Fe3O4/ZrO2-H2O2非均相类Fenton体系对3,4-二氯三氟甲苯的降解

以浸渍法制备的新型纳米Fe3O4/ZrO2为催化剂,3,4-二氯三氟甲苯(3,4-DCBTE)为目标污染物,用Fe3O4/ZrO2-H2O2非均相类Fenton体系对目标污染物进行降解,考察催化剂的催化效果和温度、pH、H2O2投加量和掺杂比等因素对催化剂催化效果的影响。结果表明,以纳米Fe3O4/ZrO2作为催化剂的非均相类Fenton体系对3,4-二氯三氟甲苯的处理效果极佳;随着温度的升高,纳米Fe3O4/ZrO2的催化效果不断提高;当pH降低时,催化剂的催化效果有明显提升,原始pH(pH=5.7)时反应去除效果最佳,去除率可达88.6%;催化剂用量的增加同样可以提高3,4-二氯三氟甲苯的降解效率;催化剂中Fe3O4:ZrO2的物质的量比为1:2时效果较其他掺杂比的催化剂效果更好,去除率最终可以达到96.82%;当H2O2投加量增加时,3,4-二氯三氟甲苯的降解效率先提高后降低,投加量为0.3 mL时去除效果最好,几乎可以完全去除目标有机物。以Fe3O4/ZrO2-H2O2非均相类Fenton体系处理3,4-二氯三氟甲苯时,目标污染物的降解符合一级反应动力学。     

Heterogeneous Fenton degradation of bisphenol A catalyzed by efficient adsorptive Fe3O4/GO nanocomposites

A new method for the degradation of bisphenol A (BPA) in aqueous solution was developed. The oxidative degradation characteristics of BPA in a heterogeneous Fenton reaction catalyzed by Fe₃O₄/graphite oxide (GO) were studied. Transmission electron microscopic images showed that the Fe₃O₄ nanoparticles were evenly distributed and were ～6 nm in diameter. Experimental results suggested that BPA conversion was affected by several factors, such as the loading amount of Fe₃O₄/GO, pH, and initial H₂O₂ concentration. In the system with 1.0 g L^?1 of Fe₃O₄/GO and 20 mmol L^?1 of H₂O₂, almost 90 % of BPA (20 mg L^?1) was degraded within 6 h at pH 6.0. Based on the degradation products identified by GC–MS, the degradation pathways of BPA were proposed. In addition, the reused catalyst Fe₃O₄/GO still retained its catalytic activity after three cycles, indicating that Fe₃O₄/GO had good stability and reusability. These results demonstrated that the heterogeneous Fenton reaction catalyzed by Fe₃O₄/GO is a promising advanced oxidation technology for the treatment of wastewater containing BPA.     

Nanoscale zero-valent iron/AC as heterogeneous Fenton catalysts in three-dimensional electrode system

In the present work, nanoscale zero-valent iron/activated carbon (NZVI/AC) was investigated as heterogeneous Fenton catalyst in three-dimensional (3D) electrode system for methyl orange (MO) degradation. Some important operating parameters such as cathodic potential, pH, and O₂ flow rate were investigated, exhibiting good decolorization. The mineralization of MO was significantly improved by 20–35 % compared to two-dimensional (2D) AC system at the optimum conditions. Although the TOC removal of AC was higher than NZVI/AC due to its good adsorption capacity initially, heterogeneous Fenton catalysis played a more and more important roles in the following test. After eight runs, NZVI/AC still exhibited excellent catalytic properties with low iron leaching. Further, a relatively comprehensive mechanism of NZVI/AC as particle electrodes in 3D system was proposed.     

