Pressure-Responsive Two-Dimensional Metal–Organic Framework Composite Membranes for CO₂ Separation

The regulation of permeance and selectivity in membrane systems may allow effective relief of conventional energy-intensive separations. Here, pressure-responsive ultrathin membranes (≈100 nm) fabricated by compositing flexible two-dimensional metal–organic framework nanosheets (MONs) with graphene oxide nanosheets for CO₂ separation are reported. By controlling the gas permeation direction to leverage the pressure-responsive phase transition of the MONs, CO₂-induced gate opening and closing behaviors are observed in the resultant membranes, which are accompanied with the sharp increase of CO₂ permeance (from 173.8 to 1144 gas permeation units) as well as CO₂/N₂ and CO₂/CH₄ selectivities (from 4.1 to 22.8 and from 4 to 19.6, respectively). The flexible behaviors and separation mechanism are further elucidated by molecular dynamics simulations. This work establishes the relevance of structural transformation-based framework dynamics chemistry in smart membrane systems.