Disordered metallic carbon materials from graphene edge chemistry

The creation of three dimensional (3D) structures out of two-dimensional (2D) materials while retaining their extraordinary mechanical and transport properties after processing is one of the current great challenges in materials sciences (Ruoff, 2008; Kong et al., 2019; Lin et al., 2019). Guided by density functional theory (DFT) and molecular dynamics (MD) simulations we found a successful route for a sustainable production of 3D metallic carbon materials that are synthesized from pristine 2D graphene flakes with hydrolyzed edges. The edge hydrolysis lead to strong geometrical anisotropy and self-organization in solution before processing. After processing we obtain a 3D carbon structure where 2D graphene flakes are crosslinked by carbon chains with aromatic groups at very mild annealing temperatures (∼150 °C), eliminating the constraints for achieving the in-situ preparation of conductive carbon structures. These 3D carbon structures preserve microscopic order but are macroscopically disordered, presenting physical properties of anisotropic metallic carbon with large Young modulus (E ≈ 20 GPa), and room temperature thermal (k ≈ 180 W/mK) and electrical (σ ≈ 300 kS/m) conductivities comparable to ordinary metals.