The sulfate pollution in water environment gains more and more concerns in recent years. The discharge of domestic, municipal, and industrial wastewaters increases the riverine sulfate concentrations, which may cause local health and ecological problems. To better understand the sources of sulfate, this study collected water samples in a typical agricultural watershed in East Thailand. The source apportionment of sulfide was conducted by using stable isotopes and receptor models. The δ³⁴SSO₄ value of river water varied from 1.2‰ to 16.4‰, with a median value of 8.9‰. The hydrochemical data indicated that the chemical compositions of Mun river water were affected by the anthropogenic inputs and natural processes such as halite dissolution, carbonate, and silicate weathering. The positive matrix factorization (PMF) model was not suitable to trace source of riverine sulfate, because the meaning of the extracted factors seems to be vague. Based on the elemental ratio and isotopic composition, the inverse model yielded the relative contribution of sulfide oxidation (approximately 46.5%), anthropogenic input (approximately 41.5%), and gypsum dissolution (approximately 12%) to sulfate in Mun river water. This study indicates that the selection of models for source apportionment should be careful. The large contribution of anthropogenic inputs calls an urgent concern of the Thai government to establish effective management strategies in the Mun River basin.

Sulfate (SO₄²⁻) contamination in groundwater and surface water is an environmental problem of widespread concern. In this study, we combined stable isotope analyses of SO₄²⁻ (δ³⁴S and δ¹⁸O) and water (δ²H and δ¹⁸O) with a Bayesian mixing model (SIAR), for the first time, to identify sources and transformation of SO₄²⁻ in an area of northern China with multiple potential sources of pollution. The overall values of δ³⁴S and δ¹⁸O-SO₄²⁻ ranged from 1.3‰ to 16.3‰ and −3.8‰–8.8‰ in groundwater, and from −1.1‰ to 9.3‰ and 2.7‰–9.2‰ in surface waters, respectively. Analyses of SO₄²⁻ isotopes and water chemistry indicated that SO₄²⁻ in groundwater and surface water mainly originated from mixing of oxidation of sulfate, sewage, chemical fertilizers, dissolution of evaporite and precipitation. There was no significant correlation between δ³⁴S and δ¹⁸O and SO₄²⁻ concentration in groundwater, indicating that bacterial sulfate reduction did not affect the SO₄²⁻ isotopic composition. SIAR model showed the main sources of SO₄²⁻ in groundwater and surface water comprised oxidation of sulfide minerals and sewage. In groundwater, oxidation of sulfide minerals and sewage accounted for 37.5–44.5% and 35.5–42.7% of SO₄²⁻, respectively. In regard to surface waters, the contribution of oxidation of sulfide minerals to SO₄²⁻ was higher in the wet season (31.8 ± 9.9%) than in the intermediate (22.4 ± 7.8%) and dry (20.9 ± 8.2%) seasons, but the contribution proportion of sewage was slightly lower in the wet season (19.9 ± 8.5%) than in the intermediate (23.8 ± 8.7%) and dry (24.2 ± 8.5%) seasons. This study indicates that it is necessary for local government to improve the treatment infrastructure for domestic sewage and optimize methods of agricultural fertilization and irrigation to prevent SO₄²⁻ contamination of groundwater and surface water.

Mass concentrations of chemical compounds in both PM2.5 (particle aerodynamic diameter, Dp < 2.5 μm) and PM2.5-10 (2.5 < Dp < 10 μm), and acidity of aerosol particles were measured at an urban site in western Japan using a continuous dichotomous Aerosol Chemical Speciation Analyzer (ACSA-12) throughout 2014. Mass concentrations of both PM2.5 and sulfate had distinct seasonal variabilities with maxima in spring and winter, mostly due to long-range transport with the prevailing westerly wind. Mass concentration of nitrate in PM2.5 (fNO3) showed an obvious warm-season-low and cold-season-high pattern as a result of both gas-aerosol phase equilibrium processes under high temperature conditions as well as transport. Nitrate in PM2.5-10 (cNO3) increased during long-range transport of dust, implying the great importance of heterogeneous processes at the surface of coarse mode particles. In this study, Δ[H+] (derived from the difference in pH of extract liquid with/without sampling) was used to indicate the acidity of particles. We found that acidity of particles in PM2.5 (fΔH) was mostly positive with a maximum in August because of the large fraction of nitrate and sulfate. Acidity of particles in PM2.5-10 (cΔH) was negative in winter and spring due to presence of alkaline matter from crustal sources. This study highlights the great importance of anthropogenic pollutants on the acidity of particles in the western Pacific Ocean and further impact on the marine environment and climate.

