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High emissions of air pollutants from Northeast Asia are strongly influenced by air quality as well as by ecosystems. This study investigated the spatiotemporal variations in the sulfur isotopic ratio (δ34S) in atmospheric deposition at eleven monitoring stations in Japan from 2011 to 2016 and estimated the amount of transboundary transported anthropogenic sulfate (TRB) deposition using mass balance calculations. The δ34S of sulfate in precipitation ranged from −0.42 to +22.7‰. Sea salt (SS), TRB, and domestic anthropogenic sources (DOM) were the dominant sources of sulfate deposition in Japan. TRB sulfate deposition was largest on the Sea of Japan side, with an annual average value of 1.5 ± 0.3–6.9 ± 0.5 mg m−2 d−1 (36–44%), followed by Mt. Happo (4.5 ± 0.1 mg m−2 d−1; 88%), the Pacific Ocean side (1.5 ± 0.8, 4.3 ± 0.9 mg m−2 d−1; 24–50%), and the remote islands in the North Pacific Ocean (1.1 ± 0.2, 2.0 ± 0.8 mg m−2 d−1; 19–32%). TRB sulfate deposition on the Sea of Japan side was 2–12 times higher in winter and 1–2 times higher in summer than that of DOM. In contrast, TRB sulfate deposition on the Pacific Ocean side was 1.5–3 times higher in summer than in winter due to high precipitation levels. In Tokyo, the annual contribution from DOM sulfate deposition is approximately three times higher than that from TRB. Annual TRB sulfate deposition is lowest at Ogasawara at 1.1 ± 0.2 mg m−2 d−1, and the annual oceanic DMS contribution to sulfate deposition is high, accounting for 1.3 mg m−2 d−1 (20 ± 6%). The contribution of Asian dust was estimated to be 1–5.2 mg m−2 d−1(3–6%), which occurred in a single Asian dust event on the Sea of Japan side. Unlabelled Image • Spatiotemporal variations of the sulfur isotopic ratio in atmospheric deposition in Japan were investigated. • δ34S of sulfate in precipitation were seasonal variation with high in winter. • Contribution from transbundary transported sulfur deposition was larger than those of domestic sources. • Contribution from domestic sulfur deposition was larger in the Pacific Ocean site. [ABSTRACT FROM AUTHOR]

Sulfate (SO 4 2−) has received attention as means of monitoring water quality and pollution. However, the SO 4 2− content of rivers, lakes, and reservoirs varies significantly by season, so environmental factors such as temperature can affect it. An experiment was conducted with a series of aerobic and anaerobic tanks containing Pearl River sediments and distilled water to assess the release of SO 4 2− from sediments under controlled conditions. "Black-odor river" refers to near anoxic conditions in the water column and foul odors emanating from affected rivers in southeastern China. These river systems typical have sediments containing ammonia (NH 3), hydrogen sulfide (H 2 S), and organic sulfide compounds in excess, and precipitates of sulfide (S2−), with ferrous (Fe2+) or manganese (Mn2+). SO 4 2− concentration was measured at various depths in pore water and in the water column while controlling temperature and dissolved oxygen (DO) concentrations. Interpolation of study results revealed that SO 4 2− content was highest between temperatures of 20 °C and 25 °C. The relationship between SO 4 2− concentration, which varied with temperature and time, was fit using a linearized Michaelis-Menten function (R2 = 0.69). The release of SO 4 2− to the water column was accelerated during the experiment (for temperatures higher than 20 °C), and led to higher SO 4 2− content in the water column than in pore water. The maximum concentration of SO 4 2− within the sediment occurred at a temperature of 20 °C. Comparing aerated and non-aerated tanks at 20 °C, we found that O 2 restricted SO 4 2− content in the water column; DO could, in turn, also be controlled by temperature. Fe2+ and Mn2+ had a negative correlation with SO 4 2−. Unlabelled Image • Derived a general relationship for sulfate concentration in the water column. • Assessed distribution of sulfate in water column and sediment with temperature. • Estimated sulfate flux at the sediment-water interface at different temperatures. • Assessed the effect of ferrous and manganese ions on sulfate content. • Assessed effects of dissolved oxygen, pH, etc., on sulfate release from sediments. [ABSTRACT FROM AUTHOR]

