Lemon oil solubilization in mixed surfactant solutions: Rationalizing microemulsion & nanoemulsion formation

Lipophilic functional ingredients are usually incorporated into aqueous-based foods and beverages in the form of colloidal dispersions. In this study, we investigated the rate and extent of solubilization of emulsified lemon oil in mixed non-ionic surfactant solutions (buffer: propylene glycol = 2:1): sucrose monopalmitate (SMP) and/or Tween 80 (T80). The influence of surfactant concentration, type, and mixing ratio on lemon oil solubilization was investigated, with the aim of identifying suitable conditions for preparing stable microemulsions and nanoemulsions. Solubilization was monitored by measuring changes in light scattering by lemon oil droplets after they were dispersed in surfactant solutions (pH 7). The solubilization process was rapid (<few minutes), with the rate increasing with increasing surfactant concentration. For a particular surfactant type and concentration, lemon oil was transferred from nanoemulsion droplets into microemulsion droplets until a critical lemon oil concentration (C_sat) was reached, after which it remained as nanoemulsion droplets. The value of C_sat increased with increasing surfactant concentration and was higher for SMP than Tween 80. The impact of storage at pH 3.5 on the physical stability of microemulsions and nanoemulsions was examined. Acid stable colloidal dispersions could not be formed using SMP alone. However, relatively stable nanoemulsions and microemulsions could be formed when ≥75 or 50 wt% Tween 80 was incorporated into the surfactant phase, respectively. This study provides important information for the rational design of food-grade colloidal delivery systems for encapsulating and delivering functional lipids for food and beverage applications.     

Impact of lemon oil composition on formation and stability of model food and beverage emulsions

Lemon oil is a complex organic compound isolated from citrus peel, which is commonly used as a flavouring agent in beverages, foods, cosmetics, and household products. We have studied the influence of lemon oil fold (1×, 3×, 5× and 10×) on the formation and properties of oil-in-water emulsions. Initially, the composition, molecular characteristics, and physicochemical properties of the four lemon oils were established. The main constituents in single-fold lemon oil were monoterpenes (>90%), whereas the major constituents in 10-fold lemon oil were monoterpenes (≈35%), sesquiterpenes (≈14%) and oxygenates (≈33%). The density, interfacial tension, viscosity, and refractive index of the lemon oils increased as the oil fold increased (i.e., 1× < 3× < 5× < 10×). The stability of oil-in-water emulsions produced by high pressure homogenisation was strongly influenced by lemon oil fold. The lower fold oils were highly unstable to droplet growth during storage (1×, 3×, and 5×) with the growth rate increasing with increasing storage temperature and decreasing oil fold. Droplet growth was attributed to Ostwald ripening, i.e., diffusion of lemon oil molecules from small to large droplets. The highest fold oil (10×) was stable to droplet growth, which was attributed to the presence of an appreciable fraction of constituents with very low water-solubility that inhibited droplet growth through a compositional ripening effect. This study provides important information about the relationship between lemon oil composition and its performance in emulsions suitable for use in food and beverage products.     

Encapsulation of functional lipophilic components in surfactant-based colloidal delivery systems: Vitamin E,vitamin D,and lemon oil

The fabrication and stability of surfactant-based colloidal delivery systems (microemulsions and emulsions) suitable for encapsulation of lipophilic active agents (vitamins and flavours) was investigated. An emulsion titration method was used to study the influence of surfactant type (Tween 20, 60 and 80) and oil type (Vitamin E, vitamin D₃ and lemon oil) on the incorporation of lipophilic components into surfactant micelles. Oil-in-water emulsions were formed and then different amounts were titrated into surfactant micelle solutions. The influence of surfactant-to-oil ratio (SOR) and oil type on the formation of colloidal dispersions was examined using dynamic light scattering and turbidity measurements. SOR, oil type, and surfactant type had a pronounced influence on the nature of the colloidal dispersions formed. Microemulsions could not be formed using vitamin D or E in 1% Tween solutions, due to the relatively large size of the lipophilic molecules relative to the hydrophobic interior of the surfactant micelles. On the other hand, microemulsions could be formed from lemon oil at relatively high SORs. There was not a major impact of non-ionic surfactant type (Tween 20, 60 or 80) on the formation and properties of the colloidal dispersions. However, Tween 20 micelles did appear to be able to solubilise less lemon oil than Tween 60 or 80 micelles, presumably due to their smaller dimensions. This study provides useful information for the rational design of food grade colloidal delivery systems for encapsulating flavour oils, oil-soluble vitamins, and other functional lipids for application in foods and beverages.     

