Salt marsh estuaries serve as sources and sinks for nutrients and elements to and from estuarine water, which enhances and alleviates watershed fluxes to the coastal ocean. We assessed sources and sinks of mercury in the intertidal Plum Island Sound estuary in Massachusetts, the largest salt marsh estuary of New England, using 25-km spatial water sampling transects. Across all seasons, dissolved (FHg) and total (THg) mercury concentrations in estuarine water were highest and strongly enhanced in upper marshes (1.31 ± 0.20 ng L⁻¹ and 6.56 ± 3.70 ng L⁻¹, respectively), compared to riverine Hg concentrations (0.86 ± 0.17 ng L⁻¹ and 0.88 ± 0.34 ng L⁻¹, respectively). Mercury concentrations declined from upper to lower marshes and were lowest in ocean water (0.38 ± 0.10 ng L⁻¹ and 0.56 ± 0.25 ng L⁻¹, respectively). Conservative mixing models using river and ocean water as endmembers indicated that internal estuarine Hg sources strongly enhanced estuarine water Hg concentrations. For FHg, internal estuarine Hg contributions were estimated at 26 g yr⁻¹ which enhanced Hg loads from riverine sources to the ocean by 44%. For THg, internal sources amounted to 251 g yr⁻¹ and exceeded riverine sources six-fold. Proposed sources for internal estuarine mercury contributions include atmospheric deposition to the large estuarine surface area and sediment re-mobilization, although sediment Hg concentrations were low (average 23 ± 2 μg kg⁻¹) typical of uncontaminated sediments. Soil mercury concentrations under vegetation, however, were ten times higher (average 200 ± 225 μg kg⁻¹) than in intertidal sediments suggesting that high soil Hg accumulation might drive lateral export of Hg to the ocean. Spatial transects of methylated Hg (MeHg) showed no concentration enhancements in estuarine water and no indication of internal MeHg sources or formation. Initial mass balance considerations suggest that atmospheric deposition may either be in similar magnitude, or possibly exceed lateral tidal export which would be consistent with strong Hg accumulation observed in salt marsh soils sequestering Hg from current and past atmospheric deposition.

The use of mercury in small-scale gold mining is globally the largest anthropogenic source of mercury in the environment. In countries like Ghana, where small-scale gold mining is a highly important economic sector, the activity is also expected to cause local pollution. This study is based on a hypothesis that the mining activity in Ghana is causing more widespread soil pollution also outside active mining sites, and that the main part of regional differences in soil concentrations of mercury might come from pollution. Little systematic and dependable data has been collected to assess the extent of mercury contamination of soils in areas outside active mining areas. The regional aspect of mercury pollution from mining has not been studied in Ghana or other countries with a large small-scale gold mining sector. Systematic collection of soil samples on a 25 × 25 km² net covering the entire country was carried out to ensure the representativeness of data and to allow calculation of spatial trends. The soil concentrations found in one-third of the country, where most intensive mining takes place, are three times higher than concentrations in the rest of the country. This difference cannot be explained by sources of natural variation in mercury concentrations but can be explained by decades of atmospheric deposition. It is therefore likely that the mining activity has caused a more widespread increase in soil concentrations, also outside active mining sites. The mercury concentrations found are on average 0.024 mg kg⁻¹, which is low compared to published studies from other countries and regions and estimated world averages. All measured concentrations are well below soil quality criteria for human health. The build-up of soil concentrations in the mining area is still problematic because mercury is a hazardous substance in the environment.

Antarctic trace element records could provide important insights into the impact of human activities on the environment over the past few centuries. In this study, we investigated the atmospheric concentrations of 14 representative heavy metals (Al, As, Cd, Co, Cu, Fe, K, Mg, Mn, Pb, Sb, Sr, Tl and V) from 174 samples collected in a 4-m snow pit at Dome Argus (Dome A) on the East Antarctic Plateau, covering the period from 1950 to 2016 A.D. We found great variability in the annual concentration of all metals. The crustal enrichment factors suggest that the concentrations of some heavy metals (Cd, Sb, Cu, As and Pb) were likely influenced by anthropogenic activities in recent decades. An analysis of source regions suggests that heavy metal pollution at Dome A was largely caused by human activities in Australia and South America (e.g. mining production, leaded gasoline). Based on the relationship between the trace elements fluxes and sea ice concentration (SIC), sea surface temperature (SST) and annual mean air temperature at 2 m above the ground (T₂ₘ), our analysis shows that deposition and transport of atmospheric aerosol at Dome A were influenced by circum-Antarctic atmospheric circulations.

