二茂铁催化光助非均相类Fenton氧化法处理含罗丹明B废水

采用二茂铁(Fc)替代UV/Fenton体系中的催化剂Fe2+,构建了一个新的UV/H2O2/Fc非均相Fenton反应体系,研究了该反应体系对含罗丹明B模拟废水的脱色性能.结果表明,Fc对水中UV/Fenton反应具有良好的催化活性,对罗丹明B起氧化作用的主要物质是·OH和其他活性物质.对水中罗丹明B的氧化脱色反应的催化性稳定,对Fc重复回收利用3次后对模拟废水仍有99%以上的脱色率;UV/H2O2/Fc体系处理罗丹明B的最佳工艺条件是H2O2的浓度为1.5′10-2mol/L,Fc的投加量为0.13g/L,初始pH值在2~6之间.证实了Fc作为光助非均相Fenton体系催化剂的可能性.     

氯氧铁非均相催化过氧化氢降解罗丹明B

传统芬顿(Fenton)法因反应pH值低、产生大量铁泥等限制其规模化应用.采用化学气相转变法制备氯氧铁(FeOCl)纳米片,选择罗丹明B为模型污染物,研究FeOCl作为类芬顿催化剂催化过氧化氢(H_2O_2)降解罗丹明B性能.通过扫描电镜(FE-SEM)和X射线衍射光谱(XRD)等表征结果显示,FeOCl晶型结构完整、呈现纳米片状,可充分暴露催化活性位点.罗丹明B降解实验结果表明,H_2O_2投量为1. 67 mmol·L~(-1)时,投加200 mg·L~(-1)FeOCl,可使得罗丹明B去除率由15. 5%提高至100%(15 min). FeOCl的催化性能随pH升高而降低,初始pH为3、5和7时,反应15 min后罗丹明B去除率分别为100%、100%和84. 0%,初始pH提升至9,去除率则显著降低至57. 6%.与传统Fenton法比较,FeOCl催化H_2O_2的pH值范围明显拓展,在弱酸性和中性条件下表现出优良的催化性能.自由基淬灭实验表明,FeOCl/H_2O_2体系催化降解罗丹明B起主要作用的是羟基自由基(·OH).电子自旋共振波谱仪测定(EPR)结果表明,单独H_2O_2体系未检测出明显的自由基信号,而投加FeOCl使得·OH信号显著增强,·OH是降解罗丹明B的主要氧化活性物种.     

微米α-Fe_2O_3非均相电Fenton降解罗丹明B

以考察非均相电Fenton法处理罗丹明B(RhB)的影响因素为目的,采用水热法制备α-Fe_2O_3微米颗粒,钛涂钌铱(Ti/RuO_2-IrO_2)电极为阳极和阴极,组成非均相电Fenton体系降解RhB废水,探讨了微米α-Fe_2O_3投加质量浓度、pH和电流密度对RhB降解效果的影响,以及催化剂的循环使用效果。结果表明:当微米α-Fe_2O_3投加质量浓度为0.5 g/L,pH为3.0,电流密度为12 mA/cm~2时,反应60 min后,非均相电Fenton体系对RhB的去除率可达97.42%,且催化剂循环使用3次后,仍可以保持95%以上的去除率,具有较好的稳定性。     

Ni/GF复合材料的制备及电Fenton降解罗丹明B的研究

采用浸渍浓缩法将二价镍盐负载到石墨毡(GF)上,再在N2氛围下700~℃焙烧得到Ni/GF复合材料,运用XRD、TG、XPS和SEM等测试方法对电极材料的结构、组成和形貌等进行分析。在双室电解池中,将制备的Ni/GF复合材料作为阴极,石墨棒为阳极,50mmol/L的Na_2SO_4为电解质,-2 V电压下对罗丹明B实施电Fenton降解。结果表明:所得Ni/GF复合材料中Ni的负载量为32%;电Fenton降解反应1 h后,罗丹明B的脱色率达到99%以上;Ni/GF复合材料经过8次循环使用后,罗丹明B脱色率仍维持在97%以上,表明复合材料有良好的EF催化稳定性。     

