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1.
This paper tries to discern the mechanistic features of sonochemical degradation of recalcitrant organic pollutants using five model compounds, viz. phenol (Ph), chlorobenzene (CB), nitrobenzene (NB), p-nitrophenol (PNP) and 2,4-dichlorophenol (2,4-DCP). The sonochemical degradation of the pollutant can occur in three distinct pathways: hydroxylation by OH radicals produced from cavitation bubbles (either in the bubble–bulk interfacial region or in the bulk liquid medium), thermal decomposition in cavitation bubble and thermal decomposition at the bubble–liquid interfacial region. With the methodology of coupling experiments under different conditions (which alter the nature of the cavitation phenomena in the bulk liquid medium) with the simulations of radial motion of cavitation bubbles, we have tried to discern the relative contribution of each of the above pathway to overall degradation of the pollutant. Moreover, we have also tried to correlate the predominant degradation mechanism to the physico-chemical properties of the pollutant. The contribution of secondary factors such as probability of radical–pollutant interaction and extent of radical scavenging (or conservation) in the medium has also been identified. Simultaneous analysis of the trends in degradation with different experimental techniques and simulation results reveals interesting mechanistic features of sonochemical degradation of the model pollutants. The physical properties that determine the predominant degradation pathway are vapor pressure, solubility and hydrophobicity. Degradation of Ph occurs mainly by hydroxylation in bulk medium; degradation of CB occurs via thermal decomposition inside the bubble, degradation of PNP occurs via pyrolytic decomposition at bubble interface, while hydroxylation at bubble interface contributes to degradation of NB and 2,4-DCP.  相似文献   

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3.
    
The sonochemical activity and the radial dynamics of a harmonically excited spherical bubble are investigated numerically. A detailed model is employed capable to calculate the chemical production inside the bubble placed in water that is saturated with oxygen. Parameter studies are performed with the control parameters of the pressure amplitude, the forcing frequency and the bubble size. Three different definitions of collapse strengths (extracted from the radius vs. time curves) are examined and compared with the chemical output of various species. A mathematical formula is established to estimate the chemical output as a function of the collapse strength; thus, the chemical activity can be predicted without taking into account the chemical kinetics into the bubble model. The calculations are carried out by an in-house code exploiting the high processing power of professional graphics cards (GPUs).The results shown that chemical activity can be approximated qualitatively from the values of relative expansion. This could be helpful in order to optimise chemical output of sonochemical reactors either from measurement data or simulations as well.  相似文献   

4.
This paper addresses the matter of mechanistic features of ultrasound-assisted permanganate oxidation of organic compounds in aqueous phase. This reaction system is essentially a liquid–liquid heterogeneous one, which is limited by the mass transfer characteristics. Previous research has established that ultrasound irradiation of reaction mixture enhances the kinetics and yield of permanganate oxidation. The principal physical effect of ultrasonic cavitation is formation of fine emulsion between immiscible phases that eliminates the mass transfer resistance, while principal chemical effect is production of radicals through transient collapse of cavitation bubbles, which accelerate the reaction. In this paper, we have tried to discriminate between these physical and chemical effects by coupling experiments with different conditions (which alter the nature of cavitation phenomena in the medium) to simulations of cavitation bubble dynamics. It is revealed that in absence of radical conserving agent, the enhancement effect is merely physical. Diffusion of radicals towards interface between phases, where the oxidation reaction occurs is the limiting factor in contribution of chemical effect of ultrasonic cavitation towards enhancement of oxidation. Enhancement of total radical production in the aqueous phase (by degassing of the medium) increases the overall oxidation yield, but only marginally. On the other hand, addition of a radical conserver such as FeSO4·7H2O results in marked enhancement in oxidation yield, as the conserver assists deeper penetration of radicals in the aqueous medium and diffusion towards interface.  相似文献   

5.
    
