Degrading a mixture of three textile dyes using photo-assisted electrochemical process with BDD anode and O2–diffusion cathode

In this paper, degradation of a mixture of three azo dyes was studied by the photo-assisted electrochemical process using an O₂-diffusion cathode containing carbon nanotubes and boron-doped diamond (BDD) anode. The concentration of three textile dyes (C.I. Acid Orange 8 (AO8), C.I. Acid Orange 10 (AO10), and C.I. Acid Orange 12 (AO12)) was determined simultaneously despite the severe overlap of their spectra. For this purpose, partial least square (PLS), as a multivariate calibration method, was utilized based on recording UV–Vis spectra during the decolorization process. Moreover, the central composite design was used for the modeling of photo-assisted electrochemical decolorization of the aqueous solutions containing three dyes. The investigated parameters were the initial concentration of three dyes, applied current and reaction time. Analysis of variance (ANOVA) revealed that the obtained regression models match the experimental results well with R (Khataee et al. 2010, Clean-Soil Air Water 38 (1):96–103, 2010) of 0.972, 0.971, and 0.957 for AO8, AO10, and AO12, respectively. Three-dimensional surface and contour plots were applied to describe the relation between experimental conditions and the observed response. The results of TOC analysis confirmed good ability of proposed photo-assisted electrochemical process for degradation and mineralization of textile industry wastewater.     

Reducing degradation of azo dye by zero-valent iron in aqueous solution

The reducing degradation kinetics of five azo dyes, Acid orange II, Acid orange IV, Acid orange GG, Acid red 3B and Orange I, by zero-valent iron powder in aqueous solution were studied. It showed that the degradation is a two-step reaction, with the first step being reversible. Solution acidity and iron surface area are the factors greatly influencing the degradation rates, and with increasing of acidity and iron surface area, the degradation rates increase.     

The influence of FeCl3 on the photocatalytic degradation of dissolved azo dyes in aqueous TiO2 suspensions

The study concerned decolouration of solutions of azo, anionic (Acid Orange 7, Reactive Red 45, Acid Yellow 23) and cationic (Basic Blue 41 and Basic Orange 66) dyes during illumination with UV (lambdamax 366 nm) irradiation in the presence of TiO2 and FeCl3. The process of decolouration during illumination of the solutions studied containing FeCl3 underwent significant intensification in the case of anionic dyes and unfavourable inhibition in case of cationic dyes. It was also observed that FeCl3 had a diverse influence on the adsorption of the dyes studied on TiO2. The adsorption of anionic dyes and decolouration of solutions before the illumination was observed only in the presence of FeCl3. In case of cationic dyes the addition of FeCl3 caused elimination of these phenomena. An additional cause of decolouration of anionic dyes solutions before illumination was the precipitation of their poorly soluble compounds from Fe3+. The processes of degradation and mineralization of the dye that accompanied decolouration of Acid Orange 7 solutions were also observed. It was stated that similarly to the case of Acid Orange 7, the decolouration of the studied anionic dyes' solutions can depend on the concentration of FeCl3, the amount of TiO2 and the initial concentration of the dye in its solution.     

真菌和细菌对染料吸附脱色的高效共培养体系研究

在含有真菌G 1培养液中加入染料厂污水排放口的污泥样品 ,从发生快速脱色降解染料的混合培养液中分离出 2株染料脱色细菌L_1和L_2 ,经API鉴定系统鉴定 ,确定菌株L_1为Enterobactersp .,菌株L_2为Peudomonassp .。研究比较了单一和不同组合混合的真菌G_1菌株 (Penicilliumsp .)、细菌L_1菌株 (Enterobactersp .)和L_2菌株 (Pseu domonassp .)对偶氮染料红M - 3BE(C .I .ReactiveRed 2 41)和蒽醌染料艳蓝KN -R(C .1.ReactiveBlue 19)的去除情况 ,发现G - 1真菌和 2种细菌组合的共培养体系对 5 0mg/L红M - 3BE和艳蓝KN -R处理 5h去除率达 10 0 %和 97.9% ,并且是以脱色降解作用为主 ,建立了染料脱色降解菌的最佳组合 ;进一步测定了此最佳共培养体系对另外 13种不同结构染料的脱色降解 ,结果表明 ,除对蒽醌染料R - 478脱色降解较差外 ,对其他染料均可在lh— 3d被完全脱色降解 ,表现出脱色降解染料的广谱性 ;向培养 4d的共培养体系中依次加入 8种染料 ,菌体可对染料连续脱色 ,维持脱色能力达 8d左右     

Enhanced biodegradation of azo dyes using an integrated elemental iron-activated sludge system: I. Evaluation of system performance.

