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Understanding Carbon Dioxide Adsorption on Univalent Cation Forms of the Flexible Zeolite Rho at Conditions Relevant to Carbon Capture from Flue Gases
Abstract
A series of univalent cation forms of zeolite Rho (M(9.8)Al(9.8)Si(38.2)O(96), M = H, Li, Na, K, NH(4), Cs) and ultrastabilized zeolite Rho (US-Rho) have been prepared. Their CO(2) adsorption behavior has been measured at 298 K and up to 1 bar and related to the structures of the dehydrated forms determined by Rietveld refinement and, for H-Rho and US-Rho, by solid state NMR. Additionally, CO(2) adsorption properties of the H-form of the silicoalumino-phosphate with the RHO topology and univalent cation forms of the zeolite ZK-5 were measured for comparison. The highest uptakes at 0.1 bar, 298 K for both Rho and ZK-5 were obtained on the Li-forms (Li-Rho, 3.4 mmol g(-1); Li-ZK-5, 4.7 mmol g(-1)). H- and US-Rho had relatively low uptakes under these conditions: extra-framework Al species do not interact strongly with CO(2). Forms of zeolite Rho in which cations occupy window sites between α-cages show hysteresis in their CO(2) isotherms, the magnitude of which (Na(+),NH(4)(+) < K(+) < Cs(+)) correlates with the tendency for cations to occupy double eight-membered ring sites rather than single eight-membered ring sites. Hysteresis is not observed for zeolites where cations do not occupy the intercage windows. In situ synchrotron X-ray diffraction of the CO(2) adsorption on Na-Rho at 298 K identifies the adsorption sites. The framework structure of Na-Rho "breathes" as CO(2) is adsorbed and desorbed and its desorption kinetics from Na-Rho at 308 K have been quantified by the Zero Length Column chromatographic technique. Na-Rho shows much higher CO(2)/C(2)H(6) selectivity than Na-ZK-5, as determined by single component adsorption, indicating that whereas CO(2) can diffuse readily through windows containing Na(+) cations, ethane cannot.
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Silicoaluminophosphates as CO2 sorbents
Cheung, O., Liu, Q., Bacsik, Z., & Hedin, N. (2012) · Microporous and Mesoporous Materials · doi:10.1016/j.micromeso.2012.02.003 · Cited by 80
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Self-citationZeolites in Adsorption Processes: State of the Art and Future Prospects
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Georgieva, V. M., Bruce, E. L., Verbraeken, M. C., Scott, A. R., Casteel, W. J., Brandani, S., & Wright, P. A. (2019) · Journal of the American Chemical Society · doi:10.1021/jacs.9b05539 · Cited by 147
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Metadata
- Authors
- Lozinska, M. M., Mangano, E., Mowat, J. P. S., Shepherd, A. M., Howe, R. F., Thompson, S. P., Parker, J. E., Brandani, S., & Wright, P. A.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2012-10-11
- Volume
- 134
- Issue
- 42
- Pages
- 17628-17642
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2117816816
- Cited by
- 211
- References
- 3
- FWCI
- 16.17
- Type
- journal article
- Language
- en
- Open access
- closed
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- Lozinska, M. M., Mangano, E., Mowat, J. P. S., Shepherd, A. M., Howe, R. F., Thompson, S. P., Parker, J. E., Brandani, S., & Wright, P. A. (2012). Understanding Carbon Dioxide Adsorption on Univalent Cation Forms of the Flexible Zeolite Rho at Conditions Relevant to Carbon Capture from Flue Gases. Journal of the American Chemical Society. https://doi.org/10.1021/ja3070864
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