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Adsorption and oxidation of 3-nitro-1,2,4-triazole-5-one (NTO) and its transformation product (3-amino-1,2,4-triazole-5-one, ATO) at ferrihydrite and birnessite surfaces Texto completo
2018
Khatiwada, Raju | Abrell, Leif | Li, Guangbin | Root, Robert A. | Sierra-Alvarez, Reyes | Field, James A. | Chorover, Jon
The emerging insensitive munitions compound (IMC) 3-nitro-1,2,4-triazole-5-one (NTO) is currently being used to replace conventional explosives such as 1,3,5-trinitro-1,3,5-triazacyclohexane (RDX), but the environmental fate of this increasingly widespread IMC remains poorly understood. Upon release from unexploded solid phase ordinances, NTO exhibits high aqueous solubility and, hence, potential mobilization to groundwater. Adsorption and abiotic transformation at metal oxide surfaces are possible mechanisms for natural attenuation. Here, the reactions at ferrihydrite and birnessite surfaces of NTO and its biotransformation product, 3-amino-1, 2, 4-triazol-5-one (ATO), were studied in stirred batch reactor systems at controlled pH (7.0). The study was carried out at metal oxide solid to solution ratios (SSR) of 0.15, 1.5 and 15 g kg−1. The samples were collected at various time intervals up to 3 h after reaction initiation, and analyzed using HPLC with photodiode array and mass spectrometric detection. We found no detectable adsorption or transformation of NTO upon reaction with birnessite, whereas ATO was highly susceptible to oxidation by the same mineral, showing nearly complete transformation within 5 min at 15 g kg−1 SSR to urea, CO2(g) and N2(g). The mean surface-area-normalized pseudo-first order rate constant (k) for ATO oxidation by birnessite across all SSRs was 0.05 ± 0.022 h−1 m−2, and oxidation kinetics were independent of dissolved O2 concentration. Both NTO and ATO were resistant to oxidation by ferrihydrite. However, NTO showed partial removal from solution upon reaction with ferrihydrite at 0.15 and 1.5 g kg−1 SSR and complete loss at 15 g kg−1 SSR due to strong adsorption. Conversely, ATO adsorption to ferrihydrite was much weaker than that measured for NTO.
Mostrar más [+] Menos [-]Geochemistry and carbon isotopic ratio for assessment of PM10 composition, source and seasonal trends in urban environment Texto completo
2018
Di Palma, A. | Capozzi, F. | Agrelli, D. | Amalfitano, C. | Giordano, S. | Spagnuolo, V. | Adamo, P.
Investigating the nature of PM₁₀ is crucial to differentiate sources and their relative contributions. In this study we compared the levels, and the chemical and mineralogical properties of PM₁₀ particles sampled in different seasons at monitoring stations representative of urban background, urban traffic and suburban traffic areas of Naples city. The aims were to relate the PM₁₀ load and characteristics to the location of the monitoring stations, to investigate the different sources contributing to PM₁₀ and to highlight PM₁₀ seasonal variability. Bulk analyses of chemical species in the PM₁₀ fraction included total carbon and nitrogen, δ¹³C and other 20 elements. Both natural and anthropogenic sources were found to contribute to the exceedances of the EU PM₁₀ limit values. The natural contribution was mainly related to marine aerosols and soil dust, as highlighted by X-ray diffractometry and SEM-EDS microscopy. The percentage of total carbon suggested a higher contribution of biogenic components to PM₁₀ in spring. However, this result was not supported by the δ¹³C values which were seasonally homogeneous and not sufficient to extract single emission sources. No significant differences, in terms of PM₁₀ load and chemistry, were observed between monitoring stations with different locations, suggesting a homogeneous distribution of PM₁₀ on the studied area in all seasons. The anthropogenic contribution to PM₁₀ seemed to dominate in all sites and seasons with vehicular traffic acting as a main source mostly by generation of non-exhaust emissions Our findings reinforce the need to focus more on the analysis of PM₁₀ in terms of quality than of load, to reconsider the criteria for the classification and the spatial distribution of the monitoring stations within urban and suburban areas, with a special attention to the background location, and to emphasize all the policies promoting sustainable mobility and reduction of both exhaust and not-exhaust traffic-related emissions.