磁性Fen+@GO非均相Fenton催化氧化亚甲基蓝

采用化学共沉淀法制备了磁性Feⁿ⁺@GO（MFGO）纳米复合材料,并将其用于非均相Fenton催化氧化亚甲基蓝（MB）.扫描电镜、透射电镜和光电子能谱分析表明,催化活性粒子（Feⁿ⁺/铁氧化物）成功负载在GO表面.实验研究了pH值、H₂O₂初始浓度、催化剂投加量等因素对MB降解效果的影响.结果表明,H₂O₂、MFGO和H₂O₂+MFGO体系在反应120min后,MB降解率分别达到7.83%、25.58%和99.19%;在优化条件为H₂O₂浓度0.79mol/L、MFGO用量0.75g/L、pH值8时,MB降解率可达99.90%;在pH值为3~11范围内,MB降解率均在99%以上;MFGO经过6次重复使用后对MB的降解率仍可达到95.08%,是一种pH值响应宽、可磁分离回收的新型非均相催化剂.     

非均相Fenton反应的研究进展

Fenton试剂氧化法在实际应用中会产生大量含铁污泥,导致二次污染,且对p H值要求严格。而非均相Fenton反应能克服上述不足,使反应在较宽p H值范围内进行,且有利于催化剂的回收利用。文章总结了常见的非均相Fenton反应催化剂载体,包括有机载体、无机载体、铁氧化物和其它金属载体等,并展望非均相Fenton反应的发展趋势。     

光电芬顿氧化反应降解染料罗丹明B

以有机染料罗丹明B为目标污染物,利用光电芬顿方法对其进行降解研究。研究汇总考察了芬顿试剂（二价铁盐、双氧水）的用量及比例、初始pH值、电流强度等对罗丹明B降解效果的影响。实验结果表明：芬顿试剂H₂O₂?/?Fe²⁺的最佳物质的量比为1∶1,Fe²⁺浓度降低或H₂O₂浓度升高,罗丹明B降解效果增强;罗丹明B在pH＝3.0的酸性体系中降解效果最好;电流强度为0.005 A时,罗丹明B降解效果好且耗能最低。在H₂O₂?/?Fe²⁺物质的量比为1∶1、电流为0.005 A、初始pH＝3.0、H₂O₂初始浓度为1.0 mM条件下,以350 nm紫外光照射的光电芬顿反应降解初始浓度为0.1 mM的罗丹明B溶液,处理10 min后罗丹明B去除效率可达99%以上。     

非均相Fenton技术降解有机污染物的研究进展

Fenton技术在处理难降解有机物的研究中被广泛应用,较之于传统均相Fenton体系,非均相Fenton体系具有适应pH值宽、催化剂易分离回收、不易产生铁污泥等优点,已成为近年来Fenton技术领域的研究热点。文章简述了Fenton技术的发展历程,重点评述了非均相Fenton技术的研究进展。     

钒酸铁类Fenton催化剂的制备及性能研究

在不同酸碱条件下,采用水热法制备了FeVO4催化剂,利用XRD、TEM、FTIR对产物表征,并将其作为非均相类Fenton催化剂氧化降解有机染料罗丹明B,研究了初始反应溶液pH值、类Fenton试剂中各组分的浓度、钒酸铁催化剂的制备条件等因素对类Fenton反应效率的影响.结果表明,制备的钒酸铁为FeVO4﹒1.25H2O,在优化条件下降解罗丹明B时60min内脱色率可达97%以上.与传统Fenton试剂相比,类Fenton催化剂具有更广泛的pH适用范围,易于与水分离,应用前景广阔.     

微米SiC/石墨烯复合物光催化降解罗丹明B

为发展低耗和环境友好的有机物降解技术,采用光催化还原制备微米级碳化硅(SiC)/石墨烯复合材料,XRD、FTIR、Raman光谱、XPS和SEM等手段表征其物相组成和形貌结构,并以罗丹明B(RhB)为模拟污染物,研究了复合材料在可见光照射下的光催化活性和稳定性;通过活性物种捕获实验初步探讨了RhB的光催化降解机制.结果表明,SiC与石墨烯复合延长了光生电子和光生空穴的寿命,提高了材料的光催化活性与稳定性.当SiC/石墨烯配比为1∶0. 8时,光照60 min时RhB的降解率可以达到92. 7%,降解过程符合一级反应动力学方程.光催化降解RhB过程中,主要活性物种的贡献依次为:光生空穴(h⁺)>超氧阴离子自由基(·O₂^-)>光生电子(e^-)>羟基自由基(·OH).     

