改性沸石负载纳米铁/镍去除地下水中2,4-二氯苯酚的渗透反应格栅研究

为研究新制备复合材料改性沸石负载纳米零价铁/镍去除水中2,4-二氯苯酚效果以及该材料在地下水污染原位修复中的应用情况,开展了2,4-二氯苯酚的批实验和柱实验。结果表明,材料的双金属颗粒分散性良好,避免了团聚现象的出现。水中2,4-二氯苯酚的去除是在复合材料表面降解和吸附协同作用的结果,且降解在整个过程发挥更大的作用。通过渗透反应格栅实验中不同孔隙体积下p H、ORP、温度的考察发现,溶液处于弱碱性状态,不利于脱氯反应的进行,而体系ORP和温度均有利于2,4-二氯苯酚的脱氯反应。     

零价铁对2,4-二氯酚的还原脱氯研究

氯酚是环境中常见的难降解污染物,氯酚中氯原子的脱除可以提高其生化性。在恒温条件下,利用零价铁(Fe0)还原2,4-二氯酚(2,4-DCP)的模拟废水,研究得出在不同条件下溶液的脱氯率,表明在初始溶液pH=4.2时有利于脱氯反应的进行,Fe/C和Fe/Cu体系形成原电池,脱氯能力大大提高,Fe/Cu体系的脱氯率达到了60%,Fe/C体系的脱氯率达到了44%。溶解氧对2,4-DCP的脱氯反应有明显的抑制作用,厌氧条件下过6个小时脱氯率能够达到50%,而在好氧条件下的脱氯率为40%左右。通过XRD检测,分析了使零价铁钝化的原因。     

纳米零价铁/过硫酸盐去除2,4-二氯酚的动力学研究

为更好地理解纳米零价铁(nZVI)激活过硫酸盐(PS)的机制和动力学,基于Langmuir-Hinshelwood机理,结合nZVI/PS体系中主要的反应步骤对2,4-二氯酚(2,4-DCP)的降解过程建立动力学模型。使用不同影响因素下(包括nZVI投加量、初始PS浓度和初始2,4-DCP浓度)PS,2,4-DCP浓度变化数据拟合动力学模型并确定速率常数,通过对速率常数的敏感性分析得到：2,4-DCP降解的整体反应动力学是由前体表面复合物内部发生电子转移反应形成硫酸根自由基SO₄^·-以及2,4-DCP被羟基自由基OH^·降解这两个过程来控制的。     

零价铁对2,4-二氯酚的还原脱氯研究

氯酚是环境中常见的难降解污染物,氯酚中氯原子的脱除可以提高其生化性。在恒温条件下,利用零价铁(Fe0)还原2,4-二氯酚(2,4-DCP)的模拟废水,研究得出在不同条件下溶液的脱氯率,表明在初始溶液pH=4.2时有利于脱氯反应的进行,Fe/C和Fe/Cu体系形成原电池,脱氯能力大大提高,Fe/Cu体系的脱氯率达到了60%,Fe/C体系的脱氯率达到了44%。溶解氧对2,4-DCP的脱氯反应有明显的抑制作用,厌氧条件下过6个小时脱氯率能够达到50%,而在好氧条件下的脱氯率为40%左右。通过XRD检测,分析了使零价铁钝化的原因。     

超声波/零价铁协同降解2,4-二氯苯酚和五氯苯酚的研究

以2,4-二氯苯酚和五氯苯酚为目标污染物,分别在单一超声波体系、单一零价铁还原体系和超声波/零价铁协同体系下进行间歇性试验,结果表明:超声波/零价铁协同体系对2,4二氯苯酚和五氯苯酚的降解率明显高于单一超声波体系或单一零价铁体系下的降解率,也高于两单一体系下的降解率之和,表现出显著的协同作用,各反应体系下的降解规律符合一级反应动力学方程;同时考察了初始pH、初始浓度、零价铁投加量以及超声波声功率等控制参数对协同体系下降解率的影响。     

