Controlling the cell and surface architecture of cellulose nanofiber/PVA/ Ti3C2TX MXene hybrid cryogels for optimized permittivity and EMI shielding performance

Anisotropic, nanoporous structures are promising materials for manipulating the propagation of electromagnetic waves at millimeter and sub-THz frequencies as well as for electromagnetic interference (EMI) shielding with rapidly evolving green electronics. In this work, cell and surface architecture of sustainable hybrid cryogels of cellulose nanofibers, polyvinyl alcohol (PVA) and Ti₃C₂TX MXene was controlled to adjust their GHz and THz dielectric permittivity and EMI shielding performance. Temperature gradient freeze-drying was used to obtain aligned honeycomb and lamellar pore structures with specific surface layer designs. The millimeter wave permittivity varied relative to thickness direction as the side of cryogels that was directly exposed to cold gradient had systematically a higher permittivity. This anisotropy was caused by a thin, smooth outermost surface layer covering the open core structure. The surface designs of all cryogels dominated signal permittivity, and the effects of higher MXene dosages could be offset by the surface layer. Cryogels with dense surface layer containing 70 and 50 wt % of MXene displayed very high average attenuation levels of 52.1 and 37.2 dB, respectively. Overall, the results show that the structural design of porous hybrid material can be used to adjust their EMI shielding performance at GHz and THz frequencies.