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PubMed2006

Removal of pharmaceuticals in drinking water treatment: effect of chemical coagulation.

The removal of selected pharmaceuticals (diclofenac, ibuprofen, bezafibrate, carbamazepine and sulfamethoxazole) by chemical coagulation was studied. Jar test experiments were done in MilliQ water, in lake water and in commercial humic acid solutions using aluminium (pH 6) and ferric sulphate (pH 4.5). The concentrations of the pharmaceuticals in the studied water samples were determined by HPLC analysis and UV detection. In MilliQ water coagulation, the pharmaceuticals were poorly removed (< 10%) with the exception of diclofenac, which was removed up to 66% with ferric sulphate. This compound was also the only pharmaceutical removed (30%) during the lake water coagulation with ferric sulphate. In the presence of dissolved humic matter, diclofenac as well as ibuprofen and bezafibrate could be removed by ferric sulphate coagulation. The removal of diclofenac reached a maximum of 77%, while 50% of ibuprofen and 36% of bezafibrate were removed. Hence, a high amount of high-molecular-weight dissolved organic matter enhanced the removal of ionisable pharmaceuticals. The non-ionisable compounds, carbamazepine and sulfamethoxazole, were not affected by the coagulation processes studied. Although conditions such as high humic material content, low coagulation pH and ferric coagulant increase the removal of certain ionic pharmaceuticals, it can be concluded that by coagulation it is not possible to entirely remove pharmaceuticals from water.

Alum Compounds↗

PubMed2000

Mobilization and retardation of uranium DOC species at three mine piles in Schlema/Alberoda, Saxony, Germany.

The modeling of geo-chemical processes needs the detailed and comprehensive knowledge of all chemical interactions existing in the flow path of waste dumps, subsoil and aquifer. This includes the adsorption, displacement and transport of heavy metal species of fulvic and humic acids, which represent the main amount of DOC in the liquid/solid system of the flow path. Comparative measurements of DOC concentrations in the input and output flow at the three waste dumps in the district Schlema/Alberoda indicated that DOC is produced and/or supplied within the waste dumps. The speciation of heavy metal compounds of fulvic and humic acids was achieved by means of sequential chromatographic analysis SCA and isoelectric focusing IEF. Between 5% and 20% of uranium exist in the flow path in the form of stable fulvic and humic acid species. Their distribution coefficients are strongly correlated with the pH values of the geo-chemical system.

Benzopyrans↗

PubMed2006

Kinetics of chloroform formation from humic and fulvic acid chlorination.

Chloroform formation from chlorination of aquatic humic and fulvic acid solutions was studied. Second order overall kinetic model was assumed, first order with respect to chlorine and precursor content. Rate constants have been measured, resulting in values that varied significantly with reaction conditions, in the range of 0.177-7.206 [L/ mmol h], mainly for fulvic acid. The activation energy deduced from experiments carried out at different temperatures also increased notably when decreasing pH from 8 to 7. Increases of up to 60% were computed, where highest values were measured for humic acid. It is noteworthy the dependence observed on reaction time: higher activation energy resulted for longest reaction periods. Differences in the range of 40% have been reported. This effect is attributed to the existence of simultaneous reactions, each with different activation energy, competing for trihalomethanes formation.

Benzopyrans↗

PubMed2006

Bioavailability and toxicity of heavy metals in the presence of natural organic matter.

The effect of humic acids (HA) on the toxicity of copper, zinc and lead was investigated in this study, using the photobacterium Vibrio fischeri (Microtox test) as a test organism. The metal species and the complexation capacity of HA were predicted using model WinHumicV for speciation modeling. The toxicities of copper and lead were generally comparable, while the toxicity of zinc was lower than the ones of the other two method. The toxicity of copper decreased with the addition of HA, while the toxicity of zinc remained almost constant. The complexation of Zn with HA was low. Thus the presence of HA did not significantly influence the toxicity of Zn. For Cu and Zn, the free metal ion species showed to be basically responsible for the toxicity of these metals, while for Pb the chlorocomplexes and Pb-HA complexes contributed to the toxicity of Pb, indicating that the toxicity of heavy metals depends not only on the free metal ion species concentration but on different metal species that may be bioavailable.

