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Subcomponent self-assembly of circular helical Dy$_{6}$(L)$_{6}$ and bipyramid Dy$_{12}$(L)$_{8}$ architectures directed via second-order template effects

Li, Xiao-Lei; Zhao, Lang; Wu, Jianfeng; Shi, Wei ; Struch, Niklas; Lützen, Arne ; Powell, Annie K. 1; Cheng, Peng; Tang, Jinkui
1 Institut für Nanotechnologie (INT), Karlsruher Institut für Technologie (KIT)

Abstract:

In situ metal-templated (hydrazone) condensation also called subcomponent self-assembly of 4,6-dihydrazino-pyrimidine, o-vanillin and dysprosium ions resulted in the formation of discrete hexa- or dodecanuclear metallosupramolecular Dy$_{6}$(L)$_{6}$ or Dy$_{12}$(L)$_{8}$ aggregates resulting from second-order template effects of the base and the lanthanide counterions used in these processes. XRD analysis revealed unique circular helical or tetragonal bipyramid architectures in which the bis(hydrazone) ligand L adopts different conformations and shows remarkable differences in its mode of metal coordination. While a molecule of trimethylamine acts as a secondary template that fills the void of the Dy$_{6}$(L)$_{6}$ assembly, sodium ions take on this role for the formation of heterobimetallic Dy$_{12}$(L)$_{8}$ by occupying vacant coordination sites, thus demonstrating that these processes can be steered in different directions upon subtle changes of reaction conditions. Furthermore, Dy$_{6}$(L)$_{6}$ shows an interesting spin-relaxation energy barrier of 435 K, which is amongst the largest values within multinuclear lanthanide single-molecular magnets.


Verlagsausgabe §
DOI: 10.5445/IR/1000150653
Veröffentlicht am 27.09.2022
Originalveröffentlichung
DOI: 10.1039/D2SC03156F
Scopus
Zitationen: 22
Web of Science
Zitationen: 22
Dimensions
Zitationen: 23
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Nanotechnologie (INT)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 31.08.2022
Sprache Englisch
Identifikator ISSN: 2041-6520, 2041-6539
KITopen-ID: 1000150653
HGF-Programm 47.11.02 (POF IV, LK 01) Emergent Quantum Phenomena
Erschienen in Chemical Science
Verlag Royal Society of Chemistry (RSC)
Band 13
Heft 34
Seiten 10048–10056
Vorab online veröffentlicht am 22.07.2022
Nachgewiesen in Dimensions
Web of Science
Scopus
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