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Inhalation bioaccessibility of multi-class organic pollutants associated to atmospheric PM2.5: Correlation with PM2.5 properties and health risk assessment
2022
Sánchez-Piñero, Joel | Novo-Quiza, Natalia | Pernas-Castaño, Cristina | Moreda-Piñeiro, Jorge | Muniategui-Lorenzo, Soledad | López-Mahía, Purificación
Inhalation exposure to fine particulate matter (PM₂.₅) represents a global concern due to the adverse effects in human health. In the last years, scientific community has been adopted the assessment of the PM₂.₅-bound pollutant fraction that could be released (bioaccessible fraction) in simulated lung fluids (SLFs) to achieve a better understanding of PM risk assessment and toxicological studies. Thus, bioaccessibility of 49 organic pollutants, including 18 polycyclic aromatic hydrocarbons (PAHs), 12 phthalate esters (PAEs), 11 organophosphorus flame retardants (OPFRs), 6 synthetic musk compounds (SMCs) and 2 bisphenols in PM₂.₅ samples was evaluated. The proposed method consists of a physiologically based extraction test (PBET) by using artificial lysosomal fluid (ALF) to obtain bioaccessible fractions, followed by a vortex-assisted liquid-liquid microextraction (VALLME) and a final analysis by programmed temperature vaporization-gas chromatography-tandem mass spectrometry (PTV-GC-MS/MS). The highest inhalation bioaccessibility ratio was found for bisphenol A (BPA) with an average of 83%, followed by OPFRs, PAEs and PAHs (with average bioaccessibilities of 68%, 41% and 34%, respectively). Correlations between PM₂.₅ composition (major ions, trace metals, equivalent black carbon (eBC) and UV-absorbing particulate matter (UVPM)) and bioaccessibility ratios were also assessed. Principal Component Analysis (PCA) suggested that PAHs, PAES and OPFRs bioaccessibility ratios could be positively correlated with PM₂.₅ carbonaceous content. Furthermore, both inverse and positive correlations on PAHs, PAEs and OPFRs bioaccessibilites could be accounted for some major ions and metal (oid)s associated to PM₂.₅, whereas no correlations comprising considered PM₂.₅ major ions and metal (oid)s contents and BPA bioaccessibility was observed. In addition, health risk assessment of target PM₂.₅-associated PAHs via inhalation was assessed in the study area considering both total and bioaccessible concentrations, being averaged human health risks within the safe carcinogenic and non-carcinogenic levels.
Show more [+] Less [-]Versatile in silico modeling of XAD-air partition coefficients for POPs based on abraham descriptor and temperature
2022
Tao, Cuicui | Chen, Ying | Tao, Tianyun | Cao, Zaizhi | Chen, Wenxuan | Zhu, Tengyi
The concentration of persistent organic pollutants (POPs) makes remarkable difference to environmental fate. In the field of passive sampling, the partition coefficients between polystyrene-divinylbenzene resin (XAD) and air (i.e., KXAD₋A) are indispensable to obtain POPs concentration, and the KXAD₋A is generally thought to be governed by temperature and molecular structure of POPs. However, experimental determination of KXAD₋A is unrealistic for countless and novel chemicals. Herein, the Abraham solute descriptors of poly parameter linear free energy relationship (pp-LFER) and temperature were utilized to develop models, namely pp-LFER-T, for predicting KXAD₋A values. Two linear (MLR and LASSO) and four nonlinear (ANN, SVM, kNN and RF) machine learning algorithms were employed to develop models based on a data set of 307 sample points. For the aforementioned six models, R²ₐdⱼ and Q²ₑₓₜ were both beyond 0.90, indicating distinguished goodness-of-fit and robust generalization ability. By comparing the established models, the best model was observed as the RF model with R²ₐdⱼ = 0.991, Q²ₑₓₜ = 0.935, RMSEₜᵣₐ = 0.271 and RMSEₑₓₜ = 0.868. The mechanism interpretation revealed that the temperature, size of molecules and dipole-type interactions were the predominant factors affecting KXAD₋A values. Concurrently, the developed models with the broad applicability domain provide available tools to fill the experimental data gap for untested chemicals. In addition, the developed models were helpful to preliminarily evaluate the environmental ecological risk and understand the adsorption behavior of POPs between XAD membrane and air.
