Bull. Soc. Sea Water Sci., Jpn., 63, Bulletin of the Society of Sea Water Science, Japan Development of Novel Ion-Exchange Membranes for
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1 Bull. Soc. Sea Water Sci., Jpn., 63, Bulletin of the Society of Sea Water Science, Japan Development of Novel Ion-Exchange Membranes for Electrodialysis of Seawater by Electron-Beam-Induced Graft Polymerization I Selection of Trunk Polymeric Films Kazuyoshi MIYOSHI 1, Tadashi MIYAZAWA 1, Naohiro SATO 1, Daisuke UMENO 1, Kyoichi SAITO 1, Takeshi NAGATANI 2 and Naohito YOSHIKAWA 2 Cation- and anion-exchange membranes were prepared by electron-beam-induced graft polymerization of an epoxy-group-containing vinyl monomer, glycidyl methacrylate, onto trunk polymeric films and subsequent introduction of sulfonic acid and trimethylammonium groups into the epoxy group, respectively. Nine kinds of commercially available polymeric films were used as a trunk polymeric film: low-density and high-density polyethylene LDPE and HDPE, ultra-high-molecular-weight polyethylene UHMW-PE, polyacrylonitrile PAN, polyamide NY, polyethylene terephthalate PET, polyethylene naphthalate PEN, copolymer of ethylene and tetrafluoroethylene ETFE, and copolymer of tetrafluoroethylene and perfluoroalkoethylene PFA. HDPE- and NY-made films were selected as favorable trunk polymeric films according to the grafting rate of GMA and the strength of the resultant GMA-grafted membranes. Small angle X-ray scattering SAXS analysis demonstrated that the distance between the crystalline regions of HDPE increased from 25 to 49 and 38 nm, accompanied by the graft polymerization of GMA and introduction of sulfonic acid and trimethylammonium groups, respectively. Ion-exchange membranes, Seawater, Electrodialysis, Electron-beam-induced graft polymerization, Trunk polymeric films GMA 2 GMA 1-5 GMA LDHD UHMW 3 GMA PAN 6 NY 16 4 PET PEN ETFE PFA 2 1 GMA Department of Applied Chemistry and Biotechnology, Faculty of Engineering, Chiba University, 1-33 Yayoi-cho, Inage-ku, Chiba , Japan Research Institute of Salt and Sea Water Science, the Salt Industry Center of Japan, Sakawa, Odawara-shi, Kanagawa , Japan
2 Polyethylene Trunk polymeric films used in this study Membrane Density thickness m g/cm 3 Suppliers LDPE Okura Industrial, Japan HDPE Tamapoly, Japan UHMWPE Saxin, Japan Polyacrylonitrile PAN Tamapoly, Japan Nylon-6 NY Unitika, Japan Aromatic series PET Tamapoly, Japan PEN Teijin DuPont Films Japan, Japan Fluorine series ETFE PFA Asahi Glass, Japan Abbreviations : LDPE; low-density polyethylene, HDPE; high-density polyethylene, UHMWPE; ultra high molecular weight polyethylene, PAN; polyacrylonitrile, NY; 6-nylon, PET; polyethylene terephthalate, PEN; polyetylene naphthalate, ETFE; copolymer of ethylene and tetrafluoroethylene, PFA; perfluoroalkoxy; copolymer of tetrafluoroethylene and perfluoroalkoxyethylene. Preparation scheme of ion-exchange membranes using electron-beam-induced graft polymerization 12 GMA GMA GMA/ 100 GMA / 100 W 1 W 0 / W 0 1
3 1 W 0 W 1 GMA GMA GMA dg -TP dg TP trunk polymer3 GMA GMA GMA 0.5 M NaCl Na Cl GMA D 1 /D 0 4 D 0 D 1 GMA 100 W w W 2 /W 2 5 / 100 / 18 / / 100 W 2 W 1 / M r / W 1 W 0 / meq/g - dry / W 2 W 1 / M r / W 2 3 W 2 M r NaHSO 3 N CH 3 3 HCl GMA SS dg, x -TP TMA dg, x -TP x GMA LZ-200J W w 18 HDPE X XRD HDPE GMA 98 - SS 97, 80 - TMA 107, 99 -HDPE X SAXS 1.50 cm 5.5 cm 1.77 cm 2 1 cm 433B 0.5 M NaCl 1 khz R m cm 2 R m S 7 S cm 2 Preparation conditions of cation- and anion-exchange membranes 1 Electron-beam irradiation 200 kgy N 2 atmosphere room temperature 2 Graft polymerization of GMA 10 vol% GMA / methanol 40 3 Introduction of ion-exchange groups sulfonic acid group SS : IPA : water = 10 : 15 : 75 wt% 80 trimethylammonium group 0.5 mol-tma/l DMSO : water = 50 : 50 vol% 80 Abbreviations: GMA; glycidyl methacrylate, SS; sodium sulfite, IPA; isopropanol, TMA; trimethylammonium chloride, DMSO; dimethylsulfoxide.
