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The Membrane Society of Korea (한국막학회)
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Fabrication and Characterization of Alumina Hollow Fiber Ultrafiltration Membrane

알루미나 중공사 한외여과막 제조 및 특성평가

  • Kim, Yeo-Jin (Membrane Research Center, Advanced Materials Division, Korea Research Institute of Chemical Technology (KRICT)) ;
  • Kim, Seong-Joong (Membrane Research Center, Advanced Materials Division, Korea Research Institute of Chemical Technology (KRICT)) ;
  • Kim, Jeong (Membrane Research Center, Advanced Materials Division, Korea Research Institute of Chemical Technology (KRICT)) ;
  • Cho, Young-Hoon (Membrane Research Center, Advanced Materials Division, Korea Research Institute of Chemical Technology (KRICT)) ;
  • Park, Hosik (Membrane Research Center, Advanced Materials Division, Korea Research Institute of Chemical Technology (KRICT)) ;
  • Lee, Pyung-Soo (Membrane Research Center, Advanced Materials Division, Korea Research Institute of Chemical Technology (KRICT)) ;
  • Park, You-In (Membrane Research Center, Advanced Materials Division, Korea Research Institute of Chemical Technology (KRICT)) ;
  • Park, Ho-Bum (Department of Energy Engineering, Hanyang University) ;
  • Nam, Seung-Eun (Membrane Research Center, Advanced Materials Division, Korea Research Institute of Chemical Technology (KRICT))
  • 김여진 (한국화학연구원 그린화학소재연구본부 분리막연구센터) ;
  • 김성중 (한국화학연구원 그린화학소재연구본부 분리막연구센터) ;
  • 김정 (한국화학연구원 그린화학소재연구본부 분리막연구센터) ;
  • 조영훈 (한국화학연구원 그린화학소재연구본부 분리막연구센터) ;
  • 박호식 (한국화학연구원 그린화학소재연구본부 분리막연구센터) ;
  • 이평수 (한국화학연구원 그린화학소재연구본부 분리막연구센터) ;
  • 박유인 (한국화학연구원 그린화학소재연구본부 분리막연구센터) ;
  • 박호범 (한양대학교 에너지공학과) ;
  • 남승은 (한국화학연구원 그린화학소재연구본부 분리막연구센터)
  • Received : 2017.12.15
  • Accepted : 2018.01.26
  • Published : 2018.02.28
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Abstract

In this study, homogeneous and defect-free ceramic ultrafiltration membranes were fabricated by using the sol-gel method. A boehmite sol was synthesized and coated onto the surface of alumina hollow fiber microfiltration membranes. The effect of sol viscosity and surface tension on the coating layer homogeneity and thickness was investigated. The optimum coating repetition using pristine sol was determined to be 3 times, as the samples coated more than 4 times showed delamination. Fixing the coating repetition to 3 times, the effect of sintering temperature was also studied in this work. The samples sintered at $1000^{\circ}C$ exhibited the highest pure water permeability with the molecular weight cut-off (MWCO) of approximately 51 kDa (10 nm dextran), and the samples sintered at 600, $800^{\circ}C$ displayed the MWCO of 12 kDa (5 nm dextran). The ultrafiltration membranes prepared in this work showed competitive performance compared to the reported ceramic ultrafiltration membranes.

본 연구에서는 sol-gel법을 이용하여 균일하고 결함을 최소화한 세라믹 한외여과막을 제조하였다. 알루미나 중공사 정밀여과막 지지체의 기공 크기를 줄이기 위해, 합성된 boehmite sol과 sol-ethanol 혼합 용액을 사용하여 dip coating법으로 지지체 표면 위에 ${\gamma}$-알루미나 활성층을 형성시켰다. pristine sol을 이용하여 4회 이상 코팅했을 경우 박막층의 두께가 상당히 증가하여 균열 및 박리현상을 야기시키고, 3회 코팅을 진행하였을 경우 표면 결함이 최소화된 최적의 시료를 얻을 수 있었다. 또한, 소결 온도가 ${\gamma}$-알루미나 활성층의 기공 크기에 미치는 영향을 분석하였다. 소결 온도가 $1000^{\circ}C$일 때 가장 높은 순수 투과도 값을 보였으며, 10 nm 크기의 dextran 분획분자량(molecular weight cut-off (MWCO) : 51 kDa)이 관찰되었다. 600, $800^{\circ}C$에서 소결한 막의 경우, 12 kDa MWCO (dextran 5 nm)를 갖는 것으로 확인되었다. 결과적으로, 코팅 용액의 조성은 박막층의 두께에 큰 영향을 주었고, 소결 온도에 따라 분획분자량이 크게 영향을 받는 것을 알 수 있었다.

