nZVI@SiO_2-NH_2对合成染料脱色效果及其对大肠杆菌生物毒性研究
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摘要
采用液相还原法并使用氨基修饰的二氧化硅合成包覆型的纳米零价铁(nZVI@SiO_2-NH_2),同时,采用XRD、FT-IR及TEM等多种方法对所制备的材料进行表征.TEM表征结果表明,nZVI@SiO_2-NH_2粒径分布在10～50 nm之间,壳层厚度为15 nm.XRD和FTIR分析表明,复合颗粒具有Fe~0晶型结构的内核,表面SiO_2壳层存在氨基化修饰.使用nZVI@SiO_2-NH_2和nZVI对各类染料进行脱色处理,结果表明,nZVI@SiO_2-NH_2对上述染料的脱色效果都优于nZVI,且nZVI@SiO_2-NH_2具有对染料进行连续脱色的能力.大肠杆菌的存活情况和细胞内酶LDH和SOD的活性变化表明,nZVI@SiO_2-NH_2对生物的毒性更小.
In this study, the novel core-shell amino-functionalized silica coated nanoscale zerovalent iron(nZVI@SiO_2-NH_2) particles were prepared by using the liquid phase reduction method. The synthesized materials were characterized with different methods such as TEM, FT-IR and XRD. The TEM image showed that the average grain diameter of nZVI@SiO_2-NH_2 was about 10 to 50 nm, and the thickness of the silica shell was approximately 15 nm. The XRD and the FTIR results revealed that the core of the synthesized materials was mainly composed of Fe~0. Moreover, the silicon shell was modified by amino successfully. Both nZVI and nZVI@SiO_2-NH_2 nanoparticles(NPs) were used in dye decolorizion tests. The results showed that dye decolorization rate was significantly higher with the use of the nZVI@SiO_2-NH_2 NPs compared to that with the use of nZVI. Moreover, the nZVI@SiO_2-NH_2 NPs had the ability to decolorize repeated additions of dye. The survival rate of E. coli and the changes of the activities of LDH and SOD indicated that, compared with nZVI, nZVI@SiO_2-NH_2 NPs was less toxic to organisms.
In this study, the novel core-shell amino-functionalized silica coated nanoscale zerovalent iron(nZVI@SiO_2-NH_2) particles were prepared by using the liquid phase reduction method. The synthesized materials were characterized with different methods such as TEM, FT-IR and XRD. The TEM image showed that the average grain diameter of nZVI@SiO_2-NH_2 was about 10 to 50 nm, and the thickness of the silica shell was approximately 15 nm. The XRD and the FTIR results revealed that the core of the synthesized materials was mainly composed of Fe~0. Moreover, the silicon shell was modified by amino successfully. Both nZVI and nZVI@SiO_2-NH_2 nanoparticles(NPs) were used in dye decolorizion tests. The results showed that dye decolorization rate was significantly higher with the use of the nZVI@SiO_2-NH_2 NPs compared to that with the use of nZVI. Moreover, the nZVI@SiO_2-NH_2 NPs had the ability to decolorize repeated additions of dye. The survival rate of E. coli and the changes of the activities of LDH and SOD indicated that, compared with nZVI, nZVI@SiO_2-NH_2 NPs was less toxic to organisms.
