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Physicochemical factors affecting the spatial variance of monomethylmercury in artificial reservoirs
2016
Noh, Seam | Kim, Chan-Kook | Lee, Jong Hyeon | Kim, Younghee | Choi, Kyunghee | Han, Seunghee
The aim of this study was to identify how hydrologic factors (e.g., rainfall, maximum depth, reservoir and catchment area, and water residence time) and water chemistry factors (e.g., conductivity, pH, suspended particulate matter, chlorophyll-a, dissolved organic carbon, and sulfate) interact to affect the spatial variance in monomethylmercury (MMHg) concentration in nine artificial reservoirs. We hypothesized that the MMHg concentration of reservoir water would be higher in eutrophic than in oligotrophic reservoirs because increased dissolved organic matter and sulfate in eutrophic reservoirs can promote in situ production of MMHg. Multiple tools, including Pearson correlation, a self-organizing map, and principal component analysis, were applied in the statistical modeling of Hg species. The results showed that rainfall amount and hydraulic residence time best explained the variance of dissolved Hg and dissolved MMHg in reservoir water. High precipitation events and residence time may mobilize Hg and MMHg in the catchment and reservoir sediment, respectively. On the contrary, algal biomass was a key predictor of the variance of the percentage fraction of unfiltered MMHg over unfiltered Hg (%MMHg). The creation of suboxic conditions and the supply of sulfate subsequent to the algal decomposition seemed to support enhanced %MMHg in the bloom reservoirs. Thus, the nutrient supply should be carefully managed to limit increases in the %MMHg/Hg of temperate reservoirs.
Показать больше [+] Меньше [-]Adsorption and desorption of dissolved organic matter by carbon nanotubes: Effects of solution chemistry
2016
Engel, Maya | Chefetz, Benny
Increasing use of carbon nanotubes (CNTs) has led to their introduction into the environment where they can interact with dissolved organic matter (DOM). This study focuses on solution chemistry effects on DOM adsorption/desorption processes by single-walled CNTs (SWCNTs). Our data show that DOM adsorption is controlled by the attachment of DOM molecules to the SWCNTs, and that the initial adsorption rate is dependent on solution parameters. Adsorbed amount of DOM at high ionic strength was limited, possibly due to alterations in SWCNT bundling. Desorption of DOM performed at low pH resulted in additional DOM adsorption, whereas at high pH, adsorbed DOM amount decreased. The extent of desorption conducted at increased ionic strength was dependent on pre-adsorbed DOM concentration: low DOM loading stimulated additional adsorption of DOM, whereas high DOM loading facilitated release of adsorbed DOM. Elevated ionic strength and increased adsorbed amount of DOM reduced the oxidation temperature of the SWCNTs, suggesting that changes in the assembly of the SWCNTs had occurred. Moreover, DOM-coated SWCNTs at increased ionic strength provided fewer sites for atrazine adsorption. This study enhances our understanding of DOM–SWCNT interactions in aqueous systems influenced by rapid changes in salinity, and facilitates potential use of SWCNTs in water-purification technologies.
