Nanoemulsification of soybean oil using ultrasonic microreactor: Process optimization,scale-up and numbering-up in series

Ultrasonically-induced nanoemulsions have been widely investigated for the development of functional food, cosmetics, and pharmaceuticals due to ideal droplet sizes (DS), low polydispersity index (PDI), and superior physical stability. However, a series of frequently-used ultrasonic set-ups mainly suffered from a low ultrasonic energy efficiency caused by the large acoustic impedance and energy consumption, subordinately confronted with a low throughput, complicated fabrication with complex structure and weak ultrasonic cavitation. Herein, we employed a typical ultrasonic microreactor (USMR) that ensured the high-efficient energy input and generated intense cavitation behavior for efficient breakage of droplets and continuous production of unified oil-in-water (O/W) nanoemulsions in a single cycle and without any pre-emulsification treatment. The emulsification was optimized by tuning the formula indexes, technological parameters, and numerical analysis using Response Surface Methodology (RSM), followed by a comparison with the emulsification by a traditional ultrasonic probe. The USMR exhibited superior emulsification efficiency and easy scale-up with remarkable uniformity by series mode. In addition, concurrent and uniform nanoemulsions with high throughput could also be achieved by a larger USMR with high ultrasonic power. Based on RSM analysis, uniform DS and PDI of 96.4 nm and 0.195 were observed under the optimal conditions, respectively, well consistent with the predicted values. Impressively, the optimal nanoemulsions have a uniform spherical morphology and exhibited superior stability, which held well in 45 days at 4℃ and 25℃. The results in the present work may provide a typical paradigm for the preparation of functional nanomaterials based on the novel and efficient emulsification tools.     

Ultrasound-assisted sequentially precipitated nickel-silica catalysts and its application in the partial hydrogenation of edible oil

Sequentially precipitated Mg-promoted nickel-silica catalysts with ageing performed under various ultrasonic intensities were employed to study the catalyst performance in the partial hydrogenation of sunflower oil. Results from various characterisation studies showed that increasing ultrasonic intensity caused a higher degree of hydroxycarbonate erosion and suppressed the formation of Ni silicates and silica support, which improved Ni dispersion, BET surface area and catalyst reducibility. Growth of silica clusters on the catalyst aggregates were observed in the absence of ultrasonication, which explained the higher silica and nickel silicate content on the outer surface of the catalyst particle. Application of ultrasound also altered the electron density of the Ni species, which led to higher activity and enhanced product selectivity for sonicated catalysts. The catalyst synthesised with ultrasonic intensity of 20.78 Wcm⁻² achieved 22.6% increase in hydrogenation activity, along with 28.5% decrease in trans-C18:1 yield at IV = 70, thus supporting the feasibility of such technique.     

Effect of ultrasound on the preparation of soy protein isolate-maltodextrin embedded hemp seed oil microcapsules and the establishment of oxidation kinetics models

In this study, microcapsules were prepared by spray drying and embedding hemp seed oil (HSO) with soy protein isolate (SPI) and maltodextrin (MD) as wall materials. The effect of ultrasonic power on the microstructure and characteristics of the composite emulsion and microcapsules was studied. Studies have shown that ultrasonic power has a significant impact on the stability of composite emulsions. The particle size of the composite emulsion after 450 W ultrasonic treatment was significantly lower than the particle size of the emulsion without the ultrasonic treatment. Through fluorescence microscopy observation, HSO was found to be successfully embedded in the wall materials to form an oil/water (O/W) composite emulsion. The spray-dried microcapsules showed a smooth spherical structure through scanning electron microscopy (SEM), and the particle size was 10.7 μm at 450 W. Fourier transform infrared (FTIR) spectroscopy analysis found that ultrasonic treatment would increase the degree of covalent bonding of the SPI-MD complex to a certain extent, thereby improving the stability and embedding effect of the microcapsules. Finally, oxidation kinetics models of HSO and HSO microcapsules were constructed and verified. The zero-order model of HSO microcapsules was found to have a higher degree of fit; after verification, the model can better reflect the quality changes of HSO microcapsules during storage.     

