Carbon nanotube-vertical edge rich graphene hybrid sponge as multifunctional reinforcements for high performance epoxy composites

Thermal management materials with excellent electromagnetic interference (EMI) shielding performance have attracted research interest in the field of modern electronic devices. Herein, vertical edge rich graphene (VG) was in-situ grafted on the carbon nanotube (CNT) sponge to create connective 3D hybridized carbon skeleton with covalent bonding, then CNT-VG/epoxy composites were constructed to meet the needs of multifunctional application. Impressively, mainly owing to the connectivity of 3D CNT sponge, the conduction ability of interfaces and the defect-rich structure of VG, the obtained CNT-VG/epoxy composites possessed an enhanced EMI shielding effectiveness of 46.9 dB with a thickness of 1 mm and an improved thermal conductivity of 2.23 W m⁻¹ K⁻¹ which contributes to superior thermal management capability. In addition, the excellent structural design also increases the flexural strength by 349.39% compared to pure epoxy resin, achieving a flexural strength of 275.32 MPa and a work of fracture of 9956.98 kJ m⁻³. The novel multifunctional CNT-VG/epoxy composites with enhanced mechanical property show a bright application prospect in next-generation electronic devices.