Decomposition of dimethyl phthalate in an aqueous solution by ozonation with high silica zeolites and UV radiation

This study investigates the enhanced ozonation of dimethyl phthalate (DMP), which is a pollutant of concern in water environments, with high silica zeolites and ultraviolet (UV) radiation. Semibatch ozonation experiments are performed under various reaction conditions to examine the effects of inlet gas ozone concentration, high silica zeolite dosage, and UV radiation intensity on the decomposition of DMP. The complete removal of DMP can be efficiently achieved via both O(3) and O(3)/UV treatments. Note that the presence of high silica zeolites accelerates the decomposition rate of DMP in the O(3) process. On the other hand, the removal efficiencies of both chemical oxygen demand (COD) and total organic carbons (TOC) are significantly enhanced by employing the ozonation combined with UV radiation. The O(3)/UV process is also advantageous for the utilization efficiency of fed ozone especially in the late ozonation period. Furthermore, the correlation between the COD removal percentage (%) and the mole ratio of ozone consumed to the DMP treated (mol mol(-1)) is obtained. The clear-cut removal relationship of the TOC with COD during the ozonation of DMP has also been presented. Consequently, the results evaluate the flexibility of ozonation system associated with high silica zeolites and UV radiation for the removal of DMP and provide the useful information in engineering application.     

Combined photolysis and catalytic ozonation of dimethyl phthalate in a high-gravity rotating packed bed

In this study, a high-gravity rotating packed bed (HGRPB) was used as a catalytic ozonation reactor to decompose dimethyl phthalate (DMP), an endocrine disrupting chemical commonly encountered. The HGRPB is an effective gas-liquid mixing equipment which can enhance the ozone mass transfer coefficient. Platinum-containing catalyst (Pt/-Al2O3) of Dash 220N and ultra violet (UV) lamp were combined in the high-gravity ozonation (HG-OZ) system to enhance the self-decomposition of molecular ozone in liquid to form highly reactive radical species. Different combinations of HG-OZ with Dash 220N and UV for the degradation of DMP were tested. These include HG-OZ, HG catalytic OZ (HG-Pt-OZ), HG photolysis OZ (HG-UV-OZ) and HG-UV-Pt-OZ. The result indicated that all the above four ozonation processes result in significant decomposition of DMP and mineralization of total organic carbon (TOC) at the applied ozone dosage per volume of liquid sample of 1.2gL(-1). The UV and Pt/gamma-Al2O3 combined in HG-OZ can enhance the TOC mineralization efficiency (eta(TOC)) to 56% (via HG-UV-OZ) and 57% (via HG-Pt-OZ), respectively, while only 45% with ozone only. The process of HG-UV-Pt-OZ offers the highest eta(TOC) of about 68%.     

The decolorization and mineralization of acid orange 6 azo dye in aqueous solution by advanced oxidation processes: a comparative study

The comparison of different advanced oxidation processes (AOPs), i.e. ultraviolet (UV)/TiO(2), O(3), O(3)/UV, O(3)/UV/TiO(2), Fenton and electrocoagulation (EC), is of interest to determine the best removal performance for the destruction of the target compound in an Acid Orange 6 (AO6) solution, exploring the most efficient experimental conditions as well; on the other hand, the results may provide baseline information of the combination of different AOPs in treating industrial wastewater. The following conclusions can be drawn: (1) in the effects of individual and combined ozonation and photocatalytic UV irradiation, both O(3)/UV and O(3)/UV/TiO(2) processes exhibit remarkable TOC removal capability that can achieve a 65% removal efficiency at pH 7 and O(3) dose=45mg/L; (2) the optimum pH and ratio of [H(2)O(2)]/[Fe(2+)] found for the Fenton process, are pH 4 and [H(2)O(2)]/[Fe(2+)]=6.58. The optimum [H(2)O(2)] and [Fe(2+)] under the same HF value are 58.82 and 8.93mM, respectively; (3) the optimum applied voltage found in the EC experiment is 80V, and the initial pH will affect the AO6 and TOC removal rates in that acidic conditions may be favorable for a higher removal rate; (4) the AO6 decolorization rate ranking was obtained in the order of O(3)相似文献   

Combined electrocoagulation and TiO(2) photoassisted treatment applied to wastewater effluents from pharmaceutical and cosmetic industries

