纳米铁/石墨烯插层复合材料制备及Cr~(6+)去除
|
摘要
近年来纳米铁(nZVI)技术用于废水处理受到广泛关注,因该技术具有廉价、高效、无二次污染等特点被认为是Cr~(6+)去除最有发展前景的方法之一。但nZVI技术在还原Cr~(6+)过程中因其颗粒微小易团聚、表面易钝化,导致nZVI的还原效力降低,限制了其在环境治理中的应用。为此,借用具有良好分散性的石墨烯为载体,设计nZVI纳米粒子插入石墨烯层间,构建新型纳米铁/石墨烯复合功能材料(G/nZVI)。通过探讨复合材料制备条件对G/nZVI去除Cr~(6+)效果的影响,优化制备过程,并利用红外光谱、XRD衍射光谱和TEM透射电镜技术对G/nZVI进行表层官能团、组成元素和表观形态进行研究;同时将G/nZVI应用于Cr~(6+)的去除效果分析。结果显示,将nZVI插层石墨烯片层结构可以有效地改善nZVI的分散能力,同时一定程度上提高了nZVI的抗氧化性,进而使Cr~(6+)的去除效果也得到很大提高。
Recently,a chemical reduction method using zero-valent iron(nZVI) has been widely studied for contaminated wastewater treatment.Earlier studies showed that this is a promising approach for Cr~(6+) removal because it is cheap,highly efficient,and environmentally friendly.However,using nZVI for treating Cr~(6+) has many drawbacks.For example,the high surface energy makes oxidation of n ZVI in the atmosphere easy,which means that the rate constant for the Cr~(6+) is low,and this decreases the nZVI reducing abilities.In this study,G/nZVI using a one-step liquid-phase reduction method was synthesized and the removal efficiency for Cr~(6+) and the oxidation resistance of the G-coated iron particles was investigated.The effects of G-coating preparation conditions on particle surface texture(using FTIR,XRD and TEM),size,reduction efficiency,and antioxidation abilities were also investigated.The degradation characteristics of G/nZVI and uncoated nZVI were compared with those of uncoated nZVI.
Recently,a chemical reduction method using zero-valent iron(nZVI) has been widely studied for contaminated wastewater treatment.Earlier studies showed that this is a promising approach for Cr~(6+) removal because it is cheap,highly efficient,and environmentally friendly.However,using nZVI for treating Cr~(6+) has many drawbacks.For example,the high surface energy makes oxidation of n ZVI in the atmosphere easy,which means that the rate constant for the Cr~(6+) is low,and this decreases the nZVI reducing abilities.In this study,G/nZVI using a one-step liquid-phase reduction method was synthesized and the removal efficiency for Cr~(6+) and the oxidation resistance of the G-coated iron particles was investigated.The effects of G-coating preparation conditions on particle surface texture(using FTIR,XRD and TEM),size,reduction efficiency,and antioxidation abilities were also investigated.The degradation characteristics of G/nZVI and uncoated nZVI were compared with those of uncoated nZVI.
引文
[1]耿兵.壳聚糖稳定纳米铁的制备与修复地表水中六价铬的研究[D].天津:南开大学,2009.
[2]蔺玉华,耿龙武.铬(Ⅵ)对鲤血清电解质水平的影响及其在鱼体中的蓄积[J].天津师范大学学报:自然科学版,2005,25(3):21-23.
[3]Montesinos V N,Quici N,Halac E B,et al.Litter MI highly efficient removal of Cr(Ⅵ)from water with nanoparticulated zero valent iron:understanding the Fe(Ⅲ)-Cr(Ⅲ)passive outer layer structure[J].Chem Eng J,2014,244:569-575.
[4]Huang L,Zhou S,Jin F,et al.Characterization and mechanism analysis of activated carbon fiber felt-stabilized nanoscale zero-valent iron for the removal of Cr(Ⅵ)from aqueous solution[J].Colloid Surf A:Physicochem Eng Asp,2014,447:59-66.
[5]Qiu B,Xu C,Sun D,et al.Poly aniline coating on carbon fiber fabrics for improved hexavalent chromium removal[J].RSC Adv,2014,4(56):29855-29865.
[6]Ravikumar K V G,Deepak Kumar,Rajeshwari A,et al.Acomparative study with biologically and chemically synthesized nZVI:applications in Cr(Ⅵ)removal and ecotoxicity assessment using indigenous microorganisms from chromium-contaminated site[J].Environ Sci Pollut Res,2016,23(3):2613-2627.
[7]Geranio L,Elzinga E,Geranio L.Review of zero valent iron and apatite as reactive materials for permeable reactive barrier[J].2007,7.
[8]Esfahani A R,Hojati S,Azimi A,et al.Enhanced hexavalent chromium removal from aqueous solution using a sepiolitestabilized zero-valent iron nanocomposite:impact of operational parameters and artificial neural network modeling[J].Taiwan Inst Chem Eng,2014:88-98.
