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Rivalry under Pressure: The Coexistence of Ambient‐Pressure Motifs and Close‐Packing in Silicon Phosphorus Nitride Imide SiP 2 N 4 NH
Author(s) -
Vogel Sebastian,
Buda Amalina T.,
Schnick Wolfgang
Publication year - 2019
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201813789
Subject(s) - nitride , crystallography , ambient pressure , octahedron , silicon , crystal structure , silicon nitride , x ray crystallography , materials science , chemistry , diffraction , nanotechnology , organic chemistry , physics , layer (electronics) , optics , thermodynamics
Abstract Non‐metal nitrides such as BN, Si 3 N 4 , and P 3 N 5 meet numerous demands on high‐performance materials, and their high‐pressure polymorphs exhibit outstanding mechanical properties. Herein, we present the silicon phosphorus nitride imide SiP 2 N 4 NH featuring sixfold coordinated Si. Using the multi‐anvil technique, SiP 2 N 4 NH was obtained by high‐pressure high‐temperature synthesis at 8 GPa and 1100 °C with in situ formed HCl acting as a mineralizer. Its structure was elucidated by a combination of single‐crystal X‐ray diffraction and solid‐state NMR measurements. Moreover, SiP 2 N 4 NH was characterized by energy‐dispersive X‐ray spectroscopy and (temperature‐dependent) powder X‐ray diffraction. The highly condensed Si/P/N framework features PN 4 tetrahedra as well as the rare motif of SiN 6 octahedra, and is discussed in the context of ambient‐pressure motifs competing with close‐packing of nitride anions, representing a missing link in the high‐pressure chemistry of non‐metal nitrides.