A general method to prepare polymer gels containing anisotropically oriented graphene oxide (GO) or reduced graphene oxide (RGO) was developed, by using the magnetically induced orientation of GO. Under a magnetic field, an aqueous dispersion of GO was gelated by in situ cross-linking polymerization of an acryl monomer and a cross-linker. In the resultant hydrogel, the orientation of GO was retained even in the absence of the magnetic field, because the gel network trapped GO via noncovalent interactions and efficiently suppressed the structural relaxation of GO. The locked structure enabled quantitative investigation on the magnetic orientation of GO using 2D small-Angle X-ray scattering, which revealed that GO nanosheets orient parallel to the magnetic field with an order parameter of up to 0.80. Systematic studies with varying gelation conditions indicate that the present method can afford a wide range of GO-hybridized anisotropic materials, in terms of GO alignment direction, sample shape, and GO concentration. Also by virtue of the locked structure, the orientation of GO in the hydrogel was well preserved throughout the in situ chemical reduction of GO, yielding an RGO-hybridized anisotropic hydrogel, as well as the conversion of the hydrogel into organo- and ionogels through the replacement of the internal water with solvents. As a preliminary demonstration of the present method for practical application, a polymer-composite film containing RGO oriented vertical to the film surface was prepared, and its anisotropically enhanced electroconductivity along the orientation direction of RGO was confirmed by the flash-photolysis time-resolved microwave conductivity measurement.
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