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1.
The fate and transport of highly hydrophobic chemicals are affected by the partitioning between water and dissolved organic carbon. Large variation in the partition coefficient (KDOCw) is often found, due to the selection of model organic matter or potential experimental artifacts. To investigate the roles of the type of organic matter on the partitioning of highly hydrophobic compounds, the partition coefficients of eight selected polycyclic aromatic hydrocarbons (PAHs), with 3–6 aromatic rings, were determined using a passive dosing/extraction method between water and model dissolved organic matter (humic acid, fulvic acid, sodium dodecyl sulfate micelle (SDS), and 2‐hydroxypropyl‐β‐cyclodextrin). Although the KDOCw values for 3–4 ring PAHs in this study were close to those reported in the literature, experimental KDOCw values between Aldrich humic acid (AHA) and water were higher than values reported in the literature for 5–6 ring PAHs. The KDOCw values were highest for AHA, followed by SDS and Suwannee river fulvic acid (SFA). The slopes of the linear regression between log KDOCw and log Kow were 1.23 (± 0.13), 0.82 (± 0.09), and 0.59 (± 0.13) for AHA, SDS, and SFA, respectively. The differences in the KDOCw values between AHA and the other organic matter (SDS, SFA, and CD) increased with increasing hydrophobicity of the PAHs, showing that the sorption of highly hydrophobic chemicals to the humic acid fraction may be important in the presence of mixed organic matter.  相似文献   

2.
Chemical characterization of DOM in channels of a seasonal wetland   总被引：3，自引：0，他引：3  
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3.
Andy Baker 《水文研究》2002,16(16):3203-3213
There is a need to be able to differentiate the dissolved organic matter (DOM) fraction in river waters. Research in the 1970s and 1980s has attempted to utilize both absorbance and fluorescence to distinguish between DOM fractions in river waters, but both were limited by the available technology. Total organic carbon content has, therefore, been widely used as a standard method of measuring DOM concentration, although it has little power to differentiate DOM fractions. Recent advances in fluorescence spectrophotometry enable rapid and optically precise analysis of DOM. Here, we show how a combination of both fluorescence and absorbance can be used to discriminate statistically between spatial variations of DOM in tributaries in a small catchment of the Ouseburn, NE England. The results of the discriminant analysis suggest that about 70% of the samples can be correctly classified to its tributary. Discriminant function 1 explains 60·8% of the variance in the data and the fulvic‐like fluorescence intensity has the largest absolute correlation within this function; discriminant function 2 explains a further 21·5% of the variance and the fulvic‐like fluorescence emission wavelength has the largest absolute correlation within this function. The discriminant analysis does not correctly classify all tributaries every time, and successfully discriminates between the different tributaries 70% of the time. Occasions when the tributary waters are less well discriminated are due to either episodic pollution events (at two sites) or due to tributaries that have strong seasonal trends in spectrophotometric parameters, which allows the sites to be misclassified. Results suggest that spectrophotometric techniques have considerable potential in the discrimination of DOM in rivers. Copyright © 2002 John Wiley & Sons, Ltd.  相似文献   

4.
The production and use of nanomaterials will inevitably lead to their disposal in the natural environment. To assess the risk that these materials pose to human and ecosystem health an understanding of their mobility and ultimate fate is essential. To date, however, relatively little research has been conducted on the fate of nanoparticles in subsurface systems. In this study the subsurface mobility of two carbon nanoparticles: nano-fullerenes (nC60) and multi-walled carbon nanotubes (MWCNTs) is assessed. A two-dimensional finite element model was used to simulate the movement of these nanoparticles under a range of hydrologic and geological conditions, including a heterogeneous permeability field. The numerical model is based on colloid filtration theory (CFT) with a maximum retention capacity term. For the conditions evaluated the carbon nanotubes are much more mobile than nC60 due to the smaller collector efficiency associated with carbon nanotubes. However, the mobility of nC60 increased significantly when a maximum retention capacity term was included in the model. Model results also demonstrate that, for the systems examined, nanoparticles were predicted to be less mobile in heterogeneous systems compared to the homogeneous systems with the same average hydraulic properties.  相似文献   

