声光催化降解水中有机污染物

声光催化是水处理降解有机污染物的一种新技术。在分析中 ,探讨了该技术降解有机污染物的机理 ,以及国内外研究现状 ,包括降解效果和主要的影响因素     

ZnIn2S4可见光催化降解水中的双氯芬酸

通过水热法制备了可见光下响应的光催化剂ZnIn2S4,研究了水中痕量医药类物质双氯芬酸的光解和光催化降解效果与降解途径,同时对催化剂进行了扫描电镜、X射线衍射、紫外可见漫反射、氮吸附和羟基自由基捕获的测试。结果表明,ZnIn2S4的比表面积为91.3 m2·g-1,且在可见光照射下具有良好光催化性能。以卤钨灯模拟太阳光,在双氯芬酸初始浓度100 μg·L-1,ZnIn2S4投加浓度10 mg·L-1条件下反应5 h可降解水中98%的双氯芬酸。卤钨灯直接光解5 h可降解91%的双氯芬酸。光解和光催化反应均符合假一级反应动力学,光催化反应速率是光解反应速率的1.5倍。双氯芬酸光解过程中主要发生光环化反应,生成了2-（1-氯-9H-咔吧唑-8-基）-乙酸;光催化过程则主要通过羟基自由基氧化降解双氯芬酸,中间产物主要有1-氯-8-甲基-9H-咔吧唑及2,6-二氯-N-邻甲苯基苯胺。     

Heterogeneous Fenton degradation of persistent organic pollutants using natural chalcopyrite: effect of water matrix and catalytic mechanism

Environmental Science and Pollution Research - Natural chalcopyrite was evaluated as heterogeneous Fenton catalyst. Catalytic performance was evaluated considering different systems, catalyst...     

Photocatalytic degradation of contaminants of concern with composite NF-TiO2 films under visible and solar light

This study reports the synthesis and characterization of composite nitrogen and fluorine co-doped titanium dioxide (NF-TiO₂) for the removal of contaminants of concern in wastewater under visible and solar light. Monodisperse anatase TiO₂ nanoparticles of different sizes and Evonik P25 were assembled to immobilized NF-TiO₂ by direct incorporation into the sol–gel or by the layer-by-layer technique. The composite films were characterized with X-ray diffraction, high-resolution transmission electron microscopy, environmental scanning electron microscopy, and porosimetry analysis. The photocatalytic degradation of atrazine, carbamazepine, and caffeine was evaluated in a synthetic water solution and in an effluent from a hybrid biological concentrator reactor (BCR). Minor aggregation and improved distribution of monodisperse titania particles was obtained with NF-TiO₂-monodisperse (10 and 50 nm) from the layer-by-layer technique than with NF-TiO₂?+?monodisperse TiO₂ (300 nm) directly incorporated into the sol. The photocatalysts synthesized with the layer-by-layer method achieved significantly higher degradation rates in contrast with NF-TiO₂-monodisperse titania (300 nm) and slightly faster values when compared with NF-TiO₂-P25. Using NF-TiO₂ layer-by-layer with monodisperse TiO₂ (50 nm) under solar light irradiation, the respective degradation rates in synthetic water and BCR effluent were 14.6 and 9.5?×?10^?3?min^?1 for caffeine, 12.5 and 9.0?×?10^?3?min^?1 for carbamazepine, and 10.9 and 5.8?×?10^?3?min^?1 for atrazine. These results suggest that the layer-by-layer technique is a promising method for the synthesis of composite TiO₂-based films compared to the direct addition of nanoparticles into the sol.     

