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1.
Sixteen samples of fulvic acids and XAD‐4 fractions of riverine, estuarine, coastal, and open ocean origin have been studied by emission and synchronous molecular fluorescence spectroscopy. Certain features of the molecular fluorescence are related to the nature, the content, and the origin of those aquatic humic substances (HS). Riverine HS appear several times richer in fluorophores than marine HS, which can be well observed by emission fluorescence spectroscopy. Synchronous‐scan spectra of fulvic acids and of XAD‐4 fractions from the aquatic environments studied, emphasized the quality differences of their fluorophores. These features are useful as tracers of humic substances related with their natural environment source or even with their anthropogenic origin.  相似文献   

2.
The primary objective of this study was to examine the chemical speciation of polycyclic aromatic hydrocarbons (PAHs) found in sediments endowed with different characteristics. To achieve this purpose and because the nature of the sediments influences the distribution of PAHs, we have analyzed four different types of sediments. To study the role of organic matter in the sequestration of PAHs, we fractionated humic substances into humic acids and humin-mineral fractions. After their separation and purification, the humic components were examined for their sorptive reactivity by extracting them with organic solvents; these extracts were subsequently subjected to GC/MS analysis. Our results show that PAHs are distributed between labile and sequestered fractions in sediments. A slower uptake of PAHs occurs when the sequestered fraction is formed, and this process can be prolonged and may be influenced by the characteristics if the sediment. Our study suggests that organic contaminants are available in muddy sediments for a longer period of time than in sandy sediments.  相似文献   

3.
The distribution of halogens in various fractions of humic substances (HS), separated by their molecular weight, was found to be different for the different halogens. This was demonstrated for chlorine, bromine, and iodine in sewage and brown water samples by applying inductively coupled plasma mass spectrometry coupled with size‐exclusion chromatography. Quantification of the different fractions of iodinated humic substances was obtained by quadrupole mass spectrometry in connection with the isotope dilution technique using an 129I‐enriched spike solution. Quantitative analysis was not possible for the corresponding chlorine and bromine species because of spectrometric interferences in the quadrupole instrument. The ageing of HS/halogen species was followed with respect to possible transformations of these species in a ground and sewage water sample up to eight weeks. Even if a distinct structural variation of the humic substance was observed with time by measuring the UV absorption, chlorine remained in the same molecular weight fraction and only a small change was found for the HS/bromine species after eight weeks. In contrast to these findings a substantial transformation of HS/iodine compounds took place, which demonstrated that the transfer probability of halogens from one to another HS fraction is increased with decreasing strength of the halogen bond to carbon. By comparing the results of an original sewage water sample with a filtered one and with another one which was enriched by microorganisms cultivated from the same original sample, a strong microbiological influence on the transformation of HS/iodine species was found. A quantitative balance of the corresponding HS/iodine fractions was calculated for an ageing period of eight weeks showing that iodine was preferably transferred to newly formed UV active HS substances of high molecular weight. In total, no iodine was released from the humic substances.  相似文献   

4.
《国际泥沙研究》2020,35(3):287-294
The Suquia River,the largest urban river in Cordoba(Argentina),has been severely polluted for decades.Actions must be taken to restore its environmental quality by managing riparian zones for increased water-self purification.The current study aimed to characterize organic matter(OM) dynamics and humic substances(HS) spectrochemical properties along the lower-middle basin of the Suquia River.Riparian soil(0-20 cm) and sediment(0-10 cm) samples were collected from a reference location(S1)and four polluted sites(S2-S5) during a low-flow period.The contents of soil and sedimentary OM and HS fractions were analyzed by wet oxidation,as well as HS Fourier transform infrared(FT-IR) and ultraviolet-visible(UV-Vis) spectrochemical properties.The OM and HS fractions from riparian soil were high upstream of Cordoba City(S1 and S2,50.2-50.4 g/kg OM) and within a 50 km downstream location(S5,30.9 g/kg OM) owing to a surplus of fresh plant biomass-carbon(C) inputs.Highly heterogeneous sediment samples did not show any significant differences among sites(P 0.05).The lowest values of the ratio of absorbances at 465 and 665 nm(E4/E6)(1.78) and the Δ log K(0.15) coefficient(a measure of HS maturity degree) were obtained downstream of Cordoba City,for both riparian soil and sediment,indicating that HS were enriched by more condensed aromatic structures within highly degraded portions of the river.All samples exhibited similar IR spectra,implying overlapping recalcitrant-C structures at the functional group level,but with different absorbance intensity.Data from the current study constitute a baseline for understanding the chemical nature of HS from sediment and riparian soil along the Suquia River and can be used as a reference for future studies tracking OM compositional changes over time.  相似文献   

