Abstract
The electronic properties of graphene, such as high charge carrier concentrations and mobilities, make it a promising candidate for next-generation nanoelectronic devices1,2,3. In particular, electrons and holes can undergo ballistic transport on the sub-micrometre scale in graphene and do not suffer from the scale limitations of current MOSFET technologies2,3. However, it is still difficult to produce single-layer samples of graphene1,3 and bulk processing has not yet been achieved, despite strenuous efforts to develop a scalable production method4,5. Here, we report a versatile solution-based process for the large-scale production of single-layer chemically converted graphene over the entire area of a silicon/SiO2 wafer. By dispersing graphite oxide paper in pure hydrazine we were able to remove oxygen functionalities and restore the planar geometry of the single sheets. The chemically converted graphene sheets that were produced have the largest area reported to date (up to 20 × 40 µm), making them far easier to process. Field-effect devices have been fabricated by conventional photolithography, displaying currents that are three orders of magnitude higher than previously reported for chemically produced graphene6. The size of these sheets enables a wide range of characterization techniques, including optical microscopy, scanning electron microscopy and atomic force microscopy, to be performed on the same specimen.
This is a preview of subscription content, access via your institution
Relevant articles
Open Access articles citing this article.
-
Recent biomedical advancements in graphene oxide- and reduced graphene oxide-based nanocomposite nanocarriers
Biomaterials Research Open Access 26 November 2022
-
Artificial Intelligence-Aided Low Cost and Flexible Graphene Oxide-Based Paper Sensor for Ultraviolet and Sunlight Monitoring
Nanoscale Research Letters Open Access 12 September 2022
-
Carbon-based nanomaterials engineered cement composites: a review
Journal of Infrastructure Preservation and Resilience Open Access 19 January 2022
Access options
Subscribe to Journal
Get full journal access for 1 year
$119.00
only $9.92 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Tax calculation will be finalised during checkout.
Buy article
Get time limited or full article access on ReadCube.
$32.00
All prices are NET prices.





References
Castro Neto, A. H., Guinea, F., Peres, N. M. R., Novoselov, K. S. & Geim, A. K. The electronic properties of graphene. Available at http://arxiv.org/abs/0709.1163 (2007).
Bunch, J. S. et al. Electromechanical resonators from graphene sheets. Science 315, 490–493 (2007).
Staley, N. et al. Lithography-free fabrication of graphene devices. Appl. Phys. Lett. 90, 143518 (2007).
Viculis, L. M., Mack, J. J. & Kaner, R. B. A chemical route to carbon nanoscrolls. Science 299, 1361 (2003).
Shioyama, H. & Akita, T. A new route to carbon nanotubes. Carbon 41, 179–181 (2003).
Gilje, S., Han, S., Wang, M. S., Wang, K. L. & Kaner, R. B. A chemical route to graphene for device applications. Nano Lett. 7, 3394–3398 (2007).
Berger, C. et al. Ultrathin epitaxial graphite: 2D electron gas properties and a route toward graphene-based nanoelectronics. J. Phys. Chem. B 108, 19912–19916 (2004).
Berger, C. et al. Electronic confinement and coherence in patterned epitaxial graphene. Science 312, 1191–1196 (2006).
Novoselov, K. S. et al. Two-dimensional atomic crystals. Proc. Natl Acad. Sci. USA 102, 10451–10453 (2005).
Castro, A., Guinea, F. & Peres, N. M. Drawing conclusions from grapheme. Phys. World, 33–37 (November 2006).
Ohta, T., Bostwick, A., Seyller, T., Horn, K. & Rotenberg, E. Controlling the electronic structure of bilayer graphene. Science 313, 951–954 (2006).
Stankovich, S., Piner, R. D., Nguyen, S. T. & Ruoff, R. S. Synthesis and exfoliation of isocyanate-treated graphene oxide nanoplatelets. Carbon 44, 3342–3347 (2006).
Stankovich, S. et al. Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide. Carbon 45, 1558–1565 (2007).
Gomez-Navarro, C. et al. Electronic transport properties of individual chemically reduced graphene oxide sheets. Nano Lett. 7, 3499–3503 (2007).
Hummers, W. S. Jr & Offeman, R. E. Preparation of graphitic oxide. J. Am. Chem. Soc. 80, 1339 (1958).
Li, D., Mueller, M. B., Gilje, S., Kaner, R. B. & Wallace, G. G. Processable aqueous dispersion of graphene nanosheets. Nature Nanotech. 3, 101–105 (2008).