The objective of this research is to evaluate an integrated system coupling zero-valent iron (Fe(0)) and aerobic biological oxidation for the treatment of azo dye wastewater. Zero-valent (elemental) iron can reduce the azo bond, cleaving dye molecules into products that are more amenable to aerobic biological treatment processes. Azo dye reduction products, including aniline and sulfanilic acid, were shown to be readily biodegradable at concentrations up to approximately 25 mg/L. Batch reduction and biodegradation data support the proposed integrated iron pretreatment and activated sludge process for the degradation of the azo dyes orange G and orange I. The integrated system was able to decolorize dye solutions and yield effluents with lower total organic carbon concentrations than control systems without iron pretreatment. The success of the bench-scale integrated system suggests that iron pretreatment may be a feasible approach to treat azo dye containing wastewaters.     

The evaluation of electrical energy per order (E(Eo)) for photooxidative decolorization of four textile dye solutions by the kinetic model

Photooxidative decolorization of four textile dyestuffs, C.I. Acid Orange 7 (AO7), C.I. Acid Orange 8 (AO8), C.I. Acid Orange 52 (AO52) and C.I. Acid Blue 74 (AB74), by UV/H2O2 was investigated in a laboratory scale photoreactor equipped with a 15 W low pressure mercury vapour lamp. The decolorization of the dyes was found to follow pseudo-first-order kinetics, and hence the figure-of-merit electrical energy per order (E(Eo)) is appropriate for estimating the electrical energy efficiency. The E(Eo) values were found to depend on the concentration of H2O2, concentration and basic structure of the dye. This study shows that these textile dyes can be treated easily and effectively with the UV/H2O2 process with E(Eo) values between 0.4 and 5 kW h m-3 order-1, depending on the initial concentrations of dyes and H2O2. The kinetic model, based on the initial rates of degradation, provided good prediction of the E(Eo) values for a variety of conditions.     

Decomposition pathways and reaction intermediate formation of the purified, hydrolyzed azo reactive dye C.I. Reactive Red 120 during ozonation

In this study, an aqueous solution of purified, hydrolyzed C.I. Reactive Red 120 (RR 120, Color Index), was selected as a model to investigate the degradation pathways and to obtain additional information on the reaction intermediate formation. The dye was purified to avoid the influence of the impurities on the ozonation process and on the formation of oxidation by-products. To simulate the dye-bath effluents from dyeing processes with azo reactive dyes, a hydrolyzed form of the dye was chosen as a representative compound. High performance liquid chromatography/mass spectrometry and its tandem mass spectrometry was chosen to identify the decomposition pathways and reaction intermediate formation during the ozonation process. In addition total organic carbon and high performance ion chromatography analysis were employed to obtain further information on the reaction processes during ozonation. Purified, hydrolyzed RR 120 was decomposed under the direct nucleophilic attack by ozone resulting in oxidation and cleavage of azo group and aromatic ring, while the triazine group still remained in the solution even after prolonged oxidation time (120 min) due to its high resistance to ozonation. Phenol, 1,2-dihydroxysulfobezene, 1-hydroxysulfonbezene were detected as the degradation intermediates, which were further oxidized by O(3) and *OH to other open-ring products and then eventually led to simple oxalic and formic acid identified by HPIC.     

