Evaluation and screening of porous materials containing fluorine for carbon dioxide capture and separation

There is a significant challenge to discover porous materials that can effectively capture and separate CO2 from natural gas, refining gas, and flue gas, which has attracted attention in dealing with climate warming and energy purification. Recently, hybrid microporous materials with narrow pores and containing fluorine have been rapidly used in gas separation based on physisorption. In this contribution, molecular simulations combined with high-throughput calculations were performed to calculate structural parameters and performance evaluation metrics of 1015 promising adsorbents to rank and screen out the top candidates for CO2/CH4, CO2/H2 and CO2/N2 separation. To the best of our knowledge, this is the first time to unlock this kind of fluorinated material database in CO2 separation, in which statistical information indicates that a large number of interpenetrating structures lead to 64% of ultra-microporous materials and the number of particles per unit volume of fluorine we defined also has a positive effect on the heat of adsorption of CO2. The structural performance relationship reveals a clear picture of strong CO2 capture but poor energy gas (CH4 and H2) storage. The mathematical model established from the geometry and energy descriptors has a strong correlation with the mixture adsorption selectivity in CO2/N2 separation, and the ideal selectivity can be applied to save computing resources in CO2/H2 separation. Cadmium and vanadium with high frequency may represent the new characteristics of the next generation adsorbent for capturing CO2, among the 18 high-performance materials selected according to the adsorption performance score and mixture adsorption selectivity. The centroid density distribution and radial distribution function manifest that CO2 is preferentially close to fluorine atoms and metal atoms. Here, we established an online high-throughput calculation code (https://github.com/oddthinker/HTCS) for adsorption and separation. All of this will provide guidelines for experimental synthesis and large-scale screening of target materials.