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Divide and Stack Up: Boron-Based Sandwich Cluster as a Subnanoscale Propeller.

Ying-Jin Wang1,2, Lin-Yan Feng1, Hua-Jin Zhai1

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Chemistry, an Asian Journal
|July 19, 2019
PubMed
Summary

Researchers discovered a unique boron-lithium cluster, B7Li4-, acting as a subnanoscale propeller. This cluster exhibits dynamic fluxionality with a rotating lithium ring, stabilized by strong aromaticity and ionic bonding.

Keywords:
boron-based clustersmolecular dynamicsmultifold π/σ aromaticitystructural fluxionalitysubnanoscale propeller

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Area of Science:

  • Cluster Chemistry
  • Materials Science
  • Computational Chemistry

Background:

  • Typical salts feature alternating positive and negative ions.
  • Decorated layered materials have ions fixed on polygonal sites for electrostatic stability.

Purpose of the Study:

  • To report a novel boron-lithium cluster with unique structural and dynamic properties.
  • To investigate the electronic structure, bonding, and fluxional behavior of the B7Li4- cluster.

Main Methods:

  • High-level ab initio calculations, specifically coupled-cluster with singles, doubles, and triples (CCSD(T)) at the single-point level.
  • Analysis of electronic structure, including charge transfer and aromaticity.
  • Investigation of dynamic fluxionality through rotation barrier calculations.

Main Results:

  • A disk-like B7 core is discovered, sandwiched by a Li3 ring and a single Li atom in the B7Li4- cluster.
  • The Li3 ring exhibits free rotation on the B7 disk at low temperatures (200 K) with a low rotation barrier (0.37 kcal/mol).
  • The cluster forms a salt complex [Li3]+[B7]3-[Li]+, stabilized by 2σ aromaticity in the Li3 layer and π/σ sextets in the B7 core, with strong interlayer ionic bonding (3-4 eV).

Conclusions:

  • The B7Li4- cluster represents a unique subnanoscale propeller with significant dynamic fluxionality.
  • Strong covalent and ionic interactions, coupled with multi-fold aromaticity, stabilize this dynamically active system.
  • This discovery challenges conventional notions of ion anchoring and stability in layered materials.