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Structural complexity of graphene oxide: the kirigami model

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Abstract
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.
Item Type: | Article |
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Authors/Creators: | Rawal, A and Che Man, SH and Agarwal, V and Yao, Y and Thickett, SC and Zetterlund, PB |
Keywords: | graphene oxide structure, solid-state NMR, 2D NMR, 2D 13C-1H heteronuclear correlation NMR, kirigami, furanic carbons |
Journal or Publication Title: | ACS Applied Materials & Interfaces |
Publisher: | American Chemical Society |
ISSN: | 1944-8244 |
DOI / ID Number: | 10.1021/acsami.1c01157 |
Copyright Information: | © 2021 American Chemical Society |
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