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PubMed2004

Separation of drug traces from water with particular membrane systems.

The purpose of the present project is to examine the applicability of certain natural biological and liquid membranes for the separation of drugs of environmental concern such as ibuprofen, diclofenac, carbamazepine, and sulfamethoxazol from dilute aqueous solutions. Different types of intestine parts of cattle, sheep, and pig were applied as biological flat sheet membranes after different modes of pretreatment. Best results were obtained with special parts of cattle appendix. The concentration of each drug in the aqueous feed phase was in the range of 0.1-10 mg (cm3)(-1), the pH-values adjusted between 8 and 10. Pure water was used as the permeation phase. The influence of experimental parameters such as stirring velocity, temperature, pH-value, salt concentration, and the presence of surfactants as well as humic substances was studied. Under all conditions chosen the combined drugs permeate simultaneously through the natural membranes as the permeation kinetics of the individual compounds are very similar, while humic compounds were retained. Additional treatment of the permeate with liquid or solid phase extraction techniques increases crucially the depletion of the drugs from the feed. The mass transfer of the pharmaceuticals through the liquid membranes was carried out in three-compartment transport cells and supported liquid membrane-chambers. The three-phase liquid bulk membrane systems consisted of an aqueous feed solution, an organic solvent (dihexyl ether, decane, undecane, or decanol) with and without a dissolved sulfonic acid, tertiary amine or Cu(II)-chelate compound as a liquid bulk membrane and an aqueous stripping solutions containing dilute solutiuons of Na2CO3, NaOH, HCl, or HClO4. The transport of the drugs shows some differences, which can be attributed to their acid/base-behavior and partition coefficients log Kow. High extraction yields were obtained for sulfamethoxazol and carbamazepine by using polar organic solvents. Maximum transport efficiencies were obtained for the acidic compounds ibuprofen and diclofenac. They were completely extracted by using dihexyl ether loaded with octane sulfonic acid. A pH-gradient between feed and strip increases the efficiency of the transport. Certain three-phase compositions were successfully utilized in supported liquid membrane systems (SLM) so that high enrichment factors (approximately 75) were achieved for traces of diclofenac and ibuprofen. The solid and liquid membrane systems employed aim for technical as well as analytical purposes, such as sample pretreatment prior to HPLC-UV or LC-MS analysis of drug traces.

Animals↗

PubMed1983

Endemic goiter in western Colombia.

Goiter continues to occur in some areas of western Colombia despite iodine supplementation for 30 years. In 1973-1977, an average goiter prevalence of 15% (range 1-42%) still persisted among schoolchildren of 41 localities. Significant relationships were found between goiter prevalence and both the geological composition of watersheds and bacterial contamination of water supplies. Together, these associations account for 80% of the observed variation in goiter prevalence. The presence of sedimentary rocks rich in organic matter (coals, shales, etc.) was the best indicator of disease. The second best indicator, presence of K. pneumoniae in the water source, was associated with lower goiter prevalence but, as in other investigations, contamination of the pipeline system (households and schools) with gram-negative bacteria was associated with higher disease rates. Thus, epidemiological evidence indicates a cause-effect relationship between sources of drinking water and the persistence and development of goiter in this part of the world. Furthermore, identification of resorcinol, phthalate esters, and sulfur-bearing organic compounds, possibly aliphatic disulfides, in the water supplying the endemic goiter district of Candelaria town in western Colombia adds experimental support to this hypothesis. Resorcinol is derived from coal and humic substances, high molecular weight complex polymeric organic compounds present in sedimentary rocks, soils and water. Resorcinol is goitrogenic in man and experimental animals. Phthalate esters, also related to humic materials, undergo biodegradation by gram-negative bacteria with production of intermediate metabolites possessing antithyroid activity. Like phthalates and resorcinol, organic disulfides have also been identified as water contaminants in other parts of the world, and are known to be potent antithyroid compounds. The goitrogenic effect of organic and bacterial pollutants in water supplies is more pronounced in segments of the population with dietary iodine deficiency--as seen prior to the iodine prophylaxis program--and/or poor socio-economic conditions. Studies are underway to provide both insight into the biogeochemical cycle of water-borne goitrogens and knowledge essential to the development of rapid, inexpensive, and precise methods for detecting and quantifying the offending agents, as well as devising effective sanitation techniques for their inactivation and/or elimination. The impact of such measures will be determined on goiter prevalence and other parameters of health and nutrition of the communities under study.(ABSTRACT TRUNCATED AT 400 WORDS)

Adolescent↗

PubMed2000

Humic Materials Offer Photoprotective Effect to Escherichia coli Exposed to Damaging Luminous Radiation.

