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Magnesium nitrate solutions contain solvent-shared ion pairs (SIPs) and contact ion pairs (CIPs). Their structures change with concentration, forming complex chains at higher concentrations, as revealed by spectroscopy and simulations.

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Area of Science:

  • Physical Chemistry
  • Solution Chemistry
  • Computational Chemistry

Background:

  • Understanding ion-pair formation in electrolyte solutions is crucial for various chemical processes.
  • The existence and structure of direct contact ion pairs (CIPs) in magnesium nitrate solutions remain an active area of research.

Purpose of the Study:

  • To investigate the relationship between concentration and microstructure in magnesium nitrate solutions.
  • To elucidate the detailed structure of ion pairs, including solvent-shared ion pairs (SIPs) and CIPs.
  • To explore the structural evolution of magnesium nitrate solutions with varying concentrations.

Main Methods:

  • Raman spectroscopy was employed to analyze the solution's composition and structure.
  • Molecular dynamics (MD) simulations provided insights into ion-pair dynamics and arrangements.
  • Density functional theory (DFT) calculations were used to determine the electronic structure and bonding of ion pairs.

Main Results:

  • In dilute solutions, SIPs and free hydrated ions were dominant. As concentration increased, SIPs transitioned to CIPs.
  • At WSR < 10, complex structures and CIPs predominated. Further increases in concentration led to a decrease in CIPs and an increase in complex structures.
  • SIPs and CIPs were primarily cationic triple ion clusters (two Mg²⁺ and one NO₃⁻). Nitrate ions predominantly acted as monodentate ligands in CIPs.

Conclusions:

  • The study reveals a concentration-dependent structural transformation in magnesium nitrate solutions, from simple ion pairs to complex chain structures.
  • MD simulations and DFT calculations offer a detailed understanding of the structural units and bonding within magnesium nitrate ion pairs.
  • The increasing structural complexity of magnesium nitrate solutions warrants further investigation.