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Sorption of polycyclic aromatic compounds to humic and fulvic acid HPLC column materials.

Two different humic acids (HA) and a fulvic acid (FA) were chemically immobilized to a high performance liquid chromatography (HPLC) silica column material. The immobilization was performed by binding amino groups in HA/FA to the free aldehyde group in glutardialdehyde attached to the silica gel. The HPLC column materials were compared with a blank column material made by applying the same procedure but without immobilizing HA or FA. Also, a column was made by binding carbonyl groups in HA to amino groups attached to the silica gel. The humic substances were selected to secure appropriate variation of their structural features. The retention factors of 45 polycyclic aromatic compounds (PAC) to the four columns were determined by HPLC. The advantage of the technique is a large number of compounds can easily be studied. The binding procedure does not appear to cause a drastic selection between the HA molecules. The k' values obtained for the two Aldrich HA columns agree in general reasonably. The retention or sorption of the compounds increased with the size of the PAC and the number of lipophilic substituents, but decreased when polar substituents were present. The PAC retention was much stronger to the two HA columns than to the FA and blank column, both for hydrophobic polycyclic aromatic hydrocarbons (PAH) and the polar PAC. Other factors impacting the PAC binding may be specific interactions with HA and the ionic strength of the aqueous phase. The technique has been applied to do direct determinations of Koc.

Adsorption↗

PubMed2006

Natural organic matter (NOM) induces oxidative stress in freshwater amphipods Gammarus lacustris Sars and Gammarus tigrinus (Sexton).

Humic substances comprise the majority of natural organic matter (NOM) on Earth, including dissolved organic matter in freshwater systems. Recent studies show that these substances directly interact with aquatic organisms as chemical stressors. The aim of the present study was to investigate the mode of action of dissolved NOM on the freshwater amphipods Gammarus lacustris Sars and Gammarus tigrinus (Sexton), and in particular, to determine if NOM induces or promotes internal oxidative stress. NOM was isolated by reverse osmosis from a brown-water lake in Brandenburg State, Germany. Oxidative stress markers, such as lipid peroxidation, cell internal hydrogen peroxide concentration, as well as peroxidase, catalase and glutathione S-transferase activities, were quantified. Exposure of both amphipod species to NOM caused a significant increase in lipid peroxidation, hydrogen peroxide concentration, catalase, peroxidase and glutathione S-transferase activities. Both species showed a two-stage antioxidant response: the first stage allowed the organisms to effectively eliminate ROS and to protect cells from damage, whereas the second stage leads to H2O2 accumulation in combination with destruction of lipid structures in the cells and, finally, functional damage or even death of the organism.

Amphipoda↗

PubMed2006

Sorption of humic acids and alpha-endosulfan by clay minerals.

Sorption of alpha-endosulfan by kaolinite and montmorillonite alone and in the presence of sorbed and dissolved humic acid (HA) was investigated (pH 8 and 25 degrees C). Three types of HA, Elliot soil HA (EHA), Peat HA (PHA), and Summit Hill HA (SHHA), were used to represent typical humic substances found in soils. For sorption of HA by either mineral, Freundlich sorption coefficient (K(f)) values appeared to decrease in the order of EHA > PHA > SHHA, which followed increasing polarity (expressed as the O/C atomic ratio) and decreasing percent-carbon content. For both clays, sorption of alpha-endosulfan by the HA mineral complex was greater than for sorption by the clay alone. Sorption of alpha-endosulfan by the HA mineral complexes followed the same order as the K(f) of the HAs (EHA > PHA > SHHA). Based on the amount of HA adsorbed by each mineral, organic carbon partition coefficients (K(oc)) were determined for sorption of alpha-endosulfan by two of the HA mineral complexes. The value of K(oc) for alpha-endosulfan sorption was greater for kaolinite EHA than kaolinite SHHA. However, the opposite trend was found with the montmorillonite HA complexes. Montmorillonite appeared to sorb alpha-endosulfan and/or HA with higher affinity than kaolinite, which likely is due to its 2:1 layer structure and higher surface area. Sorption of endosulfan diol, a hydrolysis product, by the minerals was much less than the parent pesticide.