Optimization of lipid nanoparticle formation for beverage applications: Influence of oil type,cosolvents, and cosurfactants on nanoemulsion properties

The influence of flavor oil composition, cosolvents (glycerol and propylene glycol), and cosurfactant (lysolecithin) on the formation and stability of lemon oil nanoemulsions stabilized by sucrose monoesters was examined. At ambient temperature, nanoemulsions containing 1-, 3-, and 5-fold lemon oils were stable to droplet growth, whereas those containing 10-fold lemon oil were unstable. For 10-fold lemon oil nanoemulsions, the droplet growth rate increased with increasing temperature, cosolvent addition, and decreasing lysolecithin concentration, which was attributed to the influence of these factors on the phase inversion temperature. Clear nanoemulsions could be formulated that maintained small mean particle diameters (d ≈ 81 nm) during storage at ambient temperature for 1 month. The information generated in this study is useful for designing stable flavor nanoemulsions for applications in functional foods and beverages.     

Food-grade microemulsions,nanoemulsions and emulsions: Fabrication from sucrose monopalmitate & lemon oil

Sucrose monopalmitate (SMP) is a non-toxic, biodegradable, non-ionic surfactant suitable for use in foods and beverages. This study aimed to establish conditions where stable microemulsions, nanoemulsions or emulsions could be fabricated using SMP as a surfactant and lemon oil as an oil phase. Emulsions (r > 100 nm) or nanoemulsions (r < 100 nm) were formed at low surfactant-to-oil ratios (SOR < 1) depending on homogenization conditions, whereas microemulsions (r < 10 nm) were formed at higher ratios (SOR > 1). The impact of simple mixing, thermal treatment, and homogenization on the formation of the different colloidal systems was investigated. Blending/heating was needed to produce microemulsions or emulsions, whereas blending/heating/homogenization was needed to produce nanoemulsions. The impact of environmental stresses (pH, ionic strength, temperature) on the functional performance of nanoemulsions and microemulsions was examined. Relatively stable nanoemulsions could be formed at pH 6 and 7 and stable microemulsions at pH 5 and 6, but extensive particle growth/aggregation occurred at lower and higher pH values. Microemulsions were relatively stable to salt addition (0–200 mM NaCl), but nanoemulsions exhibited droplet aggregation/growth at ≥50 mM NaCl after 1 month storage at pH 7. Microemulsions formed gels at low temperatures (5 °C), were stable at ambient temperatures (23 °C), and exhibited particle growth at elevated temperatures (40 °C). Nanoemulsions were stable at refrigerator (5 °C) and ambient (23 °C) temperatures, but exhibited coalescence at elevated temperatures (40 °C). This study provides important information for optimizing the application of sucrose monoesters to form colloidal dispersions in food and beverage products.     

Effect of oxidative deterioration on flavour and aroma components of lemon oil

Reactions of five major components (citral, α- and β-pinene, limonene and γ-terpinene) of lemon oil in the presence of Cu catalysts and air have been shown to lead to significant oxidation of α- and β-pinene and γ-terpinene, even when the catalyst concentration was comparable to that present in copper-plumbed tap water. Addition of commercial antioxidants (BHA and tocopherol) generally led to suppression of oxidation. UV degradation of these compounds in the presence of air was most significant for γ-terpinene and limonene which gave products similar to those obtained from the Cu-catalysed thermal reactions. Citral gave different products, mainly photocitrals, in contrast to the thermal reactions. The sensitivity of lemon oil to temperature and the presence of air was confirmed.     

