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Sorption and transport of aluminum dialkyl phosphinate flame retardants and their hydrolysates in soils
2019
Shi, Fengqiong | Hao, Zhineng | Liang, Yong | Liu, Jiyan | Liu, Jingfu
Aluminum dialkyl phosphinates (ADPs) are a class of promising phosphorus-containing flame retardants, but their environmental fate is not well understood. Sorption and transport behaviors of ADPs, and their hydrolysates dialkyl phosphinic acids (DPAs) were studied by batch and column experiments. ADPs are less mobile in soil columns with more than half (>52.6%) of ADPs retained in the soil and residues in the topmost 2-cm layer account for more than 57% of total residues. Dissolution and dispersion of fine grain ADPs were responsible for the transport of ADPs. Sorption DPAs (logKₒc) was significantly related to the lipophilicity of DPAs (logD) (p < 0.05). Soil pH and clay content were the dominant factors governing the sorption and transport of DPAs in soils, indicating the importance of electrostatic interactions. The retardation factors (R) of DPAs derived from leaching experiments were pH-dependent with larger R values in the acidic soil (pH = 4.0) where anionic and neutral species of DPAs coexisted. Both physical and chemical non-equilibrium convection-dispersion equations (CDE) yield appropriate modeling for DPAs transport. In most cases, R values estimated from column tests differed from those derived from the batch experiments, which might be attributed to non-equilibrium sorption processes in dynamic conditions.
Показать больше [+] Меньше [-]Atmospheric concentrations and trends of poly- and perfluoroalkyl substances (PFAS) and volatile methyl siloxanes (VMS) over 7 years of sampling in the Global Atmospheric Passive Sampling (GAPS) network
2018
Rauert, Cassandra | Shoieb, Mahiba | Schuster, Jasmin K. | Eng, Anita | Harner, Tom
Poly- and per-fluoroalkyl substances (PFAS) and volatile methyl siloxanes (VMS) were monitored at 21 sites in the Global Atmospheric Passive Sampling (GAPS) Network. Atmospheric concentrations previously reported from 2009 were compared to concentrations measured at these sites in 2013 and 2015, to assess trends over 7 years of monitoring. Concentrations of the fluorotelomer alcohols (FTOHs) and fluorinated sulfonamides and sulfonamidoethanols (FOSAs and FOSEs) were stable at these sites from 2009 to 2015 with no significant difference (p > 0.05) in concentrations. Elevated concentrations of all the neutral PFAS were detected at the urban sites as compared to the polar/background sites. The perfluorosulfonic acids (PFSAs), meanwhile, saw a significant increase (p < 0.001) in concentrations from 2009 to 2015. The perfluorocarboxylic acids (PFCAs) had elevated concentrations in 2015, however, the difference was not statistically significant (p > 0.05). Concentrations of the PFSAs and the PFCAs were similar at all location types, showing the global reach of these persistent compounds. Concentrations of the cyclic VMS (cVMS) were at least an order of magnitude higher than the linear VMS (lVMS) and the PFAS. Octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5) and dodecamethylcyclohexasiloxane (D6) saw a weak significant increase in concentrations from 2009 to 2013 (p < 0.05), however, hexamethylcyclotrisiloxane (D3) had a strong significant decrease in concentrations from 2009 to 2015 (p < 0.01).
Показать больше [+] Меньше [-]Source tagging modeling study of regional contributions to acid rain in summer over Liaoning Province, Northeastern China
2018
Gbaguidi, Alex E. | Wang, Zifa | Wang, Wei | Yang, Ting | Chen, Huan-Sheng
Strong acid rain was recently observed over Northeastern China, particularly in summer in Liaoning Province where alkaline dust largely neutralized acids in the past. This seems to be related to the regional transboundary pollution and poses new challenges in acid rain control scheme in China. In order to delve into the regional transport impact, and quantify its potential contributions to such an “eruption” of acid rain over Liaoning, this paper employs an online source tagging model in coupling with the Nested Air Quality Prediction Modeling System (NAQPMS). Validation of predictions shows the model capability in reproducing key meteorological and chemical features. Acid concentration over Liaoning is more pronounced in August (average of 0.087 mg/m³) with strong pollutant import from regional sources against significant depletion of basic species. Seasonal mean contributions from regional sources are assessed at both lower and upper boundary layers to elucidate the main pathways of the impact of regional sources on acid concentration over Liaoning. At the upper layer (1.2 km), regional sources contribute to acid concentration over Liaoning by 67%, mainly from Shandong (16%), Hebei (13%), Tianjin (11%) and Korean Peninsula (9%). Identified main city-receptors in Liaoning are Dandong, Dalian, Chaohu, Yingkou, Liaoyang, Jinfu, Shengyang, Panjin, Tieling, Benxi, Anshan and Fushun. At lower layer (120 m) where Liaoning local contribution is dominant (58%), regional sources account for 39% in acid concentration. However, inter-municipal acid exchanges are prominent at this layer and many cities in Liaoning are revealed as important sources of local acid production. Seasonal acid contribution average within 1.2 km-120 m attains 55%, suggesting dominance of vertical pollutant transport from regional sources towards lower boundary layer in Liaoning. As direct environmental implication, this study provides policy makers with a perspective of regulating the regional transboundary environmental impact assessment in China with application to acid rain control.
