The effect of ultrasonic waves on the nucleation of pure water and degassed water

In order to clarify the mechanism of nucleation of ice induced by ultrasound, ultrasonic waves have been applied to supercooled pure water and degassed water, respectively. For each experiment, water sample is cooled at a constant cooling rate of 0.15 °C/min and the ultrasonic waves are applied from the water temperature of 0 °C until the water in a sample vessel nucleates. This nucleation temperature is measured. The use of ultrasound increased the nucleation temperature of both degassed water and pure water. However, the undercooling temperature for pure water to nucleate is less than that of degassed water. It is concluded that cavitation and fluctuations of density, energy and temperature induced by ultrasound are factors that affect the nucleation of water. Cavitation is a major factor for sonocrystallisation of ice.     

Theoretical model of ice nucleation induced by inertial acoustic cavitation. Part 2: Number of ice nuclei generated by a single bubble

In the preceding paper (part 1), the pressure and temperature fields close to a bubble undergoing inertial acoustic cavitation were presented. It was shown that extremely high liquid water pressures but quite moderate temperatures were attained near the bubble wall just after the collapse providing the necessary conditions for ice nucleation. In this paper (part 2), the nucleation rate and the nuclei number generated by a single collapsing bubble were determined. The calculations were performed for different driving acoustic pressures, liquid ambient temperatures and bubble initial radius. An optimal acoustic pressure range and a nucleation temperature threshold as function of bubble radius were determined. The capability of moderate power ultrasound to trigger ice nucleation at low undercooling level and for a wide distribution of bubble sizes has thus been assessed on the theoretical ground.     

液态Ti-Al合金的深过冷与快速枝晶生长

采用电磁悬浮和自由落体两种试验技术研究了液态Ti-25 wt.%Al合金的亚稳过冷能力、晶体形核机制和枝晶生长过程. 试验发现, 即使电磁悬浮无容器状态下仍难以消除润湿角θ ≥60°的异质晶核, 合金熔体过冷度可达210 K (0.11T_L). β-Ti相形核的热力学驱动力随过冷度近似以线性方式增大, 其枝晶生长速度高达11.2 m/s, 从而在慢速冷却条件下实现了快速凝固. 理论计算表明, 随着过冷度的逐步增大, β相枝晶生长从溶质扩散控制转变为热扩散控制. 当过冷度超过100 K时, 非平衡溶质截留效应可使合金熔体发生无偏析凝固. 然而, 单靠深过冷状态不足以抑制β相的后续固态相变. 对于落管中快速凝固的直径77-1048 μm合金液滴, 其冷却速率最高达1.05×10⁵ K/s, 深过冷与快速冷却的耦合作用能更有效地调控凝固组织形成过程.     

Dendrite growth characteristics within liquid Fe-Sb alloy

Bulk samples and small droplets of liquid Fe-10%Sb alloys are undercooled up to 429 K (0.24TL) and 568 K (0.32TL), respectively, with glass fluxing and free fall techniques. The high undercooling does not change the phase constitution, and only the αFe solid solution is found in the rapidly solidified alloy. The experimental results show that when the undercooling is below 296 K, the growth velocity of αFe dendrite rises exponentially with the increase of undercooling and reaches a maximum value 1.38 m/s. S...     

A study on the primary and secondary nucleation of ice by power ultrasound

Several different investigations have been carried out to study the primary and secondary nucleation of ice by sonocrystallisation. Firstly, the primary nucleation of discrete ice crystals in a supercooled sucrose solution has been observed. For increasing concentrations of sucrose solutions from 0 to 45 wt%, the nucleation temperature consistently occurs at a higher nucleation temperature in the presence of ultrasound. The nucleation temperature also increases as the power output and duty cycle of a commercial ultrasonic horn are increased. Snap shot images of the bubble clouds obtained from the ultrasonic horn also show that the number of bubbles appears to increase as the ultrasonic output is increased. This suggests that the nucleation of ice is related to the power output and number of cavitation bubbles. The effect of a single bubble on the sonocrystallisation of ice is discussed. High-speed movies (1120 fps) have shown that the crystallisation appears to occur in the immediate vicinity of the single bubble. In most cases, many crystals are observed and it is not known whether a single ice crystal is being fragmented by the bubble or whether many crystals are being initiated. The bubble appears to undergo a dancing regime, frequently splitting and rejoining and also emitting some small microbubbles. A study on the secondary nucleation of ice in sucrose solutions has been carried out using a unique ultrasonic cold stage device. Images taken using a microscope system show that the pre-existing ice dendrite crystals can be broken up into smaller fragments by an ultrasonic field. Cavitation bubbles appear to be important during the fragmentation process, possibly melting any ice crystals in their path. Flow patterns around cavitation bubbles have also been observed, and these may be responsible for the fragmentation of ice crystals.     

