Triclosan (TCS) is a broad-spectrum antimicrobial agent that is found extensively in natural aquatic environments. Enzyme-catalyzed oxidative coupling reactions (ECOCRs) can be used to remove TCS in aqueous solution, but there is limited information available to indicate how metal cations (MCs) and natural organic matter (NOM) influence the environmental fate of TCS during laccase-mediated ECOCRs. In this study, we demonstrated that the naturally occurring laccase from Pleurotus ostreatus was effective in removing TCS during ECOCRs, and the oligomerization of TCS was identified as the dominant reaction pathway by high-resolution mass spectrometry (HRMS). The growth inhibition studies of green algae (Chlamydomonas reinhardtii and Scenedesmus obliquus) proved that laccase-mediated ECOCRs could effectively reduce the toxicity of TCS. The presence of dissolved MCs (Mn²⁺, Al³⁺, Ca²⁺, Cu²⁺, and Fe²⁺ ions) influenced the removal and transformation of TCS via different mechanisms. Additionally, the transformation of TCS in systems with NOM derived from humic acid (HA) was hindered, and the apparent pseudo first-order kinetics rate constants (k) for TCS decreased as the HA concentration increased, which likely corresponded to the combined effect of both noncovalent (sorption) and covalent binding between TCS and humic molecules. Our results provide a novel insight into the fate and transformation of TCS by laccase-mediated ECOCRs in natural aquatic environments in the presence of MCs and NOM.

Knowledge of the heterogeneous distribution of humic substances (HS) reactivities along a continuum of molecular weight (MW) is crucial for the systems where the HS MW is subject to change. In this study, two dimensional correlation spectroscopy combined with size exclusion chromatography (2D-CoSEC) was first utilized to obtain a continuous and heterogeneous presence of copper binding characteristics within bulk HS with respect to MW. HS solutions with varying copper concentrations were directly injected into a size exclusion chromatography (SEC) system with Tris-HCl buffer as a mobile phase. Several validation tests confirmed neither structural disruption of HS nor competition effect of the mobile phase used. Similar to batch systems, fluorescence quenching was observed in the chromatograms over a wide range of HS MW. 2D-CoSEC maps of a soil-derived HS (Elliot soil humic acid) showed the greater fluorescence quenching degrees with respect to the apparent MW on the order of 12500 Da > 10600 Da > 7000 Da > 15800 Da. The binding constants calculated based on modified Stern-Volmer equation were consistent with the 2D-CoSEC results. More heterogeneity of copper binding affinities within bulk HS was found for the soil-derived HS versus an aquatic HS. The traditional fluorescence quenching titration method using ultrafiltered HS size fractions failed to delineate detailed distribution of the copper binding characteristics, exhibiting a much shorter range of the binding constants than those obtained from the 2D-CoSEC. Our proposed technique demonstrated a great potential to describe metal binding characteristics of HS at high MW resolution, providing a clear picture of the size-dependent metal-HS interactions.

The iSimangaliso Wetland Park World Heritage site, located on the east coast of South Africa, spans ∼3300 km2 and constitutes the largest protected estuarine environment for hippopotami, crocodiles and aquatic birds in Africa. Given the ecological importance of this site and continued use of organochlorine pesticides (OCPs) in the region, this study focused on the nature, distribution and potential sources of organochlorine contamination within iSimangaliso Wetland Park. OCPs were widely distributed in surface sediment samples obtained from the four main Ramsar wetland systems within the park (Lake St Lucia, Mkhuze, Lake Sibaya and Kosi Bay). ∑HCH and ∑DDT were the dominant contaminants detected with concentrations in the range of 26.29–282.5 ng/g and 34.49–262.4 ng/g, respectively. ∑DDT concentrations revealed a distinctive gradient, with significantly higher concentrations at Kosi Bay and Lake Sibaya attributed to the application of DDT for malaria control. p,p'-DDE and p,p'-DDD were the dominant isomers detected, but the detection of p,p'-DDT in a number of samples reflects recent inputs of technical DDT. Highest concentrations of HCH, endosulfan and heptachlor were detected in sediments from Mkhuze and reflect the substantial residue load these wetlands receive from agricultural activities within the catchment area. Isomeric compositions indicate that endosulfan and heptachlor residues are derived mainly from historical application, while inputs of HCH, aldrin and endrin could be attributed to more recent usage at several sites. OCP sediment concentrations from iSimangaliso represent the highest yet recorded in South Africa and some of the highest reported globally this century. Sediments found within the lakes and wetlands of iSimangaliso represent large reservoirs of contaminants that pose ecotoxicological threats to this globally important biodiversity hotspot. Detailed investigation into the bioaccumulation and toxicological risks of OCPs within the wetland park is urgently required.

