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Title: Stratification in Drying Films Containing Bidisperse Mixtures of Nanoparticles

Abstract

Large scale molecular dynamics simulations for bidisperse nanoparticle suspensions with an explicit solvent are used to investigate the effects of evaporation rates and volume fractions on the nanoparticle distribution during drying. Our results show that “small-on-top” stratification can occur when Pe sΦ s ≳ c with c ~1, where Pe s is the Péclet number and Φ s is the volume fraction of the smaller particles. This threshold of Pe sΦ s for “small-on-top” is larger by a factor of ~α 2 than the prediction of the model treating solvent as an implicit viscous background, where α is the size ratio between the large and small particles. Our simulations further show that when the evaporation rate of the solvent is reduced, the “small-on-top” stratification can be enhanced, which is not predicted by existing theories. This unexpected behavior is explained with thermophoresis associated with a positive gradient of solvent density caused by evaporative cooling at the liquid/vapor interface. For ultrafast evaporation the gradient is large and drives the nanoparticles toward the liquid/vapor interface. This phoretic effect is stronger for larger nanoparticles, and consequently the “small-on-top” stratification becomes more distinct when the evaporation rate is slower (but not too slow such thatmore » a uniform distribution of nanoparticles in the drying film is produced), as thermophoresis that favors larger particles on the top is mitigated. A similar effect can lead to “large-on-top” stratification for Pe sΦ s above the threshold when Pe s is large but Φ s is small. Lastly, our results reveal the importance of including the solvent explicitly when modeling evaporation-induced particle separation and organization and point to the important role of density gradients brought about by ultrafast evaporation.« less

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1457520
Report Number(s):
SAND-2018-6692J
Journal ID: ISSN 0743-7463; 664619
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Langmuir
Additional Journal Information:
Journal Volume: 34; Journal Issue: 24; Journal ID: ISSN 0743-7463
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Evaporation; Drying; Nanoparticle; Suspension; Stratification; Péclet Number; Molecular Dynamics

Citation Formats

Tang, Yanfei, Grest, Gary S., and Cheng, Shengfeng. Stratification in Drying Films Containing Bidisperse Mixtures of Nanoparticles. United States: N. p., 2018. Web. doi:10.1021/acs.langmuir.8b01334.
Tang, Yanfei, Grest, Gary S., & Cheng, Shengfeng. Stratification in Drying Films Containing Bidisperse Mixtures of Nanoparticles. United States. doi:10.1021/acs.langmuir.8b01334.
Tang, Yanfei, Grest, Gary S., and Cheng, Shengfeng. Wed . "Stratification in Drying Films Containing Bidisperse Mixtures of Nanoparticles". United States. doi:10.1021/acs.langmuir.8b01334.
@article{osti_1457520,
title = {Stratification in Drying Films Containing Bidisperse Mixtures of Nanoparticles},
author = {Tang, Yanfei and Grest, Gary S. and Cheng, Shengfeng},
abstractNote = {Large scale molecular dynamics simulations for bidisperse nanoparticle suspensions with an explicit solvent are used to investigate the effects of evaporation rates and volume fractions on the nanoparticle distribution during drying. Our results show that “small-on-top” stratification can occur when PesΦs ≳ c with c ~1, where Pes is the Péclet number and Φs is the volume fraction of the smaller particles. This threshold of PesΦs for “small-on-top” is larger by a factor of ~α2 than the prediction of the model treating solvent as an implicit viscous background, where α is the size ratio between the large and small particles. Our simulations further show that when the evaporation rate of the solvent is reduced, the “small-on-top” stratification can be enhanced, which is not predicted by existing theories. This unexpected behavior is explained with thermophoresis associated with a positive gradient of solvent density caused by evaporative cooling at the liquid/vapor interface. For ultrafast evaporation the gradient is large and drives the nanoparticles toward the liquid/vapor interface. This phoretic effect is stronger for larger nanoparticles, and consequently the “small-on-top” stratification becomes more distinct when the evaporation rate is slower (but not too slow such that a uniform distribution of nanoparticles in the drying film is produced), as thermophoresis that favors larger particles on the top is mitigated. A similar effect can lead to “large-on-top” stratification for PesΦs above the threshold when Pes is large but Φs is small. Lastly, our results reveal the importance of including the solvent explicitly when modeling evaporation-induced particle separation and organization and point to the important role of density gradients brought about by ultrafast evaporation.},
doi = {10.1021/acs.langmuir.8b01334},
journal = {Langmuir},
number = 24,
volume = 34,
place = {United States},
year = {Wed May 23 00:00:00 EDT 2018},
month = {Wed May 23 00:00:00 EDT 2018}
}

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