A hybrid material of polyaniline protonated with hydrochloric acid and conductive graphene nanosheets (PANi/GNs) has been prepared by an in situ chemical polymerization method. The interactions between PANi and GNs in the hybrid composites are investigated by utilizing XRD, FT-IR, UV–vis and Raman. It is found that the PANi are adsorbed on the surface of the GNs, and the morphology of PANi transforms from twist structure to extended structure after the GNs are introduced. The thermoelectric (TE) properties of PANi/GNs composites have been investigated in the range from 323 K to 453 K. The electrical conductivity and the Seebeck coefficient of PANi/GNs composites are obviously higher than those of the PANi, while the thermal conductivity of the composites still keeps relatively low values even with high GNs content, resulting in the increase in dimensionless figure of merit (ZT). A highest ZT value of 1.95 × 10−3 has been obtained for the composite containing 30 wt % GNs at 453 K, which is about 70 times higher than that obtained from the PANi. PANi adsorbed on the surface of the GNs possesses more extended structure. Electrical conductivity and Seebeck coefficient of PANi/GNs composites are superior to those of PANi. Thermal conductivity of the composites still keeps relatively low values.
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