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1.
Ecotoxicology ; 32(8): 959-976, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37861861

RESUMO

Mercury (Hg) inputs have particularly impacted the northeastern United States due to its proximity to anthropogenic emissions sources and abundant habitats that efficiently convert inorganic Hg into methylmercury. Intensive research and monitoring efforts over the past 50 years in New York State, USA, have informed the assessment of the extent and impacts of Hg exposure on fishes and wildlife. By synthesizing Hg data statewide, this study quantified temporal trends of Hg exposure, spatiotemporal patterns of risk, the role that habitat and Hg deposition play in producing spatial patterns of Hg exposure in fish and other wildlife, and the effectiveness of current monitoring approaches in describing Hg trends. Most temporal trends were stable, but we found significant declines in Hg exposure over time in some long-sampled fish. The Adirondack Mountains and Long Island showed the greatest number of aquatic and terrestrial species with elevated Hg concentrations, reflecting an unequal distribution of exposure risk to fauna across the state. Persistent hotspots were detected for aquatic species in central New York and the Adirondack Mountains. Elevated Hg concentrations were associated with open water, forests, and rural, developed habitats for aquatic species, and open water and forested habitats for terrestrial species. Areas of consistently elevated Hg were found in areas driven by atmospheric and local Hg inputs, and habitat played a significant role in translating those inputs into biotic exposure. Continued long-term monitoring will be important in evaluating how these patterns continue to change in the face of changing land cover, climate, and Hg emissions.


Assuntos
Mercúrio , Compostos de Metilmercúrio , Poluentes Químicos da Água , Animais , Mercúrio/análise , New York , Monitoramento Ambiental , Peixes , Biota , Animais Selvagens , Água
2.
Bioscience ; 72(9): 814-826, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-36034511

RESUMO

In this article marking the 40th anniversary of the US National Science Foundation's Long Term Ecological Research (LTER) Network, we describe how a long-term ecological research perspective facilitates insights into an ecosystem's response to climate change. At all 28 LTER sites, from the Arctic to Antarctica, air temperature and moisture variability have increased since 1930, with increased disturbance frequency and severity and unprecedented disturbance types. LTER research documents the responses to these changes, including altered primary production, enhanced cycling of organic and inorganic matter, and changes in populations and communities. Although some responses are shared among diverse ecosystems, most are unique, involving region-specific drivers of change, interactions among multiple climate change drivers, and interactions with other human activities. Ecosystem responses to climate change are just beginning to emerge, and as climate change accelerates, long-term ecological research is crucial to understand, mitigate, and adapt to ecosystem responses to climate change.

3.
Environ Sci Technol ; 56(3): 1688-1701, 2022 02 01.
Artigo em Inglês | MEDLINE | ID: mdl-35041388

RESUMO

Photochemical and microbial processing are the prevailing mechanisms that shape the composition and reactivity of dissolved organic matter (DOM); however, prior research has not comparatively evaluated the impacts of these processes on the photoproduction of reactive intermediates (RIs) from freshly sourced terrestrial DOM. We performed controlled irradiation and incubation experiments with leaf and soil samples collected from an acid-impacted lake watershed in the Adirondack Mountain region of New York to examine the effects of DOM processing on the apparent quantum yields of RIs (Φapp,RI), including excited triplet states of DOM (3DOM*), singlet oxygen (1O2), and hydroxyl radicals (•OH). Photodegradation led to net reductions in Φapp,1O2, Φapp,3DOM*, and Φapp,•OH, whereas (photo-)biodegradation resulted in increases in Φapp,1O2 and Φapp,3DOM*. Photodegradation and (photo-)biodegradation also shifted the energy distribution of 3DOM* in different directions. Multivariate statistical analyses revealed the potential relevance of photo-biodegradation in driving changes in Φapp,1O2 and Φapp,3DOM* and prioritized five bulk DOM optical and redox properties that best explained the variations in Φapp,1O2 and Φapp,3DOM* along the watershed terrestrial-aquatic continuum. Our findings highlight the contrasting impacts of photochemical and microbial processes on the photoreactivity of freshly sourced terrestrial DOM and invite further studies to develop a more holistic understanding of their implications for aquatic photochemistry.


