Surface Nanostructures Promote Droplet Splash on Hot Substrates.

Splash, one of the most visually apparent droplet dynamics, can manifest on any surface above a certain impact velocity, regardless of surface wettability. Previous studies demonstrate that elevating the substrate temperature can suppress droplet splash, which is unfavorable for many practical applications, such as spray cooling and combustion. Here, we report that the suppression effect of substrate temperature on splash is nullified by utilizing surfaces with nanostructures. By manipulating air evacuation time through surface nanostructures, we have identified a pathway for precise control over the splash threshold and the ability to tailor the dependence of the splash onset on surface temperature. We further propose a theoretical criterion to determine different splash regimes by considering the competition between air evacuation and the development of flow instabilities. Our findings underscore the crucial role of nanostructures in splash dynamics, offering valuable insights for the control of splash in various industrial scenarios.

Effect of surface viscoelasticity on top jet drops produced by bursting bubbles.

Jet drops resulting from bubble bursting at a liquid surface play a key role in various mass transfer processes across the interface, including sea spray aerosol generation and pathogen transmission. However, the impact of structurally compound interfaces, characterized by complex surface rheology introduced by surface-active contaminants, on the jet drop ejection still remains unclear. Here, we experimentally investigate the influence of surface viscoelasticity on the size and velocity of the top jet drops from surface bubble bursting, examining both pure protein and mixed protein-surfactant solutions. We document that for bubble bursting at a pure-protein-laden surface where surface elasticity dominates, the increase in Ec, i.e. the interfacial elastocapillary number as the ratio between the effects of interfacial elasticity and capillarity, efficiently increases the radius and decreases the velocity of the top jet drop, ultimately inhibiting the jet drop ejection. On the other hand, considering the mixed protein-surfactant solution, we show that the top jet drop radius and velocity exhibit a different variation trend with Ec, which is attributed to the additional dissipation on the capillary waves as well as the retardation and resistance on the converging flow for jet formation from surface viscoelasticity. Our work may advance the understanding of bubble bursting dynamics at contaminated liquid surfaces and shed light on the potential influence of surface viscoelasticity on the generation of bubble bursting aerosols.

Secondary Bubble Entrainment via Primary Bubble Bursting at a Viscoelastic Surface.

Bubble bursting at liquid surfaces is ubiquitous and plays a key role for the mass transfer across interfaces, impacting global climate and human health. Here, we document an unexpected phenomenon that when a bubble bursts at a viscoelastic surface of a bovine serum albumin solution, a secondary (daughter) bubble is entrapped with no subsequent jet drop ejection, contrary to the counterpart experimentally observed at a Newtonian surface. We show that the strong surface dilatational elastic stress from the viscoelastic surface retards the cavity collapse and efficiently damps out the precursor waves, thus facilitating the dominant wave focusing above the cavity nadir. The onset of daughter bubble entrainment is well predicted by an interfacial elastocapillary number comparing the effects of surface dilatational elasticity and surface tension. Our Letter highlights the important role of surface rheology on free surface flows and may find important implications in bubble dynamics with a contaminated interface exhibiting complex surface rheology.

Water-to-Air Transfer of Nano/Microsized Particulates: Enrichment Effect in Bubble Bursting Jet Drops.

Bubbles dispersed in liquids are widely present in many natural and industrial processes and play a key role in mediating mass transfer during their lifetime from formation to rising to bursting. In particular, nano/microsized particulates and organisms present in the bulk water can be highly enriched in the jet drops ejected during bubble bursting, impacting global climate and public health. However, the detailed mechanism of this enrichment remains obscure with the enrichment factor being difficult to predict. Here, we experimentally investigate the enrichment of nano/microsized particles in bubble bursting jet drops and highlight the underlying hydrodynamic mechanism, combining the effects of bubble scavenge and bursting on the transport of particles. Scaling laws for the enrichment factor are subsequently proposed that describe both our and prior experimental results reasonably well. Our study may provide new insights for water-to-air transfer of bulk particulates such as microbes related to bubble bursting.

Asymmetric Bubble Formation at Rectangular Orifices.

Bubble formation in liquids is frequently observed in nature and applied in various industrial processes. These include pool and flow boiling for thermal management systems, where bubbles may form asymmetrically at narrow slits and in convective flows. While previous studies have focused on symmetric bubble formation at circular orifices, the dynamics of asymmetric bubble formation remains poorly understood. Here, we experimentally investigate bubble formation at rectangular orifices and examine the effects of the orifice size and aspect ratio and the gas flow rate on the bubble size. The asymmetric bubble shape evolution at the rectangular orifice is analyzed, and we find that the size of the bubble neck is controlled either by the orifice size or by the capillary length. Based on these findings, we develop a static force balance model to predict the bubble size in the quasi-static regime, where the roles of Bond number and aspect ratio are identified. The bubble size evolution in the dynamic regime is further understood by introducing a Weber number that evaluates the effect of the virtual mass force induced by gas flow. Our study provides physical understanding of the dynamics of asymmetric bubble formation and guidance to predict the bubble size at asymmetric orifices.

