Local to regional emission sources affecting mercury fluxes to New York lakes

Lake-sediment records across the Northern Hemisphere show increases in atmospheric deposition of anthropogenic mercury (Hg) over the last 150 years. Most of the previous studies have examined remote lakes affected by the global atmospheric Hg reservoir. In this study, we present Hg flux records from lakes in an urban/suburban setting of central New York affected also by local and regional emissions. Sediment cores were collected from the Otisco and Skaneateles lakes from the Finger Lakes region, Cross Lake, a hypereutrophic lake on the Seneca River, and Glacial Lake, a small seepage lake with a watershed that corresponds with the lake area. Sediment accumulation rates and dates were established by ²¹⁰Pb. The pre-anthropogenic regional atmospheric Hg flux was estimated to be 3.0 μg m⁻² yr⁻¹ from Glacial Lake, which receives exclusively direct atmospheric deposition. Mercury fluxes peaked during 1971–2001, and were 3 to more than 30 times greater than pre-industrial deposition. Land use change and urbanization in the Otisco and Cross watersheds during the last century likely enhanced sediment loads and Hg fluxes to the lakes. Skaneateles and Glacial lakes have low sediment accumulation rates, and thus are excellent indicators for atmospheric Hg deposition. In these lakes, we found strong correlations with emission records for the Great Lakes region that markedly increased in the early 1900s, and peaked during WWII and in the early 1970s. Declines in modern Hg fluxes are generally evident in the core records. However, the decrease in sediment Hg flux at Glacial Lake was interrupted and has increased since the early 1990s probably due to the operation of new local emission sources. Assuming the global Hg reservoir tripled since the pre-industrial period, the contribution of local and regional emission sources to central New York lakes was estimated to about 80% of the total atmospheric Hg deposition.     

Pre-industrial atmospheric pollution: was it important for the pH of acid-sensitive Swedish lakes?

Acid rain has caused extensive surface water acidification in Sweden since the mid-20th century. Sulfur emissions from fossil-fuel burning and metal production were the main sources of acid deposition. In the public consciousness, acid deposition is strongly associated with the industrial period, in particular the last 50 years. However, studies of lake-water pH development and atmospheric pollution, based on analyses of lake sediment deposits, have shown the importance of a long-term perspective. Here, we present a conceptual argument, using the sediment record, that large-scale atmospheric acid deposition has impacted the environment since at least Medieval times. Sulfur sources were the pre-industrial mining and metal industries that produced silver, lead and other metals from sulfide ores. This early excess sulfur deposition in southern Sweden did not cause surface water acidification; on the contrary, it contributed to alkalization, i.e. increased pH and productivity of the lakes. Suggested mechanisms are that the excess sulfur caused enhanced cation exchange in catchment soils, and that it altered iron-phosphorus cycling in the lakes, which released phosphorus and increased lake productivity.     

Reconciling models and measurements to assess trends in atmospheric mercury deposition

Changes in atmospheric mercury deposition are used to evaluate the effectiveness of regulations controlling emissions. This analysis can be complicated by seemingly incongruent data from different model runs, model types, and field measurements. Here we present a case study example that describes how to identify trends in regional scale mercury deposition using best-available information from multiple data sources. To do this, we use data from three atmospheric chemistry models (CMAQ, GEOS-Chem, HYSPLIT) and multiple sediment archives (ombrotrophic bog, headwater lake, coastal salt marsh) from the Bay of Fundy region in Canada. Combined sediment and modeling data indicate that deposition attributable to US and Canadian emissions has declined in recent years, thereby increasing the relative significance of global sources. We estimate that anthropogenic emissions in the US and Canada account for 28-33% of contemporary atmospheric deposition in this region, with the rest from natural (14-32%) and global sources (41-53%).     