Assuntos
Matéria Orgânica Dissolvida , Lagos , Radical Hidroxila , Fotólise
4.
Environ Sci Technol ; 55(3): 2132-2142, 2021 02 02.
Artigo em Inglês | MEDLINE | ID: mdl-33434006

RESUMO

Solid-gas-water phase partitioning of mercury (Hg) and the processes governing its diffusivity within soils are poorly studied. In this study, landscape and forest species dependences of gaseous elemental Hg (Hg(0)) in soil profiles (0-50 cm) were investigated over four seasons in eight subtropical (130 days) and temperate (96 days) forest plots. The vertical soil pore Hg(0) concentrations differed between subtropical (Masson pine, broad-leaved forest, and open field) and temperate (Chinese pine, larch, mixed broad-leaf forests, and open field) catchments, with annual averages ranging from 6.73 to 15.8 and 0.95 to 2.08 ng m-3, respectively. The highest Hg(0) concentrations in soil gas consistently occurred in the upper mineral or organic horizons, indicating immobilization of Hg(0) in mineral soils. A strongly positive relationship between pore Hg(0) concentrations and ratios of Hg to organic matter (SOM) in soils suggests that the vertical distribution of Hg(0) is related to soil Hg(0) formation by Hg(II) reduction and sorption to SOM. Temperature was also an important driver of Hg(0) production in soil pores. Based on measurements of soil-air Hg(0) exchange, diffusion coefficients (Ds) of Hg(0) between soil and atmosphere were calculated for field sites, providing a foundation for future development and validation of terrestrial Hg models.


Assuntos
Mercúrio , Poluentes do Solo , Atmosfera , Monitoramento Ambiental , Mercúrio/análise , Solo , Poluentes do Solo/análise
5.
Environ Sci Technol ; 54(17): 10654-10667, 2020 09 01.
Artigo em Inglês | MEDLINE | ID: mdl-32786602

RESUMO

The Adirondack Mountain region of New York, a historical hotspot for atmospheric sulfur and nitrogen deposition, features abundant lakes that are experiencing browning associated with recovery from acidification. Yet, much remains unknown about the photoreactivity of Adirondack lake waters. We quantified the apparent quantum yields (Φapp,RI) of photochemically produced reactive intermediates (RIs), such as excited triplet states of dissolved organic matter (3DOM*), singlet oxygen (1O2), and hydroxyl radicals (•OH), for surface waters collected from 16 representative Adirondack lakes. Φapp,3DOM* and Φapp,1O2 for native Adirondack lake waters fell within ranges reported for whole waters and DOM isolates from various sources, while Φapp,•OH were substantially lower than those measured for other aquatic samples. Orthogonal partial least squares and multiple linear regression analyses identified the spectral slope coefficient from 290 to 400 nm (S290-400) as the most effective predictor of Φapp,RI among measured water chemistry parameters and bulk DOM properties. Φapp,RI also exhibited divergent responses to controlled pH adjustment and aluminum or iron addition simulating hypothetical scenarios relevant to past and future water chemistry conditions of Adirondack lakes. This study highlights the need for continued research on changes in photoreactivity of acid-impacted aquatic ecosystems in response to browning and subsequent impacts on photochemical processes.


Assuntos
Ecossistema , Lagos , Radical Hidroxila , New York , Nitrogênio
6.
Ecotoxicology ; 29(10): 1590-1601, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31586287

RESUMO

Atmospheric deposition is a major input of mercury (Hg) to aquatic and terrestrial ecosystems. To evaluate Hg pollution mitigation strategies for inland lakes, the two Great Lakes (Ontario and Erie) adjacent to New York State (NYS), and rural land areas of Upstate New York, the relative contributions to atmospheric Hg deposition from anthropogenic emission reductions and meteorological variations were investigated using a regional three-dimensional chemical transport model with detailed Hg and bromine chemistry (CMAQ-newHg-Br). Our simulations suggested that NYS in-state emissions and the Northeastern US emission reductions from 2005 to 2011 did not significantly alter Hg wet and dry deposition in all study areas when averaged over time and space. However, such emission changes significantly altered intensive emission sources (>10 lb/year) with subsequent effects on deposition to nearby water bodies. For the Great Lakes, Hg dry deposition was enhanced by a factor of 2-5 in the adjacent model grids (within distances of ~12 km downwind), and the enhancements decreased to negligible values over ~50 km distances. Over land, anthropogenic emissions contributed 30% of the spatial variation in Hg dry deposition and 46% in ambient concentrations of gaseous oxidized Hg (GOM). Spatial and temporal variations in meteorology and foliar characteristics were found to affect both Hg wet and dry deposition. Convective precipitation significantly contributed to spatial and seasonal variations (~65%) in Hg wet deposition over both lake and land surfaces, whereas wind speed and surface heat flux were the main factors contributing to the spatial variation in Hg dry deposition over the lake surfaces through their impacts on dry deposition velocities of GOM and PBM. Leaf area index, which regulates deposition velocity, contributed 14% of the spatial variation in dry deposition flux over land. Variation in solar radiation, which influences photochemical formation of GOM and PBM, explained ~10% of the spatial variation over lake and land surfaces alike. Findings from our highly focused study suggested broad implications. Future climate change will likely serve to enhance Hg concentrations in biota via increases in Hg dry and wet deposition to varying degrees contingent on land surface type. Hence, liminating the health risks of Hg requires mitigation of both anthropogenic Hg emission hotspots and human-induced climate change.


