Ultrafiltration has been proven to be very effective in the treatment of oil-in-water emulsions, since no chemical additives are required. However, ultrafiltration has its limitations, the main limits are concentration polarization resulting to permeate flux decline with time. Adsorption, accumulation of oil and particles on the membrane surface which causes fouling of the membrane. Studies have shown that the ultrasonic is effective in cleaning of fouled membrane and enhancing membrane filtration performance. But the effectiveness also, depends on the selection of appropriate membrane material, membrane geometry, ultrasonic module design, operational and processing condition. In this study, a hollow and flat-sheet polyurethane (PU) membranes synthesized with different additives and solvent were used and their performance evaluated with oil-in-water emulsion. The steady-state permeate flux and the rejection of oil in percentage (%) at two different modes were determined. A dry/wet spinning technique was used to fabricate the flat-sheet and hollow fibre membrane (HFMs) using Polyethersulfone (PES) polymer base, Polyvinylpyrrolidone (PVP) additive and N, N-Dimethylacetamide (DMAc) solvent. Ultrasonic assisted cross-flow ultrafiltration module was built to avoid loss of ultrasonic to the surrounding. The polyurethane (PU) was synthesized by polymerization and sulphonation to have an anionic group (-OH; -COOH; and -SO3H) on the membrane surface. Changes in morphological properties of the membrane had a significant effect on the permeate flow rate and oil removal. Generation of cavitation and Brownian motion by the ultrasonic were the dominant mechanisms responsible for ultrafiltration by cracking the cake layers and reducing concentration polarization at the membrane surface. The percentage of oil after ultrafiltration process with ultrasonic is about 90% compared to 49% without ultrasonic. Ultrasonic is effective in enhancing the membrane permeate flux and controlling membrane fouling.
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 work, sonication (20-kHz) was conducted to assist the biosorption of phenolics from blueberry pomace extracts by brewery waste yeast biomass. The adsorption capacity of yeast increased markedly under ultrasonic fields. After sonication at 394.2 W/L and 40 °C for 120 min, the adsorption capacity was increased by 62.7% compared with that under reciprocating shaking. An artificial neural network was used to model and visualize the effects of different parameters on yeast biosorption capacity. Both biosorption time and acoustic energy density had positive influences on yeast biosorption capacity, whereas no clear influence of temperature on biosorption process was observed. Regarding the mechanism of ultrasound-enhanced biosorption process, the amino and carboxyl groups in yeast were considered to be associated with the yeast biosorption property. Meanwhile, ultrasound promoted the decline of the structure order of yeast cells induced by phenolic uptake. The interactions between yeast cells and phenolics were also affected by the structures of phenolics. Moreover, the mass transfer process was simulated by a surface diffusional model considering the ultrasound-induced yeast cell disruption. The modeling results showed that the external mass transfer coefficient in liquid phase and the surface diffusion coefficient under sonication at 394.2 W/L and 40 °C were 128.5% and 74.3% higher than that under reciprocating shaking, respectively.
A novel organic-inorganic nile-blue - CeO2 (CeO2/NB) nanohybrid has been synthesized by environmentally benign ultrasonic irradiation method for the selective determination of the environmental pollutant, carcinogenic hydrazine (HZ) in environmental water samples. Hydrophobic dyes have generally been as redox mediators in electrochemical sensors fabrication due to strong electron transfer capacity and they would allow the oxidation and reduction of the analytes at lower potentials. The CeO2 nanoparticles were initially synthesized by the ultrasonic irradiation of Ce(NO3)2, NH4OH and ethylene glycol mixture for 6 h using probe sonicator (20 kHz, 100 W) followed by calcination. The organic-dye NB was then added and ultrasonicated further 30 min for the formation of CeO2/NB nanohybrid material. Various spectroscopic and microscopic tools such as UV-vis and FT-IR spectroscopy, XRD, SEM and high-solution TEM and surface analysis tool Brunauer-Emmett-Teller (BET) confirm the formation of the nanohybrid. HR-TEM images showed the well-covered CeO2 on NB molecules and the average size of the nanohybrid is ~35 nm. For the fabrication of environmental pollutant electrochemical sensor, the prepared CeO2/NB nanohybrid was drop-casted on the electrode surface and utilized for the determination of HZ. The nanohybrid modified electrode exhibits higher electrocatalytic activity by showing enhanced oxidation current and less positive potential shift towards HZ oxidation than the bare and individual CeO2 and NB modified electrodes. The fabricated sensor with excellent reproducibility, repeatability, long-term storage stability and cyclic stability exhibited the sensational sensitivity (484.86 µA mM-1 cm-2) and specificity in the presence of 50-fold possible interfering agents with the lowest limit of detection of 57 nM (S/N = 3) against HZ. Utilization of the present sensor in environmental samples with excellent recovery proves it practicability in the determination of HZ in real-time application.
