REMOVAL OF Cr (VI) FROM AQUEOUS SOLUTION BY AMINE-FUNCTIONALIZED MCM-41 MODIFIED ULTRAFILTRATION MEMBRANE
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摘要: 采用氨基化MCM-41介孔分子筛（NH2-MCM-41）接枝改性聚偏氟乙烯（PVDF）超滤膜，并用于水中重金属Cr（VI）的去除。NH2-MCM-41成功接枝于超滤膜表面，并在表面形成均匀的亲水层，显著提高了膜的抗污染性能，过水通量衰减率从51.4%降低到了24.8%。在pH值3.5，初始浓度20 mg/L时，改性超滤膜对Cr（VI）的吸附可以在5 min达到快速平衡，吸附容量达到2.8 mg/g。超滤实验表明，NH2-MCM-41改性超滤膜对低浓度Cr（VI）进水可以实现进一步净化，在超滤运行时长达到11 h，出水Cr（VI）浓度始终维持在0.5 mg/L以下。因此，本研究通过在膜表面接枝氨基化的MCM-41分子筛，可以有效提升膜的抗污染能力和对重金属的去除能力。
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关键词:
- 抗污染
Abstract: Amine-functionalized MCM-41 (NH2-MCM-41) modified composite PVDF ultrafiltration (UF) membrane was prepared for removing chromium (VI) in aqueous solution. The porous NH2-MCM-41 nanoparticles formed a symmetrical hydrophilic and adsorptive layer above the thin film which endowed the composite membrane with affinity to chromium (VI). The results showed that the flux attenuation ratio declined from 54.1 to 24.8 % during 1 h filtration experiment with the modified UF membrane compared to the pristine membrane. Static adsorption experiments showed that the maximum adsorption capacity of chromium (VI) on membrane was 2.8 mg/g at initial concentration of 20 mg/l and pH value of 3.5, and temperature of 25oC, and adsorption reached equilibrium within 5 min. The continuous UF experiments demonstrate that the membrane can be used as effective filter medium to purify the water with the chromium concentration less than 0.5 mg/L during 11 h filtration(initial concentration: Cr (VI) = 0.62 mg/L). It is effective to endow the UF with capacity to remove heavy metals, and to enhance its anti-fouling ability by the method reported in the study.-
Keywords:
- anti-fouling
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[1] Weiquan Cai, Lijun Tan, Jiaguo Yu, MietekJaroniec, Xiaoqin Liu, Bei Cheng, Francis Verpoort. Synthesis of amino-functionalized mesoporous alumina with enhanced affinity towards Cr (VI) and CO2[J]. Chemical Engineering Journal, 2014, 239:207-215
[2] LY Li, H Cui, JR Grace. Exploration of remediation of acid rock drainage with clinoptilolite as sorbent in a slurry bubble column for both heavy metal capture and regeneration [J]. Water Research, 2006,40:3359–3366.
[3] O Abollino, Giacomino A, Malandrino M, Mentasti E. Interaction of metal ions with montmorillonite and vermiculite [J]. Applied Clay Science, 2008,38:227-236
[4] Julin Cao, Yunhai Wu, Yanping Jin, Palizhati Yilihan, Wenfu Huang. Response surface methodology approach for optimization of the removal of chromium (VI) by NH2-MCM-41 [J]. Journal of the Taiwan Institute of Chemical Engineers,2014, 45:860-868
[5] Aghdas Heidari, Habibollah Younesi, Zahra Mehraban. Removal of Ni (II), Cd (II), and Pb (II) from a ternary aqueous solution by amino functionalized mesoporous and nano mesoporous silica [J].Chemical Engineering Journal, 2009,153 :70-79
[6] M Shariaty-Niassar A Ghaee, J Barzin, T Matsuura. Effects of chitosan membrane morphology on copper ion adsorption [J]. Chemical Engineering Journal, 2010,165:46-55