MnO2/EGM电极制备及电化学降解罗丹明B的研究

为开发高效的电化学阴极材料,提高溶解氧还原为H₂O₂的产率,利用电沉积法制备出了二氧化锰/膨胀石墨复合基(MnO₂/EGM)电极,并用于罗丹明B(RHB)电化学阴极降解过程的研究.实验以纯石墨电极片为阳极,MnO₂/EGM复合材料为阴极,分别考察了溶液初始pH值、电流密度、电解质浓度、RHB初始浓度和反应温度对RHB脱色效果的影响.结果表明:利用电沉积法在EGM电极表面均匀负载了MnO₂涂层;在二维电极体系中,当初始pH值为2,电流密度为40 mA·cm^-2,电解质浓度为0.15 mol·L^-1,罗丹明B初始浓度为8 mg·L^-1,反应体系温度为25℃时,RHB在电解30 min后达到最大脱色率为94.43%,且其降解过程符合一级反应动力学.运用循环伏安法(CV)研究了复合电极表面的电化学行为,以及在最佳降解条件下对H₂O₂浓度进行跟踪分析,并对降解机理进行了初步推测,...     

Synthesis of porous iron hydroxy phosphate from phosphate residue and its application as a Fenton-like catalyst for dye degradation

Phosphate residue is a kind of hazardous solid waste and if not properly disposed of, could cause serious environmental contaminations. The abundant iron salt available in phosphate residue can be used to prepare photo-Fenton catalytic reagent for wastewater treatment. In this study, the phosphate residue was effectively purified by a hydrothermal recrystallization method, reaching an iron phosphate purity of 94.2%. The particles of iron phosphate were further processed with ball milling with th...     

Synthesis of nitrogen-doped carbon nanotubes-FePO4 composite from phosphate residue and its application as effective Fenton-like catalyst for dye degradation

Phosphate residue is regarded as a hazardous waste, which could potentially create significant environmental and health problems if it is not properly treated and disposed of. In this study, nitrogen-doped carbon nanotubes-FePO_4(NCNTs-FePO_4) composite was successfully synthesized from phosphate residue, and its application as an effective catalyst was explored. Firstly, an effective method was developed to recover FePO_4 from phosphate residue, achieving an impressive FePO_4 mass recovery rate of 98.14%. Then, the NCNTsFePO_4 catalyst was synthesized from the recovered FePO_4 by two main reactions, including surface modification and chemical vapor deposition. Finally, the synthesized NCNTs-FePO_4 was applied to photo-degrade 15 mg/L Rhodamine B(RhB) in a Fenton-like system. The results showed that 98.9% of RhB could be degraded in 60 min, closely following the pseudofirst-order kinetics model. It was found that even after six consecutive cycles, NCNTs-FePO_4 still retained a high catalytic capacity(50%). Moreover, ·OH radicals participating in the RhB degradation process were evidenced using quenching experiments and electron paramagnetic resonance analysis, and a rational mechanism was proposed. It was demonstrated that the materials synthesized from hazardous phosphate residue can be used as an effective catalyst for dye removal.     

生物合成施氏矿物作为类芬顿反应催化剂降解甲基橙的研究

应用生物合成施氏矿物作为光助类芬顿反应催化剂促进甲基橙的降解.施氏矿物通过A.f-LX5细胞悬浮液在初始p H值2.5和28℃时氧化Fe SO43d生成,并进行X射线衍射和扫描电子显微镜表征.本研究分析了不同初始p H、H2O2浓度及催化剂装载量对在光助类芬顿反应中甲基橙氧化降解效率的影响.结果表明,生物合成施氏矿物具有较高的催化活性,并且通过羟基自由基机制使甲基橙降解.在近中性、较高Cl-、SO2-4及NO-3浓度条件下,施氏矿物仍然能保持较高催化甲基橙降解的效率.本研究验证了以生物合成施氏矿物作为催化剂的异相光助类芬顿反应是一种处理含甲基橙废水有应用前景的高级氧化技术.     

