海泡石负载型纳米零价铁对水中Cu(II)、Zn(II)的去除研究
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摘要
针对日益突出的水体重金属污染问题,采用液相还原法制备海泡石负载纳米零价铁(S-nZVI),并研究其对Cu(II)、Zn(II)的去除效果.同时,利用比表面积与孔径分析(BET)、透射电子显微镜(TEM)、X射线衍射(XRD)对制备出的材料进行表征,研究pH、S-nZVI投加量、重金属离子溶液初始浓度对去除率的影响,拟合S-nZVI材料去除Cu(II)、Zn(II)的动力学模型和吸附等温模型,并对反应后的S-nZVI进行回收及再生.结果表明,液相还原法可以成功制备出S-nZVI,且颗粒分布均匀.在60 min左右,S-nZVI对Cu(II)、Zn(II)的去除达到平衡.Cu(II)、Zn(II)的去除率随着pH值的升高而升高.当Cu(II)、Zn(II)溶液初始浓度为20 mg·L~(-1)时,最佳S-nZVI投加量分别为0.030、0.050 g,此时去除率分别为98.98%、98.97%.当Cu(II)浓度为90 mg·L~(-1)时,S-nZVI材料对Cu(II)的去除量最大,为127.57 mg·g~(-1);对Zn(II)来说,当浓度为110 mg·L~(-1)时去除量最大,为109.13 mg·g~(-1).去除过程符合准二级动力学模型和Langmuir吸附等温模型.S-nZVI可通过外加磁场进行回收,5次再生处理后其对Cu(II)、Zn(II)的去除率仍维持在96.84%、80.25%.实验结果显示,S-nZVI在废水除Cu(II)、Zn(II)领域具有很好的应用前景.
With the increasingly severe problem of heavy metal contamination in water body, this paper studies the effect of removing Cu(II) and Zn(II) by applying sepiolite-supported nanoscale zero-valent iron(S-nZVI) that was prepared by liquid phase reduction method. The prepared materials were characterized by specific surface area and pore size analysis(BET), transmission electron microscopy(TEM) and X-ray diffraction(XRD). The impacting factors including pH values, S-nZVI dosage and initial concentration of heavy metal ion solution were studied. The kinetic model and adsorption isotherm model of S-nZVI for removing Cu(II) and Zn(II) were fitted, and the reacted S-nZVI was recovered and regenerated. The results showed that the liquid phase reduction method can successfully prepare S-nZVI with uniform particle distribution. The removal of Cu(II) and Zn(II) by S-nZVI reached to a balance at about 60 min.The removal rates of Cu(II) and Zn(II) increased with pH values. When the initial concentration of Cu(II) and Zn(II) solution was 20 mg·L~(-1), the optimal S-nZVI materials dosage were 0.030 g and 0.050 g, respectively, and the removal rates were 98.98% and 98.97%, respectively. When Cu(II) concentration was 90 mg·L~(-1), the removal capacity of Cu(II) by S-nZVI material was the highest, which was 127.57 mg·g~(-1). For Zn(II), when its concentration was 110 mg·L~(-1), the maximum removal capacity was 109.13 mg·g~(-1). The removal process conformed to the pseudo-second-order kinetic model and the Langmuir adsorption isotherm model. After the reaction was removed, S-nZVI can be recovered by applied magnetic field. The removal rate of Cu(II) and Zn(II) after 5 times of regeneration treatment maintained at 96.84% and 80.25%, respectively. The results show that S-nZVI has a good prospect to application in the removal of Cu(II) and Zn(II) for wastewater treatment.
With the increasingly severe problem of heavy metal contamination in water body, this paper studies the effect of removing Cu(II) and Zn(II) by applying sepiolite-supported nanoscale zero-valent iron(S-nZVI) that was prepared by liquid phase reduction method. The prepared materials were characterized by specific surface area and pore size analysis(BET), transmission electron microscopy(TEM) and X-ray diffraction(XRD). The impacting factors including pH values, S-nZVI dosage and initial concentration of heavy metal ion solution were studied. The kinetic model and adsorption isotherm model of S-nZVI for removing Cu(II) and Zn(II) were fitted, and the reacted S-nZVI was recovered and regenerated. The results showed that the liquid phase reduction method can successfully prepare S-nZVI with uniform particle distribution. The removal of Cu(II) and Zn(II) by S-nZVI reached to a balance at about 60 min.The removal rates of Cu(II) and Zn(II) increased with pH values. When the initial concentration of Cu(II) and Zn(II) solution was 20 mg·L~(-1), the optimal S-nZVI materials dosage were 0.030 g and 0.050 g, respectively, and the removal rates were 98.98% and 98.97%, respectively. When Cu(II) concentration was 90 mg·L~(-1), the removal capacity of Cu(II) by S-nZVI material was the highest, which was 127.57 mg·g~(-1). For Zn(II), when its concentration was 110 mg·L~(-1), the maximum removal capacity was 109.13 mg·g~(-1). The removal process conformed to the pseudo-second-order kinetic model and the Langmuir adsorption isotherm model. After the reaction was removed, S-nZVI can be recovered by applied magnetic field. The removal rate of Cu(II) and Zn(II) after 5 times of regeneration treatment maintained at 96.84% and 80.25%, respectively. The results show that S-nZVI has a good prospect to application in the removal of Cu(II) and Zn(II) for wastewater treatment.