Mostrar más [+] Menos [-]The simultaneous capture of mercury and fine particles by hybrid filter with powder activated carbon injection Texto completo
2018
Jang, Ha-Na | Back, Seung-Ki | Sung, Jin-Ho | Kang, Youn-Suk | Jurng, Jongsoo | Seo, Yong-Chil
The hybrid filter (HF) was newly designed and operated with powder activated carbon (PAC) injection to capture mercury and fine particulate matter in the coal power plant. With PAC injection in HF operation, the capture efficiency of elemental mercury was clearly enhanced. When the injection rate of PAC increased from 0 to 20 mg/m3, the speciation fraction of elemental mercury significantly decreased from 85.19% to 3.76% at the inlet of the hybrid filter. The speciation fraction of oxidized mercury did not vary greatly, whereas the particulate mercury increased from 1.31% to 94.04%. It was clearly observed that the HF played a role in the capture of mercury and fine PM by leading the conversion of elemental mercury as particulate mercury and the growth of PM via electrode discharge in the HF operation with PAC injection.
Mostrar más [+] Menos [-]2,3,7,8-Tetrachlorodibenzo-p-dioxin induces alterations in myogenic differentiation of C2C12 cells Texto completo
2018
Xie, Heidi Q. | Xia, Yingjie | Xu, Tuan | Chen, Yangsheng | Fu, Hualing | Li, Yunping | Luo, Yali | Xu, Li | Tsim, Karl W.K. | Zhao, Bin
Dioxin-induced toxicities that affect the development of the motor system have been proposed since many years. However, cellular evidence and the molecular basis for the effects are limited. In this study, a cultured mouse myoblast cell line, C2C12, was utilized to examine the effects of 2,3,7,8-tetrachlorodibenzo-p-dioxin (TCDD) on myogenic differentiation and expression of acetylcholinesterase (AChE), a neuromuscular transmission-related gene. The results showed that TCDD exposure at 10⁻¹⁰ M repressed the myotube formation of C2C12 cells by disturbing the fusion process and suppressing the expression of myosin heavy chain, a myobute structural protein, and not by induction of cytotoxicity. Furthermore, TCDD dose dependently suppressed the transcriptional expression and enzymatic activity of AChE during the myogenic differentiation, particularly in the middle stage. However, the administration of aryl hydrocarbon receptor antagonists, CH223191 and alpha-naphthoflavone, did not completely reverse the TCDD-induced downregulation of muscular AChE during myogenic differentiation. These findings suggest that low dose exposure to dioxin may result in disturbances of muscle differentiation and neuromuscular transmission.
Mostrar más [+] Menos [-]Occurrence, sources and transport of antibiotics in the surface water of coral reef regions in the South China Sea: Potential risk to coral growth Texto completo
2018
Zhang, Ruijie | Zhang, Ruiling | Yu, Kefu | Wang, Yinghui | Huang, Xueyong | Pei, Jiying | Wei, Chaoshuai | Pan, Ziliang | Qin, Zhenjun | Zhang, Gan
Laboratory research has indicated that antibiotics had negative effects on coral growth by disturbing natural microbiota; however, no field studies have reported antibiotic contamination levels and their influence on coral growth in natural coral reef regions (CRRs). This study investigated antibiotic occurrence and sources in the surface water from CRRs that have suffered from rapid coral degradation and evaluated their risk to coral growth. These regions are in the South China Sea, including four coastal and two offshore CRRs. The results show that 13 antibiotics were detected in the coastal CRRs with concentrations ranging from 10⁻²–10⁰ ng L⁻¹, while 5 antibiotics occurred in offshore CRRs (300–950 km from the mainland), with concentrations ranging from 10⁻² to 10⁻¹ ng L⁻¹. Their concentrations decreased gradually from the coast to offshore in the transport process. However, Yongxing Island, which is approximately 300 km from the mainland, was an exception with relatively higher concentrations than the surrounding reefs because of the ever-increasing human activity on the island. The presence of anthropogenic contaminants antibiotics in CRRs may be a potential risk to coral growth.
