Bubble-liquid Interface Research Articles

Bubble-Assisted Sample Preparation Techniques for Mass Spectrometry.

This review delves into the efficacy of utilizing bubbles to extract analytes into the gas phase, offering a faster and greener alternative to traditional sample preparation methods for mass spectrometry. Generating numerous bubbles in liquids rapidly transfers volatile and surface-active species to the gas phase. Recently, effervescence has found application in chemical laboratories for swiftly extracting volatile organic compounds, facilitating instantaneous analysis. In the so-called fizzy extraction, liquid matrices are pressurized with gas and then subjected to sudden decompression to induce effervescence. Alternatively, specifically designed effervescent tablets are introduced into the liquid samples. In situ bubble generation has also enhanced dispersion of extractant in microextraction techniques. Furthermore, droplets from bursting bubbles are collected to analyze non-volatile species. Various methods exist to induce bubbling for sample preparation. The polydispersity of generated bubbles and the limited control of bubble size pose critical challenges in the stability of the bubble-liquid interface and the ability to quantify analytes using bubble-based sample preparation techniques. This review covers different bubble-assisted sample preparation methods and gives practical guidance on their implementation in mass spectrometry workflows. Traditional, offline, and online approaches for sample preparation relying on bubbles are discussed. Unconventional bubbling techniques for sample preparation are also covered.

Experimental investigation of local boron concentration in a 2 × 2 rod bundle channel under subcooled boiling flow

During the operation of pressured water reactors (PWRs), subcooled boiling occurring at the upper-span region of the fuel assembly causes migration of the boron concentration in the coolant. The distribution of boron concentration in the coolant is essential to predict the boron hideout within the Corrosion Related Unidentified Deposition (CRUD) and crud-induced power shift (CIPS). However, experimental data on local boron concentration of rod bundle geometries in subcooled boiling conditions are not available. In this paper, a vertical test channel is constructed to determine the distribution of the local boron concentration of a 2 × 2 rod bundle channel under subcooled boiling conditions. The bubble-boron concentration simultaneous measurement device is developed and calibrated to measure the local two-phase flow parameters and boron concentrations under the subcooled boiling conditions. The experimental results indicate that the boron concentration is highest near the narrowest gap and decreases toward the subchannel center or subchannel wall. The boron concentration increases linearly with void fraction in the central subchannel, while the boron concentration first increases rapidly and then slowly in the wall channel. The underlying mechanism for the boron concentration distribution is revealed by considering the boron enrichment on the bubble–liquid interface, diffusion of the boron concentration, boron mixing induced by bubble wake, and boron dilution caused by bubble condensation. On the basis of that, a boron equilibrium model considering the evaporation and condensation of bubbles is developed. The experimental data is used to support the development and validation of the boron equilibrium model. The comparison results show that the boron equilibrium model can predict the performance of the boron concentration in the rod bundle channel with an accuracy of 20 %.

Drop encapsulation and bubble bursting in surfactant-laden flows in capillary channels

We present a parametric study of the unsteady phenomena associated with the flow of elongated gas bubbles traveling through liquid-filled square capillaries under high Weber number conditions. These conditions induce the formation of an indentation at the back of the bubble that commonly gives way to a deep reentrant liquid jet penetrating the bubble. Subsequent steps include pinch-off events in the penetrating liquid to generate one or multiple encapsulated drops which may coalesce, in conjunction with the bursting of the bubble-liquid interface by either the liquid jet or the drops. Some of these interfacial instabilities have previously been reported experimentally and numerically for liquid-liquid flow in microchannels. We carry out three-dimensional direct numerical simulations based on a hybrid interface-tracking/level-set method capable of accounting for the presence and dynamic exchange of surfactants between the liquid bulk phase and the liquid-gas interface. Our results indicate that the delicate interplay among inertia, capillarity, viscosity, surfactant adsorption/desorption kinetics, and Marangoni stresses has a dramatic influence over the nonaxisymmetric morphological structures of the encapsulated drops-elongated bubble. This strong coupling also influences the pinch-off time, penetration depth of the liquid, and number, size, and velocity of the encapsulated drops across the bubble. The observed phenomena are summarized in three main morphological regimes based on surfactant-related parameters and dimensionless groups. A discussion of the flow regime maps is also provided. Published by the American Physical Society 2024

Mass transfer of chemical specie in acoustic cavitation bubble

In the present study, mass transfer across a gas–liquid interface of acoustic cavitation bubble is numerically investigated. The volume of fluid (VOF) method coupled with a continuous species transfer model is used to simulate the bubble dynamic behavior and mass transfer across the gas–liquid interface. Chemical species are transferred repeatedly between the liquid and gas phases in accordance with the bubble oscillation, and the chemical species are transferred into the bubble during an expansion phase, and to the outside of bubble during a compression phase. Time-averaged Sherwood number is decreased with an amplitude of sound pressure due to area effect and shell effect, and its value becomes negative at high pressure amplitude. Meanwhile, the instantaneous Sherwood number is largely varied in accordance with the bubble oscillation, and its magnitude becomes O(101) ∼ O(102).