A state-of-the-art chemical mechanism is introduced to properly describe chemical processes inside a harmonically excited spherical bubble placed in water and saturated with oxygen. The model uses up-to-date Arrhenius-constants, collision efficiency factors and takes into account the pressure-dependency of the reactions. Duplicated reactions are also applied, and the backward reactions rates are calculated via suitable thermodynamic equilibrium conditions. Our proposed reaction mechanism is compared to three other chemical models that are widely applied in sonochemistry and lack most of the aforementioned modelling issues. In the governing equations, only the reaction mechanisms are compared, all other parts of the models are identical. The chemical yields obtained by the different modelling techniques are taken at the maximum expansion of the bubble. A brief parameter study is made with different pressure amplitudes and driving frequencies at two equilibrium bubble sizes. The results show that due to the deficiencies of the former reaction mechanisms employed in the sonochemical literature, several orders of magnitude differences of the chemical yields can be observed. In addition, the trends along a control parameter can also have dissimilar characteristics that might lead to false optimal operating conditions. Consequently, an up-to-date and accurate chemical model is crucial to make qualitatively and quantitatively correct conclusions in sonochemistry.  相似文献   

6.
    
In this work, a comparison between the temperatures/pressures within acoustic cavitation bubble in an imidazolium-based room-temperature ionic liquid (RTIL), 1-butyl-3-methylimidazolium bis(triflluoromethyl-sulfonyl)imide ([BMIM][NTf2]), and in water has been made for a wide range of cavitation parameters including frequency (140–1000 kHz), acoustic intensity (0.5–1 W cm−2), liquid temperature (20–50 °C) and external static pressure (0.7–1.5 atm). The used cavitation model takes into account the liquid compressibility as well as the surface tension and the viscosity of the medium. It was found that the bubble temperatures and pressures were always much higher in the ionic liquid compared to those predicted in water. The valuable effect of [BMIM][NTf2] on the bubble temperature was more pronounced at higher acoustic intensity and liquid temperature and lower frequency and external static pressure. However, confrontation between the predicted and the experimental estimated temperatures in ionic liquids showed an opposite trend as the temperatures measured in some pure ionic liquids are of the same order as those observed in water. The injection of liquid droplets into cavitation bubbles, the pyrolysis of ionic liquids at the bubble-solution interface as well as the lower number of collapsing bubbles in the ionic liquid may be the responsible for the lower measured bubble temperatures in ionic liquids, as compared with water.  相似文献   

7.
In this review the phenomenon of ultrasonic cavitation and associated sonochemistry is presented through system parameters. Primary parameters are defined and considered, namely; pressure amplitude, frequency and reactor design; including transducer type, signal type, vessel-transducer ratio, liquid flow, liquid height, liquid temperature and the presence of a reflective plate. Secondary parameters are similarly characterised and involve the use of gas and liquid additives to influence the chemical and physical environments. Each of the parameters are considered in terms of their effect on bubble characteristics and subsequent impact on sonochemical activity. Evidence suggests that via parametric variation, the reaction products and efficiency may be controlled. This is hypothesised to occur through manipulation of the structural stability of the bubble.  相似文献   

8.
High-density controllable bubble structures are produced in the vicinity of radiating surface by artificially implant nuclei. Two kinds of typical cavitation structures produced by artificially implant nuclei are investigated. The focusing action and the physical origin of jet-induced cone-like bubble structure are analyzed. The sonochemical activity of cavitation structures is measured by using the standard method of potassium iodide dosimetry. The controllability of cavitation bubble cluster in the acoustic field is also discussed in this work.  相似文献   

9.
用脉冲激光同轴全息技术测量微射流   总被引:2,自引:2,他引:0  
 用脉冲激光同轴全息技术建立了全息照相系统和高精度同步时序系统,获得了采用爆轰加载产生高速运动的微射流全息图,并再现出微射流的全息像,得到粒子的大小和分布情况,从图像处理得到粒子尺寸的统计结果表明,最大尺寸在300μm左右,最小尺寸在30μm左右。证明了研制的全息系统和测试技术可以测量高速的微射流场。.  相似文献   

10.
    
Sonochemical synthesis (sonochemistry) is one of the most effective techniques of breaking down large clusters of nanoparticles (NPs) into smaller clusters or even individual NPs, which ensures their dispersibility (stability) in a solution over a long duration. This paper demonstrates the potential of sonochemistry becoming a valuable tool for the deposition of gold (Au) shell on iron oxide nanoparticles (Fe3O4 NPs) by explaining the underlying complex processes that control the deposition mechanism. This review summarizes the principles of the sonochemistry method and highlights the resulting phenomenon of acoustic cavitation and its associated physical, chemical and thermal effects. The effect of sonochemistry on the deposition of Au NPs on the Fe3O4 surface of various sizes is presented and discussed. A Vibra-Cell ultrasonic solid horn with tip size, frequency, power output of ½ inch, 20 kHz and 750 W respectively was used in core@shell synthesis. The sonochemical process was shown to affect the surface and structure of Fe3O4 NPs via acoustic cavitation, which prevents the agglomeration of clusters in a solution, resulting in a more stable dispersion. Deciphering the mechanism that governs the formation of Au shell on Fe3O4 core NPs has emphasized the potential of sonication in enhancing the chemical activity in solutions.  相似文献   

