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In this study, we developed a simple and powerful method to fabricate flexible and lightweight graphene-based composites that provide high electromagnetic interference (EMI) shielding performance. Electrospun waterborne polyurethane (WPU) that featured sulfonate functional groups was used as the polymer matrix, which was light and flexible. First, graphene oxide (GO)/WPU composites were prepared through layer-by-layer (L-b-L) assembly of two oppositely charged suspensions of GO, the cationic surfactant (didodecyldimethylammonium bromide, DDAB)-adsorbed GO and intrinsic negatively charged GO, depositing on the negatively charged WPU fibers. After the L-b-L assembly cycles, the GO bilayers wrapped the WPU fiber matrix completely and revealed fine connections guided by the electrospun WPU fibers. Then, we used hydroiodic acid (HI) to obtain highly reduced GO (r-GO)/WPU composites, which exhibited substantially enhanced electrical conductivity (approximately 16.8 S/m) and, moreover, showed a high EMI-shielding effectiveness (approximately 34 dB) over the frequency range from 8.2 to 12.4 GHz.

An effective method is proposed to prepare octa(aminophenyl) silsesquioxane (OAPS) functionalized graphene oxide (GO) reinforced polyimide (PI) composites with a low dielectric constant and ultrastrong mechanical properties. The amine-functionalized surface of OAPS-GO is a versatile starting platform for in situ polymerization, which promotes the uniform dispersion of OAPS-GO in the PI matrix. Compared with GO/PI composites, the strong interfacial interaction between OAPS-GO and the PI matrix through covalent bonds facilitates a load transfer from the PI matrix to the OAPS-GO. The OAPS-GO/PI composite film with 3.0 wt % OAPS-GO exhibited an 11.2-fold increase in tensile strength, and a 10.4-fold enhancement in tensile modulus compared with neat PI. The dielectric constant (D(k)) decreased with the increasing content of 2D porous OAPS-GO, and a D(k) value of 1.9 was achieved.