Growth of Continuous Monolayer Graphene with Millimeter-sized Domains Using Industrially Safe Conditions

Abstract

We demonstrate the growth of continuous monolayer graphene films with millimeter-sized domains on Cu foils under intrinsically safe, atmospheric pressure growth conditions, suitable for application in roll-to-roll reactors. Previous attempts to grow large domains in graphene have been limited to isolated graphene single crystals rather than as part of an industrially useable continuous film. With both appropriate pre-treatment of the Cu and optimization of the CH4 supply, we show that it is possible to grow continuous films of monolayer graphene with millimeter scale domains within 80 min by chemical vapour deposition. The films are grown under industrially safe conditions, i.e., the flammable gases (H2 and CH4) are diluted to well below their lower explosive limit. The high quality, spatial uniformity, and low density of domain boundaries are demonstrated by charge carrier mobility measurements, scanning electron microscope, electron diffraction study, and Raman mapping. The hole mobility reaches as high as ~5,700 cm2 V−1 s−1 in ambient conditions. The growth process of such high-quality graphene with a low H2 concentration and short growth times widens the possibility of industrial mass production.

Understanding and Controlling Cu-Catalyzed Graphene Nucleation: The Role of Impurities, Roughness, and Oxygen Scavenging

“…Different CH 4 flow rates ( V CH 4 ) are shown as solid lines for the use of 0.1% diluted CH 4 in Ar. Literature (Wu16, 54 Wu15, 18 Eres, 29 Wang14, 55 Chen13, 37 Chen15, 43 Lin, 56 Miseikis, 42 Zhou, 14 and Yan12 57 ) values are included for graphene growth on polycrystalline foil and homogeneous precursor exposure, with the exception of Wu15, 18 where local precursor feeding was used. (b) A Cu foil after graphene growth performed with 20 sccm CH 4 (0.1% diluted in Ar) and a growth time of 8 h with BO + Ar treatment (to visualize graphene grains directly on the Cu foil, it was placed on a hot plate at 250 °C for 1 min 58 ).…”

The Way towards Ultrafast Growth of Single‐Crystal Graphene on Copper

“…In addition, the inhomogeneities influence the growth rate slightly by affecting the diffusion process 53, 54, 55, 56, 57. Proper surface treatment technique, like long‐time annealing,65 polishing,56, 68, 87 melting and resolidification,72, 73, 74 and the above mentioned special Cu stacking configuration can accelerate the graphene growth by minimizing surface roughness.…”

Scaling theory for two-dimensional single domain growth driven by attachment of diffusing adsorbates

“…In general, sigmoidal domain growth follows an induction period of nucleation; domains initially grow in isolation from other domains, and domain growth slows down by diffusive interaction for diffusing adsorbates among domains [22,23,[26][27][28]. We consider domain growth under the isolated condition from other domains.…”