources of mercury. The Copper Falls Lake record highlights the sensitivity of watersheds to changes in mercury inputs from both human and natural forcings, and provides millennial-scale context for recent mercury contamination that will aid in establishing baseline values for restoration efforts.