The potential hazards of acrylamide (AA) have been proposed due to its lifelong exposure. However, the association between AA exposure and mortality remains unclear.We evaluated the prospective association of AA hemoglobin adducts (HbAA and HbGA) with all-cause and cardiovascular disease (CVD) mortality in U.S. population from National Health and Nutrition Examination Survey (NHANES) 2003–2006.We followed 5504 participants who were ≥25 years of age for an average of 6.7 years at the baseline examination with annual linkage to the NHANES statistics database. Using AA hemoglobin biomarkers [HbAA, HbGA, sum of HbAA and HbGA (HbAA + HbGA), and ratio of HbGA to HbAA (HbGA/HbAA)], we determined mortality from all-causes and CVD through Cox proportional hazard regression analysis with multivariable adjustments both in non-smoker group and smoker group. In addition, subgroup analyses and sensitivity analyses were further conducted.After adjusting for sociodemographic, life behavioral and cardiovascular risk factors in non-smoker group, HbAA was positively associated with all-cause mortality (p for trend = 0.0197) and non-CVD mortality (p for trend = 0.0124). HbGA and HbGA/HbAA were inversely associated with all-cause mortality (p for trend = 0.0117 and 0.0098, respectively) and CVD mortality (p for trend=0.0009 and 0.0036, respectively). The multivariable adjusted hazard ratios (HRs) [95% confidence intervals (CIs)] of the upper three quartiles were 0.472 (95% CI: 0.283–0.786), 0.517 (95% CI: 0.299–0.894) and 0.470 (95% CI: 0.288–0.766) between HbGA/HbAA and all-cause mortality comparing with the lowest quartile, respectively. No significant associations were found between HbAA + HbGA and mortality in non-smoker group, and between all AA hemoglobin biomarkers and mortality in smoker group.Hemoglobin biomarker levels of AA were strongly associated with mortality in general U.S. non-smoker adults. These findings proposed a continuous public health concern in relation to environmental and dietary exposure to AA.

Lijiang is a high-altitude city located on the eastern fringe of the Tibetan Plateau, with complex seasonal atmospheric circulations (i.e. westerly wind, Indian Monsoon, and East Asia Monsoon). Very few previous studies have focused on seasonal variations and sources of organic pollutants in Lijiang. In this study, a four-year air campaign from June 2009 to July 2013 was conducted to investigate the temporal trends and the sources of polycyclic aromatic hydrocarbons (PAHs) and organochlorine compounds [including organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs)]. The atmospheric PAH concentrations in winter are 2–3 times of those in summer, probably because of the combined result of enhanced local emission and long-range atmospheric transport (LRAT) during winter. Traffic pollution was the primary local source of PAHs, while biomass burning is the dominant LRAT source. OCPs and PCBs also mainly underwent LRAT to reach Lijiang. The peak concentrations of most of OCPs occurred in pre-monsoon season and winter, which were carried by air masses from Myanmar and India through westerly winds. As compared with other sites of the Tibetan Plateau, without the direct barrier of the Himalaya, Lijiang is easily contaminated by the incursion of polluted air masses.

The emission factors (EFs) of polycyclic aromatic hydrocarbons (PAHs) in PM2.5 were measured from commonly used stoves and fuels in the rural Guanzhong Plain, China. The toxicity of the PM2.5 also was measured using in vitro cellular tests. EFs of PAHs varied from 0.18 mg kg−1 (maize straw charcoal burning in a clean stove) to 83.3 mg kg−1 (maize straw burning in Heated Kang). The two largest influencing factors on PAH EFs were air supply and volatile matter proportion in fuel. Improvements in these two factors could decrease not only EFs of PAHs but also the proportion of 3-ring to 5-ring PAHs. Exposure to PM2.5 extracts caused a concentration-dependent decline in cell viability but an increase in reactive oxygen species (ROS), tumor necrosis factor a (TNF-α) and interleukin 6 (IL-6). PM2.5 emitted from maize burning in Heated Kang showed the highest cytotoxicity, and EFs of ROS and inflammatory factors were the highest as well. In comparison, maize straw charcoal burning in a clean stove showed the lowest cytotoxicity, which indicated a clean stove and fuel treatment were both efficient methods for reducing cytotoxicity of primary PM2.5. The production of these bioreactive factors were highly correlated with 3-ring and 4-ring PAHs. Specifically, pyrene, anthracene and benzo(a)anthracene had the highest correlations with ROS production (R = 0.85, 0.81 and 0.80, respectively). This study shows that all tested stoves emitted PM2.5 that was cytotoxic to human cells; thus, there may be no safe levels of exposure to PM2.5 emissions from cooking and heating stoves using solid fuels. The study may also provide a new approach for evaluating the cytotoxicity of primary emitted PM2.5 from solid fuel burning as well as other PM2.5 sources.

