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PubMed1991

Chemical topology and ecotoxicology.

The experimental determination of environmental parameters (e.g. soil sorption, bioconcentration, biodegradation and biotransformation, toxic effects, etc.) of commercial chemicals is a costly and time-consuming process. Since there is a large number of chemicals currently in common use (approximately 100,000) and new chemicals are registered at a very high rate (1000/year) it is obvious that our human and material resources are insufficient to obtain experimentally even basic information on environmental fate and effects for all those chemicals. Thus, it is necessary to develop quantitative models that will accurately and rapidly predict environmental behaviour for large sets of chemicals. Thus far, molecular connectivity indices have been shown to be the most successful structural property for describing and predicting soil sorption coefficients, association with dissolved humic substances, Henry's law constants, bioconcentration factors in aquatic organisms and vegetation, biodegradation, and acute toxicity. We describe and discuss the most recent results on modelling environmental fate of organic pollutants by the application of molecular connectivity indices. Two sections describe the usefulness of environmental QSAR models based on n-octanol/water coefficients and the systematics and possible physical interpretation of molecular connectivity indices. Some practical and theoretical weaknesses and pitfalls are discussed concerning the use of n-octanol/water partition coefficients in environmental QSAR research.

Biodegradation, Environmental↗

PubMed1991

A nation-wide survey of the chemical composition of drinking water in Norway.

Water samples were collected from 384 waterworks that supply 70.9% of the Norwegian population. The samples were collected after water treatment and were analysed for 30 constituents. Although most constituents show wide concentration ranges, Norwegian drinking water is generally soft. The median values obtained are: 0.88 mg Si l-1, 0.06 mg Al l-1, 47 micrograms Fe l-1, 0.69 mg Mg l-1, 2.9 mg Ca l-1, 3.8 mg Na l-1, 6 micrograms Mn l-1, 12 micrograms Cu l-1, 14 micrograms Zn l-1, 9 micrograms Ba l-1, 15 micrograms Sr l-1, 0.14 mg K l-1, 58 micrograms F- l-1, 6.4 mg Cl- l-1, 11 micrograms Br- l-1, 0.46 mg NO3- l-1, 5.3 mg SO4(2-) l-1, 2.4 mg TOC l-1, 6.8 (pH), 5) microseconds cm-1 (conductivity) and 11 mg Pt l-1 (colour). Titanium, Pb, Ni, Co, V, Mo, Cd, Be and Li were seldom or never quantified, due to insufficient sensitivity of the ICP (inductively coupled plasma) method. Norwegian quality criteria, which exist for 17 of the constituents examined, are generally fulfilled, indicating that the chemical quality of drinking water, by and large, is good in Norway. For Fe, Ca, Mn, Cu, pH, TOC and colour, however, the norms for good drinking water are exceeded in more than 9% of the samples, reflecting two of the major problems associated with Norwegian drinking water supplies: (i) many water sources contain high concentrations of humic substances; (ii) in large parts of the country, the waters are soft and acidic, and therefore corrosive towards pipes, plumbing and other installations. Most constituents show marked regional distribution patterns, which are discussed in the light of different mechanisms contributing to the chemical composition of drinking water, namely: chemical weathering of mineral matter; atmospheric supply of salt particles from the sea; anthropogenic pollution (including acid precipitation); corrosion of water pipes and plumbing; water treatment; decomposition of organic matter; and hydrological differences.

Anions↗

PubMed1988

Genotoxic activity of organic chemicals in drinking water.

The information summarized in this review provides substantial evidence for the widespread presence of genotoxins in drinking water. In many, if not most cases, the genotoxic activity can be directly attributed to the chlorination stage of drinking water treatment. The genotoxic activity appears to originate primarily from reactions of chlorine with humic substances in the source waters. Genotoxic activity in drinking water concentrates has been most frequently demonstrated using bacterial mutagenicity tests but results with mammalian cell assay systems are generally consistent with the findings from the bacterial assays. There is currently no evidence for genotoxic damage following in vivo exposures to animals. In some locations genotoxic contaminants of probable industrial and/or agricultural origin occur in the source waters and contribute substantially to the genotoxic activity of finished drinking waters. The method used for sample concentration can have an important bearing on study results. In particular, organic acids account for most of the mutagenicity of chlorinated drinking water, and their recovery from water requires a sample acidification step prior to extraction or XAD resin adsorption. Considerable work has been done to determine the identity of the compounds responsible for the mutagenicity of organic concentrates of drinking water. Recently, one class of acidic compounds, the chlorinated hydroxyfuranones, has been shown to be responsible for a major part of the mutagenic activity. Strategies for drinking water treatment that have been evaluated with respect to reduction of genotoxins in drinking water include granular activated carbon (GAC) filtration, chemical destruction, and the use of alternative means of treatment (i.e., ozone, chlorine dioxide, and monochloramine). GAC treatment has been found to be effective for removal of mutagens from drinking water even after the GAC is beyond its normal use for organic carbon removal. All disinfectant chemicals appear to have the capacity of forming mutagenic chemicals during water treatment. However, the levels of mutagenicity formed with the alternative disinfectants have been generally less than those seen with chlorine and, especially in the case of ozone, highly dependent on the source water.(ABSTRACT TRUNCATED AT 400 WORDS)

