Abstract

“Smart” materials have considerably evolved over the last few years for specific applications. They rely on intelligent macromolecules or (supra-)molecular motifs to adapt their structure and properties in response to external triggers. Here, a supramolecular stimuli-responsive polymer gel is constructed from heterotelechelic double hydrophilic block copolymers that incorporate thermo-responsive sequences. These macromolecular building units are synthesized via a three-step controlled radical copolymerization and then hierarchically assembled to yield coordination micellar hydrogels. The dynamic mechanical properties of this particular class of materials are studied in shear flow and finely tuned via temperature changes. Notably, rheological experiments show that structurally reinforcing the micellar network nodes leads to precise tuning of the viscoelastic response and yield behavior of the material. Hence, they constitute promising candidates for specific applications, such as mechano-sensors.

Highlights

  • Abstract: “Smart” materials have considerably evolved over the last few years for specific applications

  • We describe the synthesis of a terpyridine end-capped polystyrene-block-poly(N-isopropylacrylamide)-block-poly(2(dimethylamino)ethyl methacrylate) triblock terpolymer (PS-b-PNIPAAm-b-PDMAEMA-b-tpy) and its hierarchical assembly into a coordination micellar network

  • Rotational rheometry is used as a characterization tool to probe the thermo-mechanical properties of the supramolecular hydrogel

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Summary

Introduction

Abstract: “Smart” materials have considerably evolved over the last few years for specific applications They rely on intelligent macromolecules or (supra-)molecular motifs to adapt their structure and properties in response to external triggers. At the basis of “smart” materials lie intelligent polymer sequences or (supra-)molecular motifs having the ability to adapt their conformations and properties in response to external triggers, such as temperature [6,7,8,9], light [10,11,12] or pH [13,14,15] Those variables can notably reverse the solvophilicity of synthetic macromolecules incorporating responsive groups, which pave the way for stimuli-sensitive materials. By raising the hydrophilic nature of PDMAEMA through protonation of tertiary aminogroups [26], the overall hydrogen bonding ability of the macromolecules, as well as their electrostatic repellency are increased, which leads to higher transition temperatures [26,27,28,29]

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