DisMolGels · Dissipative Self-Assembly: A powerful but unexplored tool to create temporary supramolecular hydrogels

Dissipative Self-Assembly: A powerful but unexplored tool to create temporary supramolecular hydrogels

The main purpose of this proposal was to develop molecular temporary hydrogels coupled to an energy dissipating chemical reaction. Until now, most molecular self-assembled materials operate close to thermodynamic equilibrium and are far from the interesting features biological living “materials” display like adaptivity, self-healing or temporal control. Biological materials are thermodynamically open and are kept far from equilibrium by a constant input of energy. This mode of self-assembly, one of the requirements of life, is referred to as dissipative or dynamic self-assembly. Over the last decade, in order to overcome this gap between synthetic and biologicals materials, several researchers are trying to recreate part of such dissipative processes and translate them into the already known static materials. We envision for these materials unique properties which will expand their current applications. As an example, biomedical implants that would autonomously degrade after performing their function would diminish the need for a post-treatment surgery to remove the implant. Or, a detergent that would degrade hours after usage would be less harmful to the environment. However, the topic is still in its infancy and therefore, design rules are still missing and hampering the development of these interesting systems. In this way, our proposal aims not only at creating dynamic hydrogels with entirely new properties but also at setting new design guidelines and requirements to pave the way for the further development of dissipative materials. Our strategy is based on coupling chemical reactions to self-assembled hydrogels. Such hydrogels are maintained far from the equilibrium by the constant input of fuel and therefore endowed with tunable lifetime and stiffness. In order to be successful, the following four specific objectives were tackled: 1. Develop chemical reaction networks that can drive the transient formation of assemblies. 2. Design and synthesize precursor building blocks that can self-assemble into hydrogels. 3. Develop transient dissipative molecular hydrogels by coupling chemical reaction networks to precursor building blocks. 4. Study the relation between the kinetics of the chemical reaction networks and material properties. By the end of the project the main objectives of the proposal were achieved and published in peer review journals. Moreover, the same approach was applied to different kind of molecules which allowed us to develop a larger library of dissipative systems and explore their unique properties

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