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Guest molecule-responsive functional calcium phosphonate frameworks for tuned proton conductivity.

Montse Bazaga-García1, Rosario M P Colodrero, Maria Papadaki

  • 1Departamento de Química Inorgánica, Universidad de Málaga , Campus Teatinos s/n, Málaga 29071, Spain.

Journal of the American Chemical Society
|March 20, 2014
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This study synthesized a novel hybrid material using calcium ions and a polyfunctional ligand, demonstrating its potential for proton conductivity. Modifying the material with ammonia significantly enhanced its conductivity, highlighting new pathways for proton transfer in hybrid materials.

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Area of Science:

  • Materials Science
  • Inorganic Chemistry
  • Crystallography

Background:

  • Open-framework hybrid materials offer tunable properties for various applications.
  • Proton conductivity in materials is crucial for energy technologies like fuel cells.
  • Understanding structure-property relationships is key to designing advanced functional materials.

Purpose of the Study:

  • To synthesize and characterize a novel open-framework hybrid material combining Ca(2+) ions and 5-(dihydroxyphosphoryl)isophthalic acid (PiPhtA).
  • To investigate the framework interconversions and proton conductivity of the synthesized material and its derivatives.
  • To explore the impact of guest molecules on the material's structural and conductive properties.

Main Methods:

  • Solvothermal synthesis and slow crystallization for material preparation.
  • Synchrotron powder X-ray diffraction and Rietveld refinement for structural analysis.
  • Elemental analysis, thermal analysis (DTA-TG), FT-IR spectroscopy, and conductivity measurements.

Main Results:

  • A novel hybrid material, Ca-PiPhtA-I, was synthesized, featuring water-filled 1D channels.
  • Partial dehydration (Ca-PiPhtA-II) and ammonia vapor exposure (Ca-PiPhtA-NH3) led to framework modifications.
  • Proton conductivity was observed, with Ca-PiPhtA-NH3 exhibiting the highest value (6.6 × 10(-3) S·cm(-1)) at 98% RH.
  • Activation energies indicate proton transfer via a Grothuss mechanism.

Conclusions:

  • The synthesized hybrid material exhibits framework flexibility and proton conductivity.
  • Modification with ammonia creates new proton transfer pathways, significantly enhancing conductivity.
  • Internal hydrogen-bonding networks are critical for determining the proton conductivity of these hybrid materials.