Characterization of cavitation under ultrasonic horn tip – Proposition of an acoustic cavitation parameter

Acoustic cavitation, generated by a piezo-driven transducer, is a commonly used technique in a variety of processes, from homogenization, emulsification, and intensification of chemical reactions to surface cleaning and wastewater treatment. An ultrasonic horn, the most commonly used acoustic cavitation device, creates unique cavitation conditions under the horn tip that depend on various parameters such as the tip diameter, the driving frequency of the horn, its amplitude, and fluid properties. Unlike for hydrodynamic cavitation, the scaling laws for acoustic cavitation are poorly understood. Empirical relationships between cavitation dynamics, ultrasonic horn operating conditions, and fluid properties were found through systematic characterization of cavitation under the tip. Experiments were conducted in distilled water with various sodium chloride salt concentrations under different horn amplitudes, tip geometries, and ambient pressures. Cavitation characteristics were monitored by high-speed (200,000 fps) imaging, and numerous relations were found between operating conditions and cavitation dynamics. The compared results are discussed along with a proposal of a novel acoustic cavitation parameter and its relationship to the size of the cavitation cloud under the horn tip. Similar to the classical hydrodynamic cavitation number, the authors propose for the first time an acoustic cavitation parameter based on experimental results.     

Combining COMSOL modeling with acoustic pressure maps to design sono-reactors

Scaled-up and economically viable sonochemical systems are critical for increased use of ultrasound in environmental and chemical processing applications. In this study, computational simulations and acoustic pressure maps were used to design a larger-scale sono-reactor containing a multi-stepped ultrasonic horn. Simulations in COMSOL Multiphysics showed ultrasonic waves emitted from the horn neck and tip, generating multiple regions of high acoustic pressure. The volume of these regions surrounding the horn neck were larger compared with those below the horn tip. The simulated acoustic field was verified by acoustic pressure contour maps generated from hydrophone measurements in a plexiglass box filled with water. These acoustic pressure contour maps revealed an asymmetric and discrete distribution of acoustic pressure due to acoustic cavitation, wave interaction, and water movement by ultrasonic irradiation. The acoustic pressure contour maps were consistent with simulation results in terms of the effective scale of cavitation zones (∼10 cm and <5 cm above and below horn tip, respectively). With the mapped acoustic field and identified cavitation location, a cylindrically-shaped sono-reactor with a conical bottom was designed to evaluate the treatment capacity (∼5 L) for the multi-stepped horn using COMSOL simulations. In this study, verification of simulation results with experiments demonstrates that coupling of COMSOL simulations with hydrophone measurements is a simple, effective and reliable scientific method to evaluate reactor designs of ultrasonic systems.     

Study on degradation of dimethoate solution in ultrasonic airlift loop reactor

In this work, the degradation of dimethoate solution in ultrasonic airlift loop reactor (UALR) assisted with advanced oxidation processes was studied. The effects of O₃ flow rate, ultrasonic intensity, pH value and reaction temperature on the degradation rate were investigated. UALR imposed a synergistic effect combining sonochemical merit with high O₃ transfer rate. Under the optimal operation conditions: ultrasonic irradiation time was 4 h, O₃ flow rate was 0.41 m³ h⁻¹, ultrasonic intensity was 4.64 W cm⁻², pH value was 10.0, reaction temperature was 25 °C, and initial concentration of dimethoate was 20 mg L⁻¹, degradation rate of dimethoate increased to 90.8%. The experimental results indicated that the method of UALR degradation of organic pollutants in the presence of gas could reduce reaction time and improve degradation rate. UALR was an advisable choice for treating organic waste waters and this device could be easily scale up. Thus this process has wide application prospect in industry.     