Mostrar más [+] Menos [-]Influence of traffic on build-up of polycyclic aromatic hydrocarbons on urban road surfaces: A Bayesian network modelling approach Texto completo
2018
Li, Yingxia | Jia, Ziliang | Wijesiri, Buddhi | Song, Ningning | Goonetilleke, Ashantha
Due to their carcinogenic effects, Polycyclic Aromatic Hydrocarbons (PAHs) deposited on urban surfaces are a major concern in the context of stormwater pollution. However, the design of effective pollution mitigation strategies is challenging due to the lack of reliability in stormwater quality modelling outcomes. Current modelling approaches do not adequately replicate the interdependencies between pollutant processes and their influential factors. Using Bayesian Network modelling, this research study characterised the influence of vehicular traffic on the build-up of the sixteen US EPA classified priority PAHs. The predictive analysis was conditional on the structure of the proposed BN, which can be further improved by including more variables. This novel modelling approach facilitated the characterisation of the influence of traffic as a source of origin and also as a key factor that influences the re-distribution of PAHs, with positive or negative relationship between traffic volume and PAH build-up. It was evident that the re-distribution of particle-bound PAHs is determined by the particle size rather than the chemical characteristics such as volatility. Moreover, compared to commercial and residential land uses, mostly industrial land use contributes to the PAHs load released to the environment. Carcinogenic PAHs in industrial areas are likely to be associated with finer particles, while PAHs, which are not classified as human carcinogens, are likely to be found in the coarser particle fraction.
Mostrar más [+] Menos [-]Measurement of methane emission into environment during natural gas purging process Texto completo
2018
Farzaneh-Gord, Mahmood | Pahlevan-Zadeh, Mohammad Sadegh | Ebrahimi-Moghadam, Amir | Rastgar, Saied
The main purpose of this study is to develop accurate equation for predicting methane emission into the environment during natural gas (NG) purging process. The process is carried out regularly in NG pressure reducing stations. For this purpose, a numerical investigation has been carried out to simulate NG exit flow from a purging valve during opening time. The simulation has been carried out using Ansys-Fluent code. To make the solution and results more similar to actual scenario, the valve is continuously opened in a transient turbulent flow. Initial condition, is assumed steady flow in the pipeline. Three-dimensional modeling is used to simulate the valve and connected pipe, and all of the effective parameters including, inlet pressure, pipeline diameter, valve diameter and purging process time (including the time which valve needs to get completely opened and also purging time) are investigated. For simplicity and also as the main component of NG is methane, methane is considered as working fluid (a real compressible gas). The numerical results show that discharging gas velocity is reached to a supersonic velocity at outlet section of valve. As the highest expected exit velocity is sonic velocity, the supersonic velocity is a surprised result. Looking at the streamlines show that this is due to a convergent-divergent nozzle occurrence (due to re-circulation zone near junction) in discharging pipe. Also results show that discharged mass flow rate has liner relation with pipeline pressure, second degree relation with valve diameter and has fourth-degree relation with valve to pipeline diameter ratio. To make the results more applicable for NG industry, two correlations have been developed for calculating the amount of released gas in steady state and unsteady state condition. Unsteady state correlation is valid for valve opening time and steady state correlation could be used while the valve is completely opened.
