As the most important gas-phase alkaline species, atmospheric ammonia (NH3) contributes considerably to the formation and development of fine-mode particles (PM2.5), which affect air quality and environmental health. Recent satellite-based observations suggest that the North China Plain is the largest agricultural NH3 emission source in China. However, our isotopic approach shows that the surface NH3 in the intraregional urban environment of Beijing-Tianjin-Shijiazhuang is contributed primarily by combustion-related processes (i.e., coal combustion, NH3 slip, and vehicle exhaust). Specifically, the Batch fractionation model was used to describe the partitioning of gaseous NH3 into particles and to trace the near-ground atmospheric NH3 sources. With the development of haze pollution, the dynamics of δ15N-NH4+ were generally consistent with the fractionation model. The simulated initial δ15N-NH3 values ranged from −22.6‰ to −2.1‰, suggesting the dominance of combustion-related sources for urban NH3. These emission sources contributed significantly (92% on hazy days and 67% on clean days) to the total ambient NH3 in urban cities, as indicated by a Bayesian mixing model. Based on the Batch fractionation model, we concluded the following: 1) δ15N-NH4+ can be used to model the evolution of fine-mode aerosols and 2) combustion-related sources dominate the near-ground atmospheric NH3 in urban cities. These findings highlight the need for regulatory controls on gaseous NH3 emissions transported from local and surrounding industrial sources.

Ozone has become a major atmospheric pollutant in China as the pattern of urban energy usage has changed and the number of motor vehicles has grown rapidly. The Beijing-Tianjin-Hebei Urban Agglomeration, also known as the Jing-Jin-Ji Urban Agglomeration (hereafter, JJJUA), with a precarious balance between protecting the ecological environment and sustaining economic development, is challenged by high levels of ozone pollution. Based on ozone observation data from 13 cities in the JJJUA from 2014 to 2017, the spatio-temporal trends in the evolution of ozone pollution and its associated influencing factors were analyzed using Moran’s I Index, hot-spot analysis, and Geodetector using ArcGIS and SPSS software. Five key results were obtained. 1) There was an increase in the annual average ozone concentration, for the period 2014–2017. Comparing the 13 prefecture-level cities, ozone pollution in Chengde and Hengshui decreased, while it worsened in the remaining 11 cities. 2) Ozone pollution was worse in spring and summer than in autumn and winter; the peak ozone pollution season was from May to September; the average ozone concentration on workdays was higher than that on non-workdays, showing a counter-weekend effect. 3) Annual average concentrations were high in the central and southern parts of the study region but low in the north. 4) Prominent positive spatial correlations were observed in ozone concentration, with the best correlations shown in summer and autumn; concentrations were high in Baoding and Xingtai but low in Beijing and Chengde. 5) Concentrations of PM10, NO2, CO, SO2, and PM2.5, as well as average wind speed, sunshine duration, evaporation, precipitation, and temperature, all had significant effects on ozone pollution, and interactions between these influencing factors increased it.

The occurrence of legacy and novel per- and polyfluoroalkyl substances (PFASs) in multiple matrices from a farmland environment was investigated in the Beijing-Tianjin-Hebei core area of northern China. PFASs were ubiquitously detected in farmland soils, and the detection frequency of 6:2 chlorinated polyfluoroalkyl ether sulfonic acid (6:2 Cl-PFESA) was higher than that of perfluorooctane sulfonic acid (98% vs. 83%). Long-chain PFASs, including 6:2 Cl-PFESA, showed a centered distribution pattern around the metropolis of Tianjin, probably due to the local intensive industrial activity, while trifluoroacetic acid (TFA) showed a decreasing trend from the coast to the inland area. Other than soil, TFA was also found at higher levels than other longer-chain PFASs in dust, maize (Zea mays), poplar (Populus alba) leaf and locust (Locusta migratoria manilens) samples. Both poplar leaves and locusts can be used as promising biomonitoring targets for PFASs in farmland environments, and their accumulation potential corresponds with protein and lipid contents. Apart from being exposed to PFASs via food intake, locusts were likely exposed via uptake from soil and precipitated dust in farmland environments. The biomonitoring of locusts may be more relevant to insectivores, which is important to conducting a comprehensive ecological risk assessment of farmland environments.

Both surface and satellite observations have shown a decrease in NOₓ emissions in East Asian countries in recent years. In order to reflect the recent NOx emission reduction and to investigate its impact on surface O₃ concentrations in Asian megacities, we adjusted two bottom-up regional emission inventories of which base years are 2006 (E2006) and 2010 (E2010), respectively. We applied direct and relative emission adjustments to both E2006 and E2010 to constrain NOx emissions using OMI NO₂ vertical column densities. Except for the relative emission adjustment with E2006, modeling results with adjusted emissions exhibit that NOx emissions over East Asian megacities (Beijing, Shanghai, Seoul, and Tokyo) in the bottom-up inventories are generally overestimated. When the direct emission adjustment is applied to E2006, model biases in the Seoul Metropolitan Area (SMA), South Korea are reduced from 24 ppb to 2 ppb for NOx (=NO+NO₂) and from −9 ppb to 0 ppb for O₃. In addition, NO₂ model biases in Beijing and Shanghai in China are reduced from 8 ppb to 18 ppb–0 ppb and 1 ppb, respectively. Daily maximum 8-h average O₃ model biases over the same places are decreased by 8 ppb and 14 ppb. Further analyses suggest that the reduction in domestic South Korean NOₓ emissions plays a significant role in increasing O₃ concentrations in SMA. We conclude that the current strong drive to reduce NOₓ emissions as part of the strategy to lower particulate matter concentrations in South Korea can account for increased O₃ concentrations in recent years and suggest that more aggressive NOₓ emissions will be necessary soon.

