Graphene oxide potentially has multiple applications. The chemistry of graphene oxide and its response to external stimuli such as temperature and light are not well understood and only approximately controlled. This understanding is crucial to enable future applications of this material. Here, a combined experimental and density functional theory study shows that multilayer graphene oxide produced by oxidizing epitaxial graphene through the Hummers method is a metastable material whose structure and chemistry evolve at room temperature with a characteristic relaxation time of about one month. At the quasi-equilibrium, graphene oxide reaches a nearly stable reduced O/C ratio, and exhibits a structure deprived of epoxide groups and enriched in hydroxyl groups. Our calculations show that the structural and chemical changes are driven by the availability of hydrogen in the oxidized graphitic sheets, which favours the reduction of epoxide groups and the formation of water molecules.
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S.K., S.Z., A.B. and E.R. acknowledge the support of the National Science Foundation (NSF) (CMMI-1100290 and DMR-0820382). Y.H., C.B. and W.d.H. acknowledge the support of NSF grant DMR-0820382. A.B. acknowledges the support of the Samsung Advanced Institute of Technology (SAIT). E.R. acknowledges the support of the NSF grant DMR-0706031 and the Office of Basic Energy Sciences of the US Department of Energy (DE-FG02-06ER46293). Y.J.C. and M.A. acknowledge the support of the Office of Basic Sciences of the US Department of Energy (DE-SC001951). We thank D. Wang, P. Sheehan and A. R. Laracuente of the US Naval Research Laboratory for the 4-point electrical transport measurements.
The authors declare no competing financial interests.
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Kim, S., Zhou, S., Hu, Y. et al. Room-temperature metastability of multilayer graphene oxide films. Nature Mater 11, 544–549 (2012). https://doi.org/10.1038/nmat3316
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