skip to main content


Title: The effect of particle wettability on the stick-slip motion of the contact line
Contact line dynamics is crucial in determining the deposition patterns of evaporating colloidal droplets. Using high-speed interferometry, we directly observe the stick-slip motion of the contact line in situ and are able to resolve the instantaneous shape of the inkjet-printed, evaporating pico-liter drops containing nanoparticles of varying wettability. Integrated with post-mortem optical profilometry of the deposition patterns, the instantaneous particle volume fraction and hence the particle deposition rate can be determined. The results show that the stick-slip motion of the contact line is a strong function of the particle wettability. While the stick-slip motion is observed for nanoparticles that are less hydrophilic ( i.e. , particle contact angle θ ≈ 74° at the water–air interface), which results in a multiring deposition, a continuous receding of the contact line is observed for more hydrophilic nanoparticles ( i.e. , θ ≈ 34°), which leaves a single-ring pattern. A model is developed to predict the number of particles required to pin the contact line based on the force balance of the hydrodynamic drag, interparticle interactions, and surface tension acting on the particles near the contact line with varying particle wettability. A three-fold increase in the number of particles required for pinning is predicted when the particle wettability increases from the wetting angle of θ ≈ 74° to θ ≈ 34°. This finding explains why particles with greater wettability form a single-ring pattern and those with lower wettability form a multi-ring pattern. In addition, the particle deposition rate is found to depend on the particle wettability and vary with time.  more » « less
Award ID(s):
1705745
NSF-PAR ID:
10097282
Author(s) / Creator(s):
; ; ; ;
Date Published:
Journal Name:
Soft Matter
Volume:
14
Issue:
47
ISSN:
1744-683X
Page Range / eLocation ID:
9599 to 9608
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. The energetics of drop deposition are considered in the capillary-ballistic regime characterized by high Reynolds number and moderate Weber number. Experiments are performed impacting water/glycol drops onto substrates with varying wettability and contact-angle hysteresis. The impacting event is decomposed into three regimes: (i) pre-impact, (ii) inertial spreading and (iii) post contact-line (CL) pinning, conveniently framed using the theory of Dussan & Davis ( J. Fluid Mech. , vol. 173, 1986, pp. 115–130). During fast-time-scale inertial spreading, the only form of dissipation is CL dissipation ( $\mathcal {D}_{CL}$ ). High-speed imaging is used to resolve the stick-slip dynamics of the CL with $\mathcal {D}_{CL}$ measured directly from experiment using the $\Delta \alpha$ - $R$ cyclic diagram of Xia & Steen ( J. Fluid Mech. , vol. 841, 2018, pp. 767–783), representing the contact-angle deviation against the CL radius. Energy loss occurs on slip legs, and this observation is used to derive a closed-form expression for the kinetic K and interfacial $\mathcal{A}$ post-pinning energy $\{K+\mathcal {A}\}_p/\mathcal {A}_o$ independent of viscosity, only depending on the rest angle $\alpha _p$ , equilibrium angle $\bar {\alpha }$ and hysteresis $\Delta \alpha$ , which agrees well with experimental observation over a large range of parameters, and can be used to evaluate contact-line dissipation during inertial spreading. The post-pinning energy is found to be independent of the pre-impact energy, and it is broken into modal components with corresponding energy partitioning approximately constant for low-hysteresis surfaces with fixed pinning angle $\alpha _p$ . During slow-time-scale post-pinning, the liquid/gas ( $lg$ ) interface is found to vibrate with the frequencies and mode shapes predicted by Bostwick & Steen ( J. Fluid Mech. , vol. 760, 2014, pp. 5–38), irrespective of the pre-impact energy. Resonant mode decay rates are determined experimentally from fast Fourier transforms of the interface dynamics. 
    more » « less
  2. The evaporation of droplets on surfaces is a ubiquitous phenomenon essential in nature and industrial applications ranging from thermal management of electronics to self-assembly-based fabrication. In this study, water droplet evaporation on a thin quartz substrate is analyzed using an unsteady two-step arbitrary Lagrangian-Eulerian (ALE) moving mesh model, wherein the evaporation process is simulated during the constant contact radius (CCR) and contact angle (CCA) modes. The numerical model considers mass transfer in the gas domain, flow in the liquid and gas domains, and heat transfer in the solid, liquid, and gas domains. Besides, the model also accounts for interfacial force balance, including thermocapillary stresses, to obtain the instantaneous droplet shape. Experiments involving droplet evaporation on unheated quartz substrates agree with model predictions of contact radius, contact angle, and droplet volume. Model results indicating temperature and velocity distribution across an evaporating water droplet show that the lowest temperatures are at the liquid-gas interface, and a single vortex exists for the predominant duration of the droplet's lifetime. The temperature of the unheated substrate is also significantly reduced due to evaporative cooling. The interfacial evaporation flux distribution, which depends on heat transfer across the droplet and advection in the surrounding medium, shows the highest values near the three-phase contact line. In addition, the model also predicts evaporation dynamics when the substrate is heated and exposed to different advection conditions. Generally, higher evaporation rates result from higher substrate heating and advection rates. However, substrate heating and advection in the surrounding gas have minimal effects on the relative durations of CCR and CCA modes for a given receding contact angle. Specifically, in this case, a 40× increase in substrate heating rate or 7.5× increase in gas velocity can only change these relative durations by 3%. This study also highlights the importance of surface wettability, which affects evaporation dynamics for all the conditions explored by the numerical model. 