喷射环流三相光催化反应器可见光下降解酸性湖兰A的研究

设计了一种喷射环流三相光催化反应器。用该反应器在可见光下,对染料酸性湖兰A在不同初始浓度、催化剂浓度、pH、光照时间下光催化降解脱色率的影响进行了研究。实验结果表明,反应最佳pH为6,反应最佳时间为20min,催化剂最佳投加量为8g／L。在最优条件下,染料脱色率达90％以上。     

电化学催化降解水中有机污染物的研究进展

电化学法催化降解废水中的有机污染物已引起广泛兴趣。在电极的作用下 ,电化学反应和化学催化作用结合 ,可导致有机分子的电催化降解。选用合适的电极材料可以加速电化学反应速率 ,有助于有机物的电化学转化。本文讨论了提高电催化降解速率的方法 ,指出了在该领域的研究中存在的问题和发展方向     

模拟日光下铌酸盐/钛酸纳米片催化降解水中环丙沙星

通过一步水热法制备新型铌酸盐/钛酸纳米片(Niobate/titanate nanoflakes,Nb-TiNFs)复合材料,采用XRD、XPS、FT-IR、SEM、TEM等分析手段对其形貌和结构进行了表征,并探究其在模拟日光下对目标污染物环丙沙星(ciprofloxacin,CIP)的降解性能和内在反应机理。结果表明,Nb-TiNFs可高效、快速光催化降解水中CIP。溶液pH可通过影响静电作用以及羟基自由基的形成而影响CIP的降解,在pH为6时,光催化剂(0.1 g·L⁻¹)对水中CIP(10 mg·L⁻¹)的降解率最大,即180 min内达到96.2%;常规离子Na⁺和Fe³⁺对CIP的降解无明显影响,但Ca²⁺的存在对其产生一定抑制作用。降解过程中,超氧自由基(·O₂⁻)是主要的活性物质,材料内部形成的异质结导致带隙偏移,促进电子转移,抑制电子-空穴对的复合,从而促进了太阳光驱动的光催化活性。Nb-TiNFs合成方法简单、高效、稳定且对环境友好,在光催化去除水中新兴污染物领域具有一定的应用前景。     

外加气体对等离子体降解水相中有机污染物的影响研究

研究了等离子体在内电极通氧气、氮气、空气和氦气条件下降解甲基紫的机理。研究表明,在该等离子体发生器结构下,等离子体能降解甲基紫,且在不同气体气氛下的降解产物不同,在氧气氛围下为含—CO和—OH物质及直链烯烃,而氮气氛围下是含—N、—NH和—OH的芳香类物质及小分子烃类物质。研究同时表明,等离子体降解水相中有机物时应在氧气介质中进行,如用空气则有可能会造成水体中NO-3过高。     

光电氧化降解饮用水中有机污染物的效能

针对地表水中普遍存在的有机污染物现状和常规水处理工艺无法去除有机污染物的问题,以紫外光电氧化技术为基础,提出了以“分质供水”为目标的末端深度水处理工艺。与单独电解和光解相比,电化学氧化与紫外耦合技术可以将布洛芬、阿特拉津、三氯乙酸、乐果的降解率在15 min内分别提高到92.5%、98.1%、71.0%和94.6%,并且能耗有所降低。电流和光强对光电氧化降解有机污染物有促进作用,但污染物初始质量浓度、Cl⁻、HCO₃⁻和天然有机物(HA)和污染物去除率呈反比关系。在此基础上,以布洛芬为污染物代表,测定了布洛芬的中间产物,并计算了降解中间体的毒性变化,发现光电氧化明显降低了布洛芬的毒性。     

物理场协同作用降解有机污染物研究进展

有机污染物是环境污染物的主要类型,通过物理场外加能量的作用可实现各种有机污染物的高效降解.对微波、超声波、紫外光、电场、磁场、等离子体这几类主要物理场相互协同降解有机污染物的研究现状进行综述,重点介绍了物理场协同作用降解有机污染物的机制、效果、影响因素及污染物类型,并展望了该类研究今后的应用前景和发展趋势.     