Inhibition of BPA degradation by serum as a hydroxyl radical scavenger and an Fe trapping agent in Fenton process

Identification of reactive oxygen species (ROS) that contribute to bisphenol-A (BPA) degradation and monitoring of BPA at various concentrations in human serum under Fenton reaction conditions were carried out using electron spin resonance (ESR) spectrophotometry and high performance liquid chromatography with electrochemical detection (HPLC-ECD). BPA recovery decreased with increasing Fe concentration and time, both with a Fenton reaction using Fe(II), and with a Fenton-like reaction using Fe(III). In these reactions, BPA dose-dependently decreased the intensity of 5,5-dimethyl-1-pyrroline-N-oxide (DMPO)-*OH, up to 1 microg/ml BPA, and no change in DMPO-O(2)(?-) intensity was observed. The decrease in BPA recovery was inhibited strongly by addition of serum under Fenton-like reaction conditions, and there was a negative correlation between turbidity and BPA recovery. To clarify the mechanism by which serum inhibits BPA degradation, the relationship between BPA recovery and sample turbidity, and characteristics of the precipitates were investigated using spectrophotometry and X-ray analysis. The precipitate formed in the serum-containing sample consisted of C, S, O, P and Fe. BPA degradation was also inhibited under Fenton-like reaction conditions in phosphate buffered saline (PBS), and a precipitate consisting of O, P, and Fe appeared. Precipitates also appeared in authentic albumin and gamma-globulin when sulfate was added with Fenton reagents. After precipitate removal, both Fe and protein concentrations in the supernatant of the protein solutions with sulfate decreased with increasing Fe addition. We demonstrate here that hydroxyl radical generation from Fenton or Fenton-like reactions can degrade BPA, and that serum strongly inhibits BPA degradation, not only by competing with BPA for hydroxyl radicals, but also by trapping Fe with oxidative components present in the serum.     

Fe0/Fe3O4复合材料同时去除水中多种重金属的效果

零价铁(Fe0)具有中等还原性,可通过还原反应或通过铁腐蚀产物的吸附和共沉淀过程去除水中重金属.但由于铁表面易钝化,导致铁腐蚀反应难以持续,这是限制Fe0应用的关键.因此,本研究通过原位制备零价铁复合体系(Fe0/Fe3O4),并采用批处理和连续流的流化床反应器考察了该复合体系同时去除水中Zn2+、Ni2+和Cr(Ⅵ)...     

Controllable synthesis Fe3O4@POHABA core-shell nanostructure as high-performance recyclable bifunctional magnetic antimicrobial agent

We demonstrated a method to form magnetic antimicrobial POHABA (poly-N,N′-[(4,5-dihydroxy-1,2-phenylene)bis(methylene)]bisacrylamide)-based core-shell nanostructure by free-radical polymerization of OHABA on the Fe₃O₄ core surface. The magnetic antimicrobial agent Fe₃O₄@POHABA can be used in domestic water treatment against bacterial pathogens. The thickness of POHABA shell could be controlled from 10.4 ± 1.2 to 56.3 ± 11.7 nm by the dosage of OHABA. The results of antimicrobial-activity test indicated that POHABA-based core-shell nanostructure had broad-spectrum inhibitory against Gram-negative, Gram-positive bacteria and fungi. The minimum inhibitory concentration (MIC) values of Fe₃O₄@POHABA nanostructure against Escherichia coli and Bacillus subtilis were both 0.4 mg/mL. Fe₃O₄@POHABA nanostructures responded to a permanent magnet and were easily recycled. Fe₃O₄@POHABA nanoparticles retained 100% antimicrobial efficiency for both Gram-negative and Gram-positive bacteria throughout eight recycle procedures.

     

Synthesis and characterization of magnetic Fe3O4@CaSiO3 composites and evaluation of their adsorption characteristics for heavy metal ions