Physicochemical properties and microstructure of composite surimi gels: The effects of ultrasonic treatment and olive oil concentration

This study was conducted to evaluate the effects of extra virgin olive (EVO) oil incorporation on the physicochemical properties and microstructure of surimi gels subjected to ultrasound-assisted water-bath heating. As the oil content was increased from 0 to 5 g/100 g, the breaking force and gel strength of the surimi gels significantly decreased, while the whiteness level exhibited the opposite tendency irrespective of the heating method. Compared with the traditional water-bath heating method, the ultrasonic heating promoted the unfolding of the α-helix structure and intensified the formation of β-sheet content and non-covalent bonds (ionic bonds, hydrogen bonds, and disulfide bonds), especially disulfide bonds, which contributed to the further crosslinking of the proteins and to gelation, thereby improving the gels’ strength. In addition, smaller cavities and compact microstructures were observed in the low-oil (≤3 g/100 g) surimi gels under ultrasonic treatment, which effectively prevented water migration in the gel network and resulted in a high water holding capacity and uniform water distribution. However, the ultrasonic treatment barely remedied the poor microstructures of the high-oil (>3 g/100 g) surimi gels owing to oil coalescence, which weakened the protein–protein interaction. In conclusion, ultrasonic treatment combined with water-bath heating significantly improved the gelation properties of the low-oil surimi gels, although it did not remarkably improve those of the high-oil gels. The choice of a suitable oil concentration could be of great importance for the production and functioning of surimi products via ultrasound-assisted treatments.     

Ultrasonic-assisted preparation of eucalyptus oil nanoemulsion: Process optimization,in vitro digestive stability,and anti-Escherichia coli activity

Eucalyptus oil (EO) is a natural and effective antimicrobial agent; however, it has disadvantages such as poor water solubility and instability. The aim of this study was to investigate the effect of process vessels and preparation process parameters on the particle size of the emulsion droplets using ultrasonic technique and response surface methodology to prepare eucalyptus oil nanoemulsion (EONE). The optimal sonication process parameters in conical centrifuge tubes were confirmed: sonication distance of 0.9 cm, sonication amplitude of 18%, and sonication time of 2 min. Under these conditions, the particle size of EONE was 18.96 ± 4.66 nm, the polydispersity index was 0.39 ± 0.09, and the zeta potential was −31.17 ± 2.15 mV. In addition, the changes in particle size, potential, micromorphology, and anti-Escherichia coli activity of EONE during digestion were investigated by in vitro simulated digestion. The emulsion was stable in simulated salivary fluid, tended to aggregate in simulated gastric fluid, and increased in particle size and potential value in simulated intestinal fluid. EONE showed higher anti-E. coli activity than EO by simulated digestion. These results provide a useful reference for the in vivo antimicrobial application of the essential oil.     

Study on the emulsification and oxidative stability of ovalbumin-pectin-pumpkin seed oil emulsions using ovalbumin solution prepared by ultrasound

Pumpkin seed oil (PSO), which is a valuable compound with high nutritional value used for the prevention of various chronic diseases, is prone to oxidation. In this work, small and uniform (su) ovalbumin (OVA) and pectin (PEC) were used to stabilize PSO in the form of an emulsion. The results showed that suOVA-PEC-PSO emulsion with a droplet size of 9.82 ± 0.05 μm was successfully self-assembled from PSO, PEC, and suOVA solution (with a droplet size of 230.13 ± 14.10 nm) treated with 300 W ultrasound, owing to the formation of a more stable interfacial film on the surface of droplets. The interfacial, rheological, emulsifying, and antioxidant properties of the suOVA-PES-PSO emulsions were excellent, owing to the synergistic effects between PEC and suOVA solution. Moreover, the physical stability of the suOVA-PEC-PSO emulsions to salt stress, a freeze-thaw cycle, and heat treatment was also increased and the oxidation of linolenic acid was notably delayed. These results have extended the food-related applications of OVA and PSO, and provide a promising foundation for further exploration of the self-assembly of composite emulsions by small and uniform proteins.     

