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Combined use of daily and hourly data sets for the source apportionment of particulate matter near a waste incinerator plant
2019
Lucarelli, F. | Barrera, V. | Becagli, S. | Chiari, M. | Giannoni, M. | Nava, S. | Traversi, R. | Calzolai, G.
A particulate matter (PM) source apportionment study was carried out in one of the most polluted districts of Tuscany (Italy), close to an old waste incinerator plant. Due to the high PM10 levels, an extensive field campaign was supported by the Regional Government to identify the main PM sources and quantify their contributions. PM10 daily samples were collected for one year and analysed by different techniques to obtain a complete chemical characterisation (elements, ions and carbon fractions). Hourly fine (<2.5 μm) and coarse (2.5–10 μm) aerosol samples were collected by a Streaker sampler for a shorter period and hourly elemental concentrations were obtained by PIXE.Positive Matrix Factorization (PMF) analysis of daily and hourly data allowed the identification of 10 main sources: six anthropogenic (Biomass Burning, Traffic, Secondary Nitrates, Secondary Sulphates, Incinerator, Heavy Oil combustion), two natural (Saharan Dust and Fresh Sea Salt) and two mixed sources (Local Dust and Aged Sea Salt). Biomass burning turned out to be the main source of PM, accounting for 30% of the PM10 mass as annual average, followed by Traffic (18%) and Secondary Nitrates (14%). Emissions from the Incinerator turned out to be only 2% of PM10 mass on average.PM10 composition and source apportionment have been assessed in a polluted area near a waste incinerator, by PMF analysis on daily and hourly compositional data sets.
Show more [+] Less [-]What is the most ecologically-meaningful metric of nitrogen deposition?
2019
Payne, Richard J. | Campbell, Claire | Britton, Andrea J. | Mitchell, R. J. (Ruth J.) | Pakeman, R. J. (Robin J.) | Jones, Laurence | Ross, L. C. (Louise C.) | Stevens, Carly J. | Field, Christopher | Caporn, Simon J.M. | Carroll, Jacky | Edmondson, Jill L. | Carnell, Edward J. | Tomlinson, Sam | Dore, Anthony J. | Dise, Nancy | Dragosits, Ulrike
Nitrogen (N) deposition poses a severe risk to global terrestrial ecosystems, and managing this threat is an important focus for air pollution science and policy. To understand and manage the impacts of N deposition, we need metrics which accurately reflect N deposition pressure on the environment, and are responsive to changes in both N deposition and its impacts over time. In the UK, the metric typically used is a measure of total N deposition over 1–3 years, despite evidence that N accumulates in many ecosystems and impacts from low-level exposure can take considerable time to develop. Improvements in N deposition modelling now allow the development of metrics which incorporate the long-term history of pollution, as well as current exposure. Here we test the potential of alternative N deposition metrics to explain vegetation compositional variability in British semi-natural habitats. We assembled 36 individual datasets representing 48,332 occurrence records in 5479 quadrats from 1683 sites, and used redundancy analyses to test the explanatory power of 33 alternative N metrics based on national pollutant deposition models. We find convincing evidence for N deposition impacts across datasets and habitats, even when accounting for other large-scale drivers of vegetation change. Metrics that incorporate long-term N deposition trajectories consistently explain greater compositional variance than 1–3 year N deposition. There is considerable variability in results across habitats and between similar metrics, but overall we propose that a thirty-year moving window of cumulative deposition is optimal to represent impacts on plant communities for application in science, policy and management.