Effects of photochemical and microbial degradation on variations in composition and molecular-size of dissolved organic matter (DOM) from different sources (algal and soil) and the subsequent influence on Cu(II) binding were investigated using UV–Vis, fluorescence excitation-emission matrices coupled with parallel factor analysis, flow field-flow fractionation (FlFFF), and metal titration. The degradation processes resulted in an initial rapid decline in the bulk dissolved organic carbon and chromophoric and fluorescent DOM components, followed by a small or little decrease. Specifically, photochemical reaction decreased the aromaticity, humification and apparent molecular weights of all DOM samples, whereas a reverse trend was observed during microbial degradation. The FlFFF fractograms revealed that coagulation of both protein- and humic-like DOM induced an increase in molecular weights for algal-DOM, while the molecular weight enhancement for allochthonous soil samples was mainly attributed to the self-assembly of humic-like components. The Cu(II) binding capacity of algal-derived humic-like and fulvic-like DOM consistently increased during photo- and bio-degradation, while the soil-derived DOM exhibited a slight decline in Cu(II) binding capacity during photo-degradation but a substantial increase during microbial degradation, indicating source- and degradation-dependent metal binding heterogeneities. Pearson correlation analysis demonstrated that the Cu(II) binding potential was mostly related with aromaticity and molecular size for allochthonous soil-derived DOM, but was regulated by both DOM properties and specific degradation processes for autochthonous algal-derived DOM. This study highlighted the coupling role of inherent DOM properties and external environmental processes in regulating metal binding, and provided new insights into metal-DOM interactions and the behavior and fate of DOM-bound metals in aquatic environments.

This study uses spatiotemporal patterns in ambient concentrations to infer the contribution of regional versus local sources. We collected 12 months of monitoring data for outdoor fine particulate matter (PM₂.₅) in rural southern India. Rural India includes more than one-tenth of the global population and annually accounts for around half a million air pollution deaths, yet little is known about the relative contribution of local sources to outdoor air pollution. We measured 1-min averaged outdoor PM₂.₅ concentrations during June 2015–May 2016 in three villages, which varied in population size, socioeconomic status, and type and usage of domestic fuel. The daily geometric-mean PM₂.₅ concentration was ∼30 μg m⁻³ (geometric standard deviation: ∼1.5). Concentrations exceeded the Indian National Ambient Air Quality standards (60 μg m⁻³) during 2–5% of observation days. Average concentrations were ∼25 μg m⁻³ higher during winter than during monsoon and ∼8 μg m⁻³ higher during morning hours than the diurnal average. A moving average subtraction method based on 1-min average PM₂.₅ concentrations indicated that local contributions (e.g., nearby biomass combustion, brick kilns) were greater in the most populated village, and that overall the majority of ambient PM₂.₅ in our study was regional, implying that local air pollution control strategies alone may have limited influence on local ambient concentrations. We compared the relatively new moving average subtraction method against a more established approach. Both methods broadly agree on the relative contribution of local sources across the three sites. The moving average subtraction method has broad applicability across locations.

Despite not being used for decades in most countries, DDT remains ubiquitous in soils due to its persistence and intense past usage. Because of this it is still a pollutant of high global concern. Assessing long term dissipation of DDT from this reservoir is fundamental to understand future environmental and human exposure. Despite a large research effort, key properties controlling fate in soil (in particular, the degradation half-life (τₛₒᵢₗ)) are far from being fully quantified. This paper describes a case study in a large central European catchment where hundreds of measurements of p,p’-DDT concentrations in air, soil, river water and sediment are available for the last two decades. The goal was to deliver an integrated estimation of τₛₒᵢₗ by constraining a state-of-the-art hydrobiogeochemical-multimedia fate model of the catchment against the full body of empirical data available for this area. The INCA-Contaminants model was used for this scope. Good predictive performance against an (external) dataset of water and sediment concentrations was achieved with partitioning properties taken from the literature and τₛₒᵢₗ estimates obtained from forcing the model against empirical historical data of p,p’-DDT in the catchment multicompartments. This approach allowed estimation of p,p’-DDT degradation in soil after taking adequate consideration of losses due to runoff and volatilization. Estimated τₛₒᵢₗ ranged over 3000–3800 days. Degradation was the most important loss process, accounting on a yearly basis for more than 90% of the total dissipation. The total dissipation flux from the catchment soils was one order of magnitude higher than the total current atmospheric input estimated from atmospheric concentrations, suggesting that the bulk of p,p’-DDT currently being remobilized or lost is essentially that accumulated over two decades ago.

