MnFe2O4磁性纳米棒非均相Fenton催化降解水中四环素的研究

采用水热合成法成功制备出MnFe₂O₄磁性纳米棒（s-MnFe₂O₄）,并考察了商品化的Fe₃O₄、MnFe₂O₄和合成的s-MnFe₂O₄纳米棒这3种磁性纳米颗粒作为非均相Fenton催化剂降解水中四环素抗生素的性能.同时,采用X射线衍射（XRD）、透射电镜（TEM）、N₂吸附-脱附、振动样品磁强计（VSM）及X射线光电子能谱（XPS）等技术对催化剂的理化性质进行了表征.非均相Fenton催化降解四环素的结果表明,s-MnFe₂O₄具有最高的催化活性,反应180 min,四环素的去除率可以达到87.6%,TOC的去除率达到47.5%.自由基捕获试验证实了羟基自由基（·OH）是非均相Fenton氧化过程中的主要活性物种.s-MnFe₂O₄磁性纳米棒的高催化活性归因于其表面拥有较高含量的Mn³⁺和Fe²⁺物种,它们的存在能加速界面电子的转移效率,从而促进·OH的生成.合成的s-MnFe₂O₄催化剂具有良好的稳定性,循环使用6次,四环素的去除率仅从87.6%降低到80.2%,且氧化过程中活性组分的流失很少.     

Effect of substituents in hydroxyl radical-mediated degradation of azo pyridone dyes: Theoretical approaches on the reaction mechanism

Understanding the degradation behavior of azo dyes in photocatalytic wastewater treatment is of fundamental and practical importance for their application in textile-processing and other coloration industries. In this study, quantum chemistry, as density functional theory, was used to elucidate different degradation pathways of azo pyridone dyes in a hydroxyl radical (HO^?)-initiated photocatalytic system. A series of substituted azo pyridone dyes were synthesized by changing the substituent group in the para position of the benzene moiety, ranging from strong electron-donating to strong electron-withdrawing groups. The effect of dye molecular structure on the photocatalytic degradation reaction mechanism was analyzed and quantification of substituent effects on the thermodynamic and kinetics parameters was performed. Potential energy surface analysis revealed the most susceptible reaction site for the HO^? attack. The calculated reaction barriers are found to be strongly affected by the nature of substituent group with a good correlation using Hammett σ_p constants and experimentally determined reaction rates. The stability of pre-reaction complexes and transition state complexes were analyzed applying the distortion-interaction model. The increased stability of the transition state complexes with the distancing from the substituent group has been established.     

低温等离子体协同催化降解废气污染物的研究进展

阐述了低温等离子体协同催化工艺流程与反应机理,探讨了反应温度、废气进口组分、废气中水蒸气含量、气体流速、气溶胶等因素对降解效果的影响。分析认为:一段式低温等离子体协同催化可改变低温等离子体特征及催化剂催化特性,但尚未解决尾气臭氧逃逸、副产物产生及放电稳定性等问题;两段式低温等离子体协同催化可提高污染物分子降解效率并减少尾气臭氧逃逸,但未能有效利用等离子体的能量,气体中的水蒸气、粉尘及反应过程中产生的气溶胶均能影响后置催化剂的催化性能;两段式低温等离子体协同催化已具备工程应用条件,还需配套高效预处理单元以降低废气中水蒸气、粉尘等对催化剂的影响。     

2-chlorophenol oxidation kinetic by photo-ssisted Fenton process

IntroductionTheo chlorophenolisaverytoxicandpoorlybiodegradablepollutant,whichisusedasanintermediateinthemanufactureofhigherchlorophenolandphenolresinsandforextractingsulphurandnitrogencompoundsfromcoals.Itisalsousedinorganicsynthesis(dyesandpesticide) .Oxidationofo chlorophenolwastewaterincatalyticwetairoxidationisofpracticalinterestsinceawastewatercontainingo chlorophenolover 2 0 0ppmmaynotbetreatedeffectivelybydirectbiologicalmethods.Advancedoxidationprocesses(AOPs)havebeensuccessfullyuse…     

Synergistic effect of F and triggered oxygen vacancies over F-TiO2 on enhancing NO ozonation

Oxidation-absorption technology is a key step for NO_x removal from low-temperature gas. Under the condition of low O₃ concentration (O₃/NO molar ratio = 0.6), F-TiO₂ (F-TiO₂), which is cheap and environmentally friendly, has been prepared as ozonation catalysts for NO oxidation. Catalytic activity tests performed at 120°C showed that the NO oxidation efficiency of F-TiO₂ samples was higher than that of TiO₂ (about 43.7%), and the NO oxidation efficiency of F-TiO₂-0.15 was the highest, which was 65.3%. Combined with physicochemical characteristics of catalysts and the analysis of active species, it was found that there was a synergistic effect between F sites and oxygen vacancies on F-TiO₂, which could accelerate the transformation of monomolecular O₃ into multi-molecule singlet oxygen (¹O₂), thus promoting the selective oxidation of NO to NO₂. The oxidation reaction of NO on F-TiO₂-0.15 follows the Eley-Rideal mechanism, that is, gaseous NO reacts with adsorbed O₃ and finally form NO₂.     

