The
flow-induced supramolecular arrangement, or band texture, present
in water-soluble anisotropic films prepared from blend solutions of
hydroxypropyl cellulose and organosolv lignin is locked via esterification
with bio-based polycarboxylic acids. Subsequent to shear casting of
the blend solutions, the chemical cross-linking with citric acid-based
cross-linkers and a dimerized fatty acid yields water-insoluble, anisotropic
films prone to swelling in water. The liquid crystalline networks
are analyzed by means of polarized optical microscopy, tensile testing,
Fourier transform infrared, and swelling experiments. Depending on
the cross-linker, the dry “banded” films reach up to
3.5 GPa in tensile modulus, 80 MPa in tensile strength along the shear
direction, and 5 MJ/m3 toughness across the shear direction.
Films are softened upon water uptake causing a reversible extinguishment
of the banded texture without interfering with the specimens’
anisotropy. Rheological studies point to the applicability of highly
concentrated blend solutions to direct ink writing. The implementation
of the findings to the additive manufacturing of cross-linked 3D structures
demonstrates the potential of a resource-friendly processing of fully
bio-based materials.