To better understand the role of stationary sources during the evolution of haze, we investigated sulfate formation characteristics at different stages of four haze events in Beijing, China. The mass fraction of sulfate in PM 2.5 increased while that of nitrate declined slightly during the worsening process of most haze events, consistent with higher ratios of SO 4 2−/NO 3 − on haze days (0.50 on average) than those on clean days (0.32 on average). Further calculations indicated that sulfate had a higher mass growth rate than nitrate during the haze-worsening process, probably due to regional transport of sulfate from heavy industrial areas accompanied by increased sulfate secondary transformation during polluted periods. We quantitatively evaluated the contribution of the S(IV) + NO 2 reaction (pH-dependent) in sulfate formation during the haze evolution. The production rate (P S(IV)+NO2) of the S(IV) + NO 2 pathway ranged from 1.97 × 10−4 to 5.91 (mean: 0.39) μg·m−3·h−1. Its proportion to sulfate total heterogeneous production rate (P S(IV)+NO2 / P het) was generally correlated positively with PM 2.5 concentrations, indicating the relative importance of this pathway on haze days. Due to the mutual restriction between aerosol pH and aerosol liquid water content (ALWC) during haze evolution, the relative contribution of the S(IV) + NO 2 pathway to sulfate heterogeneous formation was generally limited to 40%. Unlabelled Image • Compositions of secondary inorganic aerosols collected during haze events in Beijing are analyzed. • Sulfate has a higher mass growth rate than nitrate during the haze-worsening process. • Rapid increase of sulfate is caused by regional-transport together with secondary transformation. • The relative contribution of the S(IV) + NO 2 pathway to sulfate heterogeneous formation is generally limited to 40%. [ABSTRACT FROM AUTHOR]

Abstract China is the largest anthropogenic aerosol-generating country worldwide; however, few studies have analyzed the PM 2.5 chemical components and their underlying precursor emissions over long periods and across the national domain. First, global 3-D tropospheric chemistry and transport model (GEOS-Chem)-integrated satellite-retrieved aerosol optical depth (AOD) and vertical profiles were used to estimate near-surface sulfate and nitrate levels at 10-km resolution over China from 2006 to 2014. Ground measurement validation of our satellite model yielded correlation coefficients (r) of 0.7 and 0.73 and normalized mean bias (NMB) values of −37.96% and − 32.73% for sulfate and nitrate, respectively. Second, analyses of the spatiotemporal distributions of sulfate and nitrate as well as the vertical density Ozone Monitoring Instrument (OMI)-measured SO 2 (PBL_SO 2) and NO 2 (TVCD_NO 2) indicated that the highest nitrate and sulfate levels occurred in the North China Plain (~25 μg/m3) and Sichuan Basin (SCB) (~30 μg/m3), respectively. The long-term variations in the estimated components and precursor gases indicated that the large sulfate decline was positively correlated with the SO 2 emission reduction due to the mandatory desulfurization implemented in 2007. The annual growth rate of sulfate relative to the national mean was −6.19%/yr, and the concentration decreased by 17.10% from 2011 to 2014. Energy consumption increases and a lack of control measures for NO 2 resulted in persistent increases in NO 2 emissions and nitrate concentrations from 2006 to 2010, particularly in the SCB. With energy consumption structure advancements, reductions in NO 2 emissions and corresponding nitrate levels over three typical regions were prominent after 2012. Third, the estimated national-scale uncertainties of satellite datasets at 0.1° × 0.1° were 26.88% for sulfate and 25.55% for nitrate. Differences in the spatial distributions and temporal trends between our estimated components and precursor gases were mainly attributed to the dataset accuracy, the data pre-processing strategy, inconsistent column density and near-surface mass concentration, meteorological variables and complex chemical reactions. Graphical abstract Spatial distributions of a) NO 3 −, b) average TVCD_NO 2 , c) sulfate and d) PBL_SO 2 for the difference between 2014 and 2006. The three red boxes in each subfigure denote the NCP, SCB and PRD regions. Unlabelled Image Highlights • Ground measurement validation of our model yielded r of 0.7 and 0.73 for sulfate and nitrate, respectively. • The highest nitrate and sulfate levels occurred in the NCP (~25 μg/m3) and SCB (~30 μg/m3), respectively. • The large sulfate decline was positively correlated with the SO 2 emission reduction due to the FGD implemented in 2007. • Reductions in NO 2 emissions and corresponding nitrate levels over three typical regions were prominent after 2012. • Meteorology and chemical reaction play different roles in the difference of secondary particle and precursor gas. [ABSTRACT FROM AUTHOR]

