全部 标题 作者
关键词 摘要

OALib Journal期刊
ISSN: 2333-9721
费用:99美元

查看量下载量

相关文章

更多...
-  2019 

Fe3O4@离子印迹聚(St-HPMA-DVB)复合材料的合成及其对水中高氯酸盐选择性吸附
Preparation of Fe3O4@ion imprinted poly(St-HPMA-DVB) magnetic composite and its selective adsorption to perchlorate

DOI: 10.13801/j.cnki.fhclxb.20180530.004

Keywords: 离子印迹聚合物,纳米Fe3O4,磁性复合材料,高氯酸根(ClO4-),选择性吸附
ion imprinted polymer (IIP)
,nano Fe3O4,magnetic composites,perchlorate (ClO4-),selective adsorption

Full-Text   Cite this paper   Add to My Lib

Abstract:

采用超声协助悬浮聚合法以高氯酸根(ClO4-)为模板制备了Fe3O4@离子印迹聚(苯乙烯-3-(2-氨基三乙基四胺)-2-甲基丙烯酸羟丙酯-二乙烯苯)(Fe3O4@ⅡP(St-HPMA-DVB))磁性复合材料,通过TEM、振动样品磁强计(VSM)、TGA、XRD、元素分析(EA)、FTIR等对其进行表征,考察了交联剂DVB用量对材料结构与性能的影响。结果表明:合成的Fe3O4@ⅡP(St-HPMA-DVB)磁性复合材料平均粒径为500~2 000 nm,随DVB用量的增加而增大;磁化强度为9.77~12.78 emu/g,随DVB用量的增加而减小;DVB的加入有利于Fe3O4@ⅡP(St-HPMA-DVB)磁性复合材料的离子印迹空腔的形成和稳定。考察了不同溶液pH值、ClO4-的初始浓度、吸附时间等条件下Fe3O4@ⅡP(St-HPMA-DVB)吸附水中ClO4-的性能,发现溶液pH值能显著影响Fe3O4@ⅡP(St-HPMA-DVB)磁性复合材料对ClO4-的吸附效果,pH为3.0时效果最佳;不同DVB用量Fe3O4@ⅡP(St-HPMA-DVB)磁性复合材料对ClO4-的吸附量和选择性有影响,当DVB用量为0.5 g时,Fe3O4@ⅡP(St-HPMA-DVB)磁性复合材料的吸附量和选择性最佳;吸附机制以离子交换和静电引力为主。等温吸附线符合Langmuir模型,Fe3O4@ⅡP(St-HPMA-DVB)磁性复合材料的饱和吸附量(qm,c=76.9~111.1 mg/g)高于非离子印迹材料Fe3O4@非离子印迹聚(NIP)(St-HPMA-DVB)磁性复合材料(qm,c=62.5 mg/g)。吸附过程可在10 min内达到平衡,符合准二级动力学模型;Fe3O4@ⅡP(St-HPMA-DVB)磁性复合材料能高选择性地有效吸附水中ClO4-,对ClO4-的印迹因子α为1.8,对几种常见共存离子的选择性因子β>5.8,是潜在的高选择性吸附和回收ClO4-的功能材料。 A Fe3O4@ion imprinted poly(Styrene-3-(2-amino triethylenetetramine)-2-hydroxypropyl methacrylate-divinylbenzene) (Fe3O4@ⅡP(St-HPMA-DVB)) magnetic composite was synthesized via ultrasonic assisted suspension polymerization with perchlorate (ClO4-) as the ion imprinting template. The Fe3O4@ⅡP(St-HPMA-DVB) magnetic composite was characterized by TEM, vibrating sample magnetometer (VSM), TGA, XRD, elemental analysis (EA). The effect of the usage amount of crosslinking agent DVB while preparation on the structure and performance of Fe3O4@ⅡP(St-HPMA-DVB) magnetic composite was investigated. The results show that the Fe3O4@ⅡP(St-HPMA-DVB) magnetic composite has an average size of 500-2 000 nm, which increases with the increase of the amount of DVB. The saturation magnetization intensity is 9.77-12.78 emu/g, which decreases with the increase of the amount of DVB. The addition of DVB is beneficial to the formation and stability of the ion imprinted cavity of Fe3O4@ⅡP(St-HPMA-DVB) magnetic composite. The effects of solution pH value, initial concentration of ClO4-, and adsorption time on the adsorption properties of ClO4- in aqueous solutions were investigated. The results show that the adsorption capability is affected significantly by solution pH value and reaches the maximum at pH=3.0. The best adsorption capacity and selectivity of Fe3O4@ⅡP(St-HPMA-DVB) magnetic composite to ClO4- can be obtained when the usage amount of DVB is 0.5 g for synthesis. The adsorption mechanisms may be including both ion exchange and electrostatic interaction. The isothermal adsorption curves mainly obey the Langmuir mode with the maximum adsorption capacity (qm, c=76.9-111.1 mg/g) much higher than that of none-ion imprinted polymer magnetic material