The treated wastewater consists of refractory materials and high organic content of hydrolyzed peptone residues from pharmaceutical factory. The combination of electrocoagulation (EC) followed by heterogeneous photocatalysis (TiO(2)) conditions was maximized. The EC: iron cathode/anode (12.50 cmx2.50 cmx0.10 cm), current density 763Am(-2), 90min and initial pH 6.0. As EC consequence, the majority of the dissolved organic and suspended material was removed (about 91% and 86% of the turbidity and chemical oxygen demand (COD), respectively). After EC, refractory residues still remained in the effluent. The subsequent photocatalysis: UV/TiO(2)/H(2)O(2) (mercury lamps), pH 3.0, 4h irradiation, 0.25gL(-1) TiO(2) and 10mmolL(-1) H(2)O(2) shows high levels of inorganic and organic compounds eliminations. The obtained COD values: 1753mgL(-1) for the sample from the factory, 160mgL(-1) after EC and 50mgL(-1) after EC/photocatalyzed effluents pointed out that the combined treatment stresses this water purification.     

Degradation of DMSO by ozone-based advanced oxidation processes

The present study investigates the oxidation of dimethyl sulfoxide (DMSO) by conventional ozonation and the advanced oxidation processes (AOPs). The major degradation products identified were methanesulfinate, methanesulfonate, formaldehyde, and formic acid in ozonation process. The subsequent degradation of intermediates shows that methanesulfonate is more resistance to ozonation, which reduces the mineralization rate of DMSO. The effect of t-butanol addition and ozone gas flow dosage on the degradation rate was evaluated. The rate constant of the reaction of ozone (k(D)) with DMSO was found to be 0.4162 M(-1)S(-1). In the second part of this study, DMSO degradation and TOC mineralization were investigated using O(3)/UV, O(3)/H(2)O(2) and UV/H(2)O(2) processes. In all theses processes the degradation of target organics is more pronounced than TOC removal. The efficiencies of these processes were evaluated and discussed. The formation of sulfate ion in all AOPs have been identified and compared with other processes. Overall it can be concluded that ozonation and ozone-based AOPs are promising processes for an efficient removal of DMSO in wastewater.     

Photochemical mineralization of di-n-butyl phthalate with H2O2/Fe3+

This study evaluated the performance of photo-Fenton reaction initiated by the UV irradiation with H(2)O(2)/Fe(3+), denoted as UV/H(2)O(2)/Fe(3+), to decompose di-n-butyl phthalate (DBP) in the aqueous solution. The concentration of total organic carbon (TOC) was chosen as a mineralization index of the decomposition of DBP by the UV/H(2)O(2)/Fe(3+) process. A second-order kinetic model with respect to TOC was adequately adopted to represent the mineralization of DBP by the UV/H(2)O(2)/Fe(3+) process. The experimental results of this study suggested that the dosages with 4.74 x 10(-5) mol min(-1)L(-1) H(2)O(2) and initial Fe(3+) loading concentration of 4.50 x 10(-4) mol L(-1) in the solution at pH 3.0 with 120 microW cm(-2) UV (312 nm) provided the optimal operation conditions for the mineralization of DBP (5 mg L(-1)) yielding a 92.4% mineralization efficiency at 90 min reaction time.     

Synthesis and photo-degradation application of WO3/TiO2 hollow spheres

A WO(3)/TiO(2) composite, hollow-sphere photocatalyst with average diameter of 320 nm and shell thickness of 50 nm was successfully prepared using a template method. UV-vis diffuse reflectance spectra illustrated that the main absorption edges of the WO(3)/TiO(2) hollow spheres were red-shifted compared to the TiO(2) hollow spheres, indicating an extension of light absorption into the visible region of the composite photocatalyst. The WO(3) and TiO(2) phases were confirmed by X-ray diffraction analysis. BET isotherms revealed that the specific surface area and average pore diameter of the hollow spheres were 40.95 m(2)/g and 19 nm, respectively. Photocatalytic experiments indicate that 78% MB was degraded by WO(3)/TiO(2) hollow spheres under visible light within 80 min. Under the same conditions, only 24% MB can be photodegraded by TiO(2). The photocatalytic mineralization of MB, catalyzed by TiO(2) and WO(3)/TiO(2), proceeded at a significantly higher rate under UV irradiation than that under visible light, and more significant was the increase in the apparent rate constant with the WO(3)/TiO(2) composite semiconductor material which was 3.2- and 3.5-fold higher than with the TiO(2) material under both UV and visible light irradiation. The increased photocatalytic activity of the coupled nanocomposites was attributed to photoelectron/hole separation efficiency and the extension of the wavelength range of photoexcitation.     