Studies of mercury pollution in a lake due to a thermometer factory situated in a tourist resort: Kodaikkanal, India

Kodaikkanal, India, suffered mercury contamination due to emissions and waste from a thermometer factory. Kodai Lake is situated to the north of the factory. The present study determined mercury in waters, sediment and fish samples and compared the values with those from two other lakes, Berijam and Kukkal. Total mercury (Hg(T)) of 356-465 ng l(-1), and 50 ng l(-1) of mercury in methyl mercury form were seen in Kodai waters while Berijam and Kukkal waters showed significantly lower values. Kodai sediment showed 276-350 mg/kg Hg(T) with about 6% methyl mercury. Berijam and Kukkal sediments showed Hg(T) of 189-226 mg/kg and 85-91 mg/kg and lower methylation at 3-4% and 2%, respectively. Hg(T) in fish from Kodai lake ranged from 120 to 290 mg/kg. The results show that pollution of the lake has taken place due to mercury emissions by the factory.     

Large-scale spatial variation in mercury concentrations in cattle in NW Spain

Mercury (Hg) is a highly toxic environmental contaminant and man-made emissions account for between a quarter and a third of total atmospheric levels. Point discharges, particularly coal-burning power stations, are major sources of atmospheric Hg and can result in marked spatial variation in mercury deposition and subsequent uptake by biota. The aims of this study were to quantify the extent to which major point and diffuse sources of atmospheric Hg emissions affected accumulation of Hg by biota throughout Galicia and Asturias, two of the major regions in northwest Spain. We did this by relating renal Hg concentrations in locally reared cattle (n=284) to the proximity of animals to point and diffuse sources of Hg emissions. Mercury residues in calf kidneys ranged between non-detected and 89.4 g/kg wet weight. Point discharges from coal-fired power plants in Galicia had the most dominant impact on Hg accumulation by calves in Galicia, affecting animals throughout the region and explaining some two-thirds of the variation in renal residues between animals located directly downwind from the plants. The effects of more diffuse emission sources on Hg accumulation in calves were not distinguishable in Galicia but were detected in cattle from neighbouring Asturias. The impact of both point and diffuse sources in elevating environmental levels of bioavailable Hg and subsequent accumulation by cattle extended to approximately 140-200 km downwind from source.     

Mercury accumulation in surface sediments of salt marshes of the Bay of Fundy

Mercury contamination in Canada's Bay of Fundy is a priority concern because of elevated levels observed in fish, birds and wildlife. Salt marshes constitute an important part of the Bay's coastline and are potential stores of mercury for the region. We measured the amount of mercury accumulated over a 5-yr period from 1997 to 2002 in surface sediments of seven salt marshes along the New Brunswick coast of the Bay. The seven study sites extended from outer to inner Bay, spanning a gradient in tidal range (6-12 m) and sediment characteristics such as %LOI (4-29%) and sediment deposition rate (0.27-1.76 cm yr(-1)). In each study site, mercury was measured in low and high marsh areas. Sediment mercury concentrations ranged from 7 to 79 ng g(-1) and loading rates ranged from 0.1 to 1.1 mg m(-2). Total estimated 5-yr storage of mercury in salt marsh sediments of the Bay is 854+/-465 kg. We also compared sediment mercury loading to atmospheric inputs measured at a deposition monitoring station operating in New Brunswick from 1997 to 2002 and found that direct atmospheric deposition appears to be a minor input of mercury to these sediments. We are unaware of documentation of mercury loading in salt marshes on a bay-wide scale and over a constrained (5-yr) time period elsewhere.     

