Multipoint Interactions Enhanced CO2 Uptake: A Zeolite-like Zinc–Tetrazole Framework with 24-Nuclear Zinc Cages

Abstract

A zeolite-like microporous tetrazole-based metal–organic framework (MOF) with 24 nuclear zinc cages was synthesized and characterized. It exhibits high CO₂ adsorption capacity up to 35.6 wt % (8.09 mmol/g) and excellent CO₂/CH₄ selectivity at 273 K/1 bar, being among the highest values known to date. Theoretical calculations based on simulated annealing techniques and periodic DFT revealed that CO₂ is predominantly located around the inner surface of the cages through multipoint interactions, in particular, around the aromatic tetrazole rings. Importantly, it is the first time that multipoint interactions between CO₂ molecules and frameworks resulting in high CO₂ uptake are observed.