Vats S., Khodayari A., Mugemana C., Spirk S., Schnell C.N., Seveno D., Fuentes C.A.
Carbohydrate Polymers, vol. 381, art. no. 125204, 2026
Cellulose acetate (CA) enables the production of cellulose nanofibers via electrospinning, overcoming the solubility limits of native cellulose. However, rapid regeneration of CA into cellulose remains a bottleneck for scalable manufacturing. We evaluated three regeneration methods: immersion, vapour exposure, and spray, targeting near-instant deacetylation of electrospun CA fibres. Immersion was the most effective: 0.5 N KOH in ethanol with 5% ( v /v) water achieved complete deacetylation in 30 s. Water was essential, promoting ion mobility and hydrolysis while preserving fibre integrity. FTIR and solid-state <sup>13</sup>C NMR confirmed acetyl removal, and SEM showed preserved morphology. WAXD indicated that cellulose II order developed on ~1 h timescales. Tensile tests showed immediate gains in modulus and strength after 30 s, while longer exposure improved order without further strengthening. Molecular dynamics simulations revealed how acetylation degree affects hydroxymethyl conformation, hydrogen bonding, and cellulose II-like arrangements. Low-substituted CA chains showed higher hydrogen-bond density and better structural properties, especially in hydrated environments. These findings show that full crystallinity is unnecessary for strong mechanical performance, challenging the assumption that ordered cellulose II structures are essential. Combining fast chemistry with minimal fibre damage, this approach integrates electrospinning and regeneration into a single, scalable process for sustainable cellulose materials.