甜橙油多重乳状液的稳定性研究

多重乳状液的稳定性是影响多重乳化香精效果的主要因素,它决定于体系中不同参数的影响.以多重乳状液相对体积为衡量标准,借助显微镜直接观察,探讨乳化剂的含量、乳化剂的HLB值、亲油亲水乳化剂体积比及油水相比等因素对甜橙油多重乳状液体系稳定性的影响.     

油相浓度对姜黄素纳米乳液稳定性的影响

以中链甘油三酯为油相,卵磷脂为乳化剂,采用高压均质技术制备出含不同油相浓度的姜黄素纳米乳液,于4、25和55℃条件下贮藏30 d,研究不同油相浓度对姜黄素纳米乳液稳定性的影响。结果表明:油相浓度较低(5%、10%)时,姜黄素纳米乳液具有较高的稳定性,姜黄素保留率分别达到48.50%和48.99%,粒径增加了0.79%和15.78%;且4℃贮藏时,其理化稳定性表现最好,30 d后姜黄素损失率仅为14.98%。      

Influence of chitosan and NaCl on physicochemical properties of low-acid tuna oil-in-water emulsions stabilized by non-ionic surfactant

An influence of low molecular weight (LMW) chitosan on physicochemical properties and stability of low-acid (pH 6) tuna oil-in-water emulsion stabilized by non-ionic surfactant (Tween 80) was studied. The mean droplet diameter, droplet charge (ζ-potential), creaming stability and microstructure of emulsions (5 wt% oil) were evaluated. The added chitosan was adsorbed on the surface of oil droplets stabilized by Tween 80 through electrostatic interactions. Such addition of chitosan at different concentrations (0–10 wt%) to emulsions showed slight effect on the mean droplet diameter. However, the degree of flocculation was a function of chitosan concentration assessed by emulsions' microstructure and creaming index. The impact of chitosan on the strength of the colloidal interaction between the emulsion droplets increased with increasing chitosan concentration. The mean diameter of droplet in emulsions increased with increasing NaCl because of the electrostatic screening effect. The addition of LMW chitosan could be performed to create tuna oil emulsions with low-acid to neutral character, as well as various physicochemical and stability properties suitable for health food products.     

pH对白藜芦醇-石榴籽油纳米乳理化性质的影响

考察p H对白藜芦醇-石榴籽油纳米乳理化性质的影响。以石榴籽油为油相制备白藜芦醇自纳米乳化系统（RES SNEDDS-PSO）,研究不同p H（6.8、5.8和4.8）下RES SNEDDS-PSO形成的纳米乳的理化性质。结果显示,不同p H的RES SNEDDS-PSO经10倍水稀释后均能形成粒径在100 nm以下的纳米乳,zeta电位值分别为-6.42、-2.10、-0.661 mv;随着p H的下降,白藜芦醇在纳米乳中的溶解度及物理稳定性降低,释放速率减慢。在水中,p H6.8及5.8的白藜芦醇纳米乳较对照溶液降解速率常数减小一半,p H4.8的降解速度与对照溶液近似;不同p H的纳米乳略微降低了白藜芦醇在胃液中的稳定性,但显著提高了药物在肠液中的稳定性。研究结果表明p H对游离白藜芦醇及RES SNEDDS-PSO稳定性的影响具有差异性。      

Fabrication of ultrafine edible emulsions: Comparison of high-energy and low-energy homogenization methods

Emulsions containing ultrafine droplets (r < 100 nm) have a number of potential advantages over conventional emulsions for the encapsulation and delivery of lipophilic substances in foods and beverages: high optical clarity; high physical stability; increased bioavailability. These ultrafine emulsions can be fabricated from high-energy or low-energy homogenization methods, which each have advantages and limitations. In this study, we compared a high-energy method (microfluidization) with a low-energy method (spontaneous emulsification) for forming oil-in-water emulsions from food-grade ingredients (medium chain triglycerides and Tweens). The influence of surfactant type (Tween 80, Tween 85, and Tween 80/Tween 85) and surfactant-to-oil ratio (SOR = 0.1–5) on the formation of emulsions was examined. Both the low- and high-energy methods were able to produce emulsions with ultrafine droplets (r < 100 nm). The microfluidization method required high-energy inputs and dedicated equipment, but could produce ultrafine emulsions at much lower surfactant-to-oil ratio (SOR < 0.1). On the other hand, the spontaneous emulsification method only required simple mixing, but it needed much higher surfactant-to-oil ratios (SOR > 0.5) to produce droplets with r < 100 nm. This study has important implications for the development of food-grade delivery systems to encapsulate lipophilic substances, such as flavors, colors, vitamins, and nutraceuticals.     

