High‐Performance Recycling Biobased Photopolymers for 3D Printing

ABSTRACT Developing recycling photo‐curing 3D printing materials (especially using renewable biobased feedstocks) can greatly alleviate environmental burden raised by the rapid development of 3D printing industry. Currently, it is still hard to achieve both high performance and excellent recyclability for such materials. In this study, by using a typical biobased phenol (i.e., eugenol) as starting material, we design biobased photopolymers containing dynamic dissociative phenol‐carbamate bonds, part of which come from the phenol itself. The obtained materials not only have relatively high biobased contents, but also demonstrate excellent thermal and mechanical properties. Subsequently, the materials are conveniently recycled by a proposed “mixed‐monomer assisted recycling” strategy, and high recovery efficiencies in at least three cycles were achieved. Furthermore, the materials indicate exceptional 3D printing performance and functionalities (such as oral bacteria inhibition and shape memory) as well as low environmental impacts. Overall, the combination of rigid biobased feedstocks (especially biobased phenols) and suitable dissociative covalent bonds offers the opportunity to develop high performance, recycling photopolymers with more functionalities and better sustainability.