Permeation properties of silica-zirconia composite membranes supported on porous alumina substrates

So Jin Ahn, Atsushi Takagaki, Takashi Sugawara, Ryuji Kikuchi, S. Ted Oyama

Research output: Contribution to journalArticle

15 Citations (Scopus)

Abstract

A hydrogen-selective silica-zirconia composite membrane was prepared on a macroporous alumina support by chemical vapor deposition of tetraethylorthosilicate (TEOS) and zirconium (IV) tert-butoxide (ZTB) at 923 K. The resulting membrane had a high H2permeance of 3.8×10−7 mol m−2 s−1 Pa−1with selectivities over CO2, N2and CH4of 1100, 1400 and 3700, respectively. Studies of the temperature dependence of the permeance of He, H2, and Ne demonstrated that the permeation mechanism was similar to that of dense silica membranes, involving solid-state diffusion with jumps of the permeating species between solubility sites. Parameters such as the site density, jump distance, and jump frequency were calculated and were physically plausible, and varied in reasonable manner with the mass and size of He, H2, and Ne. An alternative mechanism involving an activated gas translational mechanism was shown to fit the data but to give physically unrealistic parameters. The silica-zirconia membrane showed hydrothermal stability over a limited testing period of 48 h. After exposure to 16 mol% water vapor at 923 K for 48 h, a pure silica membrane showed a 68% decline with a H2permeance of 4.5×10−8 mol m−2 s−1 Pa−1and a H2over N2selectivity of 800, both of which continued to deteriorate. In comparison, a 10% ZrO2-SiO2membrane showed a decline of 56% but to a level of 10−7 mol m−2 s−1 Pa−1with a H2over N2selectivity of 5700. Importantly, the deterioration largely stabilized at that permeance level.

Original languageEnglish
Pages (from-to)409-416
Number of pages8
JournalJournal of Membrane Science
Volume526
DOIs
Publication statusPublished - Jan 1 2017

Fingerprint

Aluminum Oxide
Composite membranes
zirconium oxides
Permeation
Silicon Dioxide
Zirconia
Alumina
aluminum oxides
Silica
silicon dioxide
membranes
Membranes
composite materials
Substrates
permeating
Steam
Zirconium
Water vapor
Deterioration
Hydrogen

All Science Journal Classification (ASJC) codes

  • Biochemistry
  • Materials Science(all)
  • Physical and Theoretical Chemistry
  • Filtration and Separation

Cite this

Permeation properties of silica-zirconia composite membranes supported on porous alumina substrates. / Ahn, So Jin; Takagaki, Atsushi; Sugawara, Takashi; Kikuchi, Ryuji; Oyama, S. Ted.

In: Journal of Membrane Science, Vol. 526, 01.01.2017, p. 409-416.

Research output: Contribution to journalArticle

Ahn, So Jin ; Takagaki, Atsushi ; Sugawara, Takashi ; Kikuchi, Ryuji ; Oyama, S. Ted. / Permeation properties of silica-zirconia composite membranes supported on porous alumina substrates. In: Journal of Membrane Science. 2017 ; Vol. 526. pp. 409-416.
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abstract = "A hydrogen-selective silica-zirconia composite membrane was prepared on a macroporous alumina support by chemical vapor deposition of tetraethylorthosilicate (TEOS) and zirconium (IV) tert-butoxide (ZTB) at 923 K. The resulting membrane had a high H2permeance of 3.8×10−7 mol m−2 s−1 Pa−1with selectivities over CO2, N2and CH4of 1100, 1400 and 3700, respectively. Studies of the temperature dependence of the permeance of He, H2, and Ne demonstrated that the permeation mechanism was similar to that of dense silica membranes, involving solid-state diffusion with jumps of the permeating species between solubility sites. Parameters such as the site density, jump distance, and jump frequency were calculated and were physically plausible, and varied in reasonable manner with the mass and size of He, H2, and Ne. An alternative mechanism involving an activated gas translational mechanism was shown to fit the data but to give physically unrealistic parameters. The silica-zirconia membrane showed hydrothermal stability over a limited testing period of 48 h. After exposure to 16 mol{\%} water vapor at 923 K for 48 h, a pure silica membrane showed a 68{\%} decline with a H2permeance of 4.5×10−8 mol m−2 s−1 Pa−1and a H2over N2selectivity of 800, both of which continued to deteriorate. In comparison, a 10{\%} ZrO2-SiO2membrane showed a decline of 56{\%} but to a level of 10−7 mol m−2 s−1 Pa−1with a H2over N2selectivity of 5700. Importantly, the deterioration largely stabilized at that permeance level.",
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AB - A hydrogen-selective silica-zirconia composite membrane was prepared on a macroporous alumina support by chemical vapor deposition of tetraethylorthosilicate (TEOS) and zirconium (IV) tert-butoxide (ZTB) at 923 K. The resulting membrane had a high H2permeance of 3.8×10−7 mol m−2 s−1 Pa−1with selectivities over CO2, N2and CH4of 1100, 1400 and 3700, respectively. Studies of the temperature dependence of the permeance of He, H2, and Ne demonstrated that the permeation mechanism was similar to that of dense silica membranes, involving solid-state diffusion with jumps of the permeating species between solubility sites. Parameters such as the site density, jump distance, and jump frequency were calculated and were physically plausible, and varied in reasonable manner with the mass and size of He, H2, and Ne. An alternative mechanism involving an activated gas translational mechanism was shown to fit the data but to give physically unrealistic parameters. The silica-zirconia membrane showed hydrothermal stability over a limited testing period of 48 h. After exposure to 16 mol% water vapor at 923 K for 48 h, a pure silica membrane showed a 68% decline with a H2permeance of 4.5×10−8 mol m−2 s−1 Pa−1and a H2over N2selectivity of 800, both of which continued to deteriorate. In comparison, a 10% ZrO2-SiO2membrane showed a decline of 56% but to a level of 10−7 mol m−2 s−1 Pa−1with a H2over N2selectivity of 5700. Importantly, the deterioration largely stabilized at that permeance level.

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