Modeling of co-axial bubbles coalescence under moderate Reynolds regimes: A Bi-phase SPH approach

Phenomena involving bubble flow play a significant role in numerous industrial, natural, and scientific systems. Thus, liquid–gas interfaces must be considered the influence of surface tension and buoyancy. This work analyzes a complete numerical study for bi-fluid flow problems in the deformation evolution of two bubbles coalescing in a viscous liquid. This study discusses diverse configurations of the coalescence bubbles process and their effect on the displacement of the center of mass, velocity, streamlines, and evolution of the morphologies’ deformation. The resulting simulations revealed the process of the coalescence bubbles regarding three stages: approaching, drainage, and rupture of the interface. These steps reach different morphologies, defined as oblate ellipsoid, prolate ellipsoid, and ellipsoidal cap shapes between the trailing, leading, and merging bubbles. Likewise, an approximated bi-phase 2D methodology using the Navier–Stokes equations with Smoothed Particle Hydrodynamics (SPH) method and associated with the Continuous Surface Force (CSF) method was employed to approach the interaction between the bubbles, the surrounding liquid, and cavity walls. This approach with SPH and CSF for fused bubbles and their liquid interaction are validated employing numerical benchmarks in situations with high and moderate regimes of the Reynolds (Re) and Eötvös (Eo) numbers, and different sizes of diameter between coalescence bubbles. Correspondingly, examples of bubbles merging around a liquid owing to gravitational are rarely treated in the literature of mesh-free methods, especially to characterize different viscosity, density and surface tension regimes at the bubble–liquid interface, the effect of the method precision (distance between particles, Δx), the size of the surrounding liquid cavity and the initial distance between lighter domains. According to the bubbles deformation, during the coalescence is observed significant influence of Δx resolution and the cavity size, there are instances of instabilities, such as lateral tails, droplets inside the lighter domain, break-up, and satellite bubble formation. Finally, it is provided a robust numerical study of the coalescence process with a bi-phase SPH for different surfaces tension regimes (5≤Eo≤200), viscosity and density ratios (5≤λ,Φ≤100) and initial conditions in merging bubbles problems with moderates Reynolds numbers (5≤Re≤50).

Effects of SDS surface-active agents on hydrodynamics and oxygen mass transfer in a square bubble column reactor: Experimental and CFD modeling study

This work examined experimentally and numerically the effects of sodium dodecyl sulfate (SDS) surfactant agent on mass transfer coefficients kLaL and kL in a high-aspect square bubble column reactor. To this end, SDS aqueous solutions at concentrations between 5 ppm and 30 ppm were prepared. Superficial gas velocity was varied from 0.74 cm.s−1 to 9.44 cm.s−1 covering all flow regimes to analyze the interaction between different phases and the effect of liquid surface tension on gas-liquid interfaces. Experimental data indicated that the presence of the SDS in the liquid phase augmented the overall gas holdup up to 25% at a constant gas velocity (Ug = 7.3 cm.s−1) in the transition regime, which is due to the role of SDS in bubble interactions. The impact of SDS addition on the mass transfer is twofold. Firstly, it reduced kL because the SDS molecules migrate towards the bubble-liquid interface thanks to the lower O2 diffusivity in water, thus hindering the O2 transfer from one phase to the other. Secondly, it increased aL owing to the inhibition of bubbles coalescence and, therefore, the lower mean bubble size. Among these two effects, the latter is prevailing, which led to an increase in kLaL in contaminated systems. In the second part of this work, a population balance model (PBM) was coupled with a computational fluid dynamics (CFD) model based on large-eddy simulation (LES) to analyze the effect of both tap water and SDS contaminated systems on the breakage phenomena, local flow pattern, and the resulting hydrodynamics and mass transfer features in the reactor. Ultimately, experiments and numerical simulations agreed well in terms of global gas holdup and kLaL coefficient. In particular, the transition points in the case of the SDS media (except for foam formation) provided the model with adequate PBM definitions for the dispersed phase.