新型过硫酸盐活化技术降解有机污染物的研究进展

在利用过硫酸盐氧化降解有机污染物过程中,以过硫酸盐活化所产生强氧化性的硫酸根自由基至为关键,综述了近来过硫酸盐的新型活化技术,其中以零价金属材料,含铁矿石,含铁复合材料,活性炭及含碳复合材料,含醌结构有机物活化为主线展开。通过介绍各种活化机理以及相应活化技术在降解有机污染物的研究,继而提高过硫酸盐降解有机污染物的潜在研究与应用价值。     

二氧化钛纳米管光催化降解水中百草枯

二氧化钛纳米管被用于光催化氧化水体中的百草枯,对光催化反应条件、常见Fe3+离子的干扰情况和百草枯光催化降解动力学规律进行了研究。结果表明,浓度为25 mg/L的百草枯溶液,在二氧化钛纳米管(TNT)1.0 g/L,H2O20.5 mL/50 mL,pH=5.0的最优光催化氧化条件下,经过30 min反应可以被100%从水体中去除,表现出非常高的光催化降解效率;动力学方程拟合表明,百草枯光催化氧化反应符合拟一级动力学规律,动力学方程为ln(C0/C)=1.0267t-0.1282,反应速率常数K为1.0267 h-1;双氧水存在时常见的Fe3+能够进一步提高百草枯光催化降解率;该光催化反应体系对低浓度百草枯废水有很好的处理效果,预示着光催化氧化技术适合地表或地下水体中百草枯的去除。     

有机污染物的光催化降解过程中的分析技术进展

本文对有机物的光催化降解动力学研究 ,降解产物的鉴定、定量检测等过程中所使用的一些分析技术和手段 ,尤其是在有机物的光降解机理研究中羟自由基的检测技术和方法进行了综述     

Photocatalytic degradation of p,p′-DDT under UV and visible light using interstitial N-doped TiO2

1,1,1-trichloro-2,2-bis(p-chlorophenyl)ethane (or p,p′-DDT) is one of the most persistent pesticides. It is resistant to breakdown in nature and cause the water contamination problem. In this work, a major objective was to demonstrate the application of N-doped TiO₂ in degradation and mineralization of the p,p′-DDT under UV and visible light in aqueous solution. The N-doped TiO₂ nanopowders were prepared by a simple modified sol–gel procedure using diethanolamine (DEA) as a nitrogen source. The catalyst characteristics were investigated using XRD, SEM, TEM, and XPS. The adsorption and photocatalytic oxidation of p,p′-DDT using the synthesized N-doped TiO₂ under UV and visible light were conducted in a batch photocatalytic experiment. The kinetics and p,p′-DDT degradation performance of the N-doped TiO₂ were evaluated. Results show that the N-doped TiO₂ can degrade p,p′-DDT effectively under both UV and visible lights. The rate constant of the p,p′-DDT degradation under UV light was only 0.0121 min^?1, whereas the rate constant of the p,p′-DDT degradation under visible light was 0.1282 min^?1. Under visible light, the 100% degradation of p,p′-DDT were obtained from N-doped TiO₂ catalyst. The reaction rate of p,p′-DDT degradation using N-doped TiO₂ under visible light was sixfold higher than that under UV light. According to Langmuir-Hinshelwood model, the adsorption equilibrium constant (K) for the N-doped TiO₂ under visible light was 0.03078 L mg^?1, and the apparent reaction rate constant (k) was 1.3941 mg L^?1-min. Major intermediates detected during the p,p′-DDT degradation were p,p′-DDE, o,p′-DDE, p,p′-DDD and p,p′-DDD. Results from this work can be applied further for the breakdown of p,p′-DDT molecule in the real contaminated water using this technology.     

氮掺杂TiO2可见光光催化剂的制备及性能

以尿素和钛酸丁酯为原料,通过溶胶-凝胶法低温下制备了高可见光催化活性的氮掺杂TiO2(NDT)光催化剂,采用XRD、TEM、BET和UV-Vis DRS等测试手段对其进行了表征,并在自制光催化反应器中降解甲基橙评价了样品的光催化活性。结果表明,当氮与钛的摩尔比为0.5∶1时,350℃焙烧的样品(NDT350)具有最佳的可见光光谱吸收和光催化活性,该催化剂为锐钛矿晶相,平均粒径为21 nm,比表面积为89.13 m2/g。可见光辐照下,NDT350降解甲基橙的表观反应速率常数为1.381×10-2min-1,是商业P25催化剂的16.85倍。NDT350优良的可见光催化活性与其大的比表面积和强烈的可见光光谱吸收有关。     