5.
Agricultural soils have been analyzed to elucidate whether the trace metal distribution changes in relation to agricultural activities and to predict environmental risk. In addition to the extractability of Cu, Mn, Ni, Pb, and Zn in soils was compared by single extraction (hydrochloric acid (HCl), ethylenediaminetetraacetic acid (EDTA), diethylenetriaminepentaacetic acid (DTPA), calcium chloride (CaCl2), water (H2O)), and sequential extraction procedures. The modified Community Bureau of Reference (BCR) sequential extraction procedure (three‐step) used to extraction of metals in soil samples. The extraction capacity of the analyzed metals was found by using single extraction procedures in the order: HCl > EDTA > DTPA > CaCl2 > H2O. A single correlation analysis was used to investigate the relationship between extractable metal concentrations in soil solutions and metal accumulation in wheat grains. Simple correlation analyses indicated that the extractable Pb and Ni of soils by HCl, EDTA, and DTPA single extraction procedures were significantly correlated with the metal contents of wheat grains. For CaCl2, H2O, and BCR extraction procedures there was a relatively poor correlation between the extractable Cu, Mn, Ni, Pb, and Zn of soils and metal contents of wheat grains.  相似文献   

6.
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7.
We report on the concentration and compositional features of n-alkanes of natural and anthropogenic origins in the snow samples collected from the Qiyi glacier in the Qilian Mountains, the Yuzhufeng glacier in eastern Kunlun Mountains, the Xiaodongkemadi glacier in the Tanggula Mountains, and the Gurenhekou glacier in the Nyainqêntanglha Range. The results indicate a decrease in the total n-alkane concentration (T-HCs) from the northeast to the south over the Tibetan Plateau. The T-HCs in these studied areas were close to those in the Belukha and Sofiyskiy glacier, Russian Alati Mountains and the Dasuopu glacier in the Himalaya but were much higher than those in the Greenland ice sheet, suggesting that the mountain glaciers in the Asian continent may receive a higher loading of n-alkanes than the Greenland ice core. Moreover, the compositional characteristics of n-alkanes indicated that the n-alkanes in the studied areas were probably originated from the plant waxes as well as the fossil-fuel combustion exhaust, whereas the contribution from the lower organisms was small. In addition, the plant wax (Cn(wax)) and anthropogenic (non-Cn(wax)) contributions revealed that fast industrialization may have significant effects on the organic pollutant composition in glacier over the Tibetan Plateau and its circumference environment. Particularly, except for the Yuzhufeng glacier, the ΣnC21 −/ΣnC22 + and (nC15+nC17+nC19)/(nC27+nC29+nC31) ratio decreased from the Qiyi glacier to the Gurenhekou glacier over the Tibetan Plateau, while the carbon preference index (CPI) values increased. These results indicate a decrease in terrigenous input while an increase in marine input from the northeast to the south over the Tibetan Plateau. These two ratios can be used as the climatic and environmental change indicators.  相似文献   

8.
The fluorescent properties of dissolved organic matter (DOM) enable comparisons of humic‐like (H‐L) and fulvic‐like (F‐L) fluorescence intensities with dissolved organic carbon (DOC) in aquatic systems. The fluorescence‐DOC relationship differed in gradient, i.e. the fluorescence per gram of carbon, and in the strength of the correlation coefficient. We compare the fluorescence intensity of the F‐L and H‐L fractions and DOC of freshwater DOM in north Shropshire, England, featuring a river, wetland, spring, pond and sewage DOM sources. Correlations between fluorescence and DOC varied between sample sites. Wetland water samples for the F‐L peak gave the best correlation, r = 0·756; the lowest correlation was from final treated sewage effluent, r = 0·167. The relationship between fluorescence and DOC of commercially available International Humic Substances Society standards were also examined and they generally showed a lower fluorescence per gram of carbon for the F‐L peak than the natural samples, whereas peat wetland DOM gave a greater fluorescence per gram of carbon than river DOM. Here, we propose the strength of the fluorescence–DOC correlation to be a useful tool when discriminating sources of DOM in fresh water. Copyright © 2007 John Wiley & Sons, Ltd.  相似文献   

9.
The degradation of dissolved organic matter (DOM) was studied in alkaline solution. The products were characterised using UV/vis spectroscopy, size‐exclusion chromatography (SEC), and by the analysis of low‐molecular‐weight organic acids (LMWOA). The degradation experiments were performed with water from a brown water lake or its isolated fulvic acid fraction and sodium hydroxide at different reaction times and temperatures. Depending on the wavelength and the reaction time, the UV/vis absorbance between 230 nm and 600 nm increased or decreased. The behaviour of model compounds during reactions in alkaline media was compared to the UV/vis spectroscopic behaviour of DOM. The release of LMWOA was described by kinetic data and compared to the data of model reactions. Evidence was given for the carboxylic esters playing a significant role in the release of LMWOA only during the beginning of the alkaline degradation. The results gained by SEC with on‐line UV and DOC detection showed that the average size of DOM was decreasing, and that a major part of the degradation products consisted of low‐molecular‐weight mono‐ and dicarboxylic acids.  相似文献   