Abstract The Cuatro Cienegas Basin (CCB) in the Chihuahuan desert is characterized by the presence of over 500 ponds located in an endorheic basin. These ponds are subsaline ecosystems characterized by a low productivity and a particularly high sulfate concentration, comparable to marine environments. This study focused on assessing the main physicochemical parameters in these ponds along with the characterization of the CH 4 dynamics through the determination of fluxes, dissolved CH 4 concentrations, and net methanotrophic and methanogenic activity. Despite a sulfate concentration ranging from 1.06 to 4.73 g L−1, the studied ponds showed moderate but clear CH 4 production and emission, which suggests that methanogenesis is not completely outcompeted by sulfate reduction. CH 4 fluxes ranged from 0.12 to 0.98 mg m−2 d−1, which falls within the higher range of marine emissions and within the lower range reported for coastal saline lagoons and saline ponds. During summer, significant CH 4 production in the oxic water column was observed. In addition to CH 4 , CO 2 fluxes were determined at levels from 0.2 to 53 g m−2 d−1, which is within the range recorded for saline lakes in other parts of the world. Our results provide additional evidence that subsaline/saline aquatic ecosystems play an important role in the emission of greenhouse gases to the atmosphere. Graphical abstract Unlabelled Image Highlights • The ponds of the Chihuahuan Desert are subsaline ecosystems with low productivity. • These ecosystems present a sulfate concentration comparable to marine environments. • The ponds are net methane and carbon dioxide sources to the atmosphere. • Low rates of oxic methane production in the water column were also found. [ABSTRACT FROM AUTHOR]

Abstract Number of Chronic Kidney Disease patients with no identifiable cause (Chronic Kidney Disease Unknown Aetiology, CKDu) are escalating in the North Central Province (NCP) of Sri Lanka. This study examined distribution of dissolved organic carbon (DOC) in shallow groundwater of three CKDu risk zones (high risk, HR; low risk, LR and no risk, NR) and a control zone (CR) from wet to dry seasons. The interactions of DOC with calcium and magnesium ions and metabolites of selected pesticides were also examined. The lowest COD Mn DOC values of 0.60 ± 0.19, 0.58 ± 0.17 were reported in the DOC of the HR water in the wet and dry seasons, respectively, and this DOC fraction encompasses organic compounds with the lowest labile C with the highest aromaticity. Four distinct fluorescence DOC fractions in the HR water were identified with fulvic acid component associated as dominant non–labile C fraction. The essential building blocks of non–labile C were concentrated into molecular weight (MW) fraction II (900–1800 Da). The DOC source in all groundwater was identified as autochthonous (fluorescence index > 1.8). In the HR water, pentachlorophenol (PCP) was also detected in appreciable quantities. The factor loadings based on principal component analysis (PCA) showed a positive correlation between DOC and sulfate, calcium, total iron, PCP in the HR groundwater. Accordingly, it can be inferred that divalent cations (Ca2+, Mg2+) abundant in the HR groundwater interact with phenolate and carboxylate functional groups in DOC at alkaline pH. Graphical abstract Unlabelled Image Highlights • DOC in shallow groundwater of CKDu areas was characterized in dry and wet seasons. • Less oxidizable and higher aromatic fulvic acid fraction was observed in HR zone. • Autochthonous carbon source occurred in all groundwater DOC due to FI > 1.8. • 900–1800 Da MW fraction obtained as building block of refractory organic substances. • Significant correlations observed among DOC, PCP, Ca, sulfate, total Fe for HR. [ABSTRACT FROM AUTHOR]

