Tailored transition-metal coordination environments in imidazole-modified DNA G-quadruplexes

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dc.contributor.authorPunt, Philip M.
dc.contributor.authorClever, Guido H.
dc.date.accessioned2020-03-12T13:55:30Z
dc.date.available2020-03-12T13:55:30Z
dc.date.issued2019-08-29
dc.description.abstractTwo types of imidazole ligands were introduced both at the end of tetramolecular and into the loop region of unimolecular DNA G‐quadruplexes. The modified oligonucleotides were shown to complex a range of different transition‐metal cations including NiII, CuII, ZnII and CoII, as indicated by UV/Vis absorption spectroscopy and ion mobility mass spectrometry. Molecular dynamics simulations were performed to obtain structural insight into the investigated systems. Variation of ligand number and position in the loop region of unimolecular sequences derived from the human telomer region (htel) allows for a controlled design of distinct coordination environments with fine‐tuned metal affinities. It is shown that CuII, which is typically square‐planar coordinated, has a higher affinity for systems offering four ligands, whereas NiII prefers G‐quadruplexes with six ligands. Likewise, the positioning of ligands in a square‐planar versus tetrahedral fashion affects binding affinities of CuII and ZnII cations, respectively. Gaining control over ligand arrangement patterns will spur the rational development of transition‐metal‐modified DNAzymes. Furthermore, this method is suited to combine different types of ligands, for example, those typically found in metalloenzymes, inside a single DNA architecture.en
dc.identifier.urihttp://hdl.handle.net/2003/39063
dc.identifier.urihttp://dx.doi.org/10.17877/DE290R-20982
dc.language.isoende
dc.relation.ispartofseriesChem. Eur. J.;25(61)
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.subjectBioinorganic chemistryen
dc.subjectCoordination chemistryen
dc.subjectDNAen
dc.subjectG-quadruplexesen
dc.subjectImidazoleen
dc.subject.ddc540
dc.titleTailored transition-metal coordination environments in imidazole-modified DNA G-quadruplexesen
dc.typeTextde
dc.type.publicationtypearticlede
dcterms.accessRightsopen access
eldorado.secondarypublicationtruede
eldorado.secondarypublication.primarycitationPunt, PM, Clever, GH (2019). Tailored transition-metal coordination environments in imidazole-modified DNA G-quadruplexes. Chem. Eur. J. 25(61), 13987-13993.de
eldorado.secondarypublication.primaryidentifierhttps://doi.org/10.1002/chem.201903445de

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