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Title: High-pressure synthesis of ultraincompressible hard rhenium nitride pernitride Re 2(N 2)(N) 2 stable at ambient conditions

Abstract

High-pressure synthesis in diamond anvil cells can yield unique compounds with advanced properties, but often they are either unrecoverable at ambient conditions or produced in quantity insufficient for properties characterization. Here we report the synthesis of metallic, ultraincompressible ( K 0 = 28(10) GPa), and very hard (nanoindentation hardness 36.7(8) GPa) rhenium nitride pernitride Re 2(N 2)(N) 2. Unlike known transition metals pernitrides Re 2(N 2)(N) 2 contains both pernitride N 2 4– and discrete N 3– anions, which explains its exceptional properties. Re 2(N 2)(N) 2 can be obtained via a reaction between rhenium and nitrogen in a diamond anvil cell at pressures from 40 to 90 GPa and is recoverable at ambient conditions. We develop a route to scale up its synthesis through a reaction between rhenium and ammonium azide, NH 4N 3, in a large-volume press at 33 GPa. Although metallic bonding is typically seen incompatible with intrinsic hardness, Re 2(N 2)(N) 2 turned to be at a threshold for superhard materials.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [2];  [3];  [3]; ORCiD logo [4];  [4];  [5];  [5];  [6]; ORCiD logo [6];  [7]; ORCiD logo [8]; ORCiD logo [8];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Bayreuth (Germany)
  2. National Univ. of Science and Technology (MISIS), Moscow (Russia)
  3. Linköping Univ. (Sweden)
  4. Friedrich-Alexander-Univ., Erlangen (Germany)
  5. Univ. of Munich (LMU) (Germany)
  6. Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
  7. European Synchrotron Radiation Facility (ESRF), Grenoble (France)
  8. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Photon Science
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
German Research Foundation (DFG); German Federal Ministry of Education and Research (BMBF); Fonds der Chemischen Industrie (FCI); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; Russian Science Foundation (RSF); Ministry of Education and Science of the Russian Federation; Swedish Research Council (VR); Swedish Government Strategic Research Area in Materials Science on Functional Materials; VINN Excellence Center Functional Nanoscale Materials (FunMat-2); European Research Council (ERC)
OSTI Identifier:
1542989
Grant/Contract Number:  
[5K16WC1; EAR-1634415; FG02-94ER14466; AC02-06CH11357; 2015-04391; SFO-Mat-LiU No. 2009-00971; 2016–05156; 787527]
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
[ Journal Volume: 10; Journal Issue: 1]; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
ENGLISH
Subject:
36 MATERIALS SCIENCE; Mechanical properties; Solid-state chemistry

Citation Formats

Bykov, Maxim, Chariton, Stella, Fei, Hongzhan, Fedotenko, Timofey, Aprilis, Georgios, Ponomareva, Alena V., Tasnádi, Ferenc, Abrikosov, Igor A., Merle, Benoit, Feldner, Patrick, Vogel, Sebastian, Schnick, Wolfgang, Prakapenka, Vitali B., Greenberg, Eran, Hanfland, Michael, Pakhomova, Anna, Liermann, Hanns-Peter, Katsura, Tomoo, Dubrovinskaia, Natalia, and Dubrovinsky, Leonid. High-pressure synthesis of ultraincompressible hard rhenium nitride pernitride Re2(N2)(N)2 stable at ambient conditions. United States: N. p., 2019. Web. doi:10.1038/s41467-019-10995-3.
Bykov, Maxim, Chariton, Stella, Fei, Hongzhan, Fedotenko, Timofey, Aprilis, Georgios, Ponomareva, Alena V., Tasnádi, Ferenc, Abrikosov, Igor A., Merle, Benoit, Feldner, Patrick, Vogel, Sebastian, Schnick, Wolfgang, Prakapenka, Vitali B., Greenberg, Eran, Hanfland, Michael, Pakhomova, Anna, Liermann, Hanns-Peter, Katsura, Tomoo, Dubrovinskaia, Natalia, & Dubrovinsky, Leonid. High-pressure synthesis of ultraincompressible hard rhenium nitride pernitride Re2(N2)(N)2 stable at ambient conditions. United States. doi:10.1038/s41467-019-10995-3.
Bykov, Maxim, Chariton, Stella, Fei, Hongzhan, Fedotenko, Timofey, Aprilis, Georgios, Ponomareva, Alena V., Tasnádi, Ferenc, Abrikosov, Igor A., Merle, Benoit, Feldner, Patrick, Vogel, Sebastian, Schnick, Wolfgang, Prakapenka, Vitali B., Greenberg, Eran, Hanfland, Michael, Pakhomova, Anna, Liermann, Hanns-Peter, Katsura, Tomoo, Dubrovinskaia, Natalia, and Dubrovinsky, Leonid. Fri . "High-pressure synthesis of ultraincompressible hard rhenium nitride pernitride Re2(N2)(N)2 stable at ambient conditions". United States. doi:10.1038/s41467-019-10995-3. https://www.osti.gov/servlets/purl/1542989.
@article{osti_1542989,
title = {High-pressure synthesis of ultraincompressible hard rhenium nitride pernitride Re2(N2)(N)2 stable at ambient conditions},
author = {Bykov, Maxim and Chariton, Stella and Fei, Hongzhan and Fedotenko, Timofey and Aprilis, Georgios and Ponomareva, Alena V. and Tasnádi, Ferenc and Abrikosov, Igor A. and Merle, Benoit and Feldner, Patrick and Vogel, Sebastian and Schnick, Wolfgang and Prakapenka, Vitali B. and Greenberg, Eran and Hanfland, Michael and Pakhomova, Anna and Liermann, Hanns-Peter and Katsura, Tomoo and Dubrovinskaia, Natalia and Dubrovinsky, Leonid},
abstractNote = {High-pressure synthesis in diamond anvil cells can yield unique compounds with advanced properties, but often they are either unrecoverable at ambient conditions or produced in quantity insufficient for properties characterization. Here we report the synthesis of metallic, ultraincompressible (K0 = 28(10) GPa), and very hard (nanoindentation hardness 36.7(8) GPa) rhenium nitride pernitride Re2(N2)(N)2. Unlike known transition metals pernitrides Re2(N2)(N)2 contains both pernitride N24– and discrete N3– anions, which explains its exceptional properties. Re2(N2)(N)2 can be obtained via a reaction between rhenium and nitrogen in a diamond anvil cell at pressures from 40 to 90 GPa and is recoverable at ambient conditions. We develop a route to scale up its synthesis through a reaction between rhenium and ammonium azide, NH4N3, in a large-volume press at 33 GPa. Although metallic bonding is typically seen incompatible with intrinsic hardness, Re2(N2)(N)2 turned to be at a threshold for superhard materials.},
doi = {10.1038/s41467-019-10995-3},
journal = {Nature Communications},
number = [1],
volume = [10],
place = {United States},
year = {2019},
month = {7}
}

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