Food chain enrichment of organochlorine compounds and mercury in clean and polluted lakes of Finland

Lakes polluted by pulp mill and urban wastes including chlorobleaching of pulp, semipolluted lakes and reference lakes in nearly natural condition in Central Finland were studied for contents of mercury, methyl mercury and organochlorine compounds in sediment, plankton, roach and pike. Chlorobleaching had caused a 30-fold concentration of Hg in bottom sediment related to that of the purest reference lake. This was not reflected to the mercury levels in fish which were highest at one natural condition (humic) lake and rather high also at semipolluted lake Päijänne. Mercury in fish was shown to be mostly methylated but not completely and its time trends could be estimated. Chloroform showed no but carbon tetrachloride, tetrachloroethylene and chlorinated cymenes significant bioaccumulation in fish. Levels of chlorophenols from bleaching had strongly decreased but pentachlorophenol and 2,3,4,6-tetrachlorphenol levels remained related to earlier results. Using fat basis attenuated the power of estimation of food chain enrichment by a three throphic level model for lipohilic biocides and a strong proof was obtained of the enrichment of hexachlorobenzene. The time trends at Päijänne were decreasing for mercury and DDE but increasing for PCB.     

Mercury in sediment and fish communities of Lake Vänern, Sweden: recovery from contamination

The past effluents of mercury (Hg) into Lake V?nern were considerable. The consequences of, and recovery from these have been monitored through continuous measurements of mercury in sediment and fish. Mercury levels in lake sediments in the vicinity of the main source of mercury, a chloralkali plant on the northern shore, have only decreased by slightly more than a half since the mid-1970s, despite a radical decrease in effluents from the source, already during the 1960s. The mercury levels in pike (Esox lucius) have decreased to a similar extent during this time period. They are now about 30% higher in the worst affected parts of the lake compared to the least affected parts. Lower levels have been measured in perch (Perca fluviatilis) and salmonoid fish in the lake. Despite the increased presence of mercury in the sediment of Lake V?nern, the mercury levels in the fish of the lake are relatively low compared to fish in lakes situated in the same region, but not affected by any local mercury effluents. As calculated, the total fish biomass of L. V?nern holds less than 1000th of the amount of mercury contained in the upper, biologically active layers of the bottom sediment of the lake. This demonstrates the potential influence of various environmental factors and motivates continued monitoring of mercury levels in the lake in the future.     

A diagnostic evaluation of modeled mercury wet depositions in Europe using atmospheric speciated high-resolution observations

This study is part of the Global Mercury Observation System (GMOS), a European FP7 project dedicated to the improvement and validation of mercury models to assist in establishing a global monitoring network and to support political decisions. One key question about the global mercury cycle is the efficiency of its removal out of the atmosphere into other environmental compartments. So far, the evaluation of modeled wet deposition of mercury was difficult because of a lack of long-term measurements of oxidized and elemental mercury. The oxidized mercury species gaseous oxidized mercury (GOM) and particle-bound mercury (PBM) which are found in the atmosphere in typical concentrations of a few to a few tens pg/m³ are the relevant components for the wet deposition of mercury. In this study, the first European long-term dataset of speciated mercury taken at Waldhof/Germany was used to evaluate deposition fields modeled with the chemistry transport model (CTM) Community Multiscale Air Quality (CMAQ) and to analyze the influence of the governing parameters. The influence of the parameters precipitation and atmospheric concentration was evaluated using different input datasets for a variety of CMAQ simulations for the year 2009. It was found that on the basis of daily and weekly measurement data, the bias of modeled depositions could be explained by the bias of precipitation fields and atmospheric concentrations of GOM and PBM. A correction of the modeled wet deposition using observed daily precipitation increased the correlation, on average, from 0.17 to 0.78. An additional correction based on the daily average GOM and PBM concentration lead to a 50 % decrease of the model error for all CMAQ scenarios. Monthly deposition measurements were found to have a too low temporal resolution to adequately analyze model deficiencies in wet deposition processes due to the nonlinear nature of the scavenging process. Moreover, the general overestimation of atmospheric GOM by the CTM in combination with an underestimation of low precipitation events in the meteorological models lead to a good agreement of total annual wet deposition besides the large error in weekly deposition estimates. Moreover, it was found that the current speciation profiles for GOM emissions are the main factor for the overestimation of atmospheric GOM concentrations and might need to be revised in the future. The assumption of zero emissions of GOM lead to an improvement of the mean normalized bias for three-hourly observations of atmospheric GOM from 9.7 to 0.5, Furthermore, the diurnal correlation between model and observation increased from 0.01 to 0.64. This is a strong indicator that GOM is not directly emitted from primary sources but is mainly created by oxidation of GEM.     