Eutrophic freshwater lake ecosystems are receiving increasing public attention due to a global increase in large-scale harmful cyanobacterial blooms in surface waters. However, the contribution of phytodetritus accumulation in benthic sediments post-bloom remains unclear. In this study, field investigations were performed using microsensors to evaluate benthic phytodetritus mats by measuring TOC/TN ratios, pigments, biodegradable compounds and odorants as descriptive parameters. Results show that the massive amount of phytodetritus trapped by aquatic plants gradually evolved into benthic cyanobacterial detritus mats, which were characterized as anoxic, reductive and low pH. It was confirmed that the occurrence of odorants is more serious in the detritus mats due to decay and decomposition of the accumulated phytodetritus. The mean odorant content in the vegetated zones was 3–52 times higher than that in the unvegetated zones. The dominant odorants were dimethyl trisulfide (DMTS), β-ionone and β-cyclocitral, with mean contents of 52.38 ng·(g·dw)-1, 162.20 ng·(g·dw)-1 and 307.51 ng·(g·dw)-1, respectively, in the sediment. In addition, odorant production appears to be associated with the distribution of biodegradable compounds in the sediment. This is supported by the marked correlation observed between biodegradable compounds and odorants. Multiple regression analysis showed that biodegradable compounds can be used as indicators to predict odorant content in the sediment. It is noteworthy that the odorant trend in the water column and sediment is symmetrical, indicating a risk of diffusion from the sediment to the water column. This study helps to clarifying the contributions of benthic cyanobacterial detritus mats to odorant production in shallow eutrophic lakes. The information provided herein may also be useful for future management of aquatic ecosystems.

Polybrominated diphenyl ethers (PBDEs) serve as flame retardants in many household materials such as electrical and electronic devices, furniture, textiles, plastics, and baby products. Though the use of PBDEs like penta-, octa- and deca-BDE greatly reduces the fire damage, indoor pollution by these toxic emissions is ever-growing. In fact, a boom in the global market projections of PBDEs threatens human health security. Therefore, efforts are made to minimize PBDEs pollution in USA and Europe by encouraging voluntary phasing out of the production or imposing compelled regulations through Stockholm Convention, but >500 kilotons of PBDEs still exist globally. Both ‘environmental persistence’ and ‘bioaccumulation tendencies’ are the hallmarks of PBDE toxicities; however, both these issues concerning household emissions of PBDEs have been least addressed theoretically or practically. Critical physiological functions, lipophilicity and toxicity, trophic transfer and tissue specificities are of utmost importance in the benefit/risk assessments of PBDEs. Since indoor debromination of deca-BDE often yields many products, a better understanding on their sorption propensity, environmental fate and human toxicities is critical in taking rigorous measures on the ever-growing global deca-BDE market. The data available in the literature on human toxicities of PBDEs have been validated following meta-analysis. In this direction, the intent of the present review was to provide a critical evaluation of the key aspects like compositional patterns/isomer ratios of PBDEs implicated in bioaccumulation, indoor PBDE emissions versus human exposure, secured technologies to deal with the toxic emissions, and human toxicity of PBDEs in relation to the number of bromine atoms. Finally, an emphasis has been made on the knowledge gaps and future research directions related to endurable flame retardants which could fit well into the benefit/risk strategy.

A major health scandal involving DEHP-tainted (di-2-ethylhexyl phthalate) foodstuffs occurred in Taiwan in 2011. We investigated temporal relationships between urinary DEHP metabolites and biomarkers of oxidative stress in two cohorts of potentially affected children during that food scandal. One cohort was collected from Kaohsiung Medical University Hospital in southern Taiwan between May and June of 2011 (the KMUH cohort). This cohort was followed up at 2, 6, and 44 months. The other cohort was collected from a nationwide health survey conducted by Taiwan’s National Health Research Institutes (the NHRI cohort) for potentially affected people between August 2012 and January 2013. Both cohorts only included children 10 years old and younger who had provided enough urine for analysis of urinary DEHP oxidative metabolites and two markers of oxidative stress: 8-oxo-2′-deoxyguanosine (8-OHdG) and malondialdehyde (MDA). The KMUH cohort had a simultaneous and significant decrease in urinary DEHP metabolites, 8-OHdG, and MDA, with the lowest concentrations found at the 6-month follow up and maintained until the 44-month follow up, consistent with those from NHRI cohort at ∼15–18 months post-scandal (p > 0.05). There were decreases in both DEHP metabolites and oxidative stress markers across the populations, but no association was observed between DEHP metabolites and oxidative stress markers in individuals in the two cohorts. Continued follow-up is needed to determine long-term health consequences in these children.

