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Self-stratification and phase separation in drying binary colloidal films

delete2025-02-01
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E
Ellard Hooiveld
L
Lisa Rijnders
B
Berend van der Meer
J
Jasper van der Gucht
J
Joris Sprakel
H
Hanne M. van der Kooij *
DOI:10.1016/j.jcis.2024.10.102delete
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Abstract

Abstract

En 中文
Hypothesis: Films that develop compositional heterogeneity during drying offer a promising approach for achieving tailored functionalities. These functionalities can be realized by strategically directing different components during the drying process. One approach to achieve this is through spontaneous size segregation of colloidal particles. Two variants thereof have previously been observed in binary suspensions: layer formation (self-stratification) due to kinetically driven concentration gradients, and micro-domain formation (phase separation) due to thermodynamic depletion interactions between the small and large species. Surprisingly, in the context of binary colloidal films, these phenomena have never been investigated concurrently during evaporation. Experiments: We show how we can achieve both self-stratification and domain formation in a single step. Using real-time 3D confocal fluorescence microscopy, we quantitatively unravel the effects of various parameters on the emergence of compositional heterogeneity. Findings: We reveal that beyond a certain size ratio, micro-phase separation becomes a prominent mechanism dictating the final morphology. The initial volume fraction minimally affects the final domain size but significantly impacts self-stratification. Reducing the evaporation rate increases the domain size while minimizing stratification. Finally, reducing the colloidal electrostatic interaction by a small increase in salt concentration enhances phase separation yet reverses stratification. These findings unveil a strategy for harnessing two distinct size segregation mechanisms in a single film, forming a foundation for customizable self-partitioning coatings.
Keywords:
Multi-component coatings
Binary colloidal films
Phase separation
Stratification
Dispersion drying
In-situ confocal imaging
Diffusiophoresis
Non-equilibrium thermodynamics
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Journal

Journal of Colloid and Interface Science cover
Journal of Colloid and Interface Science
IF:
9.7
Papers:
3.7W
Citations:
14.7W

Organization

W
Wageningen University & Research
Scholars:
2.9W
Papers: 2.8W
Citations: 55