Adsorption↗

PubMed2006

Effects of photodegradation of dissolved organic matter on the binding of benzo(a)pyrene.

Dissolved organic matter (DOM) in natural waters can bind various organic pollutants, and the affinity of this binding is strongly influenced by the chemical characteristics of the DOM and water pH. This study examined the effects of photochemically induced alteration of the DOM's chemical properties and water pH on the binding of benzo(a)pyrene (BaP). Time- and pH-series of solar-simulated irradiations were performed on a natural water sample and aqueous DOM solutions prepared from aquatic and soil humic substances. The binding affinity of BaP, expressed as a partition coefficient of a compound to DOM, decreased substantially after the DOM samples were irradiated over environmentally relevant radiation doses and pH ranges. The lowering of the pH due to the photoproduction of acidic products often partly offsets the reduction of the binding affinity caused by direct photoalteration of the DOM's chemical structure. The decrease of the binding affinity, after correction for the photoinduced pH change, was positively correlated with the decrease in the molecular weight and the aromaticity of the DOM in the course of irradiation. Increasing O(2) abundance accelerated the decrease of the binding affinity as a result of enhanced DOM photodegradation. Visible light played a more important role in reducing the molecular weight and aromaticity of the DOM than in reducing the content of dissolved organic carbon (DOC) via photoremineralization while the reverse was true for UV radiation, indicating that photochemical reduction of the binding affinity may occur in natural waters at depths greater than UV radiation can reach. A decrease of the affinity of DOM for binding BaP will increase the free dissolved fraction of BaP and thus its availability and toxicity to aquatic organisms. The results from this study may have similar implications for organic pollutants other than BaP.

Benzo(a)pyrene↗

PubMed1993

Stimulation of endothelin production in cultured human endothelial cells by fluorescent compounds associated with blackfoot disease.

The fluorescent compounds (FC) in humic substances isolated from the drinking water of endemic areas of blackfoot disease have been characterized as the causative factor of the disease. In this report we studied the effects of these fluorescent compounds on the synthesis and secretion of endothelin-1 by cultured human umbilical cord vein endothelial cells (HUVEC) in order to explore the possible pathological mechanism(s) of FC in the development of atherothrombotic vasculopathy in blackfoot disease. Incubation of confluent HUVEC with FC (100 micrograms/ml) enhanced endothelin mRNA expression. A sensitive ELISA method was developed to quantitate secreted endothelin antigen levels in conditioned medium. Incubation of confluent HUVEC cultures with different concentrations of FC (0-200 micrograms/ml) resulted in concentration-dependent enhanced production of endothelin. No significant changes in endothelin production were observed when subconfluent HUVEC cultures were incubated with FC. FC dose-dependently reduced the growth rate of subconfluent cultured HUVEC and exerted cytotoxic effects on the viability and integrity of confluent HUVEC monolayers. Since endothelin is one of the most potent vasoconstrictors affecting blood pressure and blood flow, and is mitogenic for smooth muscle cell proliferation, these results imply that the enhanced endothelin production and the reduced cell viability and growth rate induced by FC may contribute to the atherothrombotic vasculopathy observed in blackfoot disease.

Arterial Occlusive Diseases↗

PubMed2006

Iron humate as a low-cost sorbent for metal ions.

Iron humate produced as a waste by-product during an industrial manufacture of humic substances from low-rank brown coals was tested as a sorbent for the removal of metal cations--Cd (II), Cu (II), Co (II), Ni (II), Zn (II), TI (I), Eu (III), Cr (III)--as well as hexavalent chromium from waters. The Langmuir-type isotherms were used to describe the metal sorption; the respective equations may be derived and interpreted on the basis of a concept of surface-complexation reactions. Parameters of the sorption isotherms were estimated from experimental dependencies measured in a batch arrangement. The sorption capacities ranged from 0.024 mmol g(-1)for Co (II) to 0.324 mmol g(-1)for Tl(I). The metal uptake was affected by the presence of complexing agents (EDTA, salicylate, citrate), but this effect depends strongly on pH and the kind of complexing agent. The sorption of Cu (II) ions was suppressed in the presence of EDTA in an almost whole examined pH range (ca. 1-6.5) and in the presence of citrate at higher pH values (above pH 4). In the presence of salicylate, on the other hand, a slight sorption enhancement was observed. The metal sorption was suppressed also in the presence of anionic surfactant (sodium dodecylsulfate). Both in the presence as well as in the absence of complexing agents, the metal sorption showed a strong dependence on pH--the sorption was reduced considerably at low pH values below ca. 2. A typical working range for iron humate as a sorbent is ca. pH 3-5, where it exhibits a high buffering capacity, a sufficient stability and metal-binding capability.