Free surface entrainment of oxide particles and their role in ultrasonic treatment performance of aluminum alloys

Although the ultrasonic treatment of molten aluminum has been studied for long period, there is still much to be revealed for this process. Many studies have focused on the investigation of acoustic cavitation and streaming under the horn tip and their effects on the treatment efficiency. However, to the best of our knowledge, no attempt has been done to explain phenomena occurring near or on the melt free surface. Thus, the goal of this study is to investigate phenomena occurring at the free surface during ultrasound irradiation and clarify their possible influence on the ultrasound treatment performance. The results of high temperature and water model experiments reveal that ultrasound irradiation significantly promotes the formation of alumina particles on the melt free surface around sonotrode, and part of these particles can be entrained into aluminum melts. Furthermore, TEM observation results suggested that the entrained alumina inclusions can serve as nucleation sites for the primary Al₃Zr compounds. Most importantly, the oxidation and entrainment of particles from free surface are likely to be controllable by the immersion depth of sonotrode into molten aluminum.     

Designing and characterizing a multi-stepped ultrasonic horn for enhanced sonochemical performance

The commonly used ultrasonic horn generates localized cavitation below its converging tip resulting in a dense bubble cloud near the tip and limiting diffusion of reactive components into the bubble cloud or reactive radicals out of the bubble cloud. To improve contact between reactive components, a novel ultrasonic horn design was developed based on the principles of the dynamic wave equation. The horn, driven at 20 kHz, has a multi-stepped design with a cone-shaped tip increasing the energy-emitting surface areas and creating multiple reactive zones. Through different physical and chemical experiments, performance of the horn was compared to a typical horn driven at 20 kHz. Hydrophone measurements showed high acoustic pressure areas around the horn neck and tip. Sonochemiluminescence experiments verified multiple cavitation zones consistent with hydrophone readings. Calorimetry and dosimetry results demonstrated a higher energy efficiency (31.3%) and a larger hydroxyl radical formation rate constant (0.36 μM min⁻¹) compared to typical horns. In addition, the new horn degraded naphthalene faster than the typical horn tested. The characterization results demonstrate that the multi-stepped horn configuration has the potential to improve the performance of ultrasound as an advanced oxidation technology by increasing the cavitation zone in the solution.     

碟形超声变幅杆的设计

优化超声变幅杆的形状结构可有效地提高水域声场分布和空化区域,提升对水域超声空化效果。通过模拟分析发现传统超声变幅杆在水域中具有声场分布均匀性差、变幅杆端部声压高等特征,不利于声波在水域中传播。基于此,提出并优化设计了一种具有碟形结构的变幅杆,位于变幅杆的最大振幅处的碟形结构,有更大的振动位移;模拟表明其水域声场和声压均衡度显著优于传统变幅杆,铝箔空化腐蚀实验进一步证实了其水域中的声压分布均匀性。同时,实验通过铝箔的空化腐蚀、KI剂量测定及工件表面油渍去除对比了传统变幅杆和碟形变幅杆,分析表明碟形变幅杆所在水域中有较大的空化腐蚀区域,腐蚀速率明显提升,声化学反应速率提高,油渍去除程度增强,说明了设计的碟形变幅杆能够促进空化泡的产生,增加水域空化区域。     

Effect of amplitude and frequency of ultrasonic irradiation on morphological characteristics control of calcium carbonate

We have previously reported on the morphological control of calcium carbonate by changing synthetic conditions such as temperature, pH and degree of supersaturation in liquid reaction. The present study reports the effect of amplitude and frequency of ultrasonic irradiation on the particle size of calcium carbonate using a horn type ultrasonic apparatus at two different frequencies. The calcium carbonate precipitated by mechanical stirring had a particle size of about 20 μm. By contrast, the particle size of vaterite formed under ultrasonic irradiation was about 2 μm, with a specific surface area of 25–30 m²/g. The major polymorph of calcium carbonate formed by ultrasonic irradiation was vaterite with some calcite present. For 40 kHz ultrasonic irradiation, the specific surface area of the calcium carbonate increased with increasing amplitude. The particle size of vaterite formed at this frequency was about 2 μm, and its distribution was sharper than that obtained at 20 kHz. The mode diameter of the synthesized vaterite was found to decrease with increasing amplitude at 40 kHz.     

