Endowing biodegradable plastics with easy recyclability can reduce competition with food resources and further enhance their environmental friendliness. In this work, 4-carboxyphenylboronic acid was grafted onto the side chains of hydroxyethyl cellulose and compounded with inexpensive cornstarch. Upon the introduction of tannic acid, stable and reversible borate ester bond rapidly formed, yielding composite biodegradable plastic films with outstanding mechanical properties and facile recyclability. The formation of a dynamic cross-linked network mitigates the aggregation of gelatinized starch molecules, enhancing the flexibility and durability of the crosslinked film. Testing revealed that while maintaining high tensile strength, the elongation at break of the crosslinked film increased by 952.86 %. The static water contact angle was improved from 32.74° to 78.82°, with a change of <5° within 1 min, demonstrating enhanced water resistance. Excellent antioxidant and thermal stability were also characterized, the crosslinked film can be easily dissolved by heating in water at pH = 6.5 and reshaped in water at pH = 7.2. After five times of regeneration, the tensile strength loss was as low as 5.68 %. This eco-friendly and efficient recycling process is promising during green chemistry.
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