Mercury (Hg) is a global pollutant that affects human and ecosystem health. We synthesize understanding of sources, atmosphere-land-ocean Hg dynamics and health effects, and consider the implications ...of Hg-control policies. Primary anthropogenic Hg emissions greatly exceed natural geogenic sources, resulting in increases in Hg reservoirs and subsequent secondary Hg emissions that facilitate its global distribution. The ultimate fate of emitted Hg is primarily recalcitrant soil pools and deep ocean waters and sediments. Transfers of Hg emissions to largely unavailable reservoirs occur over the time scale of centuries, and are primarily mediated through atmospheric exchanges of wet/dry deposition and evasion from vegetation, soil organic matter and ocean surfaces. A key link between inorganic Hg inputs and exposure of humans and wildlife is the net production of methylmercury, which occurs mainly in reducing zones in freshwater, terrestrial, and coastal environments, and the subsurface ocean. Elevated human exposure to methylmercury primarily results from consumption of estuarine and marine fish. Developing fetuses are most at risk from this neurotoxin but health effects of highly exposed populations and wildlife are also a concern. Integration of Hg science with national and international policy efforts is needed to target efforts and evaluate efficacy.
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IJS, KILJ, NUK, PNG, UL, UM
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 (S 290–400) 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.
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IJS, KILJ, NUK, PNG, UL, UM
We examined the response of lake water chemistry in the Adirondack Mountains of New York State, USA to decreases in acid deposition. Striking declines in the concentrations and fluxes of sulfate and ...hydrogen ion in wet deposition have been observed since the late 1970s, while significant decreases in nitrate have been evident since the early 2000s. Decreases in estimated dry sulfur and nitrate deposition have also occurred in the Adirondacks, but with no change in dry to wet deposition ratios. These patterns follow long-term decreases in anthropogenic emissions of sulfur dioxide and nitrogen oxides in the U.S. over the same interval. All of the 48 lakes monitored through the Adirondack Long-Term Monitoring program since 1992 have exhibited significant declines in sulfate concentrations, consistent with reductions in atmospheric deposition of sulfur. Nitrate concentrations have also significantly diminished at variable rates in many (33 of 48) lakes. Decreases in concentrations of sulfate plus nitrate (48 of 48) in lakes have driven widespread increases in acid neutralizing capacity (ANC; 42 of 48) and lab pH (33 of 48), and decreases in the toxic fraction, inorganic monomeric Al (45 of 48). Coincident with decreases in acid deposition, concentrations of dissolved organic carbon (DOC) have also increased in some (29 of 48) lakes. While recovery from elevated acid deposition is evident across Adirondack lakes, highly sensitive and impacted mounded seepages lakes and thin till drainage lakes are recovering most rapidly. Future research might focus on how much additional recovery could be achieved given the current deposition relative to future deposition anticipated under the Clean Power Plan, ecosystem effects of increased mobilization of dissolved organic matter, and the influence of changing climate on recovery from acidification.
•Acid deposition is decreasing in the Adirondack region of New York.•Acid neutralizing capacity in lakes is increasing with decreasing acid deposition.•Lake classes most impacted by acidification show greatest recovery.•Toxic dissolved inorganic aluminum decreases with lake recovery.•Increases in dissolved organic matter or “browning” accompanies lake recovery.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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.
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IJS, KILJ, NUK, PNG, UL, UM
Historical increases in emissions and atmospheric deposition of oxidized and reduced nitrogen (N) provided the impetus for extensive, global-scale research investigating the effects of excess N in ...terrestrial and aquatic ecosystems, with several regions within the Eastern Deciduous Forest of the United States found to be susceptible to negative effects of excess N. The Clean Air Act and associated rules have led to decreases in emissions and deposition of oxidized N, especially in eastern U.S., representing a research challenge and opportunity for ecosystem ecologists and biogeochemists. The purpose of this paper is to predict changes in the structure and function of North American forest ecosystems in a future of decreased N deposition. Hysteresis is a property of a system wherein output is not a strict function of corresponding input, incorporating lag, delay, or history dependence, particularly when the response to decreasing input is different from the response to increasing input. We suggest a conceptual hysteretic model predicting varying lag times in recovery of soil acidification, plant biodiversity, soil microbial communities, forest carbon (C) and N cycling, and surface water chemistry toward pre-N impact conditions. Nearly all of these can potentially respond strongly to reductions in N deposition. Most responses are expected to show some degree of hysteresis, with the greatest delays in response occurring in processes most tightly linked to “slow pools” of N in wood and soil organic matter. Because experimental studies of declines in N loads in forests of North America are lacking and because of the expected hysteresis, it is difficult to generalize from experimental results to patterns expected from declining N deposition. These will likely be long-term phenomena, difficult to distinguish from other, concurrent environmental changes, including elevated atmospheric CO2, climate change, reductions in acidity, invasions of new species, and long-term vegetation responses to past disturbance.
