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Vogel, Sebastian; Buda, Amalina T.; Schnick, Wolfgang (2019): Rivalry under Pressure: The Coexistence of Ambient-Pressure Motifs and Close-Packing in Silicon Phosphorus Nitride Imide SiP2N4NH. In: Angewandte Chemie-International Edition, Vol. 58, No. 11: pp. 3398-3401
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Non-metal nitrides such as BN, Si3N4, and P3N5 meet numerous demands on high-performance materials, and their high-pressure polymorphs exhibit outstanding mechanical properties. Herein, we present the silicon phosphorus nitride imide SiP2N4NH featuring sixfold coordinated Si. Using the multi-anvil technique, SiP2N4NH was obtained by high-pressure high-temperature synthesis at 8 GPa and 1100 degrees 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, SiP2N4NH was characterized by energy-dispersive X-ray spectroscopy and (temperature-dependent) powder X-ray diffraction. The highly condensed Si/P/N framework features PN4 tetrahedra as well as the rare motif of SiN6 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.