Toward large-scale CVD graphene growth by enhancing reaction kinetics via an efficient interdiffusion mediator and mechanism study utilizing CFD simulations

Background: The yield rate for the synthesis of large-area and high-quality graphene, based on the chemical vapor deposition (CVD) method, is limited by the reactor size of a tubular furnace. Additionally, the reported methods to achieve a high-throughput process are still challenging. Currently, the rolled-up or vertically stacked configuration setup is applied to increase the loading growth. However, the reported methods limit the kinetic reaction of CVD growth and lead to the degradation of the uniformity and crystallinity of as-grown graphene. Methods: Here, we propose a novel method to produce a high-yield and uniform monolayer graphene film by helical stacking of Cu with highly porous carbon cloth as an efficient interdiffusion mediator. Additionally, computational fluid dynamics (CFD) is applied to simulate the dynamic distribution within the mediator. Significant Findings: This method allows the rapid synthesis of graphene films of up to 900 cm² for each batch of growth in a 1-inch furnace. Graphene with optimized conditions exhibits a high crystallinity (I_D/I_G: 0.16) and electrical conductivity (760 Ω/sq). The comprehensive study on recipe optimization together with the multiphysical simulation suggests that the proposed carbon cloth is an ideal spacing mediator for CVD graphene with a high Cu-loading density. This enhancement is attributed to the homogeneous interdiffusion of reactive gas/species in both the transverse and radial directions, resulting in homogeneous nucleation and equivalent kinetic growth. The capacity could reach 15.56 m²/hour in an 8-inch system. The CFD simulation indicates that the porous mediator can improve gas distribution and balance the pressure between the Cu foils to enhance high-yield graphene synthesis. This method provides an efficient strategy for the synthesis of high-throughput and large-area CVD graphene films, which is beneficial for cost-effective and versatile graphene-based applications.