Показать больше [+] Меньше [-]Detachment of fullerene nC60 nanoparticles in saturated porous media under flow/stop-flow conditions: Column experiments and mechanistic explanations
2016
Wang, Zhan | Wang, Dengjun | Li, Baoguo | Wang, Jizhong | Li, Tiantian | Zhang, Mengjia | Huang, Yuanfang | Shen, Chongyang
This study was aimed at investigating the detachment of fullerene nC60 nanoparticles (NPs) in saturated sand porous media under transient and static conditions. The nC60 NPs were first attached at primary minima of Derjaguin–Landau–Verwey–Overbeek (DLVO) interaction energy profiles in electrolyte solutions with different ionic strengths (ISs). The columns were then eluted with deionized water to initiate nC60 NP detachment by decreasing solution IS. Finally, the flow of the columns was periodically interrupted to investigate nC60 NP detachment under static condition. Our results show that the detachment of nC60 NPs occurred under both transient and static conditions. The detachment under transient conditions was attributed to the fact that the attractions acting on the nC60 NPs at primary minima were weakened by nanoscale physical heterogeneities and overcome by hydrodynamic drags at lower ISs. However, a fraction of nC60 NPs remained at shallow primary minima in low flow regions, and detached via Brownian diffusion during flow interruptions. Greater detachment of nC60 NPs occurred under both transient and static conditions if the NPs were initially retained in electrolyte solutions with lower valent cations due to lower attractions between the NPs and collectors. Decrease in collector surface chemical heterogeneities and addition of dissolved organic matter also increased the extent of detachment by increasing electrostatic and steric repulsions, respectively. While particle attachment in and subsequent detachment from secondary minima occur in the same electrolyte solution, our results indicate that perturbation in solution chemistry is necessary to lower the primary minimum depths to initiate spontaneous detachment from the primary minima. These findings have important implications for predicting the fate and transport of nC60 NPs in subsurface environments during multiple rainfall events and accordingly for accurately assessing their environmental risks.
Показать больше [+] Меньше [-]Bioconcentration of perfluoroalkyl substances by Chironomus plumosus larvae in water with different types of dissolved organic matters
2016
Wen, Wu | Xia, Xinghui | Chen, Xi | Wang, Haotian | Zhu, Baotong | Li, Husheng | Li, Yang
The effects of four types of dissolved organic matters (DOM) on the bioconcentration of perfluoroalkyl substances (PFASs) in Chironomus plumosus larvae have been studied. The PFASs included perfluorooctane sulfonate (PFOS), perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA), perfluorodecanoic acid (PFDA), perfluoroundecanoic acid (PFUnA), and perfluorododecanoic acid (PFDoA). The DOM included humic acid (HA), fulvic acid (FA), tannic acid (TA), and a protein, peptone (PEP), and their concentrations ranged from 0 to 50 mg L−1. The results showed that, upon bioconcentration equilibrium, the body burdens of longer perfluoroalkyl chain PFASs (PFOS, PFDA, PFUnA and PFDoA) decreased with PEP and HA concentrations while increased with FA and TA concentrations. When FA and TA concentrations increased from 0 to 50 mg L−1, body burdens of these PFASs increased by 7.5%–148.8% and 5.7%–37.1%, respectively. However, the DOM had no significant impact on the body burdens of shorter perfluoroalkyl chain PFASs (PFOA and PFNA). All of the four types of DOM lowered not only the uptake rate constants (ku) of PFASs due to the decrease of freely dissolved PFAS concentrations, but also the elimination rate constants (ke) due to the inhibition effect of DOM on the PFAS elimination from the larvae. The reduction in the two constants varied with both DOM and PFAS types. In the presence of PEP and HA with larger molecular weights, the ku values decreased more than ke, leading to the decreased body burdens of longer perfluoroalkyl chain PFASs. As for FA and TA with smaller molecular weights, the ke values decreased more than ku, resulting in increased body burdens of longer perfluoroalkyl chain PFASs. This study suggests that the effects of DOM on PFAS bioconcentration depend not only on the concentration but also on the molecule weight of DOM, which should be considered in the bioavailability assessment of PFASs.
