Poly- and per-fluoroalkyl substances (PFAS) and volatile methyl siloxanes (VMS) were monitored at 21 sites in the Global Atmospheric Passive Sampling (GAPS) Network. Atmospheric concentrations previously reported from 2009 were compared to concentrations measured at these sites in 2013 and 2015, to assess trends over 7 years of monitoring. Concentrations of the fluorotelomer alcohols (FTOHs) and fluorinated sulfonamides and sulfonamidoethanols (FOSAs and FOSEs) were stable at these sites from 2009 to 2015 with no significant difference (p > 0.05) in concentrations. Elevated concentrations of all the neutral PFAS were detected at the urban sites as compared to the polar/background sites. The perfluorosulfonic acids (PFSAs), meanwhile, saw a significant increase (p < 0.001) in concentrations from 2009 to 2015. The perfluorocarboxylic acids (PFCAs) had elevated concentrations in 2015, however, the difference was not statistically significant (p > 0.05). Concentrations of the PFSAs and the PFCAs were similar at all location types, showing the global reach of these persistent compounds. Concentrations of the cyclic VMS (cVMS) were at least an order of magnitude higher than the linear VMS (lVMS) and the PFAS. Octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5) and dodecamethylcyclohexasiloxane (D6) saw a weak significant increase in concentrations from 2009 to 2013 (p < 0.05), however, hexamethylcyclotrisiloxane (D3) had a strong significant decrease in concentrations from 2009 to 2015 (p < 0.01).

Short chain perfluoroalkyl acids (PFAAs) have been developed since 2002 by the major manufacturers to replace the conventional C8 and higher homologues, with much of the world production shifted to China in recent years. In this study, we conducted a continuous monitoring program over the period 2011–2014 with seasonal monitoring in 2013 for PFAAs emitted from two rapidly developing fluorochemical industry parks located in the Daling River Basin, Northern China. The trend of PFAA contamination was identified, dominated by perfluorobutane sulfonic acid (PFBS), perfluorobutanoic acid (PFBA) and perfluorooctanoic acid (PFOA), with the maximum concentrations of 3.78 μg/L, 3.70 μg/L, and 1.95 μg/L, respectively. Seasonal monitoring uncovered the occasional emission of perfluorooctane sulfonic acid (PFOS). Construction trends of new facilities and associated manufacturing capacity of the main products were also analyzed to assess correlations with PFAA emissions. An assessment of the data over the period 2011–2014 found a positive correlation with fluorocarbon alcohol (FCA) production and emission of PFAAs. Groundwater and tap water around the main source indicated that the dominant PFAAs had different diffusion behaviors. PFBS levels were higher in surface water, while PFBA was dominant in groundwater and tap water, with PFOA levels being higher in downstream groundwater. Considering the continuous expansion and development of fluorochemical industry in the Daling River Basin, this study will provide abundant information on the effectiveness of risk assessment and management.

The aim of this study was to determine how dietary exposure to PFAAs has changed over the period when major production changes occurred. Archived samples (1999–2010) of eggs, milk and farmed rainbow trout were analyzed by ultra performance liquid chromatography coupled to tandem mass spectrometry. Statistically significant decreasing trends were observed for concentrations of perfluorooctane sulfonic acid (PFOS) and perfluorohexane sulfonic acid (PFHxS) in fish (p < 0.002 and p < 0.032, respectively) and eggs (p < 0.001 for both compounds). Concentrations of PFOS in fish and eggs decreased by a factor of 10 and 40, respectively. In eggs there was also a statistically significant decreasing trend in concentrations of perfluorooctanoic acid (PFOA). The results of this study demonstrate that PFAA concentrations in food items from agricultural food chains and aquatic food chains close to sources respond rapidly to changes in environmental emissions. Implications for the overall understanding of human exposure are discussed.

The effect of atmospheric nitrogen deposition on the species richness of acid grasslands was investigated by combining data from a large Danish monitoring program with a large European data set, where a significant non-linear negative effect of nitrogen deposition had been demonstrated (Stevens et al., 2010). The nitrogen deposition range in Denmark is relatively small and when only considering the Danish data a non-significant decrease in the species richness with nitrogen deposition was observed. However, when both data sets were combined, then the conclusion of the European survey was further corroborated by the results of the Danish monitoring. Furthermore, by combining the two data sets a more comprehensive picture of the threats to the biodiversity of acid grasslands emerge; i.e., species richness in remnant patches of acid grassland in intensively cultivated agricultural landscapes is under influence not only from nitrogen deposition, but also from current and historical land use.