Is PCBs concentration variability between and within freshwater fish species explained by their contamination pathways?

Many chemical, physiological, and trophic factors are known to affect bioaccumulation of polychlorinated biphenyls (PCBs) in biota. Understanding the primary factors affecting fish contamination is critical for predicting and assessing risks to upper-trophic level consumers, including humans. Here we identify PCB contamination pathways that could explain within- and between-species variability in fish concentration levels. Three freshwater river fish species (barbel, chub and bream) were sampled at three sites along the Rhone River (France) where fish consumption is partially prohibited because of PCB levels exceeding the European health-based benchmark. The trophic position was assessed using an innovative approach based on stable isotope analyses and Bayesian inference, which takes into account both isotope data variability and parameter uncertainty. The effect of foraging habitat on fish contamination was addressed using stable isotope mixing models. The fish trophic position and PCB concentrations were found to be unrelated while the exploitation of sediment detrital carbon as a food source appeared to be a critical factor affecting fish contamination. Fish length, PCB concentration of the sediment, and individual fish foraging habitat (exploitation of detrital versus planktonic carbon sources) explained 80% of within- and between-species variability observed in PCB concentrations. These results, obtained for species that have overlapping TPs and exploit different carbon sources, reveal that the important factor in fish PCB contamination is not only what fish consume, but also and essentially the feeding location.     

Effects of acidic deposition on forest and aquatic ecosystems in New York State

Acidic deposition is comprised of sulfuric and nitric acids and ammonium derived from atmospheric emissions of sulfur dioxide, nitrogen oxides, and ammonia, respectively. Acidic deposition has altered soil through depletion of labile pools of nutrient cations (i.e. calcium, magnesium), accumulation of sulfur and nitrogen, and the mobilization of elevated concentrations of inorganic monomeric aluminum to soil solutions in acid-sensitive areas. Acidic deposition leaches essential calcium from needles of red spruce, making this species more susceptible to freezing injury. Mortality among sugar maples appears to result from deficiencies of nutrient cations, coupled with other stresses such as insect defoliation or drought. Acidic deposition has impaired surface water quality in the Adirondack and Catskill regions of New York by lowering pH levels, decreasing acid-neutralizing capacity, and increasing aluminum concentrations. Acidification has reduced the diversity and abundance of aquatic species in lakes and streams. There are also linkages between acidic deposition and fish mercury contamination and eutrophication of estuaries.     

Partition and tempospatial variation of gaseous and particulate mercury at a unique mercury-contaminated remediation site

This study investigated the seasonal variation and spatial distribution of gaseous and particulate mercury at a unique mercury-contaminated remediation site located at the near-coastal region of Tainan City, Taiwan. Gaseous elemental mercury (GEM), particulate mercury (PTM), and dustfall mercury (DFM) were measured at six nearby sites from November 2009 to September 2010. A newly issued Method for Sampling and Analyzing Mercury in Air (National Institute of Environmental Analysis [NIEA] Method A304.10C) translated from U.S. Environmental Protection Agency (EPA) Method 10-5, was applied for the measurement of atmospheric mercury in this particular study. One-year field measurements showed that the seasonal averaged concentrations of GEM and PTM were in the range of 5.56-12.60 and 0.06-0.22 ng/m3, respectively, whereas the seasonal averaged deposition fluxes of DFM were in the range of 27.0-56.8 g/km2-month. The maximum concentrations of GEM and PTM were 38.95 and 0.58 ng/m3, respectively. The atmospheric mercury apportioned as 97.42-99.87% GEM and 0.13-2.58% PTM. As a whole, the concentrations of mercury species were higher in the springtime and summertime than those in the wintertime and fall. The southern winds generally brought higher mercury concentrations, whereas the northern winds brought relatively lower mercury concentrations, to the nearby fishing villages. This study revealed that the mercury-contaminated remediation site, an abandoned chlor-alkali manufacturing plant, was the major mercury emission source that caused severe atmospheric mercury contamination over the investigation region. The hot spot of mercury emissions was allocated at the southern tip of the abandoned chlor-alkali manufacturing plant. On-site continuous monitoring of GEM at the mercury-contaminated remediation site observed that GEM concentrations during the open excavation period were 2-3 times higher than those during the nonexcavation period.     

