Efficient Degradation of a Biorecalcitrant Pollutant from Wastewater Using a Fluidized Catalyst-Bed Reactor

This study investigated the treatment of an azo dye, as a biorecalcitrant model, from industrial wastewater by using Cu/Mg/Al-chitosan in a fluidized catalyst-bed reactor. A number of variables were used to study the impact they had on the oxidation process involving azo dye. The maximum degradation of the azo dye was achieved at 7 g Cu/Mg/Al-chitosan. The chloride and sulfate ions had a synergistic effect on azo dye removal. The oxidation of the azo dye under the selected conditions was of pseudo-first-order. Textile wastewater could effectively be treated using a low concentration of about 7 g of Cu/Mg/Al-chitosan in a short hydraulic retention time of 10 min. The use of Cu/Mg/Al-chitosan demonstrated a promising method to eliminate the azo dye from the wastewater.     

Interaction of dis‐azo dyes with quaternized poly(dimethylaminoethyl methacrylate) as a function of the dye structure and polycation charge density

Interactions between some dis‐azo dyes, different by either the position of their sulfonic groups or their number (Ponceau SS, Crocein Scarlet MOO, Congo Red, and Direct Blue 1), and some strong polycations (PCs), with cationic centers in their side chains and dye removal from artificial wastewaters were systematically investigated in this study. PCs with variable charge densities (CDs) were prepared from poly(dimethylaminoethyl methacrylate) by controlled quaternization with benzyl chloride. Even when the main process in the dye removal was charge neutralization (coagulation) for all of the dyes, significant effects of the CD and dis‐azo dye structure on the metachromatic behavior of the dyes in dilute aqueous solutions and on the dye removal efficiency were observed. The stability of the PC/azo dye complex and, connected with this, the flocculation window were higher when the PC with the highest CD was used. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Impact of Ozonation on Decolorization and Mineralization of Azo Dyes: Biodegradability Enhancement,By-Products Formation,Required Energy and Cost

In the present study ozonation process was implemented to analyze the effect of ozonation time on the rate of chemical oxygen demand (COD) removal, mineralization and rate of decolorization of azo dyes. Three types of azo dyes i.e. Acid Red 14, Direct Red 28 and Reactive Black 5 were selected. Decolorization and mineralization of samples were conducted in batch scale. The COD and color removal efficiency were found to be increasing at a certain time of ozonation. The results with Acid Red 14, Congo Red and Reactive Black 5 dyes solutions lead to maximum COD reduction of 75%, 67% & 50% respectively. 93%, 92% and 94% color removal were achieved after 25 min of ozonation time of the same dyes which highlighted that ozonation process was found to be more efficient for reactive dye decolorization. Ozonation by-products analyzed by ion chromatography resulted that it partially mineralized with the formation of chloride, fluoride, sulphate, nitrate and oxalate ions. During ozonation process a rapid decrease in pH value indicated the acidic nature of by-products. The effect of buffered dye solutions on the ozonoation process highlighted that the decolorization efficiency decreases in comparison to unbuffered dye solutions. Ozonation led to enhancement of biodegradability ratio (BOD₅/COD) and increased electrical conductivity of the dye solutions. Optimum ozonation time required for degradation of dye solutions reflected the evaluation of energy consumption and cost of the treatment after ozonation.     

Kinetics and equilibrium studies of removal of an azo dye from aqueous solution by adsorption onto scallop

In the present work removal of an azo dye (Reactive Black 5) was investigated from aqueous solution by adsorption onto scallop as a low-cost and widely available adsorbent. The effect of various operational parameters, such as contact time, pH, initial dye concentration and adsorbent dosage on the removal efficiency of dye was studied. Removal efficiency declined with the increase in solution pH and initial dye concentration but with the decrease in adsorbent dosage. Experimental equilibrium and kinetics data were fitted by Langmuir and Freundlich isotherms and pseudo-first-order and pseudo-second-order kinetic models, respectively.     

