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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

Lozinska, Magdalena M., Mangano, Enzo, Mowat, John P. S., Shepherd, Ashley M., Howe, Russell F., Thompson, Stephen P., Parker, Julia E., Brandani, Stefano, Wright, Paul A.·2012·Journal of the American Chemical Society
DOI 10.1021/ja3070864
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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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Cited by

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
DOI
10.1021/ja3070864
OpenAlex
W2117816816
Cited by
211
References
3
FWCI
16.17
Type
journal article
Language
en
Open access
closed

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