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1.
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   

2.
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3.
A method is described for the specific hydrolysis of amino acids from humic substances by using the proteolytic enzyme “Pronase E”. The amino acids are analyzed by a fluorescence detector after precolumn derivatization and HPLC-separation. The pattern and the concentration of amino acids after the enzymatic hydrolysis are set up for humic substances of different origin. Due to the results the enzymatic hydrolysis is suitable for the characterization of humic substances with a nitrogen content higher than 3%. As shown in a kinetic study of the hydrolysis of a fulvic acid the influence of humic substances on the enzyme activity increases in case of lower nitrogen content. Due to the specificity of the proteolytic enzyme the operationally defined method is limited as shown by a protein of a known amino acid content. The amino acids leucine, valine, tyrosine and histidine are released to the highest extent. The determined total extent for the hydrolysis of Insulin B is 26.34% and for Casein 38.37%. By comparison of the enzymatic hydrolysis with the classic acid hydrolysis the advantages of the biochemical method are the simple experimental handling and the mild reaction conditions. Amino acids which are very unstable like glutamine and asparagine can only be analyzed by the enzymatic hydrolysis.  相似文献   

4.
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   

5.
As part of a study on microbial redox alteration of humic substances we investigated the potential effect of this metabolism on the fate of heavy metals and hydrocarbons as a result of conformational alteration of the humic molecular structure due to microbial reduction. Our studies indicate that the microbial reduction of humic acids (HA) results in significant morphological and geochemical alterations. X‐ray microscopy analysis indicate that the conformational structure of the humic colloids is altered as a result of the redox change. In the reduced state, the HA appeared as small dense particles, on reoxidation, large loose aggregates were formed. In addition, spectrofluorometric studies indicated that the binding capacity of the HA for naphthalene was decreased by 10% when the HA was reduced. Similarly, the reduced HA yielded higher surface tension values at all concentrations tested which is indicative of a more hydrophilic and less hydrophobic solute. On reoxidation, the surface tension values reverted back to values similar to those obtained for the untreated oxidized HA. These data indicate that the hydrophobicity of the HA is altered on biological reduction of the HA and that this alteration is reversible. In contrast the reduced HA demonstrated a 15% higher affinity for heavy metals such as divalent cobalt than the oxidized HA. In addition to increasing the binding capacity of HA for heavy metals, the reduction of the HA also decreased the bioavailability and toxicity of bound heavy metals such as chromium. When incubated in the presence of Cr(III) and HA, cells of Escherichia coli grew much more rapidly in the presence of the reduced HA suggesting that the higher metal binding capacity of the reduced humic substances resulted in a removal of the Cr(III) from solution and hence reduced its bioavailability and toxicity. These studies demonstrate that HA redox state and reduction of humic acids by microorganisms can have a significant effect on the molecular morphology and binding constants of HA for heavy metals and hydrocarbons and also directly affects the bioavailability of these compounds in the environment.  相似文献   

6.
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   

7.
Humic acid plays an important role in the distribution of heavy metals in the environment. The aims of this study were conducted to evaluate the spectroscopic characteristics and aluminum (Al) adsorption of humic acids which were extracted from four composts. The functional groups were determined by Fourier transform infrared spectroscopy (FTIR) and solid‐state 13C nuclear magnetic resonance spectroscopy (13C‐NMR). The results showed that the aromatic groups were all found in the humic acids of the four composts, and the surface of humic acids included carboxylic group, hydroxylic group, and amino group. The experiment of Al adsorption was described by Freundlich equation. It showed that the adsorption of Al by humic acid from compost of cattle manure was higher, but that from the compost of pig manure, lemon manure, tea manure in equal preparation was lower. The adsorptive behavior was different due to the interaction by functional groups ( OH and  COOH) with Al. These results can describe the fate and transportation of Al in the soil of different organic fertilizer.  相似文献   

8.
Dissolved organic carbon (DOC) distributions in water from Lake Ipê, MS, Brazil, were investigated. The samplings were performed monthly (surface, 1 m depth, and bottom) from June 1999 to June 2000. Absorbance at 285 nm and DOC concentrations in mg dm—3, p(DOC), were highly correlated for the three depths. 77% of the surface, 85% for 1 m and bottom samples presented a variation between 20 dm3 g—1 cm—1 and 50 dm3 g—1 cm—1 of A(285 nm)/p(DOC), that characterizes the dissolved organic matter in lake water as essentially fulvic. The ratio A(254 nm)/p(DOC) was also sensitive for fulvic matter, and an A(250 nm)/A(365 nm) = 4 ratio was characteristic of strongly colored waters. The ratios A(436 nm)/p(DOC) for the three depths also showed a significant correlation. The predominance of fulvic acid is explained by environmental characteristics such as the tropical climate, temperatures above 18 °C, and the lake environment. It was demonstrated that the variation in the water carbon content due to different compartments in the lake can be monitored by UV‐vis spectroscopy ratios.  相似文献   