5.
Dissolved high molecular weight organic substances, like humic substances, can be characterized with regard to their molecular weight distribution using gel filtration chromatography (GFC). In addition, the adsorption properties, for example on activated carbon, can be described, if the substances are separated by hydrophobic interaction chromatography (HIC) in different fractions using a chromatographic column with a hydrophobic matrix. The retention time (Rt) of single chemical substances in this column can be used to characterize the hydrophobicity or hydrophility of each compound as well as of the high molecular weight organic matter. The hydrophobic interaction between the matrix of the column and the dissolved chemical compounds also depends on the hydrophobicity of the gel and the composition of the eluent. Relations between retention times, log P-coefficients (octanol/water partition) and K-values of isotherms on activated carbon (Freundlich equation) were found.  相似文献   

6.
A natural decay of plant and animal biomass in aquatic environments results in the release of different simple structured organic substances into water. In our laboratory experiments we investigated whether some of them, e.g., starch or peptone, and also a complex yeast biomass can be transformed into humic-like substances by natural assemblages and some pure cultures of aquatic microorganisms. After a 6 months incubation most of the cultural media enriched with those natural organic substrates turned dark in color and humic-like substances (HS) could be isolated. However, the original substrate organic carbon was mainly mineralized in microbial cultures, and only about 3 % C was converted into HS. Total yields of HS differed in dependence of the individual substrate used (peptone > yeast > starch), the origin of inoculum (river > lake > groundwater), and the incubation temperature (20°C > 10°C). According to their elemental composition, and their spectroscopical and electrophoretic characteristics the microbially formed HS resembled natural aquatic humic matter, but were higher in aliphatic constituents (carbohydrates, peptides) and lower in aromatic structures. HS-like substances were also obtained from pure cultures of a bacterium Bacillus sphaericus and a fungus Cladosporium cladosporioides. The 13C and 15N isotopic contents of the microbially produced HS differed in dependence on the microbial inoculum and the type of organic substrates used, but in general they indicated anabolic processes to be mainly responsible for the humification of the simple organic substrates used in our experiments.  相似文献   

7.
Continuous monitoring of dissolved organic matter (DOM) character and concentration at hourly resolution is rare, despite the importance of analysing organic matter variability at high‐temporal resolution to evaluate river carbon budgeting, river water health by detecting episodic pollution and to determine short‐term variations in chemical and ecological function. The authors report a 2‐week experiment performed on DOM sampled from Bournbrook, Birmingham, UK, an urban river for which spectrophotometric (fluorescence, absorbance), physiochemical (dissolved organic carbon [DOC], electrical conductivity, pH) and isotopic (D/H) parameters have been measured at hourly frequency. Our results show that the river had sub‐daily variations in both organic matter concentration and characteristics. In particular, after relatively high‐magnitude precipitation events, organic carbon concentration increased, with an associated increase in intensity of both humic‐like and tryptophan‐like fluorescence. D/H isotopic ratio demonstrates different hydrological responses to different rainfall events, and organic matter character reflects this difference. Events with precipitation < 2 mm typically yielded isotopically heavy water with relatively hydrophilic DOM and relatively low specific absorbance. Events with precipitation > 2 mm had isotopically lighter water with higher specific absorbance and a decrease in the proportion of microbially derived to humic‐like fluorescence. In our heavily urbanized catchment, we interpret these signals as one where riverine DOM is dominated by storm sewer‐derived ‘old’ organic matter at low‐rainfall amounts and a mixed signal at high‐precipitation amounts where ‘event’ surface runoff‐derived organic matter dominate during storm sewer and combined sewer overflow routed DOM. Copyright © 2009 John Wiley & Sons, Ltd.  相似文献   

8.
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9.
The occurrence of plutonium isotopes derived from the Windscale reprocessing facility discharges and weapons test fallout in intertidal sediments of the Wyre estuary, northwest England, is reported. Windscale plutonium appears to be slowly transported to the estuary in association with sedimentary material, and its distribution in surface and buried sediments is controlled by the variations in organic matter content of the sediments and/or their grain size characteristics. Results from chemical leaching experiments suggest that very little plutonium is ion exchangeable or in humic substances, but it is in other organic and Fe/Mn hydrous oxide fractions of the sediments. Plutonium shows a similar depositional behaviour to mercury which enters the Wyre directly in local industrial discharges.  相似文献   

