Structural Characterization of Graphene Oxide: Surface Functional Groups and Fractionated Oxidative Debris

Overview

Journal Nanomaterials (Basel)

Date 2019 Aug 21

PMID 31426617

Citations 62

Authors

Elvin Aliyev

Volkan Filiz

Muntazim M Khan

Young Joo Lee

Clarissa Abetz

Volker Abetz

Affiliations

Soon will be listed here.

Abstract

The purpose of this work is the structural analysis of graphene oxide (GO) and by means of a new structural model to answer the questions arising from the Lerf-Klinowski and the Lee structural models. Surface functional groups of GO layers and the oxidative debris (OD) stacked on them were investigated after OD was extracted. Analysis was performed successfully using Fourier transform infrared spectroscopy (FTIR), ultraviolet-visible spectroscopy (UV-Vis), X-ray photoemission spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDX), Raman spectroscopy, solid-state nuclear magnetic resonance spectroscopy (SSNMR), standardized Boehm potentiometric titration analysis, elemental analysis, X-ray diffraction (XRD), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). The analysis showed that graphene oxide layers, as well as oxidative debris contain different functional groups such as phenolic -OH, ketone, lactone, carboxyl, quinone and epoxy. Based on these results, a new structural model for GO layers is proposed, which covers all spectroscopic data and explains the presence of the other oxygen functionalities besides carboxyl, phenolic -OH and epoxy groups.

Citing Articles

Development of Superhydrophobic Reduced Graphene Oxide (rGO) for Potential Applications in Advanced Materials.

Adotey E, Kurbanova A, Ospanova A, Ardakkyzy A, Toktarbay Z, Kydyrbay N Nanomaterials (Basel). 2025; 15(5).

PMID: 40072166 PMC: 11901565. DOI: 10.3390/nano15050363.

Graphdiyne biomaterials: from characterization to properties and applications.

Zhao L, Fan Y, Zhang X, Li C, Cheng X, Guo F J Nanobiotechnology. 2025; 23(1):169.

PMID: 40038692 PMC: 11881411. DOI: 10.1186/s12951-025-03227-y.

Mussel-Inspired Hydrogels Incorporating Graphite Derivatives for Soft Tissue Regeneration.

Fernandes F, Peixoto D, Correia C, Silva M, Paiva M, Alves N Nanomaterials (Basel). 2025; 15(4).

PMID: 39997839 PMC: 11858166. DOI: 10.3390/nano15040276.

Smartphone-assisted fluorescence/colorimetric dual-mode sensing strategy for uranium ion detection using cerium-sulfonyl calix[4]arene.

Xiong L, Tong Y, Song J, Chen S, Liu Y, Liu J Mikrochim Acta. 2025; 192(3):158.

PMID: 39946020 DOI: 10.1007/s00604-025-07023-1.

Graphene oxide and its derivatives films for sustained-release trace element zinc based on cation-π interaction.

Zhang W, He Y, Zhu H, Li X, Zou Z, Luo C Sci Rep. 2025; 15(1):4255.

PMID: 39905039 PMC: 11794843. DOI: 10.1038/s41598-025-87696-z.

References

Suarez , Menendez , Fuente . Pyrone-Like Structures as Novel Oxygen-Based Organic Superbases The authors thank CSIC for computer time at the CESGA and the CIEMAT. Angew Chem Int Ed Engl. 2000; 39(7):1320-1323. DOI: 10.1002/(sici)1521-3773(20000403)39:7<1320::aid-anie1320>3.0.co;2-e. View

Verdejo R, Lamoriniere S, Cottam B, Bismarck A, Shaffer M . Removal of oxidation debris from multi-walled carbon nanotubes. Chem Commun (Camb). 2007; (5):513-5. DOI: 10.1039/b611930a. View

Kudin K, Ozbas B, Schniepp H, Prudhomme R, Aksay I, Car R . Raman spectra of graphite oxide and functionalized graphene sheets. Nano Lett. 2007; 8(1):36-41. DOI: 10.1021/nl071822y. View

Li D, Muller M, Gilje S, Kaner R, Wallace G . Processable aqueous dispersions of graphene nanosheets. Nat Nanotechnol. 2008; 3(2):101-5. DOI: 10.1038/nnano.2007.451. View

