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Classical density functional theory for associating fluids in orienting external fields.

Bennett D Marshall1, Walter G Chapman1, Margarida M Telo da Gama2

  • 1Department of Chemical and Biomolecular Engineering, Rice University, 6100 South Main Street, Houston, Texas 77005, USA.

Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics
|February 4, 2014
PubMed
Summary
This summary is machine-generated.

We developed a new density functional theory (DFT) for associating fluids. An orienting field enhances molecular association by reducing entropy, while association boosts molecular ordering in the field.

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Area of Science:

  • Statistical Mechanics
  • Physical Chemistry
  • Soft Matter Physics

Background:

  • Understanding molecular interactions in fluids is crucial for chemical processes.
  • Associating fluids exhibit complex behavior due to directional bonding.
  • External fields can influence fluid microstructure and properties.

Purpose of the Study:

  • To develop a classical density functional theory (DFT) for two-site associating fluids.
  • To investigate the interplay between orientational ordering and molecular association under external fields.
  • To quantify the effects of orienting fields on association and vice versa.

Main Methods:

  • Utilized Wertheim's thermodynamic perturbation theory to derive the Helmholtz free-energy functional.
  • Employed density functional theory (DFT) in the canonical ensemble to determine orientational distribution functions.
  • Simulated two-site associating fluids subjected to spatially homogeneous external fields.

Main Results:

  • An orienting field significantly enhances molecular association by inducing molecular order.
  • This ordering reduces the entropic penalty associated with the formation of molecular bonds.
  • Conversely, molecular association was found to increase orientational order within the applied field.

Conclusions:

  • The developed DFT provides a framework for studying associating fluids in external fields.
  • External fields and molecular association exhibit a synergistic relationship, mutually enhancing ordering and bonding.
  • Findings offer insights into controlling fluid behavior through external stimuli.