Biodegradation of organic pollutants in saline wastewater by halophilic microorganisms: a review

Agro-food, petroleum, textile, and leather industries generate saline wastewater with a high content of organic pollutants such as aromatic hydrocarbons, phenols, nitroaromatics, and azo dyes. Halophilic microorganisms are of increasing interest in industrial waste treatment, due to their ability to degrade hazardous substances efficiently under high salt conditions. However, their full potential remains unexplored. The isolation and identification of halophilic and halotolerant microorganisms from geographically unrelated and geologically diverse hypersaline sites supports their application in bioremediation processes. Past investigations in this field have mainly focused on the elimination of polycyclic aromatic hydrocarbons and phenols, whereas few studies have investigated N-aromatic compounds, such as nitro-substituted compounds, amines, and azo dyes, in saline wastewater. Information regarding the growth conditions and degradation mechanisms of halophilic microorganisms is also limited. In this review, we discuss recent research on the removal of organic pollutants such as organic matter, in terms of chemical oxygen demand (COD), dyes, hydrocarbons, N-aliphatic and N-aromatic compounds, and phenols, in conditions of high salinity. In addition, some proposal pathways for the degradation of aromatic compounds are presented.     

Degradation mechanism of azo dye C. I. reactive red 2 by iron powder reduction and photooxidation in aqueous solutions

We have made a comparison of the UV-VIS spectra of three azo dyes, C. I. reactive red 2, orange II and C. I. reactive black 8, in aqueous solutions during treatment with iron powder reduction and photooxidation. From this, we propose their mechanisms for reduction photooxidation. GC/MS analyses of the degradation products of the dye C. I. reactive red 2 demonstrated some important steps producing hydrogenated azo structure, substituted benzene and substituted naphthalene.     

Biogenic sulphide plays a major role on the riboflavin-mediated decolourisation of azo dyes under sulphate-reducing conditions

The effect of high concentrations of sulphate on the reductive decolourisation of different azo dyes by anaerobic sludge was studied in batch cultures. Sludge cultures were pre-incubated under sulphate-reducing conditions prior addition of dyes. Little or no effects of sulphate (5-10 g sulphate l(-1)) on the rate of decolourisation of Reactive Orange 14 (RO14), Direct Blue 53 (DB53) and Direct Blue 71 (DB71) were observed when no external redox mediator was provided. However, an increase in sulphate concentration, in the presence of riboflavin (20 microM), enhanced the decolourisation of all dyes. The first-rate constant of decolourisation (k) was increased up to 2-, 3.6- and 2-fold for RO14, DB53 and DB71, respectively, by supplying high sulphate concentrations, compared to the controls lacking sulphate, in the presence of the redox mediator. Sulphate reduction did not take place during the course of azo reductions, but was only evident before dye addition and after complete decolourisation, suggesting azo dyes reduction out-competed sulphate reduction for the available reducing equivalents. The experimental data suggest that reduction of azo dyes by riboflavin, which had been reduced by biogenic sulphide, was the major mechanism implicated during decolourisations, which was corroborated by abiotic incubations. Riboflavin greatly accelerated the abiotic reduction of RO14, so that the k value was increased up to 44-fold compared to the control lacking riboflavin.     

Degradation of azo dyes by algae

The degradation of azo dyes by algae was evaluated and it was found that certain algae can degrade a number of azo dyes to some extent. The reduction rate appears to be related to the molecular structure of the dyes and the species of algae used. The azo reductase of algae is responsible for degrading azo dyes into aromatic amine by breaking the azo linkage. The aromatic amine is then subjected to further metabolism by algae. It is proposed in this paper that in stabilization ponds, algae can play a direct role in the degradation of azo dyes, rather than only providing oxygen for bacterial growth.     

Decolorization and biodegradability of photocatalytic treated azo dyes and wool textile wastewater

The photodegradation and biodegradability have been investigated for four non-biodegradable commercial azo dyes, Reactive YellowKD-3G, Reactive Red 15, Reactive Red 24, Cationic Blue X-GRL, an indicator. Methyl Orange, and one industrial wool textile wastewater, using TiO2 suspensions irradiated with a medium pressure mercury lamp. The color removal of dyes solution and dyeing wastewater reached to above 90% within 20-30 min. of photocatalytic treatment. Biochemical oxygen demand (BOD) was found to increase, while chemical oxygen demand (COD), total organic carbon (TOC) decreased, so that the ratio of BOD5/COD of the wastewater increased from original zero up to 0.75. The result implies that photocatalytic oxidation enhanced the biodegradability of the dye-containing wastewater and therefore relationship between decolorization and biodegradability exists. When the color disappeared completely, the wastewater biodegraded normally and could be discharged for further treatment. The experimental results demonstrate that it is possible to combine photocatalysis with conventional biological treatment for the remedy of wastewater containing generally non-biodegradable azo dyes.     

