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  • melt processable dynamic covalent poly Hemiaminal organogels as scaffolds for uv induced polymerization
    Advanced Materials, 2015
    Co-Authors: Mareva Fevre, Gavin O. Jones, Jeannette M. García, Musan Zhang, James L. Hedrick
    Abstract:

    Hemiaminal poly(ethylene glycol) (PEG)-based organogels are formulated in polymerizable solvents. The dynamic-covalent nature of the solvent-H-bonded Hemiaminal crosslinks, together with the modification of the crosslinking density of the organogels allows for temperature-dependent viscoelastic control. The shape of uncured gels can be permanently retained by templated UV-curing of the solvent, offering great promise for complex manufacturing, printing, sealants, and materials repair.

  • Supramolecular motifs in dynamic covalent PEG-Hemiaminal organogels
    Nature Communications, 2015
    Co-Authors: Gijs M. Ter Hurrne, Rudy J. Wojtecki, Gavin O. Jones, Hans W. Horn, E. W. Meijer, Curtis W. Frank, James L. Hedrick, Jeannette M. García
    Abstract:

    Dynamic covalent materials are stable materials that possess reversible behaviour triggered by stimuli such as light, redox conditions or temperature; whereas supramolecular crosslinks depend on the equilibrium constant and relative concentrations of crosslinks as a function of temperature. The combination of these two reversible chemistries can allow access to materials with unique properties. Here, we show that this combination of dynamic covalent and supramolecular chemistry can be used to prepare organogels comprising distinct networks. Two materials containing Hemiaminal crosslink junctions were synthesized; one material is comprised of dynamic covalent junctions and the other contains hydrogen-bonding bis-Hemiaminal moieties. Under specific network synthesis conditions, these materials exhibited self-healing behaviour. This work reports on both the molecular-level detail of Hemiaminal crosslink junction formation as well as the macroscopic behaviour of Hemiaminal dynamic covalent network (HDCN) elastomeric organogels. These materials have potential applications as elastomeric components in printable materials, cargo carriers and adhesives. Control of supramolecular chemistry and dynamic covalent crosslinking are ideal ways to generate soft materials with desirable mechanical behaviours. Here, the authors report on practical and computational methods used to elucidate the structural properties of PEG-Hemiaminal organogel networks.

  • supramolecular motifs in dynamic covalent peg Hemiaminal organogels
    Nature Communications, 2015
    Co-Authors: Courtney H Fox, Rudy J. Wojtecki, Gavin O. Jones, Hans W. Horn, E. W. Meijer, Curtis W. Frank, James L. Hedrick, Gijs M Ter Hurrne, Jeannette M. García
    Abstract:

    Dynamic covalent materials are stable materials that possess reversible behaviour triggered by stimuli such as light, redox conditions or temperature; whereas supramolecular crosslinks depend on the equilibrium constant and relative concentrations of crosslinks as a function of temperature. The combination of these two reversible chemistries can allow access to materials with unique properties. Here, we show that this combination of dynamic covalent and supramolecular chemistry can be used to prepare organogels comprising distinct networks. Two materials containing Hemiaminal crosslink junctions were synthesized; one material is comprised of dynamic covalent junctions and the other contains hydrogen-bonding bis-Hemiaminal moieties. Under specific network synthesis conditions, these materials exhibited self-healing behaviour. This work reports on both the molecular-level detail of Hemiaminal crosslink junction formation as well as the macroscopic behaviour of Hemiaminal dynamic covalent network (HDCN) elastomeric organogels. These materials have potential applications as elastomeric components in printable materials, cargo carriers and adhesives.