Separation Performance of Si-CHA Zeolite Membrane for a Binary H₂/CH₄ Mixture and Ternary and Quaternary Mixtures Containing Impurities

Abstract

The separation of H2/CH4 mixtures is very common in the natural gas and petrochemical industries. There are some higher C2–C4 hydrocarbons and water vapor that are used as impurity gases. Si-CHA zeolite membranes display a high H2 permeance of 1.44 × 10–6 mol/(m2 s Pa) (permeability of 10800 barrers) and H2/CH4 selectivity of 85 for an equimolar H2/CH4 mixture at 298 K and 0.2 MPa pressure drop. A third gas decreased H2 permeance and H2/CH4 selectivity of the membrane. Hydrogen permeance was reduced in an order similar to the adsorption amount in zeolite: H2O > C3H8 > n-butane > ethane. The effects of temperature, pressure, and feed concentration were studied on separation performances of the membrane in the binary and ternary mixtures. A simple model was built up to predict the reduction of permeance and selectivity when multi impurities were contained, and the predicted value agreed well with the tested one. A stable performance was obtained within several hours in all the tests. The separation performance of the membrane was recovered to the original level when the impurity gas was removed.