Phenolic acids of oak gall were extracted using ultrasonic-probe assisted extraction (UPAE) method in the presence of ionic liquid. It was compared with classical ultrasonic-bath assisted extraction (CUBAE) and conventional aqueous extraction (CAE) method, with and without the presence of ionic liquid. Remarkably, the UPAE method yielded two-fold higher extraction yield with the presence of ionic liquid, resulting 481.04 mg/g for gallic acids (GA) and 2287.90 mg/g for tannic acids (TA), while a decreased value of 130.36 mg/g for GA and 1556.26 mg/g for TA were resulted with the absence of ionic liquid. Intensification process resulted the highest yield of 497.34 mg/g and 2430.48 mg/g for GA and TA, respectively, extracted at temperature 50 °C with sonication intensity of 8.66 W/cm2 and 10% duty cycle, diluted in ionic liquid, 1-Butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, [Bmim][Tf2N] at concentration of 0.10 M with sample-to-solvent ratio 1:10 for 8 h. Peleg's model successfully predicted the UPAE process confirming that extraction capacity is the controlling factor in extracting phenolic acids. Hence, it can be concluded that UPAE method and ionic liquid have synergistic effect as it effectively enhanced the extraction efficiency to increase the bioactive constituents yield.
The synthesis of nanoparticles often result in the generation of harmful chemical pollutants. As such, many researchers have focused on developing green processes, which include the biosynthesis. In this research, ZnO nanoparticles were prepared using the leaf extract of whortleberry (Vaccinium arctostaphylos L.) via a simple ultrasonic-assisted method. The morphology, crystal size and structure, surface, thermal, and optical properties of the bio-mediated ZnO sample (ZnOext) were analyzed and compared with that produced without incorporating the extract (ZnOchem). The ZnO samples were evaluated for their antidiabetic, antibacterial, as well as their sono- and photo-catalytic performances. Initially, the samples were intraperitoneal injected to alloxan-diabetic rats to examine their treatment efficiency in terms of effects on fasting blood glucose, insulin, cholesterol, high-density lipoprotein, and total triglyceride levels. The ZnOext showed significantly higher efficiency for improving the health status of alloxan-diabetic rats in contrast with other tested treatments, vis. ZnOchem, insulin, and only leaf extract. In addition, both the ZnO samples were assessed against gram-negative and gram-positive bacteria and through sono- and photo-catalytic processes for removing rhodamine B, respectively. The results of this study indicated that not only the ZnOext sample was pollution free, it also exhibited higher potentials for treating diabetic rats, bacterial decontamination, and also oxidative removal of organic compounds under the influences of ultrasound and UV irradiations when compared with ZnOchem sample.
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.
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.
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.
The current work proposed an alternative ultrasound (US) technology, namely the high-intensity ultrasonic tubular reactor (HUTR) for preparing Pickering emulsions. Using the non-toxic and environmentally friendly cellulose nanocrystal (CNC) as a solid stabilizer, Pickering emulsions were produced using the HUTR and the results showed that Pickering emulsions as small as 1.5 µm can be produced using HUTR at the US power and sonication time of 300 W and 15 min respectively. Additionally, the sizes of Pickering emulsion obtained are found to remain the same upon 30 days of storage. The performance of HUTR in emulsion preparation is compared to conventional US horn system at the same US power. It was observed that the use of HUTR allowed generation of Pickering emulsion that is significantly smaller (around 7.40 μm) and with better droplet size distribution (Coefficient of variation, CV = 31%) as compared to those prepared with US horn method (12.75 µm, CV = 36%). This is owing to the better distribution of cavitation activity in the treatment chamber of HUTR as compared to those in the horn, according to the sonochemiluminescence (SCL) study. From the 30-days storage stability analysis, the CNC-PE prepared using HUTR was found to more stable against droplet coalescence in comparison to those prepared using US horn. Our findings suggested that the HUTR possessed superior Pickering emulsification capacity when compared to conventional US horn. Further work will be necessary to evaluate the feasibility of such intensifying tubular reactor technology for larger scale emulsification and other process intensification applications.