This study presents the particle size distribution and respiratory deposition estimates of airborne perfluoroalkyl acids (PFAAs) during the haze period. Size-segregated haze aerosols were collected from an urban location in Shanghai using an eight-stage air sampler. The samples were analyzed for eight PFAAs using ultra-high-performance liquid chromatography tandem triple quadrupole mass spectrometry. The quantification results showed that the concentrations of particle-bound Σ 8PFAAs ranged from 0.26 to 1.90 ng m⁻³ (mean: 1.44 ng m⁻³). All of the measured PFAAs particle size distributions had a bimodal mode that peaked respectively in accumulation size range (0.4 < Dp < 2.1 μm) and coarse size ranges (Dp > 2.1 μm), but the width of each distribution somewhat varied by compound. The emission source, molecular weight, and volatility of the PFAAs were important factors influencing the size distribution of particle-bound PFAAs. Of these compounds, PFUnDA presented a strong accumulation in the fine size range (average 75% associated with particles <2.1 μm), followed by PFOA (69%) and PFDA (64%). The human risk assessment of PFOS via inhalation was addressed and followed the same pattern as the size distribution, with a 2-fold higher risk for the fine particle fraction compared to the coarse particle fraction at urban sites. Approximately 30.3–82.0% of PFAA deposition (∑PFAA: 72.5%) in the alveolar region was associated with particles <2.1 μm, although the contribution of fine particles to the total PFAAs concentration in urban air was only 28–57% (∑8PFAAs: 48%). These results suggested that fine particles are significant contributors to the deposition of PFAAs in the alveolar region of the lung.

Strong acid rain was recently observed over Northeastern China, particularly in summer in Liaoning Province where alkaline dust largely neutralized acids in the past. This seems to be related to the regional transboundary pollution and poses new challenges in acid rain control scheme in China. In order to delve into the regional transport impact, and quantify its potential contributions to such an “eruption” of acid rain over Liaoning, this paper employs an online source tagging model in coupling with the Nested Air Quality Prediction Modeling System (NAQPMS). Validation of predictions shows the model capability in reproducing key meteorological and chemical features. Acid concentration over Liaoning is more pronounced in August (average of 0.087 mg/m³) with strong pollutant import from regional sources against significant depletion of basic species. Seasonal mean contributions from regional sources are assessed at both lower and upper boundary layers to elucidate the main pathways of the impact of regional sources on acid concentration over Liaoning. At the upper layer (1.2 km), regional sources contribute to acid concentration over Liaoning by 67%, mainly from Shandong (16%), Hebei (13%), Tianjin (11%) and Korean Peninsula (9%). Identified main city-receptors in Liaoning are Dandong, Dalian, Chaohu, Yingkou, Liaoyang, Jinfu, Shengyang, Panjin, Tieling, Benxi, Anshan and Fushun. At lower layer (120 m) where Liaoning local contribution is dominant (58%), regional sources account for 39% in acid concentration. However, inter-municipal acid exchanges are prominent at this layer and many cities in Liaoning are revealed as important sources of local acid production. Seasonal acid contribution average within 1.2 km-120 m attains 55%, suggesting dominance of vertical pollutant transport from regional sources towards lower boundary layer in Liaoning. As direct environmental implication, this study provides policy makers with a perspective of regulating the regional transboundary environmental impact assessment in China with application to acid rain control.