In this study, concentrations of NOₓ, SO₂, O₃ and fine particles (PM₂.₅) were measured at three monitoring stations in Beijing during 2015. For extreme haze episodes during 25 Nov. - 3 Dec. 2015, observation data confirmed that high concentrations of NOₓ promoted the conversion of SO₂ to sulfate. Annual data confirmed that this is an important mechanism for the occurrence of heavy haze during winter in Beijing. Furthermore, in situ perturbation experiments in a potential aerosol mass (PAM) reactor were carried out at Shengtaizhongxin (STZX) station during both clean and polluted days. The concentrations of SO₄²⁻, NH₄⁺, NO₃⁻ and organic aerosol were positively related to the concentration of added NO₂. These results provide definitive evidence that NO₂ can promote the conversion of SO₂ to sulfate. At the same time, we found that NO₂ can promote the formation of NH₄⁺ and organic compounds in the aerosols. Our results illustrate that strengthened controls of nitrogen oxides is a key step in reducing the fine particles level in China.

Atmospheric acid deposition is a global environmental issue. China has been experiencing serious acid deposition, which is anticipated to become more severe with the country's economic development and increasing consumption of fossil fuels in recent decades. We explored the spatiotemporal variations of acid deposition (wet acid deposition) and its influencing factors by collecting nationwide data on pH and concentrations of sulfate (SO4²⁻) and nitrate (NO3⁻) in precipitation between 1980 and 2014 in China. Our results showed that average precipitation pH values were 4.59 and 4.70 in the 1990s and 2010s, respectively, suggesting that precipitation acid deposition in China has not seriously worsened. Average SO4²⁻ deposition declined from 40.54 to 34.87 kg S ha⁻¹ yr⁻¹ but average NO3⁻ deposition increased from 4.44 to 7.73 kg N ha⁻¹ yr⁻¹. Specifically, the area of severe precipitation acid deposition in southern China has shrunk to some extent as a result of controlling the pollutant emissions; but the area of moderate precipitation acid deposition has expanded in northern China, associated with rapid industrial and transportation development. Furthermore, we found significant positive correlations between precipitation acid deposition, energy consumption, and rainfall. Our findings provide a relatively comprehensive evaluation of the spatiotemporal dynamics of precipitation acid deposition in China over past three decades, and confirm the idea that strategies implemented to save energy and control pollutant emissions in China have been effective in alleviating precipitation acid deposition. These findings might be used to demonstrate how developing countries could achieve economic development and environmental protection through the implementation of advanced technologies to reduce pollutant emissions.

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.

In this study, we demonstrate that regression analysis of trajectories residence time estimates the contributions of geographical sectors to fine and coarse particle mass in urban receptor sites. We applied the methodology to coarse and fine particles in Amsterdam, Athens, Birmingham and Helsinki. The sectors with the highest contributions on PM2.5 and PM10–2.5 for Amsterdam and Birmingham were Central/Eastern Europe and the Atlantic Ocean/North Sea, respectively. For Athens, the four sectors within 500 km accounted for the largest fraction of PM2.5. The Mediterranean Sea and North Africa added more than half of PM10–2.5 in Athens. For Helsinki, more than 50% of PM2.5 and PM10–2.5 were from sources outside Finland. This approach may be applied to assess the impact of transport on particle mass levels, identify the spatial patterns of particle sources and generate valuable data to design national and transnational efficient emission control strategies.

The high frequency of acid rain in southern China has captured public and official concern since 1980s. Subsequently, gas emission reduction measures have been implemented to improve the air quality. Variations in SO₂ emission intensities can influence the sulfur and oxygen isotopic compositions of sulfate in rainwater, since atmospheric sulfate is mainly formed via the oxidation of sulfur gases from natural and anthropogenic sources. To evaluate the impacts of emission reduction measures on atmospheric sulfate, the seasonal and long-term trends in stable isotopic compositions of sulfate in rainwater in Guizhou province, southwestern China have been investigated based on rainwater samples collected from June 2016 to June 2018 and literature investigation (2000–2010).The results reveal that coal combustion remains a major contributor to sulfate in rainwater, although its SO₂ emission has significantly decreased over the past two decades. The δ³⁴Sₛᵤₗfₐₜₑ and δ¹⁸Oₛᵤₗfₐₜₑ values in rainwater are negatively correlated and have significant seasonal changes. The seasonality in δ³⁴Sₛᵤₗfₐₜₑ has been interpreted as due to the changes in contributions of dimethyl sulfide and coal combustion, while the seasonal pattern of δ¹⁸Oₛᵤₗfₐₜₑ is consistent with that of δ¹⁸Owₐₜₑᵣ values, indicating sulfate in rainwater is mainly formed by heterogeneous oxidation of SO₂. Combined with the data from previous studies (Xiao and Liu, 2002; Liu, 2007; Xiao et al., 2009; Xiao et al., 2014), we found that the volume weighted mean δ³⁴S values of sulfate in rainwater in Guizhou province show a marked increase between 2001 and 2018, indicating that the ³⁴S-depleted SO₂ emission from coal combustion has declined during this period. Furthermore, the synchronous changes in δ³⁴S values, sulfate concentration and pH values of rainwater suggest that the frequency of acid rain in Guizhou province has dropped over the past two decades, which is likely to result from the emission reduction measures taken in Guizhou province.