9.
采用荧光光谱区域体积积分法定量研究洱海沉积物有色可溶性有机物（CDOM）三维荧光空间分布特性,结果表明,洱海沉积物CDOM中类腐殖酸组分占比最高（44.5%~74.2%）,其次为溶解性微生物代谢产物（10.7%~20.4%）和类富里酸物质（8.19%~19.7%）,而类蛋白组分占比最低,类腐殖酸占比与H/C和N/C均呈显著负相关;南部湖心平台区域沉积物类富里酸和类蛋白组分占比较高,其CDOM自生源占比较高;北部水生植物分布区溶解性微生物代谢产物占比较高,CDOM陆源性较强;中部深水区及南北湖湾区域类腐殖酸占比较高,随水深增加沉积物CDOM自生源特征增强.随沉积物深度增加类腐殖酸和溶解性微生物代谢产物占比呈下降趋势,类富里酸占比呈上升趋势,CDOM自生源特征增强,脂肪化程度增高.随湖泊富营养化程度增加沉积物CDOM受微生物代谢产物影响增强,陆源性增加,而自生源性降低,湖泊沉积物CDOM具有富营养化指示意义.  相似文献   

10.
Attributing the start of peat growth to an absolute timescale requires dating the bottom of peat deposits overlying mineral sediment, often called the basal peat. Peat initiation is reflected in the stratigraphy as a gradual transition from mineral sediment to increasingly organic material, up to where it is called peat. So far, varying criteria have been used to define basal peat, resulting in divergent approaches to date peat initiation. The lack of a universally applicable and quantitative definition, combined with multiple concerns that have been raised previously regarding the radiocarbon dating of peat, may result in apparent ages that are either too old or too young for the timing of peat initiation. Here, we aim to formulate updated recommendations for dating peat initiation. We provide a conceptual framework that supports the use of the organic matter (OM) gradient for a quantitative and reproducible definition of the mineral-to-peat transition (i.e., the stratigraphical range reflecting the timespan of the peat initiation process) and the layer defined as basal peat (i.e., the stratigraphical layer that is defined as the bottom of a peat deposit). Selection of dating samples is often challenging due to poor preservation of plant macrofossils in basal peat, and the representativity of humic and humin dates for the age of basal peat is uncertain. We therefore analyse the mineral-to-peat transition based on three highly detailed sequences of radiocarbon dates, including dates of plant macrofossils and the humic and humin fractions obtained from bulk samples. Our case study peatland in the Netherlands currently harbours a bog vegetation, but biostratigraphical analyses show that during peat initiation the vegetation was mesotrophic. Results show that plant macrofossils provide the most accurate age in the mineral-to-peat transition and are therefore recommendable to use for 14C dating basal peat. If these are unattainable, the humic fraction provides the best alternative and is interpreted as a terminus-ante-quem for peat initiation. The potential large age difference between dates of plant macrofossils and humic or humin dates (up to ∼1700 years between macrofossil and humic ages, and with even larger differences for humins) suggests that studies reusing existing bulk dates of basal peat should take great care in data interpretation. The potentially long timespan of the peat initiation process (with medians of ∼1000, ∼1300 and ∼1500 years within our case study peatland) demonstrates that choices regarding sampling size and resolution need to be well substantiated. We summarise our findings as a set of recommendations for dating basal peats, and advocate the widespread use of OM determination to obtain a low-cost, quantitative and reproducible definition of basal peat that eases intercomparison of studies.  相似文献   

11.
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   

12.
A phenoloxidase-producing fungus – Cladosporium cladosporioides – was isolated from water of a bog lake. At high concentrations of carbon (333 mM) and nitrogen (12 mM), the fungus demonstrated the formation of a laccase and a high ligninolytic activity. After addition of riverine or groundwater humic substances into culture media (ca. 1 mg mL–1), the fungus showed the ability of degrading (utilizing) of about 60% of these substances. However, the exact quantification of the degree of degradation was difficult because of adsorption of humic matter on fungal mycelium. Reisolated humic substances were lower in aromatic and higher in aliphatic structures. A crude enzyme from the C. cladosporioides culture showed only low activity in decolorizing humic substances, whereas decolorization up to 50% was observed when using a laccase preparation from Polyporus versicolor, and especially in the presence of a redox mediator.  相似文献   

13.
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   

14.
The organic composition and organic‐inorganic interaction in paper mill sludge (PS) solvent extracts (hexane, ethyl acetate, acetone and ethanol) and humic fractions, humic acid (HA) and humin (HU) were studied by electron paramagnetic resonance spectroscopy (EPR), proton and carbon‐13 nuclear magnetic resonance spectroscopy (1H NMR; 13C NMR), Fourier‐transformed infrared spectroscopy (FTIR), and ultraviolet‐visible spectroscopy (UV‐vis). The strategy of fractionating the PS, sequentially, with organic solvents of increasing polarity is a reliable analytical procedure for humic substance sample separation because it results in more purified fractions. FTIR, 1H NMR and 13C NMR results showed that hexane extract consisted mainly of aliphatic hydrocarbon structures. Their contents in the extracts decreased as the polarity of the extracting solvent increased and the content of oxygen functional groups increased. Carboxylic and carboxylate functional groups were found in the acetone extract, and ester and ether functions were predominantly found in the ethanol extract. EPR spectra revealed some Fe3+ complexes with rhombic structure (g1 = 4.3; g2 = 9.0) in the humic fractions and in all solvent extracts, except hexane. Quasi‐octahedral Fe3+ complexes (g = 2.3; ΔHpp ≤ 400 G) were found in the HU fraction and in the acetone extract. The organic free radical content in the HA fraction was higher than the non‐fractionated PS sample and HU fraction.  相似文献   