Show more [+] Less [-]Metagenomics highlights the impact of climate and human activities on antibiotic resistance genes in China's estuaries
2022
Zheng, Dongsheng | Yin, Guoyu | Liu, Min | Hou, Lijun | Yang, Yi | Liu, Xinran | Jiang, Yinghui | Chen, Cheng | Wu, Han
Estuarine environments faced with contaminations from coastal zones and the inland are vital sinks of antibiotic resistance genes (ARGs). However, little is known about the temporal-spatial pattern of ARGs and its predominant constraints in estuarine environments. Here, we leveraged metagenomics to investigate ARG profiles from 16 China's estuaries across 6 climate zones in dry and wet seasons, and disentangled their relationships with environmental constraints. Our results revealed that ARG abundance, richness, and diversity in dry season were higher than those in wet season, and ARG abundance exhibited an increasing trend with latitude. The prevalence of ARGs was significantly driven by human activities, mobile gene elements, microbial communities, antibiotic residuals, physicochemical properties, and climatic variables. Among which, climatic variables and human activities ranked the most important factors, contributing 44% and 36% of the total variance of observed ARGs, respectively. The most important climatic variable shaping ARGs is temperature, where increasing temperature is associated with decreased ARGs. Our results highlight that the prevalence of ARGs in estuarine environments would be co-driven by anthropogenic activities and climate, and suggest the dynamics of ARGs under future changing climate and socioeconomic development.
Show more [+] Less [-]The adsorption mechanisms of oriental plane tree biochar toward bisphenol S: A combined thermodynamic evidence, spectroscopic analysis and theoretical calculations
2022
Fang, Zheng | Gao, Yurong | Zhang, Fangbin | Zhu, Kaipeng | Shen, Zihan | Liang, Haixia | Xie, Yue | Yu, Chenglong | Bao, Yanping | Feng, Bo | Bolan, Nanthi | Wang, Hailong
Garden pruning waste is becoming a problem that intensifies the garbage siege. It is of great significance to purify polluted water using biochar prepared from garden pruning waste. Herein, the interaction mechanism between BPS and oriental plane tree biochar (TBC) with different surface functional groups was investigated by adsorption experiments, spectroscopic analysis and theoretical calculations. Adsorption kinetics and isotherm of BPS on TBC can be satisfactorily fitted into pseudo-second-order kinetic and Langmuir models, respectively. A rapid adsorption kinetic toward BPS was achieved by TBC in 15 min. As compared with TBC prepared at low temperature (300 °C) (LTBC), the maximum adsorption capacity of TBC prepared at high temperature (600 °C) (HTBC) can be significantly improved from 46.7 mg g⁻¹ to 72.9 mg g⁻¹. Besides, the microstructure and surface functional groups of HTBC were characterized using SEM, BET-N₂, and XPS analysis. According to density functional theory (DFT) theoretical calculations, the higher adsorption energy of HTBC for BPS was mainly attributed to π-π interaction rather than hydrogen bonding, which was further supported by the analysis of FTIR and Raman spectra as well as the adsorption thermodynamic parameters. These findings suggested that by improving π-π interaction through high pyrolysis temperature, BPS could be removed and adsorbed by biochar with high efficacy, cost-efficiency, easy availability, and carbon-negative in nature, contributing to global carbon neutrality.
Show more [+] Less [-]Short-term effects of cold spells on plasma viscosity: Results from the KORA cohort study in Augsburg, Germany
2022
Ni, Wenli | Schneider, Alexandra | Wolf, Kathrin | Zhang, Siqi | Chen, Kai | Koenig, Wolfgang | Peters, Annette | Breitner, Susanne
As the underlying mechanisms of the adverse effects of cold spells on cardiac events are not well understood, we explored the effects of cold spells on plasma viscosity, a blood parameter linked to cardiovascular disease. This cross-sectional study involved 3622 participants from the KORA S1 Study (1984–1985), performed in Augsburg, Germany. Exposure data was obtained from the Bavarian State Office for the Environment. Cold spells were defined as two or more consecutive days with daily mean temperatures below the 3ʳᵈ, 5ᵗʰ, or 10ᵗʰ percentile of the distribution. The effects of cold spells on plasma viscosity were explored by generalized additive models with distributed lag nonlinear models (DLNM). We estimated cumulative effects at lags 0–1, 0–6, 0–13, 0–20, and 0–27 days separately. Cold spells (mean temperature <3ʳᵈ, <5ᵗʰ or <10ᵗʰ percentile) were significantly associated with an increase in plasma viscosity with a lag of 0–1 days [%change of geometric mean (95% confidence interval): 1.35 (0.06–2.68), 1.35 (0.06–2.68), and 2.49 (0.34–4.69), respectively], and a lag of 0–27 days [18.81 (8.97–29.54), 17.85 (8.29–28.25), and 7.41 (3.35–11.0), respectively]. For the analysis with mean temperature <3ʳᵈ or 10ᵗʰ percentile, we also observed significant associations at lag 0–20 days [8.34 (0.43–16.88), and 4.96 (1.68, 8.35), respectively]. We found that cold spells had significant immediate and longer lagged effects on plasma viscosity. This finding supports the complex interplay of multiple mechanisms of cold on adverse cardiac events and enriches the knowledge about how cold exposure acts on the human body.
