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Is the planar hexacoordinate nitrogen molecule NB(6)(-) viable?

Chang-Bin Shao1, Yi-Hong Ding

  • 1State Key Laboratory of Theoretical and Computational Chemistry, Institute of Theoretical Chemistry, Jilin University, Changchun 130023, People's Republic of China.

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Summary
This summary is machine-generated.

The planar hexacoordinate nitrogen (phN) unit, NB(6)(-), is thermodynamically unstable and unlikely to be isolated. Investigating intrinsic stability is crucial for predicting viable exotic molecules.

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Area of Science:

  • Computational Chemistry
  • Quantum Chemistry
  • Materials Science

Background:

  • Molecules with hypercoordinate planar centers challenge traditional chemical bonding models.
  • Planar hexacoordinate nitrogen (phN) units, NB(6)(-), have been proposed for cluster-assembly but their stability is unknown.
  • Intrinsic stability is a key factor for predicting the viability of novel molecular structures.

Purpose of the Study:

  • To investigate the thermodynamic and kinetic stability of the planar hexacoordinate nitrogen (phN) unit, NB(6)(-).
  • To assess the stability of NB(6)(-) in both free and assembled ([NB(6)](2)Fe) forms.
  • To determine the likelihood of isolating the phN structure of NB(6)(-).

Main Methods:

  • High-level ab initio calculations, specifically CCSD(T)/6-311+G(2df)//B3LYP/6-311+G(d)+ZPVE.
  • Calculation of barrier heights for phN conversion in free and assembled states.
  • Thermodynamic stability analysis by comparing phN structures to lower-lying isomers.

Main Results:

  • The planar hexacoordinate nitrogen (phN) unit exhibits low kinetic stability with small barrier heights for conversion (9.2 and 4.4 kcal mol(-1) for free and assembled forms, respectively).
  • The phN structure is significantly thermodynamically unstable, being 102.8 and 162.1 kcal mol(-1) higher in energy than its isomers.
  • Comparison with the isoelectronic planar hexacoordinate carbon (phC) unit, CB(6)(2-), highlights differences in stability.

Conclusions:

  • Isolation of the planar hexacoordinate nitrogen (phN) structure, NB(6)(-), in either the gas phase or assembled forms is unlikely due to combined thermodynamic and kinetic instability.
  • The study underscores the necessity of evaluating intrinsic stability for predicting the viability of molecules with exotic structures.
  • Future research should focus on robust theoretical investigations of stability before experimental synthesis of novel hypercoordinate species.