State transition of stable nanobubbles to unstable microbubbles on homogeneous surfaces

The widely accepted Epstein-Plesset theory (EPT) suggests that all gas bubbles are diffusively unstable in practical situations of accelerative shrinkage or unbounded growth. The stable nanobubbles confirmed by experiments go against EPT, which is verified by experiments on bubble radii down to micrometers. The theoretical gap between stable nanobubbles and unstable microbubbles requires a full-scale physical understanding. We present a model that describes the state transition from stable nanobubbles to unstable microbubbles on homogeneous surfaces, achieving diffusive equilibrium at the liquid-bubble interface and mechanical equilibrium at the triple-phase contact line simultaneously.

Urea-Bond Scission Induced by Therapeutic Ultrasound for Biofunctional Molecule Release.

Ultrasound-triggered remote control of biomolecular functions in cells provides unique advantages for us to interrogate nature. However, strategies to design therapeutic ultrasound-responsive functional molecules remain elusive, and rare ultrasound-cleavable chemical bonds have been developed to date. Herein, therapeutic ultrasound (1 MHz)-induced scission of urea bonds for drug release is demonstrated for the first time. Such a transformation has been verified to be initiated by hydroxyl radicals generated in the interior of cavitation bubbles, occurring specifically at the cavitation bubble-liquid interface. A series of urea-bond-containing prodrugs based on methylene blue (MB), namely MBUs, are designed. Upon sonication with low-intensity therapeutic ultrasound, the urea bonds linked with primary amines can be selectively cleaved, and free MB is released in a physiologically relevant environment, accompanied by recovered absorbance, fluorescence, and photosensitivity. Moreover, an FDA-approved alkylating agent (i.e., melphalan) bearing urea bond is also developed (MBU-Mel), successfully achieving ultrasound-triggered drug release in deep-seated cancer cells (mimic with 1 cm pigskin), showing the scalability of our ultrasound-responsive molecule platform in bioactive molecules release. This may set the starting point for therapeutic ultrasound-induced drug release, making a forward step in "sonopharmacology".

Ammonia chemistry: Sounds better with ultrasound

Hydrazine is a chemical of utmost importance in our society, either for organic synthesis or energy use. The direct conversion of NH3 to hydrazine is highly appealing, but it remains a very difficult task because the degradation of hydrazine is thermodynamically more feasible than the cleavage of the N−H bond of NH3. As a result, any catalyst capable of activating NH3 will thus unavoidably decompose N2H4. Here, we show that cavitation bubbles, created by ultrasonic irradiation of aqueous NH3 at a high frequency, act as microreactors to activate and convert NH3 to NH species, without assistance of any catalyst, yielding hydrazine at the bubble–liquid interface. The compartmentation of in-situ-produced hydrazine in the bulk solution, which is maintained close to 30 °C, advantageously prevents its thermal degradation, a recurrent problem faced by previous technologies. This work also points towards a path to scavenge .OH radicals by adjusting the NH3 concentration.

Conversion of Ammonia to Hydrazine Induced by High-Frequency Ultrasound.

Hydrazine is a chemical of utmost importance in our society, either for organic synthesis or energy use. The direct conversion of NH3 to hydrazine is highly appealing, but it remains a very difficult task because the degradation of hydrazine is thermodynamically more feasible than the cleavage of the N-H bond of NH3 . As a result, any catalyst capable of activating NH3 will thus unavoidably decompose N2 H4 . Here we show that cavitation bubbles, created by ultrasonic irradiation of aqueous NH3 at a high frequency, act as microreactors to activate and convert NH3 to NH species, without assistance of any catalyst, yielding hydrazine at the bubble-liquid interface. The compartmentation of in-situ-produced hydrazine in the bulk solution, which is maintained close to 30 °C, advantageously prevents its thermal degradation, a recurrent problem faced by previous technologies. This work also points towards a path to scavenge . OH radicals by adjusting the NH3 concentration.

Conversion of Ammonia to Hydrazine Induced by High‐Frequency Ultrasound

AbstractHydrazine is a chemical of utmost importance in our society, either for organic synthesis or energy use. The direct conversion of NH3 to hydrazine is highly appealing, but it remains a very difficult task because the degradation of hydrazine is thermodynamically more feasible than the cleavage of the N−H bond of NH3. As a result, any catalyst capable of activating NH3 will thus unavoidably decompose N2H4. Here we show that cavitation bubbles, created by ultrasonic irradiation of aqueous NH3 at a high frequency, act as microreactors to activate and convert NH3 to NH species, without assistance of any catalyst, yielding hydrazine at the bubble–liquid interface. The compartmentation of in‐situ‐produced hydrazine in the bulk solution, which is maintained close to 30 °C, advantageously prevents its thermal degradation, a recurrent problem faced by previous technologies. This work also points towards a path to scavenge .OH radicals by adjusting the NH3 concentration.