Keywords

References

  1. R. Nistico, D. Scalarone, and G. Magnacca, "Sol-gel chemistry, templating and spin-coating deposition: A combined approach to control in a simple way the porosity of inorganic thin films/coatings", Microporous and Mesoporous Materials, 248, 18 (2017). https://doi.org/10.1016/j.micromeso.2017.04.017
  2. X. Da, X. Chen, B. Sun, J. Wen, M. Qiu, and Y. Fan, "Preparation of zirconia nanofiltration membranes through an aqueous sol-gel process modified by glycerol for the treatment of wastewater with high salinity", Journal of Membrane Science, 504, 29 (2016). https://doi.org/10.1016/j.memsci.2015.12.068
  3. X. Chen, W. Zhang, Y. Lin, Y. Cai, M. Qiu, and Y. Fan, "Preparation of high-flux $\gamma$-alumina nanofiltration membranes by using a modified sol-gel method", Microporous and Mesoporous Materials, 214, 195 (2015). https://doi.org/10.1016/j.micromeso.2015.04.027
  4. F. Jiang, H. Li, Z. Di, S. Sui, Q. Yu, and J. Zhang, "Silica ultrafiltration membrane with tunable pore size for macromolecule separation", J. Membr. Sci., 441, 25 (2013). https://doi.org/10.1016/j.memsci.2013.04.008
  5. M. Qiu, S. Fan, Y. Cai, Y. Fan, and N. Xu, "Co-sintering synthesis of bi-layer titania ultrafiltration membranes with intermediate layer of sol-coated nanofibers", J. Membr. Sci., 365, 225 (2010). https://doi.org/10.1016/j.memsci.2010.09.005
  6. K. A. Manjumol, P. Shajesh, K. V. Baiju, and K. G. K. Warrier, "An 'Eco-friendly' all aqueous sol gel process for multi functional ultrafiltration membrane on porous tubular alumina substrate", J. Membr. Sci., 375, 134 (2011). https://doi.org/10.1016/j.memsci.2011.03.031
  7. D. Saeki and H. Matsuyama, "Ultrathin and ordered stacking of silica nanoparticles via spin-assisted layer-by-layer assembly under dehydrated conditions for the fabrication of ultrafiltration membranes", J. Membr. Sci., 523, 60 (2017). https://doi.org/10.1016/j.memsci.2016.09.056
  8. B. E. Yoldas, "Alumina gels that form porous transparent $Al_2O_3$", J. Mater. Sci., 10, 1856 (1975).
  9. C. H. Chang, R. Gopalan, and Y. S. Lin, "A comparative study on thermal and hydrothermal stability of alumina, titania and zirconia membranes", J. Membr. Sci., 91, 27 (1994). https://doi.org/10.1016/0376-7388(94)00041-7
  10. J. Livage, "Sol-gel synthesis of heterogeneous catalysts from aqueous solutions", Catalysis Today, 41, 3 (1998). https://doi.org/10.1016/S0920-5861(98)00034-0
  11. M. Bakhshayeshi, A. Teella, H. Zhou, C. Olsen, W. Yuan, and A. L. Zydney, "Development of an optimized dextran retention test for large pore size hollow fiber ultrafiltration membranes", J. Membr. Sci., 421-422, 32 (2012).
  12. J. I. Calvo, R. I. Peinador, V. Thom, T. Schleuss, K. ToVinh, P. Pradanos, and A. Hernandez, "Comparison of pore size distributions from dextran retention tests and liquid-liquid displacement porosimetry", Microporous and Mesoporous Materials, 250, 170 (2017). https://doi.org/10.1016/j.micromeso.2017.05.032
  13. M. Bakhshayeshi, H. Zhou, C. Olsen, W. Yuan, and A. L. Zydney, "Understanding dextran retention data for hollow fiber ultrafiltration membranes", J. Membr. Sci., 385-386, 243 (2011). https://doi.org/10.1016/j.memsci.2011.09.047
  14. G. Vazquez, E. Alvarez, and J. M. Navaza, "Surface tension of alcohol water+ water from 20 to 50. degree. C", Journal of chemical and engineering data, 40, 611 (1995).
  15. R. J. R. Uhlhorn, M. H. B. J. H. I. t. Veld, K. Keizer, and A. J. Burggraaf, "Synthesis of ceramic membranes", J. Mater. Sci., 27, 527 (1992).
  16. H. P. Hsieh, "Inorganic Membranes for Separation and Reaction", Elsevier Science, 58 (1996).
  17. A. F. M. Leenaars, K. Keizer, and A. J. Burggraaf, "The preparation and characterization of alumina membranes with ultra-fine pores", J. Mater. Sci., 19, 1077 (1984). https://doi.org/10.1007/BF01120016
  18. A. Boumaza, L. Favaro, J. Ledion, G. Sattonnay, J. B. Brubach, P. Berthet, A. M. Huntz, P. Roy, and R. Tetot, "Transition alumina phases induced by heat treatment of boehmite: An X-ray diffraction and infrared spectroscopy study", Journal of Solid State Chemistry, 182, 1171 (2009). https://doi.org/10.1016/j.jssc.2009.02.006
  19. Y. S. Lin, K. J. de Vries, and A. J. Burggraaf, "Thermal stability and its improvement of the alumina membrane top-layers prepared by sol-gel methods", J. Mater. Sci., 26, 715 (1991). https://doi.org/10.1007/BF00588309
  20. Z. Dong, W. Jing, and W. Xing, "Triblock polymer template assisted sol-gel process for fabrication of multi-channel $TiO_2/ZrO_2$ ultrafiltration membrane", J. Membr. Sci., 373, 167 (2011). https://doi.org/10.1016/j.memsci.2011.03.001
  21. K. Konig, V. Boffa, B. Buchbjerg, A. Farsi, M. L. Christensen, G. Magnacca, and Y. Yue, "One-step deposition of ultrafiltration SiC membranes on macroporous SiC supports", J. Membr. Sci., 472, 232 (2014). https://doi.org/10.1016/j.memsci.2014.08.058
  22. Z. Wang, Y.-M. Wei, Z.-L. Xu, Y. Cao, Z.-Q. Dong, and X.-L. Shi, "Preparation, characterization and solvent resistance of ${\gamma}-Al_2O_3/{\alpha}-Al_2O_3$ inorganic hollow fiber nanofiltration membrane", J. Membr. Sci., 503, 69 (2016). https://doi.org/10.1016/j.memsci.2015.12.039
  23. X. Ju, P. Huang, N. Xu, and J. Shi, "Influences of sol and phase stability on the structure and performance of mesoporous zirconia membranes", J. Membr. Sci., 166, 41 (2000).