Stability of a Silica Membrane in the HI-$H_2O$ Gaseous Mixture

HI-$H_2O$ 기상 혼합물에서 Silica 막의 안정성

  • 황갑진 (한국에너지기술연구원 수소에너지연구센터) ;
  • 박주식 (한국에너지기술연구원 수소에너지연구센터) ;
  • 이상호 (한국에너지기술연구원 수소에너지연구센터) ;
  • 최호상 (경일대학교 화학공학과)
  • Published : 2004.09.01

Abstract

The stability of the prepared silica membrane by chemical vapor deposition (CVD) method in the HI-$H_2O$ gaseous mixture was evaluated aiming at the application for hydrogen iodide decomposition in the thermochemical IS process. Porous $\alpha$-alumina having pore size of 100 nm was modified by the different CVD temperature using tetraethoxysilane as the Si source. The CVD temperature was $700^{\circ}C$, $650^{\circ}C$, and $600^{\circ}C$. The $H_2$/H$_2$ selectivities of the modified membranes which were measured by single-component permeation experiment showed 43.2, 12.6, and 8.7 at $600^{\circ}C$ for the M1 (CVD temperature was $700^{\circ}C$), M2 (CVD temperature was $650^{\circ}C$) and M3 membranes (CVD temperature was $600^{\circ}C$), respectively. Stability experiment in the HI-$H_2O$ gaseous mixture was carried out at $450^{\circ}C$. The prepared silica membrane at $600^{\circ}C$ of CVD temperature was more stable than that at the other CVD temperature.

열화학적 IS 공정에서 요오드화수소의 분해에 적용하기 위하여 화학증착법(CVD)으로 제조된 silica 막의 안정성을 HI-$H_2O$ 기상 혼합물에서 평가하였다. Si 원천으로 tetraethoxysilane을 사용하여 서로 다른 CVD 온도로 기공크기가 100 nm인 $\alpha$-alumina를 처리하였다. CVD온도는 $700^{\circ}C$, $650^{\circ}C$, $600^{\circ}C$이었다. $600^{\circ}C$에서 수행한 단일 성분의 투과 실험에서 측정한 막의 $H_2$/$N_2$ 선택도는 CVD 온도 $700^{\circ}C$의 M1 막은 43.2, $650^{\circ}C$의 M2 막은 12.6, $600^{\circ}C$의 M3 막은 8.7을 나타내었다. HI-$H_2O$ 기상 혼합물에서 안정성 실험은 $450^{\circ}C$에서 수행하였는데, CVD 온도 $650^{\circ}C$에서 처리된 막이 다른 온도에서 처리된 막보다 더 안정성이 더 좋은 결과를 얻었다.

Keywords

References

  1. H. Nakajima, K. Ikenoya, K. Onuki, and S. Shimizu, 'Closed cycle continuous hydrogen production test by themochemical IS process', Kagaku Kougaku Ronbunshu, 24(2), 352 (1998)
  2. G.-J. Hwang, K. Onuki, S. Shimizu, and H. Ohya, 'Hydrogen separation in $H_2-H_2O$-HI gaseous mixture using the silica membranes prepared by chemical vapor deposition', J. Memb. Sci., 162, 83 (1999)
  3. G.-J. Hwang, K. Onuki, and S. Shimizu, 'Studies on hydrogen separation membrane for IS process Membrane preparation with porous a-alumina tube', JAERI, Research Rep. 98 002, JAERI, Ibaraki, Japan (1998)
  4. G.-J. Hwang, K. Onuki, and S. Shimizu, 'Separation of Hydrogen from $H_2-H_2O$-HI gaseous mixture using a silica membrane', AIChE. J., 46(1), 92 (2000)
  5. G.-J. Hwang and K. Onuki, 'Simulation study on the catalytic decomposition of hydrogen iodide in a membrane reactor with a silica membrane for the thermochemical water splitting IS process', J. Memb. Sci., 194, 207 (2001)
  6. G.-J. Hwang, J.-W. Kim, H.-S. Choi, and K. Onuki, 'Stability of a silica membrane prepared by CVD using $\gamma$- and $\alpha$-alumina tube as the support tube in the HI-$H_2O$ gaseous mixture', J. Memb. Sci., 215, 293 (2003)
  7. S. W. Nam and G. R. Gavalas, 'Stability of $H_2$ pennselective $SiO_2$ films formed by chemical vapor deposition', AIChE Symp. Ser., 85(268), 68 (1989)
  8. G. R. Gallaher and P. K. T. Liu, 'Characterization of ceramic membranes I. Thermal an hydrothermal stabilities of commercial 40 membranes', J. Memb. Sci., 92, 29 (1994)
  9. H. Y. Ha, S. W. Nam, S.-A. Hong, and W. K. Lee, 'Chemical vapor deposition of hydrogen permselective silica film on porous glass supports from tetraethylorthosilicate', J. Memb. Sci., 85, 279 (1993)
  10. J. C. S. Wu, H. Sabol, G. W. Smith, D. L. Flowers, and P. K. T Liu, 'Characterization of hydrogen permselective microporous ceramic membranes', J. Memb. Sci., 96, 275 (1994)
  11. S. Yan, H. Maeda, K. Kusakabe, and S. Morooka, 'Hydrogen permselective $SiO_2$ membrane formed in pores of alumina support tube by chemical vapor deposition with tetraethylorthosilicate', Ind. Eng. Chem. Res., 33, 2096 (1994)
  12. M. Tsapatis and G. Gavalas, 'Structure and aging characteristics of $H_2$ permselective $SiO_2$ vycor membranes', J. Memb. Sci., 87, 281 (1994)
  13. S. Kim and G. R. Gavalas, 'Preparation of $H_2$ permselective silica membranes by alternating reactant vapor deposition', Ind. Eng. Chem. Res., 34, 168 (1995)
  14. G. Xomeritakis and Y. S. Lin, 'Fabrication of a thin palladium membrane supported in a porous ceramic substrate by chemical vapor deposition', J. Memb. Sci., 120, 261 (1996)
  15. S. Morooka, S. S. Kim, S. Yan, K. Kusakabe, and M. Watanabe, 'Separation of hydrogen from an $H_2-H_2O$-HBr system with an $SiO_2$ membrane formed in macropores of an $\alpha$-alumina support tube', Int. J. Hydrogen Energy, 21(3), 183 (1996)
  16. F. S. Becker, D. P awlik, H. Schafer, and G. Staudigl, 'Process and film characterization of low pressure tetraethylorthosilicate borophosphosilicate glass', J. Vac. Sci. Technol. B, 4(3), 732 (1986)