The behavior of Escherichia coli immersed in aqueous systems amended with humic acids, under PAR, UV-A, UV-B, and simulated solar radiation was examined. Culturability, ability to elongate, functioning of the electron transport systems, and glucose uptake were assessed. Humic substances in the range from 1 to 50 mg L-1 protected cells from photoinactivation. Decrease in culturability and cellular activities was significantly (p <0.05) less in the presence of humic material. However, humic acids were not used as nutrients. Neither irradiated nor nonirradiated humic solutions (50 mg L-1) supported the growth of 105 cells ml-1. However, humic acids dissolved in 0.9% NaC1 efficiently absorbed light over wavelengths from 270 to 500 nm. Also, a photoprotective effect against simulated sunlight was observed when humic acids were not in contact with but rather enveloped the cellular suspensions in double-wall microcosms. The protection afforded by humic acids against luminous radiation likely derives from their ability to absorb these radiations and hence reduces the amount of energy reaching the cells.

Journal Article↗

PubMed1999

Double-disk solid-phase extraction: simultaneous cleanup and trace enrichment of herbicides and metabolites from environmental samples.

Phenylurea and triazine herbicides, including some metabolites, were isolated from water and soil extracts by solid-phase extraction using a layered system of two extraction disks, a method called double-disk solid-phase extraction. The first disk consisted of strong anion exchange (SAX) of 10-micron styrene divinylbenzene (SDB) particles embedded in Teflon, and the second disk was a C18 disk of 10-micron particles also embedded in Teflon. A volume of 500 mL of water or aqueous soil extract is passed through the layered system with the SAX disk first. The purpose of the SAX disk is to remove the humic and fulvic acids from the water or aqueous soil extract by ion exchange through their carboxyl groups. Even during methanol elution of herbicides, the humic substances remain bound to the SAX disk with > 85% retention. Elution with methanol results in more than 90% recovery of the herbicides from the layered extraction disks. Removal of the humic and fulvic acids results in greater sensitivity for diode array detection quantitation (0.05 micrograms/L for herbicides) by substantially reducing the absorbance of the humic peak on the LC chromatogram. The herbicides adsorb to the SAX disk either through hydrogen bonding to the anion-exchange sites or by hydrophobic interaction with the SDB surface of the anion-exchange disk. The method was tested for the analysis of natural water samples from the Mississippi Embayment, a cotton-growing area of the southeastern United States.

Chromatography, High Pressure Liquid↗

PubMed2003

Trichloroacetic acid in Norway spruce/soil-system. I. Biodegradation in soil.

Trichloroacetic acid (TCA) as a phytotoxic substance affects health status of coniferous trees. It is known as a secondary air pollutant (formed by photooxidation of tetrachloroethene and 1,1,1-trichloroethane) and as a product of chlorination of humic substances in soil. Its break-down in soil, however, influences considerably the TCA level, i.e. the extent of TCA uptake by spruce roots. In connection with our investigations of TCA effects on Norway spruce, microbial processes in soil were studied using 14C-labeling. It was shown that TCA degradation in soil is a fast process depending on TCA concentration, soil properties, humidity and temperature. As a result, the TCA level in soil is determined by a steady state between uptake from the atmosphere, formation in soil, leaching and degradation. The process of TCA degradation in soil thus participates significantly in the chlorine cycle in forest ecosystems.

Biodegradation, Environmental↗

PubMed2005

Effect of humic material on the bacterioplankton community composition in boreal lakes and mesocosms.