Ultrasound assisted preparation of water in oil emulsions and their application in arsenic (V) removal from water in an emulsion liquid membrane process

Water in oil emulsions are prepared by using an ultra-sonication device and used in an emulsion liquid membrane process in order to recover arsenic (V) ions from an aqueous medium. The aim of this work is the investigation of the effect of emulsifier concentration and composition, and also sonication time on the emulsion droplet size and the extraction efficiency in order to obtain stable emulsions with small droplets that favor the extraction. Results show that ultrasonic waves reduce internal droplet size which enhances the extraction of arsenic. In addition, internal droplet size is decreased initially and then increased by increasing Span 80 concentration. On the other hand, by increasing Span 80 concentration, extraction amount is increased and then decreased. Furthermore, emulsifier blends provide more stability for the emulsion. Increasing concentration of Tween 20 as a hydrophilic emulsifier up to an optimum concentration decreases internal droplet size and increases extraction amount. By increasing sonication time up to 4 min, the internal droplet size is decreased and the extraction amount is increased. If sonication time is increased further, the internal droplet size is increased and the extraction amount is decreased.     

Ultrasound pre-fractured casein and in-situ formation of high internal phase emulsions

Traditional preparation of protein particles is usually complex and tedious, which is a major issue in the development of Pickering high internal phase emulsions (HIPEs). In this study, a facile and in-situ method for the preparation of food-grade Pickering HIPEs was developed using ultrasound pre-fractured casein flocs. The ultrasonic-treated casein protein and resulting Pickering HIPEs were characterised using particle size distribution, confocal laser scanning microscopy (CLSM), cryo-SEM, and rheological measurement. The results indicated that pH values of casein and ultrasonic power level were key parameters for casein protein dispersion into nanoparticles to form o/w Pickering HIPEs. In optimal conditions, the hexagons of emulsion droplets were close together, and the emulsions formed with ultrasonic caseins exhibited gel-like behaviour. Additionally, ultrasonic microscale-sized caseins (about 25 μm) disappeared upon the use of high speed homogenisation during the formation of HIPEs, while the chemical distribution revealed by confocal laser scanning microscopy indicated that the dispersive nanoparticles from casein proteins were evidently absorbed on the interface of HIPEs (cryo-SEM). These findings prove that ultrasound is an effective tool to loosen casein flocs to induce the in-situ formation of stabilised Pickering HIPEs. Overall, this work provides a green and facile route to convert edible oil into a soft solid, which has great potential for applications in biomedical materials, 3D printing technology, and various cosmetics.     

Experimental studies on the effect of ultrasonic treatment and hydrogen donors on residual oil characteristics

Residual oil, the residue after the distillation of crude oil, imposes deleterious effects on refinery due to its high viscosity and asphaltene content. In this context, ultrasonic technology has been widely applied in refining processes given its high efficiency and minimal environmental impacts. To guide the selection of operation parameters, in this work, we probed the effect of treatment duration, power, and hydrogen donor on the characteristics of residual oil under ultrasonic treatments. Underlying mechanisms of ultrasonic treatments, in the absence and presence of hydrogen donors, were verified through systematically analyzing viscosity, component conversion, molecular weight, hydrogen distribution, and functional groups of residual oil. While viscosity reductions under low-power density treatment are caused by colloidal system disaggregation, high-power density treatment can bring in both chemical bond cleavage and colloidal system disaggregation. In addition, adding hydrogen donor can effectively prevent radical recombination, and thus increases the yield of saturate. These results provide fundamental understandings on the effects of ultrasonic treatments.     