Catalysis of advanced oxidation reactions by ultrasound: a case study with phenol

The present study is about the enhancement in ozone-mediated degradation and UV (254nm) photolysis of phenol in aqueous solutions by 300kHz acustic cavitation and the selection of operating parameters for optimum phenol removal efficiency. The method was based on monitoring of the concentration of phenol during 90min exposure to ozonation, sonication, UV photolysis, O(3)/ultrasound, UV/ultrasound and O(3)/UV/ultrasound operations. It was found that ozonation at alkaline pH was an effective method of phenol destruction, but it was considerably more effective when applied simultaneously with ultrasonic irradiation. The observed synergy particularly at alkaline pH was attributed to combined effects of: (i) increased ozone mass transfer (upon hydrodynamic shear forces created by ultrasonic bubbles) and (ii) excess hydroxyl radical formation (upon thermal decomposition of ozone in the gaseous cavity bubbles). Degradation of phenol by photolysis alone was negligible, while combination of UV-irradiation and ultrasound rendered considerable degrees of decay. The synergy here was explained by excess hydroxyl radicals that are formed by photolysis of ultrasound-generated H(2)O(2). Maximum rate of phenol degradation was observed in case of combined application of ozone, UV and ultrasound at basic pH.     

硫掺杂TiO2/Ti光电极制备及其可见光光电催化性能

为了提高TiO2/Ti光电极在可见光下的光电催化活性,采用阳极氧化法制备了一种新型的硫掺杂TiO2/Ti光电极.采用扫描电子显微镜、X射线衍射、X射线荧光光谱等技术对光电极进行了表面形貌、结晶形态、晶粒尺寸、硫的掺杂量和价态以及吸光性能表征.研究表明:硫掺杂TiO2/Ti光电极的最佳制备条件为:成膜电压160V、电流密度100mA/cm2、Na2SO3质量浓度750mg/L;所制备的光电极具有良好的光电催化氧化降解邻苯二甲酸二甲酯活性,并能有效地矿化其中间产物;与TiO2/Ti电极相比,硫的掺杂可以显著提高其在可见光下的光电催化性能.     

Microwave assisted rapid and complete degradation of atrazine using TiO(2) nanotube photocatalyst suspensions

A technology, microwave-assisted photocatalysis on TiO(2) nanotubes, which can be applied to degrade atrazine rapidly and completely, was investigated. TiO(2) nanotubes were prepared, and confirmed by XRD, TEM and ESR. Microwave-assisted photocatalytic degradation of atrazine in aqueous solution was investigated. The result indicates that atrazine is completely degraded in 5min and the mineralization efficiency is 98.5% in 20min, which is obviously more efficient than that by the traditional photocatalytic degradation methods. It may be attributed to the intense UV radiation generated by electrodeless discharge lamps under microwave irradiation, the increased number of OH, additional defect sites on TiO(2) under the irradiation of microwave and larger specific surface area of TiO(2) nanotubes which could adsorb more organic substances to degrade than TiO(2) nanoparticles. Along with the degradation of atrazine, the concentrations of Cl(-) and NO(3)(-) increase gradually. In 20min [Cl(-)] and [NO(3)(-)] are 3, 27.8mg/L, respectively, which are close to their stoichiometric values. The major intermediates of atrazine were identified by HPLC/MS and possible degradation pathways of atrazine in microwave-assisted photocatalysis on TiO(2) nanotubes were proposed.     

Degradation of 4-chlorophenol by a microwave assisted photocatalysis method

In this work, the degradation of 4-chlorophenol (4CP) under simultaneous microwave assisted UV (electrodeless discharge lamp) photocatalysis technique (MW/UV/TiO2) was investigated. Several factors affecting the degradation of 4CP by MW/UV/TiO2 method, such as the dosage of photocatalysts, the initial pH value of the solutions, gas bubbling, light intensity and addition of H2O2 oxidant, were studied in detail. The synergistic effects between microwave irradiation and TiO2 photocatalysis were also studied. The major intermediates were found to be chlorobenzene, phenol, hydroquinone, benzoquinone and 4-chlorocatechol. Based on the results, a general reaction pathway for the degradation of 4CP was proposed.     

