Tailoring Pore Environments in Metal–Organic Framework for C ₂ H ₂ /CO ₂ Separation and Organic Dyes Removal

The development of effective physical adsorbent for simultaneous C₂H₂/CO₂ separation and organic dyes removal is crucial for environmental remediation. Herein, we report a multifunctional anionic metal-organic framework (MOF), <b>SDU-CP-4</b>, featuring partitioned pore spaces engineered through the cooperative action of polar aromatic microenvironments and a symmetrically matched partitioning agent. This design enhances host-guest interactions and produces dual microporous cages within an anionic framework, collectively enabling exceptional performance in both gas separation and dye adsorption. <b>SDU-CP-4</b> exhibits preferential uptake of C₂H₂ over CO₂ with an IAST selectivity of 4.8, as further confirmed by breakthrough experiments. Meanwhile, <b>SDU-CP-4</b> shows remarkable adsorption capacities toward cationic dyes, achieving up to 2230 mg g^-1 for safranine T and 1404 mg g^-1 for rhodamine B, outperforming most reported MOFs. These results indicate <b>SDU-CP-4</b> as a robust multifunctional adsorbent with strong potential for gas purification and dyes removal applications.