Computational Screening of Metal-Organic Frameworks for Carbon Capture: Insights from Flue Gas and Direct Air Capture Condition

Metal-organic frameworks (MOFs) have emerged as highly promising materials for carbon dioxide (CO₂) capture, owing to their exceptional tunability, high surface areas, and versatile chemical properties. In this study, we employ Grand Canonical Monte Carlo (GCMC) simulations to systematically screen 1,670 experimentally synthesized MOFs from the CoRE database, focusing on their potential for carbon capture applications. The screening process prioritizes flue gas conditions (0.15 bar CO₂, 298 K), identifying MOFs with CO₂ adsorption capacities exceeding 0.16 g/g and heats of adsorption below 40 kJ/mol. Among the screened materials, 18 structures met these criteria, with the majority featuring open metal sites (OMS); a key structural feature that enhances CO₂ binding affinity. To further evaluate the versatility of MOFs, some MOFs were also selected from results of flue gas screening and tested under direct air capture (DAC) conditions (285 K, 400 ppm CO₂). Remarkably, 18 out of the 20 MOFs demonstrated CO₂ adsorption capacities above 1 mmol/g, with some achieving capacities as high as 4 mmol/g. The study emphasizes the critical role of structural and chemical properties, particularly the presence of OMS and functional groups, in determining adsorption performance. By providing a rapid and efficient computational screening approach, this work offers valuable insights into identifying high performing MOFs tailored to both flue gas and DAC applications.