Theoretical investigation of mixed-metal metal-organic frameworks as H2 adsorbents: insights from GCMC and DFT simulations

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dc.authoridGurdal, Yeliz/0000-0002-6245-891X
dc.authoridGOKDEMIR, TUGCE/0000-0002-7475-6797
dc.contributor.authorGokdemir, Tugce
dc.contributor.authorGurdal, Yeliz
dc.date.accessioned2025-01-06T17:44:01Z
dc.date.available2025-01-06T17:44:01Z
dc.date.issued2024
dc.description.abstractMolecular 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.
dc.description.sponsorshipScientific and Technological Research Council of Turkiye (TuBiTAK) [120Z160]
dc.description.sponsorshipY.G acknowledges The Scientific and Technological Research Council of Turkiye (TuBiTAK) for funding through 1002 Short Term Support Module, grant agreement No: 120Z160. The calculations reported in this paper were performed using TRUBA computing resources, based in Turkiye.
dc.identifier.doi10.1080/08927022.2024.2395569
dc.identifier.endpage1245
dc.identifier.issn0892-7022
dc.identifier.issn1029-0435
dc.identifier.issue15
dc.identifier.scopus2-s2.0-85203274723
dc.identifier.scopusqualityQ2
dc.identifier.startpage1233
dc.identifier.urihttps://doi.org/10.1080/08927022.2024.2395569
dc.identifier.urihttps://hdl.handle.net/20.500.14669/2868
dc.identifier.volume50
dc.identifier.wosWOS:001303569500001
dc.identifier.wosqualityN/A
dc.indekslendigikaynakWeb of Science
dc.indekslendigikaynakScopus
dc.language.isoen
dc.publisherTaylor & Francis Ltd
dc.relation.ispartofMolecular Simulation
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanı
dc.rightsinfo:eu-repo/semantics/closedAccess
dc.snmzKA_20241211
dc.subjectPhysisorption
dc.subjectthe density derived electrostatic and chemical charges (DDEC)
dc.subjectfive-site H-2 model
dc.subjectH-2 adsorption sites
dc.titleTheoretical investigation of mixed-metal metal-organic frameworks as H2 adsorbents: insights from GCMC and DFT simulations
dc.typeArticle

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