10.
Characteristics and distributions of humic acid(HA) and soil organic matter(SOM) in a yellow soil profile and a limestone soil profile of the southwest China Karst area were systematically investigated to reveal their evolutions in different soils of the study area. The results showed that characteristics and distribution of SOM along the two soil profiles were notably different. Total organic carbon(TOC) contents of soil samples decreased just slightly along the limestone soil profile but sharply along the yellow soil profile. TOCs of the limestone soils were significantly higher than those of the corresponding yellow soils, and C/N ratios of SOMs showed a similar variation trend to that of TOCs, indicating that SOM can be better conserved in the limestone soil than in the yellow soil. The soil humic acids were exhaustively extracted and further fractionated according to their apparent molecular weights using ultrafiltration techniques to explore underlying conservation mechanisms. The result showed that C/N ratios of HAs from different limestone soil layers were relatively stable and that large molecular HA fractions predominated the bulk HA of the top soil, indicating that HA in the limestone profile was protected while bio and chemical degradations were retarded. Combined with organic elements contents and mineral contents of two soils, weconcluded that high calcium contents in limestone soils may play a key role in SOM conservation by forming complexation compounds with HAs or/and enclosing SOMs with hypergene CaCO_3 precipitation.  相似文献   

11.
Properties of suspended particulate matter play a vital role in transport processes, but information from boreal lowland river systems with high organic loads is limited. This study analysed data from 2 years of sampling at 30 locations in Finland (204 samples in total) using suspended particulate matter samplers to determine effective and absolute particle size and organic fractions. Mean d50 value was 22 and 49 µm for absolute and effective particle size, respectively. The organic fraction content ranged from 2.1% to 36% (mean 9.6%), highlighting the importance of particle organic matter for suspended particulate matter flux in the region. The results indicated that the suspended particulate matter particle size distribution and load in the study region is dominated by composite particles. There were considerable spatial and temporal variations in transport of organic fractions, effective particle size and degree of aggregation (range 1.5–93%). Headwaters and, in particular, late summer and spring flood conditions with flow peaks produced the largest composite particles, whereas agriculture‐dominated sites produced smaller but more tightly compacted particles. Organic plant fibres appeared to play a vital role in floc formation in peat‐covered catchments, whereas in agriculture‐dominated catchments, land use‐derived aggregates dominated the composition. This study provides empirical evidence of the importance of effective particle size measurement in understanding the dynamics of suspended particulate matters in boreal lowland river systems. Copyright © 2014 John Wiley & Sons, Ltd.  相似文献   

12.
Three‐dimensional fluorescence spectra of water samples from an eucalyptus bleached kraft pulp mill and from a river, upstream and downstream of the discharge of the effluent, revealed the existence of a peak at δexc = 280 nm and δem = 340 nm Δδ = 60 nm), characteristic of effluentπs organic matter. Humic substances were isolated from the effluent by sequential adsorption onto resins XAD‐8 and XAD‐4 in series. Their synchronous fluorescence spectra with Δδ = 60 nm do also exhibit an intense signal at δexc = 280 nm (≈ 300 nm in the humic acid fraction). The peak is absent in the spectra of humic substances isolated from a non‐polluted site of the river, but it is clearly seen in the spectra of the humic substances from a site downstream of the discharge of the effluent. Synchronous fluorescence spectra (Δδ = 60 nm) of water samples from the river and its lagoon were recorded and revealed to be an easy and fast way of tracing the organic contamination from the effluent.  相似文献   

13.
Organic matter can be considered one of the most important indicators of the extent of soil desertification processes. Among the causes of desertification, salinization induced by different factors is raising the greatest concern in the Mediterranean area. In the present research, hydrophilic (HI) and hydrophobic (HO) fractions of dissolved organic matter (DOM) extracted from soils at different degrees of salinization have been investigated by means of spectroscopic techniques such as tridimensional fluorescence spectroscopy in the mode of emission excitation matrix (EEM) and Fourier transform infrared spectroscopy (FT‐IR). The FT‐IR spectra were distinctive in differentiating HI from HO fractions and each DOM fraction as a function of soil salinity. The EEM spectra of HO fractions exhibited a shift toward longer emission wavelengths and higher fluorescence intensity (FI) values as compared to that of the HI fractions. These results could be ascribed to the different molecular complexities of HI and HO fractions. Further, a marked quenching effect was observed in the FI of both the DOM fractions with increasing soil salinity, which allowed to obtain immediate information on the soil salinity degree by comparing the fluorescence intensity.  相似文献   

