The Cleveland airshed comprises a complex mixture of industrial source emissions that contribute to periods of non-attainment for fine particulate matter (PM2.5) and are associated with increased adverse health outcomes in the exposed population. Specific PM sources responsible for health effects however are not fully understood. Size-fractionated PM (coarse, fine, and ultrafine) samples were collected using a ChemVol sampler at an urban site (G.T. Craig (GTC)) and rural site (Chippewa Lake (CLM)) from July 2009 to June 2010, and then chemically analyzed. The resulting speciated PM data were apportioned by EPA positive matrix factorization to identify emission sources for each size fraction and location. For comparisons with the ChemVol results, PM samples were also collected with sequential dichotomous and passive samplers, and evaluated for source contributions to each sampling site. The ChemVol results showed that annual average concentrations of PM, elemental carbon, and inorganic elements in the coarse fraction at GTC were ∼2, ∼7, and ∼3 times higher than those at CLM, respectively, while the smaller size fractions at both sites showed similar annual average concentrations. Seasonal variations of secondary aerosols (e.g., high NO3− level in winter and high SO42− level in summer) were observed at both sites. Source apportionment results demonstrated that the PM samples at GTC and CLM were enriched with local industrial sources (e.g., steel plant and coal-fired power plant) but their contributions were influenced by meteorological conditions and the emission source's operation conditions. Taken together the year-long PM collection and data analysis provides valuable insights into the characteristics and sources of PM impacting the Cleveland airshed in both the urban center and the rural upwind background locations. These data will be used to classify the PM samples for toxicology studies to determine which PM sources, species, and size fractions are of greatest health concern.

To investigate the size distributions of chemical compositions and sources of particulate matter (PM) at ground level and from the urban canopy, a study was conducted on a 255 m meteorological tower in Tianjin from December 2013 to January 2014. Thirteen sets of 8 size-segregated particles were collected with cascade impactor at 10 m and 220 m. Twelve components of particles, including water-soluble inorganic ions and carbonaceous species, were analyzed and used to apportion the sources of PM with positive matrix factorization. Our results indicated that the concentrations, size distributions of chemical compositions and sources of PM at the urban canopy were affected by regional transport due to a stable layer approximately 200 m and higher wind speed at 220 m. The concentrations of PM, Cl− and elemental carbon (EC) in fine particles at 10 m were higher than that at 220 m, while the reverse was true for NO3− and SO42−. The concentrations of Na+, Ca2+, Mg2+, Cl− and EC in coarse particles at 10 m were higher than that at 220 m. The size distributions of major primary species, such as Cl−, Na+, Ca2+, Mg2+ and EC, were similar at two different heights, indicating that there were common and dominant sources. The peaks of SO42−, NH4+, NO3− and organic carbon (OC), which were partly secondary generated species, shifted slightly to the smaller particles at 220 m, indicating that there was a different formation mechanism. Industrial pollution and coal combustion, re-suspended dust and marine salt, traffic emissions and transport, and secondary inorganic aerosols were the major sources of PM at both heights. With the increase in vertical height, the influence of traffic emissions, re-suspended dust and biomass burning on PM weakened, but the characteristics of regional transport from Hebei Province and Beijing gradually become obvious.

To design effective PM2.5 control strategies in urban centers, there is a need to better understand local and remote sources influencing PM2.5 levels and associated risk to public health. An investigation of PM2.5 levels, sources and potential human health risk associated with trace elements in the PM2.5 was undertaken in Edmonton over a 6-year period (September 2009–August 2015). The geometric mean PM2.5 concentration of was 7.11 μg/m3 (interquartile range, IQR = 4.83–10.08 μg/m3). Positive matrix factorization (PMF) receptor modeling identified secondary organic aerosol (SOA) as the major contributor (2.2 μg/m3, 27%), followed by secondary nitrate (1.3 μg/m3, 17%) and secondary sulfate (1.2 μg/m3, 15%). Other local sources included transportation (1.1 μg/m3, 14%) and industry-related emissions (0.26 μg/m3, 3.4%), biomass burning (1.0 μg/m3, 13%) and soil (0.54 μg/m3, 6.8%). Five factors (i.e., SOA, secondary nitrate, secondary sulfate, transportation and biomass burning) contributed more than 85% to PM2.5 for the 2009–2015 period. Geometric (arithmetic) mean and maximum ambient air concentrations for hazardous trace elements of public health concern in PM2.5 during the study period were below United States regulatory agency chronic and acute health risk screening criteria. Carcinogenic and non-carcinogenic risk of trace elements and source-specific risk values were well below acceptable and safe levels of risks recommended by regulatory agencies. More work is needed to understand the origin of potential SOA and wintertime wood burning sources in Edmonton and the surrounding region and to apply source-risk apportionment using all available hazardous air pollutants (HAPs) including organic compounds to better interpret the potential health risk posed by various sources in urban areas.

