Structure Regulation of MOF Nanosheet Membrane for Accurate H₂/CO₂ Separation

High-purity H2 production accompanied with a precise decarbonization opens an avenue to approach a carbon-neutral society. Metal-organic framework nanosheet membranes provide great opportunities for an accurate and fast H2 /CO2 separation, CO2 leakage through the membrane interlayer galleries decided the ultimate separation accuracy. Here we introduce low dose amino side groups into the Zn2 (benzimidazolate)4 conformation. Physisorbed CO2 served as interlayer linkers, gently regulated and stabilized the interlayer spacing. These evoked a synergistic effect of CO2 adsorption-assisted molecular sieving and steric hinderance, whilst exquisitely preserving apertures for high-speed H2 transport. The optimized amino membranes set a new record for ultrathin nanosheet membranes in H2 /CO2 separation (mixture separation factor: 1158, H2 permeance: 1417 gas permeation unit). This strategy provides an effective way to customize ultrathin nanosheet membranes with desirable molecular sieving ability.