Influence of interfacial composition on oxidative stability of oil-in-water emulsions stabilized by biopolymer emulsifiers

The objective of this research was to evaluate the influence of storage pH (3 and 7) and biopolymer emulsifier type (Whey protein isolate (WPI), Modified starch (MS) and Gum arabic (GA)) on the physical and oxidative stability of rice bran oil-in-water emulsions. All three emulsifiers formed small emulsion droplets (d₃₂ < 0.5 μm) when used at sufficiently high levels: 0.45%, 1% and 10% for WPI, MS and GA, respectively. The droplets were relatively stable to droplet growth throughout storage (d₃₂ < 0.6 μm after 20 days), although there was some evidence of droplet aggregation particularly in the MS-stabilized emulsions. The electrical charge on the biopolymer-coated lipid droplets depended on pH and biopolymer type: −13 and −27 mV at pH 3 and 7 for GA; −2 and −3 mV at pH 3 and 7 for MS; +37 and −38 mV at pH 3 and 7 for WPI. The oxidative stability of the emulsions was monitored by measuring peroxide (primary products) and hexanal (secondary products) formation during storage at 37 °C, for up to 20 days, in the presence of a pro-oxidant (iron/EDTA). Rice bran oil emulsions containing MS- and WPI-coated lipid droplets were relatively stable to lipid oxidation, but those containing GA-coated droplets were highly unstable to oxidation at both pH 3 and 7. The results are interpreted in terms of the impact of the electrical characteristics of the biopolymers on the ability of cationic iron ions to interact with emulsified lipids. These results have important implications for utilizing rice bran oil, and other oxidatively unstable oils, in commercial food and beverage products.     

Monitoring air/liquid partition of mastic gum oil volatiles in model alcoholic beverage emulsions: Effect of emulsion composition and oil droplet size

The purpose of this work was to study the impact of the structure and composition of hydroalcoholic emulsions on the air–liquid partition of aroma compounds of the essential oil of Pistacia lentiscus var. chia, commonly known as mastic gum oil (mainly consists of terpenes). Oil-in-water emulsions (φ = 0.17), containing 15% (v/v) ethanol, stabilized by three different emulsifiers (sodium caseinate, whey protein isolate and Tween 40), were prepared by using two different lipid phases (sunflower oil and anhydrous butter fat). The homogenization conditions were varied to obtain emulsions with different volume–surface mean diameters. The partition of the volatile compounds between air phase and emulsions at three different temperatures (25, 37 and 50 °C) was monitored by applying the Headspace Solid Phase Microextraction technique, followed by gas chromatography–mass spectrometry (GC–MS) analysis. In general, the results obtained showed that sodium caseinate was the most effective in retaining mastic aroma compounds, while WPI was the least effective. This could partly be explained by the different structure of the two proteins which, when adsorbed at the interface, form a membrane that acts as a barrier and influences the partition of the aroma compounds between the air and the liquid. At the same time interactions of aroma compounds with the two proteins in the bulk phase may also play a role. The retention of the aroma compounds depended on the oil droplet size only in the case of sodium caseinate containing emulsions at 37 and 50 °C. This behaviour could be due to the substantial increase in the thickness of the adsorbed casein layer when moving from a fine sized emulsion to one with a much larger size as well as to differences in the ratio of free to adsorbed emulsifier. The composition of the lipid phase also appeared to have a significant impact on the concentration of volatile compounds in the headspace of mastic gum oil containing emulsions stabilized by proteins. This was lower in the case of butter fat probably due to differences in composition with regard to fatty acid degree of saturation as well as to volatile absorption by the liquid lipid at 40 °C and subsequent entrapment in the semisolid fat at 25 °C.     

