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PubMed2002

Electrochemical removal of bromide and reduction of THM formation potential in drinking water.

Trihalomethanes (THMs), a by-product of the chlorination of natural waters containing dissolved organic carbon and bromide, are the focus of considerable public health concern and regulation due to their potential as a carcinogen by ingestion. This paper presents a promising new water treatment process that lowers the concentration of bromide in drinking water and thus, lowers the THM formation potential. Bromide is oxidized by electrolysis to bromine and then the bromine apparently volatilized. The electrolyzed water, when chlorinated, produces measurably lower amounts of THMs and proportionately fewer brominated THMs, which are of greater public health concern than the chlorinated THMs. Removing bromide should also reduce the formation of other disinfection by-products such as bromate and haloacetic acids.

Bromides↗
PubMed2000

Levels of exposure from drinking water.

The relative exposure from drinking water is generally small, although there is a lack of information on total daily intake of individual organic micropollutants. There are, however, a few exceptions. Materials used in domestic distribution systems (lead, copper and plastics) may cause a deterioration of the water quality, especially in stagnant water. The relative exposure to the related compounds may increase considerably. Monitoring data from the tap (with defined sampling techniques) are needed. Also, disinfection/oxidation by-products (bromate, trihalomethanes) can be present in drinking water in considerable amounts and the relative exposure from drinking water may even approach 100%. Especially for volatile organic micropollutants, exposure routes from drinking water other than ingestion must be taken into account (inhalation, percutaneous uptake). When there is a need for detection of substances at very low levels it is important that the measurements are reliable. International interlaboratory comparisons for organic micropollutants are lacking at the moment.

Disinfection↗
PubMed2003

Heterogeneous photocatalysed degradation of a herbicide derivative, isoproturon in aqueous suspension of titanium dioxide.

Heterogeneous photocatalysed degradation of a herbicide derivative, N-(4-isopropylphenyl)-N',N'-dimethylurea (Isoproturon, 1) was investigated in aqueous suspensions of titanium dioxide by monitoring the change in absorption intensity and depletion in Total Organic Carbon content as a function of irradiation time. The degradation kinetics was studied under different conditions such as pH, catalyst concentration, substrate concentration, different types of TiO(2) and in the presence of electron acceptors such as hydrogen peroxide (H(2)O(2)), potassium bromate (KBrO(3)) and potassium persulphate (K(2)S(2)O(8)) besides molecular oxygen. The degradation rates were found to be strongly influenced by all the above parameters. The photocatalyst Degussa P25 was found to be more efficient as compared with other photocatalysts. An attempt was made to identify the degradation product through GC-MS analysis technique.

Catalysis↗
PubMed2003

Determination of inorganic anions via postcolumn reaction with iodide in ion chromatography.

Inorganic anions were determined as triiodide by postcolumn reaction with iodide under an acidic condition with help of alpha-cyclodextrin in ion chromatography. Analytes reacting with iodide to produce iodine could be determined by the present method. The analytes were indirectly detected at 287 or 355 nm. The presence of alpha-cyclodextrin caused an increase in the concentration of triiodide, leading to improvement of the sensitivity. The present system achieved good selectivity to iodate, bromate and nitrite as well as good repeatability under the optimum conditions. The determination of nitrite in river water was possible.

Anions↗
PubMed2003

Determination of caffeine using oscillating chemical reaction in a CSTR.

A new analytical method for the determination of caffeine by the sequential perturbation caused by different amounts of caffeine on the oscillating chemical system involving the manganese(II)-catalyzed reaction between potassium bromate and tyrosine in acidic medium in a CSTR was proposed. The method exposed for the first time in this work. It relies on the relationship between the changes in the oscillation amplitude of the chemical system and the concentration of caffeine. The calibration curve fits a second-order polynomial equation very well when the concentration of caffeine over the range 4.0 x 10(-6) - 1.2 x 10(-4) M (r = 0.9968). The effect of influential variables, such as the concentration of reaction components, injection point, temperature, flow rate and stirring rate were studied. Some aspects of the potential mechanism of action of caffeine on the chemical oscillating system were also discussed. A real sample was determined and the result was satisfactory.