Assuntos
Poluentes Atmosféricos/análise , Monitoramento Ambiental , Mercúrio/análise , Poluição Ambiental , Lagos , Meteorologia , Modelos Químicos , New York , Processos Fotoquímicos
7.
Ecotoxicology ; 29(10): 1614-1626, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31925621

RESUMO

Mercury (Hg) concentrations and speciation were measured in nine tributaries to Lake Ontario as part of two independent field-sampling programs. Among the study tributaries, mean total Hg (THg) concentrations ranged from 0.9 to 2.6 ng/L; mean dissolved Hg (THgD) ranged from 0.5 to 1.5 ng/L; mean particulate Hg (THgP) ranged from 0.3 to 2.0 ng/L; and mean methylmercury (MeHg) ranged from 0.06 to 0.14 ng/L. Watershed land cover, total suspended solids (TSS), and dissolved organic carbon (DOC) were evaluated as potential controls of tributary Hg. Significant relationships between THgD and DOC were limited, whereas significant relationships between THgP and TSS were common across watersheds. Total suspended solids was strongly correlated with the percentage of agricultural land in watersheds. Particle enrichment of Hg (mass Hg/mass TSS) was highly variable, but distinctly higher in US tributaries likely due to higher TSS in Canadian tributaries associated with higher urban and agricultural land cover. MeHg was largely associated with the aqueous phase, and MeHg as a fraction of THg was positively correlated to percent open water coverage in the watershed. Wetland cover was positively correlated to THg and MeHg concentrations, while urban land cover was only related to higher THgP.


Assuntos
Monitoramento Ambiental , Mercúrio/análise , Poluentes Químicos da Água/análise , Agricultura , Lagos/química , Compostos de Metilmercúrio , Ontário , Rios , Estações do Ano , Áreas Alagadas
8.
Ecotoxicology ; 29(10): 1602-1613, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31974921

RESUMO

Nearly half of freshwater wetlands have been lost due to human disturbance. In response, wetlands are being restored to retain their ecosystem services. A potentially adverse consequence of wetland function is the production of methylmercury (MeHg). We measured concentrations of mercury (Hg) species and ancillary parameters in groundwaters and surface waters from four natural and 16 restored wetlands in northern New York State, USA to investigate differences in concentrations of Hg species among wetlands. We found no obvious differences in concentrations of total mercury (THg) and methylmercury in pond waters between natural and restored wetlands. High values of %methylmercury were evident in both ground (38.8 ± 27.6%) and surface waters (43.4 ± 25.6%) suggesting these wetland complexes are highly efficient in converting ionic Hg to methylmercury, regardless if restored or natural. High methylation efficiency may be due to observed drying and rewetting cycles. Hg in pond waters is likely derived from direct atmospheric deposition or by mobilization from near-wetland shallow sediments, in addition to groundwater inflows. Water flow of groundwaters from the associated watershed into pond waters resulted in increases in concentrations of THg and methylmercury. Dissolved organic matter likely plays an important role in the supply of Hg to pond waters. Relationships between methylmercury and %methylmercury with sulfate and nitrate in groundwaters may suggest some chemical limitation on Hg methylation at higher concentrations of these anions. Because of the similarity in Hg dynamics for natural and restored wetlands, the most effective strategy to mitigate methylmercury production would be to decrease atmospheric Hg deposition.