有机膨润土负载纳米铁去除2,4-二氯酚

用具有良好吸附能力的有机膨润土作载体,通过FeSO4与NaBH4反应制得有机膨润土负载的纳米铁(nanoscale zero-valent iron supported onorganobentonite,NZVI/CTMAB-Bent).用X射线衍射、Brunauer-Emmett-Teller法对NZVI/CTMAB-Bent进行了结构表征,并将NZVI/CTMAB-Bent作催化剂用于2,4-二氯酚的去除.考察了NZVI/CTMAB-Bent与2,4-二氯酚反应过程中,介质pH值、不同起始浓度的2,4-二氯酚对其去除率的影响,并与相同铁含量的纳米铁(nanoscale zero-valent iron,NZW)进行了比较.结果表明:在相同实验条件下,2,4-二氯酚与NZVI/CTMAB-Bent反应120 min后去除率达90.6%,不仅远高于相同铁含量NZVI对2,4-二氯酚去除率(23.2%),而且也明显优于相同铁含量的NZVI和含土量相同的有机膨润土对2,4-二氯酚去除率的加和(39.0%).     

改性纳米零价铁去除地下水硝酸盐的研究

采用提纯凹凸棒土(ATP)负载纳米零价铁(nZVI)制备得到改性材料ATP-nZVI,将其用于对地下水硝酸盐的去除研究。通过静水实验考察了溶液中共存阴离子和反应温度对ATP-nZVI去除NO₃^--N的影响,通过模拟可渗透反应墙(PRB)考察了溶液初始pH、初始NO₃^--N浓度、材料装填方式、流速对ATP-nZVI去除NO₃^--N的影响,并通过更换PRB装填材料将ATP-nZVI与石英砂、ATP、铁粉、nZVI等材料对NO₃^--N的去除效果进行了比较。结果表明：共存阴离子对ATP-nZVI去除NO₃^--N具有抑制作用,其抑制作用的顺序为PO₄^3->CO₃^2->SO₄^2->Cl^-;ATP-nZVI对NO<...     

2,4-二氯苯酚的分离纯化

采用固-液萃取法分离纯化2,4-二氯苯酚。其中的杂质成分与正丙醇胺结合溶解于水中,留下固体状态的2,4-二氯苯酚。纯化所得2,4-二氯苯酚的纯度大于99%,收率大于90%。该方法操作简便,成本低,收率高,适于工业化生产。     

醇水体系制备纳米Pd/Fe颗粒去除水中2,4-DCP

为了提高纳米铁的活性和分散性,在醇水体系下制备出纳米钯铁(Pd/Fe)双金属颗粒并表征,将制得的纳米Pd/Fe颗粒应用于水中2,4-二氯苯酚(2,4-DCP)的去除,考察了材料投加量、反应温度、初始pH值、2,4-二氯苯酚初始浓度等因素对2,4-DCP去除的影响,分析了2,4-DCP的去除机理并进行动力学拟合。结果表明,在醇水体系中制备纳米铁有利于纳米颗粒的稳定分散;钯的加入将脱氯途径转变为催化加氢,极大改善了2,4-DCP的去除效果;当2,4-DCP初始浓度为20 mg/L、反应温度30℃、纳米Pd/Fe颗粒投加量为2 g/L时,2,4-DCP可在5 h内去除99.9%;反应过程符合修正的一级反应动力学方程。     

改性纳米铁镍去除水中2,4-DCP的研究

采用Pluronic F-127改性纳米零价铁后负载镍,形成改性纳米铁镍(F-NZVI/Ni)。探讨了Ni的负载量、F-NZVI/Ni的投加量、2,4-DCP初始浓度、pH及反应温度对2,4-DCP去除率的影响。同时探究了F-NZVI/Ni去除2,4-DCP的最佳条件下F-NZVI/Ni去除2,4-DCP的反应过程。结果表明,F-NZVI/Ni去除2,4-DCP的能力优于NZVI,当F-NZVI/Ni投加量为3 g/L,镍负载率为5%,2,4-DCP初始浓度为20 mg/L,反应温度为35℃,初始pH值为7时,2,4-DCP的去除率为97%。F-NZVI/Ni去除2,4-DCP主要是先吸附,然后在镍催化剂作用下将2,4-DCP降解为苯酚。     

