High-Pressure Synthesis of Metal–Inorganic Frameworks Hf4N20·N2, WN8·N2, and Os5N28·3 N2 with Polymeric Nitrogen Linkers
Abstract
Polynitrides are intrinsically thermodynamically unstable at ambient conditions and require peculiar synthetic approaches. Now, a one-step synthesis of metal–inorganic frameworks Hf4N20·N2, WN8·N2, and Os5N28·3 N2 via direct reactions between elements in a diamond anvil cell at pressures exceeding 100 GPa is reported. The porous frameworks (Hf4N20, WN8, and Os5N28) are built from transition-metal atoms linked either by polymeric polydiazenediyl (polyacetylene-like) nitrogen chains or through dinitrogen units. Triply bound dinitrogen molecules occupy channels of these frameworks. Owing to conjugated polydiazenediyl chains, these compounds exhibit metallic properties. The high-pressure reaction between Hf and N2 also leads to a non-centrosymmetric polynitride Hf2N11 that features double-helix catena-poly[tetraz-1-ene-1,4-diyl] nitrogen chains [–N–N–N=N–]∞.
- Authors:
-
[1];
[8];
[11];
[4]
- Howard Univ., Washington, DC (United States). Dept. of Mathematics; Univ. of Bayreuth (Germany). Bayerisches Geoinstitut; Carnegie Institution for Science, Washington, DC (United States). The Earth and Planets Lab.
- Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources
- Carnegie Institution for Science, Washington, DC (United States). The Earth and Planets Lab.
- Univ. of Bayreuth (Germany). Bayerisches Geoinstitut
- Univ. of Bayreuth (Germany). Material Physics and Technology at Extreme Conditions. Lab. of Crystallography
- National Univ. of Science and Technology “MISIS”, Moscow (Russian Federation). Materials Modeling and Development Lab.
- Linköping Univ. (Sweden). Dept. of Physics, Chemistry and Biology
- European Synchrotron Radiation Facility (ESRF), Grenoble (France)
- Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Photon Science
- Howard Univ., Washington, DC (United States). Dept. of Mathematics
- Univ. of Bayreuth (Germany). Material Physics and Technology at Extreme Conditions. Lab. of Crystallography; Linköping Univ. (Sweden). Dept. of Physics, Chemistry and Biology
- Publication Date:
- Research Org.:
- Univ. of Chicago, IL (United States); Howard Univ., Washington, DC (United States); Univ. of Bayreuth (Germany); National Univ. of Science and Technology “MISIS”, Moscow (Russian Federation); Linköping Univ. (Sweden)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); US Army Research Office (ARO); German Research Foundation (DFG); German Federal Ministry of Education and Research (BMBF); Russian Science Foundation; Swedish Government Strategic Research Area in Materials Science on Functional Materials; Knut and Alice Wallenberg Foundation (Sweden); Swedish Research Council (VR)
- OSTI Identifier:
- 1646607
- Grant/Contract Number:
- FG02-94ER14466; EAR-1634415; W911NF-19-2-0172; DU 954-11/1; DU 393-9/2; DU 393-13/1; 05K19WC1; 18-12-00492; 2009 00971; KAW-2018.0194; 2019-05600; 2016-05156
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 26; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Bykov, Maxim, Chariton, Stella, Bykova, Elena, Khandarkhaeva, Saiana, Fedotenko, Timofey, Ponomareva, Alena V., Tidholm, Johan, Tasnádi, Ferenc, Abrikosov, Igor A., Sedmak, Pavel, Prakapenka, Vitali, Hanfland, Michael, Liermann, Hanns‐Peter, Mahmood, Mohammad, Goncharov, Alexander F., Dubrovinskaia, Natalia, and Dubrovinsky, Leonid. High-Pressure Synthesis of Metal–Inorganic Frameworks Hf4N20·N2, WN8·N2, and Os5N28·3 N2 with Polymeric Nitrogen Linkers. United States: N. p., 2020.
