High-Throughput Screening of Experimental Metal–organic Frameworks for High Water Content Syngas Hydrogen Purification under Pressure Swing Adsorption Conditions

Metal–organic frameworks (MOFs) are promising sorbents for adsorption-based hydrogen (H 2 ) 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 H 2 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 (H 2 /CO 2 /CO/CH 4 /N 2 ) at three temperatures (30–70 °C) and five pressures (1–30 bar); 1080 Pareto-optimal MOFs are selected based on nondominated sorting of CO 2, CO, and CH 4 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 CO 2 working capacities above 15 mmol/g and CO 2 /H 2 selectivities exceeding 1000, while maintaining appreciable adsorption for CO and CH 4 . Adsorption capabilities of the three carbon impurities for most MOFs are severely suppressed when 35 vol % H 2 O 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 % H 2 O 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.