A Hybrid Zeolite Membrane-Based Breakthrough for Simultaneous CO2 Capture and CH4 Upgrading from Biogas

Yanghwan Jeong, Sejin Kim, Minseong Lee, Sungwon Hong, Mun Gi Jang, Nakwon Choi, Kyo Seon Hwang, Hionsuck Baik, Jin Kuk Kim, Alex C.K. Yip, Jungkyu Choi

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12 Citations (Scopus)


Biogas is an environmentally friendly and sustainable energy resource that can substitute or complement conventional fossil fuels. For practical uses, biogas upgrading, mainly through the effective separation of CO2 (0.33 nm) and CH4 (0.38 nm), is required to meet the approximately 90–95% purity of CH4, while CO2 should be concomitantly purified. In this study, a high CO2 perm-selective zeolite membrane was synthesized by heteroepitaxially growing a chabazite (CHA) zeolite seed layer with a synthetic precursor that allowed the formation of all-silica deca-dodecasil 3 rhombohedral (DDR) zeolite (with a pore size of 0.36 × 0.44 nm2). The resulting hydrophobic DDR@CHA hybrid membrane on an asymmetric α-Al2O3 tube was thin (ca. 2 μm) and continuous, thus providing both high flux and permselectivity for CO2 irrespective of the presence or absence of water vapor (the third largest component in the biogas streams). To the best of our knowledge, the CO2 permeance of (2.9 ± 0.3) × 10–7 mol m–2 s–1 Pa–1 and CO2/CH4 separation factor of ca. 274 ± 73 at a saturated water vapor partial pressure of ca. 12 kPa at 50 °C have the highest CO2/CH4 separation performance yet achieved. Furthermore, we explored the membrane module properties of the hybrid membrane in terms of the recovery and purity of both CO2 and CH4 under dry and wet conditions. Despite the high intrinsic membrane properties of the current hybrid membrane, reflected by the high permeance and SF, the corresponding module properties indicated that high-performance separation of CO2 and CH4 for the desired biogas upgrading was achieved at a limited processing capacity. This supports the importance of understanding the correlation between the membrane and module properties, as this will provide guidance for the optimal operating conditions.

Original languageEnglish
Pages (from-to)2893-2907
Number of pages15
JournalACS Applied Materials and Interfaces
Issue number2
Publication statusPublished - 2022 Jan 19

Bibliographical note

Funding Information:
This work was supported by a Korea Institute of Energy Technology Evaluation and Planning grant (20202020800330) and by the Mid-Career Researcher Program (2020R1A2C1101974) through the National Research Foundation of Korea, funded by the Korean government. In addition, this work was supported by the Ministry of Business, Innovation & Employment in New Zealand under the MBIE Endeavour “Smart Ideas” grant (UOCX1905). TEM characterizations were conducted at the KBSI.

Publisher Copyright:
© 2022 American Chemical Society


  • biogas upgrading
  • CO permselectivities
  • DDR zeolite
  • heteroepitaxial growth
  • hybrid zeolite membrane
  • module properties

ASJC Scopus subject areas

  • General Materials Science


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