3D Lamellar-Structured Graphene Aerogels for Thermal Interface Composites with High Through-Plane Thermal Conductivity and Fracture Toughness

Although thermally conductive graphene sheets are efficient in enhancing in-plane thermal conductivities of polymers,the resulting nanocomposites usually exhibit low through-plane thermal conductivities,limiting their application as thermal interface materials.Herein,lamellarstructured polyamic acid salt/graphene oxide(PAAS/GO)hybrid aerogels are constructed by bidirectional freezing of PAAS/GO suspension followed by lyophilization.Subsequently,PAAS monomers are polymerized to polyimide(PI),while GO is converted to thermally reduced graphene oxide(RGO)during thermal annealing at 300℃.Final graphitization at 2800℃ converts PI to graphitized carbon with the inductive effect of RGO,and simultaneously,RGO is thermally reduced and healed to high-quality graphene.Consequently,lamellar-structured graphene aerogels with superior through-plane thermal conduction capacity are fabricated for the first time,and its superior through-plane thermal conduction capacity results from its vertically aligned and closely stacked high-quality graphene lamellae.After vacuum-assisted impregnation with epoxy,the resultant epoxy composite with 2.30 vol% of graphene exhibits an outstanding through-plane thermal conductivity of as high as 20.0 W m^−1 K^−1,100 times of that of epoxy,with a record-high specific thermal conductivity enhancement of 4310%.Furthermore,the lamellar-structured graphene aerogel endows epoxy with a high fracture toughness,~1.71 times of that of epoxy.