Effect of ultrasound on the structural characteristics and oxidative stability of walnut oil oleogel coated with soy protein isolate-phosphatidylserine

In this study, the three-dimensional network system formed by rice bran wax (RBW) was used as the internal structure, and the external structure formed by soybean protein isolate (SPI) and phosphatidylserine (PS) was added on the basis of the internal structure to prepare walnut oil oleogel (SPI-PS-WOG). Ultrasonic treatment was applied to the mixed solution to make SPI-PS-WOG, on the basis, the effects of ultrasonic treatment on SPI-PS-WOG were investigated. The results showed that both β and β’ crystalline forms were present in all SPI-PS-WOG samples. When the ultrasonic power was 450 W, the first weight loss peak in the thermogravimetric (TGA) curve appeared at 326 °C, which was shifted to the right compared to the peak that occurred when the ultrasonic power was 0 W, indicating that the thermal stability of the SPI-PS-WOG was improved by the ultrasonic treatment. Moreover, when the ultrasonic power was 450 W, the oil holding capacity (OHC) reached 95.3 %, which was the best compared with other groups. Both confocal laser scanning microscopy (CLSM) and scanning electron microscopy (SEM) showed that the ultrasonic treatment of appropriate power succeeded in making the SPI-PS-WOG samples more evenly dispersed in the internal structure and denser in the external structure. In terms of oxidative stability, it was found that the peroxide value of SPI-PS-WOG remained at 9.8 mmol/kg oil for 50 days under 450 W ultrasonic power treatment, which was significantly improved compared with liquid walnut oil (WO). These results provide a new idea for the preparation of oleogels, and also lay a theoretical foundation for the application of ultrasonic treatment in oleogels.     

Ultrasound-assisted desalination of crude oil: The influence of mixing extent,crude oil species,chemical demulsifier and operation variables

Coalescence of water droplets in crude oil has been effectively promoted by chemical demulsifiers integrated with ultrasound. Temporary images of water droplets in W/O emulsions were directly monitored using a metallurgical microscope. Water droplets achieved expansion of 118% at 40 min ultrasonic irradiation time under well mixing conditions. However, water droplets in heavy crude oil undergo less aggregation than those in light crude oil, due to resistance of mobility in highly viscous fluid. In the absence of chemical demulsifiers, water droplets enveloped by native surfactants appeared to aggregate arduously because of occurrence of interfacial tension gradients. Influential significance analyses have been executed by a factorial design method on operation variables, including acoustic power intensity, operation temperature, ultrasonic irradiation time and chemical demulsifier dosages. In this work, the outcomes indicate that the optimal operating conditions for desalination of crude oil assisted by ultrasound were as follows: acoustic power intensity = 300 W, operation temperature = 90℃, ultrasonic irradiation time = 75 min and chemical demulsifier dosages = 54 mg/L. Besides, it was found that the most influential importance of operation parameter was temperature, followed with acoustic power intensity, ultrasonic irradiation time and chemical demulsifier dosages.     

声空化工程初步*

声空化气泡内的高温、高压和高密度是声空化工程的机理和基础。该文简要回顾了国内外声空化理论和实验研究的进展,针对当前在液体中进行工业规模声处理等声能应用方面的现状和存在的问题,提出了扩大声能应用的一种可能途径——声空化空间分布控制并在实验室内进行了实验研究。结果表明该方法具有可行性。在此基础上,文中给出了基于空化空间分布控制方法在稠油井口辅助降粘和高固污泥预处理方面取得声空化工程初步应用的两个例子。现场的试验结果表明,这两种声空化工程化样机在实际现场工况条件下,均取得了较好的应用效果。最后,对当前声空化工程应用前景进行了初步探讨。     

Applying ultrasonic fields to separate water contained in medium-gravity crude oil emulsions and determining crude oil adhesion coefficients