Nationwide monitoring of mercury in wild and farmed fish from fresh and coastal waters of Korea

Mercury (Hg) concentrations were monitored in wild and cultured fish collected from fresh and coastal waters in the Korean peninsula from April 2006 to August 2008 nationwide. Total Hg concentrations were reported for 5043 fish samples, including 78 species from 133 locations. Significant interspecies variation was noted in the Hg levels. The average Hg concentration in each fish species ranged from 6.31 μg kg⁻¹ for mullet (Mugil cephalus) to 200 μg kg⁻¹ for mandarin fish (Siniperca scherzeri). Among the species collected, the maximum concentration of Hg, 1720 μg kg⁻¹, was measured in an Amur catfish (Silurus asotus). Only wild freshwater fish exceeded the WHO ingestion standard. Wild freshwater piscivorous fish samples from a large artificial upstream lake contained the highest Hg levels. Hg concentrations were compared between fish groups categorized as wild and farmed fish from freshwater and coastal waters. Although the wild freshwater fish had similar size ranges, their Hg concentrations were higher than those of the other groups. Compared to the feed of farmed marine and freshwater fishes, the prey of wild freshwater fish had a higher Hg concentration, and the total Hg concentrations in freshwater and associated sediment samples were higher than those in coastal water and associated sediment samples. In the freshwater environment, piscivorous fish bioaccumulated two times more Hg than carnivorous and omnivorous fish and four times more than planktivorous fish. The difference in Hg concentrations among trophic groups might have been due to differences in the size of fish, in addition to the variations among different trophic groups. These data will be useful for developing the fish consumption advisory as a management measure to reduce Hg exposure.     

Levels and possible sources of PCDD/PCDF in sediment and pike samples from Swedish lakes and rivers. (Part one)

One goal of the Swedish survey project is to discover possible sources of PCDD/F. Bottom sediment and pike were sampled at various sites near different types of industries along the coast line of two lakes and one river. The results show background levels of PCDD/F in some lakes which can only be explained by atmospheric input. In some lakes paper mill emissions of chlorinated PCDD/F give high levels of local contamination (≈1 ng/g IG) within short distances (<1 km) from the source. PCDD/F from paper mill effluents are transported long distances and traces can be detected over the entire lake area. The PCDD/F levels in pike are correlated with levels in the underlying sediment.     

Mercury Levels in Pristine and Gold Mining Impacted Aquatic Ecosystems of Suriname, South America

Mercury levels in sediment and predatory fish were measured for 53 localities in Suriname. The average mercury level in bottom sediment surpassed the Canadian standard for sediment in most localities, except the coastal plains. Of the predatory fish, 41 % had a mercury level above the European Union standard for human consumption of 0.5 μg g⁻¹. Highest mercury levels were found in fish from the Brokopondo Reservoir and from the Upper Coppename River. High levels of mercury in fish in pristine areas are explained by atmospheric transportation of mercury with the northeastern trade winds followed by wet deposition. Contrary to gold mining areas, where mercury is bound to drifting sediments, in “pristine” areas the mercury is freely available for bio-accumulation and uptake. Impacts on piscivorous reptiles, birds, and mammals are unknown, but likely to be negative.     

