基于纳米零价铁的类芬顿体系降解土霉素的研究
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摘要
通过FeSO_4与NaBH_4在碱性条件下反应,制备纳米零价铁颗粒。X射线衍射表明产物是α-Fe~0,扫描电子显微镜得到纳米零价铁的粒径大约为20nm,氮吸附比表面积为19.607m~2·g~(-1),等电点为7.2。研究该纳米零价铁对水溶液中的土霉素的去除作用,发现纳米零价铁的投加量、土霉素初始浓度和溶液的pH值均对其去除效果产生影响。在纳米零价铁投加量为1.0g·L~(-1),pH值为6.5的条件下,在4h内将质量浓度为100mg·L~(-1)的土霉素基本完全降解,去除率为98.8%。该研究结果表明,纳米零价铁对水溶液中的土霉素有很好的去除效果。
Zero-valent iron particles(NZVI)were prepared with a method of reduction in liquid phase by the reaction of FeSO_4 and NaBH_4. X-ray diffraction analysis indicated the α-Fe~0 characteristic of this NZVI. Scanning electron micrographs(SEM)showed that the mean particle size of NZVI was about 20 nm. The results of BET surface area and Zeta-potential analyses indicated that the surface area of NZVI was of 19.607 m~2·g~(-1), and the iso-electric point was of 7.2. The removal of oxytetracycline(OTC) using the prepared NZVI at ambient temperature and pressure were investigated. The results indicated that degradation of OTC was strongly dependent on the dosage of NZVI, reactant concentration and pH value. Under pH 6.5, after 4 h of reaction, the removal efficiency can reach98.8% when the quality of NZVI is 1.0 g·L~(-1) and the initial concentration of OTC is 100 mg·L~(-1). All these results revealed that NZVI can be applied in the reduction of potential contaminants such as tetracyclines.
Zero-valent iron particles(NZVI)were prepared with a method of reduction in liquid phase by the reaction of FeSO_4 and NaBH_4. X-ray diffraction analysis indicated the α-Fe~0 characteristic of this NZVI. Scanning electron micrographs(SEM)showed that the mean particle size of NZVI was about 20 nm. The results of BET surface area and Zeta-potential analyses indicated that the surface area of NZVI was of 19.607 m~2·g~(-1), and the iso-electric point was of 7.2. The removal of oxytetracycline(OTC) using the prepared NZVI at ambient temperature and pressure were investigated. The results indicated that degradation of OTC was strongly dependent on the dosage of NZVI, reactant concentration and pH value. Under pH 6.5, after 4 h of reaction, the removal efficiency can reach98.8% when the quality of NZVI is 1.0 g·L~(-1) and the initial concentration of OTC is 100 mg·L~(-1). All these results revealed that NZVI can be applied in the reduction of potential contaminants such as tetracyclines.
引文
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[20]D.R.Burris,T.J.Campbell,V.S.Manoranjan.Sorption of Trichloroethylene and Tetrachloroethylene in a Batch Reactive Metallic Iron-Water System[J].Environmental Science&Technology,1995,29:2850-2855.
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[2]杨晓芳,杨涛,王莹,等.四环素类抗生素污染现状及其环境行为研究进展[J].环境工程,2014,32:123-127.
[3]Y.G.Zhu,T.A.Johnson,J.Q.Su,M.Qiao,J.M.Tiedje,Diverse and abundant antibiotic resistance genes in Chinese swine farms[J].Proceedings of the National Academy of Sciences of the United States of America,2013,110:3435-3440.
[4]苟世霞,王春荣,于晓华,等.Photo-Fenton高级氧化技术处理土霉素废水的研究[J].甘肃科学学报,2013,25:43-46.
[5]秦松岩,李杭,山丹,等.四环素类抗生素生产废水处理现状与研究进展[J].天津理工大学学报,2016,32:50-54.
[6]V.Homem,L.Santos.Degradation and removal methods of antibiotics from aqueous matrices-A review[J].Journal of Environmental Management,2011,92:2304-2347.
[7]M.Stieber,A.Putschew,M.Jekel.Treatment of Pharmaceuticals and Diagnostic Agents Using Zero-Valent Iron-Kinetic Studies and Assessment of Transformation Products Assay[J].Environmental Science&Technology,2011,45:4944-4950.
[8]S.E.Mylon,Q.Sun,T.D.Waite.Process optimization in use of zero valent iron nanoparticles for oxidative transformations[J].Chemosphere,2010,81:127-131.
[9]C.R.Keenan,D.L.Sedlak.Factors affecting the yield of oxidants from the reaction of manoparticulate zero-valent iron and oxygen[J].Environmental Science&Technology,2008,42:1262-1267.
[10]D.-h.Kim,J.Kim,W.Choi.Effect of magnetic field on the zero valent iron induced oxidation reaction[J].Journal of Hazardous materials,2011,192:928-931.
[11]L.J.Xu,J.L.Wang.A heterogeneous Fenton-like system with nanoparticulate zero-valent iron for removal of 4-chloro-3-methyl phenol[J].Journal of Hazardous materials,2011,186:256-264.
[12]D.H.Bremner,A.E.Burgess,D.Houllemare,Phenol degradation using hydroxyl radicals generated from zero-valent iron and hydrogen peroxide[J].Applied Catalysis B-Environmental,2006,63:15-19.
[13]K.-C.Huang,S.H.Ehrman.Synthesis of Iron Nanoparticles via Chemical Reduction with Palladium Ion Seeds[J].Langmuir,2007,23:1419-1426.
[14]C.Gu,K.G.Karthikeyan.Interaction of Tetracycline with Aluminum and Iron Hydrous Oxides[J].Environmental Science&Technology,2005,39:2660-2667.
[15]H.Chen,H.Luo,Y.Lan,et al.Removal of tetracycline from aqueous solutions using polyvinylpyrrolidone(PVP-K30)modified nanoscale zerovalent iron[J].Journal of Hazardous Materials,2011,192:44-53.
[16]X.Zhang,F.Wu,N.Deng.Degradation of paracetamol in self assemblyβ-cyclodextrin/Ti O2suspension under visible irradiation[J].Catalysis Communications,2010,11:422-425.
[17]S.H.Joo,A.J.Feitz,T.D.Waite.Oxidative Degradation of the Carbothioate Herbicide,Molinate,Using Nanoscale Zero-Valent Iron[J].Environmental Science&Technology,2004,38:2242-2247.
[18]M.Arias,M.S.García-Falcón,L.García-Río,et al.Binding constants of oxytetracycline to animal feed divalent cations[J].Journal of Food Engineering,2007,78:69-73.
[19]Y.-P.Sun,X.-Q.Li,W.-X.Zhang,et al.A method for the preparation of stable dispersion of zero-valent iron nanoparticles[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects2007,308:60-66.
[20]D.R.Burris,T.J.Campbell,V.S.Manoranjan.Sorption of Trichloroethylene and Tetrachloroethylene in a Batch Reactive Metallic Iron-Water System[J].Environmental Science&Technology,1995,29:2850-2855.
[21]李魁晓,曹楠,张昱,等.Fenton法氧化处理水中土霉素的研究[J].环境工程学报,2008,865-868.