Non-enzymatic reduction of azo dyes by NADH

Nicotinamide adenine dinucleotide (NADH) reduces a variety of azo dyes by four electrons to generate the corresponding aromatic amines. This reduction is pH-dependent and increases with decreasing pH. Reduction of 4-(4'-sulfophenylazo)-phenol and 2-(4'-sulfophenylazo)-phenol, specifically substituted with methyl, methoxy, halo, and nitro groups, was examined to determine the susceptibility of azo dyes to reduction by NADH. Except for the nitro-substituted azo dyes, all other azo dyes were reduced. Possible mechanisms of reduction are proposed. The implications of our findings to microbial degradation and mammalian metabolism of azo dyes are discussed.     

New catalyst comprising Silicotungstic acid and MCM-22 for degradation of some organic dyes

A heterogeneous catalyst comprising Keggin type polyoxometalate, silicotungstic acid (SiW₁₂), and MCM-22 was synthesized using wet impregnation method and characterized by acidity measurement, BET, FT-IR, XRD, and SEM. Their catalytic activity was evaluated for the degradation of cationic organic dyes like methylene blue (MB), crystal violet (CV), and an azo dye Chryosidine Y (CY) in an aqueous solution. The experimental parameters such as catalyst amount, initial dye concentration, and contact time were studied for the degradation of dyes, and it was found that the cationic dyes like methylene blue and crystal violet show better activity as compared to azo dye Chryosidine Y. This may be attributed to better electrostatic interaction of these cationic dyes with the residual negative surface charge of the catalyst, due to presence of SiW₁₂ ion as it is rich in surface oxygens and surface hydroxyl groups. The control experimental results showed that the presence of SiW₁₂ at the surface of MCM-22 promoted the degradation reactions, and presence of multiple W–O bonds in polyoxometalate also played a key role in this reaction. The catalyst exhibits recycling ability without any significant loss in activity up to four cycles.

     

Degradation of reactive dyes I. A comparative study of ozonation, enzymatic and photochemical processes

The environmental problems associated with textile activities are represented mainly by the extensive use of organic dyes. A great number of these compounds are recalcitrant and shown carcinogenic or mutagenic character. In this work three processes were studied for degradation of an anthraquinone dye (C.I. reactive blue-19). The ozonation process leads to complete decolorization with a very short reaction time; however, effective mineralization of the dye was not observed. The enzymatic process promotes quick decolorization of the dye; nevertheless, maximum decolorization degrees of about 30% are insignificant in relation to the decolorization degree achieved by the other processes. The best results were found for the photocatalytical process. The use of ZnO or TiO2 as photocatalysts, permits total decolorization and mineralization of the dye with reaction times of about 60 min.     

NaNO(2)/FeCl(3) catalyzed wet oxidation of the azo dye Acid Orange 7

A combination of ferric chloride and sodium nitrite significantly improved the wet oxidation of the azo dye Acid Orange 7 (AO7) in acid aqueous media (pH 2.6) under moderate conditions (T=150 degrees C; oxygen pressure=0.5 MPa). To evaluate the catalytic system, wet oxidation of AO7 was carried out at temperatures between 90 and 150 degrees C and oxygen pressures ranging from 0.1 to 0.5 MPa. The effect of initial solution pH from 2.6 to 11.4 and the amount of catalyst on the degradation of AO7 were also investigated. AO7 initial concentration was kept 200 mg L(-1). The degradation process was monitored by UV-visible spectroscopy, HPLC, IC (ion chromatography), GC-MS and TOC analysis. At 150 degrees C and 0.5 MPa oxygen pressure, 56% TOC was removed after 4h of treatment, while no obvious TOC removal were achieved without catalyst at the same experimental condition. The main degradation products were some small organic acids: formic acid, acetic acid, pyruvic acid, oxalic acid, succinic acid (identified and quantified by IC) and phthalic acid (identified by GC-MS).     

