Synthesizing Polymer Woven Metal–Organic Framework Glass Membranes for Exceptional Pressure-Tolerant Carbon Capture

Liquid-processable metal-organic framework (MOF) glasses well redefine the ideal materials for energy-efficient carbon capture membranes. However, MOF glass membranes still suffer from poor pore connectivity, inadequate porosity and severe pressure vulnerability, hindering the sustainable deployment of membrane technologies in flue gas decarbonization, natural gas valorization, etc. Herein, we report a nature-inspired molecular weaving method to synthesize a de novo pw-MOF (polymer woven MOF) glass family. During melting, the woven polymer protects against lattice deformation while undergoing a nanophase interface segregation (nano-IS) evolution, which effectively regulates the kinetic mass transfer efficiency and thermodynamic polar adsorption effect. The newly synthesized pw-MOF glass membranes contain connected subnanometer penetrating channel networks with high-density polar domains for adsorption along the polymer chains to achieve a recorded performance, exemplified by the CO₂/N₂ and CO₂/CH₄ systems, surpassing the most recent upper bound. Owing to the unique woven reinforced framework, our pw-MOF glass membranes demonstrate an unprecedented pressure tolerance of up to 7.5 atm, which has not been realized by contemporary MOF membranes, which usually malfunction at 1 atm. This nature-inspired weaving design philosophy for synthesizing unconventional materials and constructing exceptional architectures is versatile for cultivating next-generation sustainable materials.