Thermoformed, thermostable, waterproof and mechanically robust cellulose-based bioplastics enabled by dynamically reversible thia-Michael reaction.

Cellulose is a renewable biodegradable polymer derived from abundant natural resources. Substituting petroleum-based polymers with cellulose-based bioplastics is an effective way to alleviate environmental issues like resource depletion and white pollution. However, challenges such as poor thermostability, difficulty in thermoforming and water sensitivity seriously hinder the fabrication and use of cellulose-based bioplastics. Herein, a thermoformed, thermostable, waterproof and mechanically robust cellulose-based bioplastic (H-HEC) is fabricated by introducing thia-Michael-based reversible crosslinked structure into hydroxyethyl cellulose. This is the first instance of integrating thia-Michael-based crosslinked structure into cellulose derivatives. The resulting H-HEC can be thermoformed and remolded without adding any plasticizers. Besides, the obtained H-HEC exhibit excellent overall properties, such as a high thermal decomposition temperature of 366 °C, a high water contact angle of 108°, a high transmittance of 90 % and good mechanical properties. Additionally, H-HEC combines impressive transparency with effective UV-shielding properties. We envision that this work provides a novel method to prepare thermoformable cellulose-based bioplastics with good water resistance, thermostability, transparency and mechanical properties. The combined thermoformability and superior overall performances will promote the practical application of cellulose-based bioplastics and contribute to the replacement of petroleum-based polymer by cellulose-based bioplastics.