Ultrasound-enhanced diffusion through isolated frog skin

The effect of ultrasound on the transport of oxygen across excised frog abdominal skin has been studied. Samples were mounted in an exposure chamber in which the Ringer's solution on one side was saturated with oxygen while the other side of the skin had a low initial oxygen concentration. They were treated with ultrasound at 1, 1.5 and 2 W cm⁻² SATA c.w., respectively, and increases in the rate of oxygen transport were observed at all intensities. These increases ranged from 38 ± 4% at 1 W cm⁻² to 55 ± 8% at 2 W cm⁻². Variation in the pulse lengths from 25 to 200 ms and a constant average intensity did not affect the rate of transport significantly provided that the temporal intensity was constant. Since the peak acoustic pressure within the pulse increased with decreasing pulse length and increasing acoustic pressure increases the probability of cavitation occurring, the mechanism responsible for this phenomenon is probably not cavitation.     

Cavitation in a periodontal pocket by an ultrasonic dental scaler: A numerical investigation

Periodontal pockets are spaces or holes surrounded by teeth under the gum line. These pockets can become filled with infection-causing bacteria resulting in tissue, bone, and tooth loss. Cavitation produced by the oscillating tip of dental ultrasonic scalers plays a significant role in routine periodontal therapy to clean these areas. Numerical studies were conducted for a scaler vibrating in a periodontal pocket which was simplified to a hole, using ABAQUS based on the finite element method. The simulations consider the three-dimensional, nonlinear, and transient interaction between the vibration and deformation of the scaler tip, the water flow around the scaler and the cavitation formation. The numerical model was validated by comparing results with experimental data for a scaler vibrating in an unbounded liquid, the displacement at the free end of the scaler and the cavitation pattern near the scaler tip displaying excellent agreement. A parametric study for a scaler vibrating in a hole has been carried out in terms of the volume of the hole, the taper ratio (the radius ratio between the circular opening and bottom of the hole), and the immersion depth of the scaler tip in the hole. The amount of cavitation generated is evaluated by the cavitation density (or the void fraction) which is the ratio of the volume of the cavitation occupied in the hole to the total volume of the hole. Numerical results indicate that the cavitation density in the hole increases with the decreasing hole volume and the increasing taper ratio. It is inferred that cleaning effects could be increased if some modifications to the scaler design could be made to increase the blocking effect of the hole during the cleaning process. Cavitation is observed in the hole even if the scaler is placed above the hole and increases with the immersion depth.     

A novel liquid plasma AOP device integrating microwaves and ultrasounds and its evaluation in defluorinating perfluorooctanoic acid in aqueous media

A simplified and energy-saving integrated device consisting of a microwave applicator and an ultrasonic homogenizer has been fabricated to generate liquid plasma in a medium possessing high dielectric factors, for example water. The microwave waveguide and the ultrasonic transducer were interconnected through a tungsten/titanium alloy stick acting both as the microwave antenna and as the horn of the ultrasonic homogenizer. Both microwaves and ultrasonic waves are simultaneously transmitted to the aqueous media through the tungsten tip of the antenna. The microwave discharge liquid plasma was easily generated in solution during ultrasonic cavitation. The simple device was evaluated by carrying out the degradation of the perfluorooctanoic acid (PFOA), a system highly recalcitrant to degradation by conventional advanced oxidation processes (AOPs). PFOA is 59% degraded in an aqueous medium after only 90 s of irradiation by the plasma. Intermediates were identified by electrospray mass spectral techniques in the negative ion mode.     

Modeling cavitation in a rapidly changing pressure field – Application to a small ultrasonic horn

Ultrasonic horn transducers are frequently used in applications of acoustic cavitation in liquids. It has been observed that if the horn tip is sufficiently small and driven at high amplitude, cavitation is very strong, and the tip can be covered entirely by the gas/vapor phase for longer time intervals. A peculiar dynamics of the attached cavity can emerge with expansion and collapse at a self-generated frequency in the subharmonic range, i.e. below the acoustic driving frequency. The term “acoustic supercavitation” was proposed for this type of cavitation Žnidarčič et al. (2014) [1].We tested several established hydrodynamic cavitation models on this problem, but none of them was able to correctly predict the flow features. As a specific characteristic of such acoustic cavitation problems lies in the rapidly changing driving pressures, we present an improved approach to cavitation modeling, which does not neglect the second derivatives in the Rayleigh–Plesset equation. Comparison with measurements of acoustic supercavitation at an ultrasonic horn of 20 kHz frequency revealed a good agreement in terms of cavity dynamics, cavity volume and emitted pressure pulsations.The newly developed cavitation model is particularly suited for simulation of cavitating flow in highly fluctuating driving pressure fields.     