A two-component material (Fe₃O₄@CaSiO₃) with an Fe₃O₄ magnetite core and layered porous CaSiO₃ shell from calcium nitrate and sodium silicate was synthesized by precipitation. The structure, morphology, magnetic properties, and composition of the Fe₃O₄@CaSiO₃ composite were characterized in detail, and its adsorption performance, adsorption kinetics, and recyclability for Cu²⁺, Ni²⁺, and Cr³⁺ adsorption were studied. The Fe₃O₄@CaSiO₃ composite has a 2D core–layer architecture with a cotton-like morphology, specific surface area of 41.56 m²/g, pore size of 16 nm, and pore volume of 0.25 cm³/g. The measured magnetization saturation values of the magnetic composite were 57.1 emu/g. Data of the adsorption of Cu²⁺, Ni²⁺, and Cr³⁺ by Fe₃O₄@CaSiO₃ fitted the Redlich–Peterson and pseudo-second-order models well, and all adsorption processes reached equilibrium within 150 min. The maximum adsorption capacities of Fe₃O₄@CaSiO₃ toward Cu²⁺, Ni²⁺, and Cr³⁺ were 427.10, 391.59, and 371.39 mg/g at an initial concentration of 225 mg/L and a temperature of 293 K according to the fitted curve with the Redlich–Peterson model, respectively. All adsorption were spontaneous endothermic processes featuring an entropy increase, including physisorption, chemisorption, and ion exchange; among these process, chemisorption was the primary mechanism. Fe₃O₄@CaSiO₃ exhibited excellent adsorption, regeneration, and magnetic separation performance, thereby demonstrating its potential applicability to removing heavy metal ions.

     

Potential application of highly reactive Fe(0)/Fe3O4 composites for the reduction of Cr(VI) environmental contaminants

We describe the use of highly reactive Fe(0)/Fe3O4 composites for the reduction of Cr(VI) species in aqueous medium. The composites were prepared by simple mechanical alloying of metallic iron and magnetite in different proportions, i.e. Fe(0) 25, 50, 75 and 90wt%. While after 3h of reaction pure Fe(0) and pure Fe3O4 showed only a low reduction efficiency of 15% and 25% Cr(VI) conversion, respectively, the composites, in particular Fe(0)(25wt%)/Fe3O4, showed a remarkable activity with ca. 65% Cr(VI) conversion. Kinetic experiments showed a high reaction rate during the first 3h, which subsequently decreased strongly, probably due to a pH increase from 6 to 8. Experiments with composites based on Fe(0)/alpha-Fe2O3, Fe(0)/gamma-Fe2O3 and Fe(0)/FeOOH showed very low activities, suggesting that Fe(oct)2+ in the magnetite structure plays an important role in the reaction. Scanning and high resolution electron microscopies and M?ssbauer spectra (transmission and conversion electron M?ssbauer spectroscopy) indicated that the mechanical alloying process promotes a strong interaction and interface between the metallic and oxide phases, with the Fe(0) particles completely covered by Fe3O4 particles. The high efficiency of the composite Fe(0)/Fe3O4 for Cr(VI) reduction is discussed in terms of a special mechanism where an electron is transferred from Fe(0) to magnetite to reduce Fe(oct)3+ to Fe(oct)2+, which is active for Cr(VI) reduction.     

Removal of emerging pollutants in aqueous phase by heterogeneous Fenton and photo-Fenton with Fe2O3-TiO2-clay heterostructures

Environmental Science and Pollution Research - Fe2O3-TiO2-clay heterostructures have been prepared using an organo-bentonite as support, which organophilic character favored the fixation of TiO2....     

Study on the degradation mechanism of 2-amino-4-acetaminoanisole from wastewater by nano-Fe3O4-catalyzed Fenton system

Environmental Science and Pollution Research - 2-Amino-4-acetaminoanisole (AMA) is an intermediate product in the synthesis of many commercial dyes, and its wide application has led to the...     

Copper-promoted heterogeneous Fenton-like oxidation of Rhodamine B over Fe3O4 magnetic nanocatalysts at mild conditions

Environmental Science and Pollution Research - Rhodamine B (RhB) is used in various industries and its effluent must be effectively treated because of its harmful and carcinogenic nature. In this...     

Cerium-modified iron oxides applied as catalysts in the heterogeneous Fenton system for degradation of cephalexin

Environmental Science and Pollution Research - The effect of incorporation of different amounts of cerium on iron oxides and different heat treatment temperatures was evaluated for the degradation...     

