Functionalized Graphene Origami Metamaterials with Tunable Thermal Conductivity

Graphene with tunable thermo-mechanical property is of great importance for next-generation thermal management devices. Distinct from previously reported porous graphene materials that tune the thermal conductivity at the cost of degrading their mechanical properties, non-porous hydrogenated graphene origami metamaterial exhibits a unique combination of tunable thermal conductivity, high strength, and enhanced stretchability. Through molecular dynamics simulation, an extremely broad range of thermal conductivity can be obtained by tuning the geometrical parameters of the Miura-ori nanoarchitecture of graphene origami, altering the adatom types and density, designing new origami patterns, and applying mechanical strains. By analyzing and comparing the results from atomistic and continuum-based simulations, the effect of length scale on the thermal property of graphene origami metamaterials is explored. The temperature distribution and the phonon density of states of the proposed graphene origami are examined to illustrate the heat conduction mechanism. Finally, 3D graphene origami metamaterials are constructed based on the coupling and assembling of graphene origami strips, and their thermo-mechanical performance is elucidated. Negative coefficients of thermal expansion are obtained in graphene origami nanotubes. The introduced strategy for controlling the thermo-mechanical properties of graphene metamaterials can open up new avenues for developing thermoelectric devices, heat management systems, and flexible nanoelectronics.