Integrative assembly of heteroleptic tetrahedra controlled by backbone steric bulk

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dc.contributor.authorTessarolo, Jacopo
dc.contributor.authorLee, Haeri
dc.contributor.authorSakuda, Eri
dc.contributor.authorUmakoshi, Keisuke
dc.contributor.authorClever, Guido H.
dc.date.accessioned2021-05-28T05:37:20Z
dc.date.available2021-05-28T05:37:20Z
dc.date.issued2021-04-26
dc.description.abstractA bent fluorenone-based dipyridyl ligand LA reacts with PdII cations to a solvent-dependent dynamic library of [PdnL2n] assemblies, constituted by a [Pd3LA6] ring and a [Pd4LA8] tetrahedron as major components, and a [Pd6LA12] octahedron as minor component. Introduction of backbone steric hindrance in ligand LB allows exclusive formation of the [Pd6LB12] octahedron. Combining equimolar amounts of both ligands results in integrative self-sorting to give an unprecedented [Pd4LA4LB4] heteroleptic tetrahedron. Key to the non-statistical assembly outcome is exploiting the structural peculiarity of the [Pd4L8] tetrahedral topology, where the four lean ligands occupy two doubly bridged edges and the bulky ligands span the four remaining, singly bridged edges. Hence, the system finds a compromise between the entropic drive to form an assembly smaller than the octahedron and the enthalpic prohibition of pairing two bulky ligands on the same edge of the triangular ring. The emission of luminescent LA is maintained in both homoleptic [Pd3LA6] and heteroleptic [Pd4LA4LB4].en
dc.identifier.urihttp://hdl.handle.net/2003/40223
dc.identifier.urihttp://dx.doi.org/10.17877/DE290R-22096
dc.language.isoende
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.subjectPalladiumen
dc.subjectSelf organizationen
dc.subjectLigandsen
dc.subjectCrystal structureen
dc.subjectCavitiesen
dc.subject.ddc540
dc.titleIntegrative assembly of heteroleptic tetrahedra controlled by backbone steric bulken
dc.typeTextde
dc.type.publicationtypearticlede
dcterms.accessRightsopen access
eldorado.openaire.projectidentifierinfo:eu-repo/grantAgreement/EC/H2020/683083/EU/Reactivity and Assembly of Multifunctional, Stimuli-responsive Encapsulation Structures/RAMSESde
eldorado.secondarypublicationtruede
eldorado.secondarypublication.primarycitationJacopo Tessarolo, Haeri Lee, Eri Sakuda, Keisuke Umakoshi, and Guido H. Clever: Integrative assembly of heteroleptic tetrahedra controlled by backbone steric bulk. Journal of the American Chemical Society 2021 143 (17), 6339-6344en
eldorado.secondarypublication.primaryidentifierhttps://doi.org/10.1021/jacs.1c01931de

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Integrative Assembly of Heteroleptic Tetrahedra Controlled by Backbone Steric Bulk
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