Computational screening and functional tuning of chemically stable metal organic frameworks for I₂/CH₃I capture in humid environments

High chemical stability is of vital significance in rendering metal organic frameworks (MOFs) as promising adsorbents for capturing leaked radioactive nuclides, under real nuclear industrial conditions with high humidity. In this work, grand canonical Monte Carlo (GCMC) and density functional theory (DFT) methods have been employed to systematically evaluate I2/CH3I capture performances of 21 experimentally confirmed chemically stable MOFs in humid environments. Favorable structural factors and the influence of hydrophilicity for iodine capture were unveiled. Subsequently, the top -performing MIL -53 -Al with flexible tunability was functionalized with different functional groups to achieve the better adsorption performance. It has been revealed that the adsorption affinity and pore volume were two major factors altered by the functionalization of polar functional groups, which collectively influenced the iodine adsorption properties. In general, this work has screened the chemically stable high-performance MOF iodine adsorbents and provided comprehensive insights into the key factors affecting I2/CH3I uptake and separation in humid environments.