The bacterioplankton community composition in two Finnish forest lakes with different content of humic substances was studied by denaturing gradient gel electrophoresis (DGGE) and sequencing of the major bands. The same dominant bacterial phylotypes were detected in the bacterioplankton communities of clear-water Lake Ahvenlammi and humic Lake Sammalisto. For 4 years, in every water layer, Actinobacteria was the dominant and Verrucomicrobia the second most common phylum. In the hypolimnion, other dominant phyla were also found. We set up a mesocosm experiment to assess the effect of a sudden load of allochthonous humus extract to the bacterioplankton community composition. Changes in the bacterial communities were followed in four control and four humus extract-added mesocosms for 50 days. In the humic mesocosms the phylotypes of allochthonous Proteobacteria arriving with the humus extract were initially prevalent but disappeared during the first weeks. After this the Actinobacteria-dominated communities resembled the bacterioplankton communities of the control mesocosms and Lake Ahvenlammi. Towards the end of the experiment the community patterns in all the mesocosms started to change slightly because of erratic occurrence of new proteobacterial phylotypes. Thus the effects of a sudden load of allochthonous humic material and bacteria to the bacterioplankton community composition were transient.

Actinobacteria↗

PubMed1988

Impact of bleached kraft mill effluents on drinking water quality.

Bleaching effluents from kraft pulp mills contain large quantities of chlorinated organic compounds, some of which are mutagenic. Mutagenic chloro-organic compounds are also formed as by-products in chlorination of drinking water. The work reported here was a combined field and laboratory study aimed at comparing the evidence of health risks from pulp mill contaminants in drinking water, with corresponding evidence from normal, chlorine disinfection by-products. The study was performed in a Swedish river basin with a large, public water works located downstream from a bleached kraft mill. Chemical analyses (gas chromatography and determination of adsorbable organic halogen) and bioassays for mutagenic activity (bacterial and mammalian cell bioassays) were performed on samples of river water, drinking water and laboratory produced drinking water. The study showed that the bleached kraft effluents caused a considerable, long-range transport of chloro-organic substances in the receiving waters, and a substantial increase in the total amount of organic chlorine in drinking water produced downstream from the mill. As regards Ames mutagenic compounds, however, chlorination of naturally occurring humic substances during the chlorine disinfection step in drinking water production, proved to be a far more important source. The contribution of volatile chloro-organic compounds from the kraft mill was also much smaller than the contribution from normal disinfection by-products. The chromosome aberration tests gave no clear evidence of a positive response for any of the samples tested.

Cells, Cultured↗

PubMed2002

Complexation with dissolved organic matter and solubility control of heavy metals in a sandy soil.

The complexation of heavy metals with dissolved organic matter (DOM) in the environment influences the solubility and mobility of these metals. In this paper, we measured the complexation of Cu, Cd, Zn, Ni, and Pb with DOM in the soil solution at pH 3.7-6.1 using a Donnan membrane technique. The results show that the DOM-complexed species is generally more significant for Cu and Pb than for Cd, Zn, and Ni. The ability of two advanced models for ion binding to humic substances, e.g., model VI and NICA-Donnan, in the simulation of metal binding to natural DOM was assessed by comparing the model predictions with the measurements. Using the default parameters of fulvic and humic acid, the predicted concentrations of free metal ions from the solution speciation calculation using the two models are mostly within 1 order of magnitude difference from the measured concentrations, except for Ni and Pb in a few samples. Furthermore, the solid-solution partitioning of the metals was simulated using a multisurface model, in which metal binding to soil organic matter, dissolved organic matter, clay, and iron hydroxides was accounted for using adsorption and cation exchange models (NICA-Donnan, Donnan, DDL, CD-MUSIC). The model estimation of the dissolved concentration of the metals is mostly within 1 order of magnitude difference from those measured except for Ni in some samples and Pb. The solubility of the metals depends mainly on the metal loading over soil sorbents, pH, and the concentration of inorganic ligands and DOM in the soil solution.

Hydrogen-Ion Concentration↗

PubMed2006

Soil aquifer treatment (SAT) as a natural and sustainable wastewater reclamation/reuse technology: fate of wastewater effluent organic matter (EfOM) and trace organic compounds.