Caffeine↗
PubMed1999

All-trans retinoic acid enhances gap junctional intercellular communication among renal epithelial cells in vitro treated with renal carcinogens.

Epidemiological and clinical studies imply that retinoids have a chemopreventative action against cancer and can suppress the growth of cancer cells. The regulation of connexin (Cx) expression by retinoids varies among tissues and organs. In this study, we investigated whether all-trans retinoic acid (ATRA) upregulates gap junctional intercellular communication (GJIC) in renal epithelial cells exposed to renal carcinogens. Madin Darby canine kidney (MDCK) cells were incubated with ATRA for 3 days, then briefly exposed to 12-O-tetradecanoyl-phorbol-13-acetate (TPA) or renal carcinogens potassium bromate (KBrO3) and dimethylnitrosamine (DMN). ATRA increased the expression of connexin 43 mRNA and protein without affecting Cx 43 phosphorylation and prevented inadequate Cx 43 localisation caused by TPA/KBrO3 or DMN. Consequently, ATRA prevented the disruption of GJIC in MDCK cells. These data suggest that ATRA enhanced GJIC by upregulating Cx 43 expression and that ATRA might be useful for prevention of renal cell carcinoma.

Blotting, Western↗
PubMed2001

Effects of liquid phase composition on salt cluster formation in positive ion mode electrospray mass spectrometry: implications for clustering mechanism in electrospray.

Potassium bromate salt clusters, [KBrO3]nKx(x+), formed by electrospray ionization were studied as a function of solution properties. Clusters with up to 4 positive charges were observed. Their abundance, charge state and distribution were shown to vary with the organic solvent in solution. The effects of 7 solvents, including methanol, ethanol, isopropanol, acetonitrile, acetone, pyridine, and 1,4-dioxane, were thoroughly investigated. Solvents with a low dielectric constant and a high viscosity seem to favor clustering in solution but do not systematically allow high charge state ion formation. On the other hand, cluster charge reduction during desolvation was not correlated with solvent cation affinity over the range of solvents examined. However, ion distribution in mass spectra could be rationalized as a combination of these two competing phenomena. Charge state increases with the cluster size but may be reduced during ion desolvation when high cation affinity solvent molecules are actually involved in the ion solvation shell. This assumption could be envisaged in either Iribarne or Dole mechanisms of ion release in the gas phase. However, intensity profiles of multiply charged clusters could only be understood in terms of the ion evaporation mechanism.

Journal Article↗
PubMed2001

Spectrofluorimetric flow injection determination of trace amounts of periodate.

A sensitive, rapid and selective procedure is proposed for the flow injection determinations of periodate by spectrofluorometric detection. The method is based on the reaction of periodate with Alizarin Navy Blue in basic solution. The reagents and manifold variables influence on the sensitivity have been investigated and the optimum conditions are established. Periodate can be determined for the range of 0.250-5.00 microg ml(-1) with a limit of detection of 0.08 microg ml(-1), and with a sample rate of 15 +/- 2 samples h(-1). The relative standard deviations for eight replicate determination of 0.500 and 5.00 microg ml(-1) was 1.3 and 1.1%, respectively. Periodate can be determined in the presence of iodate and bromate. The proposed method was used to determination of periodate in water samples.

Anthraquinones↗
PubMed2003

A user-friendly programme 'SIMKINERSQUO; for simulation of kinetics involving complex reaction mechanisms.

A programme, 'SIMKINERSQUO; is developed using a semi-implicit extrapolation method (SIEM) which uses the implicit midpoint rule and extrapolation to simulate complex mechanisms based on the kinetics of homogeneous chemical systems. The chemical kinetics pre-processor code is designed to translate a user-specified system of chemical rate equations into a system of chemical kinetic differential equations. The developed programme is applied to the 13-step mechanism of the reaction between Nile blue and acidic bromate. The results obtained compare well with the curves drawn using the other method, reported in literature.

