TY - JOUR AU - Shi, Lijuan AU - Sun, Deyun AU - Xu, Hongxue AU - Maqsood, Zunaira AU - Chen, Shangqing AU - Yi, Qun PY - 2026 TI - Shell engineering on mesoporous metal organic frameworks: beyond microporous restriction in core-shell architecture JO - Green Chemical Engineering SN - 2096-9147 SP - 327 EP - 335 VL - 7 IS - 3 AB - Core-shell metal organic frameworks (MOFs) have emerged as a promising platform for efficient separation and sensing, benefiting from the sieving effect of the shell and the large storage capacity of the core. However, conventional core-shell MOFs often encounter challenges with compromised pore integrity, which predominantly restricts their design to microporous cores. In this study, a straightforward strategy to construct functional shells on mesoporous MOFs is proposed. By leveraging dynamic imine chemistry, small-molecule amines are assembled into supramolecular polymers and anchored onto the surface of mesoporous MOFs through metal coordination. This approach preserves the mesoporous structure of the core while introducing hydrogen-bonding channels in the shell, facilitating the selective capture and storage of polar gases. The resulting core-shell MOF demonstrates exceptional CO2/N2 selectivity of up to 10,943 and a high CO2 adsorption capacity, enabling the direct production of high-purity CO2 (99.7 vol.%) from humid flue gas in a single breakthrough experiment. Furthermore, this strategy exhibits excellent stability and versatility across various mesoporous MOFs, underscoring its potential for practical industrial gas separation applications. UR - https://doi.org/10.1016/j.gce.2025.02.002 DO - 10.1016/j.gce.2025.02.002