Through the use of innovative analytical tools, the removal/transformation of wastewater effluent organic matter (EfOM) have been tracked through soil aquifer treatment (SAT). While the total amount of EfOM is significantly reduced by SAT, there are trends of shorter term versus longer term removals of specific EfOM fractions. The preferential removal of non-humic components (e.g., proteins, polysaccharides) of EfOM occurs over shorter travel times/distances while humic components (i.e., humic substances) are removed over longer travel times/distances, with the removal of both by sustainable biodegradation. Dissolved organic nitrogen (DON), a surrogate for protein-like EfOM, is also effectively removed over shorter term SAT. There is some background humic-like natural organic matter (NOM), associated with the drinking water source within the watershed, that persists through SAT. While most effluent-derived trace organic compounds are removed to varying degrees as a function of travel time and redox conditions, a few persist even through longer term SAT.

Adsorption↗

PubMed2003

Tangential-flow ultrafiltration: a versatile methodology for determination of complexation parameters in refractory organic matter from Brazilian water and soil samples.

In this work the copper(II) complexation parameters of aquatic organic matter, aquatic and soil humic substances from Brazilian were determined using a new versatile approach based on a single-stage tangential-flow ultrafiltration (TF-UF) technique (cut-off 1 kDa) and sensitive atomic spectrometry methods. The results regarding the copper(II) complexation capacity and conditional stability constants obtained for humic materials were compared with those obtained using direct potentiometry with a copper-ion-selective electrode. The analytical procedure based on ultrafiltration is a good alternative to determine the complexation parameters in natural organic material from aquatic and soil systems. This approach presents additional advantages such as better sensibility, applicability for multi-element capability, and its possible to be used under natural conditions when compared with the traditional ion-selective electrode.

Brazil↗

PubMed2004

Simultaneous determination of endocrine disrupting phenolic compounds and steroids in water by solid-phase extraction-gas chromatography-mass spectrometry.

A solid-phase extraction (SPE)-gas chromatography (GC)-mass spectrometry (MS) analytical method for the simultaneous separation and determination of endocrine disrupting chemicals (EDCs) from water samples is described in detail. Important and contrasting EDCs including estrone, 17beta-estradiol, 17beta-ethynylestradiol, 16beta-hydroxyestrone, 4-nonylphenol, bisphenol A and 4-tert-octylphenol were selected as the target compounds. The SPE technique, followed by the derivatisation with bis (trimethylsilyl) trifluoroacetamide was used for the extraction recoveries of target compounds from water samples. A number of parameters that may affect the recovery of EDCs, such as the type of SPE cartridges, eluents, as well as water properties including pH value, and concentration of salts and humic substances were investigated. It is shown that the Oasis cartridges produced the best recoveries of target EDCs while ethyl acetate was efficient in eluting EDCs from SPE cartridges. The recovery of some EDCs was enhanced by the addition of salt, but reduced by the increase in pH value and humic acid concentration. The optimised method was further verified by performing spiking experiments in natural river water and seawater matrices, with good recovery and reproducibility for all the selected compounds. The established method was successfully applied to environmental water samples from East and West Sussex, UK, for the determination of the target EDCs.

Calibration↗

PubMed2006

Investigating sorption-driven dissolved organic matter fractionation by multidimensional fluorescence spectroscopy and PARAFAC.

Soil organic matter is involved in many ecosystem processes, such as nutrient supply, metal solubilization, and carbon sequestration. This study examined the ability of multidimensional fluorescence spectroscopy and parallel factor analysis (PARAFAC) to provide detailed chemical information on the preferential sorption of higher-molecular-weight components of natural organic matter onto mineral surfaces. Dissolved organic matter (DOM) from soil organic horizons and tree leaf tissues was obtained using water extracts. The suite of fluorescence spectra was modeled with PARAFAC and it was revealed that the DOM extracts contained five fluorescing components: tryptophan-like (peak location at excitation <255 nm:emission 342 nm), tyrosine-like (276 nm:312 nm), and three humic-substance-like components (<255 nm:456 nm, 309 nm:426 nm, <255 nm:401 nm). In general, adsorption onto goethite and gibbsite increased with increasing DOM molecular weight and humification. PARAFAC analysis of the pre- and post-sorption DOM indicated that the ordering of sorption extent was humic-like components (average 91% sorption) > tryptophan-like components (52% sorption) > tyrosine-like components (29% sorption). This differential sorption of the modeled DOM components in both the soil organic horizon and leaf tissue extracts led to the fractionation of DOM. The results of this study demonstrate that multidimensional fluorescence spectroscopy combined with PARAFAC can quantitatively describe the chemical fractionation process due to the interaction of DOM with mineral surfaces.