Show more [+] Less [-]Cd contamination status and cost-benefits analysis in agriculture soils of Yangtze River basin
2019
Zhou, Xi-Yin | Wang, Xiuru
Soil is a fundamental carrier to support for human living and development and has been polluted seriously by heavy metals. This fact highlights the urgency to realize soil heavy metal pollution prevention through soil heavy metals contamination status assessment and root cause analysis. The previous research tends to focus status assessment and source identification without consideration of economic aspect. This study realized the systematic analysis from status assessment, sources identification and economic-environmental cost-benefits analysis in the Yangtze River basin. Through the spatial difference comparison among the provinces of upper, middle and lower in the Yangtze River basin, it revealed that anthropogenic influence is the main reason caused the current Cd contamination in Yangtze River basin. An interesting finding is that the human caused Cd concentration contribution amount is nearly the same between upstream and downstream which is all about 0.1 mg/kg, while they have quite different economic scale. It indicated that due to the difference of the scale and structure of local economy, and the level of cleaner production and pollution treatment, some regions could own high economic-benefits and low environmental cost, which it is opposite in other regions. The geographic location and natural resources is the root cause to form the environmental cost-economic benefits difference among regions. The convenient traffic promoted downstream to develop large amount and high quality of economy. The natural mineral resources promoted midstream to develop resources based economy. The poor condition of traffic and natural resources has restricted the development of Qinghai province, and made it has the highest Cd pollution intensity. The results would provide effective economic management measures for better soil quality and sustainable development goals achievement.
Show more [+] Less [-]Characterization of a multianalyte GC-MS/MS procedure for detecting and quantifying polycyclic aromatic hydrocarbons (PAHs) and PAH derivatives from air particulate matter for an improved risk assessment
2019
Mueller, Andrea | Ulrich, Nadin | Hollmann, Josef | Zapata Sanchez, Carmen E. | Rolle-Kampczyk, Ulrike E. | von Bergen, Martin
A correct description of the concentration and distribution of particle bound polycyclic aromatic hydrocarbons is important for risk assessment of atmospheric particulate matter. A new targeted GC-MS/MS method was developed for analyzing 64 PAHs including compounds with a molecular weight >300, as well as nitro-, methyl-, oxy- and hydroxyl derivatives in a single analysis. The instrumental LOD ranged between 0.03 and 0.7 pg/μL for PAHs, 0.2–7.9 pg/μL for hydroxyl and oxy PAHs, 0.1–7.4 pg/μL for nitro PAHs and 0.06–0.3 pg/μL for methyl-PAHs. As an example for the relevance of this method samples of PM₁₀ were collected at six sampling sites in Medellin, Colombia, extracted and the concentration of 64 compounds was determined. The 16 PAHs from the EPA priority list contributed only from 54% to 69% to the sum of all analyzed compounds, PAH with high molecular weight accounted for 8.8%–18.9%. Benzo(a)pyrene equivalents (BaPₑq) were calculated for the estimation of the life time cancer (LCR). The LCR according to the samples ranged from 2.75 × 10⁻⁵ to 1.4 × 10⁻⁴ by a calculation with toxic equivalent factors (TEF) and 5.7 × 10⁻⁵ to 3.8 × 10⁻⁴ with potency equivalent factor (PEF). By using the new relative potency factors (RPF) recommended by US Environmental Protection Agency (U.S.EPA) the LCR ranged from 1.3 × 10⁻⁴ to 7.2 × 10⁻⁴. Hence, it was around six times higher than the well-known TEF. The novel method enables the reliable quantification of a more comprehensive set of PAHs bound on PM and thus will facilitate and improve the risk assessment of them.
Show more [+] Less [-]Insight into the nitrification kinetics and microbial response of an enriched nitrifying sludge in the biodegradation of sulfadiazine
2019
Wang, Bingzheng | Ni, Bing-Jie | Yuan, Zhiguo | Guo, Jianhua
The intensive use of antibiotics results in the continuous release of antibiotics into wastewater treatment systems, leading to the spread of antibiotic resistance. Nitrifying system is reported to be capable of degrading antibiotics, yet few studies have systematically investigated the inherent correlation among ammonium oxidation rate, antibiotic degradation and genetic expression of nitrifying bacteria along the process. This study selected a widely used sulfonamide antibiotic, sulfadiazine (SDZ), to investigate its biodegradation potential by an enriched nitrifying culture and the response of nitrifying bacteria against antibiotic exposure. Our results demonstrated that SDZ degradation was mainly contributed by cometabolism of ammonia-oxidizing bacteria (AOB), rather than biomass adsorption. The quantitative reverse transcription PCR (RT-qPCR) analysis revealed that the expression level of amoA gene was down-regulated due to the SDZ exposure. In addition, the degradation products of SDZ did not exhibit inhibitory effect on Escherichia coli K12, indicating the biotoxicity of SDZ could be mitigated after biodegradation. The findings offer insights regarding the biodegradation process of sulfonamide antibiotics via cometabolism by AOB.
