Zeolite‐Based “Particle Board” Membranes for Rapid and Selective Hydrogen Permeation

Abstract Zeolites, with their well‐defined pore sizes and outstanding stability, are regarded as the quintessential material for precise molecular separation tasks. However, the leap from easily produced zeolite powders to synthesizing free‐standing zeolite membranes, which can fully leverage their ordered porosity, presents substantial technical hurdles. Addressing this challenge, this study introduces polymers of intrinsic microporosity (PIM‐1) as adhesives through a wrapping‐compression method for the facile fabrication of high‐performance and free‐standing zeolite (FAU) “particle board” membranes. The 3D tomogram reconstruction from the focused ion beam‐scanning electron microscope images reveals the “particle board” membranes exhibit hierarchical porous structures. The non‐interconnecting macropores between zeolite particles facilitate the rapid H 2 permeation, and the zeolites’ ordered micropores sieve the gas molecules. The optimized FAU@PIM‐1 free‐standing membrane with hierarchically pore structures demonstrated hydrogen permeance (2240 GPU) alongside H 2 /CH 4 selectivity (31.68) for mixed gas and maintained this performance level under pressure ranges from 1.2 to 4.0 bar and over protracted operational periods (up to 3200 h). Meanwhile, EMT and MFI‐type zeolites have also been successfully applied to validate the versatility of this method, demonstrating its widespread potential for the fabrication of various free‐standing zeolite membranes.