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Phase separation of binary mixtures induced by soft centrifugal fields

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2021

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Zemb, Thomas
Marčelja, Stjepan
Dufrêche, Jean-François
Kunz, Werner
Horinek, Dominik

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Physical Chemistry Chemical Physics. Royal Society of Chemistry (RSC). 2021, 23(14), pp. 8261-8272. ISSN 1463-9076. eISSN 1463-9084. Available under: doi: 10.1039/D0CP01527J

Zusammenfassung

We use the model system ethanol–dodecane to demonstrate that giant critical fluctuations induced by easily accessible weak centrifugal fields as low as 2000g can be observed above the miscibility gap of a binary liquid mixture. Moreover, several degrees above the phase transition, i.e. in the one-phase region, strong gradients of ethanol concentration occur upon centrifugation. In this case, the standard interpretation of sedimentation equilibrium in the analytical ultracentrifuge (AUC) yields an apparent molar mass of ethanol three orders of magnitude higher than the real value. Notably, these composition gradients have no influence on the distribution gradient of solutes such as dyes like Nile red. The thick opaque interphase formed upon centrifugation does not appear as the commonly observed sharp meniscus, but as a turbidity zone, similar to critical opalescence. This layer is a few millimeters thick and separates two fluids with low compositional gradients. All these effects can be qualitatively understood and explained using the Flory–Huggins solution model coupled to classical density functional theory (DFT). In this domain hetero-phase fluctuations can be triggered by gravity even far from the critical point. Taking into account Jean Perrin's approach to external fields in colloids, a self-consistent definition of the Flory effective volume and an explicit calculation of the total free energy per unit volume is possible.

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540 Chemie

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ISO 690ZEMB, Thomas, Rose ROSENBERG, Stjepan MARČELJA, Dirk HAFFKE, Jean-François DUFRÊCHE, Werner KUNZ, Dominik HORINEK, Helmut CÖLFEN, 2021. Phase separation of binary mixtures induced by soft centrifugal fields. In: Physical Chemistry Chemical Physics. Royal Society of Chemistry (RSC). 2021, 23(14), pp. 8261-8272. ISSN 1463-9076. eISSN 1463-9084. Available under: doi: 10.1039/D0CP01527J
BibTex
@article{Zemb2021Phase-54060,
  year={2021},
  doi={10.1039/D0CP01527J},
  title={Phase separation of binary mixtures induced by soft centrifugal fields},
  number={14},
  volume={23},
  issn={1463-9076},
  journal={Physical Chemistry Chemical Physics},
  pages={8261--8272},
  author={Zemb, Thomas and Rosenberg, Rose and Marčelja, Stjepan and Haffke, Dirk and Dufrêche, Jean-François and Kunz, Werner and Horinek, Dominik and Cölfen, Helmut}
}
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