In this work, the effects of thickeners and tonicity towards producing stable palm oil-based water-in-oil-in-water (W/O/W) multiple nanoemulsion using ultrasound and microfluidizer were investigated. Palm oil, Sucragel, polyglycerol polyricinoleate, Tween 80, Xanthan gum, and NaCl were used. W/O/W was formed under the optimized conditions of ultrasound at 40% amplitude and for 180 s of irradiation time, whereas for the microfluidizer, the optimized conditions were 350 bar and 8 cycles. This is the first work that successfully utilized Sucragel (oil-based thickener) in imparting enhanced stability in W/O/W. W/O/W with isotonic stabilization produced the lowest change in the mean droplet diameter (MDD), NaCl concentration, and water content by 1.5%, 2.6%, and 0.4%, respectively, due to reduced water movement. The final optimized W/O/W possessed MDD and dispersity index of 175.5 ± 9.8 and 0.232 ± 0.012, respectively. The future direction of formulating stable W/O/W would be by employing oil phase thickeners and isotonicity. The observed ~12 times lesser energy consumed by ultrasound than microfluidizer to generate a comparable droplet size of ~235 nm, further confirms its potential in generating the droplets energy-efficiently.
A rapid and green method for the synthesis of novel N-thiazolidine-2,4-dione isoxazoline derivatives 5 from N-allyl-5-arylidenethiazolidine-2,4-diones 3 as dipolarophiles with arylnitrile oxides via 1,3-dipolar cycloaddition reaction. The corresponding N-allyl substituted dipolarophiles were prepared by one-pot method from thiazolidine-2,4-dione with aldehydes using Knoevenagel condensation followed by N-allylation of thiazolidine-2,4-dione in NaOH aqueous solution under sonication. In addition, the isoxazoline derivatives 5 were synthesized by regioselective and chemoselective 1,3-dipolar cycloaddition using inexpensive and mild NaCl/Oxone/Na3PO4 as a Cl source, oxidant and/or catalyst under ultrasonic irradiation in EtOH/H2O (v/v, 2:1) as green solvent. All synthesized products are furnished in good yields in the short reaction time, and then their structures were confirmed by NMR, mass spectrometry and X-ray crystallography analysis.
The leaf extract of a medicinally important plant, watercress (Nasturtium officinale), was obtained through an ultrasound-facilitated method and utilized for the preparation of ZnO nanoparticles via a joint ultrasound-microwave assisted procedure. The characteristics of the extract enriched nanoparticles (Ext/ZnO) were determined by SEM, TEM, XRD, EDX, BET, FTIR, TGA, and UV-Vis DRS analyses and compared to that of ZnO prepared in the absence of the extract (ZnO). The presence of carbon and carbonaceous bonds, changes in the morphology, size, band gap energy, and weight-decay percentage were a number of differences between ZnO and Ext/ZnO that confirmed the link of extract over nanoparticles. Ext/ZnO, watercress leaf extract, ZnO, and insulin therapies were administrated to treat alloxan-diabetic Wister rats and their healing effectiveness results were compared to one another. The serum levels of the main diabetic indices such as insulin, fasting blood glucose, and lipid profile (total triglyceride, total cholesterol, and high-density lipoprotein cholesterol) were estimated for healthy, diabetic, and the rats rehabilitated with the studied therapeutic agents. The watercress extract-enriched ZnO nanoparticles offered the best performance and suppressed the diabetic status of rats. Moreover, both ZnO samples satisfactory inhibited the activities of Staphylococcus aureus and Escherichia coli bacteria. Based on the results, the application of Nasturtium officinale leaf extract can strongly empower ZnO nanoparticles towards superior antidiabetic and enhanced antibacterial activities.
