Multi-Modal Melt-Processing of Birefringent Cellulosic Materials for Eco-Friendly Anti-Counterfeiting.

ABSTRACT

Ubiquitous anti-counterfeiting materials with a rapidly rising annual consumption (over 1010 m2) can pose a serious environmental burden. Biobased cellulosic materials with birefringence offer attractive sustainable alternatives, but their scalable solvent-free processing remain challenging. Here, a dynamic chemical modification strategy is proposed for multi-modal melt-processing of birefringent cellulosic materials for eco-friendly anti-counterfeiting. Relying on the thermal-activated dynamic covalent-locking of the spatial topological structure of preferred oriented cellulose, the strategy balances the contradiction between the strong confinement of long-range ordered structures and the molecular motility required for entropically-driven reconstruction. Equipped with customizable processing forms including mold-pressing, spinning, direct-ink-writing, and blade-coating, the materials exhibit a wide color gamut, self-healing efficiency (94.5%), recyclability, and biodegradability. Moreover, the diversified flexible elements facilitate scalable fabrication and compatibility with universal processing techniques, thereby enabling versatile and programmable anti-counterfeiting. The strategy is expected to provide references for multi-modal melt-processing of cellulose and promote sustainable innovation in the anti-counterfeiting industry.