Numerical 3D flow simulation of ultrasonic horns with attached cavitation structures and assessment of flow aggressiveness and cavitation erosion sensitive wall zones

As a contribution to a better understanding of cavitation erosion mechanisms, a compressible inviscid finite volume flow solver with barotropic homogeneous liquid–vapor mixture cavitation model is applied to ultrasonic horn set-ups with and without stationary specimen, that exhibit attached cavitation at the horn tip. Void collapses and shock waves, which are closely related to cavitation erosion, are resolved. The computational results are compared to hydrophone, shadowgraphy and erosion test data. At the horn tip, vapor volume and topology, subharmonic oscillation frequency as well as the amplitude of propagating pressure waves are in good agreement with experimental data. For the evaluation of flow aggressiveness and the assessment of erosion sensitive wall zones, statistical analyses of wall loads and of the multiplicity of distinct collapses in wall-adjacent flow regions are applied to the horn tip and the stationary specimen. An a posteriori projection of load collectives, i.e. cumulative collapse rate vs. collapse pressure, onto a reference grid eliminates the grid dependency effectively for attached cavitation at the horn tip, whereas a significant grid dependency remains at the stationary specimen. The load collectives show an exponential decrease towards higher collapse pressures. Erosion sensitive wall zones are well predicted for both, horn tip and stationary specimen, and load profiles are in good qualitative agreement with measured topography profiles of eroded duplex stainless steel samples after long-term runs. For the considered amplitude and gap width according to ASTM G32-10 standard, the analysis of load collectives reveals that the distinctive erosive ring shape at the horn tip can be attributed to frequent breakdown and re-development of a small portion of the tip-attached cavity. This partial breakdown of the attached cavity repeats at each driving cycle and is associated with relatively moderate collapse peak pressures, whereas the stationary specimen is rather unfrequently stressed at the end of each subharmonic oscillation cycle by the violent collapse of the complete cavity.     

Long-term trend in CHF2Cl (HCFC-22) from high spectral resolution infrared solar absorption measurements and comparison with in situ measurements

The average tropospheric volume mixing ratio of CHF₂Cl (HCFC-22) has been retrieved from a time series of high spectral resolution ground-based infrared solar absorption spectra recorded with the McMath Fourier transform spectrometer located at the U.S. National Solar Observatory facility on Kitt Peak in southern Arizona (31.9°N, 111.6°W, 2.09 km altitude) for the time period October 1987–November 2002. The retrievals are based on fits to the well-isolated, unresolved 2ν₆ Q branch at 829.05 cm⁻¹ and the SFIT2 retrieval algorithm. The measured daily averages show a near linear rise per year in the mean tropospheric volume mixing ratio as a function of time with a best fit yielding an average increase rate of (5.66±0.15) parts per trillion (10⁻¹²) by volume per year, corresponding to (6.47±0.17)%yr⁻¹, 1 sigma, at the beginning of the time series. The tropospheric mixing ratios retrieved from the solar spectra have been compared with monthly average surface flask sampling measurements from the Climate Monitoring and Diagnostic Laboratory (CMDL) station at Niwot Ridge, Colorado (40.0°N, 105.5°W, 3013 m altitude), archived measurement from the same location, and early CMDL northern hemisphere Pacific cruise measurements. The average ratio of the retrieved tropospheric mixing ratio relative to the CMDL surface mixing ratio is 1.053 for the overlapping 1987 to 2002 time period. The retrieved mean tropospheric mixing ratio is consistent with the surface measurements within the errors estimated for the remote sensing observations.     

