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PubMed2002

Removal of arsenic from contaminated water sources by sorption onto iron-oxide-coated polymeric materials.

The modification of polymeric materials (polystyrene and polyHIPE) by coating their surface with appropriate adsorbing agents (i.e. iron hydroxides) was investigated in the present work, in order to apply the modified media in the removal of inorganic arsenic anions from contaminated water sources. The method, termed adsorptive filtration, has been classified as an emerging technology in water treatment processes as it presents several advantages towards conventional technologies: the production of high amounts of toxic sludge can be avoided and it is considered as economically more efficient; whereas it has not yet been applied in full-scale treatment plants for low-level arsenic removal. The present experiments showed that both modified media were capable in removing arsenic from the aqueous stream, leading to residual concentration of this toxic metalloid element below 10 microg/L, which is the new maximum concentration limit set recently by the European Commission and imposed by the USEPA. Though, among the examined materials, polyHIPE was found to be more effective in the removal of arsenic, as far as it concerns the maximum sorptive capacity before the filtration bed reaches the respective breakthrough point.

Adsorption↗
PubMed2003

A method for preparing silica-containing iron(III) oxide adsorbents for arsenic removal.

A method for preparing iron(III)-based binary oxide adsorbents in a granulated form for arsenic removal was studied. The key step in the method was the simultaneous generation of hydrous ferric oxide (FeOOH) sol and silica sol in situ in one reactor. This eventually led to the formation of Fe-Si complexes. The addition of silica enhanced the granulated adsorbent strength but reduced the arsenic adsorption capacity. An optimum Si/Fe molar ratio in the balance of adsorbent strength and arsenic adsorption capacity was found to be approximately 0.33. The effects of aging time, drying temperature and process pH on adsorbents were also evaluated in the study. X-ray diffraction analysis confirmed that the iron(III) oxide in the Fe-Si binary oxide adsorbents was amorphous, largely due to the retardation of the iron oxide crystallization by the presence of silicate species. The surface area of the Fe-Si adsorbents and the particle size of Fe-Si complexed suspensions were determined as well. The batch strength testing procedure introduced in this study can provide a simple and quick evaluation of granulate strength in a wet status. Generally, this developed method can prepare granulated Fe-Si binary oxide adsorbents for column adsorption of arsenic from water.

Adsorption↗
PubMed2003

Arsenic contaminated site at an abandoned copper smelter plant: waste characterization and solidification/stabilization treatment.

A preliminary survey of an arsenic contaminated site from an abandoned copper smelting facility and feasibility study of using solidification/stabilization (S/S) process to treat the contaminant waste were undertaken. It was found that the waste, located in the three-flue gas discharge tunnels, contained 2-40% arsenic. The pH of the contaminated waste is extremely low (ranging from 1.8 to 3.6). The X-ray diffraction evidence indicates that the arsenic particles present in the flue gas mainly exist as As(III), or As(2)O(3). The total amount of arsenic contaminated waste is estimated to be 700 ton in the studied area. About 50% of the particle sizes are less than 2 mm. Arsenic is easily extracted from wastes with a variety of leaching solutions. In order to meet the arsenic leaching standard of the toxicity characteristic leaching procedure (TCLP), an extremely high cement dosage is required in the S/S process (cement/waste weight ratio>6). The waste with lower particle size having higher specific surface area exhibits somewhat positive effect on the S/S performance. The use of fly ash from municipal waste incinerators, in conjunction with the reduced amount of cement, is able to meet the TCLP arsenic and lead standards. The use of lime alone could meet the TCLP arsenic standard, but lead leaching concentrations exceeded leaching Pb standard. The results of semi-dynamic leaching tests of some solidified samples indicate higher accumulated arsenic leaching concentrations after only a few leachant renewals.

Arsenic↗
PubMed1990

Acute toxicity testing in the nonlethal dose range: a new approach.