Mostrar más [+] Menos [-]Satellite-based high-resolution PM2.5 estimation over the Beijing-Tianjin-Hebei region of China using an improved geographically and temporally weighted regression model Texto completo
2018
He, Qingqing | Huang, Bo
Ground fine particulate matter (PM2.5) concentrations at high spatial resolution are substantially required for determining the population exposure to PM2.5 over densely populated urban areas. However, most studies for China have generated PM2.5 estimations at a coarse resolution (≥10 km) due to the limitation of satellite aerosol optical depth (AOD) product in spatial resolution. In this study, the 3 km AOD data fused using the Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 6 AOD products were employed to estimate the ground PM2.5 concentrations over the Beijing-Tianjin-Hebei (BTH) region of China from January 2013 to December 2015. An improved geographically and temporally weighted regression (iGTWR) model incorporating seasonal characteristics within the data was developed, which achieved comparable performance to the standard GTWR model for the days with paired PM2.5- AOD samples (Cross-validation (CV) R2 = 0.82) and showed better predictive power for the days without PM2.5- AOD pairs (the R2 increased from 0.24 to 0.46 in CV). Both iGTWR and GTWR (CV R2 = 0.84) significantly outperformed the daily geographically weighted regression model (CV R2 = 0.66). Also, the fused 3 km AODs improved data availability and presented more spatial gradients, thereby enhancing model performance compared with the MODIS original 3/10 km AOD product. As a result, ground PM2.5 concentrations at higher resolution were well represented, allowing, e.g., short-term pollution events and long-term PM2.5 trend to be identified, which, in turn, indicated that concerns about air pollution in the BTH region are justified despite its decreasing trend from 2013 to 2015.
Mostrar más [+] Menos [-]Multibiomarker interactions to diagnose and follow-up chronic exposure of a marine crustacean to Hazardous and Noxious Substances (HNS) Texto completo
2018
Abreu, Isabel Oliveira | Monteiro, Catarina | Rocha, A. Cristina S. | Reis-Henriques, Maria Armanda | Teixeira, Catarina | Basto, Maria Clara Pires | Ferreira, Marta | Almeida, C. Marisa R. | Oliva-Teles, Luís | Guimarães, Laura
Multibiomarker interactions to diagnose and follow-up chronic exposure of a marine crustacean to Hazardous and Noxious Substances (HNS) Texto completo
2018
Abreu, Isabel Oliveira | Monteiro, Catarina | Rocha, A. Cristina S. | Reis-Henriques, Maria Armanda | Teixeira, Catarina | Basto, Maria Clara Pires | Ferreira, Marta | Almeida, C. Marisa R. | Oliva-Teles, Luís | Guimarães, Laura
Integrated compensatory responses of physiological systems towards homeostasis are generally overlooked when it comes to analysing alterations in biochemical parameters indicative of such processes. Here an hypothesis-driven multivariate analysis accounting for interactive multibiomarker responses was used to investigate effects of long-term exposure of Carcinus maenas to Hazardous and Noxious Substances (HNS). Adult male crabs were exposed to low and high post-spill levels of acrylonitrile (ACN) or aniline (ANL) for 21d. Bioaccumulation, feeding behaviour, and biomarkers related to mode-of-action (MoA) (detoxification, neurotransmission and energy production) were evaluated over time. Distinct temporal patterns of response to low and high exposure concentrations were depicted, with a main set of interactive multibiomarker predictors identified for each HNS (five for ACN and three for ANL), useful to follow coupled evolvement of biomarker responses. ACN caused peripheral neurotoxic effects coupled with enhanced biotransformation and significant oxidative damage particularly relevant in gills. ANL elicited alterations in central neurotransmission affecting ventilation coupled with very low levels of oxidative damage in gills. Results indicate chronic toxicity data are determinant to improve HNS hazard assessment if the aim is to obtain reliable risk calculations, and develop effective predictive models avoiding overestimation but sufficiently protective. Accounting for multibiomarker interactions brought otherwise overlooked information about C. maenas responses and MoA of ACN and ANL.