Adsorption↗

PubMed2006

Theoretical study on fulvic acid structure, conformation and aggregation. A molecular modelling approach.

The ubiquitous presence of humic substances (HS), combined with their ability to provide multiple sites for chemical reaction, makes them relevant to numerous biogeochemical processes such as mineral weathering, nutrient bioavailability, and contaminant transport. The reactivity of HS depends on their functional group chemistry and microstructure, which are in turn influenced by the composition of the surrounding media. In order to help towards an understanding of structure conformations and aggregation process of HS in soils and waters and to get a better knowledge of these kinds of materials, a fulvic acid (FA) has been modelled as a function of its ionic state under different conditions. Our proposed theoretical model based on the Temple-Northeastern-Birmingham (TNB) monomer fits well with experimental observations on the solubility (dipolar moment) and electronic and vibrational spectra of FAs. The presence of water molecules has a great stabilization effect on the electrostatic energy; this effect is greater as ionized rate increases. In vacuum, the non-ionized aggregated species are more stable than monomers because of the increase in their interaction due to H-bonding and non-bonding forces. When the molecules are ionized, no aggregation process takes place. In solution, the FA concentration is a critical factor for the aggregation. The system containing two FA molecules probably did not form aggregates because its equivalent concentration was too low. When the concentration was increased, the system gave rise to the formation of aggregates. The ionic state is another critical factor in the aggregation process. The ionized FA has a higher electric negative charge, which increases the energetic barriers and inhibits the approximation of FA caused by the Brownian movement.

Animals↗

PubMed2004

Ultrafiltration of nonionic surfactants and dissolved organic matter.

A brownwater sample with a high content of humic substances (HS) was fractionated by multistage ultrafiltration (mst-UF) into five fractions with nominal molecular weights ranging from >30 to <1 kDa. Fractions were characterized with respect to molecular size distribution and structure. Size exclusion chromatography with online DOC detection revealed that mst-UF yielded fractions with decreasing Mp (molecular weight at peak maximum) and polydispersities from nominally large to small mst-UF fractions. 13C MAS NMR analysis showed that the content of carbohydrate structures decreased from the original sample toward smaller molecular weight (MW) fractions, which in turn contained more carboxylic groups and branched aliphatic structures. Specific UV absorbances (SUVA254) were highest in the >30 kDa fraction and decreased with decreasing MW. To evaluate whether separation mechanisms other than size exclusion were of importance during the fractionation, the behavior of low molecular weight model compounds (MC) with a range of polarities was studied. Recoveries decreased with increasing hydrophobicity of the MC. For selected nonylphenol ethoxylates and 4-nonylphenol the recovery correlated well with the hydrophile-lipophile balance value. The presence of dissolved organic matter (DOM) caused an additional loss of hydrophobic MC, possibly because of sorption of the compounds onto DOM fouling layers. The hydrophilic MC caffeine was recovered almost completely (85-86%) regardless of the DOM content of the model solution. It was concluded that size exclusion was the dominant fractionation mechanism for caffeine, whereas hydrophobic interactions played a major role during the mst-UF fractionation of nonpolar contaminants. For a better understanding of the behavior of polyfunctional molecules such as HS, the effect of other physicochemical properties needs to be investigated in further studies.

Caffeine↗

PubMed2003

Fluorescence characterization of the interaction of Al3+ and Pd2+ with Suwannee River fulvic acid in the absence and presence of the herbicide 2,4-dichlorophenoxyacetic acid.