Understanding the ultrasound field of high viscosity mixtures: Experimental and numerical investigation of a lab scale batch reactor

In this work, mixtures of increasing viscosity (from 0.9 to ≈720 mPas) are sonicated directly using an ultrasonic horn at 30 kHz to investigate the effect of viscosity on the ultrasound field both from an experimental and numerical point of view. The viscosity of the mixtures is modified by preparing water-polyethylene glycol solutions. The impact of the higher viscosity on the acoustic pressure distribution is studied qualitatively and semi-quantitatively using sonochemiluminescence. The velocity of light scattering particles added in the mixtures is also explored to quantify acoustic streaming effects using Particle Image Velocimetry (PIV). A numerical model is developed that is able to predict cavitationally active zones accounting for both thermoviscous and cavitation based attenuation. The results show that two cavitation zones exist: one directly under the horn tip and one around the part of the horn body that is immersed in the liquid. The erosion patterns on aluminum foil confirm the existence of both zones. The intensity of the cavitationally active zones decreases considerably with increasing viscosity of the solutions. A similar reduction trend is observed for the velocity of the particles contained in the jet directly under the tip of the horn. Less erratic flow patterns relate to the high viscosity mixtures tested. Finally, two numerical models were made combining different boundary conditions related to the ultrasonic horn. Only the model that includes the radial horn movements is able to qualitatively predict well the location of the cavitation zones and the decrease of the zones intensity, for the highest viscosities studied. The current findings should be taken into consideration in the design and modelling phase of horn based sonochemical reactors.     

超声搅拌磁流变抛光液的声场仿真分析

为了探究超声搅拌磁流变抛光液的制备及优化工艺,利用多物理场数值计算方法,建立了超声搅拌磁流变抛光液的声场仿真模型,并进行了频域分析。研究了不同液位深度、超声变幅杆探入深度,不同功率下磁流变抛光液的声场分布。通过测量磁流变抛光液的声场强度对声场仿真进行了验证。结果表明：随着距变幅杆距离的增加,声强逐渐减弱,高声强区域主要分布在换能器轴线附近。声强在距变幅杆20mm范围内急剧衰减,变幅杆最佳探入深度为10mm,增大功率有助于空化区域的扩大。声场仿真结果与实验测量结果基本一致,对磁流变抛光液的制备提供了数值计算基础。     

Radon and its short-lived progeny: variations near the ground

In the atmosphere above the surface of the Earth the concentrations of radon and its progeny are measured, along with the meteorological parameters from December 1997 to December 2000 for a continental location, Pune (18°N,74°E), India. The concentrations show maxima in the early morning hours when the turbulence mixing is minimum; whereas in the afternoon the turbulence mixing is maximum and concentrations exhibit minima. The median values of concentration are 9.70 and 2.84 Bqm⁻³, respectively, for radon and its progeny, during the observation period. Ionization rates in the atmosphere are derived for the same period. It is found that the ionization rate exhibits a median value of 5.48 ionpairscm⁻³ s⁻¹. The diurnal and seasonal variations in the concentrations of radon and its progeny, and the ionization rate due to radioactivity are found to exhibit correlation with the relative humidity, and anti-correlation with the temperature.     

Ultrasound influence upon calcium carbonate precipitation on bacterial cellulose membranes

The effect of ultrasonic irradiation (40 kHz) on the calcium carbonate deposition on bacterial cellulose membranes was investigated using calcium chloride (CaCl₂) and sodium carbonate (Na₂CO₃) as starting reactants. The composite materials containing bacterial cellulose-calcium carbonate were characterized by means of scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR) and color measurements. The polymorphs of calcium carbonate that were deposited on bacterial cellulose membranes in the presence or in the absence of ultrasonic irradiation were calcite and vaterite. The morphology of the obtained crystals was influenced by the concentration of starting solutions and by the presence of ultrasonic irradiation. In the presence of ultrasonic irradiation the obtained crystals were bigger and in a larger variety of shapes than in the absence of ultrasounds: from cubes of calcite to spherical and flower-like vaterite particles. Bacterial cellulose could be a good matrix for obtaining different types of calcium carbonate crystals.     

