Synthesis and Permeation Properties of a DDR-Type Zeolite Membrane for Separation of CO₂/CH₄ Gaseous Mixtures

TLDR

A highly hydrophobic DDR‑type zeolite membrane was hydrothermally synthesized on the outer surface of a porous α‑alumina tube and its single‑ and binary‑gas permeation properties were measured up to 5 MPa. The membrane achieved a CO₂/CH₄ ideal selectivity of 340, a CO₂ permeance of 3.0 × 10⁻⁷ mol m⁻² s⁻¹ Pa⁻¹, and outperformed other zeolite membranes in CO₂/CH₄ separation.

Abstract

Using hydrothermal synthesis, a highly hydrophobic DDR-type zeolite membrane was prepared on the outer surface of a porous α-alumina tube. The results of this study show that it is useful for CO2/CH4 separation. Single-gas permeation for CO2, CH4, H2, He, N2, and O2, and CO2/CH4 binary gas permeation, were measured, respectively, at pressures up to 5 and 2 MPa. The respective single-gas permeances of CO2 and CH4 at 298 K at a feed pressure of 0.2 MPa and a permeate pressure of 0.1 MPa were 4.2 × 10-7 and 1.2 × 10-9 mol m-2 s-1 Pa-1; the ideal selectivity for CO2/CH4 was 340. The permeances were in the following order: CO2 > H2 > He > O2 > N2 > CH4. Single-gas permeance was dependent on the relative molecular size of the DDR pore diameter. However, CO2 permeance dominated the adsorption affinity to the pore wall of DDR zeolite. In mixed-gas permeation experiments using the sweep method, the DDR-type zeolite membrane showed high selectivity for CO2/CH4 mixtures of 200 and high CO2 permeance of 3.0 × 10-7 mol m-2 s-1 Pa-1 at 298 K with a feed pressure of 0.2 MPa. Furthermore, the DDR zeolite membranes were compared to other zeolite membranes for evaluation of their CO2/CH4 selectivity and CO2 permeance; the DDR-type zeolite membranes show better CO2/CH4 separation and CO2 permeance.