nav emailalert searchbtn searchbox tablepage yinyongbenwen piczone journalimg journalInfo journalinfonormal searchdiv searchzone qikanlogo popupnotification paper paperNew
2021, 01, v.37 76-87
Fe_3O4@还原氧化石墨烯纳米复合材料及其对四环素类抗生素的吸附研究
基金项目(Foundation): 辽宁省科技厅博士启动基金指导计划项目(No.20170520285); 辽宁省教育厅青年项目(No.LQ2017004); 沈阳化工大学青年育苗项目(No.XXLQ2019005)
邮箱(Email): yywwddsshh@sina.com;daliangliu@lnu.edu.cn;
DOI: 10.16026/j.cnki.iea.2021010076
发布时间: 2021-02-20
出版时间: 2021-02-20
移动端阅读
摘要:

金霉素、四环素和土霉素等是常用兽用抗生素,随着家畜排泄物堆肥的使用,3种抗生素进入到环境中成为新兴的污染物。本文采用一锅法,以葡萄糖为还原剂,制备了自组装的Fe_3O4纳米颗粒与还原氧化石墨烯的纳米复合材料(Fe_3O4@rGO),采用平衡吸附法研究了Fe_3O4@rGO对3种抗生素的吸附性能和行为。表征结果显示,Fe_3O4@rGO具有两种前驱体的特征,Fe_3O4纳米颗粒均匀分散在rGO表面上。吸附结果表明,Fe_3O4@rGO对3种抗生素的吸附速率很快,20min基本达到吸附平衡;当溶液pH值在4~8时,pH值对3种抗生素的吸附容量没有显著性的影响;Fe_3O4@rGO对3种抗生素的吸附容量均大于单纯的Fe_3O4和rGO;Fe_3O4@rGO对金霉素(189.2mg/g)和四环素(199.7mg/g)有较高的吸附容量,而对土霉素(112.5mg/g)的吸附容量相对较低,这是由于土霉素与Fe_3O4和rGO的结合力均相对较弱造成的;3种抗生素在Fe_3O4@rGO上的吸附过程可用Langmuir等温吸附模型和准二级动力学方程来描述。

Abstract:

Tetracycline(TC), oxytetracycline(OTC) and chlortetracycline(CTC) antibiotics as the veterinary drugs with widespread use can be exported to the environment through the manure application and have been classified as the emerging pollutants. A self-assemble nanocomposite of the nano-Fe_3O4 and the reduced graphene oxide(Fe_3O4@rGO) with D-glucose as the reductant was prepared by a one-pot method. The adsorption performances and behavior of 3 antibiotics onto the Fe_3O4@rGO were investigated using batch method. The results of characterization showed that there were the characteristic peaks of Fe_3O4 and rGO in the proposed nanocomposite and the nano-Fe_3O4 dispersed uniformly on the surface of rGO. The adsorptive results indicated that the adsorption equilibrium for 3 antibiotics was performed within 20 min with rapid rate. The high and stable adsorption amounts of 3 antibiotics were achieved in the p H range of 4~8. The adsorption capacities of the nanocomposite for 3 antibiotics were much higher than that of the pure nano-Fe_3O4 and rGO. The nanocomposite for CTC(189.2 mg/g) and TC(199.7 mg/g) had higher adsorption capacity than OTC(112.5 mg/g) due to the relatively weak binding force of OTC with Fe_3O4 and rGO. The Langmuir and Pseudo-second-order equations provided the best correlation for the adsorption process of 3 antibiotics onto the nanocomposite.

参考文献

[1]鲍艳宇,周启星,鲍艳姣,刘雨霞,李伟明,谢秀杰.3种四环素类抗生素在石油污染土壤上的吸附解吸[J].中国环境科学,2012,32(7):1257-1262.

[2]邹勇,胡秀虹,曹晖,阮运飞.N掺杂Ti O2纳米材料对盐酸四环素废水吸附性能研究[J].离子交换与吸附,2018,34(1):63-72.

[3]You N,Chen S,Wang Y,Fan H T,Sun L N,Sun T.In situ sampling of tetracycline antibiotics in culture wastewater using diffusive gradients in thin films equipped with graphene nanoplatelets[J].Environmental Research,2020,191:Art no 110089.

[4]张俊,杨晓洪,葛峰,王娜,焦少俊,叶波平.长期施用四环素残留猪粪对土壤中耐药菌及抗性基因形成的影响[J].环境科学,2014,35(6):2374-2380.

[5]张剑桥,楼耀尹,叶志隆,陈少华,魏群山.混凝前处理对猪场沼液MAP回收时抗生素残留的影响[J].中国环境科学,2018,38(7):2483-2489.

[6]李伟明,鲍艳宇,周启星.四环素类抗生素降解途径及其主要降解产物研究进展[J].应用生态学报,2012,23(8):2300-2308.

[7]Aga D S,Goldfish R,Kulshrestha P.Application of elisa in determining the fate of tetracyclines in land-applied livestock wastes[J].Analyst,2003,128(6):658-662.