14.
Mobilization Potential of Hydrophobic Organic Compounds (HOCs) in Contaminated Soils and Waste Materials. Part I: Mobilization Potential of PCBs, PAHs, and Aliphatic Hydrocarbons in the Presence of Solubilizing Substances When using an elution procedure for organic pollutants to estimate the leaching behaviour of contamined soils and waste deposits, the influence of organic matter in solids and eluates adequately has to be considered. In batch tests with a solid/liquid ratio of 1:10, various aqueous solutions were composed, the solubilizing effect of which can be attributed to ubiquitous natural compounds (e. g., phospholipids, humic and carbonic acids). These solutions were evaluated in regard to the mobilization of PAHs, PCBs, and aliphatic hydrocarbons in soil and waste samples. The results were compared with batch tests containing sodium dodecyl sulfate (SDS), the properties and applications of which are selected and optimized in order to simulate the chemical interactions between pollutant and solubilizing substances of natural sources. Under alkaline conditions, the part of eluated pollutants was high because of the release of humic substances indigenous to the sample. Low concentrations of phospholipids and humic acid could decrease the mobility of aliphatic hydrocarbons. The extend of HOC mobilization is affected by specific interdependences between solubilizing substances and reactive matter of the samples. For most samples, 5.0 g/L concentrated SDS solution was able to simulate the most effective natural solutizer potential in regard to the mobilization of PAHs, PCBs, and aliphatic hydrocarbons within the system of batch tests. Whereas elution with pure water caused significant deviations in pollutant composition and too low yields, the use of SDS effected à good conformity. Modified in such a manner, the elution procedure can follow DIN 38414 part 4, when loss of pollutants will be minimized; e. g., centrifugation is needed to separate phases.  相似文献   

15.
The electroendosmotic flow (EOF), generated by the migration of solvated ions near the charged capillary surface, is an important factor in determining the capillary electrophoretic behaviour of humic substances (HS). We investigated the electrophoretic mobilities of HS fractions of reduced molecular-weight polydispersity extracted from peat and from a spodosol either in the presence or after suppression of the EOF. When the EOF was not suppressed, HS migrated to the cathode in spite of their negative charge. Fractionation of HS according to molecular size was achieved in polyacrylamide-coated capillaries filled with 0.05 M tris-phosphate buffer. In uncoated capillaries filled with the same buffer, all fractions had very close mobilities. Addition of polyethylene glycol MW 4000 at concentrations above its entanglement threshold caused the migration times of larger molecules to increase more than those of smaller molecules. The separation was a linear function of molecular size up to 75000 g mol–1 for peat HS and to 50000 g mol–1 for HS extracted from the spodosol.  相似文献   

16.
乌梁素海沉积物腐殖质的组成及分布特征   总被引：4，自引：2，他引：2  
以乌梁素海为研究对象,应用化学方法对乌梁素海湖泊表层沉积物有机质含量、腐殖质组成、影响腐殖质的环境因子及腐殖化程度进行了研究,结果表明:乌梁素海表层沉积物有机质含量变化范围为1.06%~5.38%.有机质分布特征与表层沉积物所处的水力条件、水生植物分布、人为活动有关;腐殖质组成中,胡敏酸含量为0.65~2.78 g/kg,富里酸含量为2.19~8.72 g/kg,胡敏素是主体,含量在3.28~20.92 g/kg之间;腐殖质与环境因子的相关性分析中,各组分含量与有机质含量呈极显著相关.pH值与胡敏素含量呈显著负相关.溶解氧与富里酸、胡敏素含量分别呈极显著正相关、显著正相关.腐殖化程度分析中,随着有机质含量的上升,可提取腐殖质的相对含量下降.PQ值介于9.50%~27.06%之间,平均值为21.47%,变异较大,且腐殖化程度较低.  相似文献   

17.
The spatial and temporal distribution of humic substances in aquatic ecosystems can have important effects on ecosystem productivity, negatively impacting primary productivity while positively impacting secondary productivity. In the present investigation, a large shallow lake ecosystem was studied to determine the spatial and seasonal variation of the composition and concentration of humic substances. Concentrations of total dissolved organic matter, humic acid, and fulvic acid were found to display significant spatial distributions (1.3…13.5 mg/L, DOM; 0.1…5.4 mg/L, HA). The distribution is described by using mapping techniques and the analysis of the spatial distribution of the lake. An analysis of the seasonal variations also indicated the dependence of the occurrence of these compounds on meteorological and hydrological conditions. To identify the potential sources of these organic materials, an analysis was made of the ratio of humic and fulvic acid fractions and total DOM. It was found that areas of high DOM concentration coincided with the areas of highest HA percentage of total DOM. Furthermore using the ratio of the normalised concentrations of HA, FA, and residual DOM (< 5000 g/mol) it was found that areas dominated by each are spatially distinct. This confirms the hypothesis that in these shallow lakes, photodegradation and bacterioplankton activity will create a residence time dependent zonation of each component of the total DOM.  相似文献   

