▎ 摘　　要

We have established a simple method for drastically improving the productivity of chemical vapor deposition in large-area graphene synthesis using a roll-stacked Ni coil as a catalyst. Our systematic investigation of the effects of a confined catalytic geometry has shown that the gas flow through interfacial gaps within the stack follows non-continuum fluid dynamics when the size of the gap decreases sufficiently, which enhances the dissolution of the carbon sources into the catalyst during synthesis. Quantitative criteria for graphene growth in the confined geometry are established through the introduction of the Knudsen number, Kn, which is the ratio of the mean-free-path of the gas molecules to the size of the gap. The criteria provided in this article for the synthesis of graphene in the confined geometry are expected to provide the foundations for the efficient mass production of large-area graphene. We also show that the evolution of the catalytic Ni surface in a stacked system results in larger grains in the (111) plane, and consequently in reproducible, uniform, and high-quality multi-layered graphene.