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1.
Oxidation of As(Ⅲ) by potassium permanganate   总被引:3,自引:1,他引:2  
The oxidation of As(Ⅲ) with potassium permanganate was studied under conditions including pH, initial As(Ⅲ) concentration and dosage of Mn(Ⅶ). The results have shown that potassium permanganate was an effective agent for oxidation of As(Ⅲ) in a wide pH range. The pH value of tested water was not a significant factor affecting the oxidation of As(Ⅲ) by Mn(Ⅲ). Although theoretical redox analyses suggest that Mn(Ⅶ) should have better performance in oxidization of As(Ⅲ) within lower pH ranges, the experimental results show that the oxidation efficiencies of As(Ⅲ) under basic and acidic conditions were similar, which may be due to the adsorption of As(Ⅲ) on the Mn(OH)2 and MnO2 resulting from the oxidation of As(Ⅲ).  相似文献   

2.
Sediments from an arsenic(As) contaminated groundwater vent site were used to investigate As( Ⅲ) binding, transformation and redistribution in native and iron oxide amended lake sediments using aging spiked batch reactions and a sequential extraction procedure that maintains As(V) and As( Ⅲ) speciation. In the native sediments, fractionation analysis revealed that 10% of the spiked As( Ⅲ) remained intact after a 32-day aging experiment and was predominantly adsorbed to the strongly sorbed(NH_4H_2PO_4 extractable) and amorphous Fe oxide bound(H_3PO_4 extractable) fractions. Kinetic modelling of the experimental results allowed identifying the dominant reaction path for depletion of dissolved As( Ⅲ) to As( Ⅲ)absorbed on to the solid phase, followed by oxidation in the solid phase. Arsenite was initially adsorbed primarily to the easily exchangeable fraction((NH_4)_2SO_4 extractable), then rapidly transformed into As(V) and redistributed to the strongly sorbed and amorphous Fe oxide bound fractions. Oxidation of As( Ⅲ) in recalcitrant fractions was less efficient. The iron oxide amendments illustrated the controls that iron oxides can have on As( Ⅲ) binding and transformation rates. In goethite amended samples As( Ⅲ) oxidation was faster and primarily occurred in the strongly sorbed and amorphous Fe oxide bound fractions. In these samples,19.3 μg Mn was redistributed(compared to the native sediment) from the easily exchangeable and crystalline Fe oxide bound fractions to the strongly sorbed and amorphous Fe oxide bound fractions, indicating that goethite may act as a catalyst for Mn(Ⅱ) oxidation, thereby producing sorbed Mn( Ⅲ/Ⅳ ), which then appears to be involved in rapidly oxidizing As( Ⅲ).  相似文献   

3.
Removal of 2-methylisoborneol (MIB) in drinking water by ozone, powdered activated carbon (PAC), potassium permanganate and potassium ferrate was investigated. The adsorption kinetics of MIB by both wood-based and coat-based PACs show that main removal of MIB occurs within contact time of 1 h. Compared with the wood-based PAC, the coat-based PAC evidently improved the removal efficiency of MIB. The removal percentage of trace MIB at any given time for a particular carbon dosage was irrelative to the initial concentration of MIB. A series of experiments were performed to determine the effect of pH on the ozonation of MIB. The results show that pH has a significant effect on the ozonation of MIB. It is conclusive that potassium permanganate and potassium ferrate are ineffective in removing the MIB in drinking water.  相似文献   

4.
5.
Oxidation of aniline by persulfate in aqueous solutions was investigated and the reaction kinetic rates under different temperature, persulfate concentration and pH conditions were examined in batch experiments. The results showed that, the aniline degradation followed pseudo first-order reaction model. Aniline degradation rate increased with increasing temperature or persulfate concentration. In the pH range of 3 to 11, a low aniline degradation rate was obtained at strong acid system (pH 3), while a high degradation rate was achieved at strong alkalinity (pH 11). Maximum aniline degradation occurred at pH 7 when the solution was in a weak level of acid and alkalinity (pH 5, 7 and 9). Produced intermediates during the oxidation process were identified using liquid chromatography-mass spectrometry technology. And nitrobenzene, 4-4’-diaminodiphenyl and 1-hydroxy-1,2-diphenylhydrazine have been identified as the major intermediates of aniline oxidation by persulfate and the degradation mechanism of aniline was also tentatively proposed.  相似文献   