Mercury methylation in aquatic systems affected by acid deposition

Recently, it has been noted that fish in acidified lakes may contain elevated levels of mercury. While there is correlation among lakes between depressed pH and high mercury concentrations in fish, the cause of this problem is unknown. A number of hypotheses have been advanced in explanation, including increased mercury deposition, changes in mercury mobility due to acidification, pH dependent changes in mercury uptake by biota, and alterations in population size and/or structure which result in increased bioaccumulation in fish. Because fish accumulate mercury mainly in an organic form, methylmercury, changes in the biogeochemical cycling of this compound might account for elevated bioaccumulation. Mercury methylation is predominantly a microbial process which occurs in situ in lakes. This review focuses on microbiological and biogeochemical changes that may lead to increased levels of methylmercury in fresh waters impacted by acid-deposition. In particular, we focus on the hypothesis that sulfate-reducing bacteria are important mediators of metal methylation in aquatic systems and, moreover, that sulfate-deposition may stimulate methylmercury production by enhancing the activity of sulfate-reducing bacteria in sediments.     

Wet deposition mercury fluxes in the Canadian sub-Arctic and southern Alberta,measured using an automated precipitation collector adapted to cold regions

This paper reports mercury (Hg) concentrations and fluxes in precipitation that was collected from 2006 to 2008 at three sites in Canada: sub-Arctic boreal forest, sub-Arctic coast, and southern Alberta, using cold-adapted precipitation collectors which operated reliably at temperatures below ?30 °C during the study. The southern Alberta site (Crossfield) may be influenced by Calgary urban air, whereas the sub-Arctic coastal (Churchill, Manitoba) and boreal forest (Fort Vermilion, Alberta) sites are in more remote northern areas. Annual mean Hg concentrations in precipitation (5.0–9.2 ng L^?1) at the study sites were in the lower half of the range reported for southern Canada and the USA by the Mercury Deposition Network (MDN). But owing to typically low precipitation rates, gross wet Hg fluxes (0.54–2.0 μg m^?2 yr^?1) were among the lowest reported by MDN, with Crossfield having about twice the flux in 2007 of the other two sites. Flux was significantly correlated with precipitation, and thus was highest in summer (June–August) and lowest during winter, a pattern typical of other temperate continental locations. There was no evidence of higher wet Hg fluxes or concentrations in springtime at Churchill where atmospheric mercury depletion events (AMDEs) occur. Measured gross deposition fluxes at the study locations were ～2–8 times lower than estimated by GEOS-Chem and GRAHM atmospheric models. The largest discrepancy occurred for Churchill, which raises the question of how well Hg deposition from AMDEs is described by current models. Better agreement between measurements and models was obtained from MDN stations in Alberta and Alaska, where wet Hg fluxes were 2–10 times higher than the study sites either because of power plant emissions (Alberta), or because of high precipitation rates (Alaska).     

Mercury in fish in Swedish lakes

The aim of this work has been to try to obtain a picture of the past, present and future mercury situation in fish in Swedish lakes, to make an estimate of the number of lakes threatened by 'blacklisting', and to see if the data can be used to reveal anything about the impact of liming on the Hg content in pike. The register contains a broad set of data from 1456 lakes. The main results are as follows. Trend analyses indicate that the Hg content in 1-kg pike seems to increase with time. This is interesting since there has been a significant decrease in mercury emissions from Swedish industries during the last two decades. High Hg contents in 1-kg pike appear in a very characteristic pattern, linked to specific sources of Hg emission. The data indicate that old Swedish 'sins' are still causing a lot of problems. The factors governing the leakage of Hg from soils to water ought to be a very important topic for further studies. The Hg content in pike shows the highest correlation with the following parameters: Hg in surficial sediments, pH, distance from point source and water hardness, lake water alkalinity and conductivity, water retention time, size of drainage area and lake surface. A formula which provides the best possible degree of explanation (r2 = 0.78) has been derived. At present there are about 250 lakes 'blacklisted' in Sweden due to high Hg content in fish. Our data show that there are at least 9400 lakes that ought to be 'blacklisted' today. A successful liming operation will alter the chemical conditions in lakes and also decrease the Hg content in fish.     