丁香油微乳的制备及抑菌活性研究

为了改善丁香油水相溶解性及储藏稳定性差的应用缺陷,以可稀释微乳包载丁香油。通过比较丁香油微乳拟三元相图中微乳区面积(S_(ME))和最小可稀释比(DR),选择聚氧乙烯蓖麻油(Cremophor)EL 30与无水乙醇以21(质量比)为混合表面活性剂,水相环境为中性制备丁香油微乳。进一步采用电导率法和流变法对微乳构型进行鉴定,并选择O/W中心区域微乳:混合表面活性剂/丁香油/水(质量比)=16/4/80,Km=2,进行抑菌活性评价。结果表明,微乳包埋体系并未改变丁香油的抑菌活性。同时,通过检测丁香油微乳在稀释和储藏过程中的粒径变化,发现此微乳能保持良好的稀释和储藏稳定性。因此,该微乳在有效改善丁香油的水溶性和储藏稳定性的同时,对其抑菌活性没有影响。     

Chemical composition, in vitro anti-yeast activity and fruit juice preservation potential of lemon grass oil

The anti-yeast activity of lemon grass oil was evaluated against several food spoiling yeasts (Saccharomyces cerevisiae, Zygosaccharomyces bailii, Aureobasidium pullulans, Candida diversa, Pichia fermentans, Pichia kluyveri, Pichia anomala and Hansenula polymorpha) through disc diffusion and microbroth dilution method. The minimum inhibitory concentration (MIC) and minimum fungicidal concentration (MFC) varied from 0.28 to 1.3 mg/ml and 0.56 to 4.5 mg/ml, respectively, where highest MIC (2.25 mg/ml) was shown by A. pullulans and lowest MIC (0.28 mg/ml) was shown by C. diversa and P. anomala. Kill time assay was conducted for selected three yeast strains where S. cerevisiae showed highest reduction (3 log cfu) in viability within 24 h exposure of lemon grass oil at MFC level. Further, the anti-yeast efficacy of lemon grass oil alone and in combination with thermal treatment was evaluated in real food system i.e. mixed fruit juices. Chemical composition analysis of lemon grass oil by gas chromatography–mass spectrometry (GC–MS) revealed that the dominant compounds were geranial (40.5%), neral (30.7%), geranyl acetate (5.1%), caryophyllene (2.5%). Present results established the superior performance of integrated (thermal–lemon grass oil) treatment over the individual exposure (lemon grass oil or thermal treatment alone) for fruit juice preservation.     

Oxidative stability of olive oil–lemon juice salad dressings stabilized with polysaccharides

Lipid oxidation is a major cause of quality deterioration in food emulsions. Polysaccharides used to improve emulsion stability and texture may also affect lipid oxidation. In the present study, the oxidative stability of olive oil–lemon juice salad dressings, stabilized with gum arabic or propylene glycol alginate in admixture with xanthan, was investigated. Oil-in-water emulsions (50:50, v/v) were prepared with lemon juice and extra virgin olive oil and then homogenized at various homogenization rates to form different particle sizes. Keepability was followed by storing at room temperature for 6–8 months and measuring the formation of primary and secondary oxidation products. The shelf life was compared to that of the bulk olive oil. It was shown that the polysaccharides had the ability to inhibit lipid oxidation, probably due to their amphiphilic character (gum arabic and propylene glycol alginate) as well as their ability to induce viscosity increase. Olive oil–lemon juice emulsions were also assessed for consumer acceptance. The panellists were asked to smell the samples and rate them according to rancidity using a four-point (1 = no perception, 4 = extreme) intensity scale. The results were in accordance to those of chemical analysis. Lipid oxidation was not affected by the oil droplet size, as demonstrated by peroxide value measurements and sensory evaluation.     