Ozonation of an azo dye C.I. Remazol Black 5 and toxicological assessment of its oxidation products

The effect of ozonation (20.5 mgl(-1)) on the degradation processes of an azo dye, Remazol Black 5 (RB5; CI) was studied. Conventional parameters such as chemical oxygen demand (COD), total organic carbon (TOC), pH, conductivity, colour removal, biodegradability (BOD(5/28)), and toxic potential of the dye and its degradation products were monitored during the process. The results obtained indicated that ozonation is a highly effective way to remove the colour of a corresponding dye solution. However, a considerable organic load still remained as indicated by high COD and TOC residues. The COD, TOC reductions were about 40% and 25% for 6 h ozonation of 2 gl(-1) RB5 aqueous solution. During the ozonation process the rapid decrease of pH and the sharp increase of conductivity indicated the formation of acidic by-products and small fragments and ions which were identified by high performance ion chromatography. The BOD28 data revealed that first by-products after partial ozonation (10-150 min) of RB5 were more biodegradable than the parent compound and ozonation can enhance the biodegradability of azo dyes. During the first 150 min of total 360 min of oxidation, the formation of first by-products with high toxic potential took place as it could be confirmed by two acute toxicity-screening tests, the bioluminescence test (Vibrio fischerii) and the neutral red cytotoxicity assay (rat hepatoma cells). The significant enhancement of microbial biodegradability after long-term ozonation could also be seen as a decrease of toxic intermediates in correlation with the ozonation time as indicated in BOD28 biological degradation test results.     

Kinetics of chemical decolorization of the azo dye C.I. Reactive Orange 96 by sulfide

The mechanism of decolorization of azo dyes based on the extracellular chemical reduction with sulfide (H2S, HS-, S2-) was postulated for sulfate reducing environments. To design technical decolorization processes of textile wastewater treatment with sulfide produced by sulfate reducing bacteria (SRB), kinetics is of great significance. Batch experiments were made in order to investigate the kinetics of abiotic decolorization of the reactive mono-azo dye C.I. Reactive Orange 96 (RO 96) with sulfide, with varying pH. The decolorization of RO 96 by sulfide under the exclusion of O2 corresponded to first-order kinetics with respect to both dye and sulfide concentration. The decolorization of RO 96 with sulfide at neutral pH (7.1) was advantageous compared with that at pH for 4.1, 6.3, and 6.5. This is attributed to an increase in the fraction of HS- of total sulfide species at neutral pH. The rate constants k for the decolorization at 37 degrees C were obtained as 0.01 for pH = 4.1, 0.06 for pH = 6.3, 0.08 for pH = 6.5, and 0.09 for pH = 7.1 in mM(-1) min(-1). The high rate constants for sulfide at pH 6.5-7.1 support that the decolorization through SRB (i.e. by bio-sulfide) can be effective in anaerobic bacterial systems with sulfate.     

Degradation of azo dyes using low iron concentration of Fenton and Fenton-like system

This study investigated Fenton and Fenton-like reactions at low iron concentration (相似文献   

Decolorization of mono-azo dyes in wastewater by advanced oxidation process: A case study of acid red 1 and acid yellow 23

Advanced Oxidation Processes (AOPs) have been used as emerging wastewater treatment technologies which can effectively handle various hazardous organics in wastewater and groundwater. The photooxidation of two non-biodegradable azo dyes, acid red 1 and acid yellow 23, were studied in an UV/hydrogen peroxide photochemical reactor with a 5 kW low pressure mercury lamp. It was observed that the decomposition of both azo dyes were pseudo-first order reactions with respect to the azo dye concentrations. Simultaneously, the effects of hydrogen peroxide dosage, pH, initial concentration of the azo dyes and intensity of UV light were also studied. Moreover, the time required for the 50% removal of azo dyes and observed pseudo-first order rate constants were used as parameters to show the efficiency of azo dye treatment.