Green and stable lignin-based nanofillers reinforced poly(l-lactide) with supertough and strong performance

Lignin nanoparticles (LNPs), as a new type of green nanomaterial, initiate many promising applications in polymer composites. However, their heterogeneity, dissolution in organic solvents, and poor compatibility in the polymer matrix greatly limited the applications of LNPs fillers. Herein, we proposed an antisolvent precipitation of the fractionations by combining a hydrothermal treatment-assisted synthesis to fabricate self-crosslinked LNPs (ScLNPs), which have good stability in the organic solvent and controllable sizes. After surface grafting modification with d-lactide, ScLNPs-graft-poly(d-lactide) (ScLNPs-g-PDLA) exhibited excellent dispersion and compatibility in PLLA matrix. Using the rational design and addition of ScLNPs-g-PDLA fillers, the strength and toughness of the generated PLLA composite reached 31.6 MPa and 396 % (the highest value among the PLLA materials), respectively. Furthermore, the mechanical performance can also be well-tuned by the sizes and amounts of LNPs fillers. This strategy involving only green and recyclable materials provides an effective route to producing sustainable polymeric plastics with integrated strength and super-toughness.