ZnO薄膜光电催化降解乙酰甲胺磷

采用溶胶-凝胶法制备了ZnO薄膜,并通过光电流响应、EIS、SEM、XRD等分析方法对其光电化学性能、表面形貌和结构进行表征.以制备的ZnO薄膜为工作电极对乙酰甲胺磷进行光电催化降解.实验表明,ZnO薄膜电极在UV照射下能够有效地光电催化降解乙酰甲胺磷,加入适量H2O2后具有一定的协同作用.在H2O2浓度为9.908 mmol.L-1,外加电压为1.2 V,支持电解液Na2SO4浓度为0.01 mol.L-1,溶液pH值为5.4的条件下,对0.1 mmol.L-1的乙酰甲胺磷180 min的降解率可达到89.6%.     

Photocatalytic degradation of methyl orange using ZnO/TiO2 composites

ZnO/TiO₂ composites were synthesized by using the solvothermal method and ultrasonic precipitation followed by heat treatment in order to investigate their photocatalytic degradation of methyl orange (MO) in aqueous suspension under UV irradiation. The composition and surface structure of the catalyst were characterized by X-ray diffraction (XRD), field emission scanning electron microscope (FE-SEM), and transmission electron microscopy (TEM). The degradation efficiencies of MO at various pH values were obtained. The highest degradation efficiencies were obtained before 30 min and after 60 min at pH 11.0 and pH 2.0, respectively. A sample analysis was conducted using liquid chromatography coupled with electrospray ionization ion-trap mass spectrometry. Six intermediates were found during the photocatalytic degradation process of quinonoid MO. The degradation pathway of quinonoid MO was also proposed.     

Ce掺杂TiO2固相光催化降解塑料薄膜

采用溶胶凝胶法合成了纯TiO2和掺杂Ce原子比例(Ce/Ti)为1.2%的TiO2粉末(Ce1.2%-TiO2)光催化剂,分别制备了纯聚乙烯薄膜、添加纯TiO2和Ce1.2%-TiO2粉末的复合聚乙烯薄膜,并于紫外、可见光照下进行了薄膜光催化降解实验;采用X射线衍射、紫外-可见漫反射分析表征了光催化剂的晶体结构及紫外可见光吸收性能;通过激光扫描共焦显微镜和傅立叶红外光谱对薄膜光催化降解过程进行测试.实验结果表明,添加光催化剂可有效降解聚乙烯薄膜,其中Ce掺杂TiO2的活性明显优于纯TiO2;在紫外光照下的降解效果优于在可见光照下的降解效果,且随着光催化剂投加量的增大,光催化效果越来越好,当添加量为5.0 %(质量分数)的Ce1.2%-TiO2时复合薄膜经紫外光照300 h后,光催化降解失重率达到33%(质量分数).     

纳米TiO2光催化降解有机磷农药的研究

通过实验,探讨了用纳米TiO2光催化处理有机磷农药模拟废水和实际应用的有机磷农药的可行性.实验表明,以测定不同时间PO43-的浓度来衡量有机磷的降解率,并以此来衡量有机磷农药及其中间产物降解的程度是合理的.光催化降解甲胺磷和水胺硫磷的结果,显示了有机磷农药的降解率与其结构有关.实际应用的有机磷农药也可用光催化降解.     

Photocatalytic degradation of methyl orange using ZnO/TiO composites

ZnO/TiO₂ composites were synthesized by using the solvothermal method and ultrasonic precipitation followed by heat treatment in order to investigate their photocatalytic degradation of methyl orange (MO) in aqueous suspension under UV irradiation. The composition and surface structure of the catalyst were characterized by X-ray diffraction (XRD), field emission scanning electron microscope (FE-SEM), and transmission electron microscopy (TEM). The degradation efficiencies of MO at various pH values were obtained. The highest degradation efficiencies were obtained before 30min and after 60min at pH 11.0 and pH 2.0, respectively. A sample analysis was conducted using liquid chromatography coupled with electrospray ionization ion-trap mass spectrometry. Six intermediates were found during the photocatalytic degradation process of quinonoid MO. The degradation pathway of quinonoid MO was also proposed.     

