We demonstrate that large scale high quality graphene synthesis can be performed using atmospheric pressure chemical vapor deposition (CVD) on Cu and illustrate how this procedure eliminates major difficulties associated with the low pressure CVD approach while allowing straightforward expansion of this technology to the roll-to-roll industrial scale graphene production. The detailed recipes evaluating the effects of copper foil thicknesses, purity, morphology and crystallographic orientation on the graphene growth rates and the number of graphene layers were investigated and optimized. Various foil cleaning protocols and growth conditions were evaluated and optimized to be suitable for production of large scale single layer graphene that was subsequently transferred on transparent flexible polyethylene terephthalate (PET) polymer substrates. Such “ready to use” graphene–PET sandwich structures were as large as 40" in diagonal and >98% single layer, sufficient for many commercial and research applications. Synthesized large graphene film consists of domains exceeding 100 μm. Some curious behavior of high temperature graphene etching by oxygen is described that allows convenient visualization of interdomain boundaries and internal stresses.

This paper was originally published in Carbon (2012) 54, 58-67.

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