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Synthesis of Nine-atom Deltahedral Zintl Ions of Germanium and their Functionalization with Organic Groups
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Threefold coordinated germanium in a GeO2 melt.

Songming Wan1,2,3, Shujie Zhang4, Bin Li4

  • 1Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei, 230031, China. smwan@aiofm.ac.cn.

Nature Communications
|November 3, 2023
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Researchers discovered a new chain structure in germanium dioxide (GeO2) melt, challenging the long-held view of germanium coordination. This finding clarifies germanate chemistry and resolves a decades-old debate in material science.

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Area of Science:

  • Material science
  • Geochemistry
  • Solid-state chemistry

Background:

  • The local structure of germanium in GeO2 melt is a fundamental, debated topic.
  • Prevailing view suggests germanium is coordinated by at least four oxygen atoms.
  • Unexplained bands in Raman spectra challenge existing models of GeO2 melt structure.

Purpose of the Study:

  • To investigate the local structure of germanium in GeO2 melt.
  • To resolve the longstanding debate regarding germanium coordination in GeO2.
  • To provide a new perspective on germanate chemistry.

Main Methods:

  • In situ Raman spectroscopy was employed to analyze GeO2 melt.
  • Density functional theory (DFT) computations were utilized for structural analysis.
  • Computational electronic structure analysis elucidated bonding characteristics.

Main Results:

  • A novel [GeOØ2]n chain structure was identified in GeO2 melt, where Ø represents bridging oxygen.
  • In this structure, germanium is primarily coordinated by three oxygen atoms.
  • A weak interaction was observed between germanium and neighboring non-bridging oxygen atoms.

Conclusions:

  • The identified chain structure provides a resolution to the ongoing debate on GeO2 melt structure.
  • The findings necessitate a revision of the prevailing viewpoint on germanium coordination.
  • This study offers new insights into the fundamental aspects of germanate chemistry.