Issue 34, 2022

Subcomponent self-assembly of circular helical Dy6(L)6 and bipyramid Dy12(L)8 architectures directed via second-order template effects

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 Dy6(L)6 or Dy12(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 Dy6(L)6 assembly, sodium ions take on this role for the formation of heterobimetallic Dy12(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, Dy6(L)6 shows an interesting spin-relaxation energy barrier of 435 K, which is amongst the largest values within multinuclear lanthanide single-molecular magnets.

Graphical abstract: Subcomponent self-assembly of circular helical Dy6(L)6 and bipyramid Dy12(L)8 architectures directed via second-order template effects

Supplementary files

Article information

Article type
Edge Article
Submitted
03 Jun 2022
Accepted
20 Jul 2022
First published
22 Jul 2022
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2022,13, 10048-10056

Subcomponent self-assembly of circular helical Dy6(L)6 and bipyramid Dy12(L)8 architectures directed via second-order template effects

X. Li, L. Zhao, J. Wu, W. Shi, N. Struch, A. Lützen, A. K. Powell, P. Cheng and J. Tang, Chem. Sci., 2022, 13, 10048 DOI: 10.1039/D2SC03156F

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