Efficient degradation of tetrabromobisphenol A by heterostructured Ag/Bi5Nb3O15 material under the simulated sunlight irradiation

Heterostructured metallic silver-layered bismuth niobate two-component system (Ag/Bi(5)Nb(3)O(15)) was developed for the first time by a mild hydrothermal method combined with photodeposition. The Ag/Bi(5)Nb(3)O(15) exhibited single-crystalline orthorhombic structure with small particle size (50-200 nm) and octahedral as well as sheet-like shape; additionally, it possessed photoresponse in both UV and visible region. As a novel alternative photocatalysts to TiO(2), the photocatalytic activity of the Ag/Bi(5)Nb(3)O(15) was evaluated by the degradation of tetrabromobisphenol A, a member from the family of the brominated flame retardant, under solar simulating Xe lamp irradiation, and enhanced photocatalytic activity in compared to Bi(5)Nb(3)O(15) itself and Degussa P25 was obtained.     

Synthesis of a CNT-grafted TiO(2) nanocatalyst and its activity triggered by a DC voltage

Carbon nanotube (CNT)-grafted TiO(2) (CNT/TiO(2)) was synthesized as an electrically conductive catalyst that exhibits redox ability under electrical excitation besides ultraviolet (UV) irradiation. The CNT/TiO(2) material was synthesized by a two-step process. Ni nanoparticles were photodeposited onto TiO(2) first. The Ni nanoparticles then served as seeds for the growth of CNTs using the chemical vapor deposition (CVD) of C(2)H(2). The CNT/TiO(2) nanocomposite exhibits strong oxidation activity toward NO gas molecules via both photocatalysis under UV irradiation and electrocatalysis under a DC?voltage of 500?V in dark conditions.     

Titanium dioxide-mediated heterogeneous photocatalytic degradation of terbufos: parameter study and reaction pathways

The photocatalytic degradation of terbufos in aqueous suspensions was investigated by using titanium dioxide (TiO(2)) as a photocatalyst. About 99% of terbufos was degraded after UV irradiation for 90 min. Factors such as pH of the system, TiO(2) dosage, and presence of anions were found to influence the degradation rate. Photodegradation of terbufos by TiO(2)/UV exhibited pseudo-first-order reaction kinetics, and a reaction quantum yield of 0.289. The electrical energy consumption per order of magnitude for photocatalytic degradation of terbufos was calculated and showed that a moderated efficiency (E(EO)=71 kWh/(m(3)order)) was obtained in TiO(2)/UV process. To obtain a better understanding of the mechanistic details of this TiO(2)-assisted photodegradation of terbufos with UV irradiation, the intermediates of the processes were separated, identified, and characterized by the solid-phase microextraction (SPME) and gas chromatography/mass spectrometry (GC/MS) technique. The probable photodegradation pathways were proposed and discussed.     

TiO_2-Al_2O_3负载型催化剂的制备及其光催化性能

以钛酸四丁酯和氢氧化钠为反应物,采用两步水热法制备TiO2纳米线,并将其原位负载于Al2O3载体上,研究它们对甲基橙的光催化降解性能。结果表明,锐钛矿相TiO2主要呈纳米线和八面体状负载在Al2O3载体上,当TiO2负载质量分数为30%,焙烧温度为400℃,催化剂用量为1.332 0 g/L时,TiO2-Al2O3负载型催化剂光催化降解甲基橙的性能最佳,光照5 h后,甲基橙在紫外和太阳光下的降解率分别达到58.9%和55.6%。相同实验条件下,TiO2-Al2O3负载型催化剂对甲基橙的降解率比单纯TiO2提高了35.1%。     

TiO2-Al2O3复合光催化剂的制备及光催化性能

以Ti（SO4）2、Al2（SO4）3·18H2O为原料,采用乙醇助水热法制备了Al2O3-TiO2复合光催化剂,并通过改变A1／Ti物质的量之比、乙醇的体积分数、水热反应温度和反应时间等得到材料制备的最佳条件。XRD分析表明样品中的TiO2以锐钛矿晶相存在,SEM显示样品粒径范围在30-50nm之间。用最佳条件制备的复合光催化剂降解甲基橙溶液,反应30min后降解率这91％,降解过程符合一级动力学方程。     

Decolourization and mineralization of commercial reactive dyes by using homogeneous and heterogeneous Fenton and UV/Fenton processes

The oxidative decolourization and mineralization of three reactive dyes in separately prepared aqueous solutions C.I. Reactive Yellow 3 (RY3), C.I. Reactive Blue 2 (RB2) and C.I. Reactive Violet 2 (RV2) by using homogeneous and heterogeneous Fenton and UV/Fenton processes have been investigated. The effects of H(2)O(2), Fe(2+) and Fe(0) concentrations, Fe(2+)/H(2)O(2) and Fe(0)/H(2)O(2) molar ratios at pH 3 and T=23+/-1 degrees C have been studied. Optimal operational conditions for the efficient degradation of all three dye solutions (100 mg L(-1)) were found to be Fe(2+)/H(2)O(2)=0.5mM/20mM and Fe(0)/H(2)O(2)=2mM/1mM. The experimental results showed that the homogeneous Fenton process employing UV irradiation was the most effective. By using this process, the high levels of mineralization (78-84%) and decolourization (95-100%) were achieved. Pseudo-first-order degradation rate constants were obtained from the batch experimental data.     