This work studied the influences of water blanching pretreatment (30 s), surface contacting ultrasound (492.3 and 1131.1 W/m2) assisted air drying, and their combination on drying kinetics and quality of white cabbage. Contacting sonication was performed by placing samples on an ultrasonic vibration plate, and the drying temperature was 60 °C. Through drying kinetic analysis and numerical simulation considering internal and external resistances and shrinkage, it was found that both blanching pretreatment and contacting sonication during drying intensified internal water diffusion and external water exchange to shorten cabbage drying time. Meanwhile, blanching pretreatment was more effective to enhance the drying process. The largest reduction of drying time (from 145 min to 24 min) was obtained when sequential blanching and contacting sonication at 1131.1 W/m2 were conducted. Dehydrated cabbages with blanching pretreatment were characterized by green color and high retention of vitamin C, while a severe loss of vitamin C was found in dried cabbages without blanching pretreatment. Moreover, although both blanching and contacting sonication shortened the drying time, the losses of phenolics, glucosinolates and resulting breakdown products were not alleviated. Contents of total phenolics, one glucosinolates (sinigrin) and one glucobrassicin breakdown product (indole-3-acetoritrile) in only air dried cabbages were significantly (p
The nonsteroidal anti-inflammatory drug sodium diclofenac (DC) is an emerging water pollutant which resists conventional wastewater treatments. Here the sonophotocatalytic degradation of DC was carried out using micrometric TiO2 (both pristine and Ag-decorated), UV-A irradiation and 20 kHz pulsed ultrasound. Sonophotocatalytic tests were compared with photolysis, sonolysis, sonophotolysis, sonocatalysis and photocatalysis data performed in the same conditions. A synergy index of over 2 was determined for tests with pristine TiO2, while values close to 1.3 were observed for Ag-TiO2. Reaction intermediates were studied by HPLC-MS, showing degradation mechanisms activated by hydroxyl radicals. Similar pathways were identified for photocatalytic and sonophotocatalytic tests, although the latter led to more oxidized compounds. Different reactor configurations (static and dynamic set ups) were studied. Sequential and simultaneous application of UV light and ultrasound led to similar performance. The role of water matrix was investigated using ultrapure and drinking water, showing marked detrimental effects of electrolytes on the DC degradation. Overall, the combined treatment proved more efficient than photocatalysis alone especially in demanding working conditions, like in drinking water matrices.
Bifunctional electrocatalysts to enable efficient oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are essential for fabricating high performance metal-air batteries and fuel cells. Here, a defect rich nitrogen and sulfur co-doped graphene/iron carbide (NS-GR/Fe3C) nanocomposite as an electrocatalyst for ORR and OER is demonstrated. An ink of NS-GR/Fe3C is developed by homogeneously dispersing the catalyst in a Nafion containing solvent mixture using an ultrasonication bath (Model-DC150H; power - 150 W; frequency - 40 kHz). The ultrasonically prepared ink is used for preparing the electrode for electrochemical studies. In the case of ORR, the positive half-wave potential displayed by NS-GR/Fe3C is 0.859 V (vs. RHE) and for the OER, onset potential is 1.489 V (vs. RHE) with enhanced current density. The optimized NS-GR/Fe3C electrode exhibited excellent ORR/OER bifunctional activities, high methanol tolerance and excellent long-term cycling stability in an alkaline medium. The observed onset potential for NS-GR/Fe3C electrocatalyst is comparable with the commercial noble metal catalyst, thereby revealing one of the best low-cost alternative air-cathode catalysts for the energy conversion and storage application.