6.
Permanganate treatment is widely used for disinfection of bacteria in surface-contaminated water. In this paper, the fate of the dissolved permanganate in aqueous solution after contact with cells of Pseudomonas fluorescens was studied. Concomitant accumulation of divalent cations of Mg~(2+), Zn~(2+), and Co~(2+) during precipitation of Mn oxides was also studied. The time course of the Mn concentration in solution showed an abrupt decrease after contact of Mn(VII) with microbial cells, followed by an increase after ~ 24 hr.XRD analysis of the precipitated Mn oxides, called biomass Mn oxides, showed the formation of low-crystalline birnessite. Visible spectroscopy and X-ray absorption near edge structure(XANES) analyses indicated that dissolved Mn(VII) was reduced to form biomass Mn oxides involving Mn(IV) and Mn(III), followed by reduction to soluble Mn(II).The numbers of electron transferred from microbial cells to permanganate and to biomass Mn oxides for 24 hr after the contact indicated that the numbers of electron transfer from microbial cell was approximately 50 times higher to dissolved permanganate than to the biomass Mn oxides in present experimental conditions. The 24 hr accumulation of divalent cations during formation of biomass Mn oxides was in the order of Co~(2+) Zn~(2+) Mg~(2+).XANES analysis of Co showed that oxidation of Co~(2+) to Co~(3+) resulted in higher accumulation of Co than Zn and Mg. Thus, treatment of surface water by KMnO_4 solution is effective not only for disinfection of microorganisms, but also for the elimination of metal cations from surface water.  相似文献   

7.
Ru(Ⅲ) was employed as catalyst for aniline oxidation by permanganate at environmentally relevant pH for the first time. Ru(Ⅲ) could significantly improve the oxidation rate of aniline by 5-24 times with its concentration increasing from 2.5 to 15 μmol/L. The reaction of Ru(Ⅲ) catalyzed permanganate oxidation of aniline was first-order with respect to aniline, permanganate and Ru(Ⅲ), respectively. Thus the oxidation kinetics can be described by a third-order rate law. Aniline degradation by Ru(Ⅲ) catalyzed permanganate oxidation was markedly influenced by pH, and the second-order rate constant (ktapp) decreased from 643.20 to 2.67 (mol/L)^-1 sec^-1 with increasing pH from 4.0 to 9.0, which was possibly due to the decrease of permanganate oxidation potential with increasing pH. In both the uncatalytic and catalytic permanganate oxidation, six byproducts of aniline were identified in UPLC-MS/MS analysis. Ru(Ⅲ), as an electron shuttle, was oxidized by permanganate to Ru(Ⅵ) and Ru(Ⅶ), which acted the co-oxidants for decomposition of aniline. Although Ru(Ⅲ) could catalyze permanganate oxidation of aniline effectively, dosing homogeneous Ru(Ⅲ) into water would lead to a second pollution. Therefore, efforts would be made to investigate the catalytic performance of supported Ru(Ⅲ) toward permanganate oxidation in our future study.  相似文献   

8.
In this study we investigated the enrichment ability of oxidized multiwalled carbon nanotubes (MWCNTs) and established a new method for the determination of trace cadmium in environment with flame atomic absorption spectrometry.The MWCNTs were oxidized by potassium permanganate under appropriate conditions before use as preconcentration packing.Parameters influencing the recoveries of target analytes were optimized.Under optimal conditions,the target analyte exhibited a good linearity (R~2=0.9992) over the concentration range 0.5-50 ng/ml.The detection limit and precision of the proposed method were 0.15 ng/ml and 2.06%, respectively.The proposed method was applied to the determination of cadmium in real-world environmental samples and the recoveries were in the range of 91.3%-108.0%.All these experimental results indicated that this new procedure could be applied to the determination of trace cadmium in environmental waters.  相似文献   

