Lignin, a bio-derived and highly aromatic macromolecule has been identified as a potentially valuable source for next-generation of bio-derived structural materials. The complex agglomerated molecular architecture and compositional variability limit its use as a component for high-performance materials. Here we report simple chemistries that utilize the inherently rich lignin functionalities to induce nanoscale dispersion of lignin agglomerates and synthesize high-strength renewable lignin compositions. Monomeric di and tri-carboxylic acid derivatives with varying molecular architectures act as esterifying crosslinkers in an equal mass mixture of lignin and acrylonitrile−butadiene copolymers in a highly scalable, solvent-free process. These “inverse thermoplastic vulcanizates” (iTPVs) unique in their approach of crosslinking the rigid lignin phase rather than the soft phase exhibit ordered self-assembly and tunable nanoscale morphology. Using advanced bimodal dual AC atomic force microscopy and coarse-grained molecular dynamics simulations, we observe that the morphology and properties of iTPVs are strongly correlated to the architecture of the utilized monomers. We discuss how these approaches can be extended to synthesize reinforced composite materials with superior strength. We explore tailoring lignin functionality for the synthesis of polymeric materials with enhanced strain hardening behavior, as well as vitrimeric materials with enhanced creep resistance and reprocessability. Thus, a greater understanding of lignin self-assembly can help us exploit processing and chemistries to synthesize tailored lignin-derived polymers with superior properties that ultimately contribute to its greater utilization.

Upcycling lignin into high-performance polymers with tailored morphology and properties

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ACS Fall 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.