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Title: Fe-N system at high pressure reveals a compound featuring polymeric nitrogen chains

Abstract

Poly-nitrogen compounds have been considered as potential high energy density materials for a long time due to the large number of energetic N–N or N=N bonds. In most cases high nitrogen content and stability at ambient conditions are mutually exclusive, thereby making the synthesis of such materials challenging. One way to stabilize such compounds is the application of high pressure. Here, through a direct reaction between Fe and N 2 in a laser-heated diamond anvil cell, we synthesize three ironnitrogen compounds Fe 3N 2, FeN 2 and FeN 4. Their crystal structures are revealed by single-crystal synchrotron X-ray diffraction. Fe 3N 2, synthesized at 50 GPa, is isostructural to chromium carbide Cr 3C 2. FeN 2 has a marcasite structure type and features covalently bonded dinitrogen units in its crystal structure. FeN 4, synthesized at 106 GPa, features polymeric nitrogen chains of [N 4 2-] n units. Based on results of structural studies and theoretical analysis, [N 4 2-] n units in this compound reveal catena-poly[tetraz-1-ene-1,4-diyl] anions.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [3];  [1]; ORCiD logo [1];  [4]; ORCiD logo [1]; ORCiD logo [5];  [6];  [3];  [7];  [8];  [9]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Bayreuth (Germany)
  2. Univ. of Bayreuth (Germany); Deutsches Elektronen-Synchrotron, Hamburg (Germany)
  3. Deutsches Elektronen-Synchrotron, Hamburg (Germany)
  4. University of Münster (Germany)
  5. European Synchrotron Radiation Facility, Grenoble Cedex (France)
  6. Univ. of Chicago, Argonne, IL (United States)
  7. Linköping University (Sweden); National University of Science and Technology ‘MISIS’, Moscow (Russia)
  8. National University of Science and Technology ‘MISIS’, Moscow (Russia)
  9. Linköping University (Sweden)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1460869
Grant/Contract Number:  
FG02-94ER14466; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
ENGLISH
Subject:
36 MATERIALS SCIENCE

Citation Formats

Bykov, M., Bykova, E., Aprilis, G., Glazyrin, K., Koemets, E., Chuvashova, I., Kupenko, I., McCammon, C., Mezouar, M., Prakapenka, V., Liermann, H. -P., Tasnádi, F., Ponomareva, A. V., Abrikosov, I. A., Dubrovinskaia, N., and Dubrovinsky, L. Fe-N system at high pressure reveals a compound featuring polymeric nitrogen chains. United States: N. p., 2018. Web. doi:10.1038/s41467-018-05143-2.
Bykov, M., Bykova, E., Aprilis, G., Glazyrin, K., Koemets, E., Chuvashova, I., Kupenko, I., McCammon, C., Mezouar, M., Prakapenka, V., Liermann, H. -P., Tasnádi, F., Ponomareva, A. V., Abrikosov, I. A., Dubrovinskaia, N., & Dubrovinsky, L. Fe-N system at high pressure reveals a compound featuring polymeric nitrogen chains. United States. doi:10.1038/s41467-018-05143-2.
Bykov, M., Bykova, E., Aprilis, G., Glazyrin, K., Koemets, E., Chuvashova, I., Kupenko, I., McCammon, C., Mezouar, M., Prakapenka, V., Liermann, H. -P., Tasnádi, F., Ponomareva, A. V., Abrikosov, I. A., Dubrovinskaia, N., and Dubrovinsky, L. Mon . "Fe-N system at high pressure reveals a compound featuring polymeric nitrogen chains". United States. doi:10.1038/s41467-018-05143-2. https://www.osti.gov/servlets/purl/1460869.
@article{osti_1460869,
title = {Fe-N system at high pressure reveals a compound featuring polymeric nitrogen chains},
author = {Bykov, M. and Bykova, E. and Aprilis, G. and Glazyrin, K. and Koemets, E. and Chuvashova, I. and Kupenko, I. and McCammon, C. and Mezouar, M. and Prakapenka, V. and Liermann, H. -P. and Tasnádi, F. and Ponomareva, A. V. and Abrikosov, I. A. and Dubrovinskaia, N. and Dubrovinsky, L.},
abstractNote = {Poly-nitrogen compounds have been considered as potential high energy density materials for a long time due to the large number of energetic N–N or N=N bonds. In most cases high nitrogen content and stability at ambient conditions are mutually exclusive, thereby making the synthesis of such materials challenging. One way to stabilize such compounds is the application of high pressure. Here, through a direct reaction between Fe and N2 in a laser-heated diamond anvil cell, we synthesize three ironnitrogen compounds Fe3N2, FeN2 and FeN4. Their crystal structures are revealed by single-crystal synchrotron X-ray diffraction. Fe3N2, synthesized at 50 GPa, is isostructural to chromium carbide Cr3C2. FeN2 has a marcasite structure type and features covalently bonded dinitrogen units in its crystal structure. FeN4, synthesized at 106 GPa, features polymeric nitrogen chains of [N42-]n units. Based on results of structural studies and theoretical analysis, [N42-]n units in this compound reveal catena-poly[tetraz-1-ene-1,4-diyl] anions.},
doi = {10.1038/s41467-018-05143-2},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {7}
}

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