Adsorption↗

PubMed2006

Ozonation of algae and odor causing substances in eutrophic waters.

Consumers generally concern taste and odor in drinking water. In the Southern Taiwan, more than 5,000,000 people are suffered from earth/musty odor in drinking water, especially in the summer. Thus, ozonation of geosmin (GSM), 2-methylisoborneol (2-MIB), and 2-furfural (2-FF) in eutrophic surface waters has been studied in the present work. Experimentally, it was found that the water contained high dissolved organic carbon (DOC), humic substances, and specific ultraviolet absorbance (SUVA) resulting the highly ozone (O3) demand. The natural organic matters (NOM) in the waters had a significant effect on the ozonation of GSM, 2-MIB and 2-FF. Their destruction rates were increased with high contents of aromatics, phenolics, and SUVAs. In addition, during ozonation of raw waters, O3 and OH. played an important role in destruction of algae cells and caused excretion of extracellular organic matter (EOM) to the bulk phase.

Camphanes↗

PubMed2002

Chromium speciation and fractionation in ground and surface waters in the vicinity of chromite ore processing residue disposal sites.

Chromium concentrations of up to 91 mg l(-1) were found by ICP-OES for ground water from nine boreholes at four landfill sites in an area of S.E. Glasgow/S. Lanarkshire where high-lime chromite ore processing residue (COPR) from a local chemical works had been deposited from 1830 to 1968. Surface water concentrations of up to 6.7 mg l(-1) in a local tributary stream fell to 0.11 mg l(-1) in the River Clyde. Two independent techniques of complexation/colorimetry and speciated isotope dilution mass spectrometry (SIDMS) showed that Cr was predominantly (>90%) in hexavalent form (CrVI) as CrO4(2-), as anticipated at the high pH (7.5-12.5) of the sites. Some differences between the implied and directly determined concentrations of dissolved CrIII, however, appeared related to the total organic carbon (TOC) content. This was most significant for the ground water from one borehole that had the highest TOC concentration of 300 mg l(-1) and at which < 3% of Cr was in the form of CrVI. Subsequent ultrafiltration produced significant decreases in Cr concentration with decreasing size fractions, e.g. <0.45 microm, < 100 kDa, <30 kDa and < 1 kDa by the tangential-flow method. As this appeared related more to concentrations of humic substances than of TOC per se, horizontal bed gel electrophoresis of freeze-dried ultrafilter retentates was carried out to further characterise the CrIII-organic complex. This showed for the main Cr-containing fraction, 100 kDa-0.45 microm, that the Cr was associated with a dark brown band characteristic of organic (humic) matter. Comparison of gel electrophoresis and FTIR results for ultrafilter retentates of ground water from this borehole with those for a borehole at another site where CrVI predominated suggested the influence of carboxylate groups, both in reducing CrVI and in forming soluble CrIII-humic complexes. The implications of this for remediation strategies (especially those based on the addition of organic matter) designed to reduce highly mobile and carcinogenic Cr(VI)O4(2-) to the much less harmful CrIII as insoluble Cr(OH)3 are discussed.

Carcinogens, Environmental↗

PubMed1983

Gamma ray decomposition of dissolved organic substances in river water without compositional change of metallic elements.

A river water sample was irradiated with 60Co gamma-rays under aerobic conditions, and the changes of the organic substances in the sample were examined by the analyses of the dissolved organic carbon (DOC), organic composition, UV spectrum and molecular-weight distribution. By the irradiation, the DOC decreased with irradiation dose following the first-order kinetics. In addition, the changes of UV absorption and molecular-weight distribution showed that the considerable decomposition of polymeric aromatic structure, which is the characteristic of humic substances, took place by irradiation of relatively low dose. Since the gamma-ray decomposition does not require any oxidizing agents and pH control, it will cause no compositional change of metallic elements in the water samples and has less chance of contamination. Therefore the method will be useful in, for example, geochemical studies of trace metals in natural waters.