RAPID DENDRITIC GROWTH INVESTIGATED WITH ARTIFICIAL NEURAL NETWORK METHOD

Rapid dendritic growth of γ-(Ni, Fe) phase, β-CoSb intermetallic compound and α-Fe phase was realized by undercooling Ni-10%Fe single phase alloy, Co-60.5%Sb intermetallic alloy and Fe-40%Sn hypomonotectic alloy to a substantial extent. Their experimentally measured dendrite growth velocities were 79.5m/s, 12m/s and 0.705m/s, corresponding to undercooling levels of 303K(0.18T_L), 168K(0.11 T_L) and 219K(0.15 T_L) respectively. Since the usual dendrite growth theory deviates significantly from reality at great undercoolings, an artificial neural network incorporated with stochastic fuzzy control was developed to explore rapid dendrite growth kinetics. It leads to the reasonable prediction that dendritic growth always exhibits a maximum velocity at a certain undercooling, beyond which dendrite growth slows down as undercooling increases still further. In the case of Fe-Sn monotectic alloys, α-Fe dendrite growth velocity was found to depend mainly on undercooling rather than alloy composition.     

过冷熔体中枝晶生长的相场模拟

本文利用相场方法对过冷镍熔体中枝晶生长过程进行了模拟,发现在过冷度低于 200 K时,生长速度与过冷度之间近似呈幂函数关系,当过冷度高于 200 K时,生长速度与过冷度之间基本呈线性关系。伴随着速度/过冷度之间关系的变化,枝晶尖端半径/过冷度的关系则呈现先减小后增加的趋势,并在 200 K时达到最小。本文还将模拟结果与实验值和经典LKT理论进行了比较,对上述关系转变的物理机制进行了分析。     

Metastable phase separation and rapid solidification of undercooled Co_(40)Fe_(40)Cu_(20) alloy

The metastable liquid phase separation and rapid solidification behaviors of Co_(40) Fe_(40) Cu_(20) alloy were investigated by using differential thermal analysis(DTA) in combination with glass fluxing and electromagnetic levitation(EML) techniques. The critical liquid phase separation undercooling for this alloy was determined by DTA to be 174 K. Macrosegregation morphologies are formed in the bulk samples processed by both DTA and EML. It is revealed that undercooling level, cooling rate, convection, and surface tension difference between the two separated phases play a dominant role in the coalescence and segregation of the separated phases. The growth velocity of the(Fe,Co) dendrite has been measured as a function of undercooling up to 275 K. The temperature rise resulting from recalescence increases linearly with the increase of undercooling because of the enhancement of recalescence. The slope change of the recalescence temperature rise versus undercooling at the critical undercooling also implies the occurrence of liquid demixing.     

无容器条件下Cu-Pb偏晶的快速生长

在落管无容器条件下实现了Cu-10%Pb亚偏晶和Cu_374%Pb偏晶的快速生长. 发现随着液滴 过冷度的增大, 亚偏晶中初生(Cu)相的生长形态经历“粗大枝晶→碎断枝晶→等轴晶”的转 变. 偏晶的组织形态从多个偏晶胞组织演化为单个偏晶胞组织. 理论计算表明，直径在1000 —60 μm之间的亚偏晶和偏晶合金液滴, 最大过冷度分别为269 K (02 TL_L )和245 K (02 TM_M). 亚偏晶合金中初生(Cu)枝晶的最大生长速度为24 m/s , 关键词： 无容器处理 深过冷 晶体生长 相分离     

Can secondary nucleation exist in ice banding of freezing colloidal suspensions?

The formation mechanism of ice banding in the system of freezing colloidal suspensions, which is of significance in frost heaving, ice-templating porous materials and biological materials, is still a mystery. Recently, the theory of secondary nucleation and growth of ice has been proposed to explain the emergence of a new ice lens. However, this theory has not been quantitatively examined. Here, we quantitatively measure the initial interfacial undercooling of a new ice lens and the nucleation undercoolings of suspensions. We find that the interfacial undercooling cannot satisfy the nucleation undercooling of ice and hence disprove the secondary nucleation mechanism for ice banding.     