Response surface methodology (RSM) was used to optimize the formulation of a nanoemulsion for central delivery following parenteral administration. A mixture of medium-chain triglyceride (MCT) and safflower seed oil (SSO) was determined as a sole phase from the emulsification properties. Similarly, a natural surfactant (lecithin) and non-ionic surfactant (Tween 80) (ratio 1:2) were used in the formulation. A central composite design (CCD) with three-factor at five-levels was used to optimize the processing method of high energy ultrasonicator. Effects of pre-sonication ultrasonic intensity (A), sonication time (B), and temperature (C) were studied on the preparation of nanoemulsion loaded with valproic acid. Influence of the aforementioned specifically the effects of the ultrasonic processing parameters on droplet size and polydispersity index were investigated. From the analysis, it was found that the interaction between ultrasonic intensity and sonication time was the most influential factor on the droplet size of nanoemulsion formulated. Ultrasonic intensity (A) significantly affects the polydispersity index value. With this optimization method, a favorable droplet size of a nanoemulsion with reasonable polydispersity index was able to be formulated within a short sonication time. A valproic acid loaded nanoemulsion can be obtained with 60% power intensity for 15 min at 60 °C. Droplet size of 43.21±0.11 nm with polydispersity index of 0.211 were produced. The drug content was then increased to 1.5%. Stability study of nanoemulsion containing 1.5% of valproic acid had a good stability as there are no significant changes in physicochemical aspects such as droplet size and polydispersity index. With the characteristisation study of pH, viscosity, transmission electron microscope (TEM) and stability assessment study the formulated nanoemulsion has the potential to penetrate blood-brain barrier in the treatment of epilepsy.
Mitragyna speciosa, a tropical plant indigenous to Southeast Asia, is well known for its psychoactive properties. Its leaves are traditionally chewed by Thai and Malaysian farmers and manual labourers as it causes a numbing, stimulating effect. The present study aims to evaluate alkaloid yield and composition in the leaf extracts. For this purpose we have compared several non-conventional extraction techniques with classic procedures (room temperature or under heating). Dried M. speciosa leaves belonging to three batches of different origin (from Thailand, Malaysia and Indonesia) were extracted using ultrasound-assisted extraction (UAE), microwave-assisted extraction (MAE) and supercritical carbon dioxide extraction SFE-CO(2), using methanol, ethanol, water and binary mixtures. The extracts were compared using an HPLC/ESI-MS analysis of mitragynine and four other related alkaloids which were present in the alkaloid fraction. The extraction technique influences both the raw product yield and the relative alkaloid content of M. speciosa leaves. Of the several methods tested, MAE in a closed vessel at 110 °C (60 W, methanol/water 1:1) gave the highest alkaloid fraction amount, while UAE with an immersion horn at 25 °C (21.4 kHz, 50 W, methanol) showed the best yield for mitragynine. This work may prove to be a useful contribution to forensic, toxicological and pharmacognosy studies. Although the potential applications of M. speciosa alkaloids clearly need further investigation, these results may facilitate the scaling-up of their extraction.
With rising consumer demand for natural products, a greener and cleaner technology, i.e., ultrasound-assisted extraction, has received immense attention given its effective and rapid isolation for nanocellulose compared to conventional methods. Nevertheless, the application of ultrasound on a commercial scale is limited due to the challenges associated with process optimization, high energy requirement, difficulty in equipment design and process scale-up, safety and regulatory issues. This review aims to narrow the research gap by placing the current research activities into perspectives and highlighting the diversified applications, significant roles, and potentials of ultrasound to ease future developments. In recent years, enhancements have been reported with ultrasound assistance, including a reduction in extraction duration, minimization of the reliance on harmful chemicals, and, most importantly, improved yield and properties of nanocellulose. An extensive review of the strengths and weaknesses of ultrasound-assisted treatments has also been considered. Essentially, the cavitation phenomena enhance the extraction efficiency through an increased mass transfer rate between the substrate and solvent due to the implosion of microbubbles. Optimization of process parameters such as ultrasonic intensity, duration, and frequency have indicated their significance for improved efficiency.