[7] E Salehi, S S Madaeni, L Rajabi, V Vatanpour, A A Derakhshan, S Zinadini, S Ghorabi, H Ahmadi Monfared. Novel chitosan/poly(vinyl) alcohol thin adsorptive membranes modified with amino functionalized multi-walled carbon nanotubes for Cu (II) removal from water: Preparation, characterization, adsorption kinetics and thermodynamics [J]. Separation and Purification Technology,2012,89 :309-319
[8] R Jamshidi Gohari, W J Lau, T Matsuur, E Halakoo, A F Ismail. Adsorptive removal of Pb (II) from aqueous solution by novel PES/HMO ultrafiltration mixed matrix membrane [J]. Separation and Purification Technology, 2013,120:59–68
[9] Y Shao, X Wang, Y Kang, Y Shu, Q Sun, L Li. Application of Mn/MCM-41 as an adsorbent to remove methyl blue from aqueous solution [J]. Journal of Colloid Interface Science, 2014,429:25-33
[10] Yunhai Wu, Yanping Jin, Julin Cao,Palizhati Yilihan, Yajun Wen, Jianxin Zhou. Optimizing adsorption of arsenic (III)by NH2-MCM-41 using response surface methodology [J]. Journal of Industrial and Engineering Chemistry, 2014,20:1285-1292
[11] Jun Yin, Eun-Sik Kim, John Yang, Baolin Deng. Fabrication of a novel thin-film nanocomposite (TFN) membrane containing MCM-41 silica nanoparticles (NPs) for water purification [J]. Journal of Membrane Science, 2012,423-424 :238-246
[12] D Rana B J A Tarboush, T Matsuura, H A Arafat, R M Narbaitz. Preparation of thin-film-composite polyamide membranes for desalination using novel hydrophilic surface modifying macromolecules [J]. Journal of Membrane Science, 2008,325 :166-175
[13] Julin Cao，Yunhai Wu, Yanping Jin, PalizhatiYilihan, Wenfu Huang. Response surface methodology approach for optimization of the removal of chromium(VI) by NH2-MCM-41 [J]. Journal of the Taiwan Institute of Chemical Engineers, 2014,45:860-868
[14] Kulamani Parida, Krushna Gopal Mishra, Suresh Kumar Dash. Adsorption of toxic metal ion Cr (VI) from aqueous state by TiO2-MCM-41:Equilibrium and kinetic studies [J]. Journal of Hazardous Materials, 2012,241-242 : 395–403
[15] Hu Tang, Chunyu Chang, Lina Zhang. Efficient adsorption of Hg2+ ions on chitin/cellulose composite membranes prepared via environmentally friendly pathway [J]. Chemical Engineering Journal, 2011,173:689-697
[16] Ye Tian, Min Wu, Ruigang Liu, Yanxiang Li, Deqian Wang, Junjun Tan, Rongcheng Wu, Yong Huang. Electrospun membrane of cellulose acetate for heavy metal ion adsorption in water treatment [J]. Carbohydrate Polymers,2011, 83:743-748
[17] Mohamed Mahmoud Nasef, Abdul Hamid Yahaya. Adsorption of some heavy metal ions from aqueous solutions on Nafion 117 membrane [J]. Desalination, 2009,249:677-681
[18] RajangamVinodh, Rajangam Padmavathi, Dharmalingam Sangeetha. Separation of heavy metals from water samples using anion exchange polymers by adsorption process [J]. Desalination, 2011,267 : 267-276
[1] Weiquan Cai, Lijun Tan, Jiaguo Yu, MietekJaroniec, Xiaoqin Liu, Bei Cheng, Francis Verpoort. Synthesis of amino-functionalized mesoporous alumina with enhanced affinity towards Cr (VI) and CO2[J]. Chemical Engineering Journal, 2014, 239:207-215
[2] LY Li, H Cui, JR Grace. Exploration of remediation of acid rock drainage with clinoptilolite as sorbent in a slurry bubble column for both heavy metal capture and regeneration [J]. Water Research, 2006,40:3359–3366.
