Chemical vapor deposition (CVD) has emerged as a promising approach for the controlled growth of graphene films with appealing scalability, controllability, and uniformity. However, the synthesis of high-quality graphene films still suffers from low production capacity and high energy consumption in the conventional hot-wall CVD system. In contrast, owing to the different heating mode, cold-wall CVD (CW-CVD) system exhibits promising potential for the industrial-scale production, but the quality of as-received graphene remains inferior with limited domain size and high defect density. Herein, we demonstrated an efficient method for the batch synthesis of high-quality graphene films with millimeter-sized domains based on CW-CVD system. With reduced defect density and improved properties, the as-received graphene was proven to be promising candidate material for electronics and anti-corrosion application. This study provides a new insight into the quality improvement of graphene derived from CW-CVD system, and paves a new avenue for the industrial production of high-quality graphene films for potential commercial applications.

Chemical vapor deposition (CVD)-grown graphene films on Cu foils, exhibiting fine scalability and high quality, are still suffering from the adverse impact of surface contamination, i.e., amorphous carbon. Despite the recent successful preparation of superclean graphene through Cu-vapor-assisted reactions, the formation mechanism of amorphous carbon remains unclear, especially with regard to the functions of substrates. Herein, we have found that the crystallographic orientations of underlying metal substrates would determine the cleanness of graphene in such a way that slower diffusion of active carbon species on as-formed graphene-Cu(100) surface is the key factor that suppresses the formation of contamination. The facile synthesis of clean graphene is achieved on the meter-sized Cu(100) that is transformed from the polycrystalline Cu foils. Furthermore, a clean surface of graphene on Cu(100) ensures the reduction of transfer-related polymer residues, and enhanced optical and electrical performance, which allows for versatile applications of graphene in biosensors, functioning as flexible transparent electrodes. This work would offer a promising material platform for the fundamental investigation and create new opportunities for the advanced applications of high-quality graphene films.