温敏型表面离子印迹聚合物的制备及性能
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摘要
以多壁碳纳米管为(MWCNTs)为基质,N-异丙基丙烯酰胺(NIPAM)为温敏单体,丙烯酰胺、丙烯酸为功能单体,N,N-亚甲基双丙烯酰胺为交联剂,Ni2+为模板,采用反相悬浮法制得温敏型离子印迹材料(IIPs)。采用FTIR、XRD、TG、SEM等对其进行了结构表征,采用丁二酮肟可见分光光度法对印迹聚合物的吸附性能进行了考察。结果表明,通过改变温度可以控制印迹聚合物的吸附与脱附效率,在最佳吸附温度(40℃)下,IIPs对Ni2+最大吸附量为33.80mg/g,该吸附过程符合热力学Langmuir模型和准二级动力学模型,在25℃时脱附效率远大于50℃时脱附效率。在竞争离子Pb2+和Cd2+存在时,Ni2+/Pb2+和Ni2+/Cd2+的选择系数分别为12.62和16.12,说明IIPs具有对Ni2+较强的识别能力。
A novel temperature-sensitive nickel ion imprinted polymer(IIPs) based on multi-walled carbon nanotubes(MWCNTs) was synthesized by inverse suspension method using N-isopropyl acrylamide(NIPAM), acrylamide and acrylic acid as functional monomers, N,N-methylene bis-acrylamide as cross-linker, and Ni(II) as template molecule. The sample was characterized by Fourier transform infrared spectrometer(FTIR), X-ray diffraction(XRD), thermogravimetry(TG) and scanning electron microscopy(SEM). The adsorption properties of the imprinted polymer were investigated by ultraviolet-visible spectrophotometry. The adsorption properties of ion imprinted polymer were investigated by dimethylglyoxime visible spectrophotometry. The results indicated that changing the temperature could control the adsorption and desorption efficiency of imprinted polymer. The maximum adsorption capacity of IIPs to Ni2+ was 33.80 mg/g at the optimum adsorption temperature of 40 ℃. The adsorption isotherm obeyed Langmuir model, and the adsorption kinetics could be represented by pseudo second-order kinetic. The desorption efficiency of IIPs to Ni2+ at 25 ℃ was much greater than that at 50 ℃. In the presence of competitive ions Pb2+ and Cd2+, the selectivity coefficients of Ni2+/Pb2+ and Ni2+/Cd2+ were 12.62 and 16.12, respectively, indicating that IIPs had a strong ability to recognize Ni2+.
A novel temperature-sensitive nickel ion imprinted polymer(IIPs) based on multi-walled carbon nanotubes(MWCNTs) was synthesized by inverse suspension method using N-isopropyl acrylamide(NIPAM), acrylamide and acrylic acid as functional monomers, N,N-methylene bis-acrylamide as cross-linker, and Ni(II) as template molecule. The sample was characterized by Fourier transform infrared spectrometer(FTIR), X-ray diffraction(XRD), thermogravimetry(TG) and scanning electron microscopy(SEM). The adsorption properties of the imprinted polymer were investigated by ultraviolet-visible spectrophotometry. The adsorption properties of ion imprinted polymer were investigated by dimethylglyoxime visible spectrophotometry. The results indicated that changing the temperature could control the adsorption and desorption efficiency of imprinted polymer. The maximum adsorption capacity of IIPs to Ni2+ was 33.80 mg/g at the optimum adsorption temperature of 40 ℃. The adsorption isotherm obeyed Langmuir model, and the adsorption kinetics could be represented by pseudo second-order kinetic. The desorption efficiency of IIPs to Ni2+ at 25 ℃ was much greater than that at 50 ℃. In the presence of competitive ions Pb2+ and Cd2+, the selectivity coefficients of Ni2+/Pb2+ and Ni2+/Cd2+ were 12.62 and 16.12, respectively, indicating that IIPs had a strong ability to recognize Ni2+.
引文
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[29]SongWQ,QianLW.Synthesisofl-phenylalanineimprinted hydrogels with anti-biofouling capability by using a novel zwitterionic functional monomer[J]. Separation&Purification Technology, 2017,182:247-254.
[30]WangJ,WangQM,TianLL,etal.Researchprogressofthe molecularlyimprintedcryogel[J].ChineseJournalofAnalytical Chemistry, 2015, 43(11):1777-1784.
[31]Wang Yujie(王于杰), Jiang Guoqiang(蒋国强), Sun Jiali(孙佳丽),et al. Research development of in situ implant drug delivery based on thermosensitivehydrogel[J].FineChemicals(精细化工),2013,30(1):1-7.
