Food Research International 134 (2020) 109231

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Food Research International

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Tailoring physical properties of monoglycerides oleogels using high- T

intensity ultrasound
⁎
Anabella Giacomozzia,b, , Camila Pallaa,b, María Elena Carrína,b, Silvana Martinic
a
Departamento de Ingeniería Química, Universidad Nacional del Sur (UNS). Bahía Blanca, Argentina
b
Planta Piloto de Ingeniería Química - PLAPIQUI (UNS-CONICET). Bahía Blanca, Argentina
c
Department of Nutrition, Dietetics, and Food Science, Utah State University, Logan, UT, USA

A R T I C LE I N FO A B S T R A C T

Keywords: The effects of high-intensity ultrasound application (HIU-20 kHz, 96 W, 3 pulses: 10 s on/5s off) and cooling rate
Cooling rate (0.1 and 10 °C/min) on physical properties of monoglycerides (MG) oleogels (3, 4.5, and 6 wt%) were evaluated.
Elasticity Oleogels melting profile, rheological and textural properties, crystal microstructure, crystal length (Lc), poly-
Microstructure morphic behavior, oil binding capacity (OBC), and solid fat content (SFC) were determined after 24 h of storage
Oil binding capacity
at 5 or 25 °C. HIU caused significant changes in the MG crystallization behavior, producing a decrease in Lc and a
Oleogels
Solid fat content
stronger and more elastic network with higher OBC. HIU increased the adhesiveness of all samples whereas did
Sonication not affect their cohesiveness. The effects of HIU application were enhanced by cooling at 0.1 °C/min and storing
Textural properties at 5 °C. Neither SFC nor thermal behavior were affected by HIU and the desired β' polymorphism was obtained in
all oleogels. This study shows that physical properties of MG oleogels can be significantly improved by HIU
application to obtain suitable fats with low level of saturated fatty acids for food applications.

1. Introduction promising technology to change the crystallization behavior of fats ,

Edible oils structuration by forming oleogels is one of the most
promising strategies to replace trans and saturated fatty acids in food
products such as margarines, spreads, and shortenings. Monoglycerides
(MG) oleogels are semisolid materials obtained by entrapping liquid
oils into a crystalline network of self-assembled gelators. Oleogels can
mimic the physical and functional properties of shortenings even
though they contain high and low amounts of unsaturated and satu-
rated fatty acids, respectively (Da Pieve, Calligaris, Panozzo, Arrighetti,
& Nicoli, 2011).
Monoglycerides are very efficient gelators since they can structure
oils at low concentrations (2 wt%). The crystalline network structure in
MG-based oleogels is influenced by their chemical composition as well
as by processing conditions used to induce MG crystallization (López-
Martínez et al., 2014; Palla, Giacomozzi, Genovese, & Carrín, 2017).
Previous studies have shown that HIU can be used as an emerging and
generate small crystals, and improve the material texture and elasticity.
These effects are attributed to the acoustic waves propagated in the
liquid, which create pressure variations, resulting in the formation of
bubbles. Depending on the acoustic intensity, frequency, and duration
of the pulses in the HIU application, bubbles can collapse, generating
very high and localized temperatures, pressures, and shear forces
(Wagh, Birkin, & Martini, 2016). The effect of sonication on lipid
crystallization can be explained by (a) presence of bubbles that act as
nuclei and induce primary nucleation, (b) generation of high shear
forces that break growing crystals promoting secondary crystallization,
(c) increase in supercooling due to localized increases in pressures, and
(d) a combination of all the effects mentioned above. Few studies used
HIU to prepare oleogels (Sharifi, Goli, & Fayaz, 2018; da Silva,
Arellano, & Martini, 2019). Sharifi et al. (2018) reported that HIU in-
duced nucleation in an olive oil/propolis oleogel by creating small
crystals that formed a strong network with high oil binding capacity

Abbreviations: AD, adhesiveness; CO, cohesiveness; DAG, diacylglycerols; ΔHM, melting enthalpy; D, fractal dimension; DSC, differential scanning calorimetry; FFA,
fatty acids; G', elastic modulus; GC, gas chromatography; HA, hardness; HIU, high-intensity ultrasound; HOSO, high oleic sunflower oil; L, linoleic acid; LC, crystals
length; MAG, monoacylglycerols; MG, monoglycerides; MP, melting point; OBC, oil binding capacity; PLM, polarized light microscopy; O, oleic acid; P, palmitic acid;
S, span; SFC, solid fat content; St, stearic acid; TAG, triacylglycerols; To, melting onset temperature; Tp, melting peak temperature; Ts, storage temperature
⁎
Corresponding author at: Departamento de Ingeniería Química, Universidad Nacional del Sur (UNS); Planta Piloto de Ingeniería Química, PLAPIQUI (UNS-
CONICET), 8000 Bahía Blanca, Argentina.
E-mail addresses: agiacomozzi@plapiqui.edu.ar (A. Giacomozzi), cpalla@plapiqui.edu.ar (C. Palla), mcarrin@plapiqui.edu.ar (M.E. Carrín),
silvana.martini@usu.edu (S. Martini).