Show more [+] Less [-]Identification of 7–9 ring polycyclic aromatic hydrocarbons in coals and petrol coke using High performance liquid chromatography – Diode array detection coupled to Atmospheric pressure laser ionization – Mass spectrometry (HPLC-DAD-APLI-MS)
2019
Thiäner, Jan B. | Nett, Linus | Zhou, Shangbo | Preibisch, Yves | Hollert, Henner | Achten, Christine
Polycyclic aromatic hydrocarbons containing at least 24 carbon atoms (≥C₂₄-PAH) are often associated with pyrogenic processes such as combustion of fuel, wood or coal, and occur in the environment in diesel particulate matter, black carbon and coal tar. Some of the ≥C₂₄-PAH, particularly the group of dibenzopyrenes (five isomers, six aromatic rings) are known to show high mutagenic and carcinogenic activita.Gas chromatography – mass spectrometry is a well-established method for the analysis of lower molecular weight PAH but is not optimally suited for the analysis of ≥C₂₄-PAH due to their low vapor pressures. Also, hundreds of ≥C₂₄-PAH isomers are possible but only a few compounds are commercially available as reference standards. Therefore, in this study, a combination of multidimensional liquid chromatography, UV–Vis diode array detection, PAH selective and highly sensitive atmospheric pressure laser ionization – mass spectrometry is used to detect and unequivocally identify PAH. For identification of PAH in two bituminous coals and one petrol coke sample, unique and compound specific UV–Vis spectra were acquired. It was possible to identify ten compounds (naphtho[1,2,3,4-ghi]perylene, dibenzo[b,ghi]perylene, dibenzo[e,ghi]perylene, dibenzo[cd,lm]perylene, benzo[a]coronene, phenanthrol[5,4,3,2-abcde]perylene, benzo[ghi]naphtho[8,1,2-bcd]perylene, benzo[pqr]naphtho[8,1,2-bcd]perylene, naphtho[8,1,2-abc]coronene and tribenzo[e,ghi,k]perylene) by comparison of acquired spectra with spectra from literature. Additionally, it was possible to detect similar distribution patterns in different samples and signals related to alkylated naphthopyrenes, naphthofluoranthenes or dibenzopyrenes. Subsequent effect-directed analysis of a bituminous coal sample using the microEROD (ethoxyresorufin-O-deethylase) bioassay showed high suitability and revealed lower EROD induction for the ≥C₂₄-PAH (TEQ range 0.67–10.07 ng/g) than for the allover < C₂₄-PAH containing fraction (TEQ 84.00 ng/g). Nevertheless, the toxicity of ≥C₂₄-PAH has a significant impact compared with <C₂₄-PAH and must be considered for risk assessment. The LC-DAD-APLI-MS method, presented in this study, is a powerful tool for the unequivocal identification of these ≥ C₂₄-PAH.