In the Athabasca Oil Sands Region in northeastern Alberta, Canada, oil sands operators are testing the feasibility of peatland construction on the post-mining landscape. In 2009, Syncrude Canada Ltd. began construction of the 52 ha Sandhill Fen pilot watershed, including a 15 ha, hydrologically managed fen peatland built on sand-capped soft oil sands tailings. An integral component of fen reclamation is post-construction monitoring of water quality, including salinity, fluvial carbon, and priority pollutant elements. In this study, the effects of fen reclamation and elevated sulfate levels on mercury (Hg) fate and transport in the constructed system were assessed. Total mercury (THg) and methylmercury (MeHg) concentrations in the fen sediment were lower than in two nearby natural fens, which may be due to the higher mineral content of the Sandhill Fen peat mix and/or a loss of Hg through evasion during the peat harvesting, stockpiling and placement processes. Porewater MeHg concentrations in the Sandhill Fen typically did not exceed 1.0 ng L−1. The low MeHg concentrations may be a result of elevated porewater sulfate concentrations (mean 346 mg L−1) and an increase in sulphide concentrations with depth in the peat, which are known to suppress MeHg production. Total Hg and MeHg concentrations increased during a controlled mid-summer flooding event where the water table rose above the ground surface in most of the fen. The Hg dynamics during this event showed that hydrologic fluctuations in this system exacerbate the release of THg and MeHg downstream. In addition, the elevated SO42− concentrations in the peat porewaters may become a problem with respect to downstream MeHg production once the fen is hydrologically connected to a larger wetland network that is currently being constructed.

Rigorous studies of recovery from soil acidification are rare. Hence, we resampled 97 old-growth beech stands in the Vienna Woods. This study exploits an extensive data set of soil (infiltration zone of stemflow and between trees area at different soil depths) and foliar chemistry from three decades ago. It was hypothesized that declining acidic deposition is reflected in soil and foliar chemistry. Top soil pH within the stemflow area increased significantly by 0.6 units in both H2O and KCl extracts from 1984 to 2012. Exchangeable Ca and Mg increased markedly in the stemflow area and to a lower extent in the top soil of the between trees area. Trends of declining base cations in the lower top soil were probably caused by mobilization of organic S and associated leaching with high amounts of sulfate. Contents of C, N and S decreased markedly in the stemflow area from 1984 to 2012, suggesting that mineralization rates of organic matter increased due to more favorable soil conditions. It is concluded that the top soil will continue to recover from acidic deposition. However, in the between trees areas and especially in deeper soil horizons recovery may be highly delayed. The beech trees of the Vienna Woods showed no sign of recovery from acidification although S deposition levels decreased. Release of historic S even increased foliar S contents. Base cation levels in the foliage declined but are still adequate for beech trees. Increasing N/nutrient ratios over time were considered not the result of marginally higher N foliar contents in 2012 but of diminishing nutrient uptake due to the decrease in ion concentration in soil solution. The mean foliar N/P ratio already increased to the alarming value of 31. Further nutritional imbalances will predispose trees to vitality loss.

Perennial plant communities in the proximity of metal smelters and refineries may receive substantial inputs of base metal particulate as well as sulphate from the co-emission of sulphur dioxide. The Ni refinery at Port Colborne (Canada) operated by Inco (now Vale Canada Ltd.) emitted Ni, Co and Cu, along with sulphur dioxide, between 1918 and 1984. The objectives were to determine if vascular plant community composition, including standing litter, in twenty-one woodlots on clay or organic soil, were related to soil Ni concentration which decreased in concentration with distance from the Ni refinery. The soil Ni concentration in the clay woodlots ranged from 16 to 4130 mg Ni/kg, and in the organic woodlots, ranged from 98 to 22,700 mg Ni/kg. The concentrations of Co and Cu in the soils were also elevated, and highly correlated with soil Ni concentration. In consequence, each series of woodlots constituted a ‘fixed ratio ray’ of metal mixture exposure. For each of the woodlots, there were 16 independent measurements of ‘woodlot status’ which were correlated with elevated soil Ni concentration. Of the 32 combinations, there were eight linear correlations with soil Ni concentration, considerably more than would be expected by chance alone at a p-value of 0.05. With the exception of mean crown rating for shrubs at the clay sites, the correlations were consistent with the hypothesis that increased soil metal concentrations would be correlated with decreased diversity, plant community health or fitness, and increased accumulation of litter. Only five of the eight linear correlations were from the organic woodlots, suggesting that the observations were not confounded with soil type nor range in soil metal concentrations.