To elucidate the sorption affinity of biochars for neonicotinoid pesticides and the influence of biochar structure on sorption mechanisms therein, 24 biochar samples were obtained by pyrolyzing maize straw and pig manure at pyrolyzing temperatures (PTs) of 200–700 °C and by further deashing them using acids, and the sorption of three typical neonicotinoids, imidacloprid, clothianidin and thiacloprid on untreated and acid-deashed biochars were evaluated. All the biochar samples could efficiently adsorb the three neonicotinoids and multiple mechanisms were involved in sorption. With the increasing PTs, hydrophobic partition sorption increased, but had a declined contribution to the total sorption as revealed by a dual-mode model. Besides hydrophobic partition, specific interactions like cation-π electron donor acceptor (EDA) interactions (only for protonated IMI and CLO) and hydrogen bond and contributed much to the sorption on low-PT (≤500 °C) biochars, while the sorption on those high-PT (>500 °C) biochars mainly depended on pore-filling strengthened by cation-π and p/π-π EDA interactions. Thiacloprid showed stronger sorption on untreated biochars compared to imidacloprid and clothianidin, due to its greater ability to form hydrogen bond and hydrophobic interactions. Acid-deashing treatments increased the relative percentage contents of organic carbon, bulk O, aromaticity and O-containing functional groups, surface area and pore volume of biochars. The ash can bind neonicotinoids by specific interactions but played a negative role in the whole sorption on high-PT biochars by covering the inner sorption sites of organic moieties and blocking the micropores in biochars. The results acquired in the present study will help us to get deep insight in the comprehensive sorption mechanisms of polar pesticides on biochar and the effects of biochar structure.

The occurrence of 17 target PFAA analytes was determined in surface sediments (n = 37) of the East China Sea and potential influencing factors were examined. ΣPFAAs ranged from 0.41 ng/g dw to 3.06 ng/g dw, with perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) as the most abundant perfluorocarboxylic acid and perfluoroalkyl sulfonate, respectively. PFAAs in the sediments were strongly influenced by terrigenous input. Analysis of the relationship between dynamic influence factors and PFAA concentrations showed that the characteristics of PFAA distribution were rather complex. ΣPFAA concentrations and TOC were positively correlated (p < 0.0001). Circumfluence also influenced the whole PFAA distribution and seasonal variation. In addition, correlation analysis suggested that log Koc values increased with increasing perfluoroalkyl chain length. Given the rapid economic development of eastern coastal cities of China, the environmental hazards of land source pollution cannot be ignored.

Groundwater serves as a main drinking water source for rural residents in China. However, little is known regarding the pollution of organic micropollutants in groundwater that may pose health risks. In this study, more than 1300 organic micropollutants were screened in the groundwater samples collected from 13 drinking water wells distributed across five rural regions of Liaodong Peninsula in China. A total of 80 organic micropollutants including 12 polycyclic aromatic hydrocarbons, 11 alkanes, 9 pesticides, 7 substituted phenols, 7 perfluoroalkyl acids, 6 heterocyclic compounds, 5 alcohols, 5 phthalic acid esters, 5 pharmaceutical and personal care products, 3 ketones, 2 polychlorinated biphenyls (PCBs), 2 alkylbenzenes and 2 chlorinated benzenes were detected, with their total concentration of 32–1.5 × 104 ng/L. Noncarcinogenic and carcinogenic risks of a part of pollutants were assessed. Exposure through skin absorption and oral ingestion was considered in the assessment. Generally the risks are within the acceptable limits, except for that the carcinogenic risk at two sites in Jinzhou is higher than 10−6. To the best of our knowledge, this is the first report on health risks of groundwater micropollutants in China.

Concentrations (including isomer patterns) and temporal changes (1997–2012) of perfluoroalkyl acids (PFAAs) and selected perfluorooctane sulfonate (PFOS) and perfluoroalkyl carboxylic acid (PFCA) precursors were determined in serum samples from Swedish women. Perfluorooctane sulfonamide (FOSA) and perfluorooctane sulfonamidoacetic acid (FOSAA), as well as its N-methyl and N-ethyl derivatives (MeFOSAA and EtFOSAA) were consistently detected. Highest PFOS precursor concentrations were found for EtFOSAA (before year 2000) or MeFOSAA and FOSAA (after 2000). Disappearance half-lives for all PFOS precursors were shorter compared to PFOS. 4:2/6:2 and 6:2/6:2 polyfluoroalkyl phosphate diesters (diPAPs) were detected in <60% of the samples, whereas 6:2/8:2 and 8:2/8:2 diPAPs were detected in >60% of the samples, but showed no significant change in concentrations over time. Linear and sum-branched isomers were quantified separately for three PFAAs and three precursors. Significant changes between 1997 and 2012 in the % linear isomer were observed for PFOA and FOSA (increase) and PFOS (decrease).