Waterproof architectures through subcomponent self-assembly

Edmundo G. Percástegui, Jesús Mosquera, Tanya K. Ronson, Alex J. Plajer, Marion Kieffer, Jonathan R. Nitschke

Research output: Contribution to journalArticle

22 Citations (Scopus)

Abstract

Metal-organic containers are readily prepared through self-assembly, but achieving solubility and stability in water remains challenging due to ligand insolubility and the reversible nature of the self-assembly process. Here we have developed conditions for preparing a broad range of architectures that are both soluble and kinetically stable in water through metal(ii)-templated (MII = CoII, NiII, ZnII, CdII) subcomponent self-assembly. Although these structures are composed of hydrophobic and poorly-soluble subcomponents, sulfate counterions render them water-soluble, and they remain intact indefinitely in aqueous solution. Two strategies are presented. Firstly, stability increased with metal-ligand bond strength, maximising when NiII was used as a template. Architectures that disassembled when CoII, ZnII and CdII templates were employed could be directly prepared from NiSO4 in water. Secondly, a higher density of connections between metals and ligands within a structure, considering both ligand topicity and degree of metal chelation, led to increased stability. When tritopic amines were used to build highly chelating ligands around ZnII and CdII templates, cryptate-like water-soluble structures were formed using these labile ions. Our synthetic platform provides a unified understanding of the elements of aqueous stability, allowing predictions of the stability of metal-organic cages that have not yet been prepared.

Original languageEnglish
Pages (from-to)2006-2018
Number of pages13
JournalChemical Science
Volume10
Issue number7
Early online date12 Dec 2018
DOIs
Publication statusPublished - 21 Feb 2019

Keywords

  • metal-organic containers
  • solubility
  • aqueous stability

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