References

[1]  YAO L, YANG L X, CHEN J M, et al. Levels, indoor-outdoor relationships and exposure risks of airborne particle-associated perchlorate and chlorate in two urban areas in Eastern Asia[J]. Chemosphere, 2015, 135:31-37.
[2]  吴春笃, 李顺, 许小红, 等. 高氯酸盐的环境毒理学效应及其机制的研究进展[J]. 环境与健康杂志, 2013, 30(1):85-89. WU C D, LI S, XU X H, et al. Environmental toxicological effect and mechanism of perchlorate[J]. Journal of Environment and Health, 2013, 30(1):85-89(in Chinese).
[3]  刘燕燕, 吴耀国, 晁吉福, 等. 含高氯酸盐废水处理技术的研究进展[J]. 工业水处理, 2010, 30(7):1-4. LIU Y Y, WU Y G, CHAO J F, et al. Research progress in the perchlorate-containing wastewater treatment techniques[J]. Industrial Water Treatment, 2010, 30(7):1-4(in Chinese).
[4]  GAO M C, WANG S, REM Y, et al. Simultaneous removal of perchlorate and nitrate in a combined reactor of sulfur autotrophy and electrochemical hydrogen autotrophy[J]. Chemical Engineering Journal, 2016, 284:1008-1016.
[5]  LIN S Y, CHEN W F, CHENG M T, et al. Investigation of factors that affect cationic surfactant loading on activated carbon and perchlorate adsorption[J]. Colloids and Surfaces A:Physicochemical and Engineering Aspects, 2013, 434:236-242.
[6]  XIE Y H, LI S Y, WANG F, et al. Removal of perchlorate from aqueous solution using protonated cross-linked chitosan[J]. Chemical Engineering Journal, 2010, 156(1):56-63.
[7]  张媛媛, 郭延凯, 张超, 等. 非水溶性醌加速菌GWF生物还原高氯酸盐的研究[J]. 环境科学, 2016, 37(3):988-993. ZHANG Y Y, GUO Y K, ZHANG C, et al. Effect of non-dissolved quinone on perchlorate reduction by strain GWF[J]. Environmental Science, 2016, 37(3):988-993(in Chinese).
[8]  傅骏青, 王晓艳, 李金花, 等. 重金属离子印迹技术[J]. 化学进展, 2016, 28(1):83-90. FU J Q, WANG X Y, LI J H, et al. Ion imprinting technology for heavy metal ions[J]. Progress in Chemistry, 2016, 28(1):83-90(in Chinese).
[9]  GIL R, AMORIM C G, CROMBIE L, et al. Study of a novel bisnaphthalimidopropyl polyamine as electroactive material for perchlorate-selective potentiometric sensors[J]. Electroanalysis, 2015, 27(12):2809-2819.
[10]  CARUSO F, SPASOVA M, MACEIRA V S, et al. Nan engineering of particle surfaces[J]. Advanced Materials, 2001, 13(1):11-22.
[11]  陈君良, 姚屠鹏, 朱宏亮, 等. 巯基功能化纳米Fe3O4磁性高分子复合材料的合成及其对水中亚甲基蓝的吸附作用[J]. 复合材料学报, 2014, 31(2):323-330. CHEN J L, YAO T P, ZHU H L, et al. Preparation of thiol-functionalized nano-Fe3O4-polymer magnetic composite material and its adsorption properties on methylene blue in water[J]. Acta Materiae Compositae Sinica, 2014, 31(2):323-330(in Chinese).
