One-pot lignocellulosic bioplastic synthesis through in situ deconstruction of deep eutectic solvents

Abstract

Conventional lignocellulose processing suffers from multi-step, energy-intensive pulping methods or structural degradation under harsh dissolution conditions, limiting efficient biomass valorization. To address this, we developed a deep eutectic solvent (DBNACl/MeC) that achieves efficient and protective dissolution of lignocellulose through in situ deconstruction, eliminating the need for pretreatment. The solvent combines a superbase ionic liquid-based hydrogen bond acceptor with a methyl carbazate-based hydrogen bond donor that thermally deconstructs to release methylamine, which simultaneously cleaves lignin–carbohydrate complex ester linkages and disrupts the physical hierarchy of the biomass. The DBNACl/MeC system achieves complete dissolution of bagasse, while maintaining a high cellulose polymerization degree and suppressing lignin condensation. Water regeneration yields films with high mechanical strength, thermal stability, and UV shielding performance. Additionally, the solution can be processed into coatings to reinforce paper/wood composites. This work not only provides an efficient green solvent for biomass processing, but also demonstrates a practical pathway for upcycling low-value agricultural residues into high-performance, multifunctional materials, offering substantial potential for sustainable biomanufacturing.