Assuntos
Ecossistema , Monitoramento Ambiental , Compostos de Metilmercúrio/análise , Poluentes Químicos da Água/análise , Áreas Alagadas , Água Doce , Água Subterrânea , New York , Lagoas
9.
Ecotoxicology ; 29(10): 1830-1842, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-32232628

RESUMO

Mercury (Hg) is a potent neurotoxin that biomagnifies within food webs. Adverse effects have been documented for avian species related to exposure of elevated Hg levels. High elevation, boreal forests generally receive higher atmospheric Hg deposition and regional studies have subsequently identified elevated blood Hg concentrations in songbird species inhabiting these montane habitats. The overall goal of this study was to investigate spatial and seasonal Hg exposure patterns in songbird species along an elevational gradient on Whiteface Mountain in the Adirondack Park of New York State. Songbird blood samples were collected from June-July in 2009 and 2010 along an elevational gradient at 13 study plots (450-1400 m) with a focus on Catharus thrushes, including the hermit thrush, Swainson's thrush, and Bicknell's thrush. The main results of this study documented: (1) an overall linear pattern of increasing blood Hg concentrations with increasing elevation, with additional analysis suggesting a nonlinear elevational pattern of increasing blood Hg concentrations to 1075 m, followed by decreasing concentrations thereafter, for all Catharus thrush species across the elevational gradient; and (2) an overall nonlinear seasonal pattern of increasing, followed by decreasing blood Hg concentrations across target species. Avian exposure patterns appear driven by elevated atmospheric Hg deposition and increased methylmercury bioavailability within high elevation habitats as compared with low elevation forests. Seasonal patterns are likely influenced by a combination of complex and dynamic variables related to dietary selection and annual molting cycles. Considering that few high elevation analyses have been conducted within the context of regional songbird research, this project complements the results from similar studies and highlights the need for further monitoring efforts to investigate environmental Hg contamination within avian communities.


Assuntos
Poluentes Ambientais/metabolismo , Mercúrio/metabolismo , Aves Canoras/metabolismo , Animais , Poluentes Ambientais/análise , Cadeia Alimentar , Florestas , Mercúrio/análise , Compostos de Metilmercúrio , New York , Árvores
10.
Ecotoxicology ; 29(10): 1815-1829, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-32037482

RESUMO

Mercury (Hg) is a potent neurotoxin that biomagnifies within both aquatic and terrestrial food webs resulting in adverse physiological and reproductive effects on impacted wildlife populations, including songbird communities. Due to reducing conditions, wetland ecosystems promote the formation of methylmercury. Regional studies have documented elevated blood mercury concentrations in songbird species within these habitat types. The overall goal of this research was to examine spatial and seasonal patterns of Hg exposure for targeted songbird species within Sphagnum bog wetland systems and compare these patterns with adjacent upland forests in the Adirondack Park of New York State. Project sampling was conducted at study plots within four Sphagnum bog and associated upland forest sites from May - August during the 2008, 2009, and 2011 field seasons. The overall results documented: (1) blood Hg concentrations were elevated in songbird species inhabiting Sphagnum bog habitats as compared to nearby upland forest species; (2) target species within each habitat type exhibited consistent species-level patterns in blood Hg concentrations at each study site; and (3) no seasonal change in blood Hg concentrations within Sphagnum bog habitats was documented, but an increasing, followed by a decreasing seasonal pattern in mercury exposure was detected for upland forest species. Habitat type was demonstrated to influence avian Hg exposure levels. Moreover, Sphagnum bog ecosystems may be contributing to elevated Hg concentrations in biota within the surrounding environment. Seasonal patterns for blood Hg concentrations were found to vary between habitat type and are likely related to a combination of variables including habitat-driven Hg concentrations in prey items, seasonal dietary shifts, and annual molting cycles. This project emphasizes the importance of prioritizing future research efforts within identified high Hg habitat types, specifically wetland systems, to better characterize associated avian exposure levels, estimate the spatial extent of wetland systems on the surrounding environment, and identify locations of potential biological hotspots across the Adirondack Park.