The purpose of this investigation is to evaluate the implementation of ultrasound-assisted liquid biphasic flotation (LBF) system for the recovery of natural astaxanthin from Haematococcus pluvialis microalgae. Various operating conditions of ultrasound-assisted LBF systems such as the position of ultrasound horn, mode of ultrasonication (pulse and continuous), amplitude of ultrasonication, air flowrate, duration of air flotation, and mass of H. pluvialis microalgae were evaluated. The effect of ultrasonication on the cellular morphology of microalgae was also assessed using microscopic analysis. Under the optimized operating conditions of UALBF, the maximum recovery yield, extraction efficiency, and partition coefficient of astaxanthin were 95.08 ± 3.02%, 99.74 ± 0.05%, and 185.09 ± 4.78, respectively. In addition, the successful scale-up operation of ultrasound-assisted LBF system verified the practicability of this integrated approach for an effective extraction of natural astaxanthin.
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.
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.
Sugarcane juice (Saccharum officinarum) is a proven nutritious beverage with high levels of antioxidants, polyphenols, and other beneficial nutrients. It has recently gained consumer interest due to its high nutritional profile and alkaline nature. Still, high polyphenolic and sugar content start the fermentation in juice, resulting in dark coloration. Lately, some novel techniques have been introduced to extend shelf life and improve the nutritional value of sugarcane juice. The introduction of such processing technologies is beneficial over conventional processes and essential for producing chemical-free, high-quality, fresh juices. The synergistic impact of these novel technologies is also advantageous for preserving sugarcane juice. In literature, novel thermal, non-thermal and hurdle technologies have been executed to preserve sugarcane juice. These technologies include high hydrostatic pressure (HHP), ultrasound (US), pulsed electric field (PEF), ultraviolet irradiation (UV), ohmic heating (OH), microwave (MW), microfludization and ozone treatment. This review manifests the impact of novel thermal, non-thermal, and synergistic technologies on sugarcane juice processing and preservation characteristics. Non-thermal techniques have been successfully proved effective and showed better results than novel thermal treatments. Because they reduced microbial load and retained nutritional content, while thermal treatments degraded nutrients and flavor of sugarcane juice. Among non-thermal treatments, HHP is the most efficient technique for the preservation of sugarcane juice while OH is preferable in thermal techniques due to less nutritional loss.
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.
Innovative technologies for the pasteurization of food products have increased due to the global demand for higher-quality food products. In this regard, the current article aimed to provide an overview regarding the latest research on US application in the decontamination of fungi in food products and highlight the parameters influencing the effectiveness of this method. Therefore, the related article with inactivation of fungi and mycotoxins by ultrasound among last four years (2018-2021) by using terms such as 'mycotoxin,' 'inactivation,' 'ultrasound,' 'decontamination' among some international databases such as PubMed, Web of Science, Embase and Google Scholar" was retrieved. Ultrasound (US) is considered a non-thermal decontamination method for food products. In US, the release of energy due to the acoustic phenomenon destroys microorganisms. This technology is advantageous as it is inexpensive, eco-friendly, and does not negatively affect food products' food structure and organoleptic properties. The influence of the US on food structure and organoleptic properties dramatically depends on the intensity and energy density applied In addition, it can preserve higher levels of ascorbic acid, lycopene, and chlorophyll in sonicated food products. The treatment conditions, including frequency, intensity, duration, temperature, and processing pressure, influence the effectiveness of decontamination. However, US displays synergistic or antagonistic effects on bacteria, yeasts, molds, and mycotoxins when combined with other types of decontamination methods such as chemical and thermal approaches. Thus, further research is needed to clarify these effects. Overall, the application of US methods in the food industry for decreasing the microbial content of food products during processing has been applied. However, the use of US with other techniques needs to be studied further.
Methods of NMR relaxation and differential scanning calorimetry (DSC) were used to study the crystallization of anhydrous milk fat (AMF) obtained from milk and subjected to ultrasonic (US) processing. Amongst the changes in the crystallization nature under the influence of ultrasound are the decrease in the crystallization temperature and the increase in the melting enthalpy of the anhydrous milk fat samples. The increase is ∼30% at 20 min of isothermal crystallization and is presumably explained by the additional formation of β'-form crystals from the melt. The parameters of the Avrami equation applied to the description of experimental data show an increase in the crystallization rate in samples with ultrasonic treatment and a change in the dimension of crystallization with a change in melting temperature.