https://doi.org/10.1016/j.foodres.2020.109231
Received 19 November 2019; Received in revised form 8 April 2020; Accepted 9 April 2020
Available online 13 April 2020
0963-9969/ © 2020 Elsevier Ltd. All rights reserved.
A. Giacomozzi, et al.
(OBC). In another study, da Silva et al. (2019) found that HIU reduced
the crystal size of candelilla wax/MG/hardfat oleogel and increased its
hardness with no change neither in elasticity nor in OBC compared to
the non-sonicated oleogel. In our previous research (Giacomozzi, Palla,
Carrín, & Martini, 2019) no or little improvement in OBC was observed
in sonicated MG oleogels cooled to 25 °C at 0.1 and 10 °C/min. We
hypothesized that crystallization occurred too fast (10 °C/min) or too
slow (0.1 °C/min) hindering the sonication effect. Slow cooling after
sonication might promote the formation of bigger crystals and therefore
less HIU effect on the crystallization process. When samples were
cooled slowly and HIU was applied at the onset of crystallization as
described in previous paper (Giacomozzi et al., 2019), the crystal-
lization occurred so slowly that the bubbles and cavitation events
generated during sonication dissipated before the sample achieved a
significant degree of crystallization. Similar results regarding the lack of
effect on samples that crystallize very slowly were reported by Martini,
Suzuki, and Hartel (2008). They found that, even if the formation of
bubbles took place as HIU was applied in anhydrous milk fat, when
bubbles collapsed, the triacylglycerol molecules were not yet in their
right conformation to crystallize (due to the low cooling rate) and
therefore, no effect on the crystallization behavior was observed. On the
other hand, Rincón‐Cardona, Agudelo‐Laverde, Herrera, & Martini
(2015) reported a low effectiveness of sonication in samples with fast
crystallization kinetics. They observed that, when samples were cooled
under a fast cooling rate, the crystallization occurred too fast and HIU
was not able to modify the crystallization kinetics of the samples.
Taking into account our previous results and that HIU is more ef-
ficient when applied in the presence of crystals (Ye, Wagh, & Martini,
2011), but is not efficient when crystallization takes place rapidly
(Rincon-Cardona et al., 2015), the objective of this work was to eval-
uate the effect of HIU on the crystallization behavior of MG oleogels
using a different processing approach that would allow to control the
first steps of crystallization process. This was achieved by cooling the
oleogels under agitation at a specific cooling rate (0.1 or 10 °C/min) to
a defined crystallization temperature (Tc) that would allow to slow
down the crystallization process of MG. In our previous work HIU was
applied when the first crystals were observed (Giacomozzi et al., 2019),
while in this work HIU was applied when the sample reached Tc (which
was determined as described in the Materials and Methods section).
HIU was used at the same conditions than in our previous work but at
different moment during the crystallization process. After that, samples
continued the cooling process under static conditions by connecting the
crystallization cell to a different water bath set at 25 °C which resulted
in an average cooling rate of 1 °C/min.
2. Materials and methods
High oleic sunflower oil (HOSO, Spectrum®) composed by: C16:0
(4.03 ± 0.03%), C18:0 (2.20 ± 0.01%), C18:1 (83.94 ± 0.07%),
and C18:2 (7.98 ± 0.02%) was purchased from a local store (Logan,
UT, USA). Monoglycerides (MG, Myverol 18–04 K SG, Kerry, Ireland)
were used as gelator. MG were mainly composed of C16:0
(37.99 ± 0.04%) and C18:0 (59.78 ± 0.01%).
2.1. Preparation of oleogels
HOSO and MG were mixed in different proportions (Table 1),
melted in a microwave and kept in an oven at 80 °C for 30 min to erase
crystal memory. Samples (100 g) were placed in a double-walled cy-
lindrical crystallization cell (50-mm diameter, 90-mm height) equipped
with a water jacket that allowed for temperature control through its
connection to an external water bath that was pre-set at the defined
crystallization temperature (Tc) similar to the one described by Martini
et al. (2008). A detailed description of the ultrasound system and the
experimental set-up can be found in Fig. 1S. Preliminary experiments
were conducted to choose the appropriate Tc for each sample as
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Food Research International 134 (2020) 109231
described in section 2.3.1. Samples were cooled under magnetic agi-
tation (200 rpm) from 80 °C to Tc at slow (S, 0.1 °C/min) and fast (F,
10 °C/min) cooling rates controlled with a programmable water bath
(Lauda Ecoline Staredition RE310, Delran, NJ, USA). A thermocouple
was placed 30 mm from the bottom and 20 mm from the wall of the cell
to monitor the sample temperature as a function of time. As soon as Tc
was reached, the agitation was stopped and HIU was applied at a fre-
quency of 20 kHz for 30 s using 3 pulses: 10 s ON/5 s OFF resulting in a
volumetric power level of 0.86 W/cm3 (Misonix S-3000 sonicator,
Misonix Inc., Farