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Microscopic structure of aqueous alkylamine mixtures: A computer simulation study.

Martina Požar1, Lena Friedrich2, Bernarda Lovrinčević1

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Aqueous amines form stable micro-heterogeneous structures due to nitrogen head groups stabilizing interfaces. This molecular arrangement generates scattering pre-peaks in x-ray scattering experiments.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Chemical Physics

Background:

  • Aqueous alkylamine mixtures exhibit pronounced x-ray scattering pre-peaks, an unexpected phenomenon compared to neat amines or aqueous alcohols.
  • The microscopic origins of these pre-peaks in water-rich solutions remain poorly understood.

Purpose of the Study:

  • To investigate the microscopic origins of x-ray scattering pre-peaks in aqueous alkylamine mixtures.
  • To elucidate the role of nitrogen head groups and hydrogen bonding in stabilizing micro-heterogeneity.

Main Methods:

  • Molecular dynamics simulations were performed for primary amines ranging from propylamine to octylamine.
  • Analysis focused on interfacial behavior, hydrogen bonding networks, and correlation functions.

Main Results:

  • Nitrogen head groups preferentially adsorb at the interfaces of water-rich domains, stabilizing both water and amine regions via hydrogen bonding.
  • This interfacial saturation prevents macroscopic phase separation until very high water concentrations.
  • The resulting disordered bilayer-like structures induce long-ranged domain oscillations, which manifest as the observed scattering pre-peaks.

Conclusions:

  • Aqueous amines serve as model systems demonstrating how stable micro-heterogeneity and supramolecular topology directly lead to scattering pre-peaks.
  • The findings provide a link between the behavior of molecular liquids and micro-emulsions.
  • The accuracy of simulations is sensitive to force field choices, with CHARMM-AA/SPC/E showing the best agreement with experimental data.