10.
Phosphorus (P) concentrations in sediments and in surface and interstitial water from three gravel bars in a large river (Garonne River, southern France) were measured daily, downstream of a wastewater treatment plant for a city of 740 000 inhabitants (Toulouse). Measurements were made of vertical hydraulic gradient (VHG), total dissolved phosphorus (TDP), soluble reactive phosphorus (SRP) and total phosphorus (TP) in water and of three extractable forms of phosphorus (water extractable, NaOH extractable and H2SO4 extractable) in hyporheic sediments from the gravel bars. Dissolved phosphorus was the major contributor to TP (74–79%) in both interstitial and surface waters on all sampling dates, and in most cases surface water P concentrations were significantly higher than interstitial concentrations. Hyporheic sediment TP concentrations ranged between 269 and 465 µg g?1 and were highest in fine sediment fractions. Acid‐extractable P, a non‐bioavailable form, represented at least 95% of sediment TP. A positive relationship was observed between VHG and TP in two of the gravel bars, with wells that were strongly downwelling having lower TP concentrations. These results suggest that in downwelling zones, hyporheic sediments can trap surface‐derived dissolved P, and that much of this P becomes stored in refractory particulate forms. Bioavailable P is mainly present in dissolved form and only occupies a small fraction of total P, with particulate P comprising the majority of total P. Copyright © 2009 John Wiley & Sons, Ltd.  相似文献   

11.
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12.
Frequent heavy rainfalls during the East Asian summer monsoon drastically increase water flow and chemical loadings to surface waters. A solid understanding of hydroclimatic controls on watershed biogeochemical processes is crucial for water quality control during the monsoon period. We investigated spatio‐temporal variations in the concentrations and spectroscopic properties of dissolved organic matter (DOM) and the concentrations of trace metals in Hwangryong River, Korea, during a summer period from the relatively dry month of June through the following months with heavy rainfall. DOM and its spectroscopic properties differed spatially along the river, and also depended on storm and flow characteristics around each sampling time. At a headwater stream draining a forested watershed, the concentrations (measured as dissolved organic carbon (DOC)), aromaticity (measured as specific UV absorbance at 254 nm), and fulvic acid‐ and protein‐like fluorescence of DOM were higher in stormflow than in baseflow waters. DOC concentrations and fluorescence intensities increased along the downstream rural and urban sites, in which DOC and fluorescence were not higher in stormflow waters, except for the ‘first flush’ at the urban site. The response of DOM in reservoir waters to monsoon rainfalls differed from that of stream and river waters, as illustrated by storm‐induced increases in DOM aromaticity and fulvic‐like fluorescence, and no significant changes in protein‐like fluorescence. The results suggest that surface water DOM and its spectroscopic properties differentially respond to changes in hydroclimatic conditions, depending on watershed characteristics and the influence of anthropogenic organic matter loadings. DOC concentrations and intensities of spectroscopic parameters were positively correlated with some of the measured trace metals (As, Co, and Fe). Further research will be needed to obtain a better understanding of climate effects on the interaction between DOM and trace metals. Copyright © 2006 John Wiley & Sons, Ltd.  相似文献   

13.
自2005年以来,程海水体的化学需氧量(COD)持续升高,而生化需氧量(BOD)却维持不变,高锰酸盐指数(COD_(Mn))升高也较缓慢.为研究程海COD持续升高的原因,选取程海水体中具有代表性的无机阴离子(Cl~-、F~-、S~(2-)、HCO_3~-)和溶解性有机质(DOM)中不同浓度的胡敏酸(HA)、富里酸(FA)和商品化腐殖酸(SHA),研究其对COD和COD_(Mn)测定的影响,探讨Cl~-和DOM共同存在下对COD测定的影响.结果表明:程海水体中Cl~-浓度对COD存在显著影响,产生的COD值为5.42 mg/L,S~(2-)、F~-和HCO_3~-对COD影响较小;各离子对COD_(Mn)的影响很小;不同浓度梯度的HA、FA和SHA与COD测定结果呈显著线性相关,氧化1 mg C HA、FA和SHA所产生的COD值分别为2.164、1.964和2.362 mg;氧化1 mg C HA和FA所产生的COD_(Mn)值分别为0.646和0.344 mg;DOM对COD测定值的影响显著大于对COD_(Mn)测定值的影响;且一定浓度Cl~-的存在增强了FA与HA对COD测定的影响.该研究为进一步阐明程海COD逐步升高,COD_(Mn)值缓慢升高的内在原因奠定了基础.  相似文献   