液体材料超声处理过程中声场和流场的分布规律研究

针对合金熔体等液体材料的超声处理过程,选取水作为透明模型材料,采用数值模拟计算和示踪粒子实验方法,研究了20和490 kHz两种频率超声作用下水中的声场和流场分布.结果表明,增大变幅杆半径能够提高水中声压水平,扩大空化效应的发生区域.当超声频率为20 kHz时,水中声压最大值出现在超声变幅杆下端面处,且声压沿传播距离的增大而显著减小.如果超声频率增加至490 kHz,水中的声压级相比于20 kHz时明显提高,且声压沿着超声传播方向呈现出周期性振荡特征.两种频率超声作用下水中的流场呈现相似的分布特征,且平均流速均随着变幅杆半径增大表现出先升高后降低的趋势.变幅杆半径相同时,20 kHz频率超声作用下水中的平均流速高于490 kHz频率超声.采用示踪粒子图像测速技术实时观察和测定了水中的流速分布,发现其与计算结果基本一致.     

液态三元Fe-Cr-Ni合金中快速枝晶生长与溶质分布规律

采用落管方法实现了液态三元Fe-Cr-Ni合金的深过冷与快速凝固,合金液滴的冷却速率和过冷度均随液滴直径的减小而迅速增大.两种成分合金近平衡凝固组织均为粗大板条状α相.在快速凝固过程中,不同直径Fe_(81.4)Cr_(13.9)Ni_(4.7)合金液滴凝固组织均为板条状α相,其固态相变特征很明显,随着过冷度增大,初生δ相由具有发达主干的粗大枝晶转变为等轴晶.Fe_(81.4)Cr_(4.7)Ni_(13.9)合金液滴凝固组织由α相晶粒组成,随着过冷度增大,初生γ相由具有发达主干的粗大枝晶转变为等轴晶,其枝晶主干长度和二次分枝间距均显著下降,晶粒内溶质的相对偏析度也明显减小,溶质Ni的相对偏析度始终大于溶质Cr.理论计算表明,与γ相相比,δ相枝晶生长速度更大.在实验获得的过冷度范围内,两种Fe-Cr-Ni合金枝晶生长过程均由热扩散控制.     

Effect of solidification temperature range on the dendritic growth mode

Electromagnetic levitation technique was used to undercool bulk samples of Co-20% Cu and Co-60% Cu alloys and high undercoolings up to 303 and 110 K were achieved,respectively.The dendritic growth velocities were measured as a function of undercooling.The dendrite growth velocity of the Co-20% Cu alloy was much higher than that of the Co-60% Cu alloy.The experimental data were analyzed on the basis of the LKT/BCT dendritic growth model by taking into account non-equilibrium interface kinetics.It has been re...     

Investigations in physical mechanism of ultrasound-assisted antisolvent batch crystallization of lactose monohydrate from aqueous solutions

Sonication is known to enhance crystallization of lactose from aqueous solutions. This study has attempted to reveal the mechanistic features of antisolvent crystallization of lactose monohydrate from aqueous solutions. Experiments were conducted in three protocols, viz. mechanical stirring, mechanical stirring with sonication and sonication at elevated static pressure. Mechanical stirring provided macroconvection while sonication induced microconvection in the system. Other experimental parameters were initial lactose concentration and rate of antisolvent (ethanol) addition. Kinetic parameters of crystallization were coupled with simulations of bubble dynamics. The growth rate of crystals, rate of nucleation, average size of crystal crop and total lactose yield in different protocols were related to nature of convection in the medium. Macroconvection assisted nucleation but could not give high growth rate. Microconvection comprised of microstreaming due to ultrasound and acoustic (or shock) waves due to transient cavitation. Sonication at atmospheric static pressure enhanced growth rate but reduced nucleation. However, with elimination of cavitation at elevated static pressure, sonication enhanced both nucleation and growth rate resulting in almost complete lactose recovery.     