Aliivibrio fischeri↗

PubMed2006

Water solubility enhancement effects of some polychlorinated organic pollutants by dissolved organic carbon from a soil with a higher organic carbon content.

To elucidate the role of a soil humic acid (HA) in the transport of polychlorinated organic pollutants (PCOPs), such as polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans and coplanar-polychlorinated biphenyls, their partition coefficients (Kdoc) into an HA were compared with their adsorption coefficients (KOC) for a soil with a higher organic carbon (OC) content. The soil sample (ando soil) used in the present study was collected in the same location as the HA. The log Kdoc values were positively correlated with logarithm of octanol-water partition coefficients (log KOW) of the PCOPs, indicating that the partitioning of PCOPs into the HA was mainly due to hydrophobic interactions. However, the correlation between log Kdoc and log KOC was negative. This can be attributed to the enhanced water solubility of the PCOPs as the result of the dissolved organic matter from the soil. That is, when the more hydrophobic PCOPs with higher log KOW values are partitioned into the HA, then the larger quantities of PCOPs that are partitioned into the HA are able to dissolve in the aqueous phase. These results suggest that, in a soil with a higher OC content, the HA can serve as more effective carrier of PCOPs from the soil to an aquatic environment.

Adsorption↗

PubMed1982

[Degradation reactions of a carbamate herbicide, chlorbufam: effect of soil factors].

Kinetics of degradation of chlorbufam is determined in aqueous solution, in aqueous solution with humic acids, argilo-humic complexes, soil and sterile soil. The adsorption is also evaluated in this different fractions. The adsorption process has a protecting effect and the chlorbufam is not chemically degraded when it is adsorbed on organic matter. The biodisponibility is also decreased by adsorption.

Adsorption↗

PubMed1985

Subchronic toxicology of humic acid following chlorination in the rat.

A subchronic 90-d study was conducted with chlorinated and nonchlorinated humic acids using male Sprague-Dawley rats. Body weight gain, terminal organ and body weights, food and fluid consumption, clinical chemistries, hematological parameters, and urinalyses were determined for all animals. Selected organs were examined microscopically. Significant findings were confined to those rats given the high dose of chlorinated humic acid (1.0 g/l total organic carbon). The terminal body weight and average weekly body weight gain were significantly lower (p less than 0.05) in the high-dose group as compared to the distilled-water control group. This difference can be partially explained by a 16% lower daily fluid consumption. The average weight of the kidneys was significantly higher in the 1.0-g/l chlorinated humic group as compared to distilled-water controls. Hematological parameters and clinical chemistry values were normal in all treatment groups. The most significant finding was the increased incidence and severity of hematuria in the 1.0-g/l chlorinated humic acid group. A thorough histopathological examination of the entire urinary tract indicated that the most likely cause of the more severe incidences of hematuria in the rats was caused by crystalline deposits in the renal pelvis.

Administration, Oral↗

PubMed2003

The effect of metal ions on humic acid removal and permeation properties in an ultrafiltration system.

With a view to improving the removal of humic acid from aqueous solution, the effect of metal ion addition on the separation of humic acid from water in an utrafiltration (UF) system was investigated. The valence of the metal ion and the molar ratio of humic acid to metal ion strongly affected the permeation flux during ultrafiltration. It was found that the ionic strength, dissociation constant and operating pressure were not major factors affecting the separation performance of the ultrafiltration process. As well as indicating that a suitable ratio of humic acid to metal ion and valence of metal ion were the key factors in improving separation efficiency. The results also showed that separation of humic acid depended on the level of formation of humic acid-metal ion complexes, and on the degree of fouling on the membrane surface.

Filtration↗

PubMed2003

Sensitive and reproducible quantification of Cu2+ by stripping with a carbon paste electrode modified with humic acid.

The preparation of a humic acid modified carbon paste electrode (HA-MCPE) as well as the behavior of its surface as complexing agent toward Cu2+ cations are described. Electrochemical studies of the reduction of the complexed cations and of the anodic stripping oxidation of the resulting copper are outlined. The anodic stripping current was correlated to the Cu2+ concentrations. A well-defined method for the preparation of reproducible electrodes is described. The effects on the current response obtained by cyclic voltammetry of the humic acid ratio, the pH, the accumulation time, and the speed scan rate were studied. Calibration graphs were linear over the range 3 x 10(-8)-10(-5) mol L(-1) Cu2+ and the relative standard deviation (R.S.D.) was 1.2% (n=5) for [Cu2+] = 1.6 x 10(-5) mol L(-1). 5 min accumulation time for [Cu2+] > 10(-7) mol L(-1) and 10 min for [Cu2+] < 10(-7) mol L(-1) were sufficient to permit sensitive and reproducible measurements. The electrode was successfully used to measure Cu2+ in real samples and the results were compared to those obtained by the standard method with differential pulse anodic stripping voltammetry.

