Anisotropic polymer composites synthesized by immobilizing cellulose nanocrystal suspensions specifically oriented under magnetic fields.

Novel polymer composites reinforced with an oriented cellulose nanocrystal (CNC) assembly were prepared from suspensions of CNC in aqueous 2-hydroxyethyl methacrylate (HEMA) via magnetic field application to the suspensions followed by polymerization treatment. The starting suspensions used at ∼6 wt % CNC separated into an upper isotropic phase and a lower anisotropic (chiral nematic) one in the course of quiescent standing. A static or rotational magnetic field was applied to the isolated isotropic and anisotropic phases. UV-induced polymerization of HEMA perpetuated the respective states of magnetic orientation invested for the CNC dispersions to yield variously oriented CNC/poly(2-hydroxyethyl methacrylate) composites. The structural characterization was carried out by use of X-ray diffractometry and optical and scanning electron microscopy. The result indicated that CNCs were aligned in the composites distinctively according to the static or rotational magnetic application when the anisotropic phases were used, whereas such a specific CNC orientation was not appreciable when the isotropic phases were sampled. This marks out effectiveness of a coherent response of CNCs in the mesomorphic assembly. In dynamic mechanical experiments in tensile or compressive mode, we observed a clear mechanical anisotropy for the polymer composites synthesized from wholly anisotropic suspensions under static or rotational magnetization. The higher modulus (in compression) was detected for a composite reinforced by locking-in the uniaxial CNC alignment attainable through conversion of the initial chiral nematic phase into a nematic phase in the rotational magnetic field.