Limit for Small Spheres To Float by Dynamic Analysis.

Small spheres released above the liquid surface experience a dynamic process to ultimately float or sink, and thus, their behaviors should be considered by dynamic analysis instead of static equilibrium. This study numerically investigates the motion of small spheres after contacting the liquid surface with zero velocity, and the flotation condition is proposed based on the analyses of acting forces and the sphere's motion. Whether the small spheres float is determined by the density ratio, Bond number, and contact angle. A critical contact angle exists, below which the flotation of small spheres is impossible. The decrease in Bond number and increase in hydrophobicity enlarge the limit density ratio for small spheres to float, while exerting little effect on large spheres. The theoretical formulas of the limit density ratio are obtained based on energy balance and agree well with numerical results. The limit density ratio predicted in consideration of a dynamic process is far less than the maximum density ratio predicted by static equilibrium.

Spreading dynamics of microdroplets on nanostructured surfaces.

HYPOTHESIS: Droplet spreading governs various daily phenomena and industrial processes. Insights about microdroplet spreading are limited due to experimental difficulties arising from microdroplet manipulation and substrate wettability control. For droplet sizes approaching the capillary length scale, the gravitational force plays an important role in spreading. In contrast, capillary and viscous forces dominate as the droplet size reduces to smaller length scales. We hypothesize that the dynamic spreading behavior of microdroplets whose radius is far lower than the capillary length differs substantially from established and well understood dynamics. EXPERIMENTS: To systematically investigate the spreading dynamics of microdroplets, we develop contact-initiated wetting techniques combined with structuring-independent wettability control to achieve microdroplet (<500 µm) spreading on arbitrary surfaces while eliminating parasitic pinning effects (pining force âˆ¼ 0) and initial impact momentum effects (Weber number âˆ¼ 0). FINDINGS: Our experiments reveal that the capillary-driven initial spreading of microdroplets is shorter, with significantly reduced oscillation dampening, when compared to millimeter-scale droplets. Furthermore, spreading along with capillary wave propagation results in coupling between the spreading velocity and dynamic contact angle at the contact line. These findings, along with our proposed microdroplet manipulation platform, may find application in microscale heat transfer, advanced manufacturing, and aerosol transmission studies.

Liquid metal droplets bouncing higher on thicker water layer.

Liquid metal (LM) has gained increasing attention for a wide range of applications, such as flexible electronics, soft robots, and chip cooling devices, owing to its low melting temperature, good flexibility, and high electrical and thermal conductivity. In ambient conditions, LM is susceptible to the coverage of a thin oxide layer, resulting in unwanted adhesion with underlying substrates that undercuts its originally high mobility. Here, we discover an unusual phenomenon characterized by the complete rebound of LM droplets from the water layer with negligible adhesion. More counterintuitively, the restitution coefficient, defined as the ratio between the droplet velocities after and before impact, increases with water layer thickness. We reveal that the complete rebound of LM droplets originates from the trapping of a thinly low-viscosity water lubrication film that prevents droplet-solid contact with low viscous dissipation, and the restitution coefficient is modulated by the negative capillary pressure in the lubrication film as a result of the spontaneous spreading of water on the LM droplet. Our findings advance the fundamental understanding of complex fluids' droplet dynamics and provide insights for fluid control.

Mechanism and performance relevance of nanomorphogenesis in polyamide films revealed by quantitative 3D imaging and machine learning.

Biological morphogenesis has inspired many efficient strategies to diversify material structure and functionality using a fixed set of components. However, implementation of morphogenesis concepts to design soft nanomaterials is underexplored. Here, we study nanomorphogenesis in the form of the three-dimensional (3D) crumpling of polyamide membranes used for commercial molecular separation, through an unprecedented integration of electron tomography, reaction-diffusion theory, machine learning (ML), and liquid-phase atomic force microscopy. 3D tomograms show that the spatial arrangement of crumples scales with monomer concentrations in a form quantitatively consistent with a Turing instability. Membrane microenvironments quantified from the nanomorphologies of crumples are combined with the Spiegler-Kedem model to accurately predict methanol permeance. ML classifies vastly heterogeneous crumples into just four morphology groups, exhibiting distinct mechanical properties. Our work forges quantitative links between synthesis and performance in polymer thin films, which can be applicable to diverse soft nanomaterials.

Particulate-Droplet Coalescence and Self-Transport on Superhydrophobic Surfaces.

