制备方法对GO/P(NIPAM-MA)水凝胶La3+吸附性能的影响

杨新蔚1,2 单国荣1,2 曹志海3 吕挺4 潘鹏举1,2

(1.化学工程联合国家重点实验室浙江大学化学工程与生物工程学院, 浙江杭州 310027)
(2.浙江大学衢州研究院, 浙江衢州 324000)
(3.浙江理工大学先进纺织材料与制备技术教育部重点实验室, 浙江杭州 310018)
(4.杭州电子科技大学材料与环境工程学院, 浙江杭州 310018)

【摘要】用冷冻聚合法和非冷冻聚合法制备了氧化石墨烯/聚(N-异丙基丙烯酰胺-顺丁烯二酸)(GO/P(NIPAM-MA))水凝胶,比较制备方法对GO/P(NIPAM-MA)水凝胶La3+吸附能力的影响,发现通过冷冻聚合法合成的水凝胶,具有更加优异的溶胀-退溶胀性能和吸附性能。NIPAM与MA摩尔比为10∶1的冷冻聚合法水凝胶,在370 mg/L的LaCl3溶液中平衡吸附量为(29.87±0.073)mg/g,而相同条件下的非冷冻聚合法水凝胶平衡吸附量仅为(20.29±0.395)mg/g。冷冻聚合法水凝胶的Freundlich等温线拟合参数n值随着MA含量的增加呈线性增加,而非冷冻聚合法水凝胶增加幅度小于冷冻聚合法。经过5次吸附-解吸循环,冷冻聚合法水凝胶的形状和体积没有明显变化且吸附能力没有明显下降,而非冷冻聚合法水凝胶经过3次吸附-解吸循环就出现破碎,无法再使用。冷冻聚合法合成的GO/P(NIPAM-MA)水凝胶具有La3+平衡吸附量大、可重复使用等优点。

【关键词】 吸附; 脱附; 水凝胶; 冷冻聚合; La3+;

【DOI】

Download this article

    References

    [1] Rabl S, Haas A, Santi D, et al. Ring opening of cis-decalin on bifunctional Ir/-and Pt/La-X zeolite catalysts[J]. Applied Catalysis a General, 2011, 400(1):131-141.

    [2] Wang F C, Zhao J M, Pan F, et al. Adsorption properties toward trivalent rare earths by alginate beads doping with silica[J].Industrial&Engineering Chemistry Research, 2013, 52(9):3453-3461.

    [3] Wilfong W C, Kai B W, Bank T L, et al. Recovering rare earth elements from aqueous solution with porous amine-epoxy networks[J]. ACS Applied Materials&Interfaces, 2017, 9(21):18283-18294.

    [4] Tan Q Y, Li J H, Zeng X L. Rare earth elements recovery from waste fluorescent lamps:a review[J]. Critical Reviews in Environmental Science&Technology, 2015, 45(7):749-776.

    [5] Brioschi L, Steinmann M, Lucot E, et al. Transfer of rare earth elements(REE)from natural soil to plant systems:implications for the environmental availability of anthropogenic REE[J]. Plant and Soil, 2013, 366(1/2):143-163.

    [6] Diniz V, Weber M E, Volesky B, et al. Column biosorption of lanthanum and europium by Sargassum[J]. Water Research, 2008,42(1/2):363-371.

    [7] Zhang S Z, Shan X Q. Speciation of rare earth elements in soil and accumulation by wheat with rare earth fertilizer application[J].Environmental Pollution, 2001, 112(3):395-405.

    [8] Zhu S G, He W Z, Li G M, et al. Recovery of Co and Li from spent lithium-ion batteries by combination method of acid leaching and chemical precipitation[J]. Transactions of Nonferrous Metals Society of China, 2012, 22(9):2274-2281.

    [9] Matlock M M, Howerton B S, Atwood D A. Chemical precipitation of heavy metals from acid mine drainage[J]. Water Research,2002, 36(19):4757-4764.

    [10] Ramakul P, Mooncluen U, Yanachawakul Y, et al. Mass transport modeling and analysis on the mutual separation of lanthanum(Ⅲ)and cerium(Ⅳ)through a hollow fiber supported liquid membrane[J]. Journal of Industrial and Engineering Chemistry, 2012, 18(5):1606-1611.

    [11] Asai S, Watanabe K, Sugo T. Preparation of an extractantimpregnated porous membrane for the high-speed separation of a metal ion[J]. Journal of Chromatography A, 2005, 1094(1/2):158-164.

    [12] Lam K F, Kassab H, Pera-titus M, et al. MCM-41“LUS”:alumina tubular membranes for metal separation in aqueous solution[J]. The Journal of Physical Chemistry C, 2010, 115(1):176-187.

    [13] Chevis D A, Johannesson K H, Burdige D J, et al. Submarine groundwater discharge of rare earth elements to a tidally-mixed estuary in Southern Rhode Island[J]. Chemical Geology, 2015,397:128-142.

    [14] Zhao Z Y, Sun X Q, Dong Y M. Synergistic effect of doped functionalized ionic liquids in silica hybrid material for rare earth adsorption[J]. Industrial&Engineering Chemistry Research,2016, 55(7):2221-2229.

    [15] Ghoul M, Bacquet M, Morcellet M. Uptake of heavy metals from synthetic aqueous solutions using modified PEI-silica gels[J].Water Research, 2003, 37(4):729-734.

    [16] Dragan E S. Design and applications of interpenetrating polymer network hydrogels. A review[J]. Chemical Engineering Journal,2014, 243(5):572-590.