TiO2 photocatalyzed degradation of diazinon in an aqueous medium

The photocatalytic degradation of diazinon was studied over TiO₂ catalysts. The kinetics obtained demonstrated that powder titania (t_1/2 = 9.7 min) was more efficient compared to pure titania thin film catalysts (t_1/2 = 29.4 min). Mineralization of organic carbon to CO₂ after 360 min of irradiation was found to be 75% while heteroatoms (P, S, N) were mineralized into phosphate, sulfate and nitrate ions, respectively. A microtox test was performed to evaluate the toxicity of solutions treated by catalysts. Illumination of diazinon in the presence of TiO₂ gave rise to several intermediates that have been identified by means of solid phase extraction and gas chromatography-mass spectrometry, while a simple degradation pathway is proposed.     

Preparation and characterization of a new TiO2/SiO2 composite catalyst for photocatalytic degradation of indigo carmin

The TiO₂/SiO₂ composite was prepared by means of the SiO₂-particle-entrapment method. The FTIR data showed the presence of Si–O–Ti stretching vibration band at 970 cm⁻¹ in the TiO₂/SiO₂ composite, suggesting a reaction between TiO₂ and silica on the TiO₂ particle surface during the silicagel formation around the TiO₂ particles. The photocatalytic efficiency of TiO₂ immobilized in silicagel was compared with that of the conventional TiO₂ Degussa P25 catalyst. For this purpose, the degradation of indigo carmin (IC) dye was used as model molecule in the tests. The effect of operational parameters such as catalyst loading and dye concentration on the photocatalytic degradation of the model dye was investigated. The rate of degradation increased with increasing catalyst loading, and when the concentration of the dye decreases.     

二氧化钛/石墨烯复合光催化剂的制备及其对水中双酚A的降解

双酚A污染问题日益严峻,已经威胁到人类的健康.半导体光催化技术可以有效去除水体中双酚A污染.近年来,二氧化钛/石墨烯复合材料,因其优越的光催化性能受到广泛关注.尤其石墨烯等新型纳米碳基材料,有较大的比表面积和丰富的官能团,为二氧化钛的负载创造了良好的条件,其表面可以形成化学键,为双酚A的吸附降解提供了更多的活性位点.本文重点介绍了国内外二氧化钛/石墨烯复合材料的制备方法及各种制备方法的优缺点;讨论了二氧化钛/石墨烯复合材料对双酚A的降解效果及其降解机理;分析了二氧化钛/石墨烯复合材料的再生性能.最后总结这种材料在实际应用中存在的问题及其前景展望.     

Photocatalytic degradation of phenol in water using TiO2 and ZnO

Photocatalytic degradation of chemical pollutants in water was investigated using semiconductor oxide catalysts, zinc oxide (ZnO) and titanium dioxide (TiO2) and phenol as the substrate. Influence of various parameters such as characteristics of the catalyst, irradiation time, substrate and catalyst concentrations, pH etc. has been studied and optimum conditions for the complete degradation of phenol in water have been identified. In terms of activity and durability TiO2 is far superior to ZnO. Mixing ZnO with TiO2 does not affect its activity significantly. The process is especially relevant in view of its potential for the treatment of wastewater containing pollutants, using solar radiation as the energy source.     

Structural effect on photocatalytic degradation of metallised azo dyes in aqueous TiO2 suspension

Three metallised azo dyes were investigated under TiO₂‐photocatalytic and photosensitised conditions in aqueous buffering solutions. The degradation follows apparent first‐order kinetics. The size and strength of intramolecular conjugation determine the light‐fastness of the investigated dyes. Compared with ¹O₂ produced in photosensitised process, the more powerful *OH radicals in TiCO₂ photocatalytic process are highly reactive towards the investigated azo dyes. And as a result, the TiO₂‐photocatalysis makes little less distinction in the degradation kinetic data of the azo dyes compared with the photosensitised degradation of them.     

MoO3/TiO2纳米管的制备及其光催化降解多环芳烃的机制

本研究将热分解法制备的MoO_3与水热法制备的TiO_2纳米管复合,得到具有高太阳光催化活性的MoO_3/TiO_2纳米管异质结催化剂.研究中以芘为模型多环芳烃(polycyclic aromatic hydrocarbons,PAHs),探究了MoO_3/TiO_2纳米管模拟在太阳光下催化降解PAHs的效果及效率提升的机制.结果表明,MoO_3和TiO_2纳米管间形成的p-n异质结结构,降低了材料的能带间隙而获得更高的可见光利用效率,并有效促进了电子和空穴的分离,从而提高了复合材料的光催化活性.1%MoO_3/TiO_2纳米管催化降解芘速率(k)较MoO_3和TiO_2(锐钛矿)分别提升了5.3倍和1.5倍.催化体系中产生的·OH和光生空穴在芘的降解中起主要作用.     

