Graphene has been attracting wide interests owing to its excellent electronic, thermal, and mechanical performances. Despite the availability of several production techniques, it is still a great challenge to achieve wafer-size graphene with acceptable uniformity and low cost, which would determine the future of graphene electronics. Here we report a universal segregation growth technique for batch production of high-quality wafer-scale graphene from non-noble metal films. Without any extraneous carbon sources, 4 in. graphene wafers have been obtained from Ni, Co, Cu-Ni alloy, and so forth via thermal annealing with over 82% being 1-3 layers and excellent reproducibility. We demonstrate the first example of monolayer and bilayer graphene wafers using Cu-Ni alloy by combining the distinct segregation behaviors of Cu and Ni. Together with the easy detachment from growth substrates, we believe this facile segregation technique will offer a great driving force for graphene research.

When two-dimensional graphene is exfoliated from three-dimensional highly oriented pyrolytic graphite (HOPG), ripples or corrugations always exist due to the intrinsic thermal fluctuations. Surface-grown graphenes also exhibit wrinkles, which are larger in dimension and are thought to be caused by the difference in thermal expansion coefficients between graphene and the underlying substrate in the cooling process after high temperature growth. For further characterization and applications, it is necessary to transfer the surface-grown graphenes onto dielectric substrates, and other wrinkles are generated during this process. Here, we focus on the wrinkles of transferred graphene and demonstrate that the surface morphology of the growth substrate is the origin of the new wrinkles which arise in the surface-to-surface transfer process; we call these morphologyinduced wrinkles. Based on a careful statistical analysis of thousands of atomic force microscopy (AFM) topographic data, we have concluded that these wrinkles on transferred few-layer graphene (typically 1-3 layers) are determined by both the growth substrate morphology and the transfer process. Depending on the transfer medium and conditions, most of the wrinkles can be either released or preserved. Our work suggests a new route for graphene engineering involving structuring the growth substrate and tailoring the transfer process.

Controlled growth of high-quality graphene is still the bottleneck of practical applications. The widely used chemical vapour deposition process generally suffers from an uncontrollable carbon precipitation effect that leads to inhomogeneous growth and strong correlation to the growth conditions. Here we report the rational design of a binary metal alloy that effectively suppresses the carbon precipitation process and activates a self-limited growth mechanism for homogeneous monolayer graphene. As demonstrated by an ni-mo alloy, the designed binary alloy contains an active catalyst component for carbon source decomposition and graphene growth and a black hole counterpart for trapping the dissolved carbons and forming stable metal carbides. This type of process engineering has been used to grow strictly singlelayer graphene with 100% surface coverage and excellent tolerance to variations in growth conditions. With simplicity, scalability and a very large growth window, the presented approach may facilitate graphene research and industrial applications.