Carbon↗

PubMed2001

Interaction of imidazolinone herbicides with soil humic acids. Experimental results and molecular modeling.

Adsorption and desorption isotherms of the herbicides imazapyr, imazethapyr and imazaquin on a soil humic acid have been performed at pH 2.8 and 4.0 (below and above the pKa of the herbicides). At both pH, adsorption increased according to the lipophilic character of the molecules (imazapyr < imazethapyr << imazaquin). The extent of adsorption was higher at pH 2.8 than at pH 4.0 because of the partial ionization of the carboxylic groups of both herbicides and humic acids at increasing pH. Desorption of imazapyr and imazethapyr was nearly complete at pH 4 and higher than 60% at pH 2.8 while desorption of imazaquin was 45 and 8% at pH 4 and 2.8, respectively. No differences between adsorption isotherms at 10 degrees C and 25 degrees C were observed a pH 4.0 indicating that adsorption involved very weak bonds while at pH 2.8, adsorption was higher at 10 degrees C than at 25 degrees C indicating an exothermic process. The isosteric enthalpy of adsorption of each herbicide was low (about -1 kJoule mole(-1)) suggesting that low energetic bonds were involved. Adsorption on different humic acids has indicated that for each herbicide, the extent of adsorption expressed as Kd was correlated with the amount of carboxylic and aromatic groups of humic acids suggesting that hydrogen bonding and/or charge-transfer complexes formation could take place. Molecular modeling and geometry optimization of humic acid and soil organic matter (SOM) herbicide complexes were also performed. The results obtained with this theoretical approach gave a consistent chemical interpretation of the experimental results. To the best of our knowledge this is the first report to contribute to a better understanding of site-specific bonding of herbicides in SOM complexes by nanochemical modeling and distinct energy descriptors.

Adsorption↗

PubMed2001

Adsorption of imidazolinone herbicides on ferrihydrite-humic acid associations.

Adsorption of the imidazolinone herbicides imazapyr, imazethapyr and imazaquin was studied on two binary systems (ferrihydrite-humic acid) prepared by treating ferrihydrite (Fh) immediately after its precipitation with a soil humic acid (HA) at different loadings (4% and 8% HA content), and on a blank ferrihydrite sample prepared in the same way, but without HA addition. Imidazolinone adsorption on pure Fh and on the 4% Fh-HA decreased with increasing of the herbicide hydrophobicity (imazaquin<imazethapyr<imazapyr), whereas on the 8% Fh-HA system the order of adsorption was nearly the same, indicating that higher amounts of HA on Fh increase the hydrophobicity of the surface and thus increases its affinity for the herbicides, specially for imazaquin. Adsorption was also enhanced by low pH values and slight changes in pH enhanced the contribution of each component in adsorption. Both the nature of the surface exposed and its ability to interact with herbicides are greatly altered by the mutual interaction of Fh and HA. The results show that albeit artificial polyphasic associations are more representative of the real situation than single model components and are thus better indicators of the behaviour of a given herbicide in the soil.

Adsorption↗

PubMed2001

Accumulation and fractionation of copper, iron, manganese, and zinc in calcareous soils amended with composts.

Amending soils with compost may lead to accumulation of metals and their fractions at various concentrations in the soil profile. The objectives of this study were to determine 1) the accumulation of Cu, Fe, Mn, and Zn with depth and 2) the distribution of water soluble, exchangeable, carbonate, Fe-Mn oxides, organic and residual forms of each metal in soils amended with MSW compost, co-compost, biosolids compost and inorganic fertilizer (as control). Total concentrations of Cu, Fe, Mn and Zn were concentrated in the 0-22 cm soil layer and scant in the rock layer. These metals were in the decreasing order of Fe >> Mn > Zn > or = Cu. Copper, Fe, and Zn were predominantly in the residual form followed by fractions associated with Fe-Mn oxides, carbonate, organic, exchangeable and water soluble in all treatments except MSW compost amended soil where the organic fraction was higher than the carbonate fraction. In fertilizer, co-compost and biosolids compost treated soils Mn concentrated mainly in the Fe-Mn oxides form followed by residual, carbonate, and organic forms whereas, in MSW compost treated soil the same pattern occurred except that Mn organic fraction was higher than that in the carbonate form. The MSW compost has a greater potential to be used as a soil amendment to supply plants with Cu, Mn and Zn than other treatments in calcareous soils of south Florida.

