Recyclable Cellulose Fiber Reinforced Vitrimer Composite

Abstract

Vitrimer is an innovative class of polymeric materials which demonstrates traditional thermoset-like mechanical and chemical resilience while still being able to flow on demand like a traditional thermoplastic through covalently adaptive dynamic linkages. Herein, high-performance cellulose fiber reinforced vitrimer composites are developed using an epoxy-based vitrimer and natural cellulose paper. The reinforced vitrimer composite was fabricated by impregnating the porous structure of cellulose paper with two curable monomers, followed by in-situ polymerization of the monomers inside the fibrous scaffold. The introduction of hydroxyl group present on the cellulosic framework assisted in a faster topological rearrangement of the crosslinked matrix through transesterification exchange reaction, thus imparting various sought-after properties like shape recovery and recyclability via simple thermal reprocessing. Moreover, the reinforced vitrimer composite exhibits superior tensile properties as high as 90 MPa with 15-25 volume% vitrimer loading due to the interfacial adhesion via ester exchange reaction between the epoxy matrix and functionalities on the cellulosic fibers. Noteworthily, the key ingredients of the resulting composite (i.e., epoxy-based vitrimer and cellulose fibers) can be comfortably recycled without using aggressive chemical treatment, enabling composite to be easily recycled or disposed of at the end of service life and assist in reducing the subsequent manufacturing cost. This study would shed light on the development of a recyclable polymer composite with exceptional mechanical properties while simultaneously demonstrating self-healing and shape memory capabilities.