9.
Arsenic in the environment is attracting increasing attention due to its chronic health effects. Although arsenite(As(III)) is generally more mobile and more toxic than arsenate(As(V)), reducing As(V) to As(III) may still be a means for decontamination, because As(III) can be removed from solution by precipitation with sulfide or by adsorption or complexation with other metal sulfides. The performance of As(V) bio-reduction under autohydrogenotrophic conditions was investigated with batch experiments. The results showed that As(V) reduction was a biochemical process while both acclimated sludge and hydrogen were essential. Most of the reduced arsenic remained in a soluble form, although 20% was removed with no addition of sulfate, while 82% was removed when sulfate was reduced to sulfide. The results demonstrated that the reduced arsenic was re-sequestered in the precipitates, probably as arsenic sulfides. Kinetic analysis showed that pseudo first-order kinetics described the bio-reduction process better than pseudo second-order. In particular, the influences of pH and temperature on As(V) reduction by acclimated sludge under autohydrogenotrophic conditions and total soluble As removal were examined. The reduction process was highly sensitive to both pH and temperature, with the optimum ranges of pH 6.5–7.0 and 30–40°C respectively. Furthermore, Arrhenius modeling results for the temperature effect indicated that the As(V) reduction trend was systematic. Total soluble As removal was consistent with the trend of As(V) reduction.  相似文献   

10.
The study was to investigate the adsorption behavior of arsenite (As(Ⅲ)) and arsenate (As(Ⅴ)) on two variable charge soils, i.e., Haplic Acrisol and Rhodic Ferralsol at different ionic strengths and pH with batch methods. Results indicated that the amount of As(Ⅲ) adsorbed by these two soils increased with increasing solution pH, whereas it decreased with increasing ionic strength under the acidic condition. This suggested that As(Ⅲ) was mainly adsorbed on soil positive charge sites through electrostatic attraction under the acidic condition. Moreover, intersects of As(Ⅴ) adsorption-pH curves at different ionic strengths (a characteristic pH) are obtained for both soils. It was noted that above this pH, the adsorption of As(Ⅴ) was increased with increasing ionic strength, whereas below it the reverse trend was true. Precisely the intersect pH was 3.6 for Haplic Acrisol and 4.5 for Rhodic Ferralsol, which was near the values of PZSE (soil point of zero salt effect) of these soils. The effects of ionic strength and pH on arsenate adsorption by these soils were interpreted by the adsorption model. The results of zeta potential suggested that the potential in adsorption plane becomes less negative with increasing ionic strength above soil PZSE and decreases with increasing ionic strength below soil PZSE. These results further supported the hypothesis of the adsorption model that the potential in the adsorption plane changes with ionic strength with an opposite trend to surface charge of the soils. Therefore, the change of the potential in the adsorption plane was mainly responsible for the change of arsenate adsorption induced by ionic strength on variable charge soils.  相似文献   

11.
Simultaneous elimination of As(Ⅲ) and Pb(Ⅱ) from wastewater is still a great challenge.In this work,an iron-sulfur codoped biochar (Fe/S-BC) was successfully fabricated in a simplified way and was applied to the remediate the co-pollution of As(Ⅲ) and Pb(Ⅱ).The positive enthalpy indicated that the adsorption in As-Pb co-pollution was an endothermic reaction.The mechanism of As(Ⅲ) removal could be illustrated by surface complexation,oxidation and precipitation.In addition to precipitation and com...  相似文献   

12.
The characteristics of Pb2+ adsorption on the surface of birnessites with different average oxidation states (AOS) of Mn, synthesized under acidic and alkali conditions, were investigated. The results indicated that the amount of adsorbed Pb2+ increased with the increase of Mn AOS in birnessites. The amount of Pb2+ adsorbed positively correlated with the amount of released Mn2+, H+, and K+ (r = 0.9962 > 0.6614, n = 14, α = 0.01). The released Mn2+, H+, and K+ were derived mostly from the corresponding catio...  相似文献   