Humans↗

PubMedDate not supplied

High levels of mutagenic activity in chlorinated drinking water in Finland.

The organic extract from the drinking water of Kuopio, Eastern Finland, turned out to be highly mutagenic in the Ames test. The direct mutagenic activities of the acid/neutral fractions of 48 drinking water samples were on an average 1700 net revertants/l in strain TA100. The highest activities were more than 6000 net revertants/l, and one drinking water sample exceeded 10 000 net revertants/l. The drinking water of Kuopio is produced from lake water which has a relatively high content of humic substances. Water processing involved two chlorination phases. The organic constituents of the water samples were isolated either by continuous liquid-liquid extraction or by absorption on XAD 8 resin.

Animals↗

PubMed1992

The effect of liming agricultural land on the chemistry and biology of the River Esk, north-west England.

A land-use study indicated that a reduction in agricultural liming may have been a major factor in the development of acid episodes and consequent fish kills in the River Esk and River Duddon. A field study was carried out to determine whether the reintroduction of catchment liming in the Esk valley could ameliorate acid episodes and thus prevent fish kills. Lime was applied to areas which had been limed in the past, comprising 10% of the Esk catchment. Flow, pH, calcium, aluminium, total humic substances, conductivity and invertebrates were monitored before and after liming. The River Duddon was monitored as a reference. There was a general reduction of the acidity of both the River Esk and the River Duddon during the study period. This appeared to be controlled by rainwater chemistry. There was little evidence for a major effect of liming on water chemistry which suggests that the mortalities of salmonids in the early 1980s were not due to a reduction in agricultural liming.

Journal Article↗

PubMed1995

Fractionation of fulvic acids: characteristics and complexation with copper.

Two fulvic acid samples isolated from Suwannee river (International Humic Substance Society) and Feeitsuey reservoir were subjected to gel filtration chromatography (GFC) for molecular size fractionation. The GFC-eluted samples were separated into three groups corresponding to the molecular weight ranges: < 220, 220-1000, and 1000-4000. Fluorescence quenching techniques were employed for determining the conditional stability coefficient and kinetic parameters of copper complexation with the three fractions of fulvic acids. Experimental conditions were pH 6, 5 x 10(-5)m total copper and 5 mg C litre(-1) of fulvic acids. The conditional stability coefficients of the fulvic acid fractions were in the order of 0.9-3.3 x 10(5)m(-1), and the forward and reverse rate constants were in the order of 6.9-12.4 x 10(3)m(-1) s(-1) and 3.5-8.0 x 10(-2) s(-1). Information could be useful in modelling copper transport in the hydrosphere.

Journal Article↗

PubMed1996

Hazards for the Rostock water supply from a tar-contaminated sediment in the river Warnow.

By the gas plant at Schwaan (a small city near Rostock), tar and other by-products were released into the river Warnow which supplies Rostock with drinking water 20 km downstream. The tar-contaminated river sediment contained phenols and polycyclic aromatic hydrocarbons (PAH), indicating a mutagenic potential. Investigations in the catchment area and on tributaries showed PAH contents up to about 10 ng/l in the water. The river sediment was found to be the sole PAH source. Although the PAH level is very low, sediment disturbances may produce an increase in concentrations. The consequences of such a worst case are difficult to estimate, even though the content of seston and humic substances in the river seems to reduce the PAH concentrations. Although this lowers the probability that increased PAH concentrations reach the Rostock water supply, the removal of the tar-contaminated sediment from the river is strongly recommended.

