Abstract
Chemical vapor deposition has been highlighted as a promising tool for facile graphene growth in a large area. However, grain boundaries impose detrimental effects on the mechanical strength or electrical mobility of graphene. Here, we demonstrate that high-pressure hydrogen treatment in the preannealing step plays a key role in fast and large grain growth and leads to the successful synthesis of large grain graphene in 10 s. Large single grains with a maximum size of ∼160 μm grow by recrystallization of nanograins, but ∼1% areal coverage of nanograins remains with 28-30° misorientation angles. Our findings will provide insights into mass production of high-quality graphene.