Show more [+] Less [-]Marine heatwaves hamper neuro-immune and oxidative tolerance toward carbamazepine in Mytilus galloprovincialis
2022
Nardi, Alessandro | Mezzelani, Marica | Costa, Silvana | d’Errico, Giuseppe | Benedetti, Maura | Gorbi, Stefania | Freitas, Rosa | Regoli, Francesco
The increased frequency and intensity of short-term extreme warming phenomena have been associated to harsh biological and ecosystem outcomes (i.e., mass mortalities in marine organisms). Marine heatwaves (MHWs), occurring when seasonal temperature threshold is exceeded for at least 5 consecutive days, may reduce the tolerance of coastal species toward additional pressures, but interactions between such multiple stressors are virtually unexplored. The present study aimed to characterize in Mytilus galloprovincialis the influence of a simulated MHW scenario on the toxicological effects of the pharmaceutical carbamazepine (CBZ), ubiquitously detected in the marine environment and chosen as model compound for this relevant class of emerging contaminants. The bioaccumulation of CBZ and responsiveness of various biological parameters, including immune system, antioxidant status, lipid metabolism and cellular integrity, were analyzed in exposed mussels both during and after the end of the heatwave. MHW appeared to strongly modulate accumulation of CBZ, paralleled by weakened immunocompetence and onset of oxidative disturbance that finally evolved to cellular damages and lipid metabolism disorders. Elaboration of the overall results through a quantitative Weight of Evidence model, revealed the highest hazard in organisms exposed to both the stressors 10 days after the end of the heatwave, suggesting that MHWs could leave a footprint on the capability of mussels to counteract CBZ toxicity, thus affecting their vulnerability and predisposition to adverse effects toward multiple stressors.
Show more [+] Less [-]A wide range of toxic VOCs measured by dual-sorbent passive sampling with validation by field online measurements
2022
Lee, Yu-Hsun | Wang, Chieh-Heng | Hsu, Pei-Hsuan | Hsieh, Hsin-Cheng | Wang, Jia-Lin
This study modified a passive sampling technique similar to the US EPA Method 325 A/B method but extended to include more toxic volatile organic compounds (VOCs) under varied climate conditions to enhance field applicability. A mixing chamber was built to determine uptake rates (Us) for the target compounds. It was found that the Us of 27 air toxics previously reported in the literature agreed reasonably well with our findings within 18%, thus proving the chamber's integrity. To broaden the compound coverage, both Carbopack X and Carboxen 569 were studied for a suite of toxic VOCs to meet stringent quality control (QC) criteria of correlation coefficients (R-square), method detection limits (MDL), back diffusion (BD), storage stability, as well as a wide range of climate conditions in temperature and humidity. After excluding the species that failed to pass any of the QC criteria, Carbopack X was found to fit 50 air toxics, whereas Carboxen 569 held 37. After excluding the overlapped species, 61 toxic VOCs can be determined with robust Us for a broad range of climate conditions when the two sorbents are used in pairs. A one-week field measurement was conducted to compare with the online thermal desorption gas chromatography-mass spectrometry (TD-GC-MS) with hourly data resolution. The field passive sampling showed comparable results to the means of the online hourly measurements, despite the high variability of selected target compounds, such as toluene from 0.3 ppbv as the 5th percentile to the maximum of about 80 ppbv. Passive sampling clearly demonstrated the ability to smooth out concentration variability and thus the time-averaging strength of toxic VOCs, revealing its ideal role as an exposure monitor over time. The passive sampling method can be more desired than active sampling or online methods when the aim is simply the knowledge of prolonged time-averaged concentrations.
Show more [+] Less [-]Separating emissions and meteorological impacts on peak ozone concentrations in Southern California using generalized additive modeling
2022
Gao, Ziqi | Ivey, Cesunica E. | Blanchard, Charles L. | Do, Khanh | Lee, Sang-Mi | Russell, Armistead G.