Efficient degradation of Rhodamine B by magnetically recoverable Fe3O4-modified ternary CoFeCu-layered double hydroxides via activating peroxymonosulfate

Environment-friendly nano-catalysts capable of activating peroxymonosulfate (PMS) have received increasing attention recently. Nevertheless, traditional nano-catalysts are generally well dispersed and difficult to be separated from reaction system, so it is particularly important to develop nano-catalysts with both good catalytic activity and excellent recycling efficiency. In this work, magnetically recoverable Fe₃O₄-modified ternary CoFeCu-layered double hydroxides (Fe₃O₄/CoFeCu-LDHs) was prepared by a simple co-precipitation method and initially applied to activate PMS for the degradation of Rhodamine B (RhB). X-ray diffraction (XRD), fourier transform infrared spectrometer (FT-IR), scanning electron microscope (SEM), transmission electron microscopy (TEM), Brunauer-Emmett-Teller method (BET), and vibrating sample magnetometer (VSM) were applied to characterize morphology, structure, specific surface area and magnetism. In addition, the effects of several key parameters were evaluated. The Fe₃O₄/CoFeCu-LDHs exhibited high catalytic activity, and RhB degradation efficiency could reach 100% within 20 min by adding 0.2 g/L of catalyst and 1 mmol/L of PMS into 50 mg/L of RhB solution under a wide pH condition (3.0-7.0). Notably, the Fe₃O₄/CoFeCu-LDHs showed good super-paramagnetism and excellent stability, which could be effectively and quickly recovered under magnetic condition, and the degradation efficiency after ten cycles could still maintain 98.95%. Both radicals quenching tests and electron spin resonance (ESR) identified both HO? and SO₄^?? were involved and SO₄^?? played a dominant role on the RhB degradation. Finally, the chemical states of the sample's surface elements were measured by X-ray photoelectron spectroscopy (XPS), and the possible activation mechanism in Fe₃O₄/CoFeCu-LDHs/PMS system was proposed according to comprehensive analysis.     

蒽醌类物质经多相类芬顿预处理前后对活性污泥特性的影响

以活性艳蓝与大黄酸为蒽醌类目标污染物,分析了其经多相类芬顿预处理前后的可生化性及对活性污泥胞外聚合物、胞内物质、脱氢酶活性、脲酶活性、微生物群落的影响.Zahn-Wellens试验表明,活性艳蓝与大黄酸不能被活性污泥有效降解,而经过多相类芬顿预处理后,其呼吸曲线均在内源呼吸线以上,去除率分别达到了84.44%和86.72%.加入蒽醌类污染物后,活性污泥胞外聚合物的三维荧光光谱中,酪氨酸蛋白的吸收峰强度降低,胞内物质的红外光谱中氨基峰变宽;而经多相类芬顿预处理后,对活性污泥特性的影响不明显.加入活性艳蓝与大黄酸后,活性污泥脲酶相对活性仍保持在80%以上,但脱氢酶活性出现了降低,特别是加入大黄酸后,相对活性仅为67.5%左右.同时活性污泥的微生物群落发生了变化,Gram Positive分别由原来的40.15%增大到了47.72%和45.78%,而Gram Negative分别由原来的39.57%减少到37%和37.15%.但加入预处理后的蒽醌类污染物,未对活性污泥的微生物群落造成明显影响.     

均相/异相催化剂光降解垃圾渗滤液效果的研究

垃圾渗滤液是一种复杂有毒的、生化降解性差的高浓度有机废水,高级氧化技术具有氧化能力强和无二次污染等特点,被认为是处理难降解有机污染物最有应用前景的方法.本研究在500 W汞灯、25℃、2.5 h反应条件下,对比了TiO_2、K2S2O_8、K2S2O_8/Fe2+、施氏矿物、施氏矿物/H2O_2、Fe2+/H2O_26种催化剂组合光化学处理垃圾渗滤液的效果.结果表明,施氏矿物/H2O_2和Fe2+/H2O_2光催化降解垃圾渗滤液中有机污染物的效果优于其它催化剂组合,渗滤液中CO_D去除率分别为41.6%和46.5%,TO_C去除率分别为76.0%和78.1%.然而,Fe2+/H2O_2组合在光催化处理垃圾渗滤液后会产生大量难以沉降的Fe(O_H)3絮状物,且渗滤液色度明显增加,由初始的40倍上升到175倍.而施氏矿物/H2O_2组合则避免了上述问题,色度去除率达100%,被认为是一种具有应用前景的光化学降解垃圾渗滤液的催化剂组合.