13.
The ubiquitous arsenic in groundwater poses a great risk to human health due to its environmental toxicity and carcinogenicity. In the present work, a new adsorbent, δ-MnO2 modified activated carbon, was prepared, and its performance for the uptake of arsenate and arsenite species from aqueous solutions was investigated by batch experiments. Various techniques, including FESEM-EDX, p-XRD, XPS and BET surface area analysis, were employed to characterize the properties of the adsorbent and the arsenic adsorption mechanisms. The results showed that δ-MnO2 covered on the surface and padded in the pores of the activated carbon. Adsorption kinetic studies revealed that approximately 90.1% and 76.8% of As(III) and As(V), respectively, were removed by the adsorbent in the first 9 hr, and adsorption achieved equilibrium within 48 hr. The maximum adsorption capacities of As(V) and As(III) at pH 4.0 calculated from Langmuir adsorption isotherms were 13.30 and 12.56 mg/g, respectively. The effect of pH on As(V) and As(III) removal was similar, and the removal efficiency significantly reduced with the increase of solution pH. Arsenite oxidation and adsorption kinetics showed that the As(V) concentration in solution due to As(III) oxidation and reductive dissolution of MnO2 increased rapidly during the first 12 min, and then gradually decreased. Based on the XPS analysis, nearly 93.3% of As(III) had been oxidized to As(V) on the adsorbent surface and around 38.9% of Mn(IV) had been reduced to Mn(II) after As(III) adsorption. This approach provides a possible method for the purification of arsenic-contaminated groundwater.  相似文献   

14.
p-Arsanilic acid(p-ASA) is widely used in China as livestock and poultry feed additive for promoting animal growth.The use of organoarsenics poses a potential threat to the environment because it is mostly excreted by animals in its original form and can be transformed by UV–Vis light excitation.This work examined the initial rate and efficiency of p-ASA phototransformation under UV-C disinfection lamp.Several factors influencing p-ASA phototransformation,namely,p H,initial concentration,temperature,as well as the presence of Na Cl,NH4+,and humic acid,were investigated.Quenching experiments and LC–MS were performed to investigate the mechanism of p-ASA phototransformation.Results show that p-ASA was decomposed to inorganic arsenic(including As(Ⅲ) and As(V))and aromatic products by UV-C light through direct photolysis and indirect oxidation.The oxidation efficency of p-ASA by direct photosis was about 32%,and those by HOU and1O2 were 19% and 49%,respectively.Cleavage of the arsenic–benzene bond through direct photolysis,HOU oxidation or1O2 oxidation results in simultaneous formation of inorganic As(Ⅲ),As(IV),and As(V).Inorganic As(Ⅲ) is oxidized to As(IV) and then to As(V) by1O2 or HOU.As(IV) can undergo dismutation or simply react with oxygen to produce As(V) as well.Reactions of the organic moieties of p-ASA produce aniline,aminophenol and azobenzene derivatives as main products.The photoconvertible property of p-ASA implies that UV disinfection of wastewaters from poultry and swine farms containing p-ASA poses a potential threat to the ecosystem,especially agricultural environments.  相似文献   

