With
the advancement of additive manufacturing (AM) and
the mass
adoption of 3D printing technology, it is essential to shift focus
to environmentally and economically sustainable materials. As the
utilization of renewable feedstocks is quite limited in this context,
the utilization of more bio-based raw materials in the ongoing development
of AM represents an essential means of achieving this shift. In this
work, vat photopolymerization 3D printing has been used to process
vegetable oil-based (VO) resins with an ultralow concentration of
0.07 vol % nanocellulose fibrils (NFC) and crystals (NCC). The developed
nanocellulose containing bio-based vat photopolymerization resin shows
excellent shelf stability, enabling high-resolution printing. Compatibilization
of the nanocellulose with the polymer matrix was achieved through
the introduction of isocyanate or acrylate groups via reactions of
acryloyl chloride (AC) and hexamethylene diisocyanate (HMDI) with
cellulose surface hydroxyls. Surface functionalization results in
∼20–30% increases in interfacial adhesion and stress
transfer, yielding significant improvements in mechanical performance
(4× higher toughness, 2.4× higher tensile strength, and
2× higher tensile strain) in 3D-printed specimens. Fourier-transformation
infrared (FTIR) spectroscopy complemented by solid-state nuclear magnetic
resonance (NMR) techniques enabled a more detailed study of the chemical
structure of these materials as well. Tensile performance comparison
with literature data on VO-based natural fiber-reinforced resins showed
that this work brought bio-based resins one step closer to competing
with petroleum-based resins. The prepared VO/nanocellulose resins
are promising candidates for high-performance bio-based resins derived
from completely renewable feedstocks.