Показать больше [+] Меньше [-]Suspension stability and aggregation of multi-walled carbon nanotubes as affected by dissolved organic matters extracted from agricultural wastes
2016
Li, Helian | Qiu, Yanhua | Wang, Xiaonuan | Liu, Wenhao | Chen, Guangcai | Ma, Yibing | Xing, Baoshan
Dissolved organic matters (DOMs) extracted from wheat straw (SDOM) and cow manure (MDOM) were used to investigate their effects on the suspension stability and aggregation of multi-walled carbon nanotubes (MWCNTs). Two types of DOM can effectively disperse and stabilize the MWCNTs. At initial MWCNT concentration of 500 mg/L, suspended MWCNT concentration ranged from 8.0 to 17.9 mg/L as DOM were varied from 50 to 200 mg/L dissolved organic carbon (DOC). The critical coagulation concentration (CCC) values were estimated to be 41.4 mM NaCl and 5.3 mM CaCl2 in the absence of DOM. The presence of SDOM and MDOM significantly retarded the aggregation rate of MWCNTs. The CCC values increased to 120 mM NaCl and 14.8 mM CaCl2 at SDOM concentration of 20 mg/L DOC. Due to its higher aromaticity and molecular weight, MDOM showed higher ability to stabilize MWCNTs, with CCC values of 201 mM and 15.8 mM at 20 mg/L DOC. These findings revealed that DOMs originated from agricultural wastes will have great impact on the dispersion and stabilization of MWCNTs, thus their fate in the aquatic environment.
Показать больше [+] Меньше [-]Evaluation of free/labile concentrations of trace metals in Athabasca oil sands region streams (Alberta, Canada) using diffusive gradient in thin films and a thermodynamic equilibrium model
2016
Zhu, Y. | Guéguen, C.
The Athabasca's oil sands exploitation is controversial due to its potential risks to water quality but little is known about the temporal changes in the most bioavailable fraction of metal, the free/labile species. In this study, diffusive gradient in thin films (DGT) and the Windermere Humic Aqueous Model (WHAM VII) equilibrium model were used to examine the temporal changes in free/labile metal (Cu, Ni, Zn, Pb) species in three tributaries of the north-flowing Athabasca River in the Athabasca oil sands region (AOSR). The influence of dissolved organic matter (DOM) composition (i.e. fulvic: humic ratio) on modeled Cu and Ni speciation showed a negligible effect on the labile concentration. The best agreements (92 ± 8%) between DGT-labile and WHAM calculated labile concentrations were found assuming the formation of iron oxyhydroxides (FeO(OH)). The agreement was only 70 ± 7% in the presence of inorganic colloidal aluminum oxyhydroxides (AlO(OH)) and in the absence of any inorganic colloids. Together these results suggest that a change in DOM composition had limited impacts on modeled free metal ion concentrations. Although the concentration of the main metal ligand (i.e. DOM), varied from 9 to 40 ppm, no significant temporal differences in the abundance of WHAM-modeled labile species were found, suggesting mobility and bioavailability of Cu, Ni, Pb and Zn were comparable over the 2003–2012 period.
Показать больше [+] Меньше [-]Transport of organic contaminants in subsoil horizons and effects of dissolved organic matter related to organic waste recycling practices
2016
Chabauty, Florian | Pot-Genty, Valerie | Deschamps, Marjolaine | Bernet, Nathalie | Labat, Christophe | Benoit, Pierre | Ecologie fonctionnelle et écotoxicologie des agroécosystèmes (ECOSYS) ; Institut National de la Recherche Agronomique (INRA)-AgroParisTech | Université Paris-Saclay | European Commission [226536]; Ile-de-France region; Veolia Environment group Funding Text : The work was carried as part of the GENESIS project on groundwater systems financed by the European Commission 7thFP contract 226536. The authors also acknowledge the Ile-de-France region for funding for ultra-performance liquid chromatography/MS-MS analyses, and the useful help of Jean-Noel Rampon for field sampling. Finally, we acknowledge the Veolia Environment group for the financial support of the QualiAgro field site.