15.
Arsenite oxidation by three types of manganese oxides   总被引:5,自引:0,他引:5  
Oxidation of As(Ⅲ) by three types of manganese oxides and the effects ofpH, ion strength and tartaric acid on the oxidation were investigated by means of chemical analysis, equilibrium redox, X-ray diffraction (XRD) and transmission electron microscopy (TEM). Three synthesized Mn oxide minerals, bimessite, cryptomelane, and hausmannite, which widely occur in soil and sediments, could actively oxidize As(Ⅲ) to As(Ⅴ). However, their ability in As(Ⅲ)-oxidation varied greatly depending on their structure, composition and surface properties. Tunnel structured cryptomelane exhibited the highest ability of As (Ⅲ) oxidation, followed by the layer structured birnessite and the lower oxide hausmannite. The maximum amount of As (Ⅴ) produced by the oxidation was in the order (mmol/kg) of cryptomelane (824.2) 〉 bimessite (480.4) 〉 hausmannite (117.9), As pH increased from the very low value(pH 2.5), the amount of As(Ⅲ) oxidized by the tested Mn oxides was firstly decreased, then negatively peaked in pH 3.0 6.5, and eventually increased remarkably. Oxidation of As(Ⅲ) by the Mn oxides had a buffering effects on the pH variation in the solution. It is proposed that the oxidative reaction processes between As (Ⅲ) and biruessite(or cryptomelane) are as follows: (1) at lower pH condition: (MnO2)x+ H3AsO3 + 0.5H^+=0.5H2AsO4^- + 0.5HAsO4^2- +Mn〉^2+ (MnO2)x-1 + H2O; (2) at higher pH condition: (MnO2)x + H3AsO3 = 0.5H2AsO4^- + 0.5HAsO4^2- + 1.5H^+ + (MnO2)x-1. MnO. With increase of ion strength, the As(Ⅲ) oxidized by bimessite and cryptomelane decreased and was negatively correlated with ion strength. However, ion strength had little influence on As (Ⅲ) oxidation by the hausmarmite. The presence of tartaric acid promoted oxidation of As(Ⅲ) by birnessite. As for cryptomelane and hansmannite, the same effect was observed when the concentration of tartaric acid was below 4 mmol/L, otherwise the oxidized As(Ⅲ) decreased. These findings are of great significance in improving our understanding of As geochemical cycling and controlling As contamination.  相似文献   

16.
The stability and parameters of a bio-ceramic filter for completely autotrophic nitrogen removal were investigated.The completely autotrophic nitrogen removal over nitrite(CANON) reactor was fed with different concentrations of ammonia(400,300,and 200mg N/L) but constant influent ammonia load.The results showed that the CANON system can achieve good treatment performance at ambient temperature(15-23°C).The average removal rate and removal loading of NH4+-N and TN was 83.90%,1.26kg N/(m3·day),and 70.14%,1.09kg N/(m3·day),respectively.Among the influencing factors like pH,dissolved oxygen and alkalinity,it was indicated that the pH was the key parameter of the performance of the CANON system.Observing the variation of pH would contribute to better control of the CANON system in an intuitive and fast way.Denaturing gradient gel electrophoresis analysis of microorganisms further revealed that there were some significant changes in the community structure of ammonium oxidizing bacteria,which had low diversity in different stages,while the species of anaerobic ammonium oxidizing(anammox) bacteria were fewer and the community composition was relatively stable.These observations showed that anaerobic ammonia oxidation was more stable than the aerobic ammonia oxidation,which could explain that why the CANON system maintained a good removal efficiency under the changing substrate conditions.  相似文献   

17.
In order to understand the similarity or difference of inorganic As species uptake and transport related to phosphorus in As-hyperaccumulator, uptake and transport of arsenate (As(Ⅴ)) and arsenite (As(Ⅲ)) were studied using Pteris vittata L. under sand culture. Higher concentrations of phosphate were found to inhibit accumulation of arsenate and arsenite in the fronds of P. vittata. The reduction in As accumulation was greater in old fronds than in young fronds, and relatively weak in root and rhizome. Moderate increases, from 0.05 to 0.3 mmol/L, in phosphate reduced uptake of As(Ⅲ) more than As(Ⅴ), while the reverse was observed at high concentrations of phosphate (≥ 1.0 mmol/L). Phosphate apparently reduced As transport and the proportion of As accumulated in fronds of P. vittata when As was supplied as As(Ⅴ). It may in part be due to competition between phosphorus and As(Ⅴ) during transport. In contrast, phosphate had a much smaller effect on As transport when the As was supplied as As(Ⅲ). Therefore, the results from present experiments indicates that a higher concentration of phosphate suppressed As accumulation and transport in P. vittata, especially in the fronds, when exposure to As(Ⅴ); but the suppression of phosphate to As transport in the root or rhizome may be insignificant when P. vittata when exposure to As(Ⅲ) under sand culture conditions. The finding will help to understand the interaction of P and As during their uptake process in P. vittata.  相似文献   