Particulate transport from surfaces governs a variety of phenomena including fungal spore dispersal, bioaerosol transmission, and self-cleaning. Here, we report a previously unidentified mechanism governing passive particulate removal from superhydrophobic surfaces, where a particle coalescing with a water droplet (∼10 to ∼100 µm) spontaneously launches. Compared to previously discovered coalescence-induced binary droplet jumping, the reported mechanism represents a more general capillary-inertial dominated transport mode coupled with particle/droplet properties and is typically mediated by rotation in addition to translation. Through wetting and momentum analyses, we show that transport physics depends on particle/droplet density, size, and wettability. The observed mechanism presents a simple and passive pathway to achieve self-cleaning on both artificial as well as biological materials as confirmed here with experiments conducted on butterfly wings, cicada wings, and clover leaves. Our findings provide insights into particle-droplet interaction and spontaneous particulate transport, which may facilitate the development of functional surfaces for medical, optical, thermal, and energy applications.

Compound jetting from bubble bursting at an air-oil-water interface.

Bursting of bubbles at a liquid surface is ubiquitous in a wide range of physical, biological, and geological phenomena, as a key source of aerosol droplets for mass transport across the interface. However, how a structurally complex interface, widely present in nature, mediates the bursting process remains largely unknown. Here, we document the bubble-bursting jet dynamics at an oil-covered aqueous surface, which typifies the sea surface microlayer as well as an oil spill on the ocean. The jet tip radius and velocity are altered with even a thin oil layer, and oily aerosol droplets are produced. We provide evidence that the coupling of oil spreading and cavity collapse dynamics results in a multi-phase jet and the follow-up droplet size change. The oil spreading influences the effective viscous damping, and scaling laws are proposed to quantify the jetting dynamics. Our study not only advances the fundamental understanding of bubble bursting dynamics, but also may shed light on the airborne transmission of organic matters in nature related to aerosol production.

A Magnetically Actuated Superhydrophobic Ratchet Surface for Droplet Manipulation.

A water droplet dispensed on a superhydrophobic ratchet surface is formed into an asymmetric shape, which creates a Laplace pressure gradient due to the contact angle difference between two sides. This work presents a magnetically actuated superhydrophobic ratchet surface composed of nanostructured black silicon strips on elastomer ridges. Uniformly magnetized NdFeB layers sputtered under the black silicon strips enable an external magnetic field to tilt the black silicon strips and form a superhydrophobic ratchet surface. Due to the dynamically controllable Laplace pressure gradient, a water droplet on the reported ratchet surface experiences different forces on two sides, which are explored in this work. Here, the detailed fabrication procedure and the related magnetomechanical model are provided. In addition, the resultant asymmetric spreading of a water droplet is studied. Finally, droplet impact characteristics are investigated in three different behaviors of deposition, rebound, and penetration depending on the impact speed. The findings in this work are exploitable for further droplet manipulation studies based on a dynamically controllable superhydrophobic ratchet surface.

Dynamic flotation conditions for elongated cylinders on liquid surfaces.

HYPOTHESIS: Although the static flotation of elongated cylinders is well understood, their flotation behavior under dynamic conditions after contacting a liquid surface, such as in situations experienced by water-walking insects, still need to be revealed. METHODOLOGY: The motion of elongated horizontal cylinders after zero-velocity contact with a liquid surface is considered, and the motion equation of the cylinder is established and solved to obtain the dynamic flotation conditions. FINDINGS: The limiting density ratios for the dynamic flotation of elongated cylinders with different Bond numbers and contact angles are determined. The results show that although increasing the hydrophobicity promotes floatability of the elongated cylinders, there is little effect for contact angles >120°. Based on the energy balance, an asymptotic formula for the limiting density ratio is proposed, which agrees well with the theoretical results. Unlike small spheres, all elongated cylinders with contact angles >0° are observed to exhibit floatability after contacting a liquid surface. In addition, we found that elongated hydrophilic cylinders exhibit better floatability compared to small hydrophilic spheres with the same contact angle and Bond number, which assists small insects float and survive in various water environments.

Structure-controlled Co-Al layered double hydroxides/reduced graphene oxide nanomaterials based on solid-phase exfoliation technique for supercapacitors.

High-efficient nanosheets exfoliation and ordered controlled stacking are in urgent need of work for electrochemistry application. Here, we have developed a high-efficient and environmentally-friendly solid-phase method for the exfoliation of Co-Al layered double hydroxide (Co-Al LDH) and graphene oxide (GO). Meanwhile, we found that there is a dynamic structure evolution in the self-assembly process between Co-Al LDH-NS and GO-NS and new theoretical structure models were proposed. With the reduction treatment, the electrochemical test results show that Co-Al LDH/rGO-3 with ideal tiling structure has better electrochemical performance, which provides a specific capacitance of 1492 F g-1 at 1 A g-1 and remains the capacitance retention at approximately 94.3% after 5000 cycles. Moreover, an energy density of 44.6 Wh kg-1 is obtained at a power density of 799.6 W kg-1. The proposed method and the structure-relationship are practically applicable for other 2D materials in the asymmetric supercapacitors.

