-NH₂ Driven Dynamic Reconstruction of Hydrogen-Bond Networks in 3-Aminopropanol-Water System Revealed by...

Area of Science:

• Physical Chemistry
• Chemical Physics
• Solution Chemistry

Background:

• Hydrogen-bond (HB) networks are crucial in determining the properties of liquid systems.
• Understanding the dynamic reorganization of these networks is essential for various chemical and biological processes.
• Amphiphilic molecules significantly influence solvent microenvironments and HB dynamics.

Purpose of the Study:

• To investigate the hydrogen-bond (HB) network dynamics and intermolecular interactions in 3-aminopropanol (3AP)-water mixtures.
• To elucidate the molecular-level mechanisms governing the reorganization of solvent structures in the presence of amphiphilic solutes.
• To provide insights into the competitive hydrogen bonding interactions in 3AP-water systems.

Main Methods:

• Spontaneous and stimulated Raman spectroscopy (SRS) for vibrational analysis.
• Two-dimensional correlation Raman spectroscopy (2D Raman-COS) for sequential response analysis.
• Density functional theory (DFT) calculations for cluster configurations and interaction elucidation.

Main Results:

• Nonlinear trends and critical transitions in vibrational modes (-OH, -NH2, -CH2) observed at specific 3AP concentrations.
• 2D Raman-COS indicated a sequential restructuring of the HB network, initiated by the -NH2 group.
• DFT calculations confirmed stable cluster configurations and the synergistic role of O-H:N/O hydrogen bonds.

Conclusions:

• The study reveals a three-stage solvation mechanism in 3AP-water mixtures.
• Molecular-level insights into the dynamic regulation of solvent microenvironments by amphiphilic molecules were provided.
• A new perspective on HB network reorganization in solution systems was offered.