Free energy of ligand removal in the metal-organic framework UiO-66

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dc.contributor.authorBristow, Jessica K.
dc.contributor.authorSvane, Katrine L.
dc.contributor.authorTiana, Davide
dc.contributor.authorSkelton, Jonathan M.
dc.contributor.authorGale, Julian D.
dc.contributor.authorWalsh, Aron
dc.contributor.funderEngineering and Physical Sciences Research Councilen
dc.contributor.funderAustralian Research Councilen
dc.contributor.funderEuropean Research Councilen
dc.date.accessioned2018-07-06T10:58:47Z
dc.date.available2018-07-06T10:58:47Z
dc.date.issued2016-05
dc.date.updated2018-07-03T11:09:17Z
dc.description.abstractWe report an investigation of the "missing-linker phenomenon" in the Zr-based metal organic framework UiO-66 using atomistic force field and quantum chemical methods. For a vacant benzene dicarboxylate ligand, the lowest energy charge-capping mechanism involves acetic acid or Cl-/H2O. The calculated defect free energy of formation is remarkably low, consistent with the high defect concentrations reported experimentally. A dynamic structural instability is identified for certain higher defect concentrations. In addition to the changes in material properties upon defect formation, we assess the formation of molecular aggregates, which provide an additional driving force for ligand loss. These results are expected to be of relevance to a wide range of metal-organic frameworks.en
dc.description.sponsorshipAustralian Research Council (Discovery Program)en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationBristow, J. K., Svane, K. L., Tiana, D., Skelton, J. M., Gale, J. D. and Walsh, A. (2016) 'Free Energy of Ligand Removal in the Metal–Organic Framework UiO-66', The Journal of Physical Chemistry C, 120(17), pp. 9276-9281. doi: 10.1021/acs.jpcc.6b01659en
dc.identifier.doi10.1021/acs.jpcc.6b01659
dc.identifier.endpage9281en
dc.identifier.issn1932-7447
dc.identifier.journaltitleJournal of Physical Chemistry Cen
dc.identifier.startpage9276en
dc.identifier.urihttps://hdl.handle.net/10468/6425
dc.identifier.volume120en
dc.language.isoenen
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.projectinfo:eu-repo/grantAgreement/RCUK/EPSRC/EP/G03768X/1/GB/Doctoral Training Centre in Sustainable Chemical Technologies/en
dc.relation.projectinfo:eu-repo/grantAgreement/EC/FP7::SP2::ERC/277757/EU/Hybrid Semiconductors: Design Principles and Material Applications/HYBRIDSen
dc.relation.projectinfo:eu-repo/grantAgreement/RCUK/EPSRC/EP/K004956/1/GB/Applying Long-lived Metastable States with Switchable Functionality via Kinetic Control of Molecular Assembly - a Programme in Functional Materials/en
dc.relation.projectinfo:eu-repo/grantAgreement/RCUK/EPSRC/EP/L000202/1/GB/MATERIALS CHEMISTRY HIGH END COMPUTING CONSORTIUM/en
dc.relation.urihttps://doi.org/10.1021/acs.jpcc.6b01659
dc.relation.urihttps://pubs.acs.org/doi/10.1021/acs.jpcc.6b01659
dc.rights© 2016 American Chemical Society. This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.en
dc.rights.urihttps://pubs.acs.org/page/policy/authorchoice_ccby_termsofuse.htmlen
dc.subjectDensity functionalsen
dc.subjectMOFSen
dc.subjectMetal organic frameworksen
dc.subjectProgramen
dc.subjectAdsorptionen
dc.subjectDefectsen
dc.subjectGULPen
dc.titleFree energy of ligand removal in the metal-organic framework UiO-66en
dc.typeArticle (peer-reviewed)en
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