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Negative Thermal Expansion of Undulating Coordination Layers through Interlayer Interaction.

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This study reveals negative thermal expansion (NTE) in two-dimensional coordination polymers. Strong interlayer interactions cause layers to expand upon cooling, a rare phenomenon in solid-state materials.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Crystallography

Background:

  • Negative thermal expansion (NTE) is a rare phenomenon in solid-state materials, crucial for applications requiring dimensional stability.
  • Two-dimensional coordination polymers offer unique structural motifs for exploring exotic thermal expansion behaviors.

Purpose of the Study:

  • To conduct a meta-analysis of anisotropic thermal expansion in [M(salen)]2[M'(CN)4(solvent)] coordination polymers.
  • To investigate the NTE mechanism in undulating coordination layers and its dependence on interlayer interactions.

Main Methods:

  • Meta-analysis of thermal expansion data for fifteen 2D coordination polymers.
  • Synthesis and characterization of a new compound, [Fe(salen)]2[MnN(CN)4(MeCN)].
  • Analysis of anisotropic thermal expansion behavior and layer deformation mechanisms.

Main Results:

  • Demonstrated unusual NTE in undulating coordination layers due to strong interlayer interactions.
  • Observed a large NTE coefficient (αlayer-volume = -27 × 10-6 K-1) in [Mn(salen)]2[ReN(CN)4] powder.
  • Showed that enhancing intralayer interactions switches behavior to positive thermal expansion (+92 × 10-6 K-1).

Conclusions:

  • Strong interlayer interactions are key to achieving NTE in these 2D coordination polymers.
  • Anisotropic layer transformation drives the NTE phenomenon despite increasing layer thickness.
  • Chemical modification offers a route to tune thermal expansion from negative to positive.