15.
The precision UV/Vis‐absorption spectra of a naturally occurring aquatic humic substance were measured in the range of concentration 0.003 to 1.4 g/L DOC (dissolved organic carbon). Lambert‐Beer law is well obeyed at low concentrations whereas deviations have been observed for DOC concentrations above 0.1 g/L: they are interpreted in terms of self‐solvation and formation of micelles.  相似文献   

16.
This paper deals with the influence of different humic substances (HS) on the enzyme activity (EA) of the proteolytic enzyme pronase E. The EA was determined by analyzing the concentration of the amino acid valine hydrolyzed from caseine. For amino acid analysis, a flourescence detector was used after precolumn derivatization and HPLC-separation of the hydrolysis products. The data show that the presence of HS has no adverse effects on amino acid analysis. Based on this result, a decrease of EA was observed in the presence of HS acting as enzyme inhibitors. Clear inhibition effects could be seen for different fulvic acids (HO3 FA, FBR FA and FBR 1.0 FA) at concentrations of 150 mg/L. In case of FBI-2 FA, higher concentrations were necessary to decrease the EA significantly. At an inhibitor concentration of 1500 mg/L the EA was mostly found to be less than 50%. The standard deviations of the results don't allow a differentiation between the HS of different origin and treatment. Specifying HS according to their influence on EA has to remain uncertain. As shown in a kinetic study of the hydrolysis of L-Leucine-2-naphthylamide-hydrochloride, the inhibitor HO3 FA decreases the maximum velocity of the reaction but has no effect on the Michaelis constant. These results indicate that this HS acts as a noncompetitive inhibitor.  相似文献   

17.
Two fulvic acid (FA) samples taken from a former gas production facility in the Southwest of Germany were characterized using advanced fluorescence techniques. Steady-state fluorescence (fluorescence excitation, synchronous fluorescence) as well as time-resolved fluorescence were applied. Distinct differences between the sample B22 FA taken within the contamination plume and the sample B53 FA taken downstream were found. Comparison with a model compound for metabolites and humic substances revealed that due to the downstream passage the characteristics of the dissolved organic matter became more humic-like. The assignment of single classes of compounds in the sample B22 FA is discussed in terms of their synchronous fluorescence spectra and fluorescence decay time distribution.  相似文献   

18.
To explore whether quinone moieties are important in chromophoric dissolved organic matter (CDOM) photochemistry in natural waters, hydrogen peroxide (H2O2) production and associated optical property changes were measured in aqueous solutions irradiated with a Xenon lamp for CDOM model compounds (dihydroquinone, benzoquinone, anthraquinone, napthoquinone, ubiquinone, humic acid HA, fulvic acid FA). All compounds produced H2O2 with concentrations ranging from 15 to 500 μM. Production rates were higher for HA vs. FA (1.32 vs. 0.176 mM h−1); values ranged from 6.99 to 0.137 mM h−1 for quinones. Apparent quantum yields (Θapp; measure of photochemical production efficiency) were higher for HA vs. FA (0.113 vs. 0.016) and ranged from 0.0018 to 0.083 for quinones. Dihydroquinone, the reduced form of benzoquinone, had a higher production rate and efficiency than its oxidized form. Post-irradiation, quinone compounds had absorption spectra similar to HA and FA and 3D-excitation–emission matrix fluorescence spectra (EEMs) with fluorescent peaks in regions associated with CDOM.  相似文献   

19.
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   

20.
Structural aspects of humic substances (HSs) in marine waters of Engaño Bay (Atlantic Ocean) and water from the Chubut River (Patagonia, Argentina) were compared. The HSs were isolated, purified, and analyzed using a multiple-method approach for structural characterization: elemental analysis, nuclear magnetic resonance (13C and 1H NMR), infrared spectroscopy (FTIR), UV-visible absorption and fluorescence. Similarities between the marine and freshwater components were evaluated on the basis of N and O contents, H/C and C/N atomic ratios, infrared bands from nitrogen-containing and carboxylic groups, percentage of functional groups obtained from NMR spectra, spectral slope coefficient of absorption spectra, absorbance ratios at 250 and 365 nm (E 2/E 3), aromaticity, excitation–emission matrices and fluorescence quantum yield. Both the Engaño Bay and Chubut River waters have HSs that are mainly composed of fulvic acids (FAs); although they are very similar, they may be distinguished from one another. Similarities include the predominance of aliphatic carbon content (low aromatic content); however, the water bodies differed in their content of proteins and carboxylic acids. The Engaño Bay FAs have mainly an aquatic origin; although the Chubut River FAs suggest a similar aquagenic origin, there is also evidence of contributions from pedogenic FAs.  相似文献   

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