Web. doi:10.1002/anie.202002487.
Bykov, Maxim, Chariton, Stella, Bykova, Elena, Khandarkhaeva, Saiana, Fedotenko, Timofey, Ponomareva, Alena V., Tidholm, Johan, Tasnádi, Ferenc, Abrikosov, Igor A., Sedmak, Pavel, Prakapenka, Vitali, Hanfland, Michael, Liermann, Hanns‐Peter, Mahmood, Mohammad, Goncharov, Alexander F., Dubrovinskaia, Natalia, & Dubrovinsky, Leonid. High-Pressure Synthesis of Metal–Inorganic Frameworks Hf4N20·N2, WN8·N2, and Os5N28·3 N2 with Polymeric Nitrogen Linkers. United States. https://doi.org/10.1002/anie.202002487
Bykov, Maxim, Chariton, Stella, Bykova, Elena, Khandarkhaeva, Saiana, Fedotenko, Timofey, Ponomareva, Alena V., Tidholm, Johan, Tasnádi, Ferenc, Abrikosov, Igor A., Sedmak, Pavel, Prakapenka, Vitali, Hanfland, Michael, Liermann, Hanns‐Peter, Mahmood, Mohammad, Goncharov, Alexander F., Dubrovinskaia, Natalia, and Dubrovinsky, Leonid. Tue .
"High-Pressure Synthesis of Metal–Inorganic Frameworks Hf4N20·N2, WN8·N2, and Os5N28·3 N2 with Polymeric Nitrogen Linkers". United States. https://doi.org/10.1002/anie.202002487. https://www.osti.gov/servlets/purl/1646607.
@article{osti_1646607,
title = {High-Pressure Synthesis of Metal–Inorganic Frameworks Hf4N20·N2, WN8·N2, and Os5N28·3 N2 with Polymeric Nitrogen Linkers},
author = {Bykov, Maxim and Chariton, Stella and Bykova, Elena and Khandarkhaeva, Saiana and Fedotenko, Timofey and Ponomareva, Alena V. and Tidholm, Johan and Tasnádi, Ferenc and Abrikosov, Igor A. and Sedmak, Pavel and Prakapenka, Vitali and Hanfland, Michael and Liermann, Hanns‐Peter and Mahmood, Mohammad and Goncharov, Alexander F. and Dubrovinskaia, Natalia and Dubrovinsky, Leonid},
abstractNote = {Polynitrides are intrinsically thermodynamically unstable at ambient conditions and require peculiar synthetic approaches. Now, a one-step synthesis of metal–inorganic frameworks Hf4N20·N2, WN8·N2, and Os5N28·3 N2 via direct reactions between elements in a diamond anvil cell at pressures exceeding 100 GPa is reported. The porous frameworks (Hf4N20, WN8, and Os5N28) are built from transition-metal atoms linked either by polymeric polydiazenediyl (polyacetylene-like) nitrogen chains or through dinitrogen units. Triply bound dinitrogen molecules occupy channels of these frameworks. Owing to conjugated polydiazenediyl chains, these compounds exhibit metallic properties. The high-pressure reaction between Hf and N2 also leads to a non-centrosymmetric polynitride Hf2N11 that features double-helix catena-poly[tetraz-1-ene-1,4-diyl] nitrogen chains [–N–N–N=N–]∞.},
doi = {10.1002/anie.202002487},
journal = {Angewandte Chemie (International Edition)},
number = 26,
volume = 59,
place = {United States},
year = {2020},
month = {3}
}
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Figure 1: a)–f) Crystal structures of a) WN8·N2, b) Os5N28·3N2, and c) Hf4N20·N2, and geometries of the channels in the crystal structures (d–f). Distances are given in . g)–i) Types of nitrogen units building the network and types of metal coordination in corresponding compounds. Blue spheres represent nitrogen atoms thatmore »
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