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Heterogeneous nucleation from a supercooled ionic liquid on a carbon surface.

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Investigating crystal nucleation in ionic liquids revealed that a graphitic surface significantly lowers the energy barrier and speeds up the process compared to bulk nucleation. This finding is crucial for understanding and controlling crystallization in confined environments.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Computational Chemistry

Background:

  • Ionic liquids (ILs) are tunable solvents with unique properties.
  • Understanding crystallization in ILs is vital for their application.
  • Nucleation processes, especially in confined systems, are complex and challenging to study.

Purpose of the Study:

  • To investigate the nucleation of the ionic liquid [dmim+][Cl-] from its supercooled liquid phase.
  • To compare homogeneous nucleation in bulk with heterogeneous nucleation on a graphitic surface.
  • To determine the free energy barriers, critical nucleus size, and nucleation rates for both scenarios.

Main Methods:

  • Classical molecular dynamics simulations.
  • String method in collective variables.
  • Markovian milestoning with Voronoi tessellations.
  • Order parameters for molecular crystals.

Main Results:

  • Homogeneous nucleation has a free energy barrier of ~85 kcal/mol and a critical nucleus size of ~3.6 nm.
  • Heterogeneous nucleation on a graphitic surface reduces the barrier by 42% (~49 kcal/mol) and the nucleus size by 17% (~3.0 nm).
  • Heterogeneous nucleation rate is ~4.8 × 10^11 cm^-3 s^-1, an order of magnitude faster than homogeneous nucleation (~6.6 × 10^10 cm^-3 s^-1).

Conclusions:

  • Graphitic surfaces significantly promote the nucleation of [dmim+][Cl-] ionic liquid crystals.
  • The study provides quantitative insights into the effects of surfaces on crystallization kinetics.
  • Results align with experimental and simulation data for other nucleation systems, validating the methodology.