Multi-stimuli control over assembly and guest binding in metallo-supramolecular hosts based on dithienylethene photoswitches
| dc.contributor.author | Li, Ru-Jin | |
| dc.contributor.author | Tessarolo, Jacopo | |
| dc.contributor.author | Lee, Haeri | |
| dc.contributor.author | Clever, Guido H. | |
| dc.date.accessioned | 2021-03-23T12:44:01Z | |
| dc.date.available | 2021-03-23T12:44:01Z | |
| dc.date.issued | 2021-03-05 | |
| dc.description.abstract | It is difficult to assemble multi-component metallo-supramolecular architectures in a non-statistical fashion, whichlimits their development toward functional materials. Herein, wereport a system of interconverting bowls and cages that are able torespond to various selective stimuli (light, ligands, anions), basedon the self-assembly of a photochromic dithienylethene (DTE)ligand,La, with PdIIcations. By combining the concept of“coordination sphere engineering”, relying on bulky quinolinedonors, with reversible photoswitching between the ligand’s open(o-La) and closed (c-La) forms, a [Pd2(o-La)4] cage (o-C) and a[Pd2(c-La)3] bowl (c-B) were obtained, respectively. This structuralrearrangement modulates the system’s guest uptake capabilities.Among three bis-sulfonate guests (G1,G2, andG3), the cage canencapsulate only the smallest (G1), while the bowl binds all of them. Bowlc-Bwas further used to synthesize a series of heterolepticcages, [Pd2LA3LB], representing a motif never reported before. Additional ligands (Lc‑f), with short or long arms, tune the cavity size,thus enabling or preventing guest uptake. Addition of Br−/Ag+makes it possible to change the overall charge, again triggering guestuptake and release, as well as fourth ligand de-/recomplexation. In combination, site-selective introduction of functionality andapplication of external stimuli lead to an intricate system of hosts with different guest preferences. A high degree of complexity isachieved through cooperativity between only a few components. | en |
| dc.identifier.uri | http://hdl.handle.net/2003/40092 | |
| dc.identifier.uri | http://dx.doi.org/10.17877/DE290R-21969 | |
| dc.language.iso | en | de |
| dc.rights.uri | https://creativecommons.org/licenses/by/4.0/ | |
| dc.subject | Palladium | en |
| dc.subject | Ligands | en |
| dc.subject | Chemical structure | en |
| dc.subject | Nuclear magnetic resonance spectroscopy | en |
| dc.subject | Titration | en |
| dc.subject.ddc | 540 | |
| dc.title | Multi-stimuli control over assembly and guest binding in metallo-supramolecular hosts based on dithienylethene photoswitches | en |
| dc.type | Text | de |
| dc.type.publicationtype | article | en |
| dcterms.accessRights | open access | |
| eldorado.openaire.projectidentifier | info:eu-repo/grantAgreement/EC/H2020/683083/EU/Reactivity and Assembly of Multifunctional, Stimuli-responsive Encapsulation Structures/RAMSES | de |
| eldorado.secondarypublication | true | de |
| eldorado.secondarypublication.primarycitation | Li, R.-J.; Tessarolo, J.; Lee, H.; Clever, G. H.Multi-stimuli control over assembly and guest binding in metallo-supramolecular hosts based on dithienylethene photoswitches.Journal of the American Chemical Society 2021 143 (10), 3865-3873. | de |
| eldorado.secondarypublication.primaryidentifier | https://doi.org/10.1021/jacs.0c12188 | de |