Defect-free high-silica CHA zeolite membranes with high selectivity for light gas separation

Pelin Karakiliç, Xuerui Wang, Freek Kapteijn, Arian Nijmeijer, Louis Winnubst*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

A systematic approach is described for the fabrication of defect-free high-silica zeolite membranes with CHA (SSZ-13) topology. Home-made hydrothermally-synthesized CHA seeds were coated on porous α-alumina substrates with a pore diameter of 80 nm and by means of a further hydrothermal treatment a zeolite membrane layer was formed. In order to obtain a thin and defect-free zeolite layer, the influence on the final microstructure of seed concentration during coating, coating method (rubbing, dip- or spin-coating) and crystal growth time was investigated. The template removal procedure was optimized to avoid the formation of cracks or defects. For an optimal thermal treatment, using a step-wise temperature increase to 500 °C, the membranes exhibit CO2/CH4 permselectivities of 25–30 with CO2 permeances of around 2 x 10−7 mol m−2 s−1 Pa−1 at 22 °C and 2 bar of pressure difference. O2 plasma pre-treatment prior to template removal increased the CO2/CH4 permselectivity to 176, while maintaining the same CO2 permeance values when no pre-treatment was used. The SF6 permeances, both at low (22 °C) and high (200 °C) temperatures, were below the detection limit (2 x 10−10 mol m−2 s−1 Pa−1), which in return results in very high N2/SF6 permselectivities of more than 700.

Original languageEnglish
Pages (from-to)34-43
Number of pages10
JournalJournal of membrane science
Volume586
Early online date22 May 2019
DOIs
Publication statusPublished - 15 Sep 2019

Fingerprint

Zeolites
Silicon Dioxide
coating
Gases
selectivity
Silica
silicon dioxide
membranes
Membranes
pretreatment
Defects
Seed
seeds
Seeds
defects
templates
gases
Coatings
Temperature
Aluminum Oxide

Keywords

  • UT-Hybrid-D
  • Natural gas purification
  • SF recovery
  • SSZ-13
  • Zeolite membrane
  • CHA zeolite

Cite this

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title = "Defect-free high-silica CHA zeolite membranes with high selectivity for light gas separation",
abstract = "A systematic approach is described for the fabrication of defect-free high-silica zeolite membranes with CHA (SSZ-13) topology. Home-made hydrothermally-synthesized CHA seeds were coated on porous α-alumina substrates with a pore diameter of 80 nm and by means of a further hydrothermal treatment a zeolite membrane layer was formed. In order to obtain a thin and defect-free zeolite layer, the influence on the final microstructure of seed concentration during coating, coating method (rubbing, dip- or spin-coating) and crystal growth time was investigated. The template removal procedure was optimized to avoid the formation of cracks or defects. For an optimal thermal treatment, using a step-wise temperature increase to 500 °C, the membranes exhibit CO2/CH4 permselectivities of 25–30 with CO2 permeances of around 2 x 10−7 mol m−2 s−1 Pa−1 at 22 °C and 2 bar of pressure difference. O2 plasma pre-treatment prior to template removal increased the CO2/CH4 permselectivity to 176, while maintaining the same CO2 permeance values when no pre-treatment was used. The SF6 permeances, both at low (22 °C) and high (200 °C) temperatures, were below the detection limit (2 x 10−10 mol m−2 s−1 Pa−1), which in return results in very high N2/SF6 permselectivities of more than 700.",
keywords = "UT-Hybrid-D, Natural gas purification, SF recovery, SSZ-13, Zeolite membrane, CHA zeolite",
author = "Pelin Karakili{\cc} and Xuerui Wang and Freek Kapteijn and Arian Nijmeijer and Louis Winnubst",
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Defect-free high-silica CHA zeolite membranes with high selectivity for light gas separation. / Karakiliç, Pelin; Wang, Xuerui; Kapteijn, Freek; Nijmeijer, Arian; Winnubst, Louis.

In: Journal of membrane science, Vol. 586, 15.09.2019, p. 34-43.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Defect-free high-silica CHA zeolite membranes with high selectivity for light gas separation

AU - Karakiliç, Pelin

AU - Wang, Xuerui

AU - Kapteijn, Freek

AU - Nijmeijer, Arian

AU - Winnubst, Louis

N1 - Elsevier deal

PY - 2019/9/15

Y1 - 2019/9/15

N2 - A systematic approach is described for the fabrication of defect-free high-silica zeolite membranes with CHA (SSZ-13) topology. Home-made hydrothermally-synthesized CHA seeds were coated on porous α-alumina substrates with a pore diameter of 80 nm and by means of a further hydrothermal treatment a zeolite membrane layer was formed. In order to obtain a thin and defect-free zeolite layer, the influence on the final microstructure of seed concentration during coating, coating method (rubbing, dip- or spin-coating) and crystal growth time was investigated. The template removal procedure was optimized to avoid the formation of cracks or defects. For an optimal thermal treatment, using a step-wise temperature increase to 500 °C, the membranes exhibit CO2/CH4 permselectivities of 25–30 with CO2 permeances of around 2 x 10−7 mol m−2 s−1 Pa−1 at 22 °C and 2 bar of pressure difference. O2 plasma pre-treatment prior to template removal increased the CO2/CH4 permselectivity to 176, while maintaining the same CO2 permeance values when no pre-treatment was used. The SF6 permeances, both at low (22 °C) and high (200 °C) temperatures, were below the detection limit (2 x 10−10 mol m−2 s−1 Pa−1), which in return results in very high N2/SF6 permselectivities of more than 700.

AB - A systematic approach is described for the fabrication of defect-free high-silica zeolite membranes with CHA (SSZ-13) topology. Home-made hydrothermally-synthesized CHA seeds were coated on porous α-alumina substrates with a pore diameter of 80 nm and by means of a further hydrothermal treatment a zeolite membrane layer was formed. In order to obtain a thin and defect-free zeolite layer, the influence on the final microstructure of seed concentration during coating, coating method (rubbing, dip- or spin-coating) and crystal growth time was investigated. The template removal procedure was optimized to avoid the formation of cracks or defects. For an optimal thermal treatment, using a step-wise temperature increase to 500 °C, the membranes exhibit CO2/CH4 permselectivities of 25–30 with CO2 permeances of around 2 x 10−7 mol m−2 s−1 Pa−1 at 22 °C and 2 bar of pressure difference. O2 plasma pre-treatment prior to template removal increased the CO2/CH4 permselectivity to 176, while maintaining the same CO2 permeance values when no pre-treatment was used. The SF6 permeances, both at low (22 °C) and high (200 °C) temperatures, were below the detection limit (2 x 10−10 mol m−2 s−1 Pa−1), which in return results in very high N2/SF6 permselectivities of more than 700.

KW - UT-Hybrid-D

KW - Natural gas purification

KW - SF recovery

KW - SSZ-13

KW - Zeolite membrane

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JO - Journal of membrane science

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