Selenium (Se) is an essential micronutrient for animals with a narrow margin between essentiality and toxicity. Se toxicity is largely related to inorganic forms of Se in soil, i.e., selenite and selenate that enter food chains through plant uptake, threatening higher trophic level organisms. This experiment investigated effects of earthworm activity on Se bioavailability in soil and the subsequent plant uptake, using earthworm Eisenia fetida and bean plant Phaseolus vulgaris L, both exposed to either selenite or selenate at 1 or 4 mg Se kg⁻¹ for 16 weeks. Plants took up selenate (up to 221-fold) faster than selenite, with up to 84% of the Se rapidly transported to shoots. In the presence of earthworms, Se accumulation obviously increased for selenate-supplied plants, leading to an up to 4% increase in Se translocation factor for all treatments except for 1 mg kg⁻¹ selenite treatment. Earthworms also concentrated Se faster in tissues (up to 274 mg kg⁻¹ DW) at exposure to selenate. For Se toxicity, Se speciation analysis was conducted on the plants and earthworms using XAS. Compared to worm-free treatments, the percentage of organo-Se, i.e., SeMet and CysSeSeCys, increased in beans (up to 34%) in the presence of earthworms for selenate, while the elemental Se portion was significantly reduced or absent, opposite to the results for selenite. Surprisingly, elemental Se (up to 65%) dominated earthworms, regardless of the form of Se supplied. In conclusion, earthworms clearly enhanced Se uptake and translocation in plants, leading to elevated Se levels in shoots. To prevent resulting hazards to humans and other animals, caution should be taken while consuming the shoots, particularly beans, harvested from the Se contaminated soil where earthworm activity is high. Finally, the significant reduction in soil Se suggests phytoextraction of Se from the soil could be improved using earthworms as an aid to plants.

Sulfitobacter porphyrae ZFX1, isolated from surface seawater of the East China Sea during a Prorocentrum donghaiense bloom recession, exhibits high algicidal activity against P. donghaiense. To evaluate the algicidal effect of ZFX1, the algicidal mode and stability were investigated. The results showed that ZFX1 indirectly attacked algae by secreting algicidal compounds, and the algicidal activity of the ZFX1 supernatant was insensitive to different temperatures, light intensities and pH values (pH 3–12). To explore the algicidal mechanism of the ZFX1 supernatant, its effects on the morphological and ultrastructural alterations, photosynthetic capacity, reactive oxygen species (ROS) and antioxidative system of P. donghaiense were investigated. Scanning and transmission electron microscopy revealed that the ZFX1 supernatant destroyed the algal cell membrane structure and caused intracellular leakage. The decrease in the chlorophyll a content and the marked declines in both the photosynthetic efficiency (Fv/Fm) and the electron transport rate (rETR) indicated that the ZFX1 supernatant could damage the photosynthetic system of P. donghaiense. The excessive production of ROS in algal cells demonstrated the oxidative damage triggered by the ZFX1 supernatant. Although the antioxidant defense system of P. donghaiense was activated to scavenge excessive ROS, lipid oxidation occurred. The fatty acid composition profile indicated that the ZFX1 supernatant markedly increased the contents of two saturated fatty acids and a monounsaturated fatty acid and decreased the proportion of two polyunsaturated fatty acids, which resulted in lipids with a lower degree of unsaturation (DU). The decline in the DU decreased the lipid fluidity and rigidified the membrane system, and these effects destroyed the function of the membrane system and ultimately resulted in algal cell death. Therefore, ZFX1 probably plays a key role in mitigating P. donghaiense bloom by inducing lipid oxidation, decreasing the DU of lipids and ultimately destroying the membrane systems of algal cells.

Erhai Lake in the Yunnan-Guizhou Plateau, a typical subtropical deep lake, experienced long-time input of nutrients and pollutants, which provides beneficial conditions for evolution and spread of resistance genes. In this study, the profile of bacterial community, antibiotic and metal resistance genes in sediments of Erhai Lake were analyzed via high-thought sequencing of 16S rRNA and metagenomic DNA. Proteobacteria, Firmicutes, Nitrospirae, and Bacteroidetes were found to be the main composition of the bacterial community. Multidrug-, bacitracin-, macrolide-lincosamide-streptogramin (MLS)- and tetracycline resistance genes were the primary antibiotic resistance gene (ARG) types with high relative abundance, whereas Multi-metal-, and arsenic- resistance genes were the primary metal resistance gene (MRG) types. The effects of nitrogen and phosphorus on the abundance of ARGs and MRGs depended on the different types. Some specific ARG (fosmidomycin resistance genes) and MRG types (multi-metal resistance genes) also showed significant geographic distribution. Bacterial community was the main driver shaping the resistome. Nutrients also played an essential role in structuring the bacterial community and resistome in the sediments of Erhai Lake. This study sheds light on the distribution and fate of resistome under a high load of nitrogen and phosphorus in a deep lake.