Compost amendment on agricultural soil is a current practice to compensate the loss of organic matter. As a consequence, dissolved organic carbon concentration in soil leachates can be increased and potentially modify the transport of other solutes. This study aims to characterize the processes controlling the mobility of dissolved organic matter (DOM) in deep soil layers and their potential impacts on the leaching of organic contaminants (pesticides and pharmaceutical compounds) potentially present in cultivated soils receiving organic waste composts. We sampled undisturbed soil cores in the illuviated horizon (60-90 cm depth) of an Albeluvisol. Percolation experiments were made in presence and absence of DOM with two different pesticides, isoproturon and epoxiconazole, and two pharmaceutical compounds, ibuprofen and sulfamethoxazole. Two types of DOM were extracted from two different soil surface horizons: one sampled in a plot receiving a co-compost of green wastes and sewage sludge applied once every 2 years since 1998 and one sampled in an unamended plot. Results show that DOM behaved as a highly reactive solute, which was continuously generated within the soil columns during flow and increased after flow interruption. DOM significantly increased the mobility of bromide and all pollutants, but the effects differed according the hydrophobic and the ionic character of the molecules. However, no clear effects of the origin of DOM on the mobility of the different contaminants were observed.
Показать больше [+] Меньше [-]A surface tension based method for measuring oil dispersant concentration in seawater
2016
Cai, Zhengqing | Gong, Yanyan | Liu, Wen | Fu, Jie | O'Reilly, S.E. | Hao, Xiaodi | Zhao, Dongye
This work developed a new method to determine concentration of Corexit EC9500A, and likely other oil dispersants, in seawater. Based on the principle that oil dispersants decrease surface tension, a linear correlation was established between the dispersant concentration and surface tension. Thus, the dispersant concentration can be determined by measuring surface tension. The method can accurately analyze Corexit EC9500A in the concentration range of 0.5–23.5mg/L. Minor changes in solution salinity (<0.3%), pH (7.9–9.0), and dissolved organic matter (<2.0mg/L as TOC) had negligible effects on the measurements. Moreover, effects of extracts from marine sediments were negligible, and thus, the method may be directly applied to seawater–sediment systems. The method accuracy was confirmed by comparing with direct TOC analysis. This simple, fast, economical method offers a convenient analytical tool for quantifying complex oil dispersants in water/seawater, which has been desired by the oil spill research community and industries.
Показать больше [+] Меньше [-]The influence of sediment particle size on the properties of adsorbed dissolved organic matter in the Yangtze Estuary and its interactions with As/Sb
2016
Wang, Ying | Zhang, Manman | Zhang, Di | Shen, Zhenyao
The characteristics of dissolved organic matter (DOM) extracted from sediments with four particle sizes (<25, 63–25, 200–63 and >200μm) in the Yangtze Estuary were compared. The differences in their binding capacities for individual fluorescent components with As/Sb were studied using fluorescence-quenching titrations combined with excitation–emission matrix (EEM) spectra. The results indicated that the particle size influenced the quality and quantity of extracted DOM. With increasing particle size, the extracted DOM content, value of UV280 and acidic functional group content of the DOM decreased. Three protein-like components (C2, C3 and C4) and one humic-like component (C1) were identified using the parallel factor analysis (PARAFAC) model. Wherein, protein-like material dominated in DOM on different particle-size fractions and possessed a stronger complex capacity with As/Sb. A significant positive correlation between the complexation capacity of extracted DOM from samples, as well as with the acidic functional group content, was observed.
Показать больше [+] Меньше [-]The new Landsat 8 potential for remote sensing of colored dissolved organic matter (CDOM)
2016
Slonecker, E Terrence | Jones, Daniel K. | Pellerin, Brian A.
Due to a combination of factors, such as a new coastal/aerosol band and improved radiometric sensitivity of the Operational Land Imager aboard Landsat 8, the atmospherically-corrected Surface Reflectance product for Landsat data, and the growing availability of corrected fDOM data from U.S. Geological Survey gaging stations, moderate-resolution remote sensing of fDOM may now be achievable. This paper explores the background of previous efforts and shows preliminary examples of the remote sensing and data relationships between corrected fDOM and Landsat 8 reflectance values. Although preliminary results before and after Hurricane Sandy are encouraging, more research is needed to explore the full potential of Landsat 8 to continuously map fDOM in a number of water profiles.
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