Gokdemir, TugceGurdal, Yeliz2025-01-062025-01-0620240892-70221029-043510.1080/08927022.2024.23955692-s2.0-85203274723https://doi.org/10.1080/08927022.2024.2395569https://hdl.handle.net/20.500.14669/2868Molecular hydrogen (H-2) is a renewable energy carrier, however, its practical applications are limited due to the challenges of developing safe and efficient H-2 storage devices. Metal Organic Frameworks (MOFs) containing at least two different metal ions in their structures are called as mixed-metal MOFs (MM-MOFs) and they could adsorb H-2 in higher amounts compared to structures containing single metal nodes. We theoretically examined the H-2 storage capacities of 26 MM-MOFs having various physical and chemical properties applying Grand Canonical Monte Carlo (GCMC) and Density Functional Theory (DFT) simulations. H-2 adsorption isotherms were calculated using a five-site anisotropic H-2 model. QIXSOG, YOMVIG, OSOYUR, Cu-Mg-BTC, Fe-Mg-BTC, and Cr-Mg-BTC were selected as top-performing MM-MOFs maximising H-2 adsorption gravimetrically and volumetrically at near-ambient conditions (233 K and 100 bar), approaching the DOE targets. YOMVIG has the largest H-2 adsorption enthalpy, calculated as -9.93kJ/mol at 233 K and 100 bar. DFT simulations have been conducted to analyse preferable H-2 adsorption sites as well as identify guest-host interactions. Electron density difference analysis showed that adsorbed H-2 molecules in the OSOYUR, Cr-Mg-BTC, Cu-Mg-BTC, and Fe-Mg-BTC are polarised. Our study challenges existing literature by identifying promising MM-MOFs as potential next-generation hydrogen storage adsorbents at near-ambient conditions.eninfo:eu-repo/semantics/closedAccessPhysisorptionthe density derived electrostatic and chemical charges (DDEC)five-site H-2 modelH-2 adsorption sitesArticle124515Q2123350WOS:001303569500001N/A