4 M NaCl AGC ASA CSO 8.0 cm cm 1.5 mm 0.50 mol/l NaCl 0.50 mol/l NaCl cm/s 30 ma/cm GMA LDPE, HDPE, UHMWPE PAN, NY PET PEN GMA PEN GMA dg -LDPE GMA dg -PET GMA dg -PAN 2 PAN GMA GMA dg -TP NY UHM- WPE HDPE GMA dg -HDPE -UHMWPE -NY Degree of GMA grafting as a function of reaction time
5 1 GMA HDPE GMA UHMWPE SS dg, x -TP SS 86-90, x -HDPE SS 42-57, x -UHMWPE HDPE UHMWPE Membrane thickness ratio vs. degree of GMA grafting Introduction of trimethylammonium group Introduction of sulfonic acid group Water uptake vs. molar conversion of epoxy group into sulfonic acid group Water uptake vs. molar conversion of epoxy group into trimethylammonium group
6 GMA dg -TP TMA dg, x -TP TMA 47-53, x -HDPE TMA 47-65, x -UHMWPE SS 88, 84 -HDPE TMA 79, 46 -HDPE HDPE nm HDPE GMA 98 - SS 97, 80 - TMA 107, 99 -HDPE SAXS , 33, nm GMA HDPE HDPE Comparison of properies among ion-exchange membranes Water uptake Ion-exchange group density mmol/g dry Number of water molecules per an ion-exchange group SS 88, 84 -HDPE membrane Selemion CSO TMA 79, 46 -HDPE membrane Selemion ASA Changes of polymer structure accompanied by graft polymerization of GMA and introduction of sulfonic acid and trimethylammonium groups
7 1 Chloride ion concentration of brine vs membrane resistance GMA GMA SS dg, x -HDPE SS dg, x -NY ASA Cl a SS dg, x -NY SS dg, x -HDPE Cl TMA dg, 12, x -HDPE TMA dg, 12, x -NY CSO Cl Fig. 9 b TMA dg, x -HDPE 80 Cl SS dg, x -HDPE TMA dg, x -HDPE TMA dg, x -NY Cl TMA dg, x -NY Cl 63 9 GMA GMA Cl 6 1 K. Mashiko, The Salt Manufacturing Technology, Bull. Soc. Sea Water Sci.,, pp Japanese 2 T. Nagatani and N. Yoshikawa, Permeability of Zinc Ions across Ion-Exchange Membrane of Ion-Exchange Electrodialyzer, J. Membr. Sci.,, pp T. Sata, Studies on Ion Exchange Membranes with Permselectivity for Specific Ions in Electrodialysis, J. Membr. Sci.,, pp T. Sata, T. Sata, and W. Yang, Studies on Cation-Exchange Membranes Having Permselectivity Between Cations in Electrodialysis, J. Membr. Sci.,, pp Y. Mizutani, Ion Exchange Membranes with Preferential
8 Permselectivity for Monovalent Ions, J. Membr. Sci.,, pp B. Pilat, Practice of Water Desalination by Electrodialysis, Desalination,, pp H. Riendinger and W. Faul, The Focusing of Membrane R&D on Areas of Commercial Potential, J. Membr. Sci.,, pp N. Yoshikawa, Simulation of the Effect of Developing the High Performance Ion-Exchange Membrane on Reducing the Production Cost in Ion-Exchange Membrane Salt Manufacturing Process, Bull. Soc. Sea Water Sci.,, pp Japanese 9 N. Yoshikawa, and K. Okuyama Simulation to Compare the Production Costs of Several Salt Manufacturing Process, Bull. Soc. Sea Water Sci.,, pp Japanese 10 N. Yoshikawa, and T. Fuchiwaki Present Status and Future Prospects of Research and Development of Salt-Manufacturing Technology, Bull. Soc. Sea Water Sci.,, pp Japanese 11 R. K. Nagarale, G. S. Gohil, and V. K. Shahi, Recent Developments on Ion-Exchange Membranes and Electro-Membrane Processes, Adv. Colloid Interface Sci.,, pp T. Xu, Ion Exchange Membranes: State of Their Development and Perspective, J. Membr. Sci.,, pp M. M. Nasef, and E. A. Hegazy, Preparation and Applications of Ion Exchange Membranes by Radiation-Induced Graft Copolymerization of Polar Monomers onto Non-Polar Films, Prog. Polym. Sci.,, pp S. Tsuneda, K. Saito, H. Mitsuhara, and T. Sugo, Novel Ion-Exchange Membranes for Electrodialysis Prepared by Radiation-Induced Graft Polmerization, J. Electrochem. Soc.,, pp K. Mashiko, K. Ohkubo, and H. Ohtaka, Synthesis of Ion Exchange Membrane by Irradiation Grafting Polymerization, Papers of Sea Water Science Research Laboratory the Salt Industry Center of Japan,, pp Japanese 16 S. M. Kolhe and A. Kumar, Radiation-Induced Grafting of Vinyl Benzyl Trimethyl Ammonium Chloride onto Nylon-6 Fabric, Radiat. Phys. Chem.,, pp Received December 25, 2008, Accepted January 22, 2009 LDHD UHMWPE PAN 6 NY PET PEN ETFE PFAHDPE 6 HDPE NY X SAXS HDPE GMA nm
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