ZnO nanorods were directly grown on four different wires (silver, nickel, copper, and tungsten) using sonochemical method. Zinc nitrate hexahydrate and hexamethylenetetramine (HMT) were used as precursors. Influence of growth parameters such as precursors' concentration and ultrasonic power on the grown nanorods were determined. The results demonstrated that the precursor concentration affected the growth structure and density of the nanorods. The morphology, distribution, and orientation of nanorods changed as the ultrasonic power changed. Nucleation of ZnO nanorods on the wire occurred at lower ultrasonic power and when the power increased, the formation and growth of ZnO nanorods on the wires were initiated. The best morphology, size, distribution, and orientation of the nanorods were observed on the Ag wire. The presence of single crystal nanorod with hexagonal shaped was obtained. This shape indicates that the ZnO nanorods corresponded to the hexagonal wurtzite structure with growth preferential towards the (002) direction.
Optimization of sonochemical method of functionalizing a Silane coupling agent, Amino-Silane on Superparamagnetic Iron Oxide Nanoparticles (SPION) using Central Composite Design is reported. The Amino-Silane is grafted on the SPION in an iced bath environment using a Vibra-Cell 20 kHz ultrasonic irradiator with 13 mm diameter horn. Throughout the experiment amplitude of the ultrasonic device is maintained at 47%. The percentage atomic compositions of various APTES elements which bind to the SPION due to the ultrasonic irradiation were determined using X-ray photoelectron spectrometer (XPS). The influence of ultrasonic irradiation time and amount of APTES required for facile, rapid and effective functionalization of Organo-metallic compound on SPION are optimized. The optimized sonication time and amount of APTES are 8.49 min and 3.40 ml, respectively. The predicted results were validated with experimental data. Using the optimized values APTES were functionalized on the SPION experimentally and the results were compared. The experimental results validate the predicted data. Results show that very minimum sonication time is required for effective grafting of APTES on SPION.
Superparamagnetic iron oxide nanoparticles (SPION) are material of interest for biomedical research and related applications. Recently, several works have reported facile sonochemical method of functionalizing nanoparticles with organic coupling agents. Herein, we present the influence of ultrasonic irradiation on the rate of functionalization of 3-amino propyl triethoxyl silane (APTES) on SPION. The effect of sonication on the process is investigated by varying the sonication period between 1 and 20min. Grafting of the organo-metallic molecules on SPION is demonstrated through FTIR and XPS. The results show that in one minute, organo-silane compound can be functionalized onto SPION through unique conditions generated from ultrasonic irradiation. The XPS survey spectra of the as-synthesized APTES-SPION at different sonication periods revealed that absorbed energy due to silanization reactions in all the samples appeared at same peaks. The percentage atomic concentrations of all the elements present in the as-synthesized APTES-SPION are determined by the software CASAXPS. The result demonstrated that highest percentage atomic concentration is observed at the one minute sonication period.
In the field of ultrasonic emulsification, the formation and cavitation collapse is one major factor contributing to the formation of micro- and nano-sized emulsion droplets. In this work, a series of experiments were conducted to examine the effects of varying the ultrasonic horn's position to the sizes of emulsion droplets formed, in an attempt to compare the influence of the simulated acoustic pressure fields to the experimental results. Results showed that the intensity of the acoustic pressure played a vital role in the formation of smaller emulsion droplets. Larger areas with acoustic pressure above the cavitation threshold in the water phase have resulted in the formation of smaller emulsion droplets ca. 250 nm and with polydispersity index of 0.2-0.3. Placing the ultrasonic horn at the oil-water interface has hindered the formation of small emulsion droplets, due to the transfer of energy to overcome the interfacial surface tension of oil and water, resulting in a slight reduction in the maximum acoustic pressure, as well as the total area with acoustic pressures above the cavitation threshold. This work has demonstrated the influence of the position of the ultrasonic horn in the oil and water system on the final emulsion droplets formed and can conclude the importance of generating acoustic pressure above the cavitation threshold to achieve small and stable oil-in-water emulsion.
