Advances in membrane technologies are significant for mitigating global climate change because of their low cost and easy operation. Although mixed-matrix membranes (MMMs) obtained via the combination of metal-organic frameworks (MOFs) and a polymer matrix are promising for energy-efficient gas separation, the achievement of a desirable match between polymers and MOFs for the development of advanced MMMs is challenging, especially when emerging highly permeable materials such as polymers of intrinsic microporosity (PIMs) are deployed. Here, we report a molecular soldering strategy featuring multifunctional polyphenols in tailored polymer chains, well-designed hollow MOF structures, and defect-free interfaces. The exceptional adhesion nature of polyphenols results in dense packing and visible stiffness of PIM-1 chains with strengthened selectivity. The architecture of the hollow MOFs leads to free mass transfer and substantially improves permeability. These structural advantages act synergistically to break the permeability-selectivity trade-off limit in MMMs and surpass the conventional upper bound. This polyphenol molecular soldering method has been validated for various polymers, providing a universal pathway to prepare advanced MMMs with desirable performance for diverse applications beyond carbon capture.
© 2023. The Author(s).