A new modification of acute toxicity testing of chemicals in rats is presented. Instead of using death as the principal criterion of toxicity, it is based on a careful, standardized clinical assessment of toxic signs measured in the nonlethal dose range. Test compounds are administered to groups of rats at four dose levels, selected on the basis of pilot experiments. General indices of toxicity, i.e., body weight gain, food and water consumption, and body temperature, are recorded at regular intervals; activity in the home cage is monitored continuously with a newly developed passive infrared device; neurobehavioral dysfunctions are assessed repeatedly with a checklist; and routine hematology is done on the 4th day after administration of the test compounds. All measured signs of toxicity are scored in relation to the control groups so that the absolute magnitude of the score increases as a function of the deviation from the normal conditions of the animals. In order to take into consideration the course of intoxication and the rate of recovery, toxicity scores are added over the duration of the whole experiment. For each variable measured, the resulting total scores are converted into a relative point system, scaling from 0 to 10 points. These points are added to a single "total ToxScore" value for each dose group. A regression line is calculated for these total ToxScore points, and the dose giving 15 total ToxScore points is determined. Based on the results obtained with nine reference substances, a classification system is proposed that is comparable to that based on LD50 values. It is concluded that the proposed test procedure provides much more information on the signs of acute toxicity, the course of the intoxication, the slope of the dose-effect curve, and the rate of recovery than does the standard LD50 test. In addition, the degree of distress and suffering of the animals is reduced.

Acetanilides↗
PubMed2001

A combined treatment approach using Fenton's reagent and zero valent iron for the removal of arsenic from drinking water.

Studies on the development of an arsenic remediation approach using Fenton's reagent (H2O2 and Fe(II)) followed by passage through zero valent iron is reported. The efficiency of the process was investigated under various operating conditions. Potable municipal water and ground water samples spiked with arsenic(III) and (V) were used in the investigations. The arsenic content was determined by ICP-QMS. A HPLC-ICPMS procedure was used for the speciation and determination of both As(III) and (V) in the processed samples, to study the effectiveness of the oxidation step and the subsequent removal of the arsenic. The optimisation studies indicate that addition of 100 microl of H2O2 and 100 mg of Fe(II) (as ferrous ammonium sulphate) per litre of water for initial treatment followed by passing through zero valent iron, after a reaction time of 10 min, is capable of removing arsenic to lower than the US Environmental Protection Agency (EPA) guideline value of 10 microg/l, from a starting concentration of 2 mg/l of As(III). Using these suggested amounts, several experiments were carried out at different concentrations of As(III). Residual hydrogen peroxide in the processed samples can be eliminated by subsequent chlorination, making the water, thus, processed, suitable for drinking purposes. This approach is simple and cost effective for use at community levels.

Arsenic↗
PubMed1999

Oxidation of arsenic bearing fly ash as pretreatment before solidification.

When a waste fly ash, containing large amounts of As(2)O(3), is solidified using cement and lime, the arsenic concentration in the leachate (extraction test DIN 38 414 S4) is determined by the solubility of CaHAsO(3) and can be lowered to a value of ca. 5 mg/l, in a saturated solution of Ca(OH)(2). One of the criteria for landfilling of hazardous waste is, however, that the arsenic concentration in the leachate must be lower than 1 mg/l. In this paper, it is shown that oxidation of the waste before solidification, whereby As(III) is oxidised to As(V) using H(2)O(2), lowers the leaching of arsenic, and other contaminants, from the solidified product. With the speciation program MINTEQA2, it is calculated that the solubility of As(V) in the presence of a pure Ca(3)(AsO(4))(2) precipitate is lower than the solubility of As(III) in the presence of a pure CaHAsO(3) precipitate. The arsenic concentration in the presence of both a Ca(OH)(2) and a Ca(3)(AsO(4))(2) precipitate can even be lowered to 0.47 mg/l (pH 12.5). The As concentration in the leachate of the extraction test on an oxidised S/S sample was indeed lowered to ca. 0.5 mg/l, which is a reduction by a factor of 10 compared to the concentration of ca. 5 mg/l, obtained in the leachate of the extraction test on a non-oxidised S/S sample. This is in very good agreement with the calculated value of 0.47 mg/l. Also, the pretreatment decreased the cumulative fraction of arsenic released over the entire test period of a semi-dynamic leach test by a factor of 7. At all times during the test, the As concentration did not exceed the norm of 1 mg/l.

Algorithms↗
PubMed2002

Arsenic removal from water using advanced oxidation processes.

