Large-Scale Screening and Machine Learning to Predict the Computation-Ready, Experimental Metal-Organic Frameworks for CO 2 Capture from Air

The rising level of CO2 in the atmosphere has attracted attention in recent years. The technique of capturing CO2 from higher CO2 concentrations, such as power plants, has been widely studied, but capturing lower concentrations of CO2 directly from the air remains a challenge. This study uses high-throughput computer (Monte Carlo and molecular dynamics simulation) and machine learning (ML) to study 6013 computation-ready, experimental metal-organic frameworks (CoRE-MOFs) for CO2 adsorption and diffusion properties in the air with very low concentrations of CO2. First, the law influencing CO2 adsorption and diffusion in air is obtained as a structure-performance relationship, and then the law influencing the performance of CO2 adsorption and diffusion in air is further explored by four ML algorithms. Random forest (RF) was considered the optimal algorithm for prediction of CO2 selectivity, with an R value of 0.981, and this algorithm was further applied to analyze the relative importance of each metal-organic framework (MOF) descriptor quantitatively. Finally, 14 MOFs with the best properties were successfully screened out, and it was found that a key to capturing a low concentration CO2 from the air was the diffusion performance of CO2 in MOFs. When the pore-limiting diameter (PLD) of a MOF was closer to the CO2 dynamic diameter, this MOF could possess higher CO2 diffusion separation selectivity. This study could provide valuable guidance for the synthesis of new MOFs in experiments that capture directly low concentration CO2 from the air.