Paredes J, Villar-Rodil S, Martinez-Alonso A, Tascon J . Graphene oxide dispersions in organic solvents. Langmuir. 2008; 24(19):10560-4. DOI: 10.1021/la801744a. View

Cai W, Piner R, Stadermann F, Park S, Shaibat M, Ishii Y . Synthesis and solid-state NMR structural characterization of 13C-labeled graphite oxide. Science. 2008; 321(5897):1815-7. DOI: 10.1126/science.1162369. View

Dreyer D, Park S, Bielawski C, Ruoff R . The chemistry of graphene oxide. Chem Soc Rev. 2009; 39(1):228-40. DOI: 10.1039/b917103g. View

Lee D, De Los Santos V L, Seo J, Felix L, Bustamante D A, Cole J . The structure of graphite oxide: investigation of its surface chemical groups. J Phys Chem B. 2010; 114(17):5723-8. DOI: 10.1021/jp1002275. View

Gao W, Alemany L, Ci L, Ajayan P . New insights into the structure and reduction of graphite oxide. Nat Chem. 2011; 1(5):403-8. DOI: 10.1038/nchem.281. View

10.

Rourke J, Pandey P, Moore J, Bates M, Kinloch I, Young R . The real graphene oxide revealed: stripping the oxidative debris from the graphene-like sheets. Angew Chem Int Ed Engl. 2011; 50(14):3173-7. DOI: 10.1002/anie.201007520. View

11.

Cancado L, Jorio A, Ferreira E, Stavale F, Achete C, Capaz R . Quantifying defects in graphene via Raman spectroscopy at different excitation energies. Nano Lett. 2011; 11(8):3190-6. DOI: 10.1021/nl201432g. View

12.

Whitby R, Gunko V, Korobeinyk A, Busquets R, Cundy A, Laszlo K . Driving forces of conformational changes in single-layer graphene oxide. ACS Nano. 2012; 6(5):3967-73. PMC: 3357922. DOI: 10.1021/nn3002278. View

13.

Dimiev A, Bachilo S, Saito R, Tour J . Reversible formation of ammonium persulfate/sulfuric acid graphite intercalation compounds and their peculiar Raman spectra. ACS Nano. 2012; 6(9):7842-9. DOI: 10.1021/nn3020147. View

14.

Ferrari A, Basko D . Raman spectroscopy as a versatile tool for studying the properties of graphene. Nat Nanotechnol. 2013; 8(4):235-46. DOI: 10.1038/nnano.2013.46. View

15.

Eigler S, Dotzer C, Hof F, Bauer W, Hirsch A . Sulfur species in graphene oxide. Chemistry. 2013; 19(29):9490-6. DOI: 10.1002/chem.201300387. View

16.

Li H, Song Z, Zhang X, Huang Y, Li S, Mao Y . Ultrathin, molecular-sieving graphene oxide membranes for selective hydrogen separation. Science. 2013; 342(6154):95-8. DOI: 10.1126/science.1236686. View

17.

Perrozzi F, Prezioso S, Ottaviano L . Graphene oxide: from fundamentals to applications. J Phys Condens Matter. 2014; 27(1):013002. DOI: 10.1088/0953-8984/27/1/013002. View

18.

Fujimoto A, Yamada Y, Koinuma M, Sato S . Origins of sp(3)C peaks in C1s X-ray Photoelectron Spectra of Carbon Materials. Anal Chem. 2016; 88(12):6110-4. DOI: 10.1021/acs.analchem.6b01327. View

19.

Naumov A, Grote F, Overgaard M, Roth A, Halbig C, Norgaard K . Graphene Oxide: A One- versus Two-Component Material. J Am Chem Soc. 2016; 138(36):11445-8. DOI: 10.1021/jacs.6b05928. View

20.

Bousa D, Friess K, Pilnacek K, Vopicka O, Lanc M, Fonod K . Thin, High-Flux, Self-Standing, Graphene Oxide Membranes for Efficient Hydrogen Separation from Gas Mixtures. Chemistry. 2017; 23(47):11416-11422. DOI: 10.1002/chem.201702233. View