Abstract Increased metal mining in the Arctic region has caused elevated loads of arsenic (As), antimony (Sb), nickel (Ni), and sulfate (SO 4 2−) to recipient surface or groundwater systems. The need for cost-effective active and passive mine water treatment methods has also increased. Natural peatlands are commonly used as a final step for treatment of mining influenced water. However, their permanent retention of harmful substances is affected by influent concentrations and environmental conditions. The effects of dilution, pH, temperature, oxygen availability, and contaminant accumulation on retention and leaching of As, Sb, Ni, and sulfate from mine process water and drainage water obtained from treatment peatlands in Finnish Lapland were studied in batch sorption experiments, and discussed in context of field data and environmental impacts. The results, while demonstrating effectiveness of peat to remove the target contaminants from mine water, revealed the risk of leaching of As, Sb, and SO 4 2− from treatment peatlands when diluted mine water was introduced. Sb was more readily leached compared to As while leaching of both was supported by higher pH of 9. No straightforward effect of temperature and oxygen availability in controlling removal and leaching was evident from the results. The results also showed that contaminant accumulation in treatment peatlands after long-term use can lead to decreased removal and escalated leaching of contaminants, with the effect being more pronounced for As and Ni. Graphical abstract Unlabelled Image Highlights • Retention of As, Sb, and Ni in peat from natural treatment wetlands was studied. • Contaminant accumulation in natural wetlands make them vulnerable to leaching. • Dilution of mining influenced water leads to leaching of As, Sb, and Ni. • Long-term use of wetlands decreases As and Ni removal/retention capacity. • Use of wetlands for treatment of wastewater should be carefully considered. [ABSTRACT FROM AUTHOR]

Abstract Twenty-six pairs of PM 2.5 and PM 10 samples were collected during haze episodes in Zhengzhou (113°28′ E, 34°37′ N), a highly populated city in North China. The samples were used to examine the inorganic ion chemistry of particulate matter (PM) of local origin at light (PM 2.5 < 60 μg m−3 and PM 10 < 135 μg m−3), medium (PM 2.5 : 60–170 μg m−3 and PM 10 : 135–325 μg m−3), and severe (PM 2.5 > 170 μg m−3 and PM 10 > 325 μg m−3) pollution levels. At the light and severe pollution levels, the increase of PM 10 was accounted for by the increase of PM 2.5 , and the variation of PM 10–2.5 was small. In contrast, the increase of PM 10 at the medium pollution level was caused by the increase in both PM 2.5 and PM 10–2.5. Sulfate (SO 4 2−), nitrate (NO 3 −), ammonium (NH 4 +), and chloride in the form of ammonium chloride (Cl− S) accounted for 47.8% and 60.3% of the PM 2.5 mass at the light and severe levels, respectively. These values indicate a large contribution of secondary inorganic species to the PM 2.5 growth. As the pollution level changed from light to medium, the contribution of SO 4 2− to the growth of PM 2.5 decreased from 49.0% to 15.1%, while those of NO 3 − and Cl− S increased from 25.1% and 0.6% to 32.5% and 2.8%, respectively, indicating the substantial production of nitrate and chloride. At the severe level, the contribution of SO 4 2− was 30.1%, while those of NO 3 − and Cl− S were 5.9% and 0.5%, respectively, suggesting a hindering effect of sulfate on the production of nitrate and chloride. These results indicate that the production of secondary species with the increase of PM 2.5 was dominated by sulfate-associated conversions at the light and severe pollution levels and was substantially influenced by nitrate- and chloride-associated conversions at the medium pollution level. The estimation of carbonate presence in the PM indicates that part of the carbonate in coarse particles (PM 10–2.5) of crustal origin enhanced sulfate production via heterogeneous surface reactions. Quantification of the contribution of primary and secondary species to PM 2.5 showed that it was dominated by both primary and secondary particles at the light pollution level, and it was mainly composed of secondary species at the severe pollution level. Graphical abstract Unlabelled Image Highlights • The particulate pollution at Zhengzhou was divided into three levels: light, medium and severe. • PM 10 increase was dominated by PM 2.5 at the light and severe levels, and by both PM 2.5 and PM 10–2.5 at the medium level. • Secondary aerosol species (inorganic and organic) are major contributors to PM 2.5 elevation. • SO 4 2− hindered NO 3 − formation in PM 2.5 when it constituted >20% of PM 2.5 in mass. [ABSTRACT FROM AUTHOR]