[32]LiuDazhong(刘大中),WangJin(王锦).Physisorptionand chemisorption[J]. Journal of Shandong Institute of Light Industry(齐鲁工业大学学报), 1999, 13(2):22-25.
[33]Yang Zichun(杨紫淳), Gao Yunling(高云玲), Yao Kejian(姚克俭).Temperature-sensitive molecularly imprinted hydrogels[J]. Chemical Industry&Engineering Progress(化工进展), 2014, 33(1):117-123.
[2]Guo N, Su S J, Liao B, et al. Preparation and properties of a novel macroporousNi2+-imprintedchitosanfoamadsorbentsfor adsorptionofnickelionsfromaqueoussolution[J].Carbohydrate Polymers, 2017, 165:376-383.
[3]RahangdaleD,KumarA.Acrylamidegraftedchitosanbasedion imprintedpolymerfortherecoveryofcadmiumfromnickelcadmiumbatterywaste[J].JournalofEnvironmentalChemical Engineering, 2018, 6(2):1828-1839.
[4]Abbasi S, Roushani M, Khani H, et al. Synthesis and application of ion-imprinted polymer nanoparticles for the determination of nickel ions[J].SpectrochimicaActa,PartA:Molecular&Biomolecular Spectroscopy, 2015, 140(5):534-543.
[5]Shang Hongzhou(尚宏周), He Junnan(何俊男), Zhao Jingdong(赵敬东),etal.Preparationandpropertiesofmulti-walledcarbon nanotubesandchitosanself-assembledionimprintedpolymers[J].Fine Chemicals(精细化工), 2016, 34(10):1213-1218.
[6]Shang Hongzhou(尚宏周), Zhao Jingdong(赵敬东), He Junnan(何俊男), et al. Absorption properties of Cd2+ion imprinted poly(fulvic acid)[J]. CIESC Journal(化工学报), 2017, 68(5):1940-1945.
[7]LuoX,LiuL,DengF,etal.Novelion-imprintedpolymerusing crown ether as a functional monomer for selective removal of Pb(Ⅱ)ionsinrealenvironmentalwatersamples[J].JournalofMaterials Chemistry A, 2013, 1(28):8280-8286.
[8]Luo X, Luo S, Zhan Y, et al. Novel Cu(Ⅱ)magnetic ion imprinted materials prepared by surface imprinted technique combined with a sol-gelprocess[J].JournalofHazardousMaterials,2011,192(3):949-955.
[9]GaoB,MengJ,XuY,etal.PreparationofFe(Ⅲ)ion surface-imprintedmaterialforremovingFe(Ⅲ)impurityfrom lanthanideionsolutions[J].JournalofIndustrial&Engineering Chemistry, 2015, 24(4):351-358.
[10]Wang J, Han Y, Li J, et al. Selective adsorption of thiocyanate anions usingstrawsupportedionimprintedpolymerpreparedbysurface imprintingtechniquecombinedwithRAFTpolymerization[J].Separation&Purification Technology, 2017, 177:62-70.
[11]Li M, Meng X, Li B, et al. A novel In(Ⅲ)ion-imprinted polymer(IIP)forselectiveextractionofIn(Ⅲ)ionsfromaqueous solutions[J]. Hydrometallurgy, 2018, 176:243-252.
[12]ShakerianF,KimKH,KwonE,etal.Advancedpolymeric materials:Synthesisandanalyticalapplicationofionimprinted polymersasselectivesorbentsforsolidphaseextractionofmetal ions[J]. Trends in Analytical Chemistry, 2016, 83:55-69.
[13]Liu H, Kong D, Sun W, et al. Effect of anions on the polymerization andadsorptionprocessesofCu(Ⅱ)ion-imprintedpolymers[J].Chemical Engineering Journal, 2016, 303:348-358.
[14]He J N, Shang H Z, Zhang X, et al. Synthesis and application of ion imprinting polymer coated magnetic multi-walled carbon nanotubes forselectiveadsorptionofnickelion[J].AppliedSurfaceScience,2018, 428:110-117.
[15]TaghizadehM,HassanpourS.SelectiveadsorptionofCr(Ⅵ)ions from aqueous solutions using a Cr(Ⅵ)-imprinted polymer supported bymagneticmultiwallcarbonnanotubes[J].Polymer,2017,132:1-11.
[16]Fayazi M, Taher M A, Afzali D, et al. Synthesis and application of novelion-imprintedpolymercoatedmagneticmulti-walledcarbon nanotubesforselectivesolidphaseextractionoflead(Ⅱ)ions[J].Materials Science&Engineering C, 2016, 60:365-373.