Separating produced water is a key part of production processing for most crude oils. It is required for quality reasons, and to avoid unnecessary transportation costs and prevent pipework corrosion rates caused by soluble salts present in the water. A complicating factor is that water is often present in crude oil in the form of emulsions. Experiments were performed to evaluate the performance of ultrasonic fields in demulsifying crude oil emulsions using novel pipe-form equipment. A horn-type piezoelectric ultrasonic transducer with a frequency of 20 kHz and power ranging from 80 W to 1000 W was used for experimental purposes. The influences of the intensity of ultrasonic fields, ultrasonic irradiation time, and the initial water content of crude oils were evaluated to establish the rate of water segregation from oil. The experiments applied ultrasonic-field intensities of $0.25$ W/cm³, $0.5$ W/cm³, $0.75$ W/cm³ and $1$ W/cm³ to synthetic emulsions with 10%, 15%, 20%, and 25% of the water in crude oil. Crude oil demulsification occurred for each ultrasonic field intensity tested for all the samples tested. Function β involving adhesion coefficients was expressed in terms of wave-field intensity and initial concentration of water in each of the three crude oil samples tested. The experiments demonstrated that despite the absence of any chemical demulsifier involved, water separation caused by applying ultrasonic fields was effective and occurred rapidly. As the intensity of the ultrasonic field applied increased, the amount of water segregated from crude oil also increased. Subjected to constant field intensity, higher initial water cuts (up to 15% or so) in the crude oil samples and higher ultrasonic irradiation times, resulted in greater segregation of water from crude oil in percentage terms. However, in samples with initial water cuts of 20+% long irradiation times (~5 min), resulted in a decline in water separation compared to 2-min tests. Ultrasonic field treatments offer commercially-viable and environmentally-friendly alternatives to treatments using chemical demulsifiers as they reduce desalination requirements of wastewater.     

Application and mechanism of ultrasonic static mixer in heavy oil viscosity reduction

In the present study, heavy oil viscosity reduction in Daqing oil field was investigated by using an ultrasonic static mixer. The influence of the ultrasonic power on the viscosity reduction rate was investigated and the optimal technological conditions were determined for the ultrasonic treatment. The mechanism for ultrasonic viscosity reduction was analyzed. The flow characteristics of heavy oil in the mixer under the effect of cavitation were investigated using numerical modeling, and energy consumptions were calculated during the ultrasonic treatment and vis-breaking processes. The experimental results indicated that the ultrasonic power made the largest impact on the viscosity reduction rate, followed by the reaction time and temperature. The highest viscosity reduction rate was 57.34%. Vacuole was migrated from the axis to the wall along the fluid, accelerating the two-phase transmission and enhancing the radial flow of the fluid, which significantly improved the ultrasonic viscosity reduction. Compared to the vis-breaking process, the energy consumption of ultrasonic treatment process was 43.03% lower when dealing with the same quality heavy oil. The optimal process conditions were found to be as follows: ultrasonic power of 1.8 kW, reaction time of 45 min and reaction temperature of 360 °C. The dissociation of the molecules of heavy oil after ultrasonication has been checked. After being kept at room temperature 12 days, some light components were produced by the cavitation cracking, so the viscosity of the residual oil could not return to that of the original residual oil, which meant that the “cage effect” was not reformed.     

Exploring the influence of ultrasound on the antibacterial emulsification stability of lysozyme-oregano essential oil

A lysozyme-oregano essential oil (Lys-OEO) antibacterial emulsion was developed via ultrasonic treatment. Based on the general emulsion materials of ovalbumin (OVA) and inulin (IN), the addition of Lys and OEO successfully inhibited the growth of E. coli and S. aureus, two representatives of which were Gram-negative and Gram-positive bacteria respectively. The emulsion system in this study was designed to compensate for the limitation that Lys could only act on Gram-positive bacteria, and the stability of the emulsion was improved using ultrasonic treatment. The optimal amounts among OVA, Lys and OEO were found to be the mass ratio of 1:1 (Lys to OVA) and 20% (w/w) OEO. The ultrasonic treatment at the power of 200, 400, 600, and 800 W and time length of 10 min improved the stability of emulsion, in which the surface tension was below 6.04 mN/m and the Turbiscan stability index (TSI) did not exceed 10. The multiple light scattering showed that sonicated emulsions were less prone to delamination; salt stability and pH stability of emulsions were improved, CLSM image showed emulsion as oil-in-water type. In the meantime, the particles of the emulsions were found to become smaller and more uniform with ultrasonic treatment. The best dispersion and stability of the emulsion were both achieved at 600 W with a zeta potential of 7.7 mV, the smallest particle size and the most uniform particle distribution.     

