A continuous
and scalable method for the wet spinning of cellulose nanofibrils
(CNFs) is introduced in a core/shell configuration. Control on the
interfacial interactions was possible by the choice of the shell material
and coagulant, as demonstrated here with guar gum (GG) and cellulose
acetate (CA). Upon coagulation in acetone, ethanol, or water, GG and
CA formed supporting polymer shells that interacted to different degrees
with the CNF core. Coagulation rate was shown to markedly influence
the CNF orientation in the filament and, as a result, its mechanical
strength. The fastest coagulation noted for the CNF/GG core/shell
system in acetone led to an orientation index of ∼0.55 (Herman’s
orientation parameter of 0.40), Young’s modulus of ∼2.1
GPa, a tensile strength of ∼70 MPa, and a tenacity of ∼8
cN/tex. The system that underwent the slowest coagulation rate (CNF/GG
in ethanol) displayed a limited CNF orientation but achieved an intermediate
level of mechanical resistance, owing to the strong core/shell interfacial
affinity. By using CA as the supporting shell, it was possible to
spin CNF into filaments with high water absorption capacity (43 g
water/g dry filament). This was explained by the fact that water (used
as the coagulant for CA) limited the densification of the CNF core
structure, yielding filaments with high accessible area and pore density.