Assuntos
Monitoramento Ambiental , Poluentes Ambientais/análise , Mercúrio/análise , Aves Canoras , Sphagnopsida/química , Animais , New York , Áreas Alagadas
11.
Ecotoxicology ; 29(10): 1627-1643, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-32557267

RESUMO

Acid deposition has declined across eastern North America and northern Europe due to reduced emissions of sulfur and nitrogen oxides. Ecosystem recovery has been slow with limited improvement in surface water chemistry. Delayed recovery has encouraged acid-neutralization strategies to accelerate recovery of impaired biological communities. Lime application has been shown to increase pH and dissolved organic carbon (DOC), which could also drive increased mobilization of mercury (Hg) to surface waters. A four-year study was conducted within Honnedaga Lake's watershed in the Adirondack region of New York to compare the effects of watershed and direct channel lime additions on Hg in stream water and macroinvertebrates. All treatments sharply increased stream pH and DOC concentrations, but large differences in the duration of impacts were apparent. The watershed treatment resulted in multi-year increases in concentrations and loads of total Hg (150%; 390%), DOC (190%; 350%) and nutrients, whereas total Hg and DOC increased for short periods (72-96 h) after channel treatments. No response of Hg in macroinvertebrates was evident following the watershed treatment, but a potential short-term and spatially constrained increase occurred after the channel treatment. Our observations indicate that both treatment approaches mobilize Hg, but that direct channel liming mobilizes considerably less than watershed liming over any period longer than a few days. During the final study year, increased methyl Hg concentrations were observed across reference and treated streams, which may reflect an extended dry period, highlighting that climate variation may also affect Hg dynamics.


Assuntos
Monitoramento Ambiental , Invertebrados/fisiologia , Rios/química , Poluentes Químicos da Água/análise , Animais , Biota , Carbono , Ecossistema , Europa (Continente) , Mercúrio/análise , Compostos de Metilmercúrio , New York
12.
Ecotoxicology ; 29(10): 1774-1785, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31691909

RESUMO

Mercury (Hg), a neurotoxic pollutant, can be transported long distances through the atmosphere and deposited in remote areas, threatening aquatic wildlife through methylation and bioaccumulation. Over the last two decades, air quality management has resulted in decreases in Hg emissions from waste incinerators and coal-fired power plants across North America. The common loon (Gavia immer) is an apex predator of the aquatic food web. Long-term monitoring of Hg in loons can help track biological recovery in response to the declines in atmospheric Hg that have been documented in the northeastern USA. To assess spatial patterns and temporal trends in Hg exposure of the common loon in the Adirondack Park of New York State, we analyzed Hg concentrations in loon blood and egg samples from 116 lakes between 1998 and 2016. We found spatially variable Hg concentrations in adult loon blood and feathers across the Park. Loon Hg concentrations (converted to female loon units) increased 5.7% yr-1 from 1998 to 2010 (p = 0.04), and then stabilized at 1.70 mg kg-1 from 2010 to 2016 (p = 0.91), based on 760 observations. Concentrations of Hg in juvenile loons also increased in the early part of the record, stabilizing 2 years before Hg concentrations stabilized in adults. For 52 individual lakes with samples from at least 4 different years, loon Hg increased in 34 lakes and decreased in 18 lakes. Overall, we found a delayed recovery of Hg concentrations in loons, despite recent declines in atmospheric Hg.


Assuntos
Aves/metabolismo , Monitoramento Ambiental , Mercúrio/metabolismo , Poluentes Químicos da Água/metabolismo , Animais , Plumas/química , Feminino , Cadeia Alimentar , Lagos , Compostos de Metilmercúrio , New York
13.
Ecotoxicology ; 29(10): 1762-1773, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31925620

RESUMO

Mercury is a neurotoxic pollutant and contamination in remote ecosystems due to atmospheric mercury deposition coupled with watershed characteristics that influence mercury bioavailability. Biological interactions that affect mercury bioaccumulation are especially relevant as fish assemblages change in response to species introductions and lake management practices. We studied the influence of shifting food web dynamics on mercury in fisheries of Little Moose Lake in the southwestern Adirondack Mountains of New York, USA. Annual removal of non-native Smallmouth Bass (Micropterus dolomieu) has been used as a management strategy since 2000 to restore the native fish assemblage and food web in favor of Lake Trout (Salvelinus namaycush). Changes in total mercury, stable carbon (13C/12C) and nitrogen (15N/14N) isotopes, and growth were evaluated for Lake Trout and Smallmouth Bass. Growth rates increased for both predators and trophic position increased for Lake Trout post-removal. Mercury concentrations in Lake Trout increased over the 16-year study period influenced by a diet shift from invertebrates to higher trophic level prey fish, regardless of increased growth. Smallmouth Bass mercury concentrations decreased with compensatory growth from a reduced population size. These contrasting trends indicate that changes in mercury deposition were not the primary driver for mercury bioaccumulation responses in Little Moose Lake. Stable isotope values changed for both predators and for several lower trophic level organisms, likely reflecting changes in nutrient cycling and/or inputs. Our findings emphasize the potential role of fisheries management on whole-lake and predatory fish responses to mercury contamination in temperate lakes.


