Truly combining the advantages of polymeric and zeolite membranes for gas separations.

Mixed-matrix membranes (MMMs) have been investigated to render energy-intensive separations more efficiently by combining the selectivity and permeability performance, robustness, and nonaging properties of the filler with the easy processing, handling, and scaling up of the polymer. However, truly combining all in one single material has proven very challenging. In this work, we filled a commercial polyimide with ultrahigh loadings of a high-aspect ratio, CO 2 -philic Na-SSZ-39 zeolite with a three-dimensional channel system that precisely separates gas molecules. By carefully designing both zeolite and MMM synthesis, we created a gas-percolation highway across a flexible and aging-resistant (more than 1 year) membrane. The combination of a CO 2 -CH 4 mixed-gas selectivity of ~423 and a CO 2 permeability of ~8300 Barrer outperformed all existing polymer-based membranes and even most zeolite-only membranes.