Preparation of Silica Particles by Emulsion-Gel Process Using Membrane Emulsification

막유화 에멀젼-겔 공정에 의한 실리카 입자의 제조

  • Yeon, Song-Hee (Department of Industrial Engineering Chemistry, College of Engineering, Chungbuk National University) ;
  • Youm, Kyung-Ho (Department of Industrial Engineering Chemistry, College of Engineering, Chungbuk National University)
  • 연송희 (충북대학교 공과대학 공업화학과) ;
  • 염경호 (충북대학교 공과대학 공업화학과)
  • Received : 2010.05.30
  • Accepted : 2010.06.14
  • Published : 2010.06.30

Abstract

We prepared spherical silica particles by controlling various conditions of emulsion-gel procedure using a lab-scale membrane emulsification system equipped with SPG (Shirasu porous glass) membrane having pore size of 2.6 ${\mu}m$. We determined the effects of process parameters of membrane emulsification (dispersed phase pressure, stabilizer and emulsifier concentration in continuous phase, $H_2O$/TEOS ratio, ratio of dispersed phase to continuous phase) on the mean size and size distribution of silica particles. The increase of the dispersed phase pressure and ratio of dispersed phase to continuous phase led to the increase in the mean size of silica particles. On the contrary, the increase in stabilizer and emulsifier concentration and $H_2O$/TEOS ratio caused the reduction of the mean size of particles. Through controlling these parameters, monodisperse spherical silica particles with about 3 ${\mu}m$ of the mean size were finally prepared.

세공 크기가 2.6 ${\mu}m$인 SPG (Shirasu porous glass) 막이 설치된 실험실 규모의 막유화 장치를 사용하여 막유화 에멀젼-겔 공정의 변수 조절을 통해 구형상의 실리카 입자를 제조하였다. 막유화 에멀젼-겔 공정의 변수로는 분산상 압력, 연속상 내 안정제 및 유화제의 농도, $H_2O$/TEOS 비율 및 연속상에 대한 분산상의 비율로 설정하고, 이들 변수가 제조된 실리카 입자의 크기와 분포에 미치는 영향을 검토하였다. 막유화의 공정변수들 중에서 분산상 압력과 연속상에 대한 분산상의 비가 증가할수록 실리카 입자의 크기가 증가하였다. 반면 안정제 및 유화제의 농도, $H_2O$/TEOS 비가 증가할수록 입자의 크기가 감소하였다. 막유화 에멀젼-겔 공정변수의 조절을 통해 최종적으로 평균 입자 크기가 3 ${\mu}m$인 비교적 입도분포가 균일한 구형상의 실리카 입자 제조가 가능하였다.

