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      Catenation and Aggregation of Multi-Cavity Coordination Cages

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          Abstract

          A series of metal-mediated cages, having multiple cavities, was synthesized from PdII cations and tris- or tetrakis-monodentate bridging ligands and characterized by NMR spectroscopy, mass spectrometry, and X-ray methods. The peanut-shaped [Pd3 L14 ] cage deriving from the tris-monodentate ligand L1 could be quantitatively converted into its interpenetrated [5Cl@Pd6 L18 ] dimer featuring a linear {[Pd-Cl-]5 Pd} stack as an unprecedented structural motif upon addition of chloride anions. Small-angle neutron scattering (SANS) experiments showed that the cigar-shaped assembly with a length of 3.7 nm aggregates into mono-layered discs of 14 nm diameter via solvophobic interactions between the hexyl sidechains. The hepta-cationic [5Cl@Pd6 L18 ] cage was found to interact with polyanionic oligonucleotide double-strands under dissolution of the aggregates in water, rendering the compound class interesting for applications based on non-covalent DNA binding.

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          Coordination assemblies from a Pd(II)-cornered square complex.

          The [enPd(II)]2+ (en = ethylenediamine) unit has emerged as a versatile building block in molecular self-assembly. In particular, the 90 degrees coordination angle of the metal has been judiciously used in the design of new discrete two- and three-dimensional structures. Our last 15 years of work with the Pd(II)-cornered unit is summarized in this Account, from the spontaneous formation of a Pd4 square metal complex to a family of architectures such as cages, bowls, boxes, tubes, catenanes, and spheres.
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            Self-assembled nanoreactors.

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              From Chemical Topology to Molecular Machines (Nobel Lecture)

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                Author and article information

                Journal
                Angewandte Chemie International Edition
                Angew. Chem. Int. Ed.
                Wiley
                14337851
                October 08 2018
                October 08 2018
                July 26 2018
                : 57
                : 41
                : 13652-13656
                Affiliations
                [1 ]Faculty of Chemistry and Chemical Biology; TU Dortmund University; Otto-Hahn-Strasse 6 44227 Dortmund Germany
                [2 ]Current affiliation: School of Chemistry and Chemical Engineering; Yangzhou University; Yangzhou 225002 Jiangsu PR China
                [3 ]Institute for Inorganic Chemistry; Heinrich-Heine University Düsseldorf; Universitätsstrasse 1 40225 Düsseldorf Germany
                [4 ]Stranski-Laboratorium für Physikalische und Theoretische Chemie; Institut für Chemie; Technische Universität Berlin; 10623 Berlin Germany
                [5 ]Institut Max von Laue-Paul Langevin (ILL); 71 avenue des Martyrs 38042 Grenoble France
                Article
                10.1002/anie.201806047
                29901844
                9620df52-98c3-4f00-bca0-35fada4c5e9e
                © 2018

                http://doi.wiley.com/10.1002/tdm_license_1.1

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