Mercury contamination in human hair and fish from Cambodia: levels, specific accumulation and risk assessment

Mercury (Hg) concentrations in human hair and fish samples from Phnom Penh, Kien Svay, Tomnup Rolork and Batrong, Cambodia, collected in November 1999 and December 2000 were determined to understand the status of contamination, and age- and sex-dependent accumulation in humans and to assess the intake of mercury via fish consumption. Mercury concentrations in human hair ranged from 0.54 to 190mug/g dry wt. About 3% of the samples contained Hg levels exceeding the no observed adverse effects level (NOAEL) of WHO (50mug/g) and the levels in some hair samples of women also exceeded the NOAEL (10mug/g) associated with fetus neurotoxicity. A weak but significant positive correlation was observed between age and Hg levels in hair of residents. Mercury concentrations in muscle of marine and freshwater fish from Cambodia ranged from <0.01 to 0.96mug/g wet wt. Mercury intake rates were estimated on the basis of the Hg content in fish and daily fish consumption. Three samples of marine fish including sharp-tooth snapper and obtuse barracuda, and one sample of sharp-tooth snapper exceeded the guidelines by US EPA and by Joint FAO/WHO Expert Committee on Food Additives (JECFA), respectively, which indicates that some fish specimens examined (9% and 3% for US EPA and JECFA guidelines, respectively) were hazardous for consumption at the ingestion rate of Cambodian people (32.6g/day). It is suggested that fish is probably the main source of Hg for Cambodian people. However, extremely high Hg concentrations were observed in some individuals and could not be explained by Hg intake from fish consumption, indicating some other contamination sources of Hg in Cambodia.     

Optimizing best management practices to control anthropogenic sources of atmospheric phosphorus deposition to inland lakes

Excessive phosphorus loading to inland freshwater lakes around the globe has resulted in nuisance plant growth along the waterfronts, degraded habitat for cold-water fisheries, and impaired beaches, marinas, and waterfront property. The direct atmospheric deposition of phosphorus can be a significant contributing source to inland lakes. The atmospheric deposition monitoring program for Lake Simcoe, Ontario, indicates roughly 20% of the annual total phosphorus load (2010–2014 period) is due to direct atmospheric deposition (both wet and dry deposition) on the lake. This novel study presents a first-time application of the genetic algorithm (GA) methodology to optimize the application of best management practices (BMPs) related to agriculture and mobile sources to achieve atmospheric phosphorus reduction targets and restore the ecological health of the lake. The novel methodology takes into account the spatial distribution of the emission sources in the airshed, the complex atmospheric long-range transport and deposition processes, cost and efficiency of the popular management practices, and social constraints related to the adoption of BMPs. The optimization scenarios suggest that the optimal overall capital investment of approximately $2M, $4M, and $10M annually can achieve roughly 3, 4, and 5 tonnes reduction in atmospheric P load to the lake, respectively. The exponential trend indicates diminishing returns for the investment beyond roughly $3M per year and that focusing much of this investment in the upwind, nearshore area will significantly impact deposition to the lake. The optimization is based on a combination of the lowest cost, most beneficial and socially acceptable management practices that develops a science-informed promotion of implementation/BMP adoption strategy. The geospatial aspect to the optimization (i.e., proximity and location with respect to the lake) will help land managers to encourage the use of these targeted best practices in areas that will most benefit from the phosphorus reduction approach.

Implications: Excessive phosphorus loading to inland freshwater lakes around the globe has resulted in nuisance plant growth along the waterfronts, degraded habitat for cold water fisheries, and impaired beaches, marinas and waterfront property. This novel study presents a first-time application of the Genetic Algorithm methodology to optimize the application of best management practices related to agriculture and mobile sources to achieve atmospheric phosphorus reduction targets and restore the ecological health of the lake. The novel methodology takes into account the spatial distribution of the emission sources in the airshed, the complex atmospheric long-range transport and deposition processes, cost and efficiency of the popular management practices and social constraints related to the adoption of BMPs.