[17]Usman I B, Matsoso B, Ranganathan K, et al. Magnetic properties of alignedironcontainingnitrogen-dopedmulti-walledcarbon nanotubes[J]. Materials Chemistry&Physics, 2018, 209:280-290.
[18]RybakA,RybakA,KaszuwaraW,etal.Poly(2,6-dimethyl-1,4-phenyleneoxide)hybridmembranesfilledwithmagnetically alignediron-encapsulatedcarbonnanotubes(Fe@MWCNTs)for enhanced air separation[J]. Diamond&Related Materials, 2018, 83:21-29.
[19]Ma Licheng(马立成), Zheng Qi(郑其), Che Xiaokui(车小奎), et al.CharacterizationandpropertiesofCu2+ion-imprintedmagnetic chitosan beads and their Cu2+adsorption performance[J]. Journal of Chemical Engineering of Chinese Universities(高校化学工程学报),2016, 30(1):174-181.
[20]Wang Z, Wu J, Zhao P, et al. Improving cracking resistance of cement mortarbythermo-sensitivepolyN-isopropylacrylamide(PNIPAM)gels[J]. Journal of Cleaner Production, 2018, 176:1292-1303.
[21]YarinAL,AgarwalS.Bucklingandunravelingpoly(N-isopropyl acrylamide)-thermoplasticpolyurethanebilayers[J].Polymer,2016,97:604-613.
[22]ErmatchkovV,NinniL,MaurerG.Thermodynamicsofphase equilibriumforsystemscontainingN-isopropylacrylamide hydrogels[J]. Fluid Phase Equilibria, 2010, 296(2):140-148.
[23]NistorMT,ChiriacAP,NitaLE,etal.Characterizationofthe semi-interpenetratednetworkbasedoncollagenandpoly(Nisopropylacrylamide-co-diethylene glycol diacrylate)[J]. International Journal of Pharmaceutics, 2013, 452(1/2):92-101.
[24]CugginoJC,StrumiaMC,IgarzabalCIA.Synthesis,characterizationandslowdrugdeliveryofhydrogelsbasedin N-acryloyl-tris-(hydroxymethyl)aminomethaneandN-isopropyl acrylamide[J].Reactive&FunctionalPolymers,2011,71(4):440-446.
[25]NistorMT,PamfilD,SchickC,etal.Studyoftheheat-induced denaturation and water state of hybrid hydrogels based on collagen andpoly(N-isopropylacrylamide)inhydratedconditions[J].Thermochimica Acta, 2014, 589(10):114-122.
[26]GuptaB,MishraS,SaxenaS.Preparationofthermosensitive membranesbyradiationgraftingofacrylicacid/N-isopropyl acrylamidebinarymixtureonPETfabric[J].RadiationPhysics&Chemistry, 2008, 77(5):553-560.
[27]LuJ,WuY,LinX,etal.Anti-foulingandthermosensitive ion-imprinted nanocomposite membranes based on grapheme oxide andsilicondioxideforselectivelyseparatingeuropiumions[J].Journal of Hazardous Materials, 2018, 353:244-253.
[28]Lin X H, Aik S X L, Angkasa J, et al. Selective and sensitive sensors basedonmolecularlyimprintedpoly(vinylidenefluoride)for determinationofpesticidesandchemicalthreatagentsimulants[J].Sensors&Actuators B Chemical, 2018, 258:228-237.
[29]SongWQ,QianLW.Synthesisofl-phenylalanineimprinted hydrogels with anti-biofouling capability by using a novel zwitterionic functional monomer[J]. Separation&Purification Technology, 2017,182:247-254.
[30]WangJ,WangQM,TianLL,etal.Researchprogressofthe molecularlyimprintedcryogel[J].ChineseJournalofAnalytical Chemistry, 2015, 43(11):1777-1784.
[31]Wang Yujie(王于杰), Jiang Guoqiang(蒋国强), Sun Jiali(孙佳丽),et al. Research development of in situ implant drug delivery based on thermosensitivehydrogel[J].FineChemicals(精细化工),2013,30(1):1-7.
[32]LiuDazhong(刘大中),WangJin(王锦).Physisorptionand chemisorption[J]. Journal of Shandong Institute of Light Industry(齐鲁工业大学学报), 1999, 13(2):22-25.
[33]Yang Zichun(杨紫淳), Gao Yunling(高云玲), Yao Kejian(姚克俭).Temperature-sensitive molecularly imprinted hydrogels[J]. Chemical Industry&Engineering Progress(化工进展), 2014, 33(1):117-123.
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