Journal Article↗
PubMed2001

Determination of picomolar levels of iron in seawater using catalytic cathodic stripping voltammetry.

A new procedure for the direct determination of picomolar levels of iron in seawater is presented. Cathodic stripping voltammetry (CSV) is preceded by adsorptive accumulation of the iron(III)-2,3-dihydroxynaphthalene (DHN) complex from seawater, containing 20 microM DHN at pH 8.0, onto a static mercury drop electrode, followed by reduction of the adsorbed species. The reduction current is catalytically enhanced by the presence of 20 mM bromate. Optimized conditions include a 60-s adsorption period at -0.1 V and a voltammetric scan using sampled dc modulation at 10 Hz. In these conditions, a detection limit of 13 pM iron in seawater was achieved which can be lowered further by extending the adsorption time to 300 s. The new catalytic CSV method is approximately 5 times more sensitive than existing CSV methods and was tested on samples from the Atlantic Ocean.

Journal Article↗
PubMed2005

Latex-coated polymeric monolithic ion-exchange stationary phases. 1. Anion-exchange capillary electrochromatography and in-line sample preconcentration in capillary electrophoresis.

A sulfonated methacrylate monolithic polymer has been synthesized inside fused-silica capillaries of diameters 50-533-microm i.d. and coated with 65-nm-diameter fully functionalized quaternary ammonium latex particles (AS18, Dionex Corp.) to form an anion-exchange stationary phase. This stationary phase was used for ion-exchange capillary electrochromatography of inorganic anions in a 75-microm-i.d. capillary with Tris/perchlorate electrolyte and direct UV detection at 195 nm. Seven inorganic anions (bromide, nitrate, iodide, iodate, bromate, thiocyanate, chromate) could be separated over a period of 90 s, and the elution order indicated that both ion exchange and electrophoresis contributed to the separation mechanism. Separation efficiencies of up to 1.66 x 10(5) plates m(-1) were achieved, and the monoliths were stable under pressures of up to 62 MPa. Another latex-coated monolith in a 250-microm-i.d. capillary was used for in-line preconcentration by coupling it to a separation capillary in which the EOF had been reversed using a coating of either a cationic polymer or cationic latex particles. Several capillary volumes of sample were loaded onto the preconcentration monolith, and the analytes (inorganic anions) were then eluted from the monolith with a transient isotachophoretic gradient before being separated by electrophoresis in the separation capillary. Linear calibration curves were obtained for aqueous mixtures of bromide, nitrite, nitrate, and iodide. Recoveries of all analytes except iodide were reduced significantly when the sample matrix contained high levels of chloride. The preconcentration method was applied to the determination of iodide in open ocean water and provided a limit of detection of 75 pM (9.5 ng/L) calculated at a signal-to-noise ratio of 3. The relative standard deviation for migration time and peak area for iodide were 1.1 and 2.7%, respectively (n = 6). Iodide was eluted as an efficient peak, yielding a separation efficiency of 5.13 x 10(7) plates m(-1). This focusing was reproducible for repeated analyses of seawater.

Journal Article↗
PubMed1985

Kinetic analysis of respiratory nitrate reductase from Escherichia coli K12.

Purified respiratory nitrate reductase from Escherichia coli is able to use either reduced viologen dyes or quinols as the electron donor and nitrate, chlorate, or bromate as the electron acceptor. When reduced viologen dyes act as the electron donor, the enzyme follows a compulsory-order, "Theorell-Chance" mechanism, in which it is an enzyme-nitrate complex that is reduced rather than the free enzyme. In contrast, if quinols are used as the electron donor, then the enzyme operates by a two-site, enzyme-substitution mechanism. Partial proteolysis of the cytochrome b containing holoenzyme by trypsin results in loss of cytochrome b and in cleavage of one of the enzyme's subunits. The cytochrome-free derivative exhibits a viologen dye dependent activity that is indistinguishable from that of the holoenzyme, but it is incapable of catalyzing the quinol-dependent reaction. The quinol-dependent, but not the viologen dye dependent, activity is inhibited irreversibly by exposure to diethyl pyrocarbonate and reversibly by treatment with 2-n-heptyl-4-hydroxyquinoline N-oxide. We conclude that the holoenzyme has two independent and spatially distinct active sites, one for quinol oxidation and the other for nitrate reduction.

