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Enhancement of Hydrate Stability through Substitutional Defects.

Megan E Fleming1, Jennifer A Swift1

  • 1Department of Chemistry, Georgetown University, 37th and O Streets NW, Washington, D.C. 20057-1227, United States.

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Defect engineering stabilizes cytosine monohydrate (CM) crystals. Doping CM with specific dyes enhances thermal stability, preventing conversion to the anhydrate form and altering dehydration properties.

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Area of Science:

  • Solid-state chemistry
  • Crystallography
  • Materials science

Background:

  • Cytosine monohydrate (CM) undergoes reversible interconversion with its anhydrate form under specific environmental conditions.
  • Controlling phase transitions in crystalline materials is crucial for their stability and application.

Purpose of the Study:

  • To investigate the potential of defect engineering in enhancing the thermal stability of cytosine monohydrate.
  • To explore the use of molecular dye dopants to create quantifiable defects and impede phase transitions.

Main Methods:

  • Screening of twelve molecular dyes as dopants for cytosine monohydrate.
  • Preparation and characterization of CM-dye phases using techniques to quantify inclusion levels and crystal structure.
  • Analysis of thermal stability, dehydration kinetics, thermal expansion, and product morphology of doped and undoped CM.

Main Results:

  • CM phases doped with Congo red (CR), Evans blue (EB), and Azocarmine G (AG) showed high dye inclusion (up to 1.1 wt %).
  • These doped phases exhibited increased thermal stability, requiring higher temperatures for dehydration with slower kinetics compared to pure CM.
  • Engineered defects reduced thermal expansion and altered the morphology of dehydration products.

Conclusions:

  • Targeted defect engineering via dye doping is an effective strategy to expand the thermal stability range of cytosine monohydrate.
  • The presence of substitutional defects impedes the cooperative molecular motions necessary for anhydrate formation.
  • This approach offers a method to control the solid-state transformations and properties of CM.