[9]Lee C,Kim J Y,Lee W I,et al.Bactericidal effect of zerovalent iron nanoparticles on Escherichia coli[J].Environ SciTechnol,2008,42(13):4927-4933.
[10]Liu T,Zhao L,Suvn D,et al.Entrapment of nano scale zerovalentironin chitosan beads for hexavalent chromium removal from wastewater[J].Hazard Mater,2010,184:724-730.
[11]Lyu Xiaoshu,Xue Xiaoqin,Jiang Guangming,et al.Nanoscale zero-valent iron(nZVI)assembled on magnetic Fe3O4/graphene for chromium(Ⅵ)removal from aqueous solution[J].Journal of Colloid and Interface Science,2014,417:51-59.
[12]Zhang K,Dwivedi V,Chi C Y,et al.Graphene oxide/ferric hydroxide composites for efficient arsenate removal from drinking water[J].Journal of Hazrdous Materials,2010,182(1/2/3):162-168.
[13]Nair R R,Blake P,Grigorenko A N,et al.Fine structure constant defines visual transparency of graphene[J].Science,2008,320(5881):1308-1308.
[14]Chandra V,Park J,Chun Y,et al.Water-dispersible magnetite-reduced graphene oxide composites for arsenic removal[J].Acs Nano,2010,4(7):3979-3986.
[15]Kim K S,Zhao Y,Jang H,et al.Large-scale pattern growth of graphene films for stretchable transparent electrodes[J].Nature,2009,457(7230):706-710.
[16]刘佩佩.石墨烯/二氧化硅负载纳米铁对水中砷的去除研究[D].广州:华南理工大学,2016.
[2]蔺玉华,耿龙武.铬(Ⅵ)对鲤血清电解质水平的影响及其在鱼体中的蓄积[J].天津师范大学学报:自然科学版,2005,25(3):21-23.
[3]Montesinos V N,Quici N,Halac E B,et al.Litter MI highly efficient removal of Cr(Ⅵ)from water with nanoparticulated zero valent iron:understanding the Fe(Ⅲ)-Cr(Ⅲ)passive outer layer structure[J].Chem Eng J,2014,244:569-575.
[4]Huang L,Zhou S,Jin F,et al.Characterization and mechanism analysis of activated carbon fiber felt-stabilized nanoscale zero-valent iron for the removal of Cr(Ⅵ)from aqueous solution[J].Colloid Surf A:Physicochem Eng Asp,2014,447:59-66.
[5]Qiu B,Xu C,Sun D,et al.Poly aniline coating on carbon fiber fabrics for improved hexavalent chromium removal[J].RSC Adv,2014,4(56):29855-29865.
[6]Ravikumar K V G,Deepak Kumar,Rajeshwari A,et al.Acomparative study with biologically and chemically synthesized nZVI:applications in Cr(Ⅵ)removal and ecotoxicity assessment using indigenous microorganisms from chromium-contaminated site[J].Environ Sci Pollut Res,2016,23(3):2613-2627.
[7]Geranio L,Elzinga E,Geranio L.Review of zero valent iron and apatite as reactive materials for permeable reactive barrier[J].2007,7.
[8]Esfahani A R,Hojati S,Azimi A,et al.Enhanced hexavalent chromium removal from aqueous solution using a sepiolitestabilized zero-valent iron nanocomposite:impact of operational parameters and artificial neural network modeling[J].Taiwan Inst Chem Eng,2014:88-98.
[9]Lee C,Kim J Y,Lee W I,et al.Bactericidal effect of zerovalent iron nanoparticles on Escherichia coli[J].Environ SciTechnol,2008,42(13):4927-4933.
[10]Liu T,Zhao L,Suvn D,et al.Entrapment of nano scale zerovalentironin chitosan beads for hexavalent chromium removal from wastewater[J].Hazard Mater,2010,184:724-730.
[11]Lyu Xiaoshu,Xue Xiaoqin,Jiang Guangming,et al.Nanoscale zero-valent iron(nZVI)assembled on magnetic Fe3O4/graphene for chromium(Ⅵ)removal from aqueous solution[J].Journal of Colloid and Interface Science,2014,417:51-59.
[12]Zhang K,Dwivedi V,Chi C Y,et al.Graphene oxide/ferric hydroxide composites for efficient arsenate removal from drinking water[J].Journal of Hazrdous Materials,2010,182(1/2/3):162-168.
[13]Nair R R,Blake P,Grigorenko A N,et al.Fine structure constant defines visual transparency of graphene[J].Science,2008,320(5881):1308-1308.
[14]Chandra V,Park J,Chun Y,et al.Water-dispersible magnetite-reduced graphene oxide composites for arsenic removal[J].Acs Nano,2010,4(7):3979-3986.
[15]Kim K S,Zhao Y,Jang H,et al.Large-scale pattern growth of graphene films for stretchable transparent electrodes[J].Nature,2009,457(7230):706-710.
[16]刘佩佩.石墨烯/二氧化硅负载纳米铁对水中砷的去除研究[D].广州:华南理工大学,2016.