引文
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Satapanajaru T,Chompuchan C,Suntornchot P,et al.2011.Enhancing decolorization of Reactive Black 5 and Reactive Red 198 during nano zerovalent iron treatment[J].Desalination,266(1):218-230
Shirin S,Balakrishnan V K.2011.Using chemical reactivity to provide insights into environmental transformations of priority organic substances: The Fe0-mediated reduction of Acid Blue 129[J].Environmental Science & Technology,45(24):10369-10377
Shu H Y,Chang M C,Chen C C,et al.2010.Using resin supported nano zero-valent iron particles for decoloration of Acid Blue 113 azo dye solution[J].Journal of Hazardous Materials,184(1):499-505
Singh R L,Singh P K,Singh R P.2015.Enzymatic decolorization and degradation of azo dyes-A review[J].International Biodeterioration & Biodegradation,104:21-31
Wang X,Yang J,Zhu M.2014.Effects of PMMA/anisole hybrid coatings on discoloration performance of nano zerovalent iron toward organic dyes[J].Journal of the Taiwan Institute of Chemical Engineers,45(3):937-946
Zhang X,Lin S,Chen Z,et al.2011.Kaolinite-supported nanoscale zero-valent iron for removal of Pb2+ from aqueous solution: reactivity,characterization and mechanism[J].Water Research,45(11):3481-3488
Fatima M,Farooq R,Lindstr?mb R W,et al.2017.A review on biocatalytic decomposition of azo dyes and electrons recovery[J].Journal of Molecular Liquids,246:275-281
Fu F,Dionysiou D D,Hong L.2014.The use of zero-valent iron for groundwater remediation and wastewater treatment: A review[J].Journal of Hazardous Materials,267(3):194-205
Gu C,Jia H,Li H,et al.2015.Synthesis of highly reactive subnano-sized zero-valent iron using smectite clay templates[J].Environmental Science & Technology, 44(11):4258-4263
关泽宇.2015.氨基修饰的壳核型纳米铁强化厌氧微生物脱氯特性及机理研究[D].广州:华南理工大学
Jiang Z,Lv L,Zhang W,et al.2011.Nitrate reduction using nanosized zero-valent iron supported by polystyrene resins: Role of surface functional groups[J].Water Research,45(6):2191-2198
Kahru A,Dubourguier H C,Blinova I,et al.2008.Biotests and biosensors for ecotoxicology of metal oxide nanoparticles: A minireview[J].Sensors,8(8):5153-5170
Keenan C R,Sedlak D L.2008.Factors affecting the yield of oxidants from the reaction of nanoparticulate zero-valent iron and oxygen[J].Environmental Science & Technology,42(14):5377-5378
Klas S,Kirk D W.2013.Advantages of low pH and limited oxygenation in arsenite removal from water by zero-valent iron[J].Journal of Hazardous Materials,252-253:77-82
Lee C,Kim J Y,Lee W I,et al.2008.Bactericidal effect of zero-valent iron nanoparticles on Escherichia coli[J].Environmental Science & Technology,42(13):4927-33
Lv X,Xue X,Jiang G,et al.2014.Nanoscale zero-valent iron(nZVI) assembled on magnetic Fe3O4/graphene for chromium(VI) removal from aqueous solution[J].Journal Colloid Interface Sciences,417(417):51-59
庞龙,周庆祥,苏现伐.2011.纳米零价铁修饰技术研究进展[J].化工进展,30(6):1361-1368
Robinson T,Mcmullan G,Marchant R,et al.2001.Remediation of dyes in textile effluent: a critical review on current treatment technologies with a proposed alternative[J].Bioresource Technology,77(3):247-255
Satapanajaru T,Chompuchan C,Suntornchot P,et al.2011.Enhancing decolorization of Reactive Black 5 and Reactive Red 198 during nano zerovalent iron treatment[J].Desalination,266(1):218-230
Shirin S,Balakrishnan V K.2011.Using chemical reactivity to provide insights into environmental transformations of priority organic substances: The Fe0-mediated reduction of Acid Blue 129[J].Environmental Science & Technology,45(24):10369-10377
Shu H Y,Chang M C,Chen C C,et al.2010.Using resin supported nano zero-valent iron particles for decoloration of Acid Blue 113 azo dye solution[J].Journal of Hazardous Materials,184(1):499-505
Singh R L,Singh P K,Singh R P.2015.Enzymatic decolorization and degradation of azo dyes-A review[J].International Biodeterioration & Biodegradation,104:21-31
Wang X,Yang J,Zhu M.2014.Effects of PMMA/anisole hybrid coatings on discoloration performance of nano zerovalent iron toward organic dyes[J].Journal of the Taiwan Institute of Chemical Engineers,45(3):937-946
Zhang X,Lin S,Chen Z,et al.2011.Kaolinite-supported nanoscale zero-valent iron for removal of Pb2+ from aqueous solution: reactivity,characterization and mechanism[J].Water Research,45(11):3481-3488