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Modeling Diffusive Mixing in Antisolvent Crystallization.

Russell Miller1,2, Jan Sefcik1,2, Leo Lue1

  • 1Department of Chemical and Process Engineering, University of Strathclyde, James Weir Building, 75 Montrose Street, Glasgow G1 1XJ, U.K.

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Summary
This summary is machine-generated.

Supersaturation overshoots in antisolvent crystallization are modeling artifacts, not physical realities. A thermodynamically consistent diffusion model reveals that diffusion does not create these overshoots, offering new insights into nucleation.

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Area of Science:

  • Chemical Engineering
  • Physical Chemistry
  • Crystallization Science

Background:

  • Diffusion significantly influences concentration profiles during fluid mixing.
  • Antisolvent crystallization models often assume Fickian diffusion, predicting supersaturation overshoots.
  • These predicted overshoots are intuitively thought to cause uncontrolled nucleation.

Purpose of the Study:

  • To investigate the role of thermodynamically consistent diffusion in antisolvent crystallization.
  • To determine if supersaturation overshoots are physical phenomena or modeling artifacts.
  • To explore the potential for spinodal demixing during diffusive mixing.

Main Methods:

  • Applied a thermodynamically consistent diffusion model based on multicomponent Maxwell-Stefan formulation.
  • Examined diffusive mixing in a nonideal antisolvent crystallization system.
  • Analyzed concentration profiles and supersaturation at fluid interfaces.

Main Results:

  • Thermodynamically consistent diffusion does not predict significant supersaturation overshoots.
  • The previously predicted overshoots are identified as modeling artifacts.
  • Localized liquid-liquid spinodal demixing is predicted under specific conditions during mixing.

Conclusions:

  • Supersaturation overshoots are not expected in physical antisolvent crystallization systems.
  • Diffusive mixing, when modeled thermodynamically, behaves nonintuitively.
  • Intermittent spinodal demixing may explain variations in nucleation behavior with different antisolvents.