In silico screening of metal-organic frameworks for CO₂ photo-hydrogenation

Metal-organic frameworks (MOFs) are a promising class of materials that can be used as catalysts for photo-hydrogenation to convert CO₂ to fuel by virtue of their nanoscale design featuring large surface area, abundant active metal sites, and ability to host dispersed co-catalysts. However, due to the vast combination of materials possible and general fragility of MOFs, experimental identification of catalytic materials is non-trivial. To aid in finding optimal catalytic candidates, we implement a multi-tiered high-throughput screening of 20 375 in silico MOFs for their porosity (≥4.5 Å), light absorption (1.7-3.5 eV), aqueous stability, and solvent removal stability. The 24 materials that passed screening were evaluated using density functional theory (DFT) applied to a proton-coupled electron transfer pathway for CO₂ to CH₄. Of eight thermodynamically favorable materials, three materials have been previously synthesized and the material precursors were analyzed for their material cost and life-cycle analysis, which revealed that Mg-MOF-74 had the lowest material cost ($15.11 per gram) and environmental impact. Five experimentally novel materials based on aluminum and zinc-based frameworks with pore diameters ranging from 4.7 to 21.6 Å, are presented for novel experimental realization.