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Conversion of silicon carbide to crystalline diamond-structured carbon at ambient pressure

Nature volume 411, pages 283–287 (2001)Cite this article

Abstract

Synthetic diamond is formed commercially using high-pressure1, chemical-vapour-deposition2 and shock-wave3 processes, but these approaches have serious limitations owing to low production volumes and high costs. Recently suggested alternative methods of diamond growth include plasma activation4, high pressures5, exotic precursors6,7 or explosive mixtures8, but they suffer from very low yield and are intrinsically limited to small volumes or thin films. Here we report the synthesis of nano- and micro-crystalline diamond-structured carbon, with cubic and hexagonal structure, by extracting silicon from silicon carbide in chlorine-containing gases at ambient pressure and temperatures not exceeding 1,000 °C. The presence of hydrogen in the gas mixture leads to a stable conversion of silicon carbide to diamond-structured carbon with an average crystallite size ranging from 5 to 10 nanometres. The linear reaction kinetics allows transformation to any depth, so that the whole silicon carbide sample can be converted to carbon. Nanocrystalline coatings of diamond-structured carbon produced by this route show promising mechanical properties, with hardness values in excess of 50 GPa and Young's moduli up to 800 GPa. Our approach should be applicable to large-scale production of crystalline diamond-structured carbon.

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Figure 1: Results of nano-indentation tests.
Figure 2: High-resolution TEM micrographs showing the structure of the carbon coating within a micrometre of the SiC/carbon interface.
Figure 3: Characterization of crystalline diamond-structured carbon embedded in amorphous carbon.
Figure 4: Microstructure of a carbon film produced in Cl2/H2.

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Acknowledgements

We thank A. Nicholls for discussions and help with TEM analysis. The work done at UIC was supported by the US NSF, and the work done at Drexel University was supported by DARPA via ONR contract. The electron microscopes used in this work are operated by the Research Resources Center at UIC. The JEM-2010F purchase was supported by the NSF.

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Authors and Affiliations

  1. Department of Materials Engineering, Drexel University, Philadelphia, 19104, Pennsylvania, USA

    Yury Gogotsi

  2. Department of Civil and Material Engineering, University of Illinois at Chicago, 842 West Taylor Street, Chicago, 60607, Illinois, USA

    Yury Gogotsi, Sascha Welz, Daniel A. Ersoy & Michael J. McNallan

Authors
  1. Yury Gogotsi
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Corresponding author

Correspondence to Yury Gogotsi.

Supplementary information

Figure 1.

(JPG 12.4 KB)

Convergent-beam electron diffraction (CBED) patterns fromnanocrystals (5-10 nm size) in a sample treated in Ar-3.5% chlorine at1000ºC. The diamond-containing area was within a micrometer from theSiC/carbon interface. a, b, may be attributed to cubic Fd3m or F43mstructures with reflections at 0.206 nm (111) and 0.126 nm (022), as well asforbidden diamond reflections. c,d, may be attributed to hexagonal diamond(lonsdaleite) with reflections at 0.219 (100) and 0.126 nm (110). e, EDSspectrum showing that the analyzed material is nearly pure carbon. Tracesof amorphous silica were present due to oxygen impurity in the gas. Thecopper peak comes from the supporting grid. Other EDS spectra from theanalyzed areas showed even lower content of impurities in carbon.

Figure 2.

(JPG 25.2 KB)

SAD pattern from the nanocrystalline film. Sharp Braggreflections are visible up to the order of (800), indicating good crystallinity.No scattering intensity from either graphite or amorphous carbon can beseen, suggesting that the film is pure diamond, but high intensity of forbiddenreflections suggests a lower symmetry (F&4macr;3m) or impurity superstructure.Sample was sintered α-SiC treated in 2.77% CI2-1.04%H2 (balance Ar) for 5hours at 1000ºC.

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Gogotsi, Y., Welz, S., Ersoy, D. et al. Conversion of silicon carbide to crystalline diamond-structured carbon at ambient pressure. Nature 411, 283–287 (2001). https://doi.org/10.1038/35077031

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