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Issue 40, 2020
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Exploring the self-assembly of dumbbell-shaped polyoxometalate hybrids, from molecular building units to nanostructured soft materials

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Abstract

The formation of hierarchical nanostructures using preformed dumbbell-like species made of covalent organic–inorganic polyoxometalate (POM)-based hybrids is herein described. In this system, the presence of charged subunits (POM, metal linkers, and counter ions) in the complex molecular architecture can drive their aggregation, which results from a competition between the solvation energy of the discrete species and intermolecular electrostatic interactions. We show that the nature of the POM and the charge of the metal linker are key parameters for the hierarchical nanoorganization. The experimental findings were corroborated with a computational investigation combining DFT and molecular dynamics simulation methods, which outlines the importance of solvation of the counter ion and POM/counter ion association in the aggregation process. The dumbbell-like species can also form gels, in the presence of a poorer solvent, displaying similar nanoorganization of the aggregates. We show that starting from the designed molecular building units whose internal charges can be controlled by redox trigger we can achieve their implementation into soft nanostructured materials through the control of their supramolecular organization.

Graphical abstract: Exploring the self-assembly of dumbbell-shaped polyoxometalate hybrids, from molecular building units to nanostructured soft materials

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Article information


Submitted
10 Jun 2020
Accepted
10 Sep 2020
First published
18 Sep 2020

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2020,11, 11072-11080
Article type
Edge Article

Exploring the self-assembly of dumbbell-shaped polyoxometalate hybrids, from molecular building units to nanostructured soft materials

M. S. Centellas, M. Piot, R. Salles, A. Proust, L. Tortech, D. Brouri, S. Hupin, B. Abécassis, D. Landy, C. Bo and G. Izzet, Chem. Sci., 2020, 11, 11072
DOI: 10.1039/D0SC03243C

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