Show more [+] Less [-]Occurrence of organophosphate flame retardants in farmland soils from Northern China: Primary source analysis and risk assessment
2019
Ji, Yan | Wang, Yu | Yao, Yiming | Ren, Chao | Lan, Zhonghui | Fang, Xiangguang | Zhang, Kai | Sun, Weijie | Alder, Alfredo C. | Sun, Hongwen
Ninety-eight soil samples were collected from farmland soils from Beijing-Tianjin-Hebei core area, Northern China, where agricultural lands were subjected to contamination from intense urban and industrial activities. Twelve organophosphates flame retardants (OPFRs) were analyzed with total soil concentrations ranging from 0.543 μg/kg to 54.9 μg/kg. Chlorinated OPFRs were dominating at mean level of 3.64 μg/kg and Tris(2-chloroisopropyl) phosphate contributed the most (mean 3.36 ± 5.61 μg/kg, 98.0%). Tris(2-ethylhexyl) phosphate was fully detected at levels of 0.041–1.95 μg/kg. Generally, tris(2-butoxyethyl) phosphate and triphenyl phosphate contributed the most to alkyl- (53.6%) and aryl-OPFRs (54.3%), respectively. The levels of ∑OPFRs close to the core urban areas were significantly higher than those from background sites. The occurrence and fate of OPFRs in soil were significantly associated with total organic carbon content and mostly with fine soil particles (<0.005 mm), and a transfer potential from the atmosphere was predicted with logKSA values. Comparable soil levels with poly brominated diphenyl ethers s in other studies suggested that the contamination of OPFRs occurred in farmland soil with an increasing trend but currently showed no significant environmental risk based on risk quotient estimation (<1). This investigation warrants further study on behaviors of OPFRs in a soil system and a continual monitoring for their risk assessment.
Show more [+] Less [-]Role of PM2.5 in the photodegradation of the atmospheric benzene
2019
Liu, Chunqiong | Zhang, Xiaohui | Wang, Qingeng | Shi, Kai
The presence of PM₂.₅ may affect the photodegradation of benzene in the natural atmosphere. On one hand, the photodegradation of benzene may be promoted with the increase in PM₂.₅ concentrations, owing to adsorption and catalysis effect of PM₂.₅ surface; On the other hand, PM₂.₅ can scatter or block ultraviolet light and lead to weakening the photochemical reactions in the atmospheric system. It is very difficult to prove which process is dominant in the real atmosphere due to the complexity of the atmosphere. Based on coupling detrended fluctuation analysis, the goal of this work is to reveal the role of PM₂.₅ in the photodegradation of benzene in real atmosphere over long time scales. The 9 years regular monitoring data from 2007 to 2016 in Puzi of Taiwan are analyzed. A new nonlinear parameter (PDB) is established to characterize the photodegradation degree of atmospheric benzene. Based on sliding window technique, the correlations between the temporal variation of PDB and PM₂.₅ are analyzed. The results show that there is a positive correlation between PDB and PM₂.₅ in daytime and little correlation between them in nighttime. It indicates that PM₂.₅ mainly plays the promoting effect on the photodegradation of atmospheric benzene. This is the first study to directly determine the role of PM₂.₅ in the photochemical behavior of atmospheric benzene based on long term field observation data. Moreover, the results suggest that the regional transport of PM₂.₅ could seriously affect the geochemistry cycle of some VOCs. This research provides a new analysis method to directly quantify the effect of PM₂.₅ on the photodegradation of VOCs in the real atmosphere. It is helpful for evaluating the role of PM₂.₅ in the complex photochemical system.
