Hollow Filaments Synthesized by Dry-Jet Wet Spinning of Cellulose Nanofibrils: Structural Properties and Thermoregulation with Phase-Change Infills

We use dry-jet wet spinning in a coaxial configuration by extruding an aqueous colloidal suspension of oxidized nanocellulose (hydrogel shell) combined with airflow in the core. The coagulation of the hydrogel in a water bath results in hollow filaments (HF) that are drawn continuously at relatively high rates. Small-angle and wide-angle X-ray scattering (SAXS/WAXS) reveals the orientation and order of the cellulose sheath, depending on the applied shear flow and drying method (free-drying and drying under tension). The obtained dry HF show Young's modulus and tensile strength of up to 9 GPa and 66 MPa, respectively. Two types of phase-change materials (PCM), polyethylene glycol (PEG) and paraffin (PA), are used as infills to enable filaments for energy regulation. An increased strain (9%) is observed in the PCM-filled filaments (HF-PEG and HF-PA). The filaments display similar thermal behavior (dynamic scanning calorimetry) compared to the neat infill, PEG, or paraffin, reaching a maximum latent heat capacity of 170 J·g^-1 (48-55 °C) and 169 J·g^-1 (52-54 °C), respectively. Overall, this study demonstrates the facile and scalable production of two-component core-shell filaments that combine structural integrity, heat storage, and thermoregulation properties.