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Improving the adhesion properties of carbon nanotubes (CNTs) at the molecular scale can significantly enhance dispersion of CNT fibers in polymer matrix and unleash the dormant extraordinary mechanical properties of CNTs in CNT-polymer nanocomposites. Inspired by the outstanding adhesion, dispersion, mechanical, and surface functionalization properties of crystalline nanocellulose (CNC), this paper studies the mechanical and adhesion properties of CNT wrapped by aligned cellulose chains around CNT using molecular dynamic simulations. The strength, elastic modulus, and toughness of CNT-cellulose fiber for different cellulose contents are obtained from tensile and compression tests. Additionally, the effect of adding cellulose on the surface energy, interfacial shear modulus, and strength is evaluated. The result shows that even adding a single layer cellulose wrap (≈55% content) significantly decreases the mechanical properties, however, it also dramatically enhances the adhesion energy, interfacial shear strength, and modulus. Adding more cellulose layers, subsequently, deceases and increases mechanical properties and adhesion properties, respectively. In addition, analysis of nanopapers of pristine CNT, pristine CNC, and CNT-wrapped cellulose reveals that CNT-wrapped cellulose nanopapers are strong, stiff, and tough, while for CNT and CNC either strength or toughness is compromised. This research shows that cellulose wraps provide CNT fibers with tunable mechanical properties and adhesion energy that could yield strong and tough materials due to the excellent mechanical properties of CNT and active surface and hydrogen bonding of cellulose.

Tuning the Mechanical and Adhesion Properties of Carbon Nanotubes Using Aligned Cellulose Wrap (Cellulose Nanotube): A Molecular Dynamics Study