Discovering Ultra-Stable Metal–Organic Frameworks for CO2 Capture from A Wet Flue Gas: Integrating Machine Learning and Molecular Simulation

The rapid increase in atmospheric CO2, arising from anthropogenic sources, has posed a severe threat to global climate and raised widespread environmental concern. Metal–organic frameworks (MOFs) are promising adsorbents to potentially reduce CO2 emissions from flue gases. However, many MOFs suffer from structural degradation and performance deterioration upon exposure to water in flue gases. Aiming to discover stable and efficient MOFs for CO2 capture from a wet flue gas, we propose a hierarchical high-throughput computational screening (HTCS) strategy. Machine learning (ML)-assisted stability analysis is incorporated within the HTCS, leveraging prior experimental experience to predict ultrastable (including water-, thermal-, and activation-stable) MOFs from ∼280,000 candidates in the ab initio REPEAT charge MOF (ARC–MOF) database. Among 9755 shortlisted MOFs, molecular simulations identify 1000 top-performing MOFs. Remarkably, several vanadium-based MOFs are revealed to be ultrastable, exhibiting high CO2 capture capability of 3–7 mmol/g and CO2/N2 selectivity of 95–401. Subsequently, ML regressors are developed to derive design principles for MOFs capable of overcoming the trade-off effect. Furthermore, an ML classifier is developed to analyze the impact of water on CO2 capture by comparing dry and wet conditions. The proposed hierarchical HTCS and developed ML models lay a solid foundation for the potential transition of MOFs into practical applications.