Immobilization horseradish peroxidase on amine-functionalized glycidyl methacrylate-<Emphasis Type="Italic">g</Emphasis>-poly(ethylene terephthalate) fibers for use in azo dye decolorization

Activated fibers were used as a new support material for the immobilization of horseradish peroxidase (HRP). Poly(ethylene terephthalate) (PET) fibers were grafted with glycidyl methacrylate (GMA) using benzoyl peroxide (Bz₂O₂) as initiator. 1,6-diaminohexane (HMDA) was then covalently attached to this GMA grafted PET fibers. HMDA-GMA-g-PET fibers were activated with glutaraldehyde and HRP was successfully immobilized. Both on the free HRP and the immobilized HRP activities, pH, temperature, thermal stability, and reusability were investigated. Both free enzyme and immobilized enzyme were used in a batch process for the degradation of azo dye. About 98% of azo dye removal was observed with immobilized HRP, while 79% of azo dye removal was found with the free HRP. 45 min of the contact time is sufficient for the maximum azo dye removal. The HRP immobilized on modified PET fibers were very effective for removal of azo dye from aqueous solutions.     

厌氧光生物转盘-好氧生物膜处理偶氮染料废水

利用厌氧光生物转盘-好氧移动床膜生物反应器处理偶氮染料废水,探讨了染料浓度、光照时间、供氧条件、硫酸盐浓度4个操作条件对组合工艺处理效果的影响。实验结果表明,厌氧光生物转盘对染料废水的脱色和COD去除起主要作用,当光生物转盘连续光照时间为12h／d,废水中染料质量浓度为100mg／L,HRT为5h时,光生物转盘的脱色率达90％左右,COD去除率达70％左右。经过后续好氧移动床处理,厌氧出水中的有毒芳香化合物得到有效降解,系统总COD去除率达90％以上。     

Removal of dyes by Moringa oleifera seed extract. Study through response surface methodology

BACKGROUND: The effect of pH and initial dye concentration (IDC) on dye removal by coagulation/flocculation process with Moringa oleifera seed extract has been studied. The study was carried out by using the response surface methodology (RSM) in an orthogonal and rotatable design of experiments. Three types of dye were studied: anthraquinonic (Alizarin Violet 3R); indigoid (Indigo Carmine); and azoic (Palatine Fast Black WAN). RESULTS: The interaction level of the two variables studied is higher in the case of azo dye, while it is almost null in the case of anthraquinonic dye. Indigoid dye presents an intermediate situation. pH has a negative influence on dye removal, and by raising IDC q capacity tends to be higher. Polynomic regression of the surface plot was carried out and the adjusted r² found for each case, this being 0.99 in the case of anthraquinonic dye, 0.94 in the case of indigoid dye, and 0.74 in the case of azoic dye. CONCLUSIONS: Moringa oleifera is an interesting natural coagulation agent for use in dye removal. pH should be taken into account in the cases of indigoid and azo dyes, while its influence is rather small in the case of anthraquinonic dye. Copyright © 2009 Society of Chemical Industry     

Fe(III)/H2O2-Like System for Removal of Azo Dye from Aqueous Solution

Fe(III)/H₂O₂ system is an effective method for separating the organic compounds from aqueous solution, whereas it is often investigated under lower pH conditions. In order to improve performance of the system, a Fe(III)/H₂O₂-like system that was composed of iron-based coagulant and H₂O₂ was developed, which has the combined effect of flocculation and oxidation. The system when used for decolorization of an organic azo dye solution, Procion Red MX-5B, under wider pH range, indicated higher decolorization efficiency. Parameters affecting the decolorization such as coagulant dosage, H₂O₂ concentration, initial solution pH, temperature, and initial dye concentration were examined in this study. The results indicated that with appropriate coagulant dosage, H₂O₂ concentration, and pH, it was more effective for the decolorization, especially in a weak alkaline environment (pH = 7-8); the pseudo-first-order kinetics could express the azo dye concentration as a function of the reaction time. This study further illustrated that the azo dye solution was degraded to a degree with 53.22% TOC removal at an initial total TOC concentration of 14.92 mg/L. Overall, the established system in this study was favorable to the decolorization of soluble azo dye.     