声速和衰减系数与含蜡原油特性的关系

当含蜡原油的温度低于蜡的析出温度后,蜡晶将不断析出并相互交联成网状结构,若网状结构达到一定强度,原油将失去流动而凝结。在该过程中不仅含蜡原油的流动特性发生变化,原油的声速和衰减系数也发生变化。本研究结果表明：含蜡原油的超速及衰减系数均随温度降低而增大;含蜡原油在凝结温度前后表现出不同的声速与温度的对应关系;含蜡原油在凝结后的声速的温度的关系同原油的含蜡量有关;含蜡原油的衰减系数在接近凝结温度时急剧     

Effect of high-intensity ultrasonic treatment on the emulsion of hemp seed oil stabilized with hemp seed protein

In this study, hemp seed oil (HSO) emulsions stabilized with hemp seed protein (HPI) were prepared and treated with high intensity ultrasonic (HIU). The effects of different treatment powers (0, 150, 300, 450, 600 W) on the properties, microstructure and stability of emulsions were investigated. HIU-treated emulsions showed improved emulsifying activity index and emulsifying stability index, reduced particle size, and increased absolute values of ζ-potential, with the extreme points of these indices occurring at a treatment power of 450 W. Here, the emulsion showed the best dispersion and the smallest particle size in fluorescence microscopy observation, with the highest adsorbed protein content (30.12%), and the highest tetrahydrocannabinol (THC) retention rate (87.64%). The best thermal and oxidative stability of the emulsions were obtained under HIU treatment with a power of 450 W. The D₄₃ and the peroxide values (POV) values after 30 d storage were the smallest at 985.74 ± 64.89 nm and 4.6 μmol/L, respectively. Therefore, 450 W was optimal HIU power to effectively improve the properties of HPI-stabilized HSO emulsion and promote the application of HSO and its derivatives in food processing production.     

Suspension characteristics of water droplet in oil under ultrasonic standing waves

The suspension characteristics of water droplet in oil were investigated under ultrasonic standing waves with high-speed photography in this paper. Firstly, the suspension position of droplet was predicted by theoretical derivation. The motion trajectory of droplet was captured and a kinetic analysis was applied to characterize the suspension position of droplet. The effects of droplet size, acoustic pressure, frequency, as well as density ratio of water and oil on the suspension position of droplet were analyzed in details. It was proved that the droplet size had little effect on the suspension position at different frequencies. The suspension zone approached minimum at 39.4 kHz, and the suspension position of droplet was insensitive to acoustic pressure amplitude and density ratio at this frequency. These would be advantageous to maintain the stability of droplet banding and shorten the width of banding. In addition, it was proved that the suspension position of droplet is approximately linear with the density ratio at different frequencies.     

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.     

Ultrasound-assisted production and optimization of mini-emulsions in a microfluidic chip in continuous-flow

The use of ultrasound to generate mini-emulsions (50 nm to 1 μm in diameter) and nanoemulsions (mean droplet diameter < 200 nm) is of great relevance in drug delivery, particle synthesis and cosmetic and food industries. Therefore, it is desirable to develop new strategies to obtain new formulations faster and with less reagent consumption. Here, we present a polydimethylsiloxane (PDMS)-based microfluidic device that generates oil-in-water or water-in-oil mini-emulsions in continuous flow employing ultrasound as the driving force. A Langevin piezoelectric attached to the same glass slide as the microdevice provides enough power to create mini-emulsions in a single cycle and without reagents pre-homogenization. By introducing independently four different fluids into the microfluidic platform, it is possible to gradually modify the composition of oil, water and two different surfactants, to determine the most favorable formulation for minimizing droplet diameter and polydispersity, employing less than 500 µL of reagents. It was found that cavitation bubbles are the most important mechanism underlying emulsions formation in the microchannels and that degassing of the aqueous phase before its introduction to the device can be an important factor for reduction of droplet polydispersity. This idea is demonstrated by synthetizing solid polymeric particles with a narrow size distribution starting from a mini-emulsion produced by the device.