Carbonates↗

PubMed2001

Sorption and desorption of the herbicide alachlor on humic acid fractions from two vermicomposts.

The present study focuses on the analysis of two vermicomposts, that have been used as alternative sources of restitution of soil organic matter, as well as sources of nutrient replacements. For this purpose, two samples of vermicomposts from different Brazilian regions (São Carlos-SP and Londrina-PR) were characterized according to their humic acid content. Both samples had a pH value near 7.0, and the humic acids present showed high cationic exchange capacities and low values for the C/N ratios. The infrared spectra showed bands that suggested the presence of aliphatic and aromatic components bound to phenolic, carboxylic and amide groups. The effect of vermicompost added to soil on the application of alachlor was evaluated. Alachlor sorption, Freundlich isotherms and alachlor desorption curves in the soil matrix and the vermicompost/soil mixture matrix were determined.

Acetamides↗

PubMed2002

Influence of soil organic matter on the leaching of polycyclic aromatic hydrocarbons in soil.

Polycyclic aromatic hydrocarbons (PAHs) are one of the main classes of contaminants in the terrestrial environment. Aside from total organic carbon, the ratio among the different organic matter fractions [dissolved organic matter, fulvic acid (FA), humic acid (HA) and humin] can also affect the mobility of these hydrocarbons in soils. In this study the effect of the whole organic carbon pool has been compared with that of HA and FA on the translocation of four PAHs (biphenyl, fluorene, phenanthrene and pyrene) in soil columns. Oxidized and untreated soil columns with and without HA or FA, were prepared, spilled with hydrocarbons and leached with a 0.01 M CaCl2 solution. The influence of HA and FA on PAH translocation was investigated through determinations of the PAH contents and total organic carbon (TOC) in the layers of the columns. All molecules were moved vertically by the percolating solutions, their concentrations decreasing with depths. The nonoxidized soil tended to retain more PAHs (96%) than the oxidized one (60%), confirming that organic matter plays an important role in controlling PAH leaching. The whole organic matter pool reduced the translocation of pollutants downward the profile. The addition of HA enhanced this behaviour by increasing the PAH retention in the top layers (7.55 mg and 4.00 mg in the top two layers, respectively) while FA increased their mobility (only 2.30 and 2.90 mg of PAHs were found in the top layers) and favoured leaching. In fact, in the presence of HA alone, the higher amounts of PAHs retained at the surface and the good correlation (r2=0.936) between TOC and hydrocarbon distribution can be attributed to a parallel distribution of PAHs and HA, while in the presence of FA, the higher mobility of PAHs can be attributed to the high mobility of the humic material, as expected by its extensive hydrophilic characteristics.

Adsorption↗

PubMed2002

Abiotic degradation of imazethapyr in aqueous solution.

The photodegradation of imazethapyr [2-(4,5-dihydro-4-méthyl-4-(1-méthylethyl)-5-oxo-1H-imidazol-2-yl)-5-ethyl-3-pyridinecarboxylic acid] in aqueous solution in the presence of titranium dioxide (TiO2) and humic acids (HA) at different ratios of herbicide/TiO2 and herbicide/humic acids was studied at pH 7.0. Irradiation was carried out with polychromatic light using Heraeus apparatus equipped with xenon lamp to simulate sunlight having a spectral energy distribution similar to solar irradiation (>290 nm). The concentration of remaining herbicide was followed using a High Pressure Liquid Chromatograph (HPLC) equipped with UV detector at 230 nm. In pure aqueous solution imazethapyr degrades slowly and the photodegradation leads to the formation of two metabolites labelled A and B. The presence of TiO2 caused enhancement of the degradation rate. The presence of HA induced an increase of the photodegradation of the pesticide with respect to pure aqueous solution.