[12]  SHEN H Y, CHEN Z X, LI Z H, et al. Controlled synthesis of 2,4,6-trichlorophenol-imprinted amino-functionalized nano-Fe3O4-polymer magnetic composite for highly selective adsorption[J]. Colloids and Surfaces A:Physicochemical and Engineering Aspects, 2015, 481:439-450.
[13]  李冉冉, 黄昊, 董星龙, 等. 碳包覆磁性镍纳米粒子对亚甲基蓝的吸附性能[J]. 材料研究学报, 2015, 29(9):663-669. LI R R, HUANG H, DONG X L, et al. Adsorption performance of methylene blue onto nanoparticles of carbon-encapsulated magnetic nickel[J]. Chinese Journal of Materials Research, 2015, 29(9):663-669(in Chinese).
[14]  PAN S D, SHEN H Y, XU Q H, et al. Surface mercapto engineered magnetic Fe3O4 nano adsorbent for the removal of mercury from aqueous solutions[J]. Journal of Colloid and Interface Science, 2012, 365(1):204-212.
[15]  ZHANG W, QIN L, HE X W, et al. Novel surface modified molecularly imprinted polymer using acryloyl-β-cyclodextrin and acrylamide as monomers for selective recognition of lysozyme in aqueous solution[J]. Journal of Chromatography A, 2009, 1216(21):4560-4567.
[16]  刘晨, 吕小王, 张少民, 等. 高氯酸红外红外光谱法鉴定爆炸物[J]. 化学推进剂与高分子材料, 2017, 15(1):82-84. LIU C, LV X W, ZHANG S M, et al. Identification of explosives by infrared spectroscopy[J]. Chemical Propellants & Polymeric Materials, 2017, 15(1):82-84(in Chinese).
[17]  WU X M, WANG Y L, XU L L, et al. Removal of perchlorate contaminants by calcined Zn/Al layered double hydroxides:Equilibrium, kinetics, and column studies[J]. Desalination, 2010, 256(1-3):136-140.
[18]  HURLEY K D, SHAPLEY J R. Efficient heterogeneous catalytic reduction of perchlorate in water[J]. Environmental Science and Technology, 2007, 41(6):2044-2049.
[19]  MAHMUDOV R, SHU Y, RYKOV S, et al. The reduction of perchlorate by hydrogenation catalysts[J]. Applied Catalysis B:Environmental, 2008, 81(1-2):78-87.
[20]  SHEN H Y, CHEN J L, DAI H F, et al. New insights into the sorption and detoxification of chromium (VI) by tetraethylenepentamine functionalized nano-sized magnetic polymer adsorbents:Mechanism and pH effect[J]. Industrial & Engineering Chemistry Research, 2013, 52(36):12723-12732.
[21]  FOO K Y, HAMEED B H. Insights into the modeling of adsorption isotherm systems[J]. Chemical Engineering Journal, 2010, 156(1):2-10.
[22]  PRASANNA K, CHRISTOPHER O, INDRARATNE S P, et al. Perchlorate as an emerging contaminant in soil, water and food[J]. Chemosphere, 2016, 150:667.
[23]  CARR J A, MURALI S, HU F, et al. Changes in gastric sodium-iodide symporter (NIS) activity are associated with differences in thyroid gland sensitivity to perchlorate during metamorphosis[J]. General and Comparative Endocrinology, 2015, 219:16-23.
