High‐Pressure Synthesis of <i>oP</i>28‐C<sub>3</sub>N<sub>4</sub> Recoverable to Ambient Conditions
Abstract The thermodynamic parameter pressure is ideal for producing novel ultraincompressible and superhard materials as it promotes the formation of polymeric frameworks and higher atomic coordination. In this regard, carbon and nitrogen are particularly attractive elements as they can produce extended arrangements of strong covalent bonds. In this study, a previously unobserved C 3 N 4 polymorph, denoted as oP 28‐C 3 N 4 ( Pnnm , #58), is synthesized at pressures between 73 and 104 GPa in laser‐heated diamond anvil cells and found recoverable to ambient conditions and stable in air. The crystal structure of oP 28‐C 3 N 4 , comprised of corner‐sharing CN 4 tetrahedra, is solved and refined using synchrotron single‐crystal X‐ray diffraction. With a bulk modulus of 334(3) GPa deduced from experimental data, the compound is highly incompressible. Based on macroscopic and microscopic calculations, its hardness may achieve 47.5 or 79.7 GPa, respectively, making it a superhard material. Incompressibility of CN 4 tetrahedra in all experimentally observed C 3 N 4 polymorphs is found to be greater than that of the CC 4 and BN 4 tetrahedra forming the structures of diamond and cubic boron nitride. Density functional theory calculations provide further insight into the electronic, vibrational, and mechanical properties of oP 28‐C 3 N 4 , as well as their stability relative to other C─N phases.
Authors
- Dominique Laniel (ORCID: https://orcid.org/0000-0002-6889-9820)
- Fariia Iasmin Akbar (ORCID: https://orcid.org/0000-0002-6016-5849)
- Umbertoluca Ranieri (ORCID: https://orcid.org/0000-0003-2026-6132)
- Vitali B. Prakapenka (ORCID: https://orcid.org/0000-0001-9270-2330)
- James Spender
- Yuqing Yin (ORCID: https://orcid.org/0000-0001-8861-8443)
- Timofey Fedotenko (ORCID: https://orcid.org/0000-0002-4602-2059)
- Natalia Dubrovinskaia (ORCID: https://orcid.org/0000-0002-8256-5675)
- Mohamed Mézouar (ORCID: https://orcid.org/0000-0001-5336-544X)
- Alena Aslandukovа (ORCID: https://orcid.org/0000-0002-4730-4197)
- Stella Chariton (ORCID: https://orcid.org/0000-0001-5522-0498)
- Ferenc Tasnádi (ORCID: https://orcid.org/0000-0001-6373-5109)
- Anna Pakhomova (ORCID: https://orcid.org/0000-0003-4014-0203)
- Akun Liang (ORCID: https://orcid.org/0000-0002-0515-0484)
- Andrey Aslandukov (ORCID: https://orcid.org/0000-0003-0988-6066)
- Michael Hanfland (ORCID: https://orcid.org/0000-0002-8904-5461)
- Gastón Garbarino (ORCID: https://orcid.org/0000-0003-4780-9520)
- Wenju Zhou (ORCID: https://orcid.org/0000-0002-9556-1147)
- Florian Trybel (ORCID: https://orcid.org/0000-0003-0514-5084)
- Igor A. Abrikosov (ORCID: https://orcid.org/0000-0001-7551-4717)
- Leonid Dubrovinsky (ORCID: https://orcid.org/0000-0002-3717-7585)
Institutions
- Linköping University (SE)
- Deutsches Elektronen-Synchrotron DESY (DE)
- European Synchrotron Radiation Facility (FR)
- University of Chicago (US)
- University of Bayreuth (DE)
- University of Edinburgh (GB)
Publication Details
- Journal
- Advanced Functional Materials
- Published
- 2024-12-13
- DOI
- https://doi.org/10.1002/adfm.202416892
- Citations
- 6
- Primary Topic
- Luminescence Properties of Advanced Materials
- Type
- article
- Field-Weighted Citation Impact
- 0.70
Funders
- UK Research and Innovation
- Deutsche Forschungsgemeinschaft
- European Synchrotron Radiation Facility
- Linköpings Universitet
- Knut och Alice Wallenbergs Stiftelse
- Vetenskapsrådet
- China Scholarship Council
- Deutsches Elektronen-Synchrotron
- HORIZON EUROPE European Research Council