The current air quality indices have been criticized for not capturing combined health effects of multiple air pollutants. We proposed an Air Quality Health Index (AQHI) based on the air pollution-mortality associations for communicating health risks of air pollution. Time-series studies were conducted to estimate the associations between air pollutants including sulfur dioxide (SO2), nitrogen dioxide (NO2), ozone (O3), suspended particulate matter smaller than 2.5 μm in aerodynamic diameter (PM2.5) and mortality in Guangzhou from 2012 to 2015. The sum of excess mortality risk was calculated to construct the AQHI, which was then adjusted to an arbitrary scale. We then assessed the validity of AQHI. An interquartile increase (IQR) of AQHI was associated with 3.61% [95% confidence interval (95% CI), 2.85%–4.37%], 3.73% (95%CI, 2.18%–5.27%) and 4.19% (95%CI, 2.87%–5.52%) increase of mortality, respiratory and cardiovascular hospital admissions, respectively. Compared with the currently used Air Quality Index (AQI), AQHI had higher effects on mortality and morbidity. Our study suggests that AQHI might comprehensively capture the combined effects of air pollution, which make it be a more valid communication tool of air pollution-related health risk.

Hazardous Trace elements (HTEs) emitted from coal combustion has raised widespread concern. Studies on the emission characteristics of five HTEs, namely arsenic (As), chromium (Cr), barium (Ba), manganese (Mn), lead (Pb) at three different loads (100%, 83%, 71% output) and different coal types were performed on a 350 MW coal-fired power plant equipped with SCR, ESP + FF, and WFGD. HTEs in the flue gas at the inlet/outlet of each air pollution control device (APCD) were sampled simultaneously based on US EPA Method 29. During flue gas HTEs sampling, coal, bottom ash, fly ash captured by ESP + FF, fresh desulfurization slurry, desulfurization wastewater were also collected. Results show that mass balance rate for the system and each APCD is in an acceptable range. The five studied HTEs mainly distribute in bottom and ESP + FF ash. ESP + FF have high removal efficiency of 99.75–99.95%. WFGD can remove part of HTEs further. Total removal rate across the APCDs ranges from 99.84 to 99.99%. Concentration of HTEs emitted to atmosphere is within the extremely low scope of 0.11–4.93 μg/m3. Emission factor of the five studied HTEs is 0.04–1.54 g/1012J. Content of As, Pb, Ba, Cr in solid samples follows the order of ESP + FF ash > bottom ash > gypsum. More focus should be placed on Mn in desulfuration wastewater, content of which is more than the standard value. This work is meaningful for the prediction and removal of HTEs emitted from coal-fired power plants.

Prenatal exposure to polycyclic aromatic hydrocarbons (PAHs) is a high-priority public health concern. However, maternal to fetal transplacental transfer of PAHs has not been systematically studied. To investigate the transplacental transfer of PAHs from mother to fetus and determine the influence of lipophilicity (octanol-water partition coefficient, KOW) on transfer process, in the present study, we measured the concentrations of 15 PAHs in 95 paired maternal and umbilical cord serum, and placenta samples (in total 285 samples) collected in Shanghai, China. The average concentration of total PAHs was the highest in maternal serums (1290 ng g−1 lipid), followed by umbilical cord serums (1150 ng g-1 lipid). The value was the lowest in placenta samples (673 ng g-1 lipid). Low molecular weight PAHs were the predominant compounds in the three matrices. Increases in fish and meat consumption did not lead to increases in maternal PAH levels, and no obvious gender differences in umbilical cord serums were observed. The widespread presence of PAHs in umbilical cord serums indicated the occurrence of transplacental transfer. The ratios of PAH concentrations in umbilical cord serum to those in maternal serum (F/M) and the concentrations in placenta to those in maternal serum (P/M) of paired samples were analyzed to characterize the transfer process of individual PAHs. Most F/M ratios on lipid basis were close to one (range: 0.79 to 1.36), which suggested that passive diffusion may control the transplacental transfer of PAHs from maternal serum to the fetal circulation. The P/M and F/M values calculated on lipid basis showed that PAHs with lower KOW were more likely to transfer from mother to fetus via the placenta.

