journal article·2016-10-11Open access

Synthesis of Ultra-incompressible sp3-Hybridized Carbon Nitride with 1:1 Stoichiometry

Elissaios Stavrou, Sergey Lobanov, Huafeng Dong, Artem R. Oganov, Vitali B. Prakapenka, Zuzana Konôpková, Alexander F. Goncharov

Chemistry of Materials· Volume 28· Issue 19

Abstract

The search of compounds with C x N y composition holds great promise for creating materials which would rival diamond in hardness due to the very strong covalent C–N bond. Early theoretical and experimental works on C x N y compounds were based on the hypothetical structural similarity of predicted C 3 N 4 phases with known binary A 3 B 4 structural types; however, the synthesis of C 3 N 4 other than g-C 3 N 4 remains elusive. Here, we explore an “elemental synthesis” at high pressures and temperatures in which the compositional limitations due to the use of precursors in the early works are substantially lifted. Using in situ synchrotron X-ray diffraction and Raman spectroscopy, we demonstrate the synthesis of a highly incompressible Pnnm CN compound ( x = y = 1) with sp 3 -hybridized carbon above 55 GPa and 7000 K. This result is supported by first-principles evolutionary search, which finds that CN is the most stable compound above 14 GPa. On pressure release below 6 GPa, the synthesized CN compound amorphizes, maintaining its 1:1 stoichiometry as confirmed by energy-dispersive X-ray spectroscopy. This work underscores the importance of understanding the novel high-pressure chemistry laws that promote extended 3D C-N structures, never observed at ambient conditions. Moreover, it opens a new route for synthesis of superhard materials based on novel stoichiometries
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Research context

OpenAlex topics: Diamond and Carbon-based Materials Research · Metal and Thin Film Mechanics · High-pressure geophysics and materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Geophysical Laboratory, Carnegie Institution of Washington, Washington, DC 20015, United States

Lawrence Livermore National Laboratory, Physical and Life Sciences Directorate, P.O. Box 808, L-350, Livermore, California 94550, United States

Sobolev Institute of Geology and Mineralogy Siberian Branch Russian Academy of Sciences, 3 Pr. Ac. Koptyga, Novosibirsk 630090, Russia

Department of Geosciences, Center for Materials by Design, Institute for Advanced Computational Science, Stony Brook University, Stony Brook, New York 11794-2100, United States

Skolkovo Institute of Science and Technology, Skolkovo Innovation Center, 5 Nobel St., Moscow 143026, Russia

Moscow Institute of Physics and Technology, 9 Institutskiy Lane, Dolgoprudny City, Moscow Region 141700, Russia

School of Materials Science, Northwestern Polytechnical University, Xi’an 710072, China

Center for Advanced Radiation Sources, University of Chicago, Chicago, Illinois 60637, United States

DESY Photon Science, D-22607 Hamburg, Germany

University of Science and Technology of China, Hefei 230026, China

Key Laboratory of Materials Physics and Center for Energy Matter in Extreme Environments, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, China

Funding

Defense Advanced Research Projects Agency · Lawrence Livermore National Laboratory · Alfred P. Sloan Foundation · Ministry of Education and Science of the Russian Federation · National Natural Science Foundation of China · Seventh Framework Programme · Chinese Academy of Sciences

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