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New cerium-nitrogen (Ce-N) compounds, including a layered molecular sieve CeN14, exhibit remarkable stability and high energy density. CeN14 shows potential as a high-energy material, stable at ambient conditions.

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Area of Science:

  • Materials Science
  • High-Pressure Physics
  • Computational Chemistry

Background:

  • Cerium-nitrogen (Ce-N) compounds are explored for novel material properties.
  • High-pressure synthesis is a key method for discovering new nitrogen-rich materials.

Purpose of the Study:

  • To investigate the structural, dynamical, and electronic properties of Ce-N compounds under high pressure.
  • To identify stable and metastable Ce-N phases with potential energetic applications.

Main Methods:

  • High-throughput computational screening.
  • Density Functional Theory (DFT) calculations.
  • Phonon and elastic stability analyses.

Main Results:

  • Prediction of four Ce-N phases: I41/a-CeN4, R3̅m-CeN6, P6mm-CeN14, and P6mm-CeN17.
  • Identification of polymeric nitrogen structures including helical chains, N6 rings, and layered molecular sieves.
  • I41/a-CeN4 is quenchable to ambient conditions with thermal stability up to 500 K.
  • P6mm-CeN14 is dynamically and mechanically stable at ambient pressure.
  • Electronic properties reveal significant charge transfer contributing to ionic (Ce-N) and covalent (N-N) bonding.
  • P6mm-CeN14 exhibits the highest energy density (8.45 kJ/g) and explosive performance among metal polynitrides.

Conclusions:

  • Ce-N compounds can form stable and metastable phases with diverse polymeric nitrogen structures.
  • The layered molecular sieve P6mm-CeN14 represents a new record for high-energy metal polynitrides.
  • Understanding charge transfer mechanisms is crucial for designing stable energetic materials.