Understanding the evolution of aerosols in the atmosphere is of great importance for improving air quality and reducing aerosol-related uncertainties in global climate simulations. Here, a unique haze episode at a regional receptor site near the East China Sea was examined as a case study of the aging process of atmospheric aerosols during transport. An increase in photochemical age from 5 h to more than 25 h and a progressive increase in the fitted mean particle diameter from 70 nm to approximately 300 nm were observed. According to the pollution features and meteorology conditions involved, pollution accumulation (PA), sea breeze (SB), and land breeze (LB) periods were identified. Concentrations of black carbon (BC), hydrocarbon-like organic aerosols (HOA), semi-volatile oxidized organic aerosols (SV-OOA), and nitrate increased by 7-fold up to 39-fold when the air masses passed through Taizhou, a nearby city. In addition, nitrate and SV-OOA dominated the aerosol composition in the urban outflow plumes (52% and 18%, respectively), yet they gradually decreased in concentration during transport. In contrast, sulfate and the low-volatile oxidized organic aerosols (LV-OOA) exhibited more regional footprints and potentially have similar formation mechanisms. The atomic oxygen-to-carbon (O/C) ratio also increased from 0.45 to 0.9, thereby suggesting that rapid formation of highly oxidized secondary organic aerosols (SOA) occurred during transport. Overall, these results provide valuable insight into the evolution of the chemical and physical features of aerosol pollution during transport and also highlight the need for regulatory controls of nitrogen oxides, sulfur dioxide, and VOCs to improve air quality on different scales.

Atmospheric black carbon (BC) is an important pollutant for both air quality and Earth's energy balance. Estimates of BC climate forcing remain highly uncertain, e.g., due to the mixing with non-absorbing components. Non-absorbing aerosols create a coating on BC and may thereby act as a lens which may enhance the light absorption. However, this absorption enhancement is poorly constrained. To this end a two-step solvent dissolution protocol was employed to remove both organic and inorganic coatings, and then investigate their effects on BC light absorption. Samples were collected at a severely polluted urban area, Jinan, in the North China Plain (NCP) during February 2014. The BC mass absorption cross-section (MAC) was measured for the aerosol samples before and after the solvent-decoating treatment, and the enhancement of MAC (EMAC) from the coating effect was defined as the ratio. A distinct diurnal pattern for the enhancement was observed, with EMAC 1.3 ± 0.3 (1 S.D.) in the morning, increasing to 2.2 ± 1.0 in the afternoon, after that dropping to 1.5 ± 0.8 in the evening-night. The BC absorption enhancement primarily was associated with urban-scale photochemical production of nitrate and sulfate aerosols. In addition to that, regional-scale haze plume with increasing sulfate levels strengthened the absorption enhancement. These observations offer direct evidence for an increased absorption enhancement of BC due to severe air pollution in China.

The aim of this study was to identify how hydrologic factors (e.g., rainfall, maximum depth, reservoir and catchment area, and water residence time) and water chemistry factors (e.g., conductivity, pH, suspended particulate matter, chlorophyll-a, dissolved organic carbon, and sulfate) interact to affect the spatial variance in monomethylmercury (MMHg) concentration in nine artificial reservoirs. We hypothesized that the MMHg concentration of reservoir water would be higher in eutrophic than in oligotrophic reservoirs because increased dissolved organic matter and sulfate in eutrophic reservoirs can promote in situ production of MMHg. Multiple tools, including Pearson correlation, a self-organizing map, and principal component analysis, were applied in the statistical modeling of Hg species. The results showed that rainfall amount and hydraulic residence time best explained the variance of dissolved Hg and dissolved MMHg in reservoir water. High precipitation events and residence time may mobilize Hg and MMHg in the catchment and reservoir sediment, respectively. On the contrary, algal biomass was a key predictor of the variance of the percentage fraction of unfiltered MMHg over unfiltered Hg (%MMHg). The creation of suboxic conditions and the supply of sulfate subsequent to the algal decomposition seemed to support enhanced %MMHg in the bloom reservoirs. Thus, the nutrient supply should be carefully managed to limit increases in the %MMHg/Hg of temperate reservoirs.

Following Europe and North America, East Asia has become a global hotspot for acid deposition, with very high deposition of both sulfur (S) and nitrogen (N) occurring in large areas of southwest and southeast China. This study shows that the outflow flux of sulfate (SO42−) in three major tributaries of the Upper Yangtze River in the Sichuan Basin in southwest China has been increasing over the last three decades, which implies the regional soil acidification caused by increasing sulfur dioxide (SO2) emissions. Since 2005, the outflow of SO42− to the Upper Yangtze River from the Sichuan Basin has even reached the atmospheric SO2 emission from the basin. In contrast to S emissions, the rapid increase in nitrogen (N) emissions, including nitrogen oxides (NOx) and ammonia (NH3), have resulted in only a slight increase in nitrate (NO3−) concentrations in surface waters, indicating a large retention of N in the basin. Although N deposition currently contributes much less than S to soil acidification in this area, it is possible that catchments receiving a high input of N may be unable to retain a large fraction of the N deposition over long periods.