Although highly loaded graphitic nanocarbon materials effectively enhance the electrical, mechanical, and thermal properties of polymeric materials, their practical implementation has been hindered by severe aggregation issues. Here, we propose a method to achieve homogeneous nanocarbon-polyimide (PI) composites by integrating graphene oxide nanoribbons (GONRs) with polyamic acid ammonium (PAA) salt, a precursor of PI. Self-assembled scaffold structure of GONRs hydrogel enables the uniform integration and immobilization of PAA within the GONR scaffold, mitigating aggregation concerns. The resulting GONR/PAA hydrogel, formed through physical interactions, can be coated onto substrates via a shear stress-induced bar coating method due to its viscoelastic rheological properties. Subsequent heat treatment at 400 °C triggers the imidization reaction of PAA and the reduction of GONR, facilitating the formation of uniformly integrated GNR/PI nanocomposite coatings. Under optimized conditions, incorporating a high-loading GONR content in PAA (95 wt% of GONR and 5 wt% of PAA) yielded GNR/PI composites with excellent mechanical properties, exhibiting a hardness of 0.75 GPa and an elastic modulus of 8.3 GPa. Additionally, this GNR/PI composite displayed a good electrical conductivity of 3890 S/m, attributed to the electrical pathways formed by GNRs within the PI matrix.
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