In an effort to understand the role of environmental metal ions in the interaction of charged pesticides with humic substances, a fluorescence study of the interaction of the widely-used herbicide 2,4-dichlorophenoxyacetic acid (DCPAA) with Al(3+) and Pd(2+) and Suwannee River fulvic acid (SRFA) was undertaken. Initial fluorescence experiments on binary solutions clearly indicated that both Al(3+) and Pd(2+) strongly interact with both SRFA and DCPAA when alone in solution with the metal ion. Titrations of SRFA with Al(3+) at pH values of 4.0, 3.0 and 2.0 revealed decreased degrees of fluorescence emission enhancement (at lambda(emission, max)=424 nm) with decreasing pH, consistent with the expected loss of rigidity in the SRFA-Al(3+) complexes formed as pH is lowered. In contrast, titrations of SRFA with Pd(2+) at all of these pH values resulted in significant fluorescence quenching. Al(3+) additions to solutions of DCPAA at pH values above the pK(a) (2.64) of DCPAA resulted primarily in significant changes in the wavelength of maximum emission (without significant quenching or enhancement of emission intensity), while Pd(2+) additions to DCPAA solutions resulted primarily in very significant fluorescence quenching. The DCPAA fluorescence results strongly support the formation of an Al(3+)-DCPAA complex at pH values above the pK(a) of DCPAA. The fluorescence results obtained for solutions of Pd(2+) and DCPAA are best explained by a collisional quenching mechanism, that is, energy transfer from excited DCPAA molecules to Pd(2+) following the collision of these two species in solution. Excitation-emission matrix plots obtained on ternary solutions (at environmentally-relevant pH 4.0) containing SRFA, DCPAA and metal ions (i.e., either Al(3+) or Pd(2+)) provides evidence (especially for systems containing Al(3+)) for the existence of ternary complexes between fulvic acid species, the herbicide DCPAA and metal ion, suggesting (at least at pH 4.0, where the predominant DCPAA species is negatively-charged) that metal ions may function to "bridge" negatively-charged fulvic acids to negatively-charged pesticides.

2,4-Dichlorophenoxyacetic Acid↗

PubMed2001

Analytical determination of the microbial utilization and transformation of humic acids extracted from municipal refuse.

Humic substances are usually the refractory part of natural organic matter, and in a landfill they can retain inorganic and organic micropollutants. This study has investigated analytically whether humic acids (HA) extracted by use of alkali from either fresh municipal refuse or from refuse disposed of in a landfill for up to 12 months can resist microbial degradation under aerobic conditions. When added as a supplementary nutrient source, up to 63.6% of HA was utilized and this percentage was enhanced to a mean value of 88.5% when different HA preparations were used as the sole source of carbon. In cultures of a soil microbial community containing the same preparations as sole sources of nitrogen, HA was usually completely utilized. The remaining HA re-isolated from some microbial cultures were highly depleted in carbon and, simultaneously, the nitrogen content was enhanced. The FTIR spectra were indicative of strong participation of aliphatic structural units in the refuse-related HA preparations. Because of the microbial activity, different carbonaceous substances were primarily removed from the HA structure, and an increase in nitrogenous molecular groups became apparent. The structural transformations brought about by soil microorganisms "in vitro" corresponded to those occurring naturally in HA obtained from refuse aged for 12 months in a landfill.

Bacteria↗

PubMed2001

Effects of Additions of DOC on Pelagic Biota in a Clearwater System: Results from a Whole Lake Experiment in Northern Sweden.

An oligotrophic clearwater lake, initially characterized by a pronounced dominance of autotrophic phytoplankton and mostly by one species, the green alga Botryococcus, was subject to additions of dissolved organic carbon in the form of white sugar (sucrose) during two consecutive years. The hypothesis tested was that it is organic carbon per se, and not other possible effects of humic substances, that determines the differences in structure of the planktonic ecosystem between humic and clearwater lakes. The additions of DOC resulted in a significant increase in bacterial biomass and a decrease in the biomass of autotrophic phytoplankton. The biomass of mixotrophic and heterotrophic flagellates instead increased significantly, whereas no effects were found to propagate to higher trophic levels. As a result of the changes among biota, total planktonic biomass also decreased to a level typical of nearby humic lakes. We suggest that it is the carbon component of humic material and its utilization by bacterioplankton that determines the structure and function of the pelagic food web in humic lakes.