Mostrar más [+] Menos [-]Multibiomarker interactions to diagnose and follow-up chronic exposure of a marine crustacean to Hazardous and Noxious Substances (HNS) Texto completo
2018
Abreu I.O. | Monteiro C. | Rocha A.C.S. | Reis-Henriques M.A. | Teixeira C. | Basto M.C.P. | Ferreira M. | Almeida C.M.R. | Oliva-Teles L. | Guimarães L. | CIIMAR - Centro Interdisciplinar de Investigação Marinha e Ambiental
Integrated compensatory responses of physiological systems towards homeostasis are generally overlooked when it comes to analysing alterations in biochemical parameters indicative of such processes. Here an hypothesis-driven multivariate analysis accounting for interactive multibiomarker responses was used to investigate effects of long-term exposure of Carcinus maenas to Hazardous and Noxious Substances (HNS). Adult male crabs were exposed to low and high post-spill levels of acrylonitrile (ACN) or aniline (ANL) for 21d. Bioaccumulation, feeding behaviour, and biomarkers related to mode-of-action (MoA) (detoxification, neurotransmission and energy production) were evaluated over time. Distinct temporal patterns of response to low and high exposure concentrations were depicted, with a main set of interactive multibiomarker predictors identified for each HNS (five for ACN and three for ANL), useful to follow coupled evolvement of biomarker responses. ACN caused peripheral neurotoxic effects coupled with enhanced biotransformation and significant oxidative damage particularly relevant in gills. ANL elicited alterations in central neurotransmission affecting ventilation coupled with very low levels of oxidative damage in gills. Results indicate chronic toxicity data are determinant to improve HNS hazard assessment if the aim is to obtain reliable risk calculations, and develop effective predictive models avoiding overestimation but sufficiently protective. Accounting for multibiomarker interactions brought otherwise overlooked information about C. maenas responses and MoA of ACN and ANL. Accounting for biomarker interactions drastically improves the quality of the model to diagnose toxic effects. © 2018 Elsevier | This article is a result of INNOVMAR - Innovation and Sustainability in the Management and Exploitation of Marine Resources (reference NORTE-01-0145-FEDER-000035), ECOSERVICES, supported by NORTE2020, PORTUGAL2020 Partnership Agreement, through ERDF . This work was partially funded by Strategic Funding UID/Multi/04423/2013 through FCT and ERDF .
Mostrar más [+] Menos [-]Baseline characterisation of source contributions to daily-integrated PM2.5 observations at Cape Grim using Radon-222 Texto completo
2018
Crawford, Jagoda | Chambers, Scott D. | Cohen, David D. | Williams, Alastair G. | Atanacio, Armand
We discuss 15 years (2000–2015) of daily-integrated PM₂.₅ samples from the Cape Grim Station. Ion beam analysis and positive matrix factorisation are used to identify six source-type fingerprints: fresh sea salt (57%); secondary sulfate (14%); smoke (13%); aged sea salt (12%); soil dust (2.4%); and industrial metals (1.5%). An existing hourly radon-only baseline selection technique is modified for use with the daily-integrated observations. Results were not significantly different for days on which >20 hours were below the baseline radon threshold compared with days when all 24 hours satisfied the baseline criteria. This relaxed daily baseline criteria increased the number of samples for analysis by almost a factor of two. Two radon baseline thresholds were tested: historic (100 mBq m⁻³), and revised (50 mBq m⁻³). Median aerosol concentrations were similar for both radon thresholds, but maximum values were higher for the 100 mBq m⁻³ threshold. Back trajectories indicated more interaction with southern Australia and the Antarctic coastline for air masses selected with the 100 mBq m⁻³ threshold. Radon-only baseline selection using the 50 mBq m⁻³ threshold was more selective of minimal terrestrial influence than a similar recent study using wind direction and back trajectories. The ratio of concentrations between terrestrial and baseline days for the primary sources soil, smoke and industrial metals was 3.4, 2.6, and 5.5, respectively. Seasonal cycles of soil dust had a summer maximum and winter minimum. Seasonal cycles of smoke were of similar amplitude for terrestrial and baseline events, but of completely different shape: peaking in autumn and spring for terrestrial events, compared to summer for baseline conditions. Seasonal cycles of industrial metals had a summer maximum and winter minimum. A significant fraction of the Cape Grim baseline smoke and industrial metal contributions appeared to be derived from long-term transport (>3 weeks since last terrestrial influence).
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