The catalytic incineration of styrene over an Mn2O3/Fe2O3 catalyst

In this study, styrene monomer (SM) was treated by a commercial catalyst, Mn2O3/Fe2O3, in a fixed-bed reactor. The study can be classified into two major parts. First, the effects of operating factors, such as temperature, SM concentration, space velocity, and O2 concentration, on the performance of the catalyst were investigated. Second, two catalyst life tests were carried out to characterize the deactivation effect of SM. The results show that the catalyst results in higher conversion of SM at a higher inlet temperature and higher O2 concentrations. The conversion of SM decreases with increasing SM concentration and space velocity. From the statistical analysis of the data, we find that temperature is the most important factor on the catalytic incineration. Oxygen concentration, SM concentration, and space velocity are significant parameters as well. This paper also provides information on the deactivation effect of SM. The catalysts were characterized by surface and pore-size analysis, X-ray diffraction (XRD), scanning electron microscopy (SEM), and electron spectroscopy for chemical analysis (ESCA) before and after the tests. The results show that the catalytic deactivation may be caused by carbon coating, and the pore size and surface area of the catalyst are smaller after deactivation.     

基于响应曲面法优化H2O2/Fe3+脱除烧结烟气中的Hg0

烧结烟气中重金属汞的含量较高,湿法氧化脱除零价汞（Hg0）是当前最受关注的技术之一,但该氧化脱除技术的操作条件仍需优化。为此,以响应曲面法对H2O2/Fe3+氧化脱除Hg0进行了研究和优化。首先参照单因素实验结果,利用Box-Behnken设计（BBD）的3因素3水平实验研究了溶液温度、H2O2浓度和Fe3+浓度3个条件的交互作用并进行分析和优化,发现以H2O2/Fe3+氧化脱除Hg0的最佳条件为溶液温度41.78 °C、H2O2浓度0.55 mol·L-1和Fe3+浓度0.007 mol·L-1,在此最佳条件下Hg0的脱除效率可高达87.28%。最后,在该条件下进行了验证研究,实验结果表明最优条件下Hg0的脱除效率为87.93%±0.87%,与模型预测值基本吻合,表明基于响应曲面分析法所得出的最佳工艺参数准确可靠,对利用H2O2/Fe3+脱除钢铁行业烧结烟气中Hg0的条件优化具有较好的指导作用。     

H2O2/Fe0、H2O2/Fe2+、H2O2/Fe3+3种体系处理印染废水

采用H2O2/Fe0、H2O2/Fe2+、H2O2/Fe3+3种体系分别对印染废水进行处理,研究pH 值、H2O2投加量、不同价态铁元素的投加量及反应时间对印染废水的COD和色度处理效果的影响。实验最佳的处理条件:H2O2/Fe0体系在pH 为3.0,Fe0投加量为3.0 mmol/L,H2O2投加量为9.0 mL/L,反应时间为40 min时,COD去除率达到95.99%,色度去除率达到100%;H2O2/Fe3+体系在pH 为3.0,Fe3+投加量为5.0 mmol/L,H2O2投加量为12.5 mL/L,反应时间为100 min时,COD去除率达到95.89%,色度去除率达到100%;H2O2/Fe2+体系在pH 为3.0,Fe2+投加量为6.0 mmol/L,H2O2投加量为12.0 mL/L,反应时间为100 min时,COD去除率达到95.85%,色度去除率达到100%。对比分析3种体系在各因素下的处理结果,H2O2/Fe0体系和H2O2/Fe3+体系都要优于H2O2/Fe2+体系,其中H2O2/Fe0体系的处理效果最好。     

