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: Controlling morphology in electrosprayed methylcellulose nanowires via nanoparticle addition: coarse-grained modeling and experiments
Electrospray deposition (ESD) has shown great promise for manufacturing micro- and nanostructured coatings at scale on versatile substrates with complex geometries. ESD exhibits a broad spectrum of morphologies depending upon the properties of spray fluids. Among them are nanowire forests or foams obtained via the in-air gelation of electrospray droplets formed from methylcellulose (MC) solutions. In this study, we explored MC ESD loaded with nanoparticles of various shapes and uncovered the effects of particle fillers on morphology evolution using coarse-grained simulations and physical experiments. Utilizing electrostatic dissipative particle dynamics, we modeled the electrohydrodynamic deformation of particle-laden MC droplets undergoing in-flight evaporation. The simulations quantitatively predict the suppression of droplet deformation as the size or concentration of spherical nanoparticles increases. While small particles can be readily encapsulated into the nanowire body, large particles can arrest nanowire formation. The model was extended to nanoparticles with complex topologies, showing MC nanowires emerging from particle edges and vertices due to curvature-enhanced electric stress. In all cases, strong agreements were found between simulation and experimental results. These results demonstrate the efficacy of the coarse-grained model in predicting the morphology evolution of electrosprayed droplets and lay the groundwork for employing MC nanowires for developing nanostructured composites.  more » « less
Award ID(s):
1939362 1911518
PAR ID:
10416997
Author(s) / Creator(s):
; ; ; ; ;
Date Published:
Journal Name:
Nanoscale
Volume:
14
Issue:
48
ISSN:
2040-3364
Page Range / eLocation ID:
17985 to 17994
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Electrospray deposition (ESD) uses strong electric fields applied to solutions and dispersions exiting a capillary to produce charged monodisperse droplets driven toward grounded targets. Self‐limiting electrospray deposition (SLED) is a phenomenon in which highly directed, uniform, and even 3D coatings can be achieved by trapping charge in the deposited film, redirecting the field lines to uncoated regions of the target. However, when inorganic particles are added to SLED sprays, the buildup of charge required to repel incoming material is disrupted as particle loading increases. Due to its fibril gelling behavior, methylcellulose (MC) SLED can form nanowire morphologies. These wires, when used as a binder, can separate particles and prevent percolation. In this work, a variety of conductive and insulating particles are explored using patterned and un‐patterned substrates. This exploration allows us to maximally load particles for high‐concentration and highly controlled self‐limiting functional sprays. This is demonstrated using Ti3C2Tx MXene to functionalize an interdigitated electrode for use as a supercapacitor. 
    more » « less
  2. Recovery plays distinct roles in nanostructured and coarse-grained metallic materials. While static and dynamic recovery usually soften work-hardened, coarse-grained materials, static recovery has been shown to strengthen nanostructured metals. This study extends this understanding by demonstrating that dynamic recovery can also strengthen nanostructured metals under deformation. Tensile, creep, and plane strain compression tests on nanostructured aluminum reveal a trend of increasing strain-hardening with decreasing strain rate and increasing temperature. Molecular dynamics simulations further indicate that sudden strain rate reductions lead to an initial drop in flow stress, followed by strain hardening. These findings suggest that dynamic recovery could serve as an effective strengthening mechanism for nanostructured metals, offering improvements in uniform elongation. 
    more » « less
  3. We address the challenge of representativity and dynamical consistency when un- bonded fine-grained particles are collected together into coarse-grained particles. We implement a hybrid procedure for identifying and tracking the underlying fine-grained particles—e.g., atoms or molecules—by exchanging them between the coarse-grained particles periodically at a characteristic time. The exchange involves a back-mapping of the coarse-grained particles into fine-grained particles, and a subsequent reassign- ment to coarse-grained particles conserving total mass and momentum. We find that an appropriate choice of the characteristic exchange time can lead to the correct effec- tive diffusion rate of the fine-grained particles when simulated in hybrid coarse-grained dynamics. In the compressed (supercritical) fluid regime, without the exchange term, fine-grained particles remain associated to a given coarse-grained particle, leading to substantially lower diffusion rates than seen in all-atom molecular dynamics of the fine- grained particles. Thus, this work confirms the need for addressing the representativity of fine-grained particles within coarse-grained particles, and offers a simple exchange mechanism so as to retain dynamical consistency between the fine- and coarse- grained scales. 
    more » « less
  4. null (Ed.)
    Gallium oxide (Ga 2 O 3 ) and its most stable modification, monoclinic β-Ga 2 O 3 , is emerging as a primary material for power electronic devices, gas sensors and optical devices due to a high breakdown voltage, large bandgap, and optical transparency combined with electrical conductivity. Growth of β-Ga 2 O 3 is challenging and most methods require very high temperatures. Nanowires of β-Ga 2 O 3 have been investigated extensively as they might be advantageous for devices such as nanowire field effect transistors, and gas sensors benefiting from a large surface to volume ratio, among others. Here, we report a synthesis approach using a sulfide precursor (Ga 2 S 3 ), which requires relatively low substrate temperatures and short growth times to produce high-quality single crystalline β-Ga 2 O 3 nanowires in high yields. Even though Au- or Ag-rich nanoparticles are invariably observed at the nanowire tips, they merely serve as nucleation seeds while the nanowire growth proceeds via supply and local oxidation of gallium at the substrate interface. Absorption and cathodoluminescence spectroscopy on individual nanowires confirms a wide bandgap of 4.63 eV and strong luminescence with a maximum ∼2.7 eV. Determining the growth process, morphology, composition and optoelectronic properties on the single nanowire level is key to further application of the β-Ga 2 O 3 nanowires in electronic devices. 
    more » « less
  5. Marine biofouling is a complex and dynamic process that significantly increases the carbon emissions from the maritime industry by increasing drag losses. However, there are no existing non‐toxic marine paints that can achieve both effective fouling reduction and efficient fouling release. Inspired by antifouling strategies in nature, herein, a superoleophobic zwitterionic nanowire coating with a nanostructured hydration layer is introduced, which exhibits simultaneous fouling reduction and release performance. The zwitterionic nanowires demonstrate >25% improvement in fouling reduction compared to state‐of‐the‐art antifouling nanostructures, and four times higher fouling‐release compared to conventional zwitterionic coatings. Fouling release is successfully achieved under a wall shear force that is four orders of magnitude lower than regular water jet cleaning. The mechanism of this simultaneous fouling reduction and release behavior is explored, and it is found that a combination of 1) a mechanical biocidal effect from the nanowire geometry, and 2) low interfacial adhesion resulting from the nanostructured hydration layer, are the major contributing factors. These findings provide insights into the design of nanostructured coatings with simultaneous fouling reduction and release. The newly established synthesis procedure for the zwitterionic nanowires opens new pathways for implementation as antifouling coatings in the maritime industry and biomedical devices. 
    more » « less