18.
Amount and composition of dissolved organic matter (DOM) were evaluated for multiple, nested stream locations in a forested watershed to investigate the role of hydrologic flow paths, wetlands and drainage scale. Sampling was performed over a 4‐year period (2008–2011) for five locations with drainage areas of 0.62, 3.5, 4.5, 12 and 79 ha. Hydrologic flow paths were characterized using an end‐member mixing model. DOM composition was determined using a suite of spectrofluorometric indices and a site‐specific parallel factor analysis model. Dissolved organic carbon (DOC), humic‐like DOM and fluorescence index were most sensitive to changes with drainage scale, whereas dissolved organic nitrogen, specific UV absorbance, Sr and protein‐like DOM were least sensitive. DOM concentrations and humic‐like DOM constituents were highest during both baseflow and stormflow for a 3.5‐ha catchment with a wetland near the catchment outlet. Whereas storm‐event concentrations of DOC and humic DOM constituents declined, the mass exports of DOC increased with increasing catchment scale. A pronounced dilution in storm‐event DOC concentration was observed at peak stream discharge for the 12‐ha drainage location, which was not as apparent at the 79‐ha scale, suggesting key differences in supply and transport of DOM. Our observations indicate that hydrologic flow paths, especially during storms, and the location and extent of wetlands in the catchment are key determinants of DOM concentration and composition. This study furthers our understanding of changes in DOM with drainage scale and the controls on DOM in headwater, forested catchments. Copyright © 2014 John Wiley & Sons, Ltd.  相似文献   

19.
Industrial park wastewater (IPWW) includes complex non‐biodegradable organic compounds. A wastewater treatability study using biodegradability assessment approach was carried out for an industrial park housing mainly textile and machinery sectors. Biodegradable and inert chemical oxygen demand (COD) fractions with soluble and particulate counterparts were experimentally estimated by implementing respirometric methods. Aerobic batch test methods and oxygen uptake rate profiles were used to map kinetic parameters and COD fractions. Denitrification potential was also determined by application of anoxic batch tests. Relevant kinetic constants, stoichiometric, and design parameters were determined for biological processes. Tests were carried out for raw and physico‐chemically pre‐treated IPWW. Hence, it was aimed to assess the effects and necessity of pre‐treatment on biological processes. Biological mineralization, nitrification, and denitrification processes were also designed and tested using a bench scale continuous treatment model for pre‐treated IPWW. The sum of initial inert soluble COD fraction and production of soluble microbial products decreased about 25% for the case of pre‐treated IPWW as compared to raw IPWW. Eighty‐three percent total COD and 89% total Kjeldahl nitrogen removal efficiencies were attained for the modeling experiments of pre‐treated IPWW. Results showed the significance of pre‐treatment if complex strength industrial wastewaters are to be biologically treated.  相似文献   

20.
The molecular characteristics of dissolved organic matter (DOM) reflect both its source material and its biogeochemical history. In glacial systems, DOM characteristics might be expected to change over the course of a melt season as changes in the glacier drainage system cause the mobilization of DOM from different OM pools. To test this hypothesis we used Principal Components Analysis (PCA) of synchronous fluorescence spectra to detect and describe changes in the DOM in meltwater from a glacier system in the Coast Mountains of northern British Columbia, Canada. For most of the melt season, the dominant component of subglacially routed meltwater DOM is characterized by a tyrosine‐like fluorophore. This DOM component is most likely derived from supraglacial snowmelt. During periods of high discharge, a second component of DOM is present which is humic in character and similar to DOM sampled from a nearby non‐glacial stream. This DOM component is inferred to be derived from a moss‐covered soil environment that has been glacially overrun. It is probably entrained into glacial melt waters when the supraglacial meltwater flux exceeds the capacity of the principal subglacial drainage channels and water floods areas of the glacier bed that are normally isolated from the subglacial drainage system. Another source of DOM also appears to be mobilized during periods of high air temperatures. It is characterized by both humic and proteinaceous fluorophores and may be derived from the drainage of supraglacial cryoconite holes. Copyright © 2009 John Wiley & Sons, Ltd.  相似文献   

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