[8]You N,Yao H,Wang Y,Fan H T,Wang C S,Sun T.Development and evaluation of diffusive gradients in thin films based on nano-sized zinc oxide particles for the in situ sampling of tetracyclines in pig breeding wastewater[J].Science of the Total Environment,2019,651:1653-1660.

[9]Fan H T,Sun W B,Jian B,Wang Q J,Li D W,Huang C C,Wang K J,Zhang Z G,Li W X.Adsorption of antimony(III) from aqueous solution by mercaptofunctionalized silica-supported organic-inorganic hybrid sorbent:Mechanism insights[J].Chemical Engineering Journal,2016,286:128-138.

[10]Fan H T,Wu J B,Fan X L,Zhang D S,Su Z J,Yan F,Sun T.Removal of cadmium(II) and lead(II) from aqueous solution using sulfur-functionalized silica prepared by hydrothermal-assisted grafting method[J].Chemical Engineering Journal,2012,198~199:355-363.

[11]Chang P H,Li Z H,Yu T L,Munkhbayera S,Kuo T H,Hung Y C,Jean J S,Lin K H.Sorptive removal of tetracycline from water by palygorskite[J].Journal of Hazardous Materials,2009,165(1/2/3):148-155.

[12]Caroni A L P F,De Lima C R M,Pereira M R,Fonseca J L C.The kinetics of adsorption of tetracycline on chitosan particles[J].Journal of Colloid and Interface Science,2009,340:182-191.

[13]Ocampo-Pérez R,Rivera-Utrilla J,Gómez-Pacheco C,Sánchez-Polo M,López-Pe?alver J J.Kinetic study of tetracycline adsorption on sludge-derived adsorbents in aqueous phase[J].Chemical Engineering Journal,2012,213:88-96.

[14]Liu P,Liu W J,Jiang H,Chen J J,Li W W,Yu H Q.Modification of bio-char derived from fast pyrolysis of biomass and its application in removal of tetracycline from aqueous solution[J].Bioresource Technology,2012,121:235-240.

[15]Fan H T,Shi L Q,Shen H,Chen X,Xie K P.Equilibrium,isotherm,kinetic and thermodynamic studies for removal of tetracyclines antibiotics by adsorption onto hazelnut shell derived activated carbons from aqueous media[J].RSC Advances,2016,6(111):109983-109991.

[16]Liu H J,Yang Y,Kang J,Fan M H,Qu J H.Removal of tetracycline from water by Fe-Mn binary oxide[J].Journal of Environmental Sciences,2012,24:242-247.

[17]Zhang M C,Li A M,Zhou Q,Shuang C D,Zhou W W,Wang M Q.Effect of pore size distribution on tetracycline adsorption using magnetic hypercrosslinked resins[J].Microporous&Microporous and Mesoporous Materials,2014,184:105-111.

[18]Zhang Z Y,Liu H J,Wu L Y,Lan H C,Qu J H.Preparation of amino-Fe(III) functionalized mesoporous silica for synergistic adsorption of tetracycline and copper[J].Chemosphere,2015,138:625-632.

[19]Hao R,Xiao X,Zuo X X,Nan J M,Zhang W D.Efficient adsorption and visible-light photocatalytic degradation of tetracycline hydrochloride using mesoporous Bi OImicrospheres[J].Journal of Hazardous Materials,2012,209~210:137-145.

[20]Sui D P,Li H H,Chai Y,Li J,Liu S,Zhao Y,Fan H T,Xu H B.Adsorption characteristics of tetracycline antibiotics from aqueous solution onto graphene nanoplatelets:Equilibrium,kinetic and thermodynamic studies[J].Desalination and Water Treatment,2017,94:263-271.

[21]Zhang L,Song X Y,Liu X Y,Yang L J,Pan F,Lv J N.Studies on the removal of tetracycline by multi-walled carbon nanotubes[J].Chemical Engineering Journal,2011,178:26-33.

[22]Dong H R,Jiang Z,Zhang C,Deng J M,Hou K J,Cheng Y J,Zhang L H,Zeng G M.Removal of tetracycline by Fe/Ni bimetallic nanoparticles in aqueous solution[J].Journal of Colloid and Interface Science,2017,513:117-125.

[23]Rathod M,Haldar S,Basha S.Nanocrystalline cellulose for removal of tetracycline hydrochloride from water via biosorption:Equilibrium,kinetic and thermodynamic studies[J].Ecological Engineering,2015,84:240-249.

[24]Huang L H,Liu G F,Dong G H,Wu X Y,Wang C,Liu Y Y.Reaction mechanism of zero-valent iron coupling with microbe to degrade tetracycline in permeable reactive barrier(PRB)[J].Chemical Engineering Journal,2017,316:525-533.

[25]Zhao X,Lv L,Pan B C,Zhang W M,Zhang S J,Zhang Q X.Polymer-supported nanocomposites for environmental application:A review[J].Chemical Engineering Journal,2011,170:381-394.

[26]Lin X C,Xie F,Yu X D,Tang X,Guan H D,Chen Y,Feng W.Ultraviolet light assisted hierarchical porous Fe2O3 catalyzing heterogeneous Fenton degradation of tetracycline under neutral condition with a low requirement of H2O2[J].Chemical Research in Chinese Universities,2019,35(2):304-310.