Показать больше [+] Меньше [-]Temporal-spatial distributions and ecological risks of perfluoroalkyl acids (PFAAs) in the surface water from the fifth-largest freshwater lake in China (Lake Chaohu)
2015
Liu, Wen-Xiu | He, Wei | Qin, Ning | Kong, Xiang-Zhen | He, Qi-Shuang | Yang, Bin | Yang, Chen | Jorgensen, Sven Erik | Xu, Fu-Liu
To investigate the residues, compositions, distributions and potential ecological risks of perfluoroalkyl acids (PFAAs), water samples were collected seasonally between August 2011 and November 2012 from 20 sites in Lake Chaohu and its tributary rivers. The mean concentration of total PFAAs (TPFAAs) was 14.46 ± 6.84 ng/L. PFOA was the predominant contaminant (8.62 ± 4.40 ng/L), followed by PFBA (2.04 ± 1.16 ng/L) and PFHxA (1.23 ± 1.50 ng/L). The TPFAAs concentrations peaked in August 2012 in each area, except for the western river. The opposite spatial trends were found for PFOA and PFOS in both the lake and river areas. Except for PFOS and PFUdA, the levels of TPFAAs and PFAAs were significantly related to the composition of fluorescent dissolved organic matter (FDOM) but not related to total DOM expressed by dissolved organic carbon (DOC). The risk of PFOS determined by a species sensitivity distribution model was notably above that of PFOA.
Показать больше [+] Меньше [-]The effect of nitrogen deposition on the species richness of acid grasslands in Denmark: A comparison with a study performed on a European scale
2011
Damgaard, Christian | Jensen, Lennarth | Frohn, Lise Marie | Borchsenius, F. (Finn) | Nielsen, Knud Erik | Ejrnæs, Rasmus | Stevens, Carly J.
The effect of atmospheric nitrogen deposition on the species richness of acid grasslands was investigated by combining data from a large Danish monitoring program with a large European data set, where a significant non-linear negative effect of nitrogen deposition had been demonstrated (Stevens et al., 2010). The nitrogen deposition range in Denmark is relatively small and when only considering the Danish data a non-significant decrease in the species richness with nitrogen deposition was observed. However, when both data sets were combined, then the conclusion of the European survey was further corroborated by the results of the Danish monitoring. Furthermore, by combining the two data sets a more comprehensive picture of the threats to the biodiversity of acid grasslands emerge; i.e., species richness in remnant patches of acid grassland in intensively cultivated agricultural landscapes is under influence not only from nitrogen deposition, but also from current and historical land use.
Показать больше [+] Меньше [-]Seasonal variation and source estimation of organic compounds in urban aerosol of Augsburg, Germany
2011
Pietrogrande, Maria Chiara | Abbaszade, Gülcin | Schnelle-Kreis, Jürgen | Bacco, Dimitri | Mercuriali, Mattia | Zimmermann, Ralf
This study reports a general assessment of the organic composition of the PM₂.₅ samples collected in the city of Augsburg, Germany in a summer (August–September 2007) and a winter (February–March 2008) campaign of 36 and 30 days, respectively. The samples were directly submitted to in-situ derivatisation thermal desorption gas chromatography coupled with time of flight mass spectrometry (IDTD–GC–TOFMS) to simultaneously determine the concentrations of many classes of molecular markers, such as n-alkanes, iso- and anteiso-alkanes, polycyclic aromatic hydrocarbons (PAHs), oxidized PAHs, n-alkanoic acids, alcohols, saccharides and others. The PCA analysis of the data identified the contributions of three emission sources, i.e., combustion sources, including fossil fuel emissions and biomass burning, vegetative detritus, and oxidized PAHs. The PM chemical composition shows seasonal trend: winter is characterized by high contribution of petroleum/wood combustion while the vegetative component and atmospheric photochemical reactions are predominant in the hot season.
