skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Modeling Solution Drying by Moving a Liquid-Vapor Interface: Method and Applications
A method of simulating the drying process of a soft matter solution with an implicit solvent model by moving the liquid-vapor interface is applied to various solution films and droplets. For a solution of a polymer and nanoparticles, we observe “polymer-on-top” stratification, similar to that found previously with an explicit solvent model. Furthermore, “polymer-on-top” is found even when the nanoparticle size is smaller than the radius of gyration of the polymer chains. For a suspension droplet of a bidisperse mixture of nanoparticles, we show that core-shell clusters of nanoparticles can be obtained via the “small-on-outside” stratification mechanism at fast evaporation rates. “Large-on-outside” stratification and uniform particle distribution are also observed when the evaporation rate is reduced. Polymeric particles with various morphologies, including Janus spheres, core-shell particles, and patchy particles, are produced from drying droplets of polymer solutions by combining fast evaporation with a controlled interaction between the polymers and the liquid-vapor interface. Our results validate the applicability of the moving interface method to a wide range of drying systems. The limitations of the method are pointed out and cautions are provided to potential practitioners on cases where the method might fail.  more » « less
Award ID(s):
1944887
PAR ID:
10357469
Author(s) / Creator(s):
; ; ;
Date Published:
Journal Name:
Polymers
Volume:
14
Issue:
19
ISSN:
2073-4360
Page Range / eLocation ID:
3996
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. In this paper, we present a mathematical model and numerical simulation for the evaporation and drying of a liquid droplet containing suspended solids, relevant to processes such as spray drying and spray pyrolysis in the food and pharmaceutical industries. The model comprises three stages: first is the evaporation of the liquid droplet consisting of solid particles, followed by the second stage starting with the formation of a porous crust around a wet-core region and, finally, the third stage with sensible heating of the dry particle. Using a finite difference method with a moving grid, we account for the moving interface between the crust and wet core. Our model incorporates spatial temperature variations and is validated against experimental data on colloidal silica droplet drying, showing good agreement. We examine model assumptions and analyze the impact of drying conditions on drying rate and final particle morphology. Along with the temperature and velocity of the drying gas, we also find that the shape of suspended solid particles inside the droplet and assuming continuum flow of vapor through the crust influence drying quality. Finally, we develop a regime map to predict whether the final particle will be solid or hollow based on operating conditions. 
    more » « less
  2. Microcapsules allow for the controlled containment, transport, and release of cargoes ranging from pharmaceuticals to fragrances. Given the interest from a variety of industries in microcapsules and other core–shell structures, a multitude of fabrication strategies exist. Here, we report on a method relying on a mixture of temperature-responsive microgel particles, poly( N -isopropylacrylamide) (pNIPAM), and a polymer which undergo fluid–fluid phase separation. At room temperature this mixture separates into colloid-rich (liquid) and colloid-poor (gas) fluids. By heating the sample above a critical temperature where the microgel particles shrink dramatically and develop a more deeply attractive interparticle potential, the droplets of the colloid-rich phase become gel-like. As the temperature is lowered back to room temperature, these droplets of gelled colloidal particles reliquefy and phase separation within the droplet occurs. This phase separation leads to colloid-poor droplets within the colloid-rich droplets surrounded by a continuous colloid-poor phase. The gas/liquid/gas all-aqueous double emulsion lasts only a few minutes before a majority of the inner droplets escape. However, the colloid-rich shell of the core–shell droplets can solidify with the addition of salt. That this method creates core–shell structures with a shell composed of stimuli-sensitive microgel colloidal particles using only aqueous components makes it attractive for encapsulating biological materials and making capsules that respond to changes in, for example, temperature, salt concentration, or pH. 
    more » « less
  3. Drop condensation and evaporation as a result of the gradient in vapor concentration are important in both engineering and natural systems. One of the interesting natural examples is transpiration on plant leaves. Most of the water in the inner space of the leaves escapes through stomata, whose rate depends on the surface topography and a difference in vapor concentrations inside and just outside of the leaves. Previous research on the vapor flux on various surfaces has focused on numerically solving the vapor diffusion equation or using scaling arguments based on a simple solution with a flat surface. In this present work, we present and discuss simple analytical solutions on various 2D surface shapes (e.g., semicylinder, semiellipse, hair). The method of solving the diffusion equation is to use the complex potential theory, which provides analytical solutions for vapor concentration and flux. We find that a high mass flux of vapor is formed near the top of the microstructures while a low mass flux is developed near the stomata at the leaf surface. Such a low vapor flux near the stomata may affect transpiration in two ways. First, condensed droplets on the stomata will not grow due to a low mass flux of vapor, which will not inhibit the gas exchange through the stomatal opening. Second, the low mass flux from the atmosphere will facilitate the release of highly concentrated vapor from the substomatal space. 
    more » « less
  4. null (Ed.)
    Solvent evaporation in unpinned droplets of colloidal suspensions leads to the formation of porous shells which buckle under the pressure differential imposed by drying. We investigate the role of aspect ratio of rod-shaped particles in suppressing such buckling instabilities. Longer, thinner rods pack into permeable shells with consequently lower Darcy's pressure and thus avoid buckling. 
    more » « less
  5. Preparation of thin films by dissolving polymers in a common solvent followed by evaporation of the solvent has become a routine processing procedure. However, modeling of thin film formation in an evaporating solvent has been challenging due to a need to simulate processes at multiple length and time scales. In this work, we present a methodology based on the principles of linear non-equilibrium thermodynamics, which allows systematic study of various effects such as the changes in the solvent properties due to phase transformation from liquid to vapor and polymer thermodynamics resulting from such solvent transformations. The methodology allows for the derivation of evaporative flux and boundary conditions near each surface for simulations of systems close to the equilibrium. We apply it to study thin film microstructural evolution in phase segregating polymer blends dissolved in a common volatile solvent and deposited on a planar substrate. Effects of the evaporation rates, interactions of the polymers with the underlying substrate and concentration dependent mobilities on the kinetics of thin film formation are studied. 
    more » « less