Template-removal-associated microstructural development of porous-ceramic-supported MFI zeolite membranes

Junhang Dong; Y. S. Lin; Michael Z.C. Hu; Roberta A. Peascoe; E. Andrew Payzant

doi:10.1016/S1387-1811(99)00175-4

Template-removal-associated microstructural development of porous-ceramic-supported MFI zeolite membranes

Junhang Dong, Y. S. Lin, Michael Z.C. Hu, Roberta A. Peascoe, E. Andrew Payzant

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249 Scopus citations

Abstract

Defect-free thin MFI zeolite films were synthesized on porous α-alumina and yttria-doped zirconia (YZ) substrates by an in situ crystallization method using tetrapropylammonium hydroxide (TPAOH) as a template. The microstructure evolution of the supported zeolite films during calcination for template removal was studied by high-temperature X-ray diffraction and in situ gas permeance. Removal of the template from the zeolite films occurs at 350-500°C and is accompanied by a substantial shrinkage in the zeolite framework. After the template is removed from the zeolite at high temperatures, the zeolite crystals expand on cooling while the support shrinks. A compressive stress develops in the zeolite film during the cooling process when the zeolite crystallites are bound to the support after template removal. Without annealing prior to template removal, this stress induces cracks in the YZ-supported MFI films. High-quality MFI membranes were obtained on both α-alumina and YZ supports by using a suitable calcination temperature program. Removal of the template can either create or enlarge intercrystalline gaps as the zeolite crystallites decrease in size and draw away from adjacent crystallites. These gaps constitute the microporous non-zeolitic pores affecting the permselectivity of single-gas permeation for H₂ and SF₆. Both alumina- and YZ-supported MFI membranes show very good separation properties for hydrogen and n-butane mixtures, although the YZ-supported MFI films appear to have larger non-zeolitic pores than the alumina-supported membranes. (C) 2000 Elsevier Science B.V. All rights reserved.

Original language	English
Pages (from-to)	241-253
Number of pages	13
Journal	Microporous and Mesoporous Materials
Volume	34
Issue number	3
DOIs	https://doi.org/10.1016/S1387-1811(99)00175-4
State	Published - Mar 2000

Funding

This work was supported by the National Science Foundation (CTS-9502437) and the Exxon Education Foundation. We also would like to acknowledge the support of the DOE/BES/DMS and use of the HTML facilities at Oak Ridge National Laboratory; sponsorship was provided by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Transportation Technologies, as part of the High Temperature Materials Laboratory User Program. Oak Ridge National Laboratory is managed by Lockheed Martin Energy Research Corporation for the US Department of Energy, under contract DE-AC05-96OR22464.

Keywords

Calcination
Crack formation
Gas separation
MFI zeolite membrane
Thermal behavior

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10.1016/S1387-1811(99)00175-4

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title = "Template-removal-associated microstructural development of porous-ceramic-supported MFI zeolite membranes",

abstract = "Defect-free thin MFI zeolite films were synthesized on porous α-alumina and yttria-doped zirconia (YZ) substrates by an in situ crystallization method using tetrapropylammonium hydroxide (TPAOH) as a template. The microstructure evolution of the supported zeolite films during calcination for template removal was studied by high-temperature X-ray diffraction and in situ gas permeance. Removal of the template from the zeolite films occurs at 350-500°C and is accompanied by a substantial shrinkage in the zeolite framework. After the template is removed from the zeolite at high temperatures, the zeolite crystals expand on cooling while the support shrinks. A compressive stress develops in the zeolite film during the cooling process when the zeolite crystallites are bound to the support after template removal. Without annealing prior to template removal, this stress induces cracks in the YZ-supported MFI films. High-quality MFI membranes were obtained on both α-alumina and YZ supports by using a suitable calcination temperature program. Removal of the template can either create or enlarge intercrystalline gaps as the zeolite crystallites decrease in size and draw away from adjacent crystallites. These gaps constitute the microporous non-zeolitic pores affecting the permselectivity of single-gas permeation for H2 and SF6. Both alumina- and YZ-supported MFI membranes show very good separation properties for hydrogen and n-butane mixtures, although the YZ-supported MFI films appear to have larger non-zeolitic pores than the alumina-supported membranes. (C) 2000 Elsevier Science B.V. All rights reserved.",

