4.7 Article

Stabilization of pentazolate anions in the high-pressure compounds Na2N5 and NaN5 and in the sodium pentazolate framework NaN5•N2

期刊

DALTON TRANSACTIONS
卷 50, 期 21, 页码 7229-7237

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1dt00722j

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资金

  1. Army Research Office [W911NF-19-2-0172]
  2. DOE Office of Science [DE-AC02-06CH11357]
  3. GeoSoilEnviroCARS (Sector 13) - National Science Foundation - Earth Sciences [EAR-1634415]
  4. NSF MRI Proposal [EAR-1531583]

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The synthesis and characterization of nitrogen-rich materials is crucial for designing novel high energy density materials. The formation of oxygen-free pentazolate salts Na2N5, NaN5 and NaN5 center dot N-2 from NaN3 and N-2 at around 50 GPa demonstrates the potential for great compositional diversity and self-templated synthesis of metal-pentazolate frameworks.
Synthesis and characterization of nitrogen-rich materials is important for the design of novel high energy density materials due to extremely energetic low-order nitrogen-nitrogen bonds. The balance between the energy output and stability may be achieved if polynitrogen units are stabilized by resonance as in cyclo-N-5(-) pentazolate salts. Here we demonstrate the synthesis of three oxygen-free pentazolate salts Na2N5, NaN5 and NaN5 center dot N-2 from sodium azide NaN3 and molecular nitrogen N-2 at similar to 50 GPa. NaN5 center dot N-2 is a metal-pentazolate framework (MPF) obtained via a self-templated synthesis method with nitrogen molecules being incorporated into the nanochannels of the MPF. Such self-assembled MPFs may be common in a variety of ionic pentazolate compounds. The formation of Na2N5 demonstrates that the cyclo-N-5 group can accommodate more than one electron and indicates the great accessible compositional diversity of pentazolate salts.

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