有机物分子结构与光催化氧化反应活性的关系

从正辛醇－水分配系数与Ｈａｍｍｅｔｔ常数，光催化氧化过程中的光解作用，表面活性剂的微环境效应及取代基的诱导效应等方面，探讨了有机物分子结构与其光催化氧化反应性之间的关系。     

超声波/Fenton联用对对硝基苯酚的处理

采用超声/Fenton联用技术对水中对硝基苯酚(P-NP)进行处理,探讨了单纯超声(US)、Fenton试剂法、US/Fenton试剂法联用对P-NP的处理效果和影响因素,结果表明,对于浓度为10mg/L的P-NP, 当pH=3、H2O2与Fe2 投加量之比为10:1、H2O2投加量为40mg/L时降解效果最好,通过动力学分析发现US/Fenton试剂法对P-NP的降解具有明显的协同效应.     

高浓度甲基橙溶液的低压湿式催化氧化处理

以高浓度甲基橙溶液模拟偶氮染料废水,采用低压湿式催化氧化法(LPWCO)进行处理,考察了H2O2投量、温度、FeSO4投量、硫酸浓度、甲基橙浓度等因素对甲基橙脱色率的影响。结果表明,LPWCO法能有效地使高浓度(大于400mg/L)甲基橙溶液脱色,脱色率大于95%,而H2O2投量不到Fenton法的5%。     

粉煤灰综合利用—制无烟型煤

粉煤灰,又称“烟道灰”,是从燃烧装置的烟道气中收集而得到的细灰.目前,国内外对粉煤灰的综合利用极为重视,但大部分都着眼于建材、建筑和农业等方面,而本发明是将粉煤灰作为型煤的掺合料配制型煤,即将粉煤灰与烟煤、褐煤和泥炭混配,再加入适量的添加剂,混匀后经压力成型制成各种形状的无烟燃料.实践证明,只要灰质、煤质和掺比相匹配,可压制成合格的掺灰型煤,达到“煤掺灰,灰代煤、效益高”的效果.该掺灰型煤,具有反应活性高,燃烧效果好,基本无烟等特点,投资少,见效快,效益高,节约能源等.经试烧证明,燃烧排烟中的各种污染物可消减50%以上,节约煤炭约30%以上,并且,每吨掺灰型煤(按售价每吨100元计算)可增收15—20元.     

Decomplexation of Cu-1-hydroxyethylidene-1,1-diphosphonic acid by a three-dimensional electrolysis system with activated biochar as particle electrodes

The feasibility of decomplexation removal of typical contaminants in electroplating wastewater, complexed Cu(II) with 1-hydroxyethylidene-1,1-diphosphonic acid (Cu-HEDP), was first performed by a three-dimensional electric reactor with activated biochar as particle electrodes. For the case of 50 mg/L Cu-HEDP, Cu(II) removal (90.7%) and PO initial pH 7, acid-treated almond shell biochar (AASB) addition 20 g/L, and reaction time 180 min, with second-order rate constants of 1.10 × 10⁻³ and 1.94 × 10⁻⁵ min⁻¹respectively. The growing chelating effect between Cu(II) and HEDP and the comprehensive actions of adsorptive accumulation, direct and indirect oxidation given by particle electrodes accounted for the enhanced removal of Cu-HEDP, even though the mineralization of HEDP was mainly dependent on anode oxidation. The performance attenuation of AASB particle electrodes was ascribed to the excessive consumption of oxygen-containing functionalities during the reaction, especially acidic carboxylic groups and quinones on particle electrodes, which decreased from 446.74 to 291.48 µmol/g, and 377.55 to 247.71 µmol/g, respectively. Based on the determination of adsorption behavior and indirect electrochemical oxidation mediated by in situ electrogenerated H₂O₂ and reactive oxygen species (e.g., •OH), a possible removal mechanism of Cu-HEDP by three-dimensional electrolysis was further proposed.