Directional-Freezing-Enabled MXene Orientation toward Anisotropic PVDF/MXene Aerogels: Orientation-Dependent Properties of Hybrid Aerogels

Polymer hybrid materials that contain reinforcements with a preferred orientation have received growing attention because of their unique properties and promising applications in multifunctional fields. Herein, anisotropic poly(vinylidene fluoride) (PVDF)/MXene hybrid aerogels with highly ordered delaminated MXene nanosheets and anisotropic porous structures were successfully fabricated by unidirectional freezing of thermoreversible gels followed by a freeze-drying process. The strong interfacial interactions between PVDF chains and abundant functional groups on the surface of MXene enabled the orientation of MXene nanosheets at the boundaries of ice crystals as the semicrystalline PVDF and delaminated MXene nanosheets are squeezed along the freezing direction. These aerogels display distinct properties along the freezing and perpendicular to the freezing (transverse) directions. These anisotropic aerogels are flexible and flame-retardant and possess an anisotropic compression performance, heat transfer, electrical conductivity, and electromagnetic interference (EMI) shielding. Further, by increasing the MXene loadings, the electrical conductivity and EMI shielding performances of hybrid aerogels were significantly improved. The PVDF aerogel showed sticky hydrophobicity with a contact angle of 139°, whereas the contact angle increased significantly in hybrid aerogels (153°) with low water adhesion, making them suitable as self-cleaning materials. The combination of the above characteristics makes these hybrid aerogels potential candidates for a wide range of electronic applications.