Cytochrome b Group↗
PubMed2006

Treatment of volatile organic chemicals on the EPA Contaminant Candidate List using ozonation and the O3/H2O2 advanced oxidation process.

Seven volatile organic chemicals (VOCs) on the EPA Contaminant Candidate List together with 1,1-dichloropropane were studied for their reaction kinetics and mechanisms with ozone and OH radicals during ozonation and the ozone/ hydrogen peroxide advanced oxidation process (O3/H2O2 AOP) using batch reactors. The three aromatic VOCs demonstrated high reactivity during ozonation and were eliminated within minutes after ozone addition. The high reactivity is attributed to their fast, indirect OH radical reactions with k(OH,M) of (5.3-6.6) x 10(9) M(-1) s(-1). Rates of aromatic VOC degradation are in the order 1,2,4-trimethylbenzene > p-cymene > bromobenzene. This order is caused by the selectivity of the direct ozone reactions (k(O3,M) ranges from 0.16 to 304 M(-1) s(-1)) and appears to be related to the electron-donating or -withdrawing ability of the substituent groups on the aromatic ring. The removal rates for the five aliphatic VOCs are much lower and are in the order 1,1-dichloropropane > 1,3-dichloropropane > 1,1-dichloroethane > 2,2-dichloropropane > 1,1,2,2-tetrachloroethane. The second-order indirect rate constants for the aliphatic VOCs range from 0.52 x 10(8) to 5.5 x 10(8) M(-1) s(-1). The relative stability of the carbon-centered intermediates seems to be related to the relative reactivity of the aliphatic VOCs with OH radicals. Except for 1,3-dichloropropane, ozonation and the O3/H2O2 AOP are not effective for the removal of other aliphatic VOCs. Bromide formation during the ozonation of bromobenzene indicates that bromate can be formed, and thus, ozonation and O3/H2O2 AOP may not be suitable for the treatment of bromobenzene.

Hydrocarbons↗
PubMed2006

Phenols and amine induced HO* generation during the initial phase of natural water ozonation.

The initial phase of ozone decomposition in natural water (t < 20 s) is poorly understood. It has recently been shown to result in very high transient HO* concentrations and, thereby, plays an essential role during processes such as bromate formation or contaminants oxidation. Phenols and amines are ubiquitous moieties of natural organic matter. Naturally occurring concentrations of primary, secondary, and tertiary amines, amino acids, and phenol were added to surface water, and ozone decomposition as well as HO* generation were measured starting 350 milliseconds after ozone addition. Six seconds into the process, 5 microM of dimethylamine and phenol had generated integral of HO* dt = 1 x 10(-10) M*s and 1.8 x 10(-10) M*s, respectively. With 10 microM dimethylamine and 1.5 mg O3/L, R(ct), (integral of HO*dt/ integral of O3dt) reached 10(-6), which is larger than in advanced oxidation processes (AOP) such as O3/H2O2. Experiments in the presence of HO*-scavengers indicated that a significant fraction of phenol-induced ozone decomposition and HO* generation results from a direct electron transfer to ozone. For dimethylamine, the main mechanism of HO* generation is direct formation of O2*- which reacts selectively with O3 to form O3*-. Pretreatment of phenol-containing water with HOCl or HOBr did not decrease HO* generation, while the same treatment of dimethylamine-containing water considerably reduced HO* generation.

Dimethylamines↗
PubMed2006

Semiconductor-mediated Photocatalyzed degradation of a herbicide derivative, chlorotoluron, in aqueous suspensions.