Pervasive particulate pollution has been observed over large areas of the North China Plain. The high level of sulfate, a major component in fine particles, is pronounced during heavy pollution periods. Being different from source apportionments by atmospheric chemistry-transport model and receptor modeling methods, here we utilize sulfur isotopes to discern the potential emission sources. Sixty-five daily PM 2.5 samples were collected at an urban site in Beijing between September 2013 and July 2014. Inorganic ions, organic/elemental carbon and stable sulfur isotopes of sulfate were analyzed. The “fingerprint” characteristics of stable sulfur isotopic composition, together with trajectory clustering modeled by HYSPLIT-4 (HYbrid Single-Particle Lagrangian Integrated Trajectory) and FLEXPART (“FLEXible PARTicle dispersion model”), was employed to identify potential aerosol sources in Beijing. Results exhibited a distinctive seasonality with sulfate, nitrate, ammonium, organic matter, and element carbon being the dominant species of PM 2.5 . Elevated concentrations of chloride with high organic matter were found in autumn and winter as a result of enhanced fossil fuel (mainly coal) combustion. The δ 34 S values of the Beijing aerosols ranged from 2.8‰ to 9.9‰ with an average of 6.0 ± 1.8‰, further indicating that the major sulfur source was direct coal burning emission. Owing to the changing patterns between oxidation pathways of S(IV) in different seasons, δ 34 S values varied with a winter maximum (8.2 ± 1.1‰) and a summer minimum (4.9 ± 1.9‰). The results of trajectory clustering and FLEXPART demonstrated that higher concentrations of sulfate with lower sulfur isotope ratios (4.6 ± 0.8‰) were associated with air masses from the south or east, whereas lower sulfate concentrations with heavier sulfur isotope ratios (6.7 ± 1.6‰) were observed when the air masses were mainly from the north or northwest. These results suggested that the fine aerosol pollution in Beijing, especially sulfate pollution, was mainly due to coal combustion sources from regional and local regions. [ABSTRACT FROM AUTHOR]

Macrophytes are shown to affect the microbial activity in different aqueous environments, with an altering of the sediment cycling of mercury (Hg) as a potential effect. Here, we investigated how a meadow with permanently submerged macrophytes in a contaminated brackish fjord in southern Norway influenced the conditions for sulfate reducing microbial activity, the methyl-Hg (MeHg) production and the availability of MeHg. Historically discharged Hg from a chlor-alkali plant (60–80 tons, 1947–1987) was evident through high Hg concentrations (491 mg Tot-Hg kg − 1 , 268 μg MeHg kg − 1 ) in intermediate sediment depths (10–20 cm) outside of the meadow, with reduced concentrations within the meadow. Natural recovery of the fjord was revealed by lower sediment surface concentrations (1.9–15.5 mg Tot-Hg kg − 1 , 1.3–3.2 μg MeHg kg − 1 ). Within the meadow, vertical gradients of sediment hydrogen sulfide (H 2 S) E h and pH suggested microbial sulfate reduction in 2–5 cm depths, coinciding with peak values of relative MeHg levels (0.5% MeHg). We assume that MeHg production rates was stimulated by the supply and availability of organic carbon, microbial activity and a sulfide oxidizing agent (e.g. O 2 ) within the rhizosphere. Following this, % MeHg in sediment (0–5 cm) within the meadow was approximately 10 × higher compared to outside the meadow. Further, enhanced availability of MeHg within the meadow was demonstrated by significantly higher fluxes ( p < 0.01) from sediment to overlying water (0.1–0.6 ng m − 2 d − 1 ) compared to sediment without macrophytes (0.02–0.2 ng m − 2 d − 1 ). Considering the productivity and species richness typical for such habitats, submerged macrophyte meadows located within legacy Hg contaminated sediment sites may constitute important entry points for MeHg into food webs. [ABSTRACT FROM AUTHOR]

