Arctic tundra soils store a globally significant amount of mercury (Hg), which could be transformed to the neurotoxic methylmercury (MeHg) upon warming and thus poses serious threats to the Arctic ecosystem. However, our knowledge of the biogeochemical drivers of MeHg production is limited in these soils. Using substrate addition (acetate and sulfate) and selective microbial inhibition approaches, we investigated the geochemical drivers and dominant microbial methylators in 60-day microcosm incubations with two tundra soils: a circumneutral fen soil and an acidic bog soil, collected near Nome, Alaska, United States. Results showed that increasing acetate concentration had negligible influences on MeHg production in both soils. However, inhibition of sulfate-reducing bacteria (SRB) completely stalled MeHg production in the fen soil in the first 15 days, whereas addition of sulfate in the low-sulfate bog soil increased MeHg production by 5-fold, suggesting prominent roles of SRB in Hg(II) methylation. Without the addition of sulfate in the bog soil or when sulfate was depleted in the fen soil (after 15 days), both SRB and methanogens contributed to MeHg production. Analysis of microbial community composition confirmed the presence of several phyla known to harbor microorganisms associated with Hg(II) methylation in the soils. The observations suggest that SRB and methanogens were mainly responsible for Hg(II) methylation in these tundra soils, although their relative contributions depended on the availability of sulfate and possibly syntrophic metabolisms between SRB and methanogens.

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.

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.

Se laden freshwater algae that enter the Salton Sea with river water pose ecorisks to wildlife in the lake by transferring selenium (Se) to higher trophic levels. The aim of this study was to investigate impacts of Se on Microcystis aeruginosa, widely distributed in freshwater bodies, and its relationship with toxicity, such as microcystins and Se residues. When supplied with selenite, the 96 h-IC50 was calculated 2.60 mg Se/L. However, these inhibitory effects did not extend to microcystin production, and the extracellular fraction significantly increased with selenite as well as sulfate. As M. aeruginosa assimilated selenite very efficiently, 97% of the removed Se was through accumulation, compared to 3% via volatilization, raising a concern about ecotoxicity caused by the remaining Se in the algae. The XAS analysis suggests the dominant Se species accumulated in the algal cells was elemental Se (81%), which is relatively nonbioavailable to aquatic organisms. We further investigated the potential fate of Se carried into the Salton Sea by M. aeruginosa with river water. Under hypersalinity stress, the biomass Se and intracellular microcystins were released and reduced by 47% and 74%, respectively, resulting in the increasing levels of Se and microcystins in the water column. CuSO4 was then applied as an algaecide to prevent M. aeruginosa from entering the lake. The results indicate a similar response to that under hypersalinity stress: the volatilization process was blocked and the Se and microcystins were released from the damaged algal cells in the presence of CuSO4, further raising toxicity levels by 8% and 60%, respectively, in the water column within 24 h. Overall, the coexistence of selenite and M. aeruginosa in river waters might negatively impact aquatic ecosystems of the Salton Sea and further research is required on how to harvest Se from M. aeruginosa to protect local wildlife.

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 Clean Air Action implemented by the Chinese government in 2013 has greatly improved air quality in the North China Plain (NCP). In this work, we report changes in the chemical components of atmospheric fine particulate matter (PM₂.₅) at four NCP sampling sites from 2012/2013 to 2017 to investigate the impacts and drivers of the Clean Air Action on aerosol chemistry, especially for secondary inorganic aerosols (SIA). During the observation period, the concentrations of PM₂.₅ and its chemical components (especially SIA, organic carbon (OC), and elemental carbon (EC)) and the frequency of polluted days (daily PM₂.₅ concentration ≥ 75 μg m⁻³) in the NCP, declined significantly at all four sites. Asynchronized reduction in SIA components (large decreases in SO₄²⁻ with stable or even increased NO₃⁻ and NH₄⁺) was observed in urban Beijing, revealing a shift of the primary form of SIA, which suggested the fractions of NO₃⁻ increased more rapidly than SO₄²⁻ during PM₂.₅ pollution episodes, especially in 2016 and 2017. In addition, unexpected increases in the sulfur oxidation ratio (SOR) and the nitrogen oxidation ratio (NOR) were observed among sites and across years in the substantially decreased PM₂.₅ levels. They were largely determined by secondary aerosol precursors (i.e. decreased SO₂ and NO₂), photochemical oxidants (e.g. increased O₃), temperature, and relative humidity via gas-phase and heterogeneous reactions. Our results not only highlight the effectiveness of the Action Plan for improving air quality in the NCP, but also suggest an increasing importance of SIA in determining PM₂.₅ concentration and composition.

Previous studies have linked ambient PM₂.₅ to decreased pulmonary function, but the influence of specific chemical elements and emission sources on the severe asthmatic is not well understood. We examined the mass, chemical constituents, and sources of PM₂.₅ for short-term associations with the pulmonary function of adults with severe asthma in a low air pollution environment in urban Nagasaki, Japan. We recruited 35 asthmatic adults and obtained the daily record of morning peak expiratory flow (PEF) in spring 2014–2016. PM₂.₅ filters were extracted from an air quality monitoring station (178 days) and measured for 27 chemical elements. Source apportionment was performed using Positive Matrix Factorization (PMF). We fitted generalized linear model with generalized estimating equation (GEE) method to estimate changes in PEF (from personal monthly maximum) and odds of severe respiratory deterioration (first ≥ 15% PEF reduction within a 1-week interval) associated with mass, constituents, and sources of PM₂.₅, with adjustment for temperature and relative humidity. Constituent sulfate (SO₄²⁻) and PM₂.₅ from oil combustion and traffic were associated with reduced PEF. An interquartile range (IQR) increase in SO₄²⁻ (3.7 μg/m³, average lags 0–1) was associated with a decrease of 0.38% (95% confidence interval = −0.75% to −0.001%). An IQR increase in oil combustion and traffic-sourced PM₂.₅ (2.64 μg/m³, lag 1) was associated with a decrease of 0.33% (−0.62% to −0.002%). We found a larger PEF decrease associated with PM₂.₅ from dust/soil on Asian Dust days. There was no evidence linking total mass and metals to reduced pulmonary function. The ventilatory capacity of adults with severe asthma is susceptible to specific constituents/sources of PM₂.₅ such as sulfate and oil combustion and traffic despite active self-management of asthma and low air pollution levels in the study location.

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.