Intracrystalline Transport Barriers Affecting the Self-Diffusion of CH4 in Zeolites |Na12|-A and |Na12–xKx|-A
Artikel i vetenskaplig tidskrift, 2019

Carbon dioxide must be removed from biogas or natural gas to obtain compressed or liquefied methane, and adsorption-driven isolation of CO2 could be improved by developing new adsorbents. Zeolite adsorbents can select CO2 over CH4, and the adsorption of CH4 on zeolite |Na12-xKx|-A is significantly lower for samples with a high K+ content, i.e., x > 2. Nevertheless, we show, using 1H NMR experiments, that these zeolites adsorb CH4 after long equilibration times. Pulsed-field gradient NMR experiments indicated that in large crystals of zeolites |Na12-xKx|-A, the long-time diffusion coefficients of CH4 did not vary with x, and the upper limit of the mean-square displacement was about 1.5 μm, irrespective of the diffusion time. Also for zeolite |Na12|-A samples of three different particle sizes (∼0.44, ∼2.9, and ∼10.6 μm), the upper limit of the mean-square displacement of CH4 was 1.5 μm and largely independent of the diffusion time. This similarity provided further evidence for an intracrystalline diffusion restriction for CH4 within the medium- and large-sized zeolite A crystals and possibly of clustering and close contact among the small zeolite A crystals. The upper limit of the long-time diffusion coefficient of adsorbed CH4 was (at 1 atm and 298 K) about 10-10 m2/s irrespective of the size of the zeolite particle or the studied content of K+ in zeolites |Na12-xKx|-A and |Na12|-A. The T1 relaxation time for adsorbed CH4 on zeolites |Na12-xKx|-A with x > 2 was smaller than for those with x < 2, indicating that the short-time diffusion of CH4 was hindered.

Författare

Niklas Hedin

Stockholms universitet

Przemyslaw Rzepka

Stockholms universitet

Alma Berenice Jasso-Salcedo

Stockholms universitet

Tamara L. Church

Stockholms universitet

Diana Bernin

Chalmers, Kemi och kemiteknik, Kemiteknik, Kemisk apparatteknik

Göteborgs universitet

Langmuir

07437463 (ISSN) 15205827 (eISSN)

Vol. 35 40 12971-12978

Ämneskategorier

Analytisk kemi

Materialkemi

Annan kemiteknik

DOI

10.1021/acs.langmuir.9b02574

PubMed

31510744

Mer information

Senast uppdaterat

2019-11-11