The 2011 Richardson wildland mega-fire in the Athabasca Oil Sands Region (AOSR) in northern Alberta, Canada had large effects on air quality. At a receptor site in the center of the AOSR ambient PM 2.5 , O 3 , NO, NO 2 , SO 2 , NH 3 , HONO, HNO 3 , NH 4 + and NO 3 − were measured during the April–August 2011 period. Concentrations of NH 3 , HNO 3 , NO 2 , SO 2 and O 3 were also monitored across the AOSR with passive samplers, providing monthly summer and bi-monthly winter average values in 2010, 2011 and 2012. During the fire, hourly PM 2.5 concentrations > 450 μg m − 3 were measured at the AMS 1 receptor site. The 24-h National Ambient Air Quality Standard (NAAQS) of 35 μg m −3 and the Canada Wide Standard (CWS) of 30 μg m − 3 were exceeded on 13 days in May and 7 days in June. During the fire emission periods, sharp increases in NH 3 , HONO, HNO 3 , NH 4 + , NO 3 − and total inorganic reactive N concentrations occurred, all closely correlated with the PM 2.5 changes. There were large differences in the relative contribution of various N compounds to total inorganic N between the no-fire emission and fire emission periods. While in the absence of fires NO and NO 2 dominated, their relative contribution during the fires was ~ 2 fold smaller, mainly due to increased NH 3 , NH 4 + and NO 3 − . Concentrations of HONO and HNO 3 also greatly increased during the fires, but their contribution to the total inorganic N pool was relatively small. Elevated NH 3 and HNO 3 concentrations affected large areas of northern Alberta during the Richardson Fire. While NH 3 and HNO 3 concentrations were not at levels considered toxic to plants, these gases contributed significantly to atmospheric N deposition. Generally, no significant changes in O 3 and SO 2 concentrations were detected and their ambient concentrations were below levels harmful to human health or sensitive vegetation. [ABSTRACT FROM AUTHOR]

A decrease in flow from the iconic travertine mound springs of the Great Artesian Basin in South Australia has led to the oxidation of hypersulfidic soils and extreme soil acidification, impacting their unique groundwater dependent ecosystems. The build-up of pyrite in these systems occurred over millennia by the discharge of deep artesian sulfate-containing groundwaters through organic-rich subaqueous soils. Rare iron and aluminium hydroxysulfate minerals form thick efflorescences due to high evaporation rates in this arid zone environment, and the oxidised soils pose a significant risk to local aquatic and terrestrial ecosystems. The distribution of extreme acidification hazard is controlled by regional variations in the hydrochemistry of groundwater. Geochemical processes fractionate acidity and alkalinity into separate parts of the discharge zone allowing potentially extreme environments to form locally. Differences in groundwater chemistry in the aquifer along flow pathways towards the spring discharge zone are related to a range of processes including mineral dissolution and redox reactions, which in turn are strongly influenced by degassing of the mantle along deep crustal fractures. There is thus a connection between shallow critical zone ecosystems and deep crustal/mantle processes which ultimately control the formation of hypersulfidic soils and the potential for extreme geochemical environments. [ABSTRACT FROM AUTHOR]