Thermal effect inside bubbles for weakly nonlinear pressure waves in bubbly liquids: Theory on short waves

In this study, weakly nonlinear pressure waves in quiescent compressible liquids comprising several uniformly-distributed spherical microbubbles, at moderately high-frequency and short-wavelength, are theoretically investigated. The energy equation at the bubble–liquid interface and the effective polytropic exponent are utilized to clarify thermal effects inside bubbles on wave dissipation. In addition, thermal conduction is investigated in detail using four temperature-gradient models. The following results are drawn: (i) Nonlinear Schrödinger equation is derived as an effective equation, wherein three types of dissipation factors, i.e., liquid viscosity, liquid compressibility, and thermal conduction, are unified into a linear combination as the dissipation coefficient. This is different from our previous result treating the low-frequency and long-wavelength case [Kamei et al., Phys. Fluids 33, 053302 (2021)], i.e., two types of dissipation terms appeared and did not unify into a linear combination. (ii) Dissipation due to thermal conduction is more than four times larger than that due to other dissipation factors. (iii) Dissipation due to thermal conduction at the bubble–liquid interface is considerably larger than that due to thermal conduction through the bubbly liquid. (iv) It is found that the dissipation effect in the short-wave case is smaller than that in the long-wave case.

An exhaustive theoretical analysis of thermal effect inside bubbles for weakly nonlinear pressure waves in bubbly liquids

Weakly nonlinear propagation of pressure waves in initially quiescent compressible liquids uniformly containing many spherical microbubbles is theoretically studied based on the derivation of the Korteweg–de Vries–Burgers (KdVB) equation. In particular, the energy equation at the bubble–liquid interface [Prosperetti, J. Fluid Mech. 222, 587 (1991)] and the effective polytropic exponent are introduced into our model [Kanagawa et al., J. Fluid Sci. Technol. 6, 838 (2011)] to clarify the influence of thermal effect inside the bubbles on wave dissipation. Thermal conduction is investigated in detail using some temperature-gradient models. The main results are summarized as follows: (i) Two types of dissipation terms appeared; one was a well-known second-order derivative comprising the effect of viscosity and liquid compressibility (acoustic radiation) and the other was a newly discovered term without differentiation comprising the effect of thermal conduction. (ii) The coefficients of the KdVB equation depended more on the initial bubble radius rather than on the initial void fraction. (iii) The thermal effect contributed to not only the dissipation effect but also to the nonlinear effect, and nonlinearity increased compared with that observed by Kanagawa et al. (2011). (iv) There were no significant differences among the four temperature-gradient models for milliscale bubbles. However, thermal dissipation increased in the four models for microscale bubbles. (v) The thermal dissipation effect observed in this study was comparable with that in a KdVB equation derived by Prosperetti (1991), although the forms of dissipation terms describing the effect of thermal conduction differed. (vi) The thermal dissipation effect was significantly larger than the dissipation effect due to viscosity and compressibility.

Sonochemical degradation of neonicotinoid pesticides in natural surface waters. Influence of operational and environmental conditions

Neonicotinoids sonochemical oxidation at high-frequency ultrasound (MHz range) has been carried out in ultrapure and natural surface-water matrices (river, reservoir and wastewater treatment plant effluent). To evaluate the influence of the operating variables, that is initial pollutant concentration, ultrasound frequency, ultrasound power, and pulse-stop time a Box-Behnken experimental design was planned. Optimal results were obtained using a frequency of 578 kHz, a power of 40 W L−1, with a pollutant concentration of 1 μM (for each pesticide), and using a pulse-stop time of 100 ms. The experimental data adjustment using the Langmuir-Hinshelwood heterogeneous kinetic model showed that neonicotinoids oxidation was carried out in the bubble-liquid interface by the attack of hydroxyl radicals. Experiments performed in the presence of radical scavengers, that is, methanol, ethanol and tert-butyl alcohol corroborated this reaction mechanism. The influence of some environmental conditions such as pH, presence of soluble inorganic species (Cl−, SO42−, NO3−, HPO42−, HCO3−) and soluble organic species (humic acids content) were established. Finally, the aqueous matrix's influence was investigated for three natural surface water cases, and the results were rationalized according to the main water physicochemical characteristics.