Consumption of groundwaters containing natural arsenic at several hundred microg/l (ppb) in countries such as Bangladesh has lead to the increased occurrence of many cancers particularly those of the skin and bladder, while concerns in the USA and Australia regarding the unknown health impact of drinking water containing tens of ppb of arsenic is leading to increasingly stringent maximum contaminant levels. The anaerobic conditions of these groundwaters result in the arsenic being present in its reduced form, hence the use of an oxidant is necessary if the arsenic is to be successfully removed by precipitation or ion exchange methods. Advance oxidation methods which utilise ultraviolet light and a photo absorber have been developed and patented, in which both iron salts and sulphite can be used as the photoabsorber. The former absorber has been developed for arsenic removal in rural areas of Bangladesh and the latter for groundwaters in countries such as the USA.

Arsenic↗
PubMed1981

Inhibition of D(--)-beta-hydroxybutyrate dehydrogenase by modifiers of disulfides, thiols, and vicinal dithiols.

D(--)-beta-hydroxybutyrate dehydrogenase of beef heart mitochondria catalyzes the reversible oxidation of D-(--)-beta-hydroxybutyrate to acetoacetate in the presence of NAD. Both the membrane-bound and the soluble forms of the enzyme are inhibited by modifiers of thiols [N-ethylmaleimide (NEM) and p-(chloromercuri)phenylsulfonate (pCMS)], vicinal dithiols [phenylarsine oxide and diazenedicarboxylic acid bis(dimethylamide) (diamide)], and disulfides (sulfite, sulfide, and cyanide). NAD and NADH, but not beta-hydroxybutyrate and acetoacetate, protect the enzyme against inhibition by NEM, pCMS, phenylarsine oxide, and diamide. As tested with NEM and diamide, the inhibitions caused by mono- and dithiol modifiers were pseudo first order, and the reaction order with respect to the concentration of either inhibitor was unity, thus indicating the modification of a single essential thiol and/or dithiol. Sulfite and sulfide inhibitions appeared to be competitive with respect to beta-hydroxybutyrate, with Ki values of 10-15 and about 240 microM, respectively. Sulfite inhibition was uncompetitive with respect to NAD, NADH, and acetoacetate. The above results have suggested the presence in D(--)-beta-hydroxybutyrate dehydrogenase of an essential thiol and/or a vicinal dithiol associated with the binding site(s) of NAD and NADH. The inhibition by sulfite, sulfide, and cyanide might be indicative of the presence of an essential disulfide or due to a ternary complex formation involving the enzyme, NAD, and the above nucleophiles.

Acetoacetates↗
PubMed1981

Affinity labeling of residues within Hv2 of guinea pig anti-azobenzenearsonate antibodies of different isotypes and from different strains.

Anti-p-azobenzenearsonate (ARS) antibodies of IgG1 and IgG2 isotypes produced in inbred strain 13 and strain 2 guinea pigs were affinity labeled with N-(bromoacetyl)-3-[(p-arsonophenyl)azo]-L-tyrosine (BAAT) or N-(bromoacetyl)-p-arsanilic acid (BAA). BAAT was shown to modify approximately 50% of the binding sites specifically and BAA approximately 30%. Both reagents preferentially modified residues in the heavy (H) chain to the extent that it contained over 80% of the affinity label associated with the native molecule. At least 80% of label borne by the variable domain of the H chain (VH) was found in the second hypervariable region (Hv2). BAAT labeled all anti-ARS antibodies exclusively at position N-59, which contains a lysyl residue. BAA labeled predominantly tyrosine at N-57 and, to a lesser extent, lysine-59 and tyrosine-50. Comparison of Hv2 sequences in anti-ARS and in antibodies reactive with other haptens has shown that tyrosine at N-50 and N-57 as well as lysine at N-59 is distinctive of antibodies with anti-ARS specificity, thus implying their involvement in antigen binding. The predominant sequence of Hv2 was identical in anti-ARS IgG1 and IgG2 molecules induced in either inbred guinea pig strain following either carrier priming or conventional immunization. Although limited variability does occur among the various populations of anti-ARS antibodies in certain residue positions in Hv2, no significant differences in the binding affinities or in the indexes of heterogeneity were seen among the various kinds of anti-ARS antibodies.

Affinity Labels↗
PubMed1976

Circular dichroism-inhibitor titrations of arsanilazotyrosine-248 carboxypeptidase A.

