Abstract Separation of inert nitrogen from natural gas by membranes is much more energy-saving than cryogenic distillation but very challenging because the size difference of both gas molecules is quite… Click to show full abstract
Abstract Separation of inert nitrogen from natural gas by membranes is much more energy-saving than cryogenic distillation but very challenging because the size difference of both gas molecules is quite small. Herein, high-quality and N2-selective SSZ-13 membranes on α-alumina tubes were prepared using a novel synthesis approach called seeded-gel synthesis. Seeded-gel synthesis was more convenient and credible than the conventional secondary growth because a seeding step on the substrate was omitted for the former method. The effect of calcination atmosphere on the quality of membranes was also discussed. SSZ-13 membranes had the fewest defects when ozone calcination was used. The predicted values of single-component N2 and CH4 permeances by the Maxwell-Stefan equations agreed well with the experimental ones. The SSZ-13 membrane exhibited ultrahigh N2 permeance of 850 × 10−9 mol m−2 s−1 Pa−1 (equals 2500 GPU) and a high N2/CH4 selectivity of 13.5 at 298 K and 0.303 MPa feed pressure (absolute). Membrane preparation by seeded-gel method had good reproducibility. The effects of temperature, pressure drop and feed flow rate on membrane performances were investigated for N2/CH4 mixture separations. The membrane also displayed good separation performance in N2/CH4 system either at 2.6 MPa feed pressure or under humid conditions. The continuous SSZ-13 thin membranes prepared by the simple seeded-gel synthesis showed great potentials for energy-efficient N2 removal from unconventional gases.
               
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