Anodic oxidation of azo dye C.I. Acid Red 73 by the yttrium-doped Ti/SnO2-Sb electrodes

This work was conducted to study the ability of anodic oxidation of azo dye C.I. Acid Red 73 (AR73) using the yttrium-doped Ti/SnO₂-Sb electrodes. The effects of Sb doping level, yttrium doping level, thermal decomposition temperature and cycle times of dip-coating thermal decomposition on the properties of the electrodes were investigated. The results showed that the excellent electrochemical activity of Ti/SnO₂-Sb-Y electrode can be achieved at a 7∶1 molar ratio of Sn∶Sb and thermal decomposition temperature of 550°C. Moreover when the cycle times of dip-coating and thermal decomposition were up to 10 times, the performance of the electrode tends to be stable. The Ti/SnO₂-Sb electrodes doped with yttrium (0.5 mol-%) showed the most excellent electrochemical activity. In addition, the influences of operating variables, including current density, initial pH, dye concentration and support electrolyte, on the colour removal, chemical oxygen demand (COD) removal and current efficiency were also investigated. Our results confirmed that the current efficiency increased with the concentrations of dye and sodium chloride. Moreover, increasing the current density and the initial pH would reduce the current efficiency.     

偶氮染料在气-液-固循环浆态光催化反应器中的降解脱氮

偶氮染料废水是一种集中量大的重要污染物,其中的偶氮键可被环境微生物降解生成具有毒性的芳香胺类化合物。本文从光量子效率、脱氮速率、脱氮能耗等方面,对比研究了一种新设计的气-液-固循环浆态光催化反应器和环隙式光催化反应器对偶氮染料降解脱氮的性能。结果表明,由于空气的引入,使气-液-固循环浆态光催化反应器的量子收率有一定程度下降,同时造成单位数量级脱氮能耗也有一定增大,但偶氮染料脱氮速率比在环隙式反应器中的情况有大幅度提高,表明气-液-固循环浆态反应器在偶氮染料废水光催化降解脱氮方面具有较大应用前景。     

Removal of Reactive Red 198 from aqueous solution by combined method multi-walled carbon nanotubes and zero-valent iron:Equilibrium,kinetics, and thermodynamic

Dyes often include toxic,carcinogenic compounds and are harmful to humans' health.Therefore,removal of dyes from textile industry wastewater is essential.The present study aimed to evaluate the efficiency of the combination of zero valent iron(ZVI) powder and multi-walled carbon nanotubes(MWCNTs) in the removal of Reactive Red 198(RR198) dye from aqueous solution.This applied research was performed in a batch system in the laboratory scale.This study investigated the effect of various factors influencing dye removal,including contact time,p H,adsorbent dose,iron powder dose,initial dye concentration,and temperature.The equilibrium adsorption data were analyzed using three common adsorption models:Langmuir,Freundlich and Temkin.Besides,kinetic and thermodynamic parameters were used to establish the adsorption mechanism.The results showed,in pH =3,contact time = 100 min,ZVI dose = 5000 mg·L~(-1),and MWCNTs dose = 600 mg·L~(-1)in 100 mg·L~(-1)dye concentration,the adsorption efficiency increased to 99.16%.Also,adsorption kinetics was best described by the pseudo-second-order model.Equilibrium data fitted well with the Freundlich isotherm(R2= 0.99).The negative values of ΔG0and the positive value of ΔH0(91.76) indicate that the RR198 adsorption process is spontaneous and endothermic.According to the results,the combination of MWCNTs and ZVI was highly efficient in the removal of azo dyes.     

Azo dye removal from aqueous solution by organic-inorganic hybrid dodecanoic acid modified layered Mg-Al hydrotalcite

Hydrotalcite (HTC), a typical layered compound, is a promising adsorbent for removal of organic pollutants. To partition azo dye from aqueous solution, Mg-Al HTCs intercalated with dodecanoic acid (DA) modifier, DAHTCs, were prepared by ion exchange and calcination-rehydration methods. The structures of HTCs and DAHTCs were characterized by powder XRD and FT-IR techniques. The introduction of DA broadened the spacing of interlayers and provided more space for ion exchange. The effects of pH value, contact time, adsorbent amount, temperature and different intercalated modifiers on the adsorption of azo dye onto HTCs and DAHTCs were determined. The optimum pH of uptake was around 3.0 and all the lower or higher pH values proved to decrease the adsorption properties. The pseudo-second-order model was found to best describe the adsorption dynamics of all adsorbents. Meanwhile, the size and polarity of intercalated modifiers might be crucial for adsorption of azo dye.     

