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dc.contributor.authorConnah, Liam
dc.contributor.authorTruffault, Vincent
dc.contributor.authorPlatas-Iglesias, Carlos
dc.contributor.authorAngelovski, Goran
dc.date.accessioned2019-10-17T10:01:12Z
dc.date.available2019-10-17T10:01:12Z
dc.date.issued2019-07-25
dc.identifier.citationL. Connah, V. Truffault, C. Platas-Iglesias and G. Angelovski, Dalt. Trans., 2019, 48, 13546–13554.es_ES
dc.identifier.issn1477-9226
dc.identifier.issn1477-9234
dc.identifier.urihttp://hdl.handle.net/2183/24142
dc.description.abstract[Abstract] Understanding the relationship between chemical structure and the effectiveness of bioresponsive magnetic resonance imaging (MRI) contrast agents can offer help to identify key components required for the future development of such probes. Here, we report the development and characterisation of two novel monomeric bifunctional chelators, L1 and L2, whose paramagnetic metal complexes can serve as calcium-responsive contrast agents. Specifically, relaxometric titrations, luminescence lifetime measurements, high resolution NMR and diffusion experiments, as well as density functional theory (DFT) calculations were carried out to assess the behaviour of each system. Minor structural differences between the probes resulted from the extension of the linker between the macrocyclic lanthanide chelator and the acyclic Ca-binding moiety. Relaxometric titrations of both systems, GdL1 and GdL2, showed an increase in r1 and r2 relaxivity upon Ca2+ addition, with the derivative bearing the longer linker showing a greater overall change. The hydration states of the europium analogues were assessed revealing a higher initial hydration state for EuL2. Diffusion ordered NMR spectroscopy revealed negligible changes in the diffusive properties of both systems upon the addition of Ca2+, while NMR studies of the Y3+, Yb3+ and Eu3+ analogues provided further insights into the structural behaviour of the linker unit in both the unsaturated and Ca-saturated states. DFT calculations supported the different coordination modes of the studied paramagnetic complexes in the presence and absence of Ca2+. Overall, our findings demonstrate the impact of subtle changes to the structure of such probes, affecting a range of properties and their coordination behaviour.es_ES
dc.description.sponsorshipGerman Research Foundation; AN 716/7-1es_ES
dc.language.isoenges_ES
dc.publisherRoyal Society of Chemistryes_ES
dc.relation.urihttps://www.doi.org/10.1039/C9DT02672Jes_ES
dc.rightsAtribución 3.0 Españaes_ES
dc.rights.urihttp://creativecommons.org/licenses/by/3.0/es/*
dc.subjectSmart contrast agentses_ES
dc.subjectWater exchange-rateses_ES
dc.subjectComplexeses_ES
dc.subjectLuminescencees_ES
dc.subjectEuropiumes_ES
dc.titleInvestigations into the effects of linker length elongation on the behaviour of calcium-responsive MRI probeses_ES
dc.typeinfo:eu-repo/semantics/articlees_ES
dc.rights.accessinfo:eu-repo/semantics/openAccesses_ES
UDC.journalTitleDalton Transactionses_ES
UDC.volume48es_ES
UDC.issue36es_ES
UDC.startPage13546es_ES
UDC.endPage13554es_ES


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