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Apr 20, 2020

ACS Spring 2020 National Meeting & Expo

Dynamic bonds in polymers: Self-healing and mechanochemistry

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Abstract

The recognition of dynamic-bonds as a structurally defining element has brought additional functionality into synthetic polymers, imparting adaptive properties, not reachable by the pure covalent bond. Especially strong hydrogen bonds and weak-metal/ligand bonds are important in the molecular design of dynamic properties in polymers, important in the areas of self-healing and mechanochemically active polymers.<br/>We do address synthetic design of self-healing polymers, achieving autonomous healing close to room-temperature. Whereas phase segregation effects can be exploited in 3D-printing-systems, crystallization or hindered network-dynamics do strongly impede and change the dynamics of the overall material, both significantly influencing macroscopic properties such as self-healing. Basic investigations on the strength of a hydrogen-bond within polymers and polymeric materials are therefore discussed, showcasing the influence of the hydrogen-bonds environment on their strength. It is shown that the (thermal) reversibility concept of hydrogen bonds is decisive in 3D-printing-processes, where a careful design of melt-flow during and after the printing process can be effected.<br/>The concept of dynamic elements in polymers is extended to chemical systems directly responding to stress via molecular force-induced chemistry. Labile chemical Cu(I)-bis-carbenes have been synthesized, able to respond to stress imparted onto attached polymer-chains attached via living polymerization methods. The Cu(I)-bis-carbene complexes, bearing attached polymer-handles, are able to transform mechanical energy into a subsequent click"-reaction. Based on the force-induced splitting of one Cu(I)-carbene bond, a fluorogenic “click”-reaction can quantitatively detect the local stress, allowing the design of stress-responsive materials.

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© Copyright 2019 Morressier GmbH.
All rights reserved.