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Vitrimers with bond exchange reactions (BERs) are a class of covalent adaptable network (CAN) polymers at the forefront of recent polymer research. They exhibit malleable and self-healable behaviors and combine the advantages of easy processability of thermoplastics and excellent mechanical properties of thermosets. For thermally sensitive vitrimers, a molecular topology melting/frozen transition is triggered when the BERs are activated to rearrange the network architecture. Notable volume expansion and stress relaxation are accompanied, which can be used to identify the BER activation temperature and rate as well as to determine the malleability and interfacial welding kinetics of vitrimers. Existing works on vitrimers reveal the rate-dependent behaviors of the nonequilibrium network during the topology transition. However, it remains unclear what the quantitative relationship with heating rate is, and how it will affect the macroscopic stress relaxation. In this paper, we study the responses of an epoxy-based vitrimer subjected to a change in temperature and mechanical loading during the topology transition. Using thermal expansion tests, the thermal strain evolution is shown to depend on the temperature-changing rate, which reveals the nonequilibrium states with rate-dependent structural relaxation. The influences of structural relaxation on the stress relaxation behaviors are examined in both uniaxial tension and compression modes. Assisted by a theoretical model, the study reveals how to tune the material and thermal-temporal conditions to promote the contribution of BERs during the reprocessing of vitrimers. 

Vitrimers have the characteristics of shape-reforming and surface-welding, and have the same excellent mechanical properties as thermosets; so vitrimers hold the promise of a broad alternative to traditional plastics. Since their initial introduction in 2011, vitrimers have been applied to many unique applications such as reworkable composites and liquid crystal elastomer actuators. A series of experiments have investigated the effects of reprocessing conditions (such as temperature, time, and pressure) on recycled materials. However, the effect of particle size on the mechanical properties of recycled materials has not been reported. In this paper, we conducted an experimental study on the recovery of epoxy-acid vitrimers of different particle sizes. Epoxy-acid vitrimer powders with different particle size distributions were prepared and characterized. The effects of particle size on the mechanical properties of regenerated epoxy-acid vitrimers were investigated by dynamic mechanical analysis and uniaxial tensile tests. In addition, other processing parameters such as temperature, time, and pressure are discussed, as well as their interaction with particle size. This study helped to refine the vitrimer reprocessing condition parameter toolbox, providing experimental support for the easy and reliable control of the kinetics of the bond exchange reaction. 

Abstract The chemically crosslinked network structures make epoxies, the most common thermosets, unable or hard to be recycled, causing environmental problems and economic losses. Epoxy‐based vitrimers, polymer networks deriving from epoxy resins, can be thermally malleable according to bond exchange reactions (BERs), opening the door to recycle epoxy thermosets. Here a series of experiments were carried out to study the effects of processing conditions (such as particle size distributions, temperature, time, and pressure) on recycling of an epoxy‐anhydride vitrimer. Polymer powders from the epoxy‐anhydride vitrimer with different size distributions were prepared and characterized, and the influence of particle size on the mechanical performance of recycled epoxy‐anhydride vitrimers was investigated by dynamic mechanical analysis and uniaxial tensile test. Experimental results demonstrated that finer polymer powders can increase the contacting surfaces of recycled materials and thus result in high quality of recycled materials. In addition, the influences of other treating parameters, such as temperature, time, and pressure, were also discussed in this study. Adjusting these treating parameters can help the design of an optimized reprocessing procedure to meet practical engineering applications.