引文
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肖燕萍,宋新山,赵志淼,等.2017.海藻酸钠/蒙脱石联合负载型纳米Fe0对Cu(Ⅱ)的去除研究[J].环境科学学报,37(1):227-233
肖燕萍.,2017.不同负载型纳米零价铁对水中Cu(Ⅱ)和Cr(Ⅵ)的去除研究[D].上海:东华大学
修瑞瑞,何世颖,宋海亮等.2018.改性硅藻土/纳米零价铁复合材料去除水中Cu2+的研究[J].环境污染与防治,40(4):414-417
徐应明,梁学峰,孙国红,等.2009.海泡石表面化学特性及其对重金属Pb2+、Cd2+、Cu2+吸附机理研究[J].农业环境科学学报,28(10):2057-2063
殷齐贺.2017.膨润土负载纳米零价铁去除废水中Cd(Ⅱ)的研究[J].福建质量管理,(13):151-152
张鑫.2010.纳米零价铁去除水中重金属离子的研究进展[J].化学研究,21(3):97-100
张亚南,骆碧君,武海虹,等.2015.重金属去除方法的研究进展[J].盐业与化工,44(10):1-6
祝爱侠.2012.超细电气石产品制备及对养殖水质改良效果和机理的研究[D].无锡:江南大学
陈健.2016.活性炭负载纳米零价铁去除矿山废水中Cu2+和Cr6+的研究[D].赣州:江西理工大学
Fu R,Yang Y,Xu Z,et al.2015.The removal of chromium(VI) and lead(II) from groundwater using sepiolite-supported nanoscale zero-valent iron(S-NZVI)[J].Chemosphere,138:726-734
郭晶晶.2014.蒙脱石/零价铁纳米复合材料修复水体重金属污染效率及机理研究[D].呼和浩特:内蒙古大学
韩占涛,吕晓立,张威,等.2013.纳米零价铁地下水修复技术的最新研究进展[J].水文地质工程地质,40(1):41-47
何桂春,陈健,丁军,等.2016.活性炭负载纳米零价铁去除矿山废水中的Cu2+[J].有色金属科学与工程,7(5):119-124
何元渊,祁彩菊,仲万军,等.2014.核桃壳负载纳米零价铁吸附废水中Pb2+[J].精细化工,31(4):480- 485
季莹.2013.纳米零价铁:固体溶液界面电化学特性和表面模型[D].上海:同济大学
李琛,于俊洋.2013.海泡石改性及其在含铬废水处理中的应用[J].杭州化工,43(3):4-7
Li S,Wang W,Liang F,et al.2017.Heavy metal removal using nanoscale zero-valent iron (nZVI): theory and application[J].Journal of Hazardous Materials,322:163-171
李亚娟,赵传起,洪沛东,等.2018.磁性还原石墨烯的制备及其对抗生素的吸附性能[J].环境工程学报,12(1):15-24
李钰婷,张亚雷,代朝猛,等.2012.纳米零价铁颗粒去除水中重金属的研究进展[J].环境化学, 31(9):1349-1354
廖润华,夏光华,成岳,等.2006.改性海泡石的制备及其吸附性能试验研究[J].中国陶瓷工业,13(4):17-21
刘玉茹,费学宁,郝亚超,等.2013.海泡石负载型纳米铁的制备及其对六氯丁二烯的降解特性[J].环境化学,32(11):2156-2161
Matheson L J,Tratnyek P G.1994.Reductive dehalogenation of chlorinated methanes by iron metal[J].Environmental Science & Technology,28(12):2045-2053
母娜.2015.海泡石负载型纳米零价铁去除水和土壤中的多溴联苯醚[D].上海:上海应用技术学院
孙国帅.2015.碳热法负载纳米零价铁对Cr(Ⅵ)和Cd(Ⅱ)的去除研究[D].哈尔滨:哈尔滨工业大学
王昕,张春丽,任广军,等.2008.碳纳米管吸附去除水溶液中锌离子的性能[J].电镀与精饰,30(10):4-6
Wu L,Liao L,Lv G,et al.2013.Micro-electrolysis of Cr(VI) in the nanoscale zero-valent iron loaded activated carbon[J].Journal of Hazardous Materials,254/255(12):277-283
Xiao J,Gao B,Yue Q,et al.2015.Characterization of nanoscale zero-valent iron supported on granular activated carbon and its application in removal of acrylonitrile from aqueous solution[J].Journal of the Taiwan Institute of Chemical Engineers,55:152-158
肖燕萍,宋新山,赵志淼,等.2017.海藻酸钠/蒙脱石联合负载型纳米Fe0对Cu(Ⅱ)的去除研究[J].环境科学学报,37(1):227-233
肖燕萍.,2017.不同负载型纳米零价铁对水中Cu(Ⅱ)和Cr(Ⅵ)的去除研究[D].上海:东华大学
修瑞瑞,何世颖,宋海亮等.2018.改性硅藻土/纳米零价铁复合材料去除水中Cu2+的研究[J].环境污染与防治,40(4):414-417
徐应明,梁学峰,孙国红,等.2009.海泡石表面化学特性及其对重金属Pb2+、Cd2+、Cu2+吸附机理研究[J].农业环境科学学报,28(10):2057-2063
殷齐贺.2017.膨润土负载纳米零价铁去除废水中Cd(Ⅱ)的研究[J].福建质量管理,(13):151-152
张鑫.2010.纳米零价铁去除水中重金属离子的研究进展[J].化学研究,21(3):97-100
张亚南,骆碧君,武海虹,等.2015.重金属去除方法的研究进展[J].盐业与化工,44(10):1-6
祝爱侠.2012.超细电气石产品制备及对养殖水质改良效果和机理的研究[D].无锡:江南大学