Assuntos
Monitoramento Ambiental , Pesqueiros , Peixes/metabolismo , Mercúrio/metabolismo , Poluentes Químicos da Água/metabolismo , Animais , Bass , Cadeia Alimentar , Invertebrados , Lagos , New York , Truta
14.
Environ Sci Technol ; 53(16): 9453-9461, 2019 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-31402663

RESUMO

Dimethyl mercury (CH3HgCH3, DMeHg) has been observed in upwelling marine environments and the deep ocean. However, little is known about the occurrence and mechanisms of DMeHg formation in freshwater environments. In this study, concentrations of dissolved gaseous DMeHg were investigated in floodwaters of rice paddies in China that have been contaminated by mercury from mining. Values of DMeHg in rice paddies were compared with measurements from nearshore surface seawater in the Bohai Gulf. High concentrations of dissolved gaseous DMeHg occurred in rice paddies. Average DMeHg concentration was 12 ± 22 pg L-1 with range of 0.39 to 91 pg L-1 in rice paddies at Shuijing, China, a site impacted by an abandoned mercury mine. These concentrations are comparable to those previously observed in the deep seawater and coastal upwelling environments (2.3-115pg L-1). An alkaline environment was found to be necessary for DMeHg formation in rice paddies. Associated incubation experiments showed that production of DMeHg in paddy soil was limited by Hg availability. Although iron amendments accelerated the production of gaseous methylmercury (MeHg) species to floodwaters, available Hg2+ is crucial for this production in flooded rice paddies. These observations are the first to demonstrate the occurrence of DMeHg and reveal factors affecting DMeHg production in rice paddies. Given the high volatility of DMeHg, these measurements also suggest a source for observations of MeHg in atmospheric deposition and advance understanding of a potentially important aspect of the biogeochemical cycling of Hg.


Assuntos
Mercúrio , Compostos de Metilmercúrio , Oryza , Poluentes do Solo , China , Monitoramento Ambiental , Solo
15.
Proc Natl Acad Sci U S A ; 113(27): 7580-3, 2016 07 05.
Artigo em Inglês | MEDLINE | ID: mdl-27335456

RESUMO

Decades of acid rain have acidified forest soils and freshwaters throughout montane forests of the northeastern United States; the resulting loss of soil base cations is hypothesized to be responsible for limiting rates of forest growth throughout the region. In 1999, an experiment was conducted that reversed the long-term trend of soil base cation depletion and tested the hypothesis that calcium limits forest growth in acidified soils. Researchers added 1,189 kg Ca(2+) ha(-1) as the pelletized mineral wollastonite (CaSiO3) to a 12-ha forested watershed within the Hubbard Brook Experimental Forest in the White Mountains of New Hampshire. Significant increases in the pH and acid-neutralizing capacity of soils and streamwater resulted, and the predicted increase in forest growth occurred. An unanticipated consequence of this acidification mitigation experiment began to emerge a decade later, with marked increases in dissolved inorganic nitrogen (DIN) exports in streamwater from the treated watershed. By 2013, 30-times greater DIN was exported from this base-treated watershed than from adjacent reference watersheds, and DIN exports resulting from this experiment match or exceed earlier reports of inorganic N losses after severe ice-storm damage within the study watershed. The discovery that CaSiO3 enrichment can convert a watershed from a sink to a source of N suggests that numerous potential mechanisms drive watershed N dynamics and provides new insights into the influence of acid deposition mitigation strategies for both carbon cycling and watershed N export.