keywords = "Calcination, Crack formation, Gas separation, MFI zeolite membrane, Thermal behavior",

author = "Junhang Dong and Lin, {Y. S.} and Hu, {Michael Z.C.} and Peascoe, {Roberta A.} and Payzant, {E. Andrew}",

year = "2000",

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AU - Dong, Junhang

AU - Lin, Y. S.

AU - Hu, Michael Z.C.

AU - Peascoe, Roberta A.

AU - Payzant, E. Andrew

PY - 2000/3

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N2 - Defect-free thin MFI zeolite films were synthesized on porous α-alumina and yttria-doped zirconia (YZ) substrates by an in situ crystallization method using tetrapropylammonium hydroxide (TPAOH) as a template. The microstructure evolution of the supported zeolite films during calcination for template removal was studied by high-temperature X-ray diffraction and in situ gas permeance. Removal of the template from the zeolite films occurs at 350-500°C and is accompanied by a substantial shrinkage in the zeolite framework. After the template is removed from the zeolite at high temperatures, the zeolite crystals expand on cooling while the support shrinks. A compressive stress develops in the zeolite film during the cooling process when the zeolite crystallites are bound to the support after template removal. Without annealing prior to template removal, this stress induces cracks in the YZ-supported MFI films. High-quality MFI membranes were obtained on both α-alumina and YZ supports by using a suitable calcination temperature program. Removal of the template can either create or enlarge intercrystalline gaps as the zeolite crystallites decrease in size and draw away from adjacent crystallites. These gaps constitute the microporous non-zeolitic pores affecting the permselectivity of single-gas permeation for H2 and SF6. Both alumina- and YZ-supported MFI membranes show very good separation properties for hydrogen and n-butane mixtures, although the YZ-supported MFI films appear to have larger non-zeolitic pores than the alumina-supported membranes. (C) 2000 Elsevier Science B.V. All rights reserved.

AB - Defect-free thin MFI zeolite films were synthesized on porous α-alumina and yttria-doped zirconia (YZ) substrates by an in situ crystallization method using tetrapropylammonium hydroxide (TPAOH) as a template. The microstructure evolution of the supported zeolite films during calcination for template removal was studied by high-temperature X-ray diffraction and in situ gas permeance. Removal of the template from the zeolite films occurs at 350-500°C and is accompanied by a substantial shrinkage in the zeolite framework. After the template is removed from the zeolite at high temperatures, the zeolite crystals expand on cooling while the support shrinks. A compressive stress develops in the zeolite film during the cooling process when the zeolite crystallites are bound to the support after template removal. Without annealing prior to template removal, this stress induces cracks in the YZ-supported MFI films. High-quality MFI membranes were obtained on both α-alumina and YZ supports by using a suitable calcination temperature program. Removal of the template can either create or enlarge intercrystalline gaps as the zeolite crystallites decrease in size and draw away from adjacent crystallites. These gaps constitute the microporous non-zeolitic pores affecting the permselectivity of single-gas permeation for H2 and SF6. Both alumina- and YZ-supported MFI membranes show very good separation properties for hydrogen and n-butane mixtures, although the YZ-supported MFI films appear to have larger non-zeolitic pores than the alumina-supported membranes. (C) 2000 Elsevier Science B.V. All rights reserved.

KW - Calcination

KW - Crack formation

KW - Gas separation

KW - MFI zeolite membrane

KW - Thermal behavior

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ER -

Template-removal-associated microstructural development of porous-ceramic-supported MFI zeolite membranes

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