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Synthesis and Characterization of Functionalized Metal-organic Frameworks
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A molecular shuttle that operates inside a metal-organic framework.

Kelong Zhu1, Christopher A O'Keefe1, V Nicholas Vukotic1

  • 1Department of Chemistry and Biochemistry, University of Windsor, Windsor, Ontario N9B 3P4, Canada.

Nature Chemistry
|May 21, 2015
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Area of Science:

  • Supramolecular Chemistry
  • Materials Science
  • Solid-State NMR Spectroscopy

Background:

  • Molecular shuttles are interlocked molecular assemblies with a movable macrocyclic ring.
  • Mechanically interlocked molecules (MIMs) mimic macroscopic machines and switches.
  • Previous studies focused on molecular shuttles in solution.

Purpose of the Study:

  • To organize and initiate the translational motion of a molecular shuttle within a solid-state material.
  • To demonstrate the operation of a molecular shuttle inside a crystalline metal-organic framework (MOF).

Main Methods:

  • Synthesis of a novel metal-organic framework (MOF), UWDM-4, incorporating a molecular shuttle linker.
  • Variable-temperature (1)H-(13)C cross-polarization/magic-angle spinning (CP/MAS) solid-state NMR.
  • (13)C 2D exchange correlation spectroscopy (EXSY) solid-state NMR on a (13)C-enriched sample at 21.1 T.

Main Results:

  • The metal-organic framework UWDM-4 was successfully prepared with a molecular shuttle linker.
  • Solid-state NMR experiments confirmed the translational motion of the macrocyclic ring.
  • The macrocyclic ring was observed to shuttle rapidly along the rigid axle within the MOF structure.

Conclusions:

  • The fundamental concept of molecular shuttle translational motion can be realized in solid-state crystalline materials.
  • Metal-organic frameworks provide a platform for organizing and operating molecular machines in the solid state.
  • This work opens possibilities for solid-state molecular devices and materials.