Effect of friction on oxidative graphite intercalation and high-quality graphene formation

Steffen Seiler, Christian E. Halbig, Fabian Grote, Philipp Rietsch, Felix Börrnert, Ute Kaiser, Bernd Meyer () and Siegfried Eigler ()
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Steffen Seiler: Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU)
Christian E. Halbig: Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU)
Fabian Grote: Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU)
Philipp Rietsch: Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU)
Felix Börrnert: Universität Ulm
Ute Kaiser: Universität Ulm
Bernd Meyer: Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU)
Siegfried Eigler: Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU)

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract Oxidative wet-chemical delamination of graphene from graphite is expected to become a scalable production method. However, the formation process of the intermediate stage-1 graphite sulfate by sulfuric acid intercalation and its subsequent oxidation are poorly understood and lattice defect formation must be avoided. Here, we demonstrate film formation of micrometer-sized graphene flakes with lattice defects down to 0.02% and visualize the carbon lattice by transmission electron microscopy at atomic resolution. Interestingly, we find that only well-ordered, highly crystalline graphite delaminates into oxo-functionalized graphene, whereas other graphite grades do not form a proper stage-1 intercalate and revert back to graphite upon hydrolysis. Ab initio molecular dynamics simulations show that ideal stacking and electronic oxidation of the graphite layers significantly reduce the friction of the moving sulfuric acid molecules, thereby facilitating intercalation. Furthermore, the evaluation of the stability of oxo-species in graphite sulfate supports an oxidation mechanism that obviates intercalation of the oxidant.

Date: 2018
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DOI: 10.1038/s41467-018-03211-1

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