Quantifying source apportionment of potentially toxic elements (PTEs) in soils and associated human health risk (HHR) is essential for soil environment regulation and pollution risk mitigation. For this purpose, an integrated method was proposed, and applied to a dataset consisting of As, Cd, Cr, Cu, Hg, Ni, Pb, Se, and Zn in 273 soil surface samples. Positive matrix factorization (PMF) was used to quantitatively examine sources contributions of PTEs in soils; and the HHR arising from the identified source was determined by combining source profiles and health risk assessment; at last, sequential Gaussian simulation (SGS) was used to identify the areas with high HHR. Four sources were identified by PMF. Natural and agricultural sources affected all 9 PTEs contents with contributions ranging from 19.2% to 62.9%. 41.9% of Cd, 40.8% of Pb, 58.6% of Se, and 29.8% of Zn were controlled by industrial and traffic emissions. Metals smelting and mining explained 35.5%, 30.5%, and 24.9% of Cr, Cu, and Ni variations, respectively. Hg was dominated by atmospheric deposition from coal combustion and coking (58.7%). The mean values of the total non-carcinogenic risks of PTEs were 1.55 × 10⁻¹ and 9.40 × 10⁻¹ for adults and children, and the total carcinogenic risk of PTEs had an average value of 8.86 × 10⁻⁵. Based on source-oriented HHR calculation, natural and agricultural sources were the most important factor influencing HHR, explaining 51.0% and 49.1% of non-carcinogenic risks for children and adults, and 44.2% of carcinogenic risk. SGS indicated that 1.1% of the total area was identified as hazardous areas with non-carcinogens risk for children.

Critical loads are thresholds of atmospheric deposition below which harmful ecological effects do not occur. Because lichens are sensitive to atmospheric deposition, lichen-based critical loads can foreshadow changes of other forest processes. Here, we derive critical loads of nitrogen (N) and sulfur (S) deposition for continental US and coastal Alaskan forests, based on nationally consistent lichen community surveys at 8855 sites. Across the eastern and western US ranges of 459 lichen species, each species' realized optimum was the N or S atmospheric deposition value at which it most frequently occurred. The mean of optima for all species at a site, weighted by their abundances, was defined as a community “airscore” indicative of species’ collective responses to atmospheric deposition. To determine critical loads for adverse community compositional shifts, we then modeled changes in airscores as a function of deposition, climate and forest habitat predictors in nonparametric multiplicative regression. Critical loads, indicative of initial shifts from pollution-sensitive toward pollution-tolerant species, occurred at 1.5 kg N ha⁻¹ y⁻¹ and 2.7 kg S ha⁻¹ y⁻¹. Importantly, these critical loads remain constant under any climate regime nationwide, suggesting both simplicity and nationwide applicability. Our models predict that preventing excess N deposition of just 0.2–2.0 kg ha⁻¹ y⁻¹ in the next century could offset the detrimental effects of predicted climate warming on lichen communities. Because excess deposition and climate warming both harm the most ecologically influential species, keeping conditions below critical loads would sustain both forest ecosystem functioning and climate resilience.

Anthropogenic activities have increased lead (Pb) emissions and impacted their spatiotemporal distributions in coastal seas. To quantify the increasing variability of Pb and identify the specific origins and their corresponding magnitudes, Pb and Pb isotopes are investigated in a well-placed sediment core covering the period of 1928–2008 in the Central Yellow Sea Mud (CYSM). The concentration of Pb varied from 27.17 μg/g to 37.30 μg/g upwardly along the core, with pronounced anthropogenic disturbance since the late 1960s. The Pb input history of the CYSM experienced five stages according to industrialization levels and Pb contamination, with relative pristine stages from 1928 to 1969 and human activity-impacted stages from 1969 to 2008. The ²⁰⁶Pb/²⁰⁷Pb ratio demonstrated an overall decreasing profile while the ²⁰⁸Pb/²⁰⁶Pb ratio displayed the reverse trend upwardly along the core, possibly due to the atmospheric delivery of anthropogenic Pb emissions from northern China. Furthermore, ²⁰⁸Pb/²⁰⁶Pb vs. ²⁰⁶Pb/²⁰⁷Pb shows certain linearity between natural sediment sources and anthropogenic emissions of Pb (atmospheric deposition); thus, atmospheric inputs account for 34–43% of the Pb in the sediment since Pb enrichment using the two-endmember mixing model. Moreover, the steep decrease in ²⁰⁶Pb/²⁰⁷Pb and rapid increase in ²⁰⁸Pb/²⁰⁶Pb since the 1970s suggest the introduction of leaded gasoline and the increasing proportionate consumption of gasoline relative to total energy consumption. The continuously decreasing ²⁰⁶Pb/²⁰⁷Pb ratio and increasing ²⁰⁸Pb/²⁰⁶Pb ratio since 2000 are the combined results of coal consumption, nonferrous smelting, and residual Pb contamination from leaded gasoline, which is quite distinctive from cases in North America and Europe. The relatively high ²⁰⁶Pb/²⁰⁷Pb and low ²⁰⁸Pb/²⁰⁶Pb ratios before 1969 represent the natural Pb isotopic signatures. Hence, Pb input is significantly affected by regional energy consumption and restructuring, and the Pb isotopic ratios may be a potential proxy for the shift in energy consumption.

