Binary Solvent Regulated Architecture of Ultra‐Microporous Hydrogen‐Bonded Organic Frameworks with Tunable Polarization for Highly‐Selective Gas Separation

A binary solvent synthetic strategy is proposed for the construction of C₂ -symmetric molecule-based hydrogen-bonded organic frameworks (HOFs) with permanent ultra-micropores and surface polarization derived from tunable coplanar open oxygen atoms. The activated HOFs BTBA-1 a and PTBA-1 a show highly selective separation of CO₂ /N₂ with a record high ideal adsorbed solution theory (IAST) selectivity >2000 under ambient temperature and pressure.