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Issue 4, 2014
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Experimentally determined model of atmospheric pressure CVD of graphene on Cu

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Abstract

We investigate the critical methane concentration (CMC) during the atmospheric-pressure chemical vapor deposition (AP-CVD) of graphene on Cu from CH4. Above the CMC, graphene both nucleates and grows; below the CMC, it etches; while at the CMC, carbon intermediate species attach and detach from graphene at equal rates. By studying how the CMC varies with [H2] and temperature, we determine the reaction mechanism and the intermediates. We find that the CMC scales with [H2]3/2 and determine a single Arrhenius temperature dependence close to the expected equilibrium value. For [CH4] > CMC, the radial growth rate is proportional to the “building unit” supersaturation indicating that graphene growth occurs under capture-limited kinetics through an intermediate hydrocarbon that is first-order dependent on [CH4] and proportional to [H2]−3/2. We develop a CH4 decomposition and capture model which is consistent with all measurements indicating that the intermediate is CH. We find that uniform monolayer graphene can only be achieved in AP-CVD near the CMC, with a nucleation density that varies 5 orders of magnitude from 880 to 1075 °C. Thus, our work also provides a roadmap for growing uniform graphene at atmospheric pressure on Cu over a broad range of experimental conditions.

Graphical abstract: Experimentally determined model of atmospheric pressure CVD of graphene on Cu

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Publication details

The article was received on 04 Sep 2013, accepted on 22 Nov 2013 and first published on 25 Nov 2013


Article type: Paper
DOI: 10.1039/C3TC31738B
J. Mater. Chem. C, 2014,2, 744-755

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    Experimentally determined model of atmospheric pressure CVD of graphene on Cu

    N. S. Safron and M. S. Arnold, J. Mater. Chem. C, 2014, 2, 744
    DOI: 10.1039/C3TC31738B

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