[24]  杨一琼, 白皓, 秦静. 磁性离子交换树脂对饮用水中高氯酸盐的去除效能[J]. 中国给水排水, 2015, 31(21):5-8. YANG Y Q, BAI H, QIN J, et al. Removal efficiency of perchlorate from drinking water by magnetic ion exchange resin[J]. China Water & Wastewater, 2015, 31(21):5-8(in Chinese).
[25]  XIONG Z, ZHAO D Y, PAN G. Rapid and complete destruction of perchlorate in water and ion-exchange brine using stabilized zero-valent iron nanoparticles[J]. Water Research, 2007, 41(15):3497-3505.
[26]  WU D L, HE P, XU X H, et al. The effect of various reaction parameters on bioremediation of perchlorate-contaminated water[J]. Journal of Hazardous Materials, 2008, 150(2):419-423.
[27]  FU J Q, CHEN L X, LI J H, et al. Current status and challenges of ion imprinting[J]. Journal of Materials Chemistry A, 2015, 3:13598-13627.
[28]  SHEN H Y, ZHU Y, WEN X E, et al. Preparation of Fe3O4-C18 nano-magnetic composite materials and their cleanup properties for organophosphorous pesticides[J]. Analytical and Bioanalytical Chemistry, 2007, 387(6):2227-2237.
[29]  王燕, 叶思, 吕珊珊, 等. 磁性Fe3O4@离子印迹聚(MMA-HPMA-DVB)复合材料的合成及其对水中Ni(Ⅱ)选择性吸附[J]. 复合材料学报, 2017, 34(12):2846-2855. WANG Y, YE S, LV S S, et al. Preparation of ion imprinted Fe3O4@ⅡP(MMA-HPMA-DVB) magnetic composite and its selective adsorption to Ni(Ⅱ)[J]. Acta Materiae Compositae Sinica, 2017, 34(12):2846-2855(in Chinese).
[30]  李小倩, 方玲, 张梦南, 等. 地下水中ClO4-浓度测定的分光光度法优化[J]. 环境科学与技术, 2014, 37(12):96-99. LI X Q, FANG L, ZHANG M N, et al. Measurement of perchlorate concentration in groundwater using methylene blue complexation-spectrophotometry[J]. Environmental Science & Technology, 2014, 37(12):96-99(in Chinese).
[31]  LU W S, SHEN Y H, XIE A J, et al. Novel bifunctional one-dimensional Fe3O4/Se nano-composites via facile green synthesis[J]. Journal of Physical Chemistry C, 2010, 114(11):4846-4851.
[32]  赵永纲, 沈昊宇, 茅旗峰, 等. 交联剂用量对氨基功能化纳米Fe3O4磁性高分子材料吸附性能的影响[J]. 科学通报, 2010, 55(12):1099-1106. ZHAO Y G, SHEN H Y, MAO Q F, et al. The effect of the crosslink agent usage amount on the NH2-functionalized nano-Fe3O4 magnetic composites[J]. Chinese Science Bulletin, 2010, 55(12):1099-1106(in Chinese).
[33]  SIMOES M C, HUGHES K J, INGHAM D B, et al. Estimation of the thermochemical radii and ionic volumes of complex ions[J]. Inorganic Chemistry, 2017, 56(13):7566-7573.
[34]  卢宁, 高乃云, 黄鑫. 水中高氯酸根的颗粒活性炭吸附过程及影响因素分析[J]. 环境科学, 2008, 29(6):1572-1577. LU N, GAO N Y, HUANG X. Adsorption of perchlorate in water by granular activated carbon and impact factors analysis[J]. Environmental Science, 2008, 29(6):1572-1577(in Chinese).

Full-Text

Contact Us

service@oalib.com

QQ:3279437679

WhatsApp +8615387084133