Theoretical elucidation of effect of drag force and translation of bubble on weakly nonlinear pressure waves in bubbly flows

Theoretical investigation of the effects of a translation of bubbles and a drag force acting on bubbles on the wave propagation in bubbly flows has long been lacking. In this study, we theoretically and numerically investigate the weakly nonlinear (i.e., finite but small amplitude) propagation of plane progressive pressure waves in compressible water flows that contain uniformly distributed spherical gas bubbles with translation and drag forces. First, we assume that the gas and liquid phases flow at independent velocities. Then, the drag force and virtual mass force are introduced in an interfacial transport across the bubble–liquid interface in the momentum conservation equations. Furthermore, we consider the translation and spherically symmetric oscillations as bubble dynamics and deploy a two-fluid model to introduce the translation and drag forces. Bubbles do not coalesce, break up, extinct, or appear. For simplicity, the gas viscosity, thermal conductivities of the gas and liquid, and phase change and mass transport across the bubble–liquid interface are ignored. The following results are then obtained: (i) Using the method of multiple scales, two types of Korteweg–de Vries–Burgers equations with a correction term due to the drag force are derived. (ii) The translation of bubbles enhances the nonlinear effect of waves, and the drag force acting on bubbles contributes the nonlinear and dissipation effects of waves. (iii) The results of long-period numerical analysis verify that the temporal evolution of the wave (not flow) dissipation due to the drag force differs from that caused by the acoustic radiation.

Protein crystallisation with air bubble templates: case of gas–liquid–solid interfaces

Crystal formation on air bubble–liquid interface, as soft template to efficiently prompt nucleation of proteins.

Weakly nonlinear theory and numerics on pressure wave propagation in a flowing water containing many translational bubbles acting a drag force

Focusing on the effect of translational motion of bubbles and drag force acting bubbles, we theotetically and numerically tackle weakly nonlinear propagation of plane progressive pressure waves in a compressible water flow uniformly containing a number of spherical gas bubbles. At an initial state, gas and liquid phases are flowing with each velocity. Drag force and virtual mass force are introduced in an interfacial transport across the bubble–liquid interface. As bubble dynamics, translation and spherically symmetric oscillation are considered. The bubbles do not coalesce, break up, disappear, and appear. The gas viscosity, the thermal conductivities of the gas and liquid are discarded. From the singular perturbation analysis up to the second order of approximation, we have two types of Korteweg–de Vries–Burgers (KdVB) equation with a newly introduced term without a differentiation due to the drag force from the basic equations for bubbly flows in a two-fluid model; the drag term is classified into the linear and nonlinear terms. The translation affects the nonlinear effect of waves and the drag force affects the dissipation effect of waves. We finally numerically solve the KdVB equation to compare three dissipation factors, i.e., acoustic radiation damping due to the liquid compressibility, liquid viscosity, and drag force for various initial void fraction and bubble radius.

Electrification of Sonoluminescing Single Bubble.

The charge of microbubbles in water is considered to be negative at the liquid-bubble interface. We investigated, for the first time, the charge of a single bubble sonoluminescence (SBSL bubble) that exhibits spatiotemporally stable light emission. When negative DC voltage was applied, the SBSL bubble was attracted to a hot electrode. Conversely, the SBSL bubble was repelled by the hot electrode when positive DC voltage was applied. The translation of the SBSL bubble under an electric field suggests that it is positively charged, and the bubble moved to an equilibrium position to balance the primary Bjerknes force and the electrostatic force. The amount of bubble translation under an electric field depended on the elapsed time of sonoluminescence, suggesting that the products generated inside the SBSL bubble affect the mechanism of bubble charging. Furthermore, we measured the electric field effects on bubble expansion and contraction by a light scattering technique. Applying a positive voltage decreased the maximum bubble diameter and also the intensity of the SBSL. Conversely, applying a negative voltage increased the maximum bubble diameter and also the intensity of the SBSL. The present study revealed that a SBSL bubble is positively charged.

Theoretical Study on an Effect of Thermal Conductivity at Bubble-Liquid Interface on Weakly Nonlinear Propagation of Pressure Waves in Bubbly Liquids

Theoretical Study on an Effect of Thermal Conductivity at Bubble-Liquid Interface on Weakly Nonlinear Propagation of Pressure Waves in Bubbly Liquids

Theoretical Elucidation of an Relationship of Thermal Conduction at Bubble-Liquid Interface on Pressure Waves in Bubbly Liquids and an Interaction between Nonlinear and Thermal Effects

Theoretical Elucidation of an Relationship of Thermal Conduction at Bubble-Liquid Interface on Pressure Waves in Bubbly Liquids and an Interaction between Nonlinear and Thermal Effects