Environmental Monitoring↗

PubMed2005

Effect of pH, ionic strength and fulvic acid on the sorption and desorption of cobalt to bentonite.

Humic substances and bentonite have attracted great interest in radioactive waste management. Here the sorption of cobalt on bentonite in the presence and absence of fulvic acid (FA) under ambient conditions was studied. The effects of pH, ionic strength, FA and solution concentrations on cobalt sorption to bentonite were also investigated using batch techniques. The results indicate that the sorption of cobalt is strongly dependent on pH and is independent of ionic strength under our experimental conditions. Surface complexation is considered the main mechanism of cobalt sorption to bentonite. In the presence of FA, little effect of FA on cobalt sorption was found at pH<6; a positive effect of FA on cobalt sorption was found for pH 6-8; and a negative effect of FA on cobalt sorption was found at pH>8. The addition sequences of FA/Co(2+) to the bentonite suspension on the sorption of cobalt to FA-coated bentonite were also studied. The results indicated that the sorption is not influenced by the addition sequences. Some possible mechanisms are discussed.

Journal Article↗

PubMed2007

Sorption of Th (IV) to silica as a function of pH, humic/fulvic acid, ionic strength, electrolyte type.

The removal behavior of thorium (Th(IV)) has been investigated in multicomponent systems containing silica (SiO2) as the model of inorganic particles because of its widespread presence in the earth's crust and soil humic acid (HA)/fulvic acid (FA) by batch experiments. The influence of pH from 2 to 12, ionic strength from 0.02 to 0.2 M KNO3, soil HA/FA concentration from 8.3 to 22.5 mg/L, and foreign cations (Li+, Na+, K+) and anions (NO3(-), Cl-) on the sorption of Th(IV) onto SiO2 was also tested. The sorption isotherms of Th(IV) at approximately constant pH (3.50+/-0.02) were determined and analyzed regressively with three kinds of sorption isotherm models, i.e., linear, Langmuir, and Freundlich models. The results demonstrated that the sorption of Th(IV) onto SiO2 increased steeply with increasing pH from 2 to 4. Generally, humic substances (HSs) were shown to enhance Th(IV) sorption at low pH, but to reduce Th(IV) sorption at intermediate and high pH. It was a hypothesis that the significantly positive influence of HA/FA at pH from 2 to 4 on the sorption of Th(IV) onto SiO2 was attributed to strong surface binding of HA/FA on SiO2 and subsequently the formation of ternary surface complexes such as [triple bond]MO-O-HA-Th or [triple bond]MO-O-FA-Th. The results also demonstrated that the sorption was strongly dependent on the concentration of HA/FA, and independent of ionic strength and foreign ions under our experimental conditions.

Journal Article↗

PubMed2004

Photosensitized degradation of Irgarol 1051 in water.

Irgarol 1051 (2-methylthio-4-tert-butylamino-6-cyclopropylamino-s-triazine) is a herbicide analogue that is added to antifouling agents used on ships. Our former study on its degradation in sunlight suggested that unknown photosensitizers in natural waters accelerated the photodegradation to the degradation product, M1. In this study, the photodegradation of Irgarol in water was investigated in the presence of some photosensitizers. Test water containing Irgarol or M1, with or without photosensitizers, was irradiated with light from a UV-A fluorescent lamp for 48h. The concentrations of Irgarol and M1 in the test water were determined by HPLC after solid-phase extraction. M1 was more stable than Irgarol when irradiated in the presence of photosensitizers such as acetone, benzophenone, tryptophan, and rose bengal. Hydrogen peroxide (HP) accelerated the photodegradation of Irgarol, and the product M1 was degraded in the presence of more than 100mgl(-1) HP after 10h. Natural humic substances (NHS) also accelerated the photodegradation of Irgarol, but in this case, the product M1 persisted even when Irgarol was completely degraded. Photosensitized degradation of Irgarol by NHS may result in the accumulation of M1 in aquatic environments.

Acetone↗

PubMed2005

Fate of polycyclic aromatic hydrocarbons during composting of lagooning sewage sludge.