Multi-Objective Optimization of Indigo Carmine Removal by an Electrocoagulation/GAC Coupling Process in a Batch Reactor

A coupling process between Electrocoagulation (EC) and GAC was employed to separate dyes from aqueous solutions. The removal of an indigoid dye, namely C.I. Acid Blue 74, was tested. A novel approach for optimizing EC-based techniques is presented. In addition to maximizing removal efficiency, minimizing consumptions of energy and electrode materials were also targeted by means of multi-objective optimization in order to reduce the specific costs. A very good cost-efficiency feature of EC/GAC coupling process operated under optimal conditions to treat wastewater from dyestuff has been revealed. The independent variables considered were the current density, influent pH, contact time, granular activated carbon dose, and initial dye concentration. Simple maximization of color removal efficiency and multi-objective optimization were compared. Two different constraints were considered for each type of optimization. The determined costs outline the cheapness feature of the EC/GAC system as a potential dye wastewater treatment technology.     

Oxidase-Peroxidase sequential polymerization for removal of a dye from contaminated water by horseradish peroxidase (HRP)/glucose oxidase (GOx)/polyurethane hybrid catalyst

Horseradish peroxidase (HRP) and glucose oxidase (GOx) were co-immobilized on polyurethane, and the resulting HRP/GOx/polyurethane biocatalyst was characterized using scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDAX) mapping techniques. The prepared biocatalyst was used for removal of acid orange 7 as model azo dye. The required H₂O₂ for activation of HRP was in-situ produced using GOx to prevent deactivation of HRP in the presence of excess chemical H₂O₂. Central composite design (CCD) was applied for modeling and optimization of parameters affecting the activity of prepared biocatalyst. Under the optimum conditions, removal efficiency of the azo dye was predicted to be 87.47%, which was in good agreement with the experimental value (89.69%). In addition, the performance of the prepared biocatalyst for removal of two other dyes with different structure was investigated at the optimum conditions, and a removal efficiency of 91.56% and 95.25% was obtained for removal of methylene blue and malachite green, respectively. The results demonstrated that the resultant HRP/GOx/Polyurethane biocatalyst was able to decrease the chemical oxygen demand (COD) of a textile effluent from 740mg/L to 96mg/L, indicating that the prepared biocatalyst is an effective enzymatic system for treatment of real wastewater.     

Decolorization of azo dye Orange II by ferrate(VI)-hypochlorite liquid mixture, potassium ferrate(VI) and potassium permanganate

Ferrate(VI)-hypochlorite liquid mixture was prepared using hypochlorite, an industrial by-product, via wet oxidation method. Its oxidizing ability was investigated by decolorizing azo dye Orange II in batch experiments, and compared with potassium ferrate(VI) and potassium permanganate. Effects of the oxidant concentration, dye concentration, initial pH of dye solutions and UV 254 nm irradiation were examined. The color removal by potassium permanganate, potassium ferrate(VI) and the ferrate(VI)-hypochlorite liquid mixture at 30 min reached 17.7%, 62.0% and 95.2%, respectively. The ferrate(VI)-hypochlorite liquid mixture maintained a high decolorization efficiency over a wide pH range from 3.0 to 11.0, indicating that the initial solution pH had little impact on its oxidizing power. However, the decolorization efficiency by potassium permanganate was proved to be highly pH dependent and the lowest efficiency was observed at neutral pH. UV 254 nm irradiation did not enhance the decolorization efficiencies significantly for both the ferrate(VI)-hypochlorite liquid mixture and potassium permanganate over a wide pH range.     

