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Vitrimers are polymer networks that, thanks to covalent bond exchange,combine desirable properties of thermoplastic and thermosets, such asflowability and insolubility. For this reason, vitrimers are considered to begood candidates for a number of innovative applications from self-healing softrobots to hard reprocessable materials. All these applications are related tothe unusual thermomechanical behavior of vitrimers, consequence of thenon-trivial interplay between the polymer network dynamics and the thermallyactivated chemical link exchange. Here we use solid-state rheology toinvestigate the properties of a recently developed epoxy-based vitrimer. Therheological analysis demonstrates that the mechanical spectrum is composed oftwo relaxation processes with distinct activation energies which are associatedwith glass dynamics and covalent bond exchange, respectively. This makes thematerial thermo-rheologically complex and time temperature equivalence does notapply. Nonetheless, thanks to mechanical spectral analysis in a wide range ofstiffness, time and temperature, we are able to depict thetime-temperature-relaxation landscape in an enough precise way to account forthe two dynamical processes and recombine them to predict the mechanical moduliin a wide (virtually unlimited) interval of frequencies, from low temperatures(close to room temperature) to high temperatures (above the Tg).

Resolving the relaxation complexity of vitrimers: time-temperature superpositions of a time-temperature non-equivalent system