Aromatic Amine-Functionalized Covalent Organic Frameworks (COFs) for CO2/N2 Separation

Abstract

CO₂ is a prominent example for an exhaust gas, and it is known for its high impact on global warming. Therefore, carbon capture from CO₂ emissions of industrial processes is increasingly important to halt and prevent the disruptive consequences of global warming. Covalent organic frameworks (COFs) as porous nanomaterials have been shown to selectively adsorb CO₂ in high quantities and with high CO₂/N₂ selectivity. Interactions with amines are recognized to selectively adsorb CO₂ and help capture it from exhaust emissions. Herein, a novel COF (Me₃TFB-(NH₂)₂BD), which was not accessible via a direct condensation reaction, was synthetized by dynamic linker exchange starting with Me₃TFB-BD. Despite the linker exchange, the porosity of the COF was largely maintained, resulting in a high BET surface area of 1624 ± 89 m²/g. The CO₂ and N₂ adsorption isotherms at 273 and 295 K were studied to determine the performance in carbon capture at flue gas conditions. Me₃TFB-(NH₂)₂BD adsorbs 1.12 ± 0.26 and 0.72 ± 0.07 mmol/g of CO₂ at 1 bar and 273 and 295 K, respectively. The COF shows a high CO₂/N₂ IAST selectivity under flue gas conditions (273 K:83 ± 11, 295 K: 47 ± 11). The interaction of the aromatic amine groups with CO₂ is based on physisorption, which is expected to make the regeneration of the material energy efficient.

Keywords: carbon capture; covalent organic frameworks; dynamic covalent chemistry; gas separation; linker exchange.