深过冷三元Ni-Cu-Co合金的快速枝晶生长

研究了深过冷条件下三元Ni₈₀Cu₁₀Co₁₀合金的快速枝晶生长, 采用电磁悬浮无容器处理方法获得了335 K(0.2T_L)的最大过冷度. X射线衍射分析与差示扫描量热分析均表明,凝固组织为α-Ni单相固溶体. 随过冷度增大, 凝固组织显著细化, 并且当过冷度达110 K时，凝固组织的形态由粗大形枝晶转变为等轴晶. 深过冷条件下溶质截留效应增强, 使得微观偏析程度减小. 对不同过冷度下合金枝晶的生长速度进 关键词： 深过冷 枝晶生长 快速凝固 溶质截留     

Respective contribution of cavitation and convective flow to local stirring in sonoreactors

The knowledge of respective parts of convection and cavitation to the stirring induced by ultrasound at one exact position into a sonoreactor is useful for all processes implementing surfaces exposed to sonication. PIV measurement allows real fluid motion determination, whereas the electrochemical technique gives an equivalent flow velocity considered as the sum of all stirring contributions to the electrode. Thus, by a simple subtraction between real fluid velocity and equivalent flow velocity, it is possible to identify the contribution of each phenomenon. Applied to low frequency reactors, it had been observed that cavitation is the preponderant phenomenon, with a contribution of stirring close to the electrode always more than 90%. High frequency reactors, frequently known to produce less cavitation, have shown that at the focal zone, if it concerns HIFU, cavitation becomes preponderant and reaches similar values to those close to the ultrasonic horn in low frequency sonoreactors.     

Liquid State Undercoolability and Crystal Growth Kinetics of Ternary Ni-Cu-Sn Alloys

The Liquid state undercoolability and crystal growth kinetics of ternary Ni-5%Cu-5%Sn and Ni-10%Cu-10%Sn alloys are investigated by the glass fluxing method.In these two alloys,experimental maximum undercoolings of 304K(0.18T_L) and 286K(0.17T_L) are achieved and the dendritic growth velocities attain 39.8 and 25.1m/s,respectively.The transition of morphology from coarse dendrite into equiaxed structure occurs and the grain size of the a(Ni) phase decreases remarkably when the undercooling increases.Both the lattice constant and microhardness increase obviously with the enhancement of undercooling.The enrichment of Cu and Sn solute contents reduces the dendritic growth velocity,while enhances the lattice constant and microhardness of a(Ni)phase.     

微重力条件下Ni-Cu合金的快速枝晶生长研究

采用落管方法实现了Ni-50%Cu过冷熔体在微重力和无容器条件下的快速枝晶生长.对微重力条件下的晶体形核和快速生长进行了研究，发现随着过冷度的增大，晶体生长形态由粗大枝晶向规划均匀的等轴晶转变.实验中最大冷却速率达到8×103K/s，获得了218K(014TL)的最大过冷度.理论分析表明，过冷熔体中优先发生异质形核，形核率可达1012m-3s-1以上；Ni-50%Cu过冷熔体中的枝晶生长随过冷度的增大发生由溶质扩散控制向热扩散控制的生长动力学机理转变.在68K过冷度条件下，生长界面前沿的偏析程序最大. 关键词： 落管 微重力 深过冷 枝晶 熔体     

Rapid growth of ternary eutectic under high undercooling conditions

~~Rapid growth of ternary eutectic un der high undercooling conditions1.Offerman, S.E., Dijk, N.H., Sietsma, J.et al., Grain nucleation and growth during phase transformations, Science, 2002, 298: 1003-1005. 2.Warren, J.A., Langer, J.S., Prediction of dendritic spacings in a directional-solidification experiment, Phys.Rev.E, 1993, 47: 2702-2712. 3.Cao, C.D., Wang, N., Wei, B., Containerless rapid solidification of undercooled Cu-Co peritectic alloys, Science in China, Ser.A, …     

The microscopic visualisation of the sonocrystallisation of ice using a novel ultrasonic cold stage

This work reports dynamic video images of the influence of ultrasonic cavitation on the sonocrystallisation of ice at a microscopic level. This has been achieved through the construction of a unique ultrasonic system for an optical microscope. The system consists of (1). an ultrasonic cold stage, (2). a temperature control system, and (3). a microscope and imaging setup. This allows the temperature of a sample to be systematically controlled while it is subjected to simultaneous excitation with alternating pressures in the ultrasonic frequency range. Both the amplitude of excitation and the frequency can be varied. Experiments on ice crystals in pure water and sucrose solutions were conducted. Three distinct phenomena were observed. Firstly, there is a tendency for cavitation bubbles to form at the grain boundaries between ice crystals. Secondly, there is a progressive melting of ice by cavitation bubbles which appear to eat their way into the ice phase. Thirdly, the dendritic ice structures may fragment under the influence of ultrasound, thus increasing the number of nuclei which may subsequently grow (secondary nucleation). These observations form the basis of a significantly enhanced understanding and exploitation of the sonocrystallisation of ice.