Uniform hexagonal graphene flakes and films grown on liquid copper surface

Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, People's Republic of China.
Proceedings of the National Academy of Sciences (Impact Factor: 9.67). 04/2012; 109(21):7992-6. DOI: 10.1073/pnas.1200339109
Source: PubMed


Unresolved problems associated with the production of graphene materials include the need for greater control over layer number, crystallinity, size, edge structure and spatial orientation, and a better understanding of the underlying mechanisms. Here we report a chemical vapor deposition approach that allows the direct synthesis of uniform single-layered, large-size (up to 10,000 μm(2)), spatially self-aligned, and single-crystalline hexagonal graphene flakes (HGFs) and their continuous films on liquid Cu surfaces. Employing a liquid Cu surface completely eliminates the grain boundaries in solid polycrystalline Cu, resulting in a uniform nucleation distribution and low graphene nucleation density, but also enables self-assembly of HGFs into compact and ordered structures. These HGFs show an average two-dimensional resistivity of 609 ± 200 Ω and saturation current density of 0.96 ± 0.15 mA/μm, demonstrating their good conductivity and capability for carrying high current density.

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    • "Our results are consistent with earlier reports indicating that preheating and annealing of Cu in presence of H 2 not only reduces surface irregularities (e.g. surface bumps and striation marks) [11] [17], but also promotes formation "
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    ABSTRACT: Understanding the mechanism of graphene synthesis by chemical vapor deposition and the effect of process parameters is critical for production of high-quality graphene. In the present work, we investigated the effect of H 2 concentration during annealing on evolution of Cu surface morphology, and on deposited graphene characteristics. Our results revealed that H 2 had a smoothening effect on Cu surface as its surface roughness was reduced significantly at high H 2 concentration along with the formation of surface facets, dents and nanometer-sized particles. Furthermore, H 2 content influenced the graphene morphology and its quality. A low H 2 concentration (0% and 2.5%) during annealing promoted uniform and good quality bilayer graphene. In contrast, a high concentration of H 2 (20% and 50%) resulted in multilayer, non-uniform and defective graphene. Interestingly, the annealed Cu surface morphology differed considerably from that obtained after deposition of graphene, indicating that graphene deposition has its own impact on Cu surface.
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    • "The continuity of polycrystalline graphene and the minimization of its grain boundaries (GBs) remains a big challenge towards its integration into large-scale applications [2] [3] [4] [5]. "
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    ABSTRACT: The effect of grain boundaries and wrinkles on the electrical properties of polycrystalline graphene is pronounced. Here we investigate the stitching between grains of polycrystalline graphene, specifically, overlapping of layers at the boundaries, grown by chemical vapor deposition (CVD) and subsequently doped by the oxidized Cu substrate. We analyze overlapped regions between 60 and 220 nm wide via Raman spectroscopy, and find that some of these overlapped boundaries contain AB-stacked bilayers. The Raman spectra from the overlapped grain boundaries are distinctly different from bilayer graphene and exhibit splitting of the G band peak. The degree of splitting, peak widths, as well as peak intensities depend on the width of the overlap. We attribute these features to inhomogeneous doping by charge carriers (holes) across the overlapped regions via the oxidized Cu substrate. As a result, the Fermi level at the overlapped grain boundaries lies between 0.3 and 0.4 eV below the charge neutrality point. Our results suggest an enhancement of electrical conductivity across overlapped grain boundaries, similar to previously observed measurements (Tsen et al., 2012). The dependence of charge distribution on the width of overlapping of grain boundaries may have strong implications for the growth of large-area graphene with enhanced conductivity.
    Carbon 12/2014; 80(1):513-522. DOI:10.1016/j.carbon.2014.08.091 · 6.20 Impact Factor
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    • "The data are to be compared with the previously reported low magnification TEM images1317252627 where atomic graphene layers cannot be confirmed, cross-sectional HRTEM images where graphene layers appear unclearly232829, and atomic resolution (in-plan) HTRTEM images showing hexagonal lattices6783031323334, which are obtainable from bi- or trilayer graphene (i.e., thin graphite)6833. ED patterns showing hexagonal symmetry131725272829303135 are also obtainable either from bilayer graphene (Fig. 5b of ref. 6) or single crystal graphite36. "
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    ABSTRACT: In this paper, we demonstrate the seeded growth of graphene under a plasma chemical vapor deposition condition. First, we fabricate graphene nanopowders (~5 nm) by ball-milling commercial multi-wall carbon nanotubes. The graphene nanoparticles were subsequently subject to a direct current plasma generated in a 100 Torr 10%CH4 - 90%H2 gas mixture. The plasma growth enlarged, over one hour, the nuclei to graphene sheets larger than one hundred nm(2) in area. Characterization by electron and X-ray diffraction, high-resolution transmission electron microscopy images provide evidence for the presence of monolayer graphene sheets.
    Scientific Reports 07/2014; 4:5682. DOI:10.1038/srep05682 · 5.58 Impact Factor
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