A comprehensive investigation on the effect of ultrasonic frequency and power on the structural transformation of CTABr/NaSal micelles has been carried out. Sonication of this micelle system at various ultrasonic frequencies and power resulted in the formation and separation of two types of micelles. High viscoelastic threadlike micelles of ∼ 2 nm in diameter and several μm in length and tubular micelles possessing a viscosity slightly above that of water with ∼ 30-50 nm diameter and few hundred nm length. The structural transformation of micelles was induced by the shear forces generated during acoustic cavitation. At a fixed acoustic power of 40 W, the structural transformation was found to decrease from 211 to 647 kHz frequency due to the decreasing shear forces generated, as evidenced by rheological measurements and cryo-TEM images. At 355 kHz, an increase in the structural transformation was observed with an increase in acoustic power. These findings provide a knowledge base that could be useful for the manipulation of viscosity of micelles that may have applications in oil industry.
Acoustic cavitation in a liquid medium generates several physical and chemical effects. The oscillation and collapse of cavitation bubbles, driven at low ultrasonic frequencies (e.g., 20 kHz), can generate strong shear forces, microjets, microstreaming and shockwaves. Such strong physical forces have been used in cleaning and flux improvement of ultrafiltration processes. These physical effects have also been shown to deactivate pathogens. The efficiency of deactivation of pathogens is not only dependent on ultrasonic experimental parameters, but also on the properties of the pathogens themselves. Bacteria with thick shell wall are found to be resistant to ultrasonic deactivation process. Some evidence does suggest that the chemical effects (radicals) of acoustic cavitation are also effective in deactivating pathogens. Another aspect of cleaning, namely, purification of water contaminated with organic and inorganic pollutants, has also been discussed in detail. Strong oxidising agents produced within acoustic cavitation bubbles could be used to degrade organic pollutants and convert toxic inorganic pollutants to less harmful substances. The effect of ultrasonic frequency and surface activity of solutes on the sonochemical degradation efficiency has also been discussed in this overview.
Acoustic cavitation and sonochemical reactions play a significant role in various applications of ultrasound. A number of dosimetry methods are in practice to quantify the amount of radicals generated by acoustic cavitation. In this study, hydroxyl radical (OH) yields measured by Weissler, Fricke and terephthalic acid dosimetry methods have been compared to evaluate the validities of these methods using a 490 kHz high frequency sonochemical reactor. The OH yields obtained after 5 min sonication at 490 kHz from Weissler and Fricke dosimetries were 200 µM and 289 µM, respectively. Whereas, the OH yield was found to be very low (8 µM) when terephthalic acid dosimetry was used under similar experimental conditions. While the results agree with those reported by Iida et al. (Microchem. J., 80 (2005) 159), further mechanistic details and interfering reactions have been discussed in this study. For example, the amount of OH determined by the Weissler and Fricke methods may have some uncertainty due to the formation of HO2 in the presence of oxygen. In order to account for the major discrepancy observed with the terephthalic acid dosimetry method, high performance liquid chromatography (HPLC) analysis was performed, where two additional products other than 2-hydroxy terephthalic acid were observed. Electrospray ionization mass spectrometry (ESI-MS) analysis showed the formation of 2,5-dihydroxyterephthalic acid as one of the by-products along with other unidentified by-products. Despite the formation of additional products consuming OH, the reason for a very low OH yield obtained by this dosimetry could not be justified, questioning the applicability of this method, which has been used to quantify OH yields generated not only by acoustic cavitation, but also by other processes such as γ-radiolysis. The authors are hoping that this Opinion Paper may initiate further discussion among researchers working in sonochemistry area that could help resolve the uncertainties around using these dosimetry methods.