Keywords

Acknowledgement

Supported by : 충북대학교

References

  1. J. H. Park, S. C. Chung, C. Oh, S. I. Shin, S. S. Im, and S. G. Oh, "Preparation and size control of spherical silica particles using W/O emulsion", J. Korean Ind Eng. Chem., 13, 502 (2002).
  2. W. Stober, A. Fink, and E. Bohn, "Controlled growth of monodisperse silica spheres in the micron size range", J. Colloid Interface Sci., 26, 62 (1968). https://doi.org/10.1016/0021-9797(68)90272-5
  3. G. H. Bogush, M. A. Tracy, and C. F. Zukoski, "Preparation of monodisperse silica particles: Control of size and mass fraction", J. Non-Cryst. Solids, 104, 95 (1988). https://doi.org/10.1016/0022-3093(88)90187-1
  4. J. L. Look, G. H. Bogush, and C. F. Zukoski, "Colloidal interactions during the precipitation of uniform submicrometre particles", Faraday Discuss. Chem. Soc., 90, 345 (1990). https://doi.org/10.1039/dc9909000345
  5. A. van Blaaderen and A. Vrij, "Synthesis and characterization of monodispcrse colloidal organosilica spheres", J. Colloid Interface Sci., 156, 1(1993). https://doi.org/10.1006/jcis.1993.1073
  6. T. B. Kang, H. K. Lee, and Y. T. Lee, "Preparation of microporous silica membrane from TEOS-$H_2O$ system and separation of $H_2-N_2$ gas mixture", Membrane Journal, 10, 55 (2000).
  7. Y. Yoshino, T. Suzuki, B.N. Nair, H. Taguchi, and N. Itoh, "Development of tubular substrates, silica based membranes and membrane modules for hydrogen separation at high temperature", J. Membr. Sci., 267, 8 (2005). https://doi.org/10.1016/j.memsci.2005.05.020
  8. S. L. Hong and T. B. Kang, "Separation of gas based on PTMSP-silica-PEI composites", Membrane Journal, 16, 123 (2006).
  9. G. Y. Choi, H. H. Han, and Y. T. Lee, "Preparation of nanoporous ceramic membranes by sol-gel method and characterization of gas permeation", Membrane Journal, 18, 176 (2008).
  10. R. Lindberg, J. Sjoblom, and G. Sundholm, "Preparation of silica particles utilizing the sol-gel and the emulsion-gel processes", Colloids & Surfaces A: Physicochem. Eng. Aspects, 99, 79 (1995). https://doi.org/10.1016/0927-7757(95)03117-V
  11. T. H. Kim and J. C. Lim, "Effect of cosurfactant on preparation of silica nanoparticles using water in oil microemulsion of nonionic surfactant", Korean Chem. Eng. Res., 46, 356 (2008).
  12. E. Kakazu, T. Murakami, K. Akamatsu, T. Sugawara, R. Kikuchi, and S.I. Nakao, "Preparation of silver nanoparticles using SPG membrane emulsification", J. Membr. Sci., 354, 1 (2010). https://doi.org/10.1016/j.memsci.2010.02.056
  13. T. Nakashima and M. Shimizu, "Preparation of monodisperscd O/W emulsion by porous glass membrane", Kagaku Kogaku Ronbunshu, 19, 984 (1993). https://doi.org/10.1252/kakoronbunshu.19.984
  14. G. T. Vladisavljevic and R. A. Williams, "Recent development in manufacturing emulsions and particulate products using membranes", Advances in Colloid & Interface Sci., 113, 1 (2005). https://doi.org/10.1016/j.cis.2004.10.002
  15. H. J. Lee and J. H. Kim, "Preparation of the large size polybutadiene latexes by membrane emulsification process", Membrane Journal, 6, 166 (1996).
  16. R. Katoh, Y. Asano, A. Furuya, K. Sotoyama, and M. Tomita, "Preparation of food emulsions using a membrane emulsification system", J. Membr. Sci., 113, 131 (1996). https://doi.org/10.1016/0376-7388(95)00227-8
  17. S. M. Joscelyne and G. Tragardh, "Membrane emulsification-A literature review", J. Membr. Sci., 169, 107 (2000). https://doi.org/10.1016/S0376-7388(99)00334-8
  18. S. Omi, K. Katami, A. Yamamoto, and M. Iso, "Synthesis of polymeric microspheres employing SPG emulsification technique", J. Appl. Polymer Sci., 51, 1 (1994). https://doi.org/10.1002/app.1994.070510101
  19. T. Nakashima, M. Shimizu, and M. Kukizaki, "Membrane emulsification by microporous glass", Key Engineering Materials, 61-62, 513 (1991).
  20. G. H. Ma, M. Nagai, and S. Omi, "Preparation of uniform poly(lacide) microsphers by employing the shirasu porous glass (SPG) emulsification technique", Colloids & Surfaces A: Physicochem. Eng. Aspects, 153, 383 (1999). https://doi.org/10.1016/S0927-7757(98)00460-9
  21. S. Nagashima, M. Koide, S. Ando, K. Makino, T. Tsukamoto, and H. Ohshima, "Surface properties of monodispers poly(acrylamide-co-acrylic acid) hydrogel microsphers prepared by a membrane emulsification technique" , Colloids & Surface A: Physicochem. Eng. Aspects, 153, 221 (1999). https://doi.org/10.1016/S0927-7757(98)00446-4
  22. S. van der Graaf, C. G. P. H. Schroen, and R. M. Boom, "Preparation of double emulsions by membrane emulsification-A review", J. Membr. Sci., 251, 7 (2005). https://doi.org/10.1016/j.memsci.2004.12.013
  23. T. Nakashima, M. Shimizu, and M. Kukizaki, "Particle control of emulsion by membrane emulsification and its applications", Advan. Drug Delivery Reviews, 45, 47 (2000). https://doi.org/10.1016/S0169-409X(00)00099-5
  24. K. Kandori, K. Kishi, and T. Ishikawa, "Preparation of uniform silica hydrogel particles by SPG filter emulsification method", Colloids & Surfaces, 62, 259 (1992) https://doi.org/10.1016/0166-6622(92)80009-Q
  25. T. Yanagishita, Y. Tomabechi, K. Nishio, and H. Masuda, "Preparation of monodisperse $SiO_2$ nanoparticles by membrane emulsification using ideally ordered anodic porous alumina", Langmuir, 20, 554 (2004). https://doi.org/10.1021/la030314a
  26. N. S. Kwak and K. H. Youm, "Preparation of silica microgels using membrane emulsification method", Membrane Journal, 19, 122 (2009).
  27. Y. H. Choi, D. E. Wiley, and K. H. Youm, "Preparation of alginate microspheres using membrane emulsification method", Membrane Journal, 14, 218 (2004).