Recyclable materials with simultaneous multifunctionality and high performance, especially polymers synthesized from biobased monomers, have recently attracted a great deal of interest. However, current traditional vitrimers exhibit trade-offs between high performance and reprocessing. To circumvent this inherent contradiction, we report the first attempt to introduce an aromatic N-heterocycles (the fixed ‘stiff’ segments) derived from biomass functionalized with ester groups (the dynamic ‘flexible’ segments) into a thermoset system. The resulting resins exhibited high flexural strength (151 MPa) and toughnesses, a high glass transition temperature (205 ℃), intrinsic flame retardancy (UL-94 V-0) and acid/base resistance. In addition, the ester groups and aromatic N-heterocycles enabled dissolution of the network in ethylene glycol without additional catalyst. Importantly, the degradation solution could be directly reused into high-value photothermal conversion coatings and adhesives with 100% recyclability just by evaporating the ethylene glycol at elevated temperatures. Additionally, the conjugated aromatic N-heterocycles enhanced the adhesive properties and photothermal conversion of the system. The ease with which biobased materials bearing N-heterocycles and ester groups can be synthesized, recycled, and reused without losing value provides a new direction for closed-loop, high-performance and versatile polymer life cycles.

同时具有多功能和高性能的可回收材料，特别是从生物基单体合成的聚合物，最近引起了人们的极大兴趣。然而，目前传统的 vitrimers 在高性能和再加工之间表现出权衡。为了规避这种固有的矛盾，我们报告了首次尝试将源自用酯基团（动态“柔性”部分）功能化的生物质的芳族 N- 杂环（固定“刚性”部分）引入热固性系统。所得树脂表现出高弯曲强度 (151 MPa) 和韧性、高玻璃化转变温度 (205 ℃)、固有阻燃性 (UL-94 V-0) 和耐酸/碱性能。此外，酯基和芳族 N-杂环使网络能够在没有额外催化剂的情况下溶解在乙二醇中。重要的是，只需在高温下蒸发乙二醇，降解溶液就可以直接重新用于具有 100% 可回收性的高价值光热转换涂层和粘合剂。此外，共轭芳族N-杂环增强了系统的粘合性能和光热转化。带有 N-杂环和酯基团的生物基材料可以很容易地合成、回收和再利用而不会损失价值，这为闭环、高性能和多功能聚合物生命周期提供了新的方向。只需在高温下蒸发乙二醇，降解溶液就可以直接重新用于高价值的光热转换涂层和粘合剂，具有 100% 的可回收性。此外，共轭芳族N-杂环增强了系统的粘合性能和光热转化。带有 N-杂环和酯基团的生物基材料可以很容易地合成、回收和再利用而不会损失价值，这为闭环、高性能和多功能聚合物生命周期提供了新的方向。只需在高温下蒸发乙二醇，降解溶液就可以直接重新用于高价值的光热转换涂层和粘合剂，具有 100% 的可回收性。此外，共轭芳族N-杂环增强了系统的粘合性能和光热转化。带有 N-杂环和酯基团的生物基材料可以很容易地合成、回收和再利用而不会损失价值，这为闭环、高性能和多功能聚合物生命周期提供了新的方向。