    [17] Demirbilek C, Dinc CÖ. Synthesis of diethylaminoethyl dextran hydrogel and its heavy metal ion adsorption characteristics[J].Carbohydrate Polymers, 2012, 90(2):1159-1167.

    [18] Ma J, Yang M X, Yu F, et al. Water-enhanced removal of ciprofloxacin from water by porous graphene hydrogel[J].Scientific Reports, 2015, 5:13578.

    [19] Kumar R, Jain S K, Verma S, et al. Mercapto functionalized silica entrapped polyacrylamide hydrogel:arsenic adsorption behaviour from aqueous solution[J]. Journal of Colloid and Interface Science,2015, 456:241-245.

    [20] Niyogi S, Bekyarova E, Itkis M E, et al. Solution properties of graphite and graphene[J]. Journal of the American Chemical Society, 2006, 128(24):7720-7721.

    [21] Geng H J. Preparation and characterization of cellulose/N, N'-methylene bisacrylamide/graphene oxide hybrid hydrogels and aerogels[J]. Carbohydrate Polymers, 2018, 196:289-298.

    [22] Lerf A, He H Y, Forster M, et al. Structure of graphite oxide revisited[J]. Journal of Physical Chemistry B, 1998, 102(23):4477-4482.

    [23] Liu M C, Chen C L, Hu J, et al. Synthesis of magnetite/graphene oxide composite and application for cobalt(Ⅱ)removal[J]. Journal of Physical Chemistry C, 2011, 115(51):25234-25240.

    [24] Zhu C H, Lu Y, Peng J, et al. Photothermally sensitive poly(Nisopropylacrylamide)/graphene oxide nanocomposite hydrogels as remote light-controlled liquid microvalves[J]. Advanced Functional Materials, 2012, 22(19):4017-4022.

    [25] Yamashita K, Nishimura T, Ohashi K, et al. Two-step imprinting procedure of inter-penetrating polymer network-type stimuliresponsive hydrogel-adsorbents[J]. Polymer Journal, 2003, 35(7):545-550.

    [26] Zhang X Z, Yang Y Y, Chung T S. Effect of mixed solvents on characteristics of poly(N-isopropylacrylamide)gels[J]. Langmuir,2002, 18(7):2538-2542.

    [27] Kim J H, Lee S L, Kim S J, et al. Rapid temperature/pH response of porous alginate-g-poly(N-isopropylacrylamide)hydrogels[J].Polymer, 2002, 43(26):7549-7558.

    [28] Wu J J, Zhao Q, Sun J Z, et al. Preparation of poly(ethylene glycol)aligned porous cryogels using a unidirectional freezing technique[J]. Soft Matter, 2012, 8(13):3620-3626.

    [29] Wu D B, Gao Y W, Li W J, et al. Selective adsorption of La3+using a tough alginate-clay poly(N-isopropylacrylamide)hydrogel with hierarchical pores and reversible re-deswelling/swelling cycles[J]. ACS Sustainable Chemistry&Engineering, 2016, 4(12):6732-6743.

    [30] Kirsebom H, Mattiasson B. Cryostructuration as a tool for preparing highly porous polymer materials[J]. Polymer Chemistry,2011, 2(5):1059-1062.

    [31] Barrow M, Zhang H F. Aligned porous stimuli-responsive hydrogels via directional freezing and frozen UV initiated polymerization[J]. Soft Matter, 2013, 9(9):2723-2729.

    [32] Cheng C, Zhang X L, Meng Y B, et al. Multiresponsive and biocompatible self-healing hydrogel:its facile synthesis in water,characterization and properties[J]. Soft Matter, 2017, 13(16):3003-3012.

    [33] Liu L, Li L, Qing Y, et al. Mechanically strong and thermosensitive hydrogels reinforced with cellulose nanofibrils[J].Polymer Chemistry, 2016, 7(46):7142-7151.

    [34] Wang E, Desai M S, Lee S W. Light-controlled graphene-elastin composite hydrogel actuators[J]. Nano Letters, 2013, 13(6):2826-2830.

    [35] Xue W, Champ S, Huglin M B, et al. Rapid swelling and deswelling in cryogels of crosslinked poly(N-isopropylacrylamideacrylic acid)[J]. European Polymer Journal, 2004, 40(4):703-712.

    [36] Cheng J J, Shan G R, Pan P J. Temperature and pH-dependent swelling and copper(Ⅱ)adsorption of poly(N-isopropylacrylamide)copolymer hydrogel[J]. RSC Advances, 2015, 5(76):62091-62100.

    [37] Cheng J J, Shan G R, Pan P J. Triple stimuli-responsive Nisopropylacrylamide copolymer toward metal ion recognition and adsorption via a thermally induced sol-gel transition[J]. Industrial&Engineering Chemistry Research, 2017, 56(5):1223-1232.

    [38] Arvidsson P, Plieva F M, Lozinsky V I, et al. Direct chromatographic capture of enzyme from crude homogenate using immobilized metal affinity chromatography on a continuous supermacroporous adsorbent[J]. Journal of Chromatography A,2003, 986(2):275-290.

This Article

ISSN:0438-1157

CN: 11-1946/TQ

Vol 70, No. 10, Pages 4072-4079+3612

October 2019

Downloads:0

Share
Article Outline

摘要

  • 引言
  • 1 实验部分
  • 2 实验结果与讨论
  • 3 结论
  • 符号说明
  • 参考文献