改性纳米铁镍去除水中2,4-DCP的研究

采用Pluronic F-127改性纳米零价铁后负载镍,形成改性纳米铁镍(F-NZVI/Ni)。探讨了Ni的负载量、F-NZVI/Ni的投加量、2,4-DCP初始浓度、pH及反应温度对2,4-DCP去除率的影响。同时探究了F-NZVI/Ni去除2,4-DCP的最佳条件下F-NZVI/Ni去除2,4-DCP的反应过程。结果表明,F-NZVI/Ni去除2,4-DCP的能力优于NZVI,当F-NZVI/Ni投加量为3 g/L,镍负载率为5%,2,4-DCP初始浓度为20 mg/L,反应温度为35℃,初始pH值为7时,2,4-DCP的去除率为97%。F-NZVI/Ni去除2,4-DCP主要是先吸附,然后在镍催化剂作用下将2,4-DCP降解为苯酚。     

Surfactant-assisted removal of 2,4-dichlorophenol from soil by zero-valent Fe/Cu activated persulfate

The organic compounds contaminated soil substantially threatens the growth of plants and food safety. In this study, we synthesis zero-valent bimetallic Fe/Cu catalysts for the degradation of 2,4-dichlorophenol (DCP) in soils with persulfate (PS) in combination of organic surfactants and exploring the main environmental impact factors. The kinetic experiments show that the 5% (mass) dosage of Fe/Cu exhibits a higher degradation efficiency (86%) of DCP in soils, and the degradation efficiency of DCP increases with the increase of the initial PS concentration. Acidic conditions are favorable for the DCP degradation in soils. More importantly, the addition of Tween-80, and Triton-100 can obviously desorb DCP from the soil surface, which enhances the degradation efficiency of DCP in soils by Fe/Cu and PS reaction system. Furthermore, the Quenching experiments demonstrate that SO₄^-· and ·OH are the predominant radicals for the degradation of DCP during the Fe/Cu and PS reaction system as well as non-radical also exist. The findings of this work provide an effective method for remediating DCP from soils.     

Adsorption of 2,4-dichlorophenol on metal-nitrate modified activated carbon

To remove 2,4-dichlorophenol (2,4-DCP) from aqueous solution, the surface of the activated carbon was first treated with HCl and then the surface was modified by using various metal ions (Cu, Co, Fe, Ni, Zn, and Mg). Metal doping significantly enhanced the adsorption efficiency of activated carbon, an effect that was further increased by HCl treatment of the modified activated carbons. Of all the preparations, the zinc(II)-modified activated carbon with HCl treatment showed the highest adsorption capacity for 2,4-DCP. Analysis of the zinc(II)-modified activated carbon by SEM and BET showed a surface area and micropore volume of around 1,154.69 m²/g and 0.291 cm³/g, respectively, values about 20% higher than in the starting material. In the pH range of 2.0–11.0, the maximum uptake of 2,4-DCP from an initial concentration of 1,000 mg/L was 508 mg/g at pH 4.0.     

Fe~0可渗透反应墙处理地下水污染的研究现状与展望

阐述了Fe⁰可渗透反应墙(permeable reactive barrier,PRB)技术在处理污染物时可能发生的反应机理及研究现状,主要介绍了零价铁的吸附共沉淀作用、电化学腐蚀作用、化学还原以及生物还原作用。同时指出零价铁作为填料的不足之处,并且展望了PRB技术今后的研究方向。     

Electrochemical degradation of 2,4-dichlorophenol on a palladium modified gas-diffusion electrode