响应曲面法分析零价铁对普施安蓝H-5R脱色的影响因素

该文分别从零价铁（zVI）投加量、粒径、pH值、盐浓度、摇床摇速对偶氮染料普施安蓝H-5R进行脱色速率研究,并通过响应曲面进行试验优化。结果表明在初始染料溶液浓度为200mg／L时,最适投加量为1．5g／L,脱色速率随着粒径和摇床摇速增大而升高,中性和偏酸条件下pH影响不大,高浓度盐可以增加染料的脱色。响应曲面法（RSM）结果还表明不同影响因素之间存在相互作用,从而影响染料脱色。     

Degradation of azo dye C.I. Acid Red 18 using an eco-friendly and continuous electrochemical process

Continuous anodic oxidation of azo dye C.I. Acid Red 18 by using PbO₂ electrode in aqueous solution was studied. To reach the best conditions of the process, the influence of various operating parameters such as pH, current density, hydraulic retention time (HRT) and dye concentration on the removal rate of chemical oxygen demand (COD) and color, as indexes showing the amount of efficiency, was investigated. The findings showed that, respectively, 99.9% and 80.0% of the dye and COD were removed (at optimized conditions). Mineralization current efficiency results indicated that at the beginning of the reaction mineralization occurred quickly at a low current density, whereas at high amounts the rate of mineralization the efficiency decreased. At the optimum conditions, the majority of COD was removed only with 38.2 kWh/kg COD of energy consumption in 120 min. By controlling HO?/dye concentration ratio via the parameters adjustment, particularly HRT and current density, this system can treat Acid Red 18 well even at high concentrations. Furthermore, the voltammetry study illustrated that electroactive intermediates created during the process were mineralized at current density of 8.6mA/cm².     

Lignocellulosic jute fiber as a bioadsorbent for the removal of azo dye from its aqueous solution: Batch and column studies

The feasibility of the use of jute fiber for the adsorption of azo dye from an aqueous solution was evaluated with batch and fixed‐bed column studies. The batch studies illustrated that dye uptake was highly dependent on different process variables, namely, the pH, initial dye concentration of the solution, adsorbent dosage, contact time, ionic strength, and temperature. The exothermic and spontaneous nature of adsorption was revealed from thermodynamic study. The equilibrium adsorption data were highly consistent with the Langmuir isotherm and yielded an R² value of 0.999. Kinetic studies divulged that the adsorption followed a pseudo‐second‐order model with regard to the intraparticle diffusion. In the column studies, the total amount of adsorbed dye and the adsorption capacity decreased with increasing flow rate and increased with increasing bed height and initial dye concentration. Also, the breakthrough time and exhaustion time increased with increasing bed depth but decreased with increasing flow rate and influent dye concentration. The column performances were predicted by the application of the bed‐depth service time model and Thomas model to the experimental data. The virgin and dye‐adsorbed jute fiber was characterized by Fourier transform infrared spectroscopy and scanning electron microscopy analyses. The investigation suggested that jute fiber could be applied as a promising low‐cost adsorbent for dye removal. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

超临界水氧化处理偶氮染料废水的实验研究

在间歇式反应器中进行偶氮染料C.I.活性橙7的超临界水氧化实验,探索染料分子中的偶氮基团在氧化反应中的转化规律.选取反应温度、氧化系数、初始COD质量浓度、反应时间和pH值为过程参数,总氮去除率和氨氮质量浓度为响应量,通过中心组合设计方法进行实验设计,设计了一个五因素、五水平包含22个实验点的实验矩阵.采用响应面分析法...     

A new electrode reactor with in-built recirculation mode for the enhancement of methylene blue dye removal from the aqueous solution: Comparison of adsorption,electrolysis and combined effect

The removal of basic dye such as methylene blue (MB) dye from the synthetic wastewater was experimentally investigated using an electrolytic cell (EC), adsorption and the combined effect of EC and adsorption technology called a three-phase three-dimensional electrode reactor (TPTDER). The performance of the each technology was checked on the basis of the efficiency of the systems. The experimental results are expressed in terms of the removal efficiency of the dye molecules. The results show that the TPTDER could efficiently remove the dye molecules from the aqueous solutions when compared with the EC and adsorption process. The removal efficiency reached as high as about 99% for an initial MB dye concentration in the range of 100–1,000 mg/L by TPTDER for 10 min at 12 V cell voltage and at specific airflow conditions. It was also observed that the removal of dye molecules depends upon the initial solution pH, applied cell voltage, contact time, and initial dye concentration. The recyclability of the particle electrodes in the TPTDER process was also checked. These findings suggest that TPTDER is a promising technology for the removal of dyes from the aqueous solution, and can be applied to the removal of dyes from the industrial effluents.