Polybrominated diphenyl ethers (PBDEs) undergo debromination when they were exposed in zerovalent metal or bimetallic systems. Yet their debromination pathways and mechanisms in these systems were not well understood. Here we reported the debromination pathways of three BDE congeners (BDE-21, 25 and 29) by nano-zerovalent iron (n-ZVI). All these BDE congeners have three bromine substituents that were located in ortho-, meta- and para-positions. Results demonstrated that BDE-21, 25 and 29 preferentially debrominate meta-, ortho- and para-bromines, respectively, suggesting that bromine substituent at each position (i.e. ortho-, meta- or para-) of PBDEs can be preferentially removed. Singly occupied molecular orbitals of BDE anions are well correlated with their actual debromination pathways, which successfully explain why these BDE congeners exhibit certain debromination pathways in n-ZVI system. In addition, microscale zerovalent zinc (m-ZVZ), iron-based bimetals (Fe/Ag and Fe/Pd) were also used to debrominate PBDEs, with BDE-21 as target pollutant. We found that the debromination pathways of BDE-21 in m-ZVZ and Fe/Ag systems are the same to those in n-ZVI system, but were partially different from those in Fe/Pd systems. The debromination of BDE-21 in Pd-H2 system as well as the solvent kinetic isotope effect in single metal and bimetallic systems suggests that H atom transfer is the dominant mechanism in Fe/Pd system, while e-transfer is still the dominant mechanism in Fe/Ag system.

The parameter AOX (adsorbable organic halogens) indicates the total amount of organic halogens in an environment. Seawater and surface sediment samples from 12 sample sites in the Hangzhou Bay (HZB), China, were analyzed for AOX to investigate its contamination status. In this study, the AOX concentration ranged from 140.6 ± 45.6 μg/L to 716.1 ± 62.3 μg/L in seawater of the HZB, and from 11.3 ± 2.4 mg/kg to 112.7 ± 7.2 mg/kg in the sediment. Ocean currents, fluvial currents and the Yangtze River exerted profound influences on the distribution of AOX in the HZB. The point sources around the HZB, represented by wastewater treatment plants, discharged at least 645.4 t AOX into the HZB every year, most of which was generated by industrial activities rather than the human daily activities.

To explore the influence of rapid urbanization development on the accumulation of 16 priority PAHs in urban environment, thirty-three surface sediments from city lakes in different urbanized areas of Shanghai were collected to evaluate the occurrence characteristic and source apportionment of PAHs. The concentrations of Σ₁₆PAHs in lake surface sediments ranged from 55.7 to 4928 ng g⁻¹ with a mean value of 1131 ng g⁻¹ (standard deviation, 1228 ng g⁻¹), of which 4-, 5- and 6-ring PAHs were the dominant components. Spatial distribution of PAHs in lake surface sediments showed a significantly declining trend along with a decreasing urbanization gradient (one-way ANOVA, p < .05). Two hotspots of sediment PAHs were mainly distributed at highly urbanized areas with intensive population density and heavy traffic activities and at burgeoning industrial towns in the suburb. Source apportionment of total PAHs identified by a constrained positive matrix factorization model revealed that vehicle emission and combustion of coal, biomass and natural gas were the absolutely predominant sources, respectively accounting for 55.0% and 40.45% of total PAHs burden in lake sediments. Land use regression (LUR) models were successfully developed to evaluate spatial variation of PAHs contamination in urban sediments based on their significant correlations with residential land, commercial land, traffic variables, industrial sources, and population density. All PAH compounds showed strong associations with one or two source indicators (the traffic congestion index and the number of industrial sources), with the fitting R² varying from 0.529 to 0.984. Our findings suggest that energy consumption related to land use activities obviously promoted PAH accumulations in urban sediment environment during rapid development of urbanization and industrialization in Shanghai.

Waterborne exposure towards fungicides is known to trigger negative effects in aquatic leaf-associated microbial decomposers and leaf-shredding macroinvertebrates. We expected similar effects when these organisms use leaf material from terrestrial plants that were treated with systemic fungicides as a food source since the fungicides may remain within the leaves when entering aquatic systems. To test this hypothesis, we treated black alder (Alnus glutinosa) trees with a tap water control or a systemic fungicide mixture (azoxystrobin, cyprodinil, quinoxyfen, and tebuconazole) at two worst-case application rates. Leaves of these trees were used in an experiment targeting alterations in two functions provided by leaf-associated microorganisms, namely the decomposition and conditioning of leaf material. The latter was addressed via the food-choice response of the amphipod shredder Gammarus fossarum. During a second experiment, the potential impact of long-term consumption of leaves from trees treated with systemic fungicides on G. fossarum was assessed. Systemic fungicide treatment altered the resource quality of the leaf material resulting in trends of increased fungal spore production and an altered community composition of leaf-associated fungi. These changes in turn caused a significant preference of Gammarus for microbially conditioned leaves that had received the highest fungicide treatment over control leaves. This higher food quality ultimately resulted in a higher gammarid growth (up to 300% increase) during the long-term feeding assay. Although the underlying mechanisms still need to be addressed, the present study demonstrates a positive indirect response in aquatic organisms due to systemic pesticide application in a terrestrial system. As the effects from the introduction of plant material treated with systemic fungicides strongly differ from those mediated via other pathways (e.g., waterborne exposure), our study provides a novel perspective of fungicide-triggered effects in aquatic detritus-based food webs.