Journal Article↗

PubMed2001

Organic matter components and aggregate stability after the application of different amendments to a horticultural soil.

The effects of usual or recommended rates of application of five organic amendments (24 t/ha yr of MSW compost, sewage sludge, and ovine manure, 2.4 t/ha yr of commercial vermicompost, and 100 l/ha yr of a commercial humic acids solution) on the soil contents of organic matter, total humified substances, humic acids, carbohydrates and microbial gums, and the structural stability of aggregates were investigated. Four and five years after the beginning of the experiment, significant increments in most of the parameters studied were found after the application of organic residues, whereas the two commercial amendments did not produce any significant change, suggesting that rates recommended by the producers and imposed by their high prices are too low to be useful. MSW compost yielded the highest increases, even if the amount of organic matter applied as ovine manure was very similar. Organic matter and carbohydrates appeared to be the parameters most closely related to soil aggregate stability.

Agriculture↗

PubMed2004

Studies on the effect of humic acids and phenol on adsorption-ultrafiltration process performance.

Application of pressure-driven membrane processes, such as ultrafiltration (UF) and microfiltration (MF) for surface water treatment have become very popular during last decades. Membrane fouling by humic substances (HS) is one of the major limiting factors in these processes. In order to alleviate the unfavorable effects of the presence of HS in the feed on the process performance UF and MF are often combined with adsorption on powdered activated carbon (PAC). The main goal of the present study was to evaluate the effect of humic acid (HA) on membrane fouling during UF. Moreover, the effect of PAC addition to the feed on UF process, especially on flux decline was determined. The applicability of the adsorption-ultrafiltration (PAC/UF) system to purification of water containing low (phenol) and high molecular (HA) was also investigated. Three different polymer UF membranes, prepared from polysulfone (PSF), cellulose acetate (CA) or polyacrylonitrile (PAN) were applied. It was found that the membranes prepared from PSF and CA are very susceptible to fouling caused by HA. The permeate flux decreased for ca. 50% during UF of HA solution through the PSF membrane and for ca. 45%-through the CA membrane. In the case of the PAN membrane, a negligible effect of HA on the flux was observed. On the basis of the FTIR spectra it was found that the drop in the permeate flux through these membranes may result from interactions between the negatively charged functional groups present on the membrane surface, such as carboxyl groups (CA) and sulfone groups (PSF) with HA, which results in coating of the membrane surface with HA. When PAC was added to the feed containing HA, the permeate flux through the CA and PAN membranes was maintained on a practically unchanged level. However, in case of the PSF membrane, a 50% drop in the permeate flux in comparison with the flux value, when process was conducted without PAC addition was observed. That was supposed to be due to attractive forces among hydrophobic PAC particles, HA molecules and PSF membrane surface. The performed studies showed that the application of PAC/UF system was very effective in the removal of organic substances having both, low and high molecular weights. The role of PAC suspended in a feed in the PAC/UF system is the adsorption of low molecular organic compounds, which cannot be removed by UF alone.

Adsorption↗

PubMed1999

Increased sequestration of organic carbon in soil by hydrophobic protection

The impact of soil organic carbon dynamics on the global carbon cycle is still largely uncertain despite studies of agricultural activities and control emissions of greenhouse gases to the earth's atmosphere. Improved knowledge of organic matter dynamics should lead to reduction in CO(2 )emissions. We used stable carbon isotope analysis to detect small changes in organic carbon storage and turnover upon soil treatments with a (13)C-labeled aliphatic alcohol previously partitioned into soluble humic substances of varying hydrophobicity. We found that labeled organic carbon is increasingly protected from mineralization with increased hydrophobic character of humic matter. The stabilization of organic carbon by hydrophobic protection significantly reduced decomposition during incubation time in soil. Hydrophobic protection can become an useful tool to limit decomposition of fresh organic matter in soil and thus reduce CO(2) emission from agricultural soils on a global scale.http://link. springer.de/link/service/journals/00114/bibs/9086010/90860496. htm</HEA

Journal Article↗

PubMed1999

Determination photostability of selected agrochemicals in water and soil.