Fe3O4纳米磁性微粒对全氟辛烷磺酸盐的吸附

采用共沉淀法合成Fe3O4纳米磁性颗粒,用透射电子显微镜（TEM）、X射线衍射仪（XRD）以及振动样品磁强计（VSM）对Fe3O4纳米磁性颗粒的粒径、形貌和磁性进行表征并研究Fe3O4纳米磁性微粒对全氟辛磺酸盐的吸附。结果表明：在PFOS初始浓度4 mg/L,pH为3,反应时间24 h,Fe3O4纳米磁性微粒投加量1.25 g/L,对全氟辛磺酸盐去除率达到90%。Fe3O4纳米磁性微粒对PFOS的吸附符合Freundlich吸附方程。     

Fe3O4/石墨烯-H2O2预处理对污泥脱水性能的影响及其作用机理

采用共沉淀法制备四氧化三铁/石墨烯（Fe3O4/GE）材料,并对其进行表征,将其与H2O2组成非均相类Fenton体系用来预处理污泥,发现此类Fenton体系能显著降低污泥比阻（SRF）,并深入分析其作用机理。研究了pH、反应时间、反应温度以及Fe3O4/GE-H2O2投加量对污泥胞外聚合物（EPS）破解的影响。结果表明,适宜反应条件为：pH 4.0,反应时间为90 min,反应温度为50 ℃,Fe3O4/GE投加量为1 g·L-1,H2O2与Fe3O4/GE投加量之比控制在8~12之间。在该条件下,污泥上清液中的SCOD、多聚糖和蛋白质浓度分别由56.47、11.48和8.21 mg·L-1增加到498.31、406.72和286.29 mg·L-1。Fe3O4/GE-H2O2非均相类Fenton体系在有效破解EPS的同时,对于污泥的脱水性能也有明显的改善作用,促进了污泥的后续处理。     

Fe3O4／Ag磁性纳米颗粒去除水中的铅离子

采用水相共沉淀法制备小尺寸磁性Fe3O4纳米颗粒,以没食子酸作为还原剂和表面修饰剂,还原Ag[（NH3）2]’制备出Fe3O4／Ag磁性纳米颗粒。研究该磁性纳米颗粒对水溶液中铅离子的吸附行为,研究结果表明,pH为7．0,吸附温度30℃时可得到最好的处理效果,铅的去除率可达99．7％以上,Fe3O4／Ag颗粒吸附行为符合二级动力学模型（R2〉0．99）。该磁性纳米颗粒经过多次再生处理后,仍具有很好的吸附效果,表明Fe3O4／Ag在水处理方面拥有良好的应用前景。     

非均相Fenton体系中无机助剂对亚甲基蓝脱色的影响

直接使用有机过渡金属化合物二茂铁作为催化剂,研究了非均相Fenton反应中亚甲基蓝的降解,并考虑了实际排放的印染废水中存在的无机助剂,进一步分析了典型无机助剂CuSO4、NaCl、Na2CO3、Na2SO4、Na2S的存在对该非均相Fenton体系的影响,结果表明：直接使用二茂铁做催化剂反应120min后,亚甲基蓝的剩余率为0．6％,羟基自由基的表观生成率为83．4％。NaCl、Na2CO3、Na2SO4、Na2S的加入会阻碍反应的进行,而CuSO4的加入会促进反应的进行。     

聚乙烯亚胺/Fe3O4杂化磁性纳米吸附剂去除甲基橙

采用戊二醛共价交联法制备出了聚乙烯亚胺/Fe3O4杂化磁性纳米吸附剂(PEI-Fe3O4)。通过TEM、XRD、FT-IR、VSM和TGA等手段表征了材料的结构和性质。以甲基橙(MO)为吸附质,系统考察了pH值、吸附时间和染料初始浓度等因素对吸附材料性能的影响。结果表明,MO在PEI-Fe3O4上的吸附具有强烈的pH依赖性,pH为3时吸附量最大;吸附平衡仅需20 min,吸附过程符合准二级动力学模型;等温吸附过程更符合Langmuir模型,MO的最大吸附量为242.4 mg/g。重复实验表明,吸附剂经过15次吸附/解吸附循环后仍可维持最初的吸附性能,显示出良好的机械和化学稳定性。因此,该杂化吸附剂在染料废水中MO的去除方面具有良好的应用前景。