Scalable synthesis of high-quality, reduced graphene oxide with a large C/O ratio and its dispersion in a chemically modified polyimide matrix for electromagnetic interference shielding applications

Abstract

High-purity reduced graphene oxide (RGO or rGO) with appreciable conductivity is a desired conductive filler for lightweight polymer composites used in coatings, electronics, catalysts, electromagnetic interference (EMI) shielding, and energy storage devices. However, the intrinsic conductivity and the uniform dispersion of RGO in relatively polar matrices are challenging, leading to poor overall conductivity and performance of the composite material. The reported study improved the RGO intrinsic conductivity by increasing its C/O ratio while also simultaneously enhancing its compatibility with the polyimide (PI) matrix through ester linkages for better dispersion. A two-step reduction method drastically increased the number of structural defects and carbon content in the resulting RGO, corresponding to a maximum I_D/I_G and C/O of 1.54 and ∼87, respectively. Moreover, the 2D nanosheets with limited hydroxyl (–OH) groups effectively interacted with anhydride-terminated polyamic acid (AT-PAA) through chemical linkages to make high-performance RGO/PI nanocomposites. Consequently, the polymer matrix composites possessed the highest direct current conductivity of 15.27 ± 0.61 S cm⁻¹ for 20 wt% of the prepared RGO. Additionally, the composite material was highly stiff (3.945 GPa) yet flexible (easily bent through 180°), lightweight (∼0.34 g cm⁻³), and capable of forming thin films (162 ± 15 μm). Unlike most polymer matrix composites, it showcased one of its class's highest thermal stabilities (a weight loss of only 5% at 638 °C). Ultimately, the composite performed as an effective electromagnetic interference (EMI) shielding material in the X-Band (8 to 12 GHz), demonstrating outstanding shielding effectiveness (SE), shielding effectiveness per unit thickness (SE_t), specific shielding effectiveness (SSE), and absolute shielding effectiveness (SSE_t) of 46 dB, 2778 dB cm⁻², 138 dB cm³ g⁻¹, and 8358 dB cm² g⁻¹, respectively. As a consequence of this research, the high-purity RGO and its high-performance PI matrix nanocomposites are anticipated to find practical applications in conductive coatings and flexible substrates demanding high-temperature stability.