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Anionic silicate organic frameworks constructed from hexacoordinate silicon centres.

Jérôme Roeser1, Dragica Prill2, Michael J Bojdys3,4

  • 1Department of Chemistry, Technische Universität Berlin, BA2, Hardenbergstraße 40, 10623 Berlin, Germany.

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Summary
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Researchers synthesized novel silicate organic frameworks using reversible silicon-oxygen chemistry. These materials feature hexacoordinate silicon and permanent microporosity, similar to zeolites.

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Area of Science:

  • Materials Science
  • Inorganic Chemistry
  • Crystallography

Background:

  • Hexacoordinate silicon species were previously limited to high-pressure silicate phases.
  • Covalent organic frameworks (COFs) offer tunable structures but typically lack hexacoordinate silicon.

Purpose of the Study:

  • To develop a simple, one-pot synthesis for novel silicate organic frameworks (SOFs).
  • To investigate the structural and porous properties of SOFs built from octahedral SiO6 units.

Main Methods:

  • Utilized reversible Si-O chemistry for framework crystallization.
  • Employed 29Si nuclear magnetic resonance (NMR) for structural analysis.
  • Characterized materials using X-ray diffraction, DFT calculations, and gas sorption.

Main Results:

  • Successfully synthesized anionic SOFs, M2[Si(C16H10O4)1.5], with hexacoordinate silicon (SiO6 building units).
  • Frameworks formed 2D hexagonal layers with eclipsed stacking and stacking disorder.
  • Achieved permanent microporosity with high surface areas up to 1,276 m²/g.

Conclusions:

  • Demonstrated a new route to crystalline materials containing hexacoordinate silicon.
  • The synthesized SOFs exhibit zeolite-like characteristics, including negative charge and permanent porosity.
  • These findings open avenues for designing new porous materials with tunable silicon coordination.