Ultratough, Processable Bioplastics Enabled by Triple Interlocking of Lignin and Cellulose

JS Sun and HZ Huang and W Wang and Y Liu and XY Lv and Z Yin and WJ Bi and ZH Zheng and X Yang and ZH Tong and S Liu and JJ Liu and JN Liu and ZY Hou and ZQ Pang and HP Yu and QQ Xia, ACS NANO, 19, 29360-29371 (2025).

DOI: 10.1021/acsnano.5c06221

Sustainable and biodegradable bioplastics from natural lignocellulose offer a promising alternative to petroleum-based plastics, yet they often exhibit limited toughness and processability due to the inherent rigidity of polymer segments. Herein, we have developed a triple interlocking strategy to fabricate a high-strength, ultratough, and processable Bioplastic (denoted as CEL Bioplastic) from cellulose and lignin in the pulp/paper industry. In this process, we leverage room- temperature esterification of long-chain fatty acids with cellulose and lignin to produce a fully biobased CEL Bioplastic, distinguished by a robust triple-interlocking architecture that combines robust physical chain entanglements, cross-linked ester bonds, and densely packed hydrogen bonds. Physical chain entanglements in CEL Bioplastic efficiently distribute tension, while ester bonds and hydrogen bonds work synergistically to prevent chain disentanglement and enhance energy dissipation. The resulting CEL Bioplastic exhibits exceptional mechanical properties, with a tensile strength of similar to 200 MPa, a fracture strain of similar to 75% and an impressive toughness of similar to 110 MJ/m(3). These values are competitive to cellulose-lignin Bioplastic (denoted as CL Bioplastic) lacking long-chain entanglements and ester bonds, in tensile strength (15 times) but far exceed them in toughness (44 times). Moreover, long alkyl substituents exert an internal plasticizing effect, enabling CEL Bioplastics to form 3D structures through simple thermal or water-assisted shaping process. Such CEL Bioplastic exhibits biodegradability, recyclability and scalability (>4m in length), offering a sustainable pathway for producing high-performance bioplastics from natural biopolymers for functional and structural applications.

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