Grain Size Engineering of CVD‐Grown Large‐Area Graphene Films

Graphene, a single atomic layer of graphitic carbon, has attracted much attention because of its outstanding properties hold great promise for a wide range of technological applications. Large-area graphene films (GFs) grown by chemical vapor deposition (CVD) are highly desirable for both investigating their intrinsic properties and realizing their practical applications. However, the presence of grain boundaries (GBs) has significant impacts on their properties and related applications. According to the different grain sizes, GFs can be divided into polycrystalline, single-crystal, and nanocrystalline films. In the past decade, considerable progress has been made in engineering the grain sizes of GFs by modifying the CVD processes or developing some new growth approaches. The key strategies involve controlling the nucleation density, growth rate, and grain orientation. This review aims to provide a comprehensive description of grain size engineering research of GFs. The main strategies and underlying growth mechanisms of CVD-grown large-area GFs with nanocrystalline, polycrystalline, and single-crystal structures are summarized, in which the advantages and limitations are highlighted. In addition, the scaling law of physical properties in electricity, mechanics, and thermology as a function of grain sizes are briefly discussed. Finally, the perspectives for challenges and future development in this area are also presented.