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Impact of Small Adsorbates in the Vibrational Spectra of Mg- and Zn-MOF-74 Revealed by First-Principles Calculations

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dc.contributor.authorRomero Muñiz, Carlos
dc.contributor.authorMerkling, Patrick
dc.contributor.authorCalero, Sofía
dc.contributor.authorGavira Vallejo, José María
dc.date.accessioned2024-05-20T11:18:29Z
dc.date.available2024-05-20T11:18:29Z
dc.date.issued2020
dc.description.abstractIn this work, we analyze the influence of small adsorbates on the vibrational spectra of Mg- and Zn-metal–organic framework MOF-74 by means of first-principles calculations. In particular, we consider the adsorption of four representative species of different interaction strengths: Ar, CO2, H2O, and NH3. Apart from a comprehensive characterization of the structural and energetic aspects of empty and loaded MOFs, we use a fully quantum ab initio approach to evaluate the Raman and IR activities of the normal modes, leading to the construction of the whole vibrational spectra. Under this approach, not only are we able to proceed with the complete assignment of the spectra in terms of the usual internal coordinates but also we can discern the most relevant vibrational fingerprints of the adsorbates and their impact on the whole MOF spectra. On the one hand, some of the typical vibrational modes of the small molecules are slightly shifted but still visible when adsorbed on the MOFs, especially those appearing at high wavenumbers where the empty MOFs lack IR/Raman signals. On the other hand, some bands arising from the organic ligands are affected by the presence of the absorbates, displaying non-negligible frequency shifts, in agreement with recent experiments. We find a strong correlation between all of these frequency shifts and the interaction strength of the adsorbate with the hosting framework. The findings presented in this work expand the capabilities of vibrational spectroscopy techniques to analyze porous materials and can be useful for the design of sensors and new devices based on MOF technology.en
dc.description.versionversión final
dc.identifier.doihttp://doi.org/10.1021/acsami.0c16629
dc.identifier.issn1944-8252
dc.identifier.urihttps://hdl.handle.net/20.500.14468/11614
dc.journal.titleACS Applied Materials & Interfaces
dc.language.isoen
dc.publisherAmerican Chemical Society
dc.relation.centerFacultad de Ciencias
dc.relation.departmentCiencias y Técnicas Fisicoquímicas
dc.rightsinfo:eu-repo/semantics/openAccess
dc.rights.urihttps://creativecommons.org/licenses/by-nc-nd/4.0/deed.es
dc.subject.keywordsmetal−organic framework
dc.subject.keywordsMOF-74
dc.subject.keywordsvibrational spectroscopy
dc.subject.keywordsdensity functional theory
dc.subject.keywordsgas adsorption
dc.titleImpact of Small Adsorbates in the Vibrational Spectra of Mg- and Zn-MOF-74 Revealed by First-Principles Calculationses
dc.typejournal articleen
dc.typeartículoes
dspace.entity.typePublication
relation.isAuthorOfPublicatione90dc241-289d-4e80-afd8-cde46576afe0
relation.isAuthorOfPublication.latestForDiscoverye90dc241-289d-4e80-afd8-cde46576afe0
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