Show more [+] Less [-]Assessment of ultrafine particles in primary schools: Emphasis on different indoor microenvironments
2019
Slezakova, Klara | Fernandes, Eduardo de Oliveira | Pereira, Maria do Carmo
Due to the negative health impacts, significant efforts have been directed towards investigating ultrafine particle (UFP) exposure in various indoor environments. As children spend approximately one third of their time in schools, educatory environments deserve particular attention; however, majority of past research has focused on UFP assessment in classrooms. Thus, this work aims to expand the characterization of UFP in primary schools by considering different indoor and outdoor school microenvironments and estimating inhalation doses for the respective students (6–11yrs old). Real-time UFP measurements were daily conducted (9:00–17:30) in 20 primary schools in Oporto (January–April 2014; October–February 2015) in classrooms, canteens, gyms, libraries, and concurrently outdoors. Overall, UFP concentrations showed large temporal and spatial variations. For classrooms (n = 73), median UFP (1.56 × 10³–16.8 × 10³ # cm⁻³) were lower than the corresponding levels in ambient air of schools (1.79 × 10³–24.1 × 10³ # cm⁻³). Outdoor emissions contributed to indoor UFP (indoor-to-outdoor ratios I/O of 0.0.30–0.85), but ventilation, room characteristics and its occupancy were identified as important parameters contributing to overall indoor UFP levels. Considering specific indoor school microenvironments, canteens were the microenvironment with the highest UFP levels (5.47 × 10³–36.4 × 10³ # cm⁻³), cooking conducted directly on school grounds resulted in significantly elevated UFP in the respective classrooms (p < 0.05); the lowest UFP were found in libraries (4.45 × 10³–8.50 × 10³ # cm⁻³) mostly due to the limited occupancies. Although students spend majority of their school time in classrooms (66–71%), classroom exposure was not consistently the predominant contributor to school total UFP inhalation dose (29–75%). Outdoor exposure contributed 23–70% of school dose (depending on UFP levels in ambient levels and/or conducted activities) whereas short periods of lunch break accounted for 8–40%. Therefore, when evaluating UFP exposure in educatory settings other microenvironments beyond classrooms should be an integral part of the study.
Show more [+] Less [-]Toxicogenomic responses of Caenorhabditis elegans to pristine and transformed zinc oxide nanoparticles
2019
Starnes, Daniel | Unrine, Jason | Chen, Chun | Lichtenberg, Stuart | Starnes, Catherine | Svendsen, Claus | Kille, Peter | Morgan, John | Baddar, Zeinah Elhaj | Spear, Amanda | Bertsch, Paul | Chen, Kuey Chu | Tsyusko, Olga
Manufactured nanoparticles (MNPs) undergo transformation immediately after they enter wastewater treatment streams and during their partitioning to sewage sludge, which is applied to agricultural soils in form of biosolids. We examined toxicogenomic responses of the model nematode Caenorhabditis elegans to pristine and transformed ZnO-MNPs (phosphatized pZnO- and sulfidized sZnO-MNPs). To account for the toxicity due to dissolved Zn, a ZnSO₄ treatment was included. Transformation of ZnO-MNPs reduced their toxicity by nearly ten-fold, while there was almost no difference in the toxicity of pristine ZnO-MNPs and ZnSO₄. This combined with the fact that far more dissolved Zn was released from ZnO- compared to pZnO- or sZnO-MNPs, suggests that dissolution of pristine ZnO-MNPs is one of the main drivers of their toxicity. Transcriptomic responses at the EC₃₀ for reproduction resulted in a total of 1161 differentially expressed genes. Fifty percent of the genes differentially expressed in the ZnSO₄ treatment, including the three metal responsive genes (mtl-1, mtl-2 and numr-1), were shared among all treatments, suggesting that responses to all forms of Zn could be partially attributed to dissolved Zn. However, the toxicity and transcriptomic responses in all MNP treatments cannot be fully explained by dissolved Zn. Two of the biological pathways identified, one essential for protein biosynthesis (Aminoacyl-tRNA biosynthesis) and another associated with detoxification (ABC transporters), were shared among pristine and one or both transformed ZnO-MNPs, but not ZnSO₄. When comparing pristine and transformed ZnO-MNPs, 66% and 40% of genes were shared between ZnO-MNPs and sZnO-MNPs or pZnO-MNPs, respectively. This suggests greater similarity in transcriptomic responses between ZnO-MNPs and sZnO-MNPs, while toxicity mechanisms are more distinct for pZnO-MNPs, where 13 unique biological pathways were identified. Based on these pathways, the toxicity of pZnO-MNPs is likely to be associated with their adverse effect on digestion and metabolism.
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