Recyclable, reprocessable, and biodegradable cellulosic bioplastics enabled by a reactive eutectic network

Abstract

Growing demand for sustainable, high-performance materials is driving research to replace petroleum-based plastics with abundant biomass, especially cellulose. However, the effective modification and functionalization of cellulose is often impeded by complex processing requirements and limited performance tunability. Here, an innovative “active” green medium strategy based on an ethyl cellulose/thymol eutectic system is reported, enabling in situ chemical modification of eutectic components and the construction of dynamic self-adaptive networks without external catalysts or initiators. Through precise molecular design, dynamic boroxine networks and acrylate crosslinking networks are synergistically integrated into the cellulosic bioplastic (CBP) matrix. The resulting CBP-A₂B₈ exhibits exceptional optical transparency (∼85%), superior mechanical properties (tensile strength ∼30 MPa), facile thermal processability, and closed-loop recyclability. Its chemical structure and mechanical performance remain highly stable even after 20 hot-compression recycling cycles. Complete biodegradation occurs under natural environmental conditions within approximately 100 days. Furthermore, the bioplastic, when combined with silver nanowires, forms high-performance flexible transparent conductive films successfully applied in customizable electroluminescent devices. Post-lifecycle, device components (silver nanowires and CBP matrix) are efficiently separated and recycled using a straightforward solvent-based method. This eutectic system-mediated strategy offers a novel pathway for the development of sustainable, high-performance bioplastics with a closed-loop lifecycle.