Abstract Permanently crosslinked polymer networks, such as fully cured thermosets derived from fossil-based epoxies, cannot be reuse after damage and/or recycled since they cannot be reprocessed by heating or solubilization as non-crosslinked thermoplastics. As a result, they are not really sustainable materials, generating non-renewable resources consumption, CO2 emissions and plastic pollution. Herein we employed a strategy to tackle the lack of sustainability in conventional thermosets by the development of a promising partially biobased epoxy for numerous applications, integrating a covalent adaptable network using associative dynamic chemistry and catalyst free mechanism. This strategy is based in two sustainable approaches. First, vegetal biomass has been used as a renewable resource for the synthesis of epoxy systems from epoxidized eugenol oil. Then, the crosslinking reaction with a diamine integrating disulfide bonds to attain a thermally induced reorganizable eugenol-derived epoxy network in a dynamic way by disulfide metathesis reaction. The viscoelastic behavior characterization of eugenol-derived epoxy network displays a fast macroscopic flow with a stress relaxation time of 37 s at 230 °C, suggesting an interesting melt-reprocessability of this network at high temperatures in short times. Moreover, this strategy has a strong potential for the progress of sustainable plastic applications as yield a synthetic procedure to develop stiff thermosets (storage modulus of around 1 GPa at glassy state) with high renewable carbon contents (around 70 wt%), enhanced thermal properties (Tg of around 190 °C) and additional properties such as promising reshaping, repairing and recycling capability.

中文翻译：

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基于丁香酚衍生环氧树脂的动态网络作为有前途的可持续热固性材料

摘要永久交联的聚合物网络，例如源自化石基环氧树脂的完全固化的热固性塑料，在损坏和/或回收后不能再利用，因为它们不能作为非交联热塑性塑料通过加热或溶解进行再加工。因此，它们并不是真正的可持续材料，会产生不可再生资源消耗、二氧化碳排放和塑料污染。在此，我们采用了一种策略来解决传统热固性塑料缺乏可持续性的问题，通过开发一种用于众多应用的有前途的部分生物基环氧树脂，使用关联动态化学和无催化剂机制整合共价适应性网络。该战略基于两种可持续的方法。第一的，植物生物质已被用作可再生资源，用于从环氧化丁香酚油合成环氧体系。然后，与整合二硫键的二胺进行交联反应，通过二硫键复分解反应以动态方式获得热诱导的可重组丁香酚衍生的环氧网络。丁香酚衍生的环氧树脂网络的粘弹性行为表征显示出快速的宏观流动，在 230°C 下应力松弛时间为 37 秒，表明该网络在短时间内在高温下具有有趣的熔融可再加工性。此外，该策略对于可持续塑料应用的发展具有巨大的潜力，因为它产生了一种合成程序来开发具有高可再生碳含量（约 70 wt%）的刚性热固性塑料（玻璃态下的储存模量约为 1 GPa）