Controlled Self-Assembled NiFe Layered Double Hydroxides/Reduced Graphene Oxide Nanohybrids Based on the Solid-Phase Exfoliation Strategy as an Excellent Electrocatalyst for the Oxygen Evolution Reaction.

Layered double hydroxides (LDHs), as an effective oxygen evolution reaction (OER) electrocatalyst, face many challenges in practical applications. The main obstacle is that bulk materials limit the exposure of active sites. At the same time, the poor conductivity of LDHs is also an important factor. Exfoliation is one of the most direct and effective strategies to increase the electrocatalytic properties of LDHs, leading to exposure of many active sites. However, developing an efficient exfoliation strategy to exfoliate LDHs into stable monolayer nanosheets is still challenging. Therefore, we report a new and efficient solid-phase exfoliation strategy to exfoliate NiFe LDH and graphene oxide (GO) into monolayer nanosheets and the exfoliating ratios of NiFe LDH and GO can reach up to 10 and 5 wt %, respectively. Based on the solid-phase exfoliation strategy, we accidentally discovered that there is a dynamic evolution process between NiFe-LDH nanosheets (NiFe-LDH-NS) and GO nanosheets (GO-NS) to assemble new NiFe-LDH/GO nanohybrids, i.e., NiFe-LDH-NS could be horizontal bespreading on GO-NS or well-organized standing on GO-NS, or both simultaneously. The electrocatalytic OER property test results show that NiFe-LDH/RGO-3 (NFRG-3) nanohybrids obtained by the reduction treatment of NiFe-LDH/GO-3 (NFGO-3) nanohybrids, in which NiFe-LDH-NS are well-organized standing on GO-NS, have excellent electrocatalytic properties for OER in an alkaline solution (with a small overpotential of 273 mV and a Tafel slope of 49 mV dec-1 at the current density of 30 mA cm-2). The excellent electrocatalytic properties for OER of NFRG-3 nanohybrids could be attributed to the unique three-dimensional arraylike structure with many active sites. At the same time, reduced graphene oxide (RGO) with excellent conductivity can improve the charge-transfer efficiency and synergistically improve OER properties of nanohybrids.

Impact of hydrophobic micron ellipsoids on liquid surfaces.

HYPOTHESIS: Hydrophobic spheres may exhibit three impact modes after impacting the liquid surface. For the impact of common non-spherical particles in practical processes, particle shape affects the flow of surrounding fluid and forces acting on them, thus the impact behaviors of non-spherical particles may differ from those of spherical particles and remain to be revealed. SIMULATION: The impact of hydrophobic micron ellipsoidal particles is numerically studied by solving the coupled equations of particle motion and surrounding fluid flow combining VOF method and dynamic meshing technique. The motion characteristics of the ellipsoids and fluids, and the main forces acting on the ellipsoids during impact are analyzed. FINDINGS: The increase in the axis ratio (AR) of ellipsoid decreases the surface tension and fluid force, resulting in a smaller total force acting on the ellipsoid. Correspondingly, the ellipsoid's impact behavior changes. An impact-mode phase diagram is presented for the studied ellipsoids. Three impact modes, namely, submergence, rebound, and oscillation, exist when AR > 0.8, while only submergence and oscillation exist when AR ≤ 0.8. The critical velocities decrease with the increase in AR, which is well illustrated by the analysis of energy conversion under critical conditions.

Thermophoretic motion behavior of submicron particles in boundary-layer-separation flow around a droplet.

As a key mechanism of submicron particle capture in wet deposition and wet scrubbing processes, thermophoresis is influenced by the flow and temperature fields. Three-dimensional direct numerical simulations were conducted to quantify the characteristics of the flow and temperature fields around a droplet at three droplet Reynolds numbers (Re) that correspond to three typical boundary-layer-separation flows (steady axisymmetric, steady plane-symmetric, and unsteady plane-symmetric flows). The thermophoretic motion of submicron particles was simulated in these cases. Numerical results show that the motion of submicron particles around the droplet and the deposition distribution exhibit different characteristics under three typical flow forms. The motion patterns of particles are dependent on their initial positions in the upstream and flow forms. The patterns of particle motion and deposition are diversified as Re increases. The particle motion pattern, initial position of captured particles, and capture efficiency change periodically, especially during periodic vortex shedding. The key effects of flow forms on particle motion are the shape and stability of the wake behind the droplet. The drag force of fluid and the thermophoretic force in the wake contribute jointly to the deposition of submicron particles after the boundary-layer separation around a droplet.