Biobased recyclable materials offer exciting opportunities as a reliable alternative to fossil fuel-based engineering plastics, but wider acceptance of these materials is often limited because of tedious synthesis routes and limited tunability of these materials. Here-in, a series of Lignin-Epoxidized natural rubber vitrimers with dynamic ester bonds were synthesized through a solvent-free high-temperature dynamic heat treatment procedure followed by a post-curing step. The multifunctional polyphenolic structure of lignin assisted in higher reactivity and imparting stiffness to the overall material matrix. The lignin content in the matrix was varied from 25% to 50% to demonstrate that the mechanical properties of the vitrimer can be tailored in a facile way. The results demonstrated that the glass-transition temperature (T<sub>g</sub>), modulus, tensile properties and crosslinking degree increased substantially with increase in lignin content. Moreover, lignin-rubber based crosslinked material exhibited fast stress relaxation above 150 Celsius enabling shape-memory, self-healing and malleability of the bio-based material. In addition, recyclability and stability of lignin derived vitrimer in different aqueous environment, ranging from basic to acidic, further indicates a promising potential of this material for use as a sustainable recyclable material.

Lignin derived fully biobased vitrimer with tunable mechanical properties

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ACS Fall 2022

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