High-Throughput Screening of Experimental Metal-organic Frameworks for High Water Content Syngas Hydrogen...

Metal-organic frameworks (MOFs) are promising sorbents for adsorption-based hydrogen (H₂) purification in blue hydrogen process, but existing large-scale computational screenings rarely examine adsorption performances of MOFs under elevated pressure, temperature and high water content, which is typical of industrial hydrogen-rich syngas. In this work, we perform a high-throughput virtual screening of 11,334 porous experimental MOFs to identify candidates for pressure swing adsorption (PSA)-based H₂ purification from syngas under a range of realistic dry and wet conditions. Grand canonical Monte Carlo simulations are carried out for five-component dry syngas (H₂/CO₂/CO/CH₄/N₂) at three temperatures (30-70 °C) and five pressures (1-30 bar); 1080 Pareto-optimal MOFs are selected based on nondominated sorting of CO₂, CO, and CH₄ working capacities under all 15 conditions from the dry simulations, without imposing arbitrary performance thresholds. Under targeted dry operating conditions (70 °C, adsorption at 30 bar and desorption at 1 bar), top materials exhibit CO₂ working capacities above 15 mmol/g and CO₂/H₂ selectivities exceeding 1000, while maintaining appreciable adsorption for CO and CH₄. Adsorption capabilities of the three carbon impurities for most MOFs are severely suppressed when 35 vol % H₂O is introduced to the guest mixture in the wet simulations for the 1080 Pareto-optimal candidates; only seven MOFs retain measurable uptakes for all three carbon species, of which only four are considered thermal and water stable in the literature. Additional screening at 1 vol % H₂O identifies 16 more MOFs with appreciable uptakes and literature validated thermal and water stability, yielding a set of 20 final candidates recommended for further investigations. Moreover, comparison to performance threshold selection methods highlights the versatility of Pareto-based candidate selection for discovering balanced MOF materials for hydrogen purification from syngas under realistic PSA conditions.