The fate of 16 polycyclic aromatic hydrocarbons (PAHs), targeted by the USEPA agency, has been investigated during composting of lagooning sludge. Composting shows efficient decrease of the content and the bioavailability of each PAH. Biodegradation and sorption are suggested as the main mechanisms contributing to this decrease. During the stabilization phase of composting, extensive microbial degradation of PAHs, mainly those with a low number of aromatic rings, was achieved following development of intense thermophilic communities. However, partial sorption of PAH to non-accessible sites temporarily limits the mobility mainly of PAHs with a high number of aromatic rings plus acenaphthene and acenaphthylene, and allows them to escape microbial attack. During the maturation phase, the development of a mesophilic population could play an important role in the degradation of the remaining PAH. During this phase of composting, PAH sequestration and binding of their oxidative metabolites within new-formed humic substances might also explain PAH decrease at the end of composting. The tendency of change of content or bioavailability of various PAH compounds during composting is found to be strongly related to the number of their aromatic rings, their molecular weight and structure.

Animals↗

PubMed2005

Heavy metals removal from electroplating wastewater by aminopropyl-Si MCM-41.

The potential of removing nickel and copper from industrial electroplating wastewaters by using mesoporous materials with MCM-41 type structure functionalised with different ratios of aminopropyl groups, namely Na50, Na25 and Na5, were evaluated. The synthesised solids sorbents obtained were characterised by X-ray diffraction, elemental chemical analysis and IR spectroscopy. In preliminary experiments, studies were carried out to determine the optimal experimental conditions for the retention of heavy ions. Effects of concentration, optimal pH, interference with humic substances and other metals were studied for Na5, which showed the best capacity of absorption determined by the corresponding isotherm. This material has a greater selectivity against sodium, indicating that ionic strength does not affect the extraction. Results of an application of this material to remove nickel and copper in synthetic and real industrial wastewater samples from an electrochemical industry area are shown with successful results. The lowest level of nickel and copper were observed when Na5 was used. This observation suggests that reactive aminopropyl-Si MCM-41 and similar materials may be a promising and provide for alternative environmental technologies in the future.

Absorption↗

PubMed2005

[14C]Pentachlorophenol mineralization in the rice rhizosphere with established oxidized and reduced soil layers.

Flooded soils with rooted aquatic macrophytes have adjacent aerobic and anaerobic zones at the soil-water interface and rhizosphere where many common soil constituents undergo sequential oxidation and reduction reactions. To investigate whether pentachlorophenol (PCP) mineralization would also be enhanced under these conditions, a laboratory study was conducted to determine the conversion of [14C]PCP to 14CO2, 14CH4 and [14C]humic substances in soil microcosms with established aerobic-anaerobic zones at the soil-water interface and rice (Oryza sativa) rhizosphere. Contrary to what was expected, PCP was least rapidly degraded in rhizosphere-soil microcosms that contained the most extensive amounts of aerobic-anaerobic interfaces (63% PCP loss in 82 d) and was most rapidly degraded in soil microcosms that lacked redox interfaces in the soil profile (94% PCP loss in 82 d). Decreased PCP mineralization in the presence of aerobic-anaerobic interfaces was explained by (i) lack of sufficient O2 for aerobic PCP mineralization, due to the oxidation of other soil constituents in aerobic zones, and (ii) lack of an adequate supply of electron equivalents for reductive dechlorination of PCP, due to the reduction of other alternate electron acceptors in anaerobic zones. It was concluded that PCP mineralization is inhibited in flooded soils that contain extensive amounts of aerobic-anaerobic interfaces, due to redox cycling of other soil constituents that occur in these zones.

Carbon Radioisotopes↗

PubMed2006

Fractionation of dissolved organic matter in mature landfill leachate and its recycling by ultrafiltration and evaporation combined processes.

XAD resin procedure was used to isolate dissolved organic matter (DOM) of a mature leachate collected from a municipal solid waste landfill in Beijing, China. The fulvic acids fraction dominated in collected leachate, accounting for 64% of DOM as dissolved organic carbon (DOC), and a high concentration of humic substances (HS) with a value of 441 mg l(-1) was found in the leachate. Molecular size distribution of DOM was also done by using batch ultrafiltration (UF) technique. Two major parts of the molecules of DOM were distributed in the regions of smaller than 1 kDa and 1-3.5 kDa, containing 45% and 43% of DOM as DOC, respectively. The laboratory-scale experiments were conducted to investigate and to develop an overall concept for mature leachate recycling based on UF and evaporation combined processes. Separation factor (SF) was applied to evaluate separation efficiency of UF. The data indicate that SF is strongly correlated with concentration factor. Second retentate from two-stage UF contained relatively high amount of DOM comprising 91% of HS and an insignificant concentration of heavy metals. The SF value for two-stage UF was more than 10. These results demonstrate that two-stage UF could effectively separate and refine HS in mature leachate from inorganic components. For achieving the main requirements as a fertilizer product, second retentate was further concentrated by evaporation, and contents of organic matter and dry-solids were obtained 13 wt.% and 25 wt.%, respectively. This study confirmed the feasibility of recycling HS from mature leachate.