18.
Antimony (Sb) is a toxic and carcinogenic element that often enters soil in the form of antimony trioxide (Sb2O3) and coexists with manganese (Mn) in weakly alkaline conditions. Mn oxides such as birnessite have been found to promote the oxidative dissolution of Sb2O3, but few researches concerned the co-transformations of Sb2O3 and Mn(II) in environment. This study investigated the mutual effect of abiotic oxidation of Mn(II) and the coupled oxidative dissolution of Sb2O3. The influencing factors, such as Mn(II) concentrations, pH and oxygen were also discussed. Furthermore, their co-transformed mechanism was also explored based on the analysis of Mn(II) oxidation products with or without Sb2O3 using XRD, SEM and XPS. The results showed that the oxidative dissolution of Sb2O3 was enhanced under higher pH and higher Mn(II) loadings. With a lower Mn(II) concentration such as 0.01 mmol/L Mn(II) at pH 9.0, the improved dissolution of Sb2O3 was attributed to the generation of dissolved intermediate Mn(III) species with strong oxidation capacity. However, under higher Mn(II) concentrations, both amorphous Mn(III) oxides and intermediate Mn(III) species were responsible for promoting the oxidative dissolution of Sb2O3. Most released Sb (∼72%) was immobilized by Mn oxides and Sb(V) was dominant in the adsorbed and dissolved total Sb. Meanwhile, the presence of Sb2O3 not only inhibited the removal of Mn(II) by reducing Mn(III) to Mn(II) but also affected the final products of Mn oxides. For example, amorphous Mn oxides were formed instead of crystalline Mn(III) oxides, such as MnOOH. Furthermore, rhodochrosite (MnCO3) was formed with the high Mn(II)/Sb2O3 ratio, but without being observed in the low Mn(II)/Sb2O3 ratio. The results of study could help provide more understanding about the fate of Sb in the environment and the redox transformation of Mn.  相似文献   

19.
Hausmannite is a common low valence Mn oxide mineral, with a distorted spinel structure, in surficial sediments. Although natural Mn oxides often contain various impurities of transitional metals (TMs), few studies have addressed the effect and related mechanism of TM doping on the reactivity of hausmannite with metal pollutants. Here, the reactivity of cobalt (Co) doped hausmannite with aqueous As(III) and As(V) was studied. Co doping decreased the point of zero charge of hausmannite and its adsorption capacity for As(V). Despite a reduction of the initial As(III) oxidation rate, Co-doped hausmannite could effectively oxidize As(III) to As(V), followed by the adsorption and fixation of a large amount of As(V) on the mineral surface. Arsenic K-edge EXAFS analysis of the samples after As(V) adsorption and As(III) oxidation revealed that only As(V) was adsorbed on the mineral surface, with an average As-Mn distance of 3.25–3.30 Å, indicating the formation of bidentate binuclear complexes. These results provide new insights into the interaction mechanism between TMs and low valence Mn oxides and their effect on the geochemical behaviors of metal pollutants.  相似文献   

20.
The kinetics of the recombinant Coprinus cinereus peroxidase-catalyzed 2-naphthol oxidation was investigated in the presence of rhamnolipid biosurfactant JBR425 and synthetic surfactant Surfynol465 at pH 5.5 and 25℃, with concentrations of (bio)surfactants both less than critical micelle concentrations (CMC) and larger than CMC. It was shown that monomers of JBR425 as well as monomers of Surfynol465 had an enhancing effect on the conversion of 2-naphthol in dose response manner and did not influence the initial rate of 2-naphthol oxidation. The results were accounted by a scheme, which contains a stadium of enzyme inhibition by oligomeric 2-naphthol oxidation products. The action of the biosurfactant's (or synthetic surfactant's) monomers was explained by avoidance of the enzyme active center clothing with oligomers. Similar results have demonstrated the potential of rhamnolipid biosurfactant JBR425 due to its biodegradability. When biosurfactants' concentrations are larger than CMC, (bio)surfactants have an opposite effect on the oxidation of 2-naphthol by peroxidase.  相似文献   

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