Physical and chemical characteristics of ultrasonically-prepared water-in-diesel fuel: Effects of ultrasonic horn position and water content

An ultrasonic technique was applied to preparation of two-phase water-in-oil (W/O) emulsified fuel of water/diesel oil/surfactant. In this study, an ultrasonic apparatus with a 28 kHz rod horn was used. The influence of the horn tip position during ultrasonic treatment, sonication time and water content (5 or 10 vol%) on the emulsion stability, viscosity, water droplet size and water surface area of emulsion fuels prepared by ultrasonication was investigated. The emulsion stability of ultrasonically-prepared fuel significantly depended on the horn tip position during ultrasonic irradiation. It was found that the change in the stability with the horn tip position was partly related to that in the ultrasonic power estimated by calorimetry. Emulsion stability, viscosity and sum of water droplets surface area increased and water droplet size decreased with an increase in sonication time, and they approached each limiting value in the longer time. The maximum values of the viscosity and water surface area increased with water content, while the limiting values of the emulsion stability and water droplet size were almost independent of water content. During ultrasonication of water/diesel oil mixture, the hydrogen and methane were identified and the cracking of hydrocarbon components in the diesel oil occurred. The combustion characteristics of ultrasonically-prepared emulsion fuel were studied and compared with those of diesel oil. The soot and NOx emissions during combustion of the emulsified fuel with higher water contents were significantly reduced compared with those during combustion of diesel oil.     

TL and PTTL in natural fluorite previously irradiated with gamma rays and heavy ions

The effect of annealing temperature on the phototransfer thermoluminescence (PTTL) signal was studied to determine the appropriate annealing temperature for treating the natural powder before irradiation. The temperatures used to anneal virgin natural fluorite samples (only natural dose without giving the samples any artificial doses) were 150, 250, 350, 450, 550, 650 and 750°C for a duration of 1 h in each case. The results show that the PTTL response did not change for anneal temperatures up to 450°C, but at higher temperatures the signal decreased rapidly. The height of the 90°C peak decreased by two orders of magnitude as the anneal temperature increased from 450 to 750°C, whilst the height of the 180°C peak decreased by three orders of magnitude between the same two annealing temperatures. In order to investigate the effect of previous gamma rays and heavy ion irradiation on thermoluminescence (TL) and PTTL signals, powdered samples of natural fluorite from Cornwall, England, were annealed at 500°C and then irradiated (at GSI, Darmstadt, Germany) with ¹⁶¹Dy ions of energy 13 Mev/n; the range of fluences used was from 10⁴ to 10¹² ion cm⁻². Identical samples were given gamma doses in the range 1 Gy to 2.6 × 10⁴ Gy in order to compare the effects of gamma rays and heavy ions. The sensitivities of TL and PTTL were studied by giving the samples a gamma test dose of 1 Gy after annealing the samples at 500°C for 30 min in order to eliminate the TL resulting from previous gamma or heavy ion irradiation.     

Measurement of the acoustic properties of a nerve-muscle preparation as a function of physiologic state

Nerve-muscle preparations of Sprague Dawley rats were exposed to low dosage ultrasound. The objectives were to measure the velocity of propagation and attenuation of ultrasonic energy in both the relaxed and contracted states. A tension-measuring system and associated ultrasonic instrumentation were designed to measure the tension developed in stimulated muscle and its corresponding acoustic parameters, ie the attenuation coefficient, (db cm^-1) and the velocity of propagation, c (ms^-1). Each test was performed at ultrasonic frequencies 3.1, 5.35, and 7.68 MHz and with the preparation maintained at 23 ± 0.5° C. Attenuation of ultrasonic energy was observed to increase by 10 ± 0.5% in the active state from its value in the relaxed state. The relation between the attenuation and the acoustic frequency was found to be approximately linear over the frequency range tested. The velocity of propagation in the active state did not change appreciably from its value in the relaxed state and was observed to be independent of the acoustic frequency in the range used.