This study examined the spatial and temporal trends of mercury (Hg) in wet deposition and air concentrations in the United States (U.S.) and Canada between 1997 and 2013. Data were obtained from the National Atmospheric Deposition Program (NADP) and Environment Canada monitoring networks, and other sources. Of the 19 sites with data records from 1997–2013, 53% had significant negative trends in Hg concentration in wet deposition, while no sites had significant positive trends, which is in general agreement with earlier studies that considered NADP data up until about 2010. However, for the time period 2007–2013 (71 sites), 17% and 13% of the sites had significant positive and negative trends, respectively, and for the time period 2008–2013 (81 sites) 30% and 6% of the sites had significant positive and negative trends, respectively. Non-significant positive tendencies were also widespread. Regional trend analyses revealed significant positive trends in Hg concentration in the Rocky Mountains, Plains, and Upper Midwest regions for the recent time periods in addition to significant positive trends in Hg deposition for the continent as a whole. Sulfate concentration trends in wet deposition were negative in all regions, suggesting a lower importance of local Hg sources. The trend in gaseous elemental Hg from short-term datasets merged as one continuous record was broadly consistent with trends in Hg concentration in wet deposition, with the early time period (1998–2007) producing a significantly negative trend (− 1.5 ± 0.2% year − 1 ) and the recent time period (2008–2013) displaying a flat slope (− 0.3 ± 0.1% year − 1 , not significant). The observed shift to more positive or less negative trends in Hg wet deposition primarily seen in the Central-Western regions is consistent with the effects of rising Hg emissions from regions outside the U.S. and Canada and the influence of long-range transport in the free troposphere. [ABSTRACT FROM AUTHOR]

Dry deposition is one of the most dangerous processes that can take place in the environment where the compounds that are suspended in the atmosphere can react directly on different surrounding materials, promoting decay processes. Usually this process is related with industrial/urban fog and/or marine aerosol in the coastal areas. Particularly, marine aerosol transports different types of salts which can be deposited on building materials and by dry deposition promotes different decay pathways. A new analytical methodology based on the combined use of Raman Spectroscopy and SEM-EDS (point-by-point and imaging) was applied. For that purpose, firstly evaporated seawater (presence of Primary Marine Aerosol (PMA)) was analyzed. After that, using a self-made passive sampler (SMPS), different suspended particles coming from marine aerosol (transformed particles in the atmosphere (Secondary Marine Aerosol (SMA)) and metallic airborne particulate matter coming from anthropogenic sources, were analyzed. Finally in order to observe if SMA and metallic particles identified in the SMPS can be deposited on a building, sandstone samples from La Galea Fortress (Getxo, north of Spain) located in front of the sea and in the place where the passive sampler was mounted were analyzed. [ABSTRACT FROM AUTHOR]

The abatement programs implanted in Europe to reduce SO 2 , NO 2 and NH 3 emissions are here evaluated by analyzing the relationships between emissions in Spain and neighboring countries and atmospheric deposition in a Mediterranean forest in the Montseny mountains (NE Spain) for the last 3 decades. A canopy budget model was applied to throughfall data measured during a period of high emissions (1995–1996) and a period of lower emissions (2011–2013) to estimate the changes in dry deposition over this time span. Emissions of SO 2 in Spain strongly decreased (77%) and that was reflected in reductions for nssSO 4 2 − in precipitation (65% for concentrations and 62% for SO 4 2 -S deposition). A lower decline was found for dry deposition (29%). Spanish NO 2 emissions increased from 1980 to 1991, remained constant until 2005, and decreased thereafter, a pattern that was paralleled by NO 3 − concentrations in bulk precipitation at Montseny. This pattern seems to be related to a higher share of renewable energies in electricity generation in Spain in recent years. However, dry deposition increased markedly between 1995 and 2012, from 1.3 to 6.7 kg ha − 1 year − 1 . Differences in meteorology between periods may have had a role, since the recent period was drier thus probably favoring dry deposition. Spanish NH 3 emissions increased by 13% between 1980 and 2012 in Spain but NH 4 + concentrations in precipitation and NH 4 + -N deposition showed a decreasing trend (15% reduction) at Montseny, probably linked to the reduction ammonium sulfate and nitrate aerosols to be scavenged by rainfall. NH 4 + -N dry deposition was similar between the compared periods. The N load at Montseny (15–17 kg ha − 1 year − 1 ) was within the critical load range proposed for Mediterranean sclerophyllous forests (15–17.5 kg ha − 1 year − 1 ). The onset of N saturation is suggested by the observed increasing N export in streamwaters. [ABSTRACT FROM AUTHOR]