Assuntos
Chuva Ácida , Compostos de Cálcio , Recuperação e Remediação Ambiental/métodos , Florestas , Ciclo do Nitrogênio , Silicatos , Fertilizantes
16.
Environ Sci Technol ; 52(17): 9749-9757, 2018 09 04.
Artigo em Inglês | MEDLINE | ID: mdl-30129363

RESUMO

Rice consumption is the primary pathway for methylmercury (MeHg) exposure at inland mercury (Hg) mining areas of China. The sources and processes of formation and translocation for MeHg in rice plant are complex and remain largely unknown. In this study, rice ( Oryza sativa L.) was exposed to isotopically labeled dimethylmercury (DMe199Hg) in field experiments using open top chambers to explore the response of MeHg accumulation in rice tissues to different levels of DMe199Hg in air. Rice leaves assimilated DMeHg from air, which was subsequently largely stored in aboveground tissues, including the rice grain, with only a small amount reaching the root. Combining these experimental results with field investigations of DMeHg concentrations in air beneath the rice canopy in a Hg mining area, we estimate that 15.5%, 10.8%, and 8.50% MeHg in the brown rice, the leaf, and the upper stalk, respectively, could be derived from atmospheric sources of DMeHg, while 99.5% of MeHg in rice root originated from the rice soil-water system. These findings help refine the mechanism of MeHg accumulation in rice that, in addition to soil, a fraction of MeHg in rice plants can be derived from DMeHg emissions from flooded rice paddies in Hg mining areas.


Assuntos
Mercúrio , Compostos de Metilmercúrio , Oryza , Poluentes do Solo , China , Monitoramento Ambiental , Mineração
17.
Environ Sci Technol ; 52(22): 13155-13165, 2018 11 20.
Artigo em Inglês | MEDLINE | ID: mdl-30379543

RESUMO

In many temperate forested watersheds, hydrologic nitrogen export has declined substantially in recent decades, and many of these watersheds show enduring effects from historic acid deposition. A watershed acid remediation experiment in New Hampshire reversed many of these legacy effects of acid deposition and also increased watershed nitrogen export, suggesting that these two phenomena may be coupled. Here we examine stream nitrate dynamics in this watershed acid remediation experiment for indicators of nitrogen saturation in the terrestrial and aquatic ecosystems. Post-treatment, the (positive) slope of the relationship between nitrate concentration and discharge increased by a median of 82% ( p = 0.004). This resulted in greater flushing of nitrate during storm events, a key indicator of early stage nitrogen saturation. Hysteretic behavior of the concentration-discharge relationship indicated that the mobilization of soil nitrate pools was responsible for this increased flushing. In contrast to this evidence for nitrogen saturation in the terrestrial ecosystem, we found that nitrogen uptake increased, post-treatment, in the aquatic ecosystem, substantially attenuating growing-season nitrate flux by up to 71.1% ( p = 0.025). These results suggest that, as forests slowly recover from acid precipitation, terrestrial, and aquatic ecosystem nitrogen balance may be substantially altered.


Assuntos
Chuva Ácida , Ecossistema , New Hampshire , Nitratos , Nitrogênio , Rios
18.
Environ Sci Technol ; 52(17): 9556-9561, 2018 09 04.
Artigo em Inglês | MEDLINE | ID: mdl-30067020

RESUMO

Mercury is a global pollutant released into the biosphere by varied human activities including coal combustion, mining, artisanal gold mining, cement production, and chemical production. Once released to air, land and water, the addition of carbon atoms to mercury by bacteria results in the production of methylmercury, the toxic form that bioaccumulates in aquatic and terrestrial food chains resulting in elevated exposure to humans and wildlife. Global recognition of the mercury contamination problem has resulted in the Minamata Convention on Mercury, which came into force in 2017. The treaty aims to protect human health and the environment from human-generated releases of mercury curtailing its movement and transformations in the biosphere. Coincident with the treaty's coming into force, the 13th International Conference of Mercury as a Global Pollutant (ICMGP-13) was held in Providence, Rhode Island USA. At ICMGP-13, cutting edge research was summarized and presented to address questions relating to global and regional sources and cycling of mercury, how that mercury is methylated, the effects of mercury exposure on humans and wildlife, and the science needed for successful implementation of the Minamata Convention. Human activities have the potential to enhance mercury methylation by remobilizing previously released mercury, and increasing methylation efficiency. This synthesis concluded that many of the most important factors influencing the fate and effects of mercury and its more toxic form, methylmercury, stem from environmental changes that are much broader in scope than mercury releases alone. Alterations of mercury cycling, methylmercury bioavailability and trophic transfer due to climate and land use changes remain critical uncertainties in effective implementation of the Minamata Convention. In the face of these uncertainties, important policy and management actions are needed over the short-term to support the control of mercury releases to land, water and air. These include adequate monitoring and communication on risk from exposure to various forms of inorganic mercury as well as methylmercury from fish and rice consumption. Successful management of global and local mercury pollution will require integration of mercury research and policy in a changing world.