可见光响应PANI/TiO_2和PoPD/TiO_2纳米材料的氧化机制及协同-光敏化作用

利用原位氧化聚合法制备pdyaniline(PANI)/TiO_2和poly-o-phenylenediamine(PoPD)/TiO_2纳米材料,通过XRD、元素分析、UV-Vis DRS和循环伏安曲线等方式进行表征,以亚甲基蓝为模拟污染物,考察p H值以及导电聚合物/TiO_2浓度对光催化效果的影响,通过捕捉实验判定不同活性物种在光催化过程中的贡献.结果表明,PANI和Po PD没有改变TiO_2的粒径和物相,PANI/TiO_2、Po PD/TiO_2和TiO_2的禁带宽度分别为2.82 e V、2.89 e V和3.09 e V;溶液p H值越高,导电聚合物/TiO_2纳米材料的光催化活性越高;PANI/TiO_2和Po PD/TiO_2纳米材料浓度在光催化降解过程中存在的最佳值分别为1 g·L-1和1.5 g·L-1,PANI/TiO_2和Po PD/TiO_2纳米材料光催化过程中活性氧物种的贡献顺序分别为·OHh+·O-2,·OH≈h+·O-2.重复利用实验结果表明制备的PANI/TiO_2和Po PD/TiO_2纳米材料具有良好的光催化稳定性.导电聚合物和TiO_2之间的协同-光敏化作用是CPs/TiO_2纳米材料光催化活性得到提高的主要原因.     

Bisphenol A endocrine disruptor complete degradation using TiO2 photocatalysis with ozone

Bisphenol A is an endocrine disruptor. Complete mineralization of bisphenol A is therefore a primary environmental issue. Here, the combination of ozonation and photocatalysis by TiO₂ is proposed for the degradation and final mineralization of bisphenol A. TiO₂ films deposited onto two sides of an Al lamina show good stability and high surface roughness. We used a specific experimental setup employing two facing ultraviolet lamps and TiO₂ layers, together with an ozone flux. High-performance liquid chromatography–mass spectrometry determinations on bisphenol A solutions sampled at different reaction times and Fourier Transform Infrared analyses of the oxide at the end of the reaction were performed to study the reaction intermediates and the overall degradation mechanism. Our results show that pollutant mineralization achieved with the combined method is far higher, of 55% in the case of 0.3 mM bisphenol A, than those obtained by individual treatments such as photolysis (<3%), ozonation (6%), photocatalysis (6%), and by other combined processes: photolytic ozonation (13%) and catalytic ozonation (15%). This finding is explained by the occurrence of highly synergistic effects.     

Effect of molecular properties on the photocatalytic degradation rates of dichlorophenols and dichloroanilines in aqueous TiO2 suspensions

The kinetics of the photocatalytic degradation of 10 different dichlorophenols and dichloroanilines have been investigated experimentally and theoretically. With the intention of finding certain molecular indices in order to determine the degradation rates of aromatic pollutants, geometry optimizations of the compounds have been performed with the semiempirical PM3 method. The molecular orbital calculations have been carried out by an SCF method using the RHF formalism. The correlations between the apparent first-order rate constants and the calculated molecular properties of the compounds have been examined. Four different structure–activity relationships have been developed expressing the logarithms of the rate constants in terms of the Hammett constants, electron densities of the substituents, the coefficients and the energies of the highest occupied molecular orbitals HOMO, and 1-octanol/water partition coefficients log?K _OW.     

Photocatalytic degradation of indole in UV/TiO2: optimization and modelling using the response surface methodology (RSM)

The aim of our research is to apply experimental design methodology to the optimization of photocatalytic degradation of indole present in wastewater. Heterogeneous photocatalysis for the oxidation of organic biorecalcitrant pollutants in water is an environmental promising method. We used the response surface methodology (RSM) for the modelization and optimization of the photodegradation of indole in the presence of titanium dioxide. The effect of indole concentration, UV intensity and stirring speed on the yield of indole degradation was determined. According to the mathematic optimization of the process, the optimum point when 100% of degradation is achieved is given by the following values: UV intensity = 250 W/m², stirring speed = 536.36 tr/min and initial indole concentration = 10.10 mg/l.     