11.
The Nd:YAG laser-induced breakdown of 20 μm glass microspheres was investigated using time-resolved optical shadow and Schlieren images. Time-resolved imaging showed the location of the initial breakdown and the shockwave motion over its first 400 μm of expansion. Measured shockwave velocities were in the range of 1–10 km/s and showed a linear dependency on laser fluence within 30 ns.  相似文献   

12.
The structure and evolution of the laser-induced vapor plume and shockwave were measured from femtosecond time resolved shadowgraph images. By changing the wavelength of the probe beam (400 and 800 nm), differences in the opacity of the vapor plume were measured as a function of delay time from the ablation laser pulse. The evolution of the temperature and electron number density during and after the ablation laser pulse were determined and compared for ablation in argon and helium background gases. A laser supported detonation wave (LSD) observed for ablation in argon, blocks the incoming laser energy and generates a high-pressure region above the vapor plume.  相似文献   

13.
We propose a 4-velocity unidimensional discrete Boltzmann model with two different speeds 2, 1 and two different masses 1, 2. With the three conservation laws of mass, momentum, and energy satisfied, we can introduce a nontrivial temperature. First, we determine the similarity shock waves satisfying physical properties: positivity, shock stability, inequalities of the subsonic and supersonic flows, increase or decrease of both mass and temperature across the shock. It results that either the speed of the shock front is higher than the speed 1 of the slow particles and the shocks are compressive or less than 1 and the shocks are rarefactive. We observe overshoots of the temperature, across the shock, with bumps higher and higher as the shock front speed increases. Second, we study the (1+1)-dimensional shock waves. They represent the superposition and collision of two compressive shocks traveling in opposite directions and we observe temperature overshoots for not too large times.  相似文献   

14.
The uses of ultrasound in food technology   总被引:23,自引:0,他引:23  
The same physical and mechanical effects which have been utilised in sonochemistry, i.e. strong shear forces, particle fragmentation, increased mass and heat transfer, nucleation of seedling, have been applied to food processing. Examples are quoted from various applications where power ultrasound has been used to influence the development of living cells, improve sterilisation and effect enzyme activity. Typically ultrasound can be used as a processing aid in extraction, crystallisation, freezing, emulsification, filtration and drying.  相似文献   

15.
This paper describes the application of a novel broadband acoustic sensor to evaluating the acoustic emissions from cavitation produced by a typical commercial 20 kHz sonochemical horn processor. Investigations of the reproducibility of the processor, and of the variation in cavitation emissions as a function of output setting and sensor location are described, and resulting trends discussed in terms of the broadband integrated power in the megahertz frequency range. Companion studies with a conventional membrane hydrophone have illustrated for the first time that cavitation emissions produced by a sonochemical horn processor can extend to frequencies beyond 20 MHz, and the sensor shows that significant nonlinearity can be seen in measured cavitation activity with increasing nominal output power.  相似文献   

16.
    
Here, we offer an easy and eco-friendly sonochemical pathway to fabricate Nd2Zr2O7 nanostructures and nanocomposites with the help of Morus nigra extract as a new kind of capping agent. For the first time, the performance of Nd2Zr2O7-based ceramic nanostructure materials has been compared upon NOx abatement. Diverse kinds of techniques have been employed to specify purity and check the attributes of the fabricated Nd2Zr2O7-based nanostructurs by Morus nigra extract. Outcomes revealed the successful fabrication of Nd2Zr2O7 nanostructures and nanocomposites applying Morus nigra extract through sonochemical pathway. All nanostructured samples have been fabricated through ultrasonic probe with power of 60 W (18 KHz). Further, the fabricated Nd2Zr2O7-based ceramic nanostructure materials can be applied as potential nanocatalysts with appropriate performance for propane-SCR-NOx, since the conversion of NOx to N2 for the best sample (Nd2Zr2O7-ZrO2 nanocomposite) was 70%. In addition, in case of Nd2Zr2O7-ZrO2 nanocomposite, the outlet quantity of CO as an unfavorable and unavoidable product was lower than the rest.  相似文献   

17.
    
