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Formation mechanism, growth kinetics, and stability limits of graphene adlayers in metal-catalyzed CVD growth

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Antonietti,  Markus
Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Willinger,  Marc Georg
Marc Willinger, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Citation

Wang, Z., Ding, F., Eres, G., Antonietti, M., Schloegl, R., & Willinger, M. G. (2018). Formation mechanism, growth kinetics, and stability limits of graphene adlayers in metal-catalyzed CVD growth. Advanced Materials Interfaces, 5(14): 1800255. doi:10.1002/admi.201800255.


Cite as: http://hdl.handle.net/21.11116/0000-0001-617F-4
Abstract
A new mechanism by which catalytic chemical vapor deposition of graphene spontaneously terminates at a single layer on Pt foils is discussed. This self-limited growth regime is identified by direct imaging of adlayer graphene evolution using in-situ environmental scanning electron microscopy. Two fundamentally different mechanisms for adlayer nucleation are revealed. Besides primary nucleation, which is the standard nucleation that occurs only at the onset of growth, a secondary nucleation of adlayers is observed near full coverage of the substrate. Direct observation reveals layer-dependent growth kinetics and the establishment of a dynamic equilibrium between the forward reaction of carbon incorporation and the reverse reaction of graphene etching. Increasing coverage of the active catalyst gives rise to a spontaneous reversal of adlayer evolution from growth to etching. The growth reversal has important practical benefits. It creates a self-limited growth regime in which all adlayer graphene is removed and it enables large-cale production of 100% single-layer graphene.