Assuntos
Poluentes Ambientais , Mercúrio , Compostos de Metilmercúrio , Animais , Poluição Ambiental , Humanos , Rhode Island
19.
Glob Chang Biol ; 23(6): 2149-2153, 2017 06.
Artigo em Inglês | MEDLINE | ID: mdl-27976837

RESUMO

From the 1970s to 1990s, more stringent air quality regulations were implemented across North America and Europe to reduce chemical emissions that contribute to acid rain. Surface water pH slowly increased during the following decades, but biological recovery lagged behind chemical recovery. Fortunately, this situation is changing. In the past few years, northeastern US fish populations have begun to recover in lakes that were historically incapable of sustaining wild fish due to acidic conditions. As lake ecosystems across the eastern United States recover from acid deposition, the stress to the most susceptible populations of native coldwater fish appears to be shifting from acidification effects to thermal impacts associated with changing climate. Extreme summer temperature events - which are expected to occur with increasing frequency in the coming century - can stress and ultimately kill native coldwater fish in lakes where thermal stratification is absent or highly limited. Based on data from northeastern North America, we argue that recovery from acid deposition has the potential to improve the resilience of coldwater fish populations in some lakes to impacts of climate change. This will occur as the amount of dissolved organic carbon (DOC) in the water increases with increasing lake pH. Increased DOC will reduce water clarity and lead to shallower and more persistent lake thermoclines that can provide larger areas of coldwater thermal refuge habitat. Recovery from acidification will not eliminate the threat of climate change to coldwater fish, but secondary effects of acid recovery may improve the resistance of coldwater fish populations in lakes to the effects of elevated summer temperatures in historically acidified ecosystems. This analysis highlights the importance of considering the legacy of past ecosystem impacts and how recovery or persistence of those effects may interact with climate change impacts on biota in the coming decades.


Assuntos
Chuva Ácida , Mudança Climática , Peixes , Animais , Europa (Continente) , Lagos , América do Norte , Dinâmica Populacional
20.
Glob Chang Biol ; 23(2): 840-856, 2017 02.
Artigo em Inglês | MEDLINE | ID: mdl-27472269

RESUMO

A cross-site analysis was conducted on seven diverse, forested watersheds in the northeastern United States to evaluate hydrological responses (evapotranspiration, soil moisture, seasonal and annual streamflow, and water stress) to projections of future climate. We used output from four atmosphere-ocean general circulation models (AOGCMs; CCSM4, HadGEM2-CC, MIROC5, and MRI-CGCM3) included in Phase 5 of the Coupled Model Intercomparison Project, coupled with two Representative Concentration Pathways (RCP 8.5 and 4.5). The coarse resolution AOGCMs outputs were statistically downscaled using an asynchronous regional regression model to provide finer resolution future climate projections as inputs to the deterministic dynamic ecosystem model PnET-BGC. Simulation results indicated that projected warmer temperatures and longer growing seasons in the northeastern United States are anticipated to increase evapotranspiration across all sites, although invoking CO2 effects on vegetation (growth enhancement and increases in water use efficiency (WUE)) diminish this response. The model showed enhanced evapotranspiration resulted in drier growing season conditions across all sites and all scenarios in the future. Spruce-fir conifer forests have a lower optimum temperature for photosynthesis, making them more susceptible to temperature stress than more tolerant hardwood species, potentially giving hardwoods a competitive advantage in the future. However, some hardwood forests are projected to experience seasonal water stress, despite anticipated increases in precipitation, due to the higher temperatures, earlier loss of snow packs, longer growing seasons, and associated water deficits. Considering future CO2 effects on WUE in the model alleviated water stress across all sites. Modeled streamflow responses were highly variable, with some sites showing significant increases in annual water yield, while others showed decreases. This variability in streamflow responses poses a challenge to water resource management in the northeastern United States. Our analyses suggest that dominant vegetation type and soil type are important attributes in determining future hydrological responses to climate change.


Assuntos
Mudança Climática , Rios , Solo , Clima , Ecossistema , Florestas , New England , Plantas
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