Показать больше [+] Меньше [-]Identification of perfluoroalkyl acid sources in Swiss surface waters with the help of the artificial sweetener acesulfame
2011
Müller, Claudia E. | Gerecke, Andreas C. | Alder, Alfredo C. | Scheringer, Martin | Hungerbühler, Konrad
Anthropogenic perfluorinated compounds (PFCs), especially the perfluoroalkyl acids (PFAAs) are ubiquitously found in surface waters around the globe. Emissions from households, industries and also atmospheric transport/deposition are discussed as the possible sources. In this study, these sources are evaluated using Switzerland as the study area. Forty-four surface water locations in different rivers and an Alpine lake were investigated for 14 PFAAs, four precursors and acesulfame, an artificial sweetener used as a population marker. Concentrations of individual PFAAs were generally low, between 0.02 and 10 ng/L. Correlation analysis showed that some PFAAs concentrations correlated well with population and less with catchment area, indicating that emissions from population, i.e., from consumer products, is the most important source to surface waters in Switzerland. The correlation with the population marker acesulfame confirmed this observation but highlighted also a few elevated PFAA levels, some of which could be attributed to industrial emissions.
Показать больше [+] Меньше [-]Long term remediation of highly polluted acid mine drainage: A sustainable approach to restore the environmental quality of the Odiel river basin
2011
Caraballo, Manuel A. | Macías, Francisco | Rötting, Tobias S. | Nieto, José Miguel | Ayora, Carlos
During 20 months of proper operation the full scale passive treatment in Mina Esperanza (SW Spain) produced around 100 mg/L of ferric iron in the aeration cascades, removing an average net acidity up to 1500 mg/L as CaCO₃ and not having any significant clogging problem. Complete Al, As, Cd, Cr, Cu, Ti and V removal from the water was accomplished through almost the entire operation time while Fe removal ranged between 170 and 620 mg/L. The system operated at a mean inflow rate of 43 m³/day achieving an acid load reduction of 597 g·(m² day)⁻¹, more than 10 times higher than the generally accepted 40 g·(m² day)⁻¹ value commonly used as a passive treatment system designing criteria. The high performance achieved by the passive treatment system at Mina Esperanza demonstrates that this innovative treatment design is a simple, efficient and long lasting remediation option to treat highly polluted acid mine drainage.
Показать больше [+] Меньше [-]Biogeochemical dynamics of perfluorinated alkyl acids and sulfonates in the River Seine (Paris, France) under contrasting hydrological conditions
2011
Labadie, Pierre | Chevreuil, Marc
The biogeochemical dynamics of 15 perfluorinated compounds (PFCs) were investigated in a heavily urbanised river (River Seine, Paris, France). The target compounds included C4-C10 sulfonates and C5-C14 acids; eleven PFCs were detected and ∑PFCs ranged between 31 and 91 ng L⁻¹ (median: 47 ng L⁻¹). The molecular pattern was dominated by the perfluoroalkyl sulfonates PFHxS and PFOS (>54% of ∑PFCs), which were the only PFCs quantified in both the dissolved and particulate phases. For these PFCs, the sorbed fraction positively correlated with suspended sediment levels. Total PFC levels negatively correlated with river flow rate, which varied between 150 and 640 m³ s⁻¹. This suggests the predominance of point sources (likely WWTP effluent discharge), but a contribution of non-point sources such as combined sewer overflow could not be excluded. The annual PFC mass flow was estimated at 500 kg, which is less than observed for other large European rivers.
Показать больше [+] Меньше [-]Copper availability and bioavailability are controlled by rhizosphere pH in rape grown in an acidic Cu-contaminated soil
2009
Chaignon, Valérie | Quesnoit, Marie | Hinsinger, Philippe
We evaluated how root-induced changes in rhizosphere pH varied and interacted with Cu availability and bioavailability in an acidic soil. Rape was grown on a Cu-contaminated acidic soil, which had been limed at 10 rates. Soil Cu bioavailability was not influenced by liming. However, liming significantly decreased CaCl2–extracted Cu for pH between 3.7 and 5.1. Little effect was found for pH above 5.1. For soil pH < 4.4, CaCl2–Cu contents were smaller in rhizosphere than uncropped soil. Rhizosphere alkalisation occurred at pH < 4.8, while acidification occurred at greater pH. This explained the changes of CaCl2–Cu in the rhizosphere at low pH and the absence of pH dependency of Cu bioavailability to rape. In addition, apoplastic Cu in roots increased with increasing soil pH, most probably as a result of increased dissociation and affinity of cell wall compounds for Cu. Root-induced increase in pH reduces Cu availability in the rhizosphere and Cu bioavailability to rape.
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