For the alkaline fuel cell cathode reaction, it is very essential to develop novel catalysts with superior catalytic properties. Here, we report the synthesis of highly active and stable MoS2/Pd composites for the oxygen reduction reaction (ORR), via a simple, eco-friendly sonochemical method. The bulk MoS2 was first transformed into single and few layers MoS2 nanosheets through ultrasonic exfoliation. Then the exfoliated MoS2 nanosheets served as supporting materials for the nucleation and further in-situ growth of Pd nanoparticles to form MoS2/Pd composites via ultrasonic irradiation. Cyclic voltammetry and rotating disk voltammetry measurements demonstrate that as-prepared MoS2/Pd composites which provides a direct four-electron pathway for the ORR, have better electrocatalytic activity, long-term operation stability than commercial Pt/C catalyst. We expect that the present work would provide a promising strategy for the development of efficient oxygen reduction electrocatalyst. In addition, this study can also be extended to the preparation of other hybrid with desirable morphologies and functions.  相似文献   

18.
    
This works is focused on the treatment by sono-electrolysis of the liquid effluents produced during the Surfactant-Aided Soil-Washing (SASW) of soils spiked with herbicide oxyfluorfen. Results show that this combined technology is very efficient and attains the complete mineralization of the waste, regardless of the surfactant/soil radio applied in the SASW process (which is the main parameter of the soil remediation process and leads to very different wastes). Both the surfactant and the herbicide are completely degraded, even when single electrolysis is used; and only two intermediates are detected by HPLC in very low concentrations. Conversely, the efficiency of single sonolysis approach, for the oxidation of pollutant, is very low and just small changes in the herbicides and surfactant concentrations are observed during the tests carried out. Sono-electrolysis with diamond electrodes achieved higher degradation rates than those obtained by single sonolysis and/or single electrolysis with diamond anodes. A key role of sulfate is developed, when it is released after the electrochemical degradation of surfactant. The efficient catalytic effect observed which can be explained by the anodic formation of persulfate and the later, a sono-activation is attained to produce highly efficient sulfate radicals. The effect of irradiating US is more importantly observed in the pesticide than in the surfactant, in agreement with the well-known behavior of these radicals which are known to oxidize more efficiently aromatic compounds than aliphatic species.  相似文献   

19.
    
The dynamics of a bubble near a corner formed by two flat rigid boundaries (walls), is studied experimentally using a spark-generated bubble. The expansion, collapse, rebound, re-collapse and migration of the bubble, along with jetting and protrusion, are captured using a high-speed camera. Our experimental observations reveal the behaviour of the bubble in terms of the corner angle and the dimensionless standoff distances to the near and far walls in terms of the maximum bubble radius. The bubble remains approximately spherical during expansion except for its surface becoming flattened when in close proximity to a wall. When a bubble is initiated at the bisector of the two walls, the bubble becomes oblate along the bisector during the late stages of collapse. A jet forms towards the end of collapse, pointing to the corner. The closer the bubble to the two walls, the more oblate along the bisector the bubble becomes, and the wider the jet. A bubble initiated near one of the two walls is mainly influenced by the nearer wall. The jet formed is pointing to the near wall but inclined towards the corner. After the jet penetrates through the bubble surface, the bubble becomes a bubble ring, and a bubble protrusion forms following the jet. The bubble ring collapses and subsequently disappears, while the protrusion firstly expands, and then collapses and migrates to the corner.  相似文献   

20.
激光驱动冲击波在铝-金阻抗匹配靶中的传播稳定性   总被引:1,自引:2,他引:1  
 针对神光Ⅱ第九路激光条件,利用1维JB程序和多台阶靶技术对冲击波在铝 金阻抗匹配靶中的传播稳定性进行了理论和实验研究,实验结果与理论结果基本吻合。结果表明,激光驱动冲击波在铝 金阻抗匹配靶中传播时,高阻抗待测材料金中的冲击波稳定传播最大距离急剧减小。因此,在进行铝-金阻抗匹配靶物理参数设计时,应保证高阻抗材料金台阶厚度满足冲击波传播稳定性,然后再按照阻抗匹配实验中两种材料的冲击波速度比来确定低阻抗标准材料铝的台阶厚度。根据神光Ⅱ第九路激光条件,铝-金阻抗匹配靶中铝基底厚度选取为30 μm左右较好,金台阶和铝台阶厚度应分别小于10 μm和17 μm。  相似文献   

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