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

Nature Communications
Steffen SeilerSiegfried Eigler

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.

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Citations

Jun 15, 2018·Chemistry : a European Journal·Christian E HalbigAndreas Hirsch
Dec 19, 2019·Chemistry : a European Journal·Zhenping WangSiegfried Eigler
May 1, 2019·Chemistry : a European Journal·Patrick FeichtSiegfried Eigler
Jun 12, 2020·Nanoscale·Yuta Nishina, Siegfried Eigler
Feb 13, 2020·Frontiers in Chemistry·Anton Kröner, Thomas Hirsch
Feb 11, 2021·Nanomaterials·Pietro BelletFrancesco Filippini
May 14, 2021·Advanced Materials·Jingyuan ZhouXiangfeng Duan
Jul 30, 2021·Langmuir : the ACS Journal of Surfaces and Colloids·Prabodha G AbeykoonDouglas H Adamson
Oct 8, 2021·The Journal of Physical Chemistry Letters·Yiqing WangSiegfried Eigler

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Methods Mentioned

BETA
delamination
transmission electron microscopy
atomic force microscopy
Raman spectroscopy

Software Mentioned

CPMD

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