Multi-layer shearing induced high orientation of graphene oxide sheets towards high-performance macrostructures

The orientation of graphene nanosheets in microstructures is directly related to the mechanical properties and thermal conductivity of graphene-based macrostructures. However, efficient and scalable modulation of the orientation of 2D graphene nanosheets remains challenging. Herein, a simple and effective approach was proposed by introducing a multi-layer shearing field in thick graphene oxide (GO) gel coatings to improve the total orientation of GO films. Hydrodynamic simulations were performed via the lattice-Boltzmann method to reveal the microscale mechanism of the flow profile in improving the orientation of GO nanosheets. The result was experimentally verified by fast Fourier transform (FFT) of the cross-section scanning electron microscope (SEM) images of freeze-dried GO films and wide-angle X-ray scattering (WAXS) patterns of 16 various samples under different shearing line distances, velocities, and GO concentrations. The obtained GO films exhibit high orientation (Herman's orientation factor ƒ = 0.922), high strength (419.2 MPa), and high modulus (26.2 GPa), respectively, which are 1.06, 5.57, and 3.49 times higher compared to GO films prepared through the frequently used doctor blade method. The good orientation of GO is remained and further improved to the ultra-high orientation (ƒ = 0.968) after being graphitized at 3150 °C and roll pressing, and the oriented thick graphene films achieved the highest thermal conductivity (1629 W m–1 K–1 for 86 μm and 1593 W m–1 K–1 for 110 μm) compared to other graphene films mentioned in the literature as having a similar thickness. The multi-layered shearing strategy represents a facile technology for assembling two-dimensional (2D) nanoscale building blocks into a macroscopic structure with good orientation and high performance.