三维电极体系中苯酚降解效率的影响因素研究

三维电极法用于处理含酚废水的影响因素研究报道较多,但并未充分在理论上阐述其影响方式及机理。采用自制的实验室小试电化学反应器对含酚自配废水进行了处理。试验结果表明:体系中苯酚降解遵循一级反应模式;通过电流效率的核算确定60min作为最佳反应时间,得到的苯酚去除率为64.3%,吨水处理能耗为14.29kW·h·t-1,实际电流效率与理论电流效率相等为0.68。对体系进水控制不同的苯酚起始质量浓度,当反应时间不变时,实际试验结果与法拉第定律一致,即电流密度与去除的污染物的量以及COD去除率与电量和进水质量浓度的比值均呈线性关系;体系中羟基自由基的产生量能够采用式[?OH]=0.1218×EC0进行计算。采用最佳反应时间t=60min、电流密度I=20A,在苯酚质量浓度为500mg·L-1时改变极板间距进行的试验结果表明电压随极板间距的增大而降低,最佳极板间距为0.21m时可获得最大去除率为78.5%,体系的启动电压为0.25V。     

The effects of different methods of catalyst preparation on the hydro-electric plasma TiO2-catalyzed degradation of 2,4-dinitrophenol

Hydro-electric plasma technology in the presence of TiO₂ catalyst used to treat 2,4-dinitrophenol (2,4-DNP) simulated wastewater is reported. The catalytic activity of TiO₂ prepared by ammonia precipitation was greater than the activity of the TiO₂ prepared by NaOH precipitation. The presence of chloride ions during the preparation process of TiO₂ had a large negative effect on the catalytic activity. The catalytic activity of TiO₂ calcined at 673 K was significantly higher than the activity of the TiO₂ that was calcined at higher and lower temperatures. After being calcined at 673 K, TiO₂ was mainly in the anatase phase and degraded 81% of the 2,4-DNP after 10 min of treatment.     

TiO2/浮石光催化降解水中邻苯二甲酸二甲酯

采用溶胶.凝胶法制备,TiO2/浮石催化剂,光催化氧化水中内分泌干扰物邻苯二甲酸二甲酯(DMP).考察催化剂用量、pH值对降解率的影响;同时分析降解动力学和有机物矿化程度.结果表明,催化剂最佳投放量为40 g·L-1,最佳pH为6.5.在最佳条件下,DMP初始质量浓度20.0 mg·L-1,5 h DMP降解率达90%以上.降解速率符合准一级动力学方程,动力学方程为:Ln(p0/p)=0.470t-0.050,速率常数=0.470h-1.考察降解过程水样的矿化程度,前4 h矿化率没有明显变化,4 h后矿化率逐渐加快,7 h矿化率达到70%.TiO2/浮石具有成本低、易回收利用、能充分与被降解物接触等优势,用于治理水体中DMP具有一定的实际可行性.     

U1WH2O2／TiO2催化氧化法对油田采出水中多环芳烃的处理效果

针对油田采出水中含有多环芳烃种类多且较难去除的特点,选取了菲和芴两种代表性多环芳烃作为研究对象,采用UV／H2O2／TiO2技术对油田采出水中多环芳烃的处理效果进行了研究;考察了在254nm波长紫外光照射下,TiO2投加量、H2O2投加量、pH值和光照时间对水样中的菲和芴处理效果的影响．实验结果显示,处理初始浓度为1000μg·L-1的菲、芴时,TiO2用量为2．2g·L-1、H2O2用量为0．12mmol·L-1、pH值为7、光照时间1．5h时,去除效果较好．     

Fe掺杂PTFE-PbO2/TiO2-NTs/Ti电极的制备、表征及电催化性能

采用电沉积法制备了Fe掺杂PTFE-PbO2/TiO2-NTs/Ti、PbO2/TiO2-NTs/Ti、PbO2/Ti 3种电极,运用扫描电镜、X射线衍射仪观察表面形貌与形态,通过线性扫描伏安法在0.1 mol·L-1的H2SO4中测定电极的析氧极化曲线.以对硝基酚(p-NP)为目标污染物,考察了电极的电催化活性,在20 mA.cm-2电流密度下降解100 mg·L-1 p-NP,120 min时表观速率常数分别为0.0370 min-1、0.0265 min-1和0.0180 min-1,COD去除率分别为77.38%、74.07%、66.18%,研究发现在相同的条件下Fe掺杂PTFE-PbO2/TiO2-NTs/Ti性能更佳,矿化更完全.