The photolysis of selected pesticides in aqueous solutions has been investigated. The photolysis produced different intermediate substances, which were also found to be soil and microbial degradation products. The phototransformation in the presence of TiO2 and humic substances leads to a disappearance of these compounds. The reaction rate is dependent on the semiconductor oxide and concentration. Photoproducts were isolated and characterized by different spectroscopic methods. Results from this study indicate that degradation products of isoproturon are more toxic on Daphnia magna than on the parent compound.

Animals↗

PubMed2000

On-line size-exclusion chromatography/electrospray ionisation mass spectrometry of aquatic humic and fulvic acids

Isolated aquatic humic and fulvic acids were analysed with on-line size exclusion chromatography/electrospray ionisation mass spectrometry (SEC/ESI-MS). An eluent composition which enabled electrospray ionisation was identified. The SEC separation improved interpretability of mass spectra and may open up new possibilities for molecular weight determination of humic substances. A linear dose-response relationship over a factor of 20 was obtained and the limit of detection was 50ng/uL for humic and fulvic acids. Spectral changes due to different ionisation conditions (pH and cone voltage) were investigated. A natural water sample from a Swedish lake was analysed. Copyright 2000 John Wiley & Sons, Ltd.

Journal Article↗

PubMed2003

Waste paper and clinoptilolite as a bulking material with dewatered anaerobically stabilized primary sewage sludge (DASPSS) for compost production.

Environmental problems associated with sewage sludge disposal have prompted strict legislative actions over the past few years. At the same time, the upgrading and expansion of wastewater treatment plants have greatly increased the volume of sludge generated. The major limitation of land application of sewage sludge compost is the potential for high heavy metal content in relation to the metal content of the original sludge. Composting of sewage sludge with natural zeolite (clinoptilolite) can enhance its quality and suitability for agricultural use. However, the dewatered anaerobically stabilized primary sewage sludge (DASPSS) contained a low concentration of humic substances (almost 2%), and the addition of the waste paper was necessary in order to produce a good soil conditioner with high concentrations of humics. The final results showed that the compost produced from DASPSS and 40-50% w/w of waste paper was a good soil fertilizer. Finally, in order to estimate the metal leachability of the final compost product, the generalized acid neutralization Capacity (GANC) procedure was used, and it was found that by increasing the leachate pH, the heavy metal concentration decreased. The application of the sequential chemical extraction indicated that metals were bound to the residual fraction characterized as a stabilize fractions.

Bacteria, Anaerobic↗

PubMed2001

Iron metabolism in anoxic environments at near neutral pH.

Anaerobic dissimilatory ferric iron-reducing and ferrous iron-oxidizing bacteria gain energy through reduction or oxidation of iron minerals and presumably play an important role in catalyzing iron transformations in anoxic environments. Numerous ferric iron-reducing bacteria have been isolated from a great diversity of anoxic environments, including sediments, soils, deep terrestrial subsurfaces, and hot springs. In contrast, only few ferrous iron-oxidizing bacteria are known so far. At neutral pH, iron minerals are barely soluble, and the mechanisms of electron transfer to or from iron minerals are still only poorly understood. In natural habitats, humic substances may act as electron carriers for ferric iron-reducing bacteria. Also fermenting bacteria were shown to channel electrons to ferric iron via humic acids. Whether quinones or cytochromes released from cells act as electron transfer components in ferric iron reduction is still a matter of debate. Anaerobic ferrous iron-oxidizing phototrophic bacteria, on the other hand, appear to excrete complexing agents to prevent precipitation of ferric iron oxides at their cell surfaces. The present review evaluates recent findings on the physiology of ferric iron-reducing and ferrous iron-oxidizing bacteria with respect to their relevance to microbial iron transformations in nature.

Journal Article↗