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Title: Synthesis of Ultra-incompressible sp 3 -Hybridized Carbon Nitride with 1:1 Stoichiometry

Journal Article · · Chemistry of Materials
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Search of materials with C-N composition hold a great promise in creating materials which would rival diamond hardness due to the very strong and relatively low-ionic C-N bond. Early experimental and theoretical works on C-N compounds were based on structural similarity with binary A3B4 structural types; however, the synthesis of C3N4 remains elusive. Here we explored an unbiased synthesis from the elemental materials at high pressures and temperatures. Using in situ synchrotron X-ray diffraction and Raman spectroscopy we demonstrate the synthesis of highly incompressible Pnnm CN compound with sp3 hybridized carbon above 55 GPa and 7000 K. This result is supported by first principles evolutionary search, which finds that Pnnm CN is the most stable compound above 10.9 GPa. On pressure release below 6 GPa the synthesized CN compound amorphizes reattaining its 1:1 stoichiometry as confirmed by Energy-Dispersive X-ray Spectroscopy. Here, this work underscores the importance of understanding of novel high-pressure chemistry rules and it opens a new route for synthesis of superhard materials.

Research Organization:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC52-07NA27344
OSTI ID:
1342047
Report Number(s):
LLNL-JRNL-669803; TRN: US1701534
Journal Information:
Chemistry of Materials, Vol. 28, Issue 19; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 38 works
Citation information provided by
Web of Science

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Cited By (8)

Predicting superhard materials via a machine learning informed evolutionary structure search journal September 2019
Chemistry through cocrystals: pressure-induced polymerization of C 2 H 2 ·C 6 H 6 to an extended crystalline hydrocarbon journal January 2018
Two isomeric solid carbon nitrides with 1 : 1 stoichiometry which exhibit strong mechanical anisotropy journal January 2017
New two-dimensional carbon nitride allotrope with 1 : 1 stoichiometry featuring spine-like structures: a structural and electronic DFT-D study journal January 2019
Helium-hydrogen immiscibility at high pressures journal March 2019
Ground-state structures, physical properties and phase diagram of carbon-rich nitride C 5 N journal August 2018
Phase diagram of carbon and the factors limiting the quantity and size of natural diamonds journal February 2018
Predicting Superhard Materials via a Machine Learning Informed Evolutionary Structure Search preprint January 2019

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