Engineering the optical response of the titanium-MIL-125 metal-organic framework through ligand functionalization

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dc.contributor.authorHendon, Christopher H.
dc.contributor.authorTiana, Davide
dc.contributor.authorFontecave, Marc
dc.contributor.authorSanchez, Clement
dc.contributor.authorD'arras, Loic
dc.contributor.authorSassoye, Capucine
dc.contributor.authorRozes, Laurence
dc.contributor.authorMellot-Draznieks, Caroline
dc.contributor.authorWalsh, Aron
dc.contributor.funderRoyal Societyen
dc.contributor.funderEuropean Research Councilen
dc.contributor.funderSeventh Framework Programmeen
dc.contributor.funderEngineering and Physical Sciences Research Councilen
dc.contributor.funderResearch Councils UKen
dc.date.accessioned2018-07-05T15:11:50Z
dc.date.available2018-07-05T15:11:50Z
dc.date.issued2013-07-10
dc.date.updated2018-07-03T11:17:16Z
dc.description.abstractHerein we discuss band gap modification of MIL-125, a TiO2/1,4-benzenedicarboxylate (bdc) metal-organic framework (MOF). Through a combination of synthesis and computation, we elucidated the electronic structure of MIL-125 with aminated linkers. The band gap decrease observed when the monoaminated bdc-NH2 linker was used arises from donation of the N 2p electrons to the aromatic linking unit, resulting in a red-shifted band above the valence-band edge of MIL-125. We further explored in silico MIL-125 with the diaminated linker bdc(NH2)(2) and other functional groups (-OH, -CH3, -Cl) as alternative substitutions to control the optical response. The bdc-(NH2)2 linking unit was predicted to lower the band gap of MIL-125 to 1.28 eV, and this was confirmed through the targeted synthesis of the bdc-(NH2)(2)-based MIL,-125. This study illustrates the possibility of tuning the optical response of MOFs through rational functionalization of the linking unit, and the strength of combined synthetic/computational approaches for targeting functionalized hybrid materials.en
dc.description.sponsorshipRoyal Society (University Research Fellowship); European Research Council (ERC Starting Grant)en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationHendon, C. H., Tiana, D., Fontecave, M., Sanchez, C., D’arras, L., Sassoye, C., Rozes, L., Mellot-Draznieks, C. and Walsh, A. (2013) 'Engineering the Optical Response of the Titanium-MIL-125 Metal–Organic Framework through Ligand Functionalization', Journal of the American Chemical Society, 135(30), pp. 10942-10945. doi: 10.1021/ja405350uen
dc.identifier.doi10.1021/ja405350u
dc.identifier.endpage10945en
dc.identifier.issn0002-7863
dc.identifier.journaltitleJournal of the American Chemical Societyen
dc.identifier.startpage10942en
dc.identifier.urihttps://hdl.handle.net/10468/6421
dc.identifier.volume135en
dc.language.isoenen
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.projectinfo:eu-repo/grantAgreement/RCUK/EPSRC/EP/F067496/1/GB/Modelling of Advanced Functional Materials using Terascale Computing/en
dc.relation.project277757
dc.relation.urihttps://pubs.acs.org/doi/10.1021/ja405350u
dc.rights© 2013 American Chemical Society. ACS AuthorChoice - This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.en
dc.rights.urihttps://pubs.acs.org/page/policy/authorchoice_termsofuse.htmlen
dc.subjectCO2 captureen
dc.subjectBand-gapsen
dc.subjectMOFSen
dc.subjectPhotocatalysten
dc.subjectSubstitutionen
dc.subjectTunabilityen
dc.subjectSeparationen
dc.subjectReductionen
dc.subjectCatalysisen
dc.subjectAminoen
dc.titleEngineering the optical response of the titanium-MIL-125 metal-organic framework through ligand functionalizationen
dc.typeArticle (peer-reviewed)en
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