    more » « less
  3. Determination of the surface hydrophobicity or wettability of nanomaterials and nanoparticles (NPs) is often challenged by the heterogeneous properties of NPs that vary with particle size, shape, surface charge, aggregation states, and surface sorption or coating. This study first summarized inherent limitations of the water contact angle, octanol–water partition coefficient ( K ow ) and surface adsorption of probe molecules in probing nanomaterial hydrophobicity. Then, we demonstrated the principle of a scanning probe method based on atomic force microscopy (AFM) for the local surface hydrophobicity measurement. Specifically, we measured the adhesion forces between functionalized AFM tips and self-assembled monolayers (SAMs) to establish a linear relationship between the adhesion forces and water contact angles based on the continuum thermodynamic approach (CTA). This relationship was used to determine the local surface hydrophobicity of seven different NPs ( i.e. , TiO 2 , ZnO, SiO 2 , CuO, CeO 2 , α-Fe 2 O 3 , and Ag), which agreed well with bulk contact angles of these NPs. Some discrepancies were observed for Fe 2 O 3 , CeO 2 and SiO 2 NPs, probably because of surface hydration and roughness effects. Moreover, the solution pH and ionic strength had negligible effects on the adhesion forces between the AFM tip and MWCNTs or C 60 , indicating that the hydrophobicity of carbonaceous nanomaterials is not influenced by pH or ionic strength (IS). By contrast, natural organic matter (NOM) appreciably decreased the hydrophobicity of MWCNTs and C 60 due to surface coating of hydrophilic NOM. This scanning probe method has been proved to be reliable and robust toward the accurate measurement of the nanoscale hydrophobicity of individual NPs or nanomaterials in liquid environments. 
    more » « less
  4. Purpose: Fine API agglomeration and its mitigation via particle engineering, i.e., dry coating, remains underexplored. The purpose was to investigate agglomeration before and after dry coating of fine cohesive APIs and impact on powder processability, i.e., flowability (FFC), bulk density (BD), and dissolution of BCS Class II drugs. Method: Ibuprofen (three sizes), fenofibrate, and griseofulvin (5-20 µm), before and after dry coating with varying amounts of hydrophobic (R972P) or hydrophilic (A200) nano- silica, were assessed for agglomeration, FFC, BD, surface energy, wettability, and dissolution. The granular Bond number (Bog), a dimensionless parameter, evaluated through material-sparing particle-scale measures and particle-contact models, was used to express relative powder cohesion. Results: Significant powder processability improvements after dry coating were observed: FFC increased by multiple flow regimes, BD increased by 25-100 %, agglomerate ratio (AR) reduction by over an order of magnitude, and greatly enhanced API dissolution rate even with hydrophobic (R972P) silica coating. Scrutiny of particle-contact models revealed non-triviality in estimating API surface roughness, which was managed through the assessment of measured bulk properties. A power-law correlation was identified between AR and Bog and subsequently, between AR and FFC & bulk density; AR below 5 ensured improved processability and dissolution. Conclusion: Agglomeration, an overlooked material-sparing measure for powder cohesiveness, was a key indicator of powder processability and dissolution. The significant agglomerate reduction was possible via dry coating with either silica type at adequate surface area coverage. Reduced agglomeration after dry coating also countered the adverse impact of increased surface hydrophobicity on dissolution. 
    more » « less
  5. Abstract

    Massive studies concern the development of low‐carbon water and energy systems. Specifically, surfaces with special wettability to promote vapor‐to‐liquid condensation have been widely studied, but current solutions suffer from poor heat transfer performances due to inefficient droplet removal. In this study, the limit of condensation on a beetle‐inspired biphilic quasi‐liquid surface (QLS) in a steam environment is pushed, which provides a heat flux 100 times higher than that in atmospheric condensation. Unlike the beetle‐inspired surfaces that have sticky hydrophilic domains, the biphilic QLS consists of PEGylated and siloxane polymers as hydrophilic and hydrophobic quasi‐liquid patterns with the contact angle hysteresis of 3° and 1°, respectively. More importantly, each hydrophilic slippery pattern behaves like a slippery bridge that accelerates droplet coalescence and removal. As a result, the condensed droplets grow rapidly and shed off. It is demonstrated that the biphilic‐striped QLS shows a 60% higher water harvesting rate in atmospheric condensation and a 170% higher heat transfer coefficient in steam condensation than the conventional beetle‐inspired surface. This study provides a new paradigm to push the limit of condensation heat transfer at a high heat flux, which sheds light on the next‐generation surface design for water and energy sustainability.

     
    more » « less