Discriminative Separation of Gases by a “Molecular Trapdoor” Mechanism in Chabazite Zeolites
Abstract
Separation of molecules based on molecular size in zeolites with appropriate pore aperture dimensions has given rise to the definition of "molecular sieves" and has been the basis for a variety of separation applications. We show here that for a class of chabazite zeolites, what appears to be "molecular sieving" based on dimension is actually separation based on a difference in ability of a guest molecule to induce temporary and reversible cation deviation from the center of pore apertures, allowing for exclusive admission of certain molecules. This new mechanism of discrimination permits "size-inverse" separation: we illustrate the case of admission of a larger molecule (CO) in preference to a smaller molecule (N(2)). Through a combination of experimental and computational approaches, we have uncovered the underlying mechanism and show that it is similar to a "molecular trapdoor". Our materials show the highest selectivity of CO(2) over CH(4) reported to date with important application to natural gas purification.
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Trapdoor phenomena were first described by Shang et al. in 2012, after observing remarkably high CO2/CH4 selectivities on low silica exchanged chabazites.
“These were first described by Shang et al. in 2012, after observing remarkably high CO2/CH4 selectivities on low silica exchanged chabazites.”
From Zeolites in Adsorption Processes: State of the Art and Future Prospects (2022) · cites this paper as [258]
Similar but more severe trapdoor effects upon CO2 adsorption are observed in low silica aluminosilicate CHA materials containing potassium and prepared in absence of an OSDA.
“Similar but more severe trapdoor effects upon CO2 adsorption are observed in low silica aluminosilicate CHA materials containing potassium and prepared in the absence of an OSDA.258,262,516”
From Zeolites in Adsorption Processes: State of the Art and Future Prospects (2022) · cites this paper as [258]
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- Authors
- Shang, J., Li, G., Singh, R., Gu, Q., Nairn, K. M., Bastow, T. J., Medhekar, N., Doherty, C. M., Hill, A. J., Liu, J. Z., & Webley, P. A.
- Affiliations
- The University of Melbourne (AU)
- Australian Synchrotron (AU)
- Australian Research Council (AU)
- Commonwealth Scientific and Industrial Research Organisation (AU)
- Monash University (AU)
- Corresponding author
- Liu, Jefferson Z.
- Webley, Paul A.
- ORCID
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2012-11-13
- Volume
- 134
- Issue
- 46
- Pages
- 19246-19253
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2048418935
- Cited by
- 436
- References
- 6
- Citations by year
- 2026: 32 · 2025: 48 · 2024: 47 · 2023: 50 · 2022: 35 · 2021: 34 · 2020: 48 · 2019: 28 · 2018: 18 · 2017: 20 · 2016: 18 · 2015: 16 · 2014: 27 · 2013: 15
- FWCI
- 10.14
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- UWA Profiles and Research Repository (UWA) (submittedVersion)
- Funders
- Australian Government
- Monash University
- National Cancer Institute
- Topics
- Physical Sciences › Chemistry › Inorganic Chemistry › Zeolite Catalysis and Synthesis
- Physical Sciences › Engineering › Mechanical Engineering › Membrane Separation and Gas Transport
- Physical Sciences › Chemistry › Inorganic Chemistry › Metal-Organic Frameworks: Synthesis and Applications
- Keywords
- chabazite zeolite, molecular sieving, CO2/CH4 separation, CO2 adsorption, natural gas purification
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