Coupling of carboxypeptidase with diazotized arsanilic acid specifically modifies a single tyrosyl residue. Yet, owing to the fact that the resultant azoTyr-248 can form an intramolecular chelate with zinc, two different circular dichroism probes result: azoTyr-248 itself and the azoTyr-248-Zn chelate. Both are environmentally sensitive and, characteristically, each can signal the same or different perturbations, as is apparent from circular dichroic spectra. This dual probe function greatly magnifies the scope of these chromophores in mapping the topography of the active center with respect to sites of interaction of inhibitors (or substrates). Titration of the azoenzyme with a series of synthetic, competitive inhibitors, e.g., L-benzylsuccinate, L-phenyllactate, and L-Phe, and with the pseudosubstrate, Gly-L-Tyr, in turn generates characteristic circular dichroic spectra. Their analysis yields a single binding constant for each of these agents, one molecule of each binding to the active center. Mixed inhibitions, as seen with beta-phenylpropionate and phenylacetate, resolved previously into competitive and noncompetitive components, are characterized by different spectral effects. Two molecules of these agents bind to the enzyme, consistent with both thermodynamic and enzymatic studies. The interactions leading to competitive and noncompetitive inhibition, respectively, can be recognized and assigned, based on the manner in which the extrema at 340 and 420 nm, reflecting azoTyr-248, and the negative 510-nm circular dichroism band, typical of its chelate with zinc, are affected and on the pH dependence of spectral and kinetic data. Certai4 noncompetitive inhibitors and modifiers induce yet other spectral features. Each probe is very sensitive to changes in its particular active center environment, though both can be relatively insensitive to inhibitors interacting at a distance from the active center.

Arsenic↗
PubMed1975

Environment and conformation dependent sensitivity of the arsanilazotyrosine-248 carboxypeptidase A chromophore.

Reaction of carboxypeptidase A crystals with diazotized arsanilic acid uniquely modifies Tyr-248 to form a monazo derivative, which-in solution-forms an intramolecular inner-sphere coordination complex in the active site zinc atom. tarsanilazocarboxypeptidase exhibits spectral properties that are closely similar to those of the model complex, tetrazolylazo-N-carbobenzoxytyrosine Zn2+, with a distinctive maximum at 510 nm. In addition, its circular dichroic spectrum reveals a negative extremum at this wavelength, also characteristic of this complex. Both spectra are exquisitely responsive to pth changes and serve to monitor formation and dissociation of the metal-azophenol complex. Two pKapp at 7.7 and 9.5 delineate the pH range over which the probe characteristics most effectively gauge conformational features of the active center of arsanilazcarboxypeptidase. Other environmental parameters, e.g., substrates and inhibitors, as well as crystallization of the enzyme also critically influence the formation and dissociation of the complex; the response of the probe suggests that they induce conformational movement of the azoTyr-248 residue away from the zinc atom. tthe now available chemical, functional, structural data bearing on the spatial relationships of Tyr-248 and Zn, both thought critical to catalysis, are evaluated, based on spectra of arsanilazo- and nitrocarboxypeptidase crystals and solutions as well as on detailed kinetic analyses of the native enzyme in both physical states and based on the X-ray structure analysis of the native enzyme and its Gly-L-Tyr complex. Collectively all of the data show that the conformation of carboxypeptidase in crystals differs from that in solution. Moreover, reexamination of the original X-ray maps reported in 1968 and thought to preclude a Tyr-248-Zn interaction now leads to the conclusion that in up to 25 per cent of the molecules in the crystals ttyr-248 interacts with the active site zinc atom (W.D. Lipscomb (1973), Proc. Nat. Acad. Sci U.S. 70, 3797). Thus, even in the crystals the enzyme exists in at least two different conformations. In one of these Tyr-248 is near while in the other it is far from the zinc atom. The spectral effects of Gly-L-Tyr and beta-phenylpropionate on solutions of arsanilazo- and of nitrocarboxypeptidase demonstrate that during the catalytic process Tyr-248 moves away from the zinc atom. This implies a mechanistic role for Tyr-248 different from that postulated on the basis of X-ray crystallographic analysis. Indeed, the proximity of ttyr-248 to the zinc atom, when altered by substrates and inhibitor, may reflect certain of the properties characteristic of the entatic, active site.

Animals↗