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•Past work on nitrogen (N) effects on ecosystems arose from increased N deposition.•Many forest ecosystems of the eastern U.S. have been sensitive to excess N inputs.•Federal laws have resulted in lower deposition of oxidized N in the eastern U.S.•A hysteretic model is proposed for forest recovery from decreased N deposition.•N-impacted forests should show time lags recovering toward pre-impact conditions.
Nitrogen (N)-impacted forest ecosystems are predicted to exhibit a time lag of varying duration toward recovery initiated by current declines in atmospheric N deposition.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Sustainable strategies such as green roofs have been implemented as stormwater management tools to mitigate disturbance of the hydrologic cycle resulting from urbanization. Green roofs, also referred ...to as vegetated roofs, can improve the urban landscape by reducing heat island effects, providing ecosystem services, and facilitating the retention and treatment of stormwater. Green roofs have received particular attention because they do not require acquisition and development of land and represent an application of biomimicry in design and construction. In this paper, we evaluate the effects of precipitation, evapotranspiration (ET), antecedent dry period (ADP), and seasonal variation on the run‐off quantity and distribution of an extensive, sedum covered, green roof on a commercial building in Syracuse, NY, USA. The green roof greatly facilitated retention of precipitation events without significant changes over the 4‐year study. The green roof retained on average 95.9 ± 3.6% (6.5 ± 5.6 mm) per rainfall event, with a range from 75% to 99.6% (33.2 to 3.3 mm). However, as precipitation quantity increased, the retention of water decreased. This high water retention capacity was the result of the combined effects of ET, stormwater storage (plants, growth media, and stormwater retention layer), and limited surface run‐off from the roof deck due to variation in the sloping of the green roof and the tapered insulation to the deck drains. The water retention capacity of the green roof did not change significantly between growing and nongrowing seasons. Slightly greater precipitation during the growing season coincided with increased ET. Average potential ET during the growing season was approximately 3 times greater than during the nongrowing season. The hydrologic performance of the green roof was not significantly impacted by an ADP greater than 2 days.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
In order to obtain a better perspective of the impacts of brownfields on the land-atmosphere exchange of mercury in urban areas, total gaseous mercury (TGM) was measured at two heights (1.8 m and ...42.7 m) prior to 2011-2012 and after 2015-2016 for the remediation of a brownfield and installation of a parking lot adjacent to the Syracuse Center of Excellence in Syracuse, NY, USA. Prior to brownfield remediation, the annual average TGM concentrations were 1.6 ± 0.6 and 1.4 ± 0.4 ng · m - 3 at the ground and upper heights, respectively. After brownfield remediation, the annual average TGM concentrations decreased by 32% and 22% at the ground and the upper height, respectively. Mercury soil flux measurements during summer after remediation showed net TGM deposition of 1.7 ng · m - 2 · day - 1 suggesting that the site transitioned from a mercury source to a net mercury sink. Measurements from the Atmospheric Mercury Network (AMNet) indicate that there was no regional decrease in TGM concentrations during the study period. This study demonstrates that evasion from mercury-contaminated soil significantly increased local TGM concentrations, which was subsequently mitigated after soil restoration. Considering the large number of brownfields, they may be an important source of mercury emissions source to local urban ecosystems and warrant future study at additional locations.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
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.
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IJS, KILJ, NUK, PNG, UL, UM
abstract
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.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Ongoing salinization and alkalinization in U.S. rivers have been attributed to inputs of road salt and effects of human-accelerated weathering in previous studies. Salinization poses a severe threat ...to human and ecosystem health, while human derived alkalinization implies increasing uncertainty in the dynamics of terrestrial sequestration of atmospheric carbon dioxide. A mechanistic understanding of whether and how human activities accelerate weathering and contribute to the geochemical changes in U.S. rivers is lacking. To address this uncertainty, we compiled dissolved sodium (salinity proxy) and alkalinity values along with 32 watershed properties ranging from hydrology, climate, geomorphology, geology, soil chemistry, land use, and land cover for 226 river monitoring sites across the coterminous U.S. Using these data, we built two machine-learning models to predict monthly-aggregated sodium and alkalinity fluxes at these sites. The sodium-prediction model detected human activities (represented by population density and impervious surface area) as major contributors to the salinity of U.S. rivers. In contrast, the alkalinity-prediction model identified natural processes as predominantly contributing to variation in riverine alkalinity flux, including runoff, carbonate sediment or siliciclastic sediment, soil pH and soil moisture. Unlike prior studies, our analysis suggests that the alkalinization in U.S. rivers is largely governed by local climatic and hydrogeological conditions.
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•Machine learning models detect causes of salinization syndrome in U.S. rivers.•Human activities, e.g., urbanization, are the main source of U.S. river salinity.•Alkalinization in U.S. rivers is governed mainly by natural processes.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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