Structural Complexity of Graphene Oxide: The Kirigami Model

Investigation of highly oxidized graphene oxide (GO) by solid-state nuclear magnetic resonance (NMR) spectroscopy has revealed an exceptional level of hitherto undiscovered structural complexity. A number of chemical moieties were observed for the first time, such as terminal esters, furanic carbons, phenolic carbons, and three distinct aromatic and two distinct alkoxy carbon moieties. Quantitative one-dimensional (1D) and two-dimensional (2D) 13C{1H} NMR spectroscopy established the relative populations and connectivity of these different moieties to provide a consistent “local” chemical structure model. An inferred 2 nm GO sheet size from a very large (∼20%) edge carbon fraction by NMR analysis is at odds with the >20 nm sheet size determined from microscopy and dynamic light scattering. A proposed kirigami model where extensive internal cuts/tears in the basal plane provide the necessary edge sites is presented as a resolution to these divergent results. We expect this work to expand the fundamental understanding of this complex material and enable greater control of the GO structure.