Terrestrial mosses are promising tracers for research concerning metal atmospheric deposition and pollution. Concentrations of Cr, Co, Ni, Zn, Sr, Cd, Ba, and Pb in different moss species from Mountain Gongga, China were analyzed to investigate the effects of growth substrates, geographic elevation, and type of moss species on the accumulation characteristics of heavy metals, as well as to identify heavy metal sources. The ability of heavy metals to accumulate in moss varied significantly, with low concentrations of Cd and Co; medium concentrations of Cr, Ni, and Pb; and high concentrations of Zn, Sr, and Ba. Elevation significantly influenced the accumulation characteristics of heavy metals, with high concentrations found at lower elevations due to proximal pollution. Growth substrate and moss species were found to have certain influence on the bioconcentration capacities of heavy metals in moss in this study. Correlation analysis showed similar sources for Sr, Zn, and Ba, as well as for Ni, Co, and Cr. The positive matrix factorization (PMF) model was consistent with atmospheric deposition of Pb and Cd; substrate sources of Cr, Co, and Ni; and anthropogenic sources of Ba, Sr, and Zn. This research characterized the accumulation characteristics of heavy metals and their influence factors in different mosses found in alpine ecosystems and provides a reference for future studies in similar areas.

Inputs of polycyclic aromatic hydrocarbons (PAHs) of regulatory interest from diffuse atmospheric sources within urban areas frequently elevate local soil concentrations to levels requiring remediation despite the lack of in-situ contamination. This research sought to determine the distribution and potential health effects of aerially deposited PAHs in soil within the urban core of metropolitan Milwaukee, Wisconsin, U.S.A. as part of a soil regulatory standards reevaluation. Park areas (n = 27) identified as undisturbed for 80+ years, containing no fill material, and receiving only atmospheric deposition were selected for composite surface and 92 cm core soil sample collection (n = 295). Samples were analyzed for the 16 USEPA priority PAHs, 1- and 2- methylnapthalene and ancillary soil properties. Soil core and ancillary data confirm lack of site disturbance. PAH diagnostic ratios and homologue summations indicate that diffuse multiple point source emissions contribute equally to PAH deposition throughout the area. Benzo(a)pyrene (BaP) and dibenz(a,h)anthracene mean concentrations exceed health-based clean up levels. Risk assessment shows only a worst-case exposure scenario (BaP at the 95% upper confidence limit) increasing cancer risk (1.67 × 10⁻⁶) over current regulatory thresholds (1.0 × 10⁻⁶). Health quotients show potential health risks from fluoranthene and pyrene for daily park users and from BaP for all others. Mean soil PAH values are similar to New Orleans, but lower than Chicago, Boston, and London reflecting industrial history and site selection protocols. The soil PAH results presented here for sites selected for non-manipulated soils combined with an almost 100-year uninterrupted atmospheric exposure effectively show the maximum potential PAH values that can be found at any given undisturbed location within the Milwaukee urban core due solely to atmospheric deposition.

The identification of nitrate (NO₃⁻) sources and biogeochemical transformations is critical for understanding the different nitrogen (N) pathways, and thus, for controlling diffuse pollution in groundwater affected by livestock and agricultural activities. This study combines chemical data, including environmental isotopes (δ²HH₂O, δ¹⁸OH₂O, δ¹⁵NNO₃, and δ¹⁸ONO₃), with land use/land cover data and a Bayesian isotope mixing model, with the aim of reducing the uncertainty when estimating the contributions of different pollution sources. Sampling was taken from 53 groundwater sites in Comarca Lagunera, northern Mexico, during 2018. The results revealed that the NO₃⁻ (as N) concentration ranged from 0.01 to 109 mg/L, with more than 32% of the sites exceeding the safe limit for drinking water quality established by the World Health Organization (10 mg/L). Moreover, according to the groundwater flow path, different biogeochemical transformations were observed throughout the study area: microbial nitrification was dominant in the groundwater recharge areas with elevated NO₃⁻ concentrations; in the transition zones a mixing of different transformations, such as nitrification, denitrification, and/or volatilization, were identified, associated to moderate NO₃⁻ concentrations; whereas in the discharge area the main process affecting NO₃⁻ concentrations was denitrification, resulting in low NO₃⁻ concentrations. The results of the MixSIAR isotope mixing model revealed that the application of manure from concentrated animal-feeding operations (∼48%) and urban sewage (∼43%) were the primary contributors of NO₃⁻ pollution, whereas synthetic fertilizers (∼5%), soil organic nitrogen (∼4%), and atmospheric deposition played a less important role. Finally, an estimation of an uncertainty index (UI90) of the isotope mixing results indicated that the uncertainties associated with atmospheric deposition and NO₃⁻−fertilizers were the lowest (0.05 and 0.07, respectively), while those associated with manure and sewage were the highest (0.24 and 0.20, respectively).