Exposure to air pollutants such as volatile organic compounds (VOCs) and fine particulate matter (PM2.5) are associated with adverse health effects. This study applied multiple time resolution data of hourly VOCs and 24-h PM2.5 to a constrained Positive Matrix Factorization (PMF) model for source apportionment in Taipei, Taiwan. Ninety-two daily PM2.5 samples and 2208 hourly VOC measurements were collected during four seasons in 2014 and 2015. With some a priori information, we used different procedures to constrain retrieved factors toward realistic sources. A total of nine source factors were identified as: natural gas/liquefied petroleum gas (LPG) leakage, solvent use/industrial process, contaminated marine aerosol, secondary aerosol/long-range transport, oil combustion, traffic related, evaporative gasoline emission, gasoline exhaust, and soil dust. Results showed that solvent use/industrial process was the largest contributor (19%) to VOCs while the largest contributor to PM2.5 mass was secondary aerosol/long-range transport (57%). A robust regression analysis showed that secondary aerosol was mostly contributed by regional transport related factor (25%).

The desorption kinetics and mechanism were investigated using a Tenax extraction technique on different sediments spiked with radiocarbon-labeled benzo[a]pyrene (BaP). Five sedimentary fractions were sequentially fractionated, and the only nonhydrolyzable organic carbon fractions (NHC) were characterized using advanced solid-state 13C nuclear magnetic resonance spectroscopy (NMR), improved six end-member model, and a CO2 gas adsorption technique. The sediments contained high percentages of algaenan and/or sporopollenin but low percentages of black carbon and lignin. A first-order, two-compartment kinetics model described the desorption process very well (R2 > 0.990). Although some of the organic carbon fractions were significantly related to the desorption kinetics parameters, the NHC fractions showed the highly significant correlation. Moreover, the nanoporosity or specific surface area (SSA) of the NHC fractions was highly related to their OC contents and aliphatic C (R2 = 0.960, p < 0.01). The multiple regression equations among the desorption kinetics parameters, structural parameters, and nanoporosity were well established (R2=>0.999). Nanoporosity and aromatic C were the dominant contributors. Furthermore, the enhanced percentages of desorbed BaP at elevated temperatures significantly showed a linear regression with the structure and nanoporosity. To our knowledge, the above evidence demonstrates for the first time that the transfer (or diffusion) of BaP in the nanopores of condensed aromatic components is the dominant mechanism of the desorption kinetics of BaP at organic matter particle scale.

The common soil arthropod Folsomia candida can survive well when fed only maize pollen and thus may be exposed to insecticidal proteins by ingesting insect-resistant genetically engineered maize pollen containing Bacillus thuringiensis (Bt) proteins when being released into the soil. Laboratory experiments were conducted to assess the potential effects of Cry1Ab/Cry2Aj-producing transgenic Bt maize (Shuangkang 12–5) pollen on F. candida fitness. Survival, development, and the reproduction were not significantly reduced when F. candida fed on Bt maize pollen rather than on non-Bt maize pollen, but these parameters were significantly reduced when F. candida fed on non-Bt maize pollen containing the protease inhibitor E-64 at 75 μg/g pollen. The intrinsic rate of increase (rm) was not significantly reduced when F. candida fed on Bt maize pollen but was significantly reduced when F. candida fed on non-Bt maize pollen containing E−64. The activities of antioxidant-related enzymes in F. candida were not significantly affected when F. candida fed on Bt maize pollen but were significantly increased when F. candida fed on non-Bt pollen containing E−64. The results demonstrate that consumption of Bt maize pollen containing Cry1Ab/Cry2Aj has no lethal or sublethal effects on F. candida.

The 22ⁿᵈ Asia-Pacific Economic Cooperation (APEC) Conference was held near Yanqi Lake, Huairou, in Beijing, China during November 10-11, 2014. To guarantee haze-free days during the APEC Conference, the Beijing government and the governments of the surrounding provinces implemented a series of controls. Three months of Aethalometer 880 nm black carbon (BC) measurements were examined to understand the hourly fluctuations in BC concentrations that resulted from emission controls and meteorology changes. Measurements were collected at the University of Chinese Academy of Sciences near the APEC Conference site and in Central Beijing at the Institute of Remote Sensing and Digital Earth of the Chinese Academy of Sciences. Synoptic conditions are successfully represented through analysis of backward trajectories in six cluster groups. The clusters are identified based on air mass transport from various areas such as Inner Mongolia, Russia, three northeastern provinces, and Hebei industrial areas, to the measurement sites. Air pollution control measures during the APEC Conference significantly reduced BC at the conference site (Huairou) and in Central Beijing, with greater reductions in BC concentrations at the conference site than in Central Beijing. The highest BC concentrations in Huairou were associated with air masses originating from Central Beijing rather than from the Hebei industrial region. The success of the control measures implemented in Beijing and the surrounding regions demonstrates that BC concentrations can be effectively reduced to protect human health and mitigate regional climate forcing. This study also demonstrates the need for regional strategies to reduce BC concentrations, since urban areas like Beijing are sources as well as downwind receptors of emissions.