14.
The fate of 14C‐labeled sulfamethoxazole and acetyl‐sulfamethoxazole in soil has been investigated with special respect to possible entry routes of human and veterinary pharmaceuticals into soil environments. Therefore, the stability of the test substances was monitored first in sewage sludge and bovine manure. Within the incubation period of 72 d, 1% at maximum of the initially applied radiotracers was released as 14C‐carbon dioxide while ?75% was transferred to non‐extractable residues that were operationally defined by the ethyl acetate extraction. Test‐sludge and test‐manure samples with defined aged residues were prepared and, supplementary to standard solutions, applied to silty‐clay soil samples. After standard and test‐sludge application, soil/water distribution coefficients of Kd < 5 L kg–1 were determined revealing both test substances as potential leachers. In contrast, the sorption of sulfamethoxazole increased after test‐manure application (Kd > 10 L kg–1). In the long‐term degradability tests, the metabolic fate of both test substances was characterized by the continuous decrease of extractable residues, resulting in disappearance times of DT90 ? 33 d, and the increase of non‐extractable residues. Mineralization reached 11% at maximum. Thereby, the dynamics of these processes differed whether the test substances were applied via standard, test‐sludge or test‐manure application. This fact emphasized the relevance of entry route specific matrix effects on the fate of both test substances in soil.  相似文献   

15.
Dissolved organic matter (DOM) concentration and composition in riverine and stream systems are known to vary with hydrological and productivity cycles over the annual and interannual time scales. Rivers are commonly perceived as homogeneous with respect to DOM concentration and composition, particularly under steady flow conditions over short time periods. However, few studies have evaluated the impact of short term variability (<1 day) on DOM dynamics. This study examined whether diurnal processes measurably altered DOM concentration and composition in the hypereutrophic San Joaquin River (California) during a relatively quiescent period. We evaluated the efficacy of using optical in situ measurements to reveal changes in DOM which may not be evident from bulk dissolved organic carbon (DOC) measurement alone. The in situ optical measurements described in this study clearly showed for the first time diurnal variations in DOM measurements, which have previously been related to both composition and concentration, even though diurnal changes were not well reflected in bulk DOC concentrations. An apparent asynchronous trend of DOM absorbance and chlorophyll‐a in comparison to chromophoric dissolved organic matter (CDOM) fluorescence and spectral slope S290–350 suggests that no one specific CDOM spectrophotometric measurement explains absolutely DOM diurnal variation in this system; the measurement of multiple optical parameters is therefore recommended. The observed diurnal changes in DOM composition, measured by in situ optical instrumentation likely reflect both photochemical and biologically‐mediated processes. The results of this study highlight that short‐term variability in DOM composition may complicate trends for studies aiming to distinguish different DOM sources in riverine systems and emphasizes the importance of sampling specific study sites to be compared at the same time of day. The utilization of in situ optical technology allows short‐term variability in DOM dynamics to be monitored and serves to increase our understanding of its processing and fundamental role in the aquatic environment. Copyright © 2007 John Wiley & Sons, Ltd.  相似文献   

16.
章奇  居琪  李健欣  曹驰程  江和龙  张晖 《湖泊科学》2020,32(4):1041-1049
为探究富营养化湖泊中自生源可溶有机质(DOM)在泥水界面的吸附行为,以马来眼子菜(Potamogeton malaianus)和铜绿微囊藻(Microcystis aeruginosa)释放的DOM为代表,考察针铁矿对草、藻源DOM中不同组分的吸附特征.三维荧光平行因子分析表明类富里酸组分C1和类胡敏酸组分C4的含量很低,而类蛋白物质(类酪氨酸组分C2和类色氨酸组分C3)分别占草、藻源DOM荧光组成的70%和93%. 2种DOM均可被针铁矿吸附,吸附过程符合伪一级动力学.通过等温线拟合发现针铁矿吸附藻源DOM的非线性更强,饱和吸附量(23.77 mg/g)高于草源DOM(19.10 mg/g).特别地,类蛋白组分呈现非线性吸附,而类腐殖物质的吸附近似线性,且针铁矿对于DOM各荧光组分的吸附量顺序为:C3C2 C4 C1,此非均质吸附特征与DOM组分的初始含量、分子大小、芳香性及有效吸附位点有关.红外光谱证实氨基、羧基和羟基是吸附过程中的重要官能团.因此,草、藻源DOM显著改变了针铁矿表面的有机物质组成,影响湖泊沉积物的生物地球化学行为.  相似文献   