Effects of pre‐emulsifying fat/oil on meat batter stability,texture and microstructure

The effects of pre‐emulsified beef fat and canola oil (CO) (25%) with Tween 80 (T‐80) or sodium caseinate (SC) were studied in beef meat batters prepared at three protein levels (9%, 12% and 15%). Raising meat protein level to 15% resulted in low emulsion stability of products prepared with CO. Using pre‐emulsified beef fat with Tween 80 (BF‐T80) showed significantly higher fat and water losses at all protein levels. There were no differences in fat and water losses between pre‐emulsified beef fat and CO when SC was used at the 9% and 12% protein levels compared to the controls (non pre‐emulsification). Light microscopy revealed fat globule coalescence in the CO meat batters prepared with 15% protein and BF‐T8 treatments, as well as formation of fat channels and more protein aggregation; both resulted in lower emulsion stability. Using SC to emulsify fat/oil produced a finer dispersion of fat globules compared to all the other treatments.     

Effects of soybean oil and oxidized soybean oil on the stability of β-carotene

The effects of 1.0%, 2.5%, and 5.0% purified soybean oil and thermally oxidized soybean oil on the stability of 100 ppm β-carotene as a fat-soluble vitamin A and singlet oxygen quencher in isooctane have been studied. The samples were stored under 1000, 2000, or 4000 lx at 20 °C for 2 days and at 50 °C for 16 days in the dark. The β-carotene was determined by high-performance liquid chromatography. The centrifugation and filtration of vegetable mixture, during sample preparation for β-carotene analysis by HPLC, decreased the coefficient of variation from 4.13% to 1.02%. The purified soybean oil and thermally oxidized soybean oil stabilized β-carotene in isooctane under light and in the dark at α = 0.05. The losses of β-carotene, with 1.0% purified oil, 1.0% thermally oxidized oil and without any oil during 48 h under light, were 11.2%, 80%, and 100%, respectively. 100 ppm TBHQ had a protective effect on the stability of β-carotene in isooctane at α = 0.05. The β-carotene stability decreased as the light intensity increased from 1000 to 2000 or 4000 lx at α = 0.05. The stability of vitamins in fruit and vegetable drinks enriched with fat-soluble vitamins and antioxidants during storage can be greatly improved by adding approximately 1.0% high quality non-oxidized soybean oil.     

Formation and characterisation of mint oil/S and CS/water microemulsions

Preparation and characterisation of microemulsions (ME) with mint oil (MO) as the oil phase were conducted to find a system which could provide a controlled, sustained, and prolonged delivery of MO. The influence of surfactant type and processing parameters on the formation of MO-ME’s was studied by comparing the areas of the monophase ME regions in pseudoternary phase diagrams. A 1:1 mixture of the surfactants, AOT and CrEL, was found to be the most effective, and it produced a ME monophase area of about 70%. The monophase regions were analysed by conductivity measurements; the results suggested that O/W regions within the ME phases were formed when the water content was higher than 60–65%. As tested with dynamic light scattering (DLS) and head space (HS) GC analysis, the particle size of O/W ME, with 60% water and AOT/CrEL = 1:1 as surfactants, was 20.0 nm and the encapsulation efficiency was 78.4%. The results indicated that a ME of MO/AOT and CrEL/ethanol/water, may be a promising dispersion for the protection of MO in food products.     

Comparing the efficiency of different food‐grade emulsifiers to form and stabilise orange oil‐in‐water beverage emulsions: influence of emulsifier concentration and storage time

The aim of this study was to compare the efficiency of three different food‐grade emulsifiers to form and stabilise an orange oil‐in‐water emulsion. The emulsifier type and concentration had a profound effect on the initial particle size of the oil droplets with Tween 80 being the most effective in reducing the particle size (1% w/w, 1.88 ± 0.01 μm) followed by sodium caseinate (10% w/w, 2.14 ± 0.03 μm) and gum arabic (10% w/w, 4.10 ± 0.24 μm). The long‐term stability of the concentrated beverages was monitored using Turbiscan analysis. The Turbiscan stability indices after 4 weeks of storage followed the order: Tween 80 (1.70 ± 0.08) < gum arabic (4.83 ± 0.53) < sodium caseinate (6.20 ± 1.56). The protein emulsifier was more capable to control the oxidation process, and this was attributed to the excess amount of emulsifier present in the aqueous phase. This study provides useful insights into the formulation of flavour emulsions by the beverage industry.