Chromatography, High Pressure Liquid↗

PubMed2004

Pyrethrins and piperonyl butoxide adsorption to soil organic matter.

The adsorption and mobility of pyrethrins (Pys), the major insecticidal components obtained from the pyrethrum daisy Tanacetum cinerariifolium, and piperonyl butoxide (PBO), a pyrethrum synergist, were determined in soil using batch-equilibrium and reverse-phase thin-layer chromatographic techniques. Two soil management practices were used, soil mixed with yard waste compost (COM) at 50 t acre(-1) on dry weight basis and no-mulch (NM) bare soil. Adsorption isotherm experiments were carried out using known concentrations of Pys (Py-I and Py-II) and PBO mixed with known amounts of COM or NM soil at constant temperature and pressure until equilibrium was attained. Pys and PBO in soil extracts were purified and concentrated using solid-phase extraction cartridges containing C18-octadecyl bonded silica. Pys and PBO residues were quantified using a high-performance liquid chromatograph equipped with a UV detector. Adsorption studies showed that compost amended soil adsorbed more Pys and PBO than native (NM) soil. Py-I adsorption was greater than Py-II and PBO. Adsorption of Pys and PBO to humic and fulvic acids was also studied by reverse-phase thin layer chromatography (RPTLC). Results indicated that humic acid, a significant component of organic matter, reduced Pys and PBO mobility. Pys and PBO mobility decreased as the concentration of humic acid in the mobile phase increased.

Adsorption↗

PubMedDate not supplied

Protection by natural blackwater against disturbances in ion fluxes caused by low pH exposure in freshwater stingrays endemic to the Rio Negro.

Stenohaline freshwater stingrays (Potamotrygon spp.) are endemic to the very dilute (Na(+), Cl(-), Ca2(+) 300 micromol L(-1) in reference water (low DOC) to about 100 micromol L(-1) in blackwater (high DOC). In reference water, both JNain and JClin were inhibited >90%, both JNaout and JClout more than doubled, and J(Amm) did not change at pH 4.0. In blackwater, the inhibition of influxes was attenuated, the increases in outflux did not occur, and J(Amm) increased by 60% at pH 4.0. Addition of 100 micromol L(-1) Ca(2+) to reference water prevented the increases in JNaout and JClout and allowed J(Amm) to increase at pH 4.0, which demonstrates that the gills are sensitive to Ca(2+). However, addition of Ca(2+) to blackwater had no effect on the responses to pH 4.0. Addition of commercial humic acid to reference water did not duplicate the effects of natural Rio Negro blackwater at the same DOC level; instead, it greatly exacerbated the increases in JNaout and JClout at low pH and prevented any protective influence of added Ca(2+). Thus, blackwater DOC appears to be very different from commercial humic acid. Biogeochemical modeling indicated that blackwater DOC prevents Ca(2+) binding, but not H(+) binding, to the gills and that the protective effects of blackwater cannot be attributed to its higher buffer capacity or its elevated Al or Fe levels. Natural DOC may act directly at the gills at low pH to exert a protective effect and, when doing so, may override any protective action of Ca(2+) that might otherwise occur.

Ammonia↗

PubMed2006

Brown ground: a soil carbon analogue for the green world hypothesis?

For many decades, ecologists have asked what prevents herbivores from consuming most of the plant biomass in terrestrial ecosystems, or "Why is the world green?" Here I ask the analogous question for detritivores: what prevents them from degrading most of the organic material in soils, or "Why is the ground brown?" For fresh plant detritus, constraints on decomposition closely parallel constraints on herbivory: both herbivore and decomposer populations may be controlled by plant tissue chemistry from the bottom up and predators from the top down. However, the majority of soil carbon is not plant litter but carbon that has been consumed by detritivores and reprocessed into humic compounds with complex and random chemical structures. This carbon persists mainly because the chemical properties of humic compounds and interactions with soil minerals constrain decomposition by extracellular enzymes in soil. Other constraints on decomposers, such as nutrient limitation of enzyme production and competition with opportunistic microbes, also contribute to brown ground. Ultimately, the oldest soil carbon persists via transformation into complex molecules that are impervious to enzymatic attack and effectively decoupled from processing by the soil food web.

Carbon↗