Synthesis of Fe(2)O(3)/TiO(2) nanorod-nanotube arrays by filling TiO(2) nanotubes with Fe

Synthesis of hematite (α-Fe(2)O(3)) nanostructures on a titania (TiO(2)) nanotubular template is carried out using a pulsed electrodeposition technique. The TiO(2) nanotubes are prepared by the sonoelectrochemical anodization method and are filled with iron (Fe) by pulsed electrodeposition. The Fe/TiO(2) composite is then annealed in an O(2) atmosphere to convert it to Fe(2)O(3)/TiO(2) nanorod-nanotube arrays. The length of the Fe(2)O(3) inside the TiO(2) nanotubes can be tuned from 50 to 550?nm by changing the deposition time. The composite material is characterized by scanning electron microscopy, transmission electron microscopy and diffuse reflectance ultraviolet-visible studies to confirm the formation of one-dimensional Fe(2)O(3)/TiO(2) nanorod-nanotube arrays. The present approach can be used for designing variable one-dimensional metal oxide heterostructures.     

The combination of rotating disk photocatalytic reactor and TiO2 nanotube arrays for environmental pollutants removal

A combined photocatalytic system on one single TiO(2)-nanotube (TNT)/Ti photocatalyst, which was indeed the functional combination of photon-efficient thin-film and conventional bulk-phase photocatalysis processes, was effectively developed in rotating disk photocatalytic reactor for environmental purification applications. The TNT/Ti rotating disk, of uniform size and well-aligned, was successfully prepared by direct anodic oxidation on a dominantly large surface area of 38 cm(2), compared to the typical 1 cm(2) in available literature. To estimate the potentials of combined photocatalytic system for environmental applications, the degradation of rhodamine B was carried out under the optimized conditions, a substrate removal efficiency of nearly 90% and a mineralization efficiency of 56% were observed for initial 20 mg/L solution after 3 h treatment. Compared with the combined photocatalytic system on TiO(2) nanoparticle disk, a significant improvement in substrate removal efficiency of about 25-40% was observed on TNT/Ti disk. It was confirmed that the main degradation of rhodamine B occurred on the upper half of TNT/Ti disk above the heavily colorized sample solution, which was attributed to the superior UV utilization efficiency and the resultant high interfacial photoactivity.     

Study on photocatalytic degradation of several volatile organic compounds

The gas-phase photolytic and photocatalytic reactions of several aromatics and chlorohydrocarbons were investigated. The experimental results revealed that chlorohydrocarbons like trichloroethylene, dichloromethane and chloroform could be degraded through either photolysis or photocatalysis under irradiation of germicidal lamp, and the elimination rate of chlorohydrocarbons through photolysis was quicker than that through photocatalysis. UV light from a germicidal lamp could directly lead to degradation of toluene but could hardly act on benzene. The photodegradation rate for these volatile organic compounds (VOCs) through photolysis followed an order: trichloroethylene>chloroform>dichloromethane>toluene>benzene>carbon tetrachloride, and through photocatalysis followed: trichloroethylene>chloroform>toluene>dichloromethane>benzene>carbon tetrachloride. Besides, a series of modified TiO2 photocatalysts were prepared by depositing noble metal, doping with transition metal ion, recombining with metal oxides and modifying with super strong acid. Activity of these catalysts was examined upon photocatalytic degradation of benzene as a typical compound that was hard to be degraded. It indicated that these modification methods could promote the activity of TiO2 catalyst to different extent. The apparent zero-order reaction rate constant for degrading benzene over SnO2/TiO2 catalyst had the highest value, which was nearly three times as that over P25 TiO2. But it simultaneously had the lowest rate for mineralizing the objective compound. In spite that Fe3+/TiO2 catalyst behaved slightly less active than SnO2/TiO2 for degradation of benzene, the mineralization rate over Fe3+/TiO2 was the highest one among the prepared catalysts.