Carbon↗

PubMed2005

Membrane fouling in pilot-scale membrane bioreactors (MBRs) treating municipal wastewater.

The main obstacle for wider use of membrane bioreactors (MBRs) for wastewater treatment is membrane fouling (i.e., deterioration of membrane permeability),which increases operating costs. For more efficient control of membrane fouling in MBRs, an understanding of the mechanisms of membrane fouling is important. However, there is a lack of information on membrane fouling in MBRs, especially information on features of components that are responsible for the fouling. We conducted a pilot-scale experiment using real municipal wastewater with three identical MBRs under different operating conditions. The results obtained in this study suggested that the food-microorganisms ratio (F/M) and membrane filtration flux were the important operating parameters that significantly influenced membrane fouling in MBRs. Neither concentrations of dissolved organic matter in the reactors nor viscosity of mixed liquor, which have been thought to have influences on fouling in MBRs, showed clear relationships with membrane fouling in this study. Organic substances that had caused the membrane fouling were desorbed from fouled membranes of the MBRs at the termination of the operation and were subjected to Fourier transform infrared (FTIR) and 13C nuclear magnetic resonance (NMR) analyses. These analyses revealed that the nature of the membrane foulant changes depending on F/M. It was shown that high F/M would make the foulant more proteinaceous. Carbohydrates were dominant in membrane foulants in this study, while features of humic substances were not apparent.

Biofilms↗

PubMed2006

Characteristics of natural organic matter degradation in water by UV/H2O2 treatment.

This study evaluated the UV/H2O2 system for degradation of natural organic matter in water. The photolysis experiments were conducted in a 10-l batch reactor using a 450-watt high-pressure mercury vapor lamp as the light source. The addition of H2O2 in water greatly improved the rate of humic acid degradation by UV light and 90% of the humic acid was removed within 30 min of photolysis. Kinetic data showed that the first-order reaction could be used to describe the kinetics of both humic acid oxidation and H2O2 decomposition, and the optimum H2O2 dose was 0.01%-0.05% for humic acid oxidation. It was also observed that the absorption of UVC (UV with wavelength between 200 and 280 nm) is responsible for the dissociation of H2O2 to generate the reactive hydroxyl radicals. Depending on the initial dosages, the H2O2 added to the system can be completely decomposed by UV within 50 to 90 minutes. Upon UV irradiation, the humic intermediates with smaller molecular sizes increase as a result of the degradation of larger humic substances. Photolysis of surface water also shows that the UV/H2O2 was effective in reducing trihalomethanes (THMs) formation in treating surface water with high contents of organic precursors. The distribution of THMs shifted from chlorine-THMs to bromine-THMs after UV/H2O2 treatments when bromide was present in water. However, higher H2O2 dosages would be necessary for the photolysis of surface water containing high concentrations of organic THM precursors. As observed from the Fourier transform infrared (FTIR) spectra, the functional groups of treated humic acids were destructed significantly, including -OH (from -COOH and -COH), aromatic -C=C, and -C=O conjugated with aromatic rings.

Hydrogen Peroxide↗

PubMed2002

Speciation of aluminum in soil extracts using cation and anion exchangers followed by a flow-injection system with fluorescence detection using lumogallion.

Flow-injection analysis (FIA) with fluorescence detection of aluminum using lumogallion was applied to the chemical speciation of aluminum in soil extracts after the separation of aluminum species with ionic exchangers. Aluminum complexes with organic substances (anion species) can be specified from other species by using a strongly acidic cation exchanger in the pH range of 3 to 5. Furthermore, aluminum can be separated into three categories, namely, (i) the Al3+ and Al-OH complex, (ii) aluminum organic complexes (cation species), and (iii) its anion species by using a strongly acidic and a weakly acidic cation exchanger at around pH 5. A considerable percentage of water-soluble aluminum in soils was found to be complexes with humic substances.

Adsorption↗