[27]Gao Y,Li Y,Zhang L,Huang H,Hu J J,Shah S M,Su X G.Adsorption and removal of tetracycline antibiotics from aqueous solution by graphene oxide[J].Journal of Colloid and Interface Science,2012,368:540-546.

[28]Hummers W S,Offeman R.Preparation of graphitic oxide[J].Journal of the American Chemical Society,1958,80:1339-1339.

[29]Lin L,Guo H B,Li Q,Zhang L Q,Liu L L,Yang C L.Determination of tetracyclines residues in aquatic products by HPLC[J].Advanced Materials Research,2014,1004~1005:914-918.

[30]Lu W S,Shen Y H,Xie A J,Zhang W Q.Green synthesis and characterization of superparamagnetic Fe3O4 nanoparticles[J].Journal of Magnetism and Magnetic Materials,2010,322:1828-1833.

[31]Zhang Y L,Guo L,Wei S,He Y Y,Xia H,Chen Q D,Sun H B,Xiao F S.Direct imprinting of microcircuits on graphene oxides film by femtosecond laser reduction[J].Nano Today,2010,5:15-20.

[32]Zhu C Z,Guo S J,Fang Y X,Dong S J.Reducing sugar:New functional molecules for the green synthesis of graphene nanosheets[J].ACS Nano,2010,4:2429-2437.

[33]Fan H T,Liu A J,Jiang B,Wang Q J,Li T,Huang C C.Sampling of dissolved inorganic Sb III by mercapto-functionalized silica-based diffusive gradients in thin-films technique[J].RSC Advances,2016,6(4):2624-2631.

[34]Tian C,Zhao J,Zhang J,Chu S Q,Dang Z,Lin Z,Xing B S.Enhanced removal of roxarsone by Fe3O4@3D graphene nanocomposite:Synergistic adsorption and mechanism[J].Environmental Science:Nano,2017,4:2134-2143.

[35]Ai Y J,Liu Y,Huo Y Z,Zhao C F,Sun L,Han B,Cao X R,Wang X K.Insights into the adsorption mechanism and dynamic behavior of tetracycline antibiotics on reduce graphene oxide (RGO) and graphene oxide (GO) materials[J].Environmental Science:Nano,2019,6:3336-3348.

[36]Jia M Y,Wang F,Bian Y R,Jin X,Song Y,Kengara F O,Xu R K,Jiang X.Effects of p Hand metal ions on oxytetracycline sorption to maize-straw-derived biochar[J].Bioresource Technology,2013,136:87-93.

[37]Ghandour M A,Azab H A,Hassan A.Potentiometric studies on the complexes of tetracycline (TC) and oxytetracyclin (OTC) with some metal ions[J].Monatshefte für Chemie/Chemical Monthly,1992,123:51-58.

[38]Sultan S M,Suliman F E O,Duffuaa S O,Abu-Abdoun I I.Simplex-optimized and flow injection spectrophotometric assay of tetracycline antibiotics in drug formulations[J].Analyst,1992,117:1179-1183.

[39]Shen Q B,Wang Z Y,Yu Q,Cheng Y,Liu Z D,Zhang T P,Zhou S Q.Removal of tetracycline from an aqueous solution using manganese dioxide modified biochar derived from Chinese herbal medicine residues[J].Environmental Research,2020,183:Art no 109195.

[40]成思敏,吴博扬,杨羽斯,沈大辉,杜巍,谢函芮,吴宏海.蒙脱石对盐酸四环素吸附特性的实验研究[J].岩石矿物学杂志,2013,32(6):925-929.

[41]Song Y X,Chen S,You N,Fan H T,Sun L N.Nanocomposites of zero-valent Iron@Activated carbon derived from corn stalk for adsorptive removal of tetracycline antibiotics[J].Chemosphere,2020,255:Art no 126917.

[42]Fan H T,Sun Y,Tang Q,Li W L,Sun T.Selective adsorption of antimony(III) from aqueous solution by ion-imprinted organic-inorganic hybrid sorbent:Kinetics,isotherms and thermodynamics[J].Journal of the Taiwan Institute of Chemical Engineers,2014,45:2640-2648.

基本信息:

DOI:10.16026/j.cnki.iea.2021010076

中图分类号:TQ424;TB332;X703

引用信息:

[1]王晓峰,张爽,刘俊竹,等.Fe_3O_4@还原氧化石墨烯纳米复合材料及其对四环素类抗生素的吸附研究[J].离子交换与吸附,2021,37(01):76-87.DOI:10.16026/j.cnki.iea.2021010076.

基金信息:

辽宁省科技厅博士启动基金指导计划项目(No.20170520285); 辽宁省教育厅青年项目(No.LQ2017004); 沈阳化工大学青年育苗项目(No.XXLQ2019005)

发布时间:

2021-02-20

出版时间:

2021-02-20

检 索 高级检索

引用

GB/T 7714-2015 格式引文
MLA格式引文
APA格式引文