17.
To develop P management guidelines for poultry litter application in Oxisols of Brazil, the relationship between water soluble P (WSP), soil test P (STP), and degree of P saturation (DPS) needs to be established. The study examined this relationship in Oxisols of Brazil receiving poultry litter. Soils were analyzed for Mehlich‐1 P (M1‐P), WSP, P fractions, P sorption index (PSI), and P saturation based on Mehlich‐1 extractable P, Al, Fe (DPSM1), and PSI (DPSPSI). Surface water bodies in the catchment area were examined for inorganic and total P. All the surface water bodies in the catchment area of the sampled plots were highly enriched in inorganic and organic P. Enrichment of soil P fractions following poultry litter application followed the order HCl‐bound > NaOH‐bound > NaHCO3‐bound fraction. M1‐P was correlated to labile (NaHCO3‐Pi), and stable P pools (NaOH‐P and HCl‐P) and reflected the cumulative P accumulation in these soils. P saturation indices increased with cumulative P addition and increasing M1‐P. WSP increased with increasing DPS and a change point was noticed at 23% DPSPSI (equivalent to DPSM1 of 16.5%) corresponding to M1‐P of 44.5 mg P kg?1, which could be regarded as threshold for P loss in these soils.  相似文献   

18.
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19.
Boreal watersheds contain a vast quantity of terrestrially derived dissolved organic matter (DOM) originating from wetland and forest soils, yet variation in the potential for photochemical transformation of boreal aquatic DOM sources remains poorly understood. Laboratory solar radiation exposure experiments were conducted on DOM samples collected in three seasons, across nine sites, representing contrasting catchment composition and watershed position to assess variation in the photochemical lability of boreal DOM source and stable carbon isotopic signature (δ13C) of photomineralized DOM. Dissolved organic carbon (DOC) loss rates during laboratory exposure were lowest in summer, suggesting that DOM may have been more photo-degraded during summer. DOM from upstream portions of forested stream sites and wetland-influenced sites was more photolabile relative to downstream portions and the river DOM, suggesting potential losses in photolabile DOM downstream and in the lower reaches of the watershed. Increased a254:a350 and spectral slope following sample exposure suggest photoproduction of low molecular weight (LMW) CDOM and/or a higher photoreactivity of high molecular weight versus LMW compounds. Photomineralization of nitrogen was regulated by organic nitrogen concentration and resulted in NH4 +-photoproduction rates between 0.01 and 0.3?μM N?h?1 and ecologically significant increases in NH4 + for these waters. The δ13C of the photomineralized DOM was positively correlated to initial DOC concentration and generally lower when initial DOC concentrations were lower, suggesting variation in photomineralized DOM δ13C may be a result of kinetic isotope fractionation. Results from this study demonstrate significant variation in the photochemical lability of boreal watershed sources of DOM. Such variation suggests landscape and environmental change has the potential to alter the biogeochemical role photochemical transformations play in downstream portions of boreal watersheds.  相似文献   

20.
A greenhouse pot experiment was conducted to investigate the effect of compost addition on the phytoremediation ability of Medicago sativa, Brassica napus, and Lolium perenne in soils contaminated with pyrene. Pyrene concentrations were evaluated after 90 days in contaminated uncultivated amended‐soil, cultivated amended‐soils, and shoots and roots of the three plant species. The addition of compost enhances significantly pyrene dissipation from 16 to 26% in uncultivated soil, whereas in cultivated soils it appears not to have any significant effect on pyrene dissipation, neither pyrene was detectable in shoots and roots of the three species examined. The high partition coefficient of pyrene to compost dissolved organic matter (DOM) and the molar absorptivity values at 280 nm (ε280) indicate a high affinity of pyrene to compost DOM molecules, likely due to their aromatic character. These results suggest that compost improves pyrene removal from soil, possibly by promoting its adsorption onto compost DOM. This property is very important in indicating that compost can be used, besides for its amendment capacity, also as a potential tool for remediation of contaminated soils.  相似文献   

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