The optimisation of the Ultrasound-Assisted Extraction (UAE) method was investigated by employing the Central Composite Rotatable Design (CCRD) of Response Surface Methodology (RSM). The UAE method was based on a simple ultrasound treatment using methanol as the extraction medium to facilitate the cell disruption of Mitragyna speciosa leaves for optimum extraction yield and Total Phenolic Content (TPC). Three different parameters comprising extraction temperature (X1: 25-50 °C), sonication time (X2: 15-50 min), and solvent to solid ratio (X3: 10-30 mL/g), and were selected as the independent variables, while two response variables were selected, namely extraction yield (Y1) and TPC (Y2). Based on the results, the developed quadratic polynomial model correlated with the experimental data is based on the coefficient of determination (R2) of extraction yield (0.9972, p
The utilization of agricultural residues to obtain biocompounds of high-added value has significantly increased in the past decades. The conversion of agro-based residues into valuable products appears to be an economically efficient, environment-friendly, and protracted waste management practice. The implementation of ultrasonic technologies in the conversion of value-added goods from agricultural waste materials through pre-treatment and valorization processes has imparted many advantageous effects including rapid processing, effective process performance, minimization of processing steps, minimal dependency on harmful chemicals, and an increased yield and properties of bio-products. To further enliven the literature and inspire new research investigations, this review covers the comprehensive work including theoretical principles, processes, and potential benefits of ultrasonic treatment technologies to assist the production of bio-products which emphasize the extraction yield and the characteristic of the end-product extracted from agriculture residues. A detailed evaluation of these methods and key aspects impacting their performance as well as the features and shortcomings of each ultrasound-assisted approach is also discussed. This review also addressed some of the challenges associated with using ultrasonic irradiation and proposed several potential techniques to maximize productivity. Understanding the concept of ultrasonication technique allow the academician and industrial practitioners to explore the possibility of applying a greener and sustainable approach of biomass extraction to be translated into higher scale production of commercial products.
Colorectal cancer (CRC) is the most common malignancy and the third primary cause of cancer-related mortalities caused by unhealthy diet, hectic lifestyle, and genetic damage. People aged ≥ 50 are more at risk for CRC. Nowadays, bioactive compounds from plants have been widely studied in preventing CRC because of their anticancer and antioxidant properties. Herein, ultrasound-assisted extraction (UAE) was used to extract the bioactive compounds of Pluchea indica (L.) leaves. The resultant total phenolic content (TPC) and total flavonoid content (TFC) of P. indica (L.) leaves were analyzed using a response surface methodology (RSM). The central composite design was implemented to evaluate the amplitude (10 %-70 %) and treatment time (2-10 min) on both responses, i.e., TPC and TFC of P. indica (L.) leaves. The optimum UAE conditions were observed 40 % amplitude and 6 min of treatment, where the TPC and TFC were 3.26 ± 0.00 mg GAE/g d.w. and 67.58 ± 1.46 mg QE/g d.w., respectively. The optimum P. indica (L.) leaf extract was then screened for its cytotoxicity on the HT-29 colorectal cancer cell line. This extract had strong cytotoxicity with a half-maximal inhibitory concentration value (IC50) of 12 µg/mL. The phytochemical screening of bioactive compounds revealed that the optimal P. indica (L.) leaf extract contains flavonoids, namely, kaempferol 3-[2''',3''',5'''-triacetyl]-alpha-L-arabinofuranosyl-(1->6)-glucoside, myricetin 3-glucoside-7-galactoside, quercetin 3-(3''-sulfatoglucoside), and kaempferol 7,4'-dimethyl ether 3-O-sulfate, which could be good sources for promising anticancer agents. This study employs the RSM approach to utilize UAE for bioactive compounds extraction of P. indica (L.) leaves, identified the specific compounds present in the optimized extract and revealed its potential in preventing CRC.
Nanofluids are promising in many fields, including engineering and medicine. Stability deterioration may be a critical constraint for potential applications of nanofluids. Proper ultrasonication can improve the stability, and possibility of the safe use of nanofluids in different applications. In this study, stability properties of TiO2-H2O nanofluid for varying ultrasonication durations were tested. The nanofluids were prepared through two-step method; and electron microscopies, with particle size distribution and zeta potential analyses were conducted for the evaluation of their stability. Results showed the positive impact of ultrasonication on nanofluid dispersion properties up to some extent. Ultrasonication longer than 150min resulted in re-agglomeration of nanoparticles. Therefore, ultrasonication for 150min was the optimum period yielding highest stability. A regression analysis was also done in order to relate the average cluster size and ultrasonication time to zeta potential. It can be concluded that performing analytical imaging and colloidal property evaluation during and after the sample preparation leads to reliable insights.