Ozone levels have been declining in the Los Angeles, CA, USA area for the last four decades, but there was a recent uptick in the 4th highest daily maximum 8-h (MDA8) ozone concentrations from 2014 to 2018 despite continued reductions in the estimated precursor emissions. In this study, we assess the emissions and meteorological impacts on the 4th highest MDA8 ozone concentrations to better understand the factors affecting the observed MDA8 ozone using a two-step generalized additive model (GAM)/least squares approach applied to the South Coast Air Basin (SoCAB) for the 1990 to 2019 period. The GAM model includes emissions, meteorological factors, large-scale climate variables, date, and the interactions between meteorology and emissions. A least squares method was applied to the GAM output to better capture the 4th highest MDA8 ozone. The resulting two-step model had an R² of 0.98 and a slope of 1 between the observed and predicted 4th highest MDA8 ozone. Emissions and the interactions between the maximum temperature and emissions explain most of the variation in the peak MDA8 ozone concentrations. Declining emissions have lowered the 4th highest MDA8 ozone concentration. Meteorology explains the higher than expected 4th-high, ozone levels observed in 2014–2018, indicating that meteorology was a stronger forcer than the continued reductions in emissions during that time period. The model was applied to estimate future ozone levels. Meteorology developed from climate modeling of the representative concentration pathway (RCP) scenarios, and two sets of emissions were used in the application. The modeling results indicated climate trends will push ozone levels slightly higher if no further emissions reductions are realized and that of two emissions trajectories modeled, the more stringent is required to reliably meet the federal ozone standard given annual meteorological variability.
Show more [+] Less [-]Local environment modulates whole-transcriptome expression in the seagrass Posidonia oceanica under warming and nutrients excess
2022
Pazzaglia, Jessica | Santillán-Sarmiento, Alex | Ruocco, Miriam | Dattolo, Emanuela | Ambrosino, Luca | Marín-Guirao, Lazaro | Procaccini, Gabriele
The intensification of anomalous events of seawater warming and the co-occurrence with local anthropogenic stressors are threatening coastal marine habitats, including seagrasses, which form extensive underwater meadows. Eutrophication highly affects coastal environments, potentially summing up to the widespread effects of global climate changes. In the present study, we investigated for the first time in seagrasses, the transcriptional response of different plant organs (i.e., leaf and shoot apical meristem, SAM) of the Mediterranean seagrass Posidonia oceanica growing in environments with a different history of nutrient enrichment. To this end, a mesocosm experiment exposing plants to single (nutrient enrichment or temperature increase) and multiple stressors (nutrient enrichment plus temperature increase), was performed. Results revealed a differential transcriptome regulation of plants under single and multiple stressors, showing an organ-specific sensitivity depending on plants' origin. While leaf tissues were more responsive to nutrient stress, SAM revealed a higher sensitivity to temperature treatments, especially in plants already impacted in their native environment. The exposure to stress conditions induced the modulation of different biological processes. Plants living in an oligotrophic environment were more responsive to nutrients compared to plants from a eutrophic environment. Evidences that epigenetic mechanisms were involved in the regulation of transcriptional reprogramming were also observed in both plants’ organs. These results represent a further step in the comprehension of seagrass response to abiotic stressors pointing out the importance of local pressures in a global warming scenario.
Show more [+] Less [-]Morphological, physiological and behavioral responses of an intertidal snail, Acanthina monodon (Pallas), to projected ocean acidification and cooling water conditions in upwelling ecosystems
2022
Duarte, Cristian | Jahnsen-Guzmán, Nicole | Quijón, Pedro A. | Manríquez, Patricio H. | Lardies, Marco A. | Fernández, Carolina | Reyes, Miguel | Zapata, Javier | García-Huidobro, M Roberto | Lagos, Nelson A.
Ocean acidification (OA) is expected to rise towards the end of the 21st century altering the life history traits in marine organisms. Upwelling systems will not escape OA, but unlike other areas of the ocean, cooling effects are expected to intensify in these systems. Regardless, studies evaluating the combined effects of OA and cooling remain scarce. We addressed this gap using a mesocosm system, where we exposed juveniles of the intertidal muricid snail Acanthina monodon to current and projected pCO₂ (500 vs. 1500 ppm) and temperature (15 vs. 10 °C) from the southeast Pacific upwelling system. After 9 weeks of experimental exposure to those conditions, we conducted three estimations of growth (wet weight, shell length and shell peristomal length), in addition to measuring calcification, metabolic and feeding rates and the ability of these organisms to return to the normal upright position after being overturned (self-righting). Growth, feeding and calcification rates increased in projected cooling conditions (10 °C) but were unaffected by pCO₂ or the interaction between pCO₂ and temperature. Instead, metabolic rates were driven by pCO₂, but a significant interaction with temperature suggests that in cooler conditions, metabolic rates will increase when associated with high pCO₂ levels. Snail self-righting times were not affected across treatments. These results suggest that colder temperatures projected for this area would drive this species growth, feeding and calcification, and consequently, some of its population biology and productivity. However, the snails may need to compensate for the increase in metabolic rates under the effects of ocean acidification. Although A. monodon ability to adjust to individual or combined stressors will likely account for some of the changes described here, our results point to a complex dynamic to take place in intertidal habitats associated with upwelling systems.
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