Membranes, Artificial↗

PubMed2006

Characterization of H+ and Cd2+ binding properties of the bacterial exopolysaccharides.

The proton and Cd binding capacities of microbially produced exopolysaccharides, EPS, were quantified by the determination of stability constants and the concentration of complexing sites using H(+) or Cd(2+) selective electrodes in dynamic titrations. The influence of ionic strength, pH and the Cd to EPS ratio was evaluated over large concentration ranges. The applicability of the non-ideal competitive adsorption isotherm combined with a Donnan electrostatics approach was tested with respect to the EPS. Proton and cadmium binding data were compared with literature data examining other ubiquitous environmental ligands including humic substances, alginate, bacteria, etc. Subsequent modelling of Cd speciation in aquatic (fresh and marine waters) and soil systems suggested that the exopolysaccharides would play non-negligible role, under most conditions. The quantitative information provided in this paper thus represents an important advance in our understanding of Cd transport, bioavailability and impact in aquatic and terrestrial systems.

Cadmium↗

PubMed2006

Removal of PAHs from water using an immature coal (leonardite).

It has been studied an immature coal (leonardite) as an adsorbent for removing PAHs [fluorene, pyrene, benzo(k)fluoranthene, benzo(a)pyrene and benzo(g,h,i)perylene] from water. To determine the efficiency of leonardite as an adsorbent of PAHs, factors such as pH, contact time and equilibrium sorption were evaluated in a series of batch experiments. There were no significant differences in the removal percentages for the various pH values studied, except for fluorene. The adsorption of fluorene was higher at lower pH values. The equilibrium time was reached at 24h. At this time, more than 82% of the pyrene, benzo(k)fluoranthene, benzo(a)pyrene and benzo(g,h,i)perylene had been removed. During the first 2h, the adsorption rate increased rapidly. After that time, however, there was a minor decrease. Equilibrium data were fitted to Freundlich models to determine the water-leonardite partitioning coefficient. Physical adsorption caused by the aromatic nature of the compounds was the main mechanism that governed the removal process. The polarity of the humic substances in leonardite may also have influenced the adsorption capacity.

Adsorption↗

PubMed2004

Interactions of Pb2+ with fulvic acid by electrophoretically mediated on-capillary microanalysis.

Electrophoretically mediated microanalysis (EMMA) was used to monitor the on-column complexation of Pb2+ and fulvic acid (FA). Electropherograms revealed several characteristic regions, the areas of which correlate with the metal concentration. The analysis of the electropherograms suggests that at least two different complexes are formed. Therefore, the EMMA is a prospective technique for structural investigation of humic substances (HS).

Benzopyrans↗

PubMed2004

Separation of low-molecular mass organic acid-metal complexes by high-performance liquid chromatography.

The solution speciation of metals is a critical parameter controlling the bioavailability, solution-solid phase distribution and transport of metals in soils. The natural metal-complexing ligands that exist in soil solution include inorganic anions, inorganic colloids, organic humic substances, amino acids (notably phytosiderophores and bacterial siderophores) and low-molecular mass organic acids. The latter two groups are of particular significance in the soil surrounding plant roots (the rhizosphere). A number of analytical methodologies, encompassing computational, spectroscopic, physico-chemical and separation techniques, have been applied to the measurement of the solution speciation of metals in the environment. However, perhaps with the exception of the determination of the free metal cation, the majority of these techniques rarely provide species specific information. High-performance liquid chromatography (HPLC) coupled to a sensitive detection system, such as inductively coupled plasma mass spectrometry (ICP-MS) or electrospray ionisation mass spectrometry (ESI-MS), offers the possibility of separating and detecting metal-organic acid complexes at the very low concentrations normally found in the soil environment. This review, therefore, critically examines the literature reporting the HPLC separation of metal-organic acid complexes with reference to thermodynamic equilibrium and kinetic considerations. The limitations of HPLC techniques (and the use of thermodynamic equilibrium calculations to validate analytical results) are discussed and the metal complex characteristics necessary for chromatographic separation are described.

Acids↗