Abstract

Nature suggests that complex materials result from a hierarchical organization of matter at different length scales. At the nano- and micrometer scale, macromolecules and supramolecular aggregates spontaneously assemble into supracolloidal structures whose complexity is given by the coexistence of various colloidal entities and the specific interactions between them. Here, we demonstrate how such control can be implemented by engineering specially customized bile salt derivative-based supramolecular tubules that exhibit a highly specific interaction with polymeric microgel spheres at their extremities thanks to their scroll-like structure. This design allows for hierarchical supracolloidal self-assembly of microgels and supramolecular scrolls into a regular framework of “nodes” and “linkers”. The supramolecular assembly into scrolls can be triggered by pH and temperature, thereby providing the whole supracolloidal system with interesting stimuli-responsive properties. A colloidal smart assembly is embodied with features of center-linker frameworks as those found in molecular metal–organic frameworks and in structures engineered at human scale, masterfully represented by the Atomium in Bruxelles.

Highlights

  • Nature suggests that complex materials result from a hierarchical organization of matter at different length scales

  • In a previous study,[23] it was demonstrated that a selective association of microgels can occur at the bilayer edges located at the extremities and along the lateral surface of the supramolecular rolls

  • When microgels are in excess with respect to the tubules, fully decorated rolls are observed where microgels distribute according to regular patterns following the profiles of the rolled sheet edges (Figure 1b middle, bottom)

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Summary

Introduction

Nature suggests that complex materials result from a hierarchical organization of matter at different length scales. We demonstrate how such control can be implemented by engineering specially customized bile salt derivative-based supramolecular tubules that exhibit a highly specific interaction with polymeric microgel spheres at their extremities thanks to their scroll-like structure. This design allows for hierarchical supracolloidal self-assembly of microgels and supramolecular scrolls into a regular framework of “nodes” and “linkers”. By taking advantage of the specific amphiphilic structure of natural steroidal surfactants like the bile salts (BSs)[17] it is possible to rationally design BS derivatives (BSDs) in order to direct their supramolecular self-assembly into tubular structures.[18−22] These structures provide anisotropic building blocks with selective sites for the binding of polymeric microgels, which can be used to fabricate hierarchical frameworks

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