氮掺杂TiO_2可见光光催化剂的制备及性能

以尿素和钛酸丁酯为原料,通过溶胶-凝胶法低温下制备了高可见光催化活性的氮掺杂TiO2（NDT）光催化剂,采用XRD、TEM、BET和UV-Vis DRS等测试手段对其进行了表征,并在自制光催化反应器中降解甲基橙评价了样品的光催化活性。结果表明,当氮与钛的摩尔比为0.5∶1时,350℃焙烧的样品（NDT350）具有最佳的可见光光谱吸收和光催化活性,该催化剂为锐钛矿晶相,平均粒径为21 nm,比表面积为89.13 m2/g。可见光辐照下,NDT350降解甲基橙的表观反应速率常数为1.381×10-2min-1,是商业P25催化剂的16.85倍。NDT350优良的可见光催化活性与其大的比表面积和强烈的可见光光谱吸收有关。     

Altered toxicity of organic pollutants in water originated from simultaneous exposure to UV photolysis and CdSe/ZnS quantum dots

The paper reports unforeseen results of increased toxicity of water, subsequent to interactions between CdSe/ZnS quantum dots (QDs), phenol and toluene under UV irradiation. The consistent pattern of changes in measured toxicity (TU) was observed and correlated with degradation of phenol and/or toluene. Spearman rank coefficients (SRCs) for data pairs sum-parameters vs. TU were calculated. The highest correlation between toxicity and degradation by-products was observed for hydroquinone (0.86) and catechol (0.89). The presence of QDs in tested concentration range in the absence of UV has shown low toxicity and no interactions with phenol and/or toluene. The leak of constituent core and shell metal ions was observed. The minor differences in physical characteristics of tested QDs of the same chemical composition led to rather different degradation patterns of phenol and toluene, and the amount of leak of the metal ions as well.     

COP-compost: a software to study the degradation of organic pollutants in composts

Composting has been demonstrated to be effective in degrading organic pollutants (OP) whose behaviour depends on the composting conditions, the microbial populations activated and interactions with organic matters. The fate of OP during composting involves complex mechanisms and models can be helpful tools for educational and scientific purposes, as well as for industrialists who want to optimise the composting process for OP elimination. A COP-Compost model, which couples an organic carbon (OC) module and an organic pollutant (OP) module and which simulates the changes of organic matter, organic pollutants and the microbial activities during the composting process, has been proposed and calibrated for a first set of OP in a previous study. The objectives of the present work were (1) to introduce the COP-Compost model from its convenient interface to a potential panel of users, (2) to show the variety of OP that could be simulated, including the possibility of choosing between degradation through co-metabolism or specific metabolism and (3) to show the effect of the initial characteristics of organic matter quality and its microbial biomass on the simulated results of the OP dynamic. In the model, we assumed that the pollutants can be adsorbed on organic matter according to the biochemical quality of the OC and that the microorganisms can degrade the pollutants at the same time as they degrade OC (by co-metabolism). A composting experiment describing two different ¹⁴C-labelled organic pollutants, simazine and pyrene, were chosen from the literature because the four OP fractions simulated in the model were measured during the study (the mineralised, soluble, sorbed and non-extractable fractions). Except for the mineralised fraction of simazine, a good agreement was achieved between the simulated and experimental results describing the evolution of the different organic fractions. For simazine, a specific biomass had to be added. To assess the relative importance of organic matter dynamics on the organic pollutants’ behaviour, a sensitivity analysis was conducted. The sensitivity analysis demonstrated that the parameters associated with organic matter dynamics and its initial microbial biomass greatly influenced the evolution of all the OP fractions, although the initial biochemical quality of the OC did not have a significant impact on the OP evolution.