Stankovich, S. et al. Stable aqueous dispersions of graphitic nanoplatelets via the reduction of exfoliated graphite oxide in the presence of poly(sodium 4-styrenesulfonate). J. Mater. Chem. 16, 155–158 (2006).
Liu, P. & Gong, K. Synthesis of polyaniline-intercalated graphite oxide by an in situ oxidative polymerization reaction. Carbon 37, 706–707 (1999).
Bourlinos, A. B. et al. Graphite oxide: chemical reduction to graphite and surface modification with primary aliphatic amines and amino acids. Langmuir 19, 6050–6055 (2003).
Mitzi, B. D., Copel, M. & Chey, S. J. Low-voltage transistor employing a high-mobility spin-coated chalcogenide semiconductor. Adv Mater. 17, 1289–1293 (2005).
Wang, X., Zhi, L. & Müllen, K. Transparent, conductive graphene electrodes for dye-sensitized solar cells. Nano Lett. 8, 323–327 (2008).
Schniepp, C. H. et al. Functionalized single graphene sheets derived from splitting graphite oxide. J. Phys. Chem. B 110, 8535–8539 (2006).
Ishigami, M., Chen, J. H., Cullen, W. G., Fuhrer, M. S. & Williams, E. D. Atomic structure of graphene on SiO2 . Nano Lett. 7, 1643–1648 (2007).
Moser, J., Barreiro, A. & Bachtold, A. Current-induced cleaning of graphene. Appl. Phys. Lett. 91, 163513 (2007).
Eda, G., Fanchini, G. & Chhowalla, M. Large-area ultrathin films of reduced graphene oxide as a transparent and flexible electronic material. Nature Nanotech. 3, 270–274 (2008).
Li, X., Wang, X., Zhang, L., Lee, S. & Dai, H. Chemically derived, ultrasmooth graphene nanoribbon semiconductors. Science 319, 1229–1232 (2008).
Li, X . et al. Highly conducting graphene sheets and Langmuir–Blodgett films. Nature Nanotech. 3, 538–542 (2008).
Ferrari, A. C. et al. Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97, 187401 (2006).
Graf, D. et al. Spatially resolved Raman spectroscopy of single- and few-layer graphene. Nano Lett. 7, 238–242 (2007).
Calizo, I., Balandin, A., Bao, W., Miao, F. & Lau, C. N. Temperature dependence of the Raman spectra of graphene and graphene multilayers. Nano Lett. 7, 2645–2649 (2007).
Acknowledgements
This work has been partially supported by the National Science Foundation (NSF; DMR-0507294), the NSF-IGERT programme (M.J.A.) and the Air Force Office of Scientific Research (FA95500710264; V.C.T.). The authors also thank: L. Gomez, A. Steig, G. Yang and R. Chen for their expertise with instrumentation; UCLA CNSI Pico Lab for imaging; S. Gilje for his pioneering efforts at UCLA with graphite oxide; and W. Hou and P. Li for many fruitful discussions.
Author information
Authors and Affiliations
Contributions
V.C.T. and M.J.A. conceived and performed the experiments and measurements. Y.Y. and R.B.K. conceptualized and directed the research project. All authors discussed the results and contributed to the manuscript.
Corresponding authors
Supplementary information
Supplementary Information
Supplementary Information (PDF 2105 kb)
Rights and permissions
About this article
Cite this article
Tung, V., Allen, M., Yang, Y. et al. High-throughput solution processing of large-scale graphene. Nature Nanotech 4, 25–29 (2009). https://doi.org/10.1038/nnano.2008.329
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/nnano.2008.329
This article is cited by
-
Artificial Intelligence-Aided Low Cost and Flexible Graphene Oxide-Based Paper Sensor for Ultraviolet and Sunlight Monitoring
Nanoscale Research Letters (2022)
-
Recent biomedical advancements in graphene oxide- and reduced graphene oxide-based nanocomposite nanocarriers
Biomaterials Research (2022)
-
Carbon-based nanomaterials engineered cement composites: a review
Journal of Infrastructure Preservation and Resilience (2022)
-
Graphene-Based Important Carbon Structures and Nanomaterials for Energy Storage Applications as Chemical Capacitors and Supercapacitor Electrodes: a Review
BioNanoScience (2022)
-
Flash-assisted doping graphene for ultrafast potassium transport
Nano Research (2022)