[3] O Abollino, Giacomino A, Malandrino M, Mentasti E. Interaction of metal ions with montmorillonite and vermiculite [J]. Applied Clay Science, 2008,38:227-236
[4] Julin Cao, Yunhai Wu, Yanping Jin, Palizhati Yilihan, Wenfu Huang. Response surface methodology approach for optimization of the removal of chromium (VI) by NH2-MCM-41 [J]. Journal of the Taiwan Institute of Chemical Engineers,2014, 45:860-868
[5] Aghdas Heidari, Habibollah Younesi, Zahra Mehraban. Removal of Ni (II), Cd (II), and Pb (II) from a ternary aqueous solution by amino functionalized mesoporous and nano mesoporous silica [J].Chemical Engineering Journal, 2009,153 :70-79
[6] M Shariaty-Niassar A Ghaee, J Barzin, T Matsuura. Effects of chitosan membrane morphology on copper ion adsorption [J]. Chemical Engineering Journal, 2010,165:46-55
[7] E Salehi, S S Madaeni, L Rajabi, V Vatanpour, A A Derakhshan, S Zinadini, S Ghorabi, H Ahmadi Monfared. Novel chitosan/poly(vinyl) alcohol thin adsorptive membranes modified with amino functionalized multi-walled carbon nanotubes for Cu (II) removal from water: Preparation, characterization, adsorption kinetics and thermodynamics [J]. Separation and Purification Technology,2012,89 :309-319
[8] R Jamshidi Gohari, W J Lau, T Matsuur, E Halakoo, A F Ismail. Adsorptive removal of Pb (II) from aqueous solution by novel PES/HMO ultrafiltration mixed matrix membrane [J]. Separation and Purification Technology, 2013,120:59–68
[9] Y Shao, X Wang, Y Kang, Y Shu, Q Sun, L Li. Application of Mn/MCM-41 as an adsorbent to remove methyl blue from aqueous solution [J]. Journal of Colloid Interface Science, 2014,429:25-33
[10] Yunhai Wu, Yanping Jin, Julin Cao,Palizhati Yilihan, Yajun Wen, Jianxin Zhou. Optimizing adsorption of arsenic (III)by NH2-MCM-41 using response surface methodology [J]. Journal of Industrial and Engineering Chemistry, 2014,20:1285-1292
[11] Jun Yin, Eun-Sik Kim, John Yang, Baolin Deng. Fabrication of a novel thin-film nanocomposite (TFN) membrane containing MCM-41 silica nanoparticles (NPs) for water purification [J]. Journal of Membrane Science, 2012,423-424 :238-246
[12] D Rana B J A Tarboush, T Matsuura, H A Arafat, R M Narbaitz. Preparation of thin-film-composite polyamide membranes for desalination using novel hydrophilic surface modifying macromolecules [J]. Journal of Membrane Science, 2008,325 :166-175
[13] Julin Cao，Yunhai Wu, Yanping Jin, PalizhatiYilihan, Wenfu Huang. Response surface methodology approach for optimization of the removal of chromium(VI) by NH2-MCM-41 [J]. Journal of the Taiwan Institute of Chemical Engineers, 2014,45:860-868
[14] Kulamani Parida, Krushna Gopal Mishra, Suresh Kumar Dash. Adsorption of toxic metal ion Cr (VI) from aqueous state by TiO2-MCM-41:Equilibrium and kinetic studies [J]. Journal of Hazardous Materials, 2012,241-242 : 395–403
[15] Hu Tang, Chunyu Chang, Lina Zhang. Efficient adsorption of Hg2+ ions on chitin/cellulose composite membranes prepared via environmentally friendly pathway [J]. Chemical Engineering Journal, 2011,173:689-697
[16] Ye Tian, Min Wu, Ruigang Liu, Yanxiang Li, Deqian Wang, Junjun Tan, Rongcheng Wu, Yong Huang. Electrospun membrane of cellulose acetate for heavy metal ion adsorption in water treatment [J]. Carbohydrate Polymers,2011, 83:743-748
[17] Mohamed Mahmoud Nasef, Abdul Hamid Yahaya. Adsorption of some heavy metal ions from aqueous solutions on Nafion 117 membrane [J]. Desalination, 2009,249:677-681
[18] RajangamVinodh, Rajangam Padmavathi, Dharmalingam Sangeetha. Separation of heavy metals from water samples using anion exchange polymers by adsorption process [J]. Desalination, 2011,267 : 267-276
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