Pd/C catalyst was prepared by hydrogen reduction method and used for the Pd/C gas-diffusion electrode. It was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry (CV) techniques. The electrochemical degradation of 2,4-dichlorophenol was investigated in a diaphragm electrolysis system, feeding firstly with hydrogen gas then with air, using the Pd/C gas-diffusion electrode and the carbon/polytetrafluoroethylene (C/PTFE) gas-diffusion electrode as a cathode, respectively. The results indicated that the self-made Pd/C gas-diffusion cathode can not only reductively dechlorinate 2,4-dichlorophenols by feeding hydrogen gas, but also accelerate the two-electron reduction of O₂ to hydrogen peroxide (H₂O₂) by feeding air. Therefore, both the removal efficiency and the dechlorination degree of 2,4-dichlorophenol reached about 100% after 80 min, and the average removal efficiency of 2,4-dichlorophenol in terms of total organic carbon (TOC) exceeded 76% after 160 min by using Pd/C gas-diffusion cathode, which were better than that of the C/PTFE gas-diffusion cathode. The analysis of high-performance liquid chromatography (HPLC) identified that 4-chlorophenol, 2-chlorophenol, and phenol were the dechlorination products, and hydroquinone, benzoquinone, maleic, fumaric, crylic, malonic, oxalic, acetic and formic acids were the main oxidation intermediates. A reaction scheme involving all these intermediates was proposed.     

活性炭负载纳米零价铁去除对硝基酚的实验研究

以活性炭(GAC)作为载体,采用液相还原法制备活性炭负载纳米零价铁复合材料(nZVI-GAC),利用X射线衍射(XRD)、扫描电子显微镜(SEM)、比表面积及孔径分析仪(BET)等方法对复合材料进行了表征。研究了不同材料、不同初始浓度、不同初始pH、nZVI-GAC投加量去除对硝基酚(PNP)的影响。结果表明,纳米零价铁成功负载到活性炭上,但负载后的活性炭比表面积和孔径有所降低;在酸性条件下nZVI-GAC对PNP的去除率优于碱性条件下,并且随着nZVI-GAC投加量的增加和PNP初始浓度的降低,nZVI-GAC对PNP的去除率逐渐增加。     

Walnut shell supported nanoscale Fe0 for the removal of Cu(II) and Ni(II) ions from water

The walnut shell supported nanoscale zero‐valent iron (walnut‐nZVI) was prepared from sodium borohydride, iron(II) chloride tetrahydrate, and walnut shell by liquid phase chemical reduction and characterized by FTIR, TEM, and XRD. The composites were tested as adsorbent for the removal of Cu(II) or Ni(II) ions. The equilibrium data were analyzed by the Langmuir, Freundlich, Dubinin–Radushkevich, which revealed that Langmuir isotherm was more suitable for describing Cu(II) and Ni(II) ions adsorption than the other two isotherm models. The results indicated that the maximum adsorption capacity was higher than some other modified biomass waste adsorbents under the proposed conditions, were 458.7, 327.9 mg g^?1 for Cu(II) or Ni(II). The adsorption kinetics data indicated that the adsorption fitted well with the pseudo‐second‐order kinetic model. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43304.     

海藻酸钠-氢氧化镧改性Y型分子筛颗粒除氟研究

为解决除氟吸附剂分离困难、有效成分流失等问题,以海藻酸钠（SA）与氢氧化镧改性Y型分子筛（LHMS）为原料,采用滴球法制备了SA@LHMS颗粒吸附剂,并采用模拟废水对其进行了除氟研究。通过正交实验确定了吸附剂最佳制备条件,并通过间歇吸附实验测试了吸附剂投加量、pH、共存离子等因素对吸附的影响,探究了吸附速率、吸附等温线等吸附性能。结果表明,SA@LHMS吸附速率曲线符合拟二级反应速率方程;吸附等温线符合Ⅱ型等温线,为多分子层吸附;初始pH（3~12）对吸附效果没有显著影响;高浓度共存阴离子（50 mg/L）对吸附过程有一定抑制;1 mol/L和2 mol/L氢氧化钠溶液对SA@LHMS再生效果较好,经3次再生仍然保留较高的吸附能力。SA@LHMS颗粒表面和截面形态以及吸附前后颗粒的表面形态差异明显;吸附前后颗粒表面能谱（EDS）分析以及红外光谱（FT-IR）分析结果显示,吸附过程中溶液中的氟离子（F^-）与颗粒表面及内部的羟基（—OH）发生配体交换。