The photocatalytic degradation of a herbicide derivative, chlorotoluron [3-(3-chloro-4-methylphenyl)-1,1-dimethylurea, 1], has been investigated in aqueous suspensions of titanium dioxide (TiO2) under a variety of conditions. The degradation was studied by monitoring the change in substrate concentration employing UV spectroscopic analysis technique and depletion in total organic carbon (TOC) content as a function of irradiation time. The degradation kinetics of the model compound was investigated under different conditions such as type of TiO2, pH, catalyst concentration, substrate concentration, temperature, and in the presence of different electron acceptors such as hydrogen peroxide (H2O2), potassium persulfate (K2S2O8), and potassium bromate (KBrO3) besides molecular oxygen. TiO2 Degussa P25 was found to be a more efficient photocatalyst for the degradation of the model compound as compared with other photocatalysts. The degradation products were analyzed using GC/MS analysis technique and probable pathways for the formation of different products have been proposed.

Catalysis↗
PubMed2005

Use of chemical profiling to differentiate geographic growing origin of raw pistachios.

The objective of this study was to demonstrate the feasibility of chemical profiling methods combined with multivariate methods to differentiate the geographical growing regions of pistachios (Pistachia vera). Elemental analysis (Ba, Be, Ca, Cu, Cr, K, Mg, Mn, Na, V, Fe, Co, Ni, Cu, Zn, Sr, Ti, Cd, and P) of pistachios samples was performed using inductively coupled plasma atomic emission spectrometry. Analysis of inorganic anions and organic acids (selenite, bromate, fumarate, malate, selenate, pyruvate, acetate, phosphate, and ascorbate) of pistachio samples was performed using capillary electrophoresis. Bulk carbon and nitrogen isotope ratios were performed using stable isotope MS. There were nearly 400 pistachio samples analyzed from the three major pistachio growing regions: Turkey, Iran, and California (United States). A computational evaluation of the trace element data sets was carried out using statistical pattern recognition methods including principal component analysis, canonical discriminant analysis, discriminant analysis, and neural network modeling. Several linear discriminant function models classified the data sets with 95% or higher accuracy. We report the development of a method combining elemental analysis and classification techniques that may be widely applied to the determination of the geographical origin of foods.

Analysis of Variance↗
PubMed2005

Self-oscillation of polymer chains induced by the Belousov-Zhabotinsky reaction under acid-free conditions.

A novel self-oscillating polymer was prepared by utilizing the Belousov-Zhabotinsky (BZ) reaction. In this study, a sulfonic acid group was newly introduced as a pH-control site into the copolymer of N-isopropylacrylamide, and the ruthenium complex was introduced as a catalyst site. By introducing the pH-control site, we succeed in causing the soluble-insoluble self-oscillation of the polymer solution under acid-free conditions in which only two BZ substrates, malonic acid and sodium bromate, were present as added agents. The self-oscillating behavior was remarkably influenced by the temperature and polymer concentration, which reflects the intermolecular aggregative capacity of the polymer chains in the reduced state to change the lower critical solution temperature. This achievement of self-oscillation of polymer chains under acid-free conditions may lead to their practical use as novel biomimetic materials under biological conditions.

2,2'-Dipyridyl↗
PubMed2006

Spatial quantification of Mn2+ and Mn3+ concentrations in the Mn-catalyzed 1,4-cyclohexanedione/acid/bromate reaction using magnetic resonance imaging.

This paper presents a magnetic resonance imaging (MRI) method for quantifying the spatial concentrations of the paramagnetic species Mn2+ and Mn3+, during pattern formation, in the manganese-catalyzed 1,4-cyclohexanedione-acid-bromate reaction. The relaxivity of each species was measured, which enabled their concentration to be calculated from nuclear magnetic resonance T2 relaxation times. Images were acquired using the fast spin-echo imaging method RARE. By determining the relation, in these experiments, between signal intensity and T2 relaxation time, it was possible to produce T2 maps from the images. These T2 maps were then used to produce concentration maps for the oxidized (Mn3+) and reduced (Mn2+) states of the catalyst.

Letter↗