Hydrodeoxygenation is one of the promising technologies for the transformation of triglycerides into long-chain hydrocarbon fuel commonly known as green diesel. The hydrodeoxygenation (HDO) of rubber seed oil into diesel range (C15-C18) hydrocarbon over non-sulphided bimetallic (Ni-Mo/γ-Al2O3 solid catalysts were studied. The catalysts were synthesized via wet impregnation method as well as sonochemical method. The synthesized catalysts were subjected to characterization methods including FESEM coupled with EDX, XRD, BET, TEM, XPS, NH3-TPD, CO-chemisorption and H2-TPR in order to investigate the effects of ultrasound irradiations on physicochemical properties of the catalyst. All the catalysts were tested for HDO reaction at 350 °C, 35 bar, H2/oil 1000 N (cm3/cm3) and WHSV = 1 h-1 in fixed bed tubular reactor. The catalyst prepared via sonochemical method showed comparatively higher specific surface area, particles in nano-size and uniform distribution of particle on the external surface of the support, higher crystallinity and lower reduction temperature as well as higher concentration of Mo4+ deoxygenating metal species. These physicochemical properties improved the catalytic activity compared to conventionally synthesized catalyst for HDO of rubber seed oil. The catalytic performance of sonochemically synthesized Ni-Mo/γ-Al2O3 catalyst (80.87%) was higher than the catalyst prepared via wet impregnation method (63.3%). The sonochemically synthesized Ni-Mo/γ-Al2O3 catalyst is found to be active, produces 80.87 wt% of diesel range hydrocarbons, and it gives high selectivity for Pentadecane (18.7 wt%), Hexadecane (16.65 wt%), Heptadecane (24.45 wt%) and Octadecane (21.0 wt%). The product distribution revealed that the deoxygenation reaction pathway was preferred. Higher conversion and higher HDO yield in this study are associated mainly with the change in concentration ratio between oxidation states of molybdenum (Mo4+, Mo5+, and Mo6+) on the external surface of the catalyst due to ultrasound irradiation during the synthesis process. Consequently, the application of sonochemically synthesized non-sulphided catalysts favored mainly hydrodeoxygenation of diesel range hydrocarbon.
In this study, high-frequency ultrasound wave (1.8 MHz) at low intensity was applied to improve activated sludge settleability at high MLSS concentration. The effect of irradiation intensity, sonication mode, MLSS concentration and sample volume on the physical characteristics of sludge in a pilot scale settling column were investigated for optimizing the conditions. The obtained results showed that high-frequency ultrasound decreased the height of sludge (44%) and effluent turbidity (82.2%) and increased sludge settling velocity about 3 times at high biomass concentration. Irradiation intensity of 0.4 w/cm2 and sonication mode with interval times of 10 s showed the best results on the performance of the system at MLSS concentration of 8000 mg/L with a sample volume of 3 L.
The ability of sonication phenomena in facilitating separation of azeotropic mixtures presents a promising approach for the development of more intensified and efficient distillation systems than conventional ones. To expedite the much-needed development, a mathematical model of the system based on conservation principles, vapor-liquid equilibrium and sonochemistry was developed in this study. The model that was founded on a single stage vapor-liquid equilibrium system and enhanced with ultrasonic waves was coded using MATLAB simulator and validated with experimental data for ethanol-ethyl acetate mixture. The effects of both ultrasonic frequency and intensity on the relative volatility and azeotropic point were examined, and the optimal conditions were obtained using genetic algorithm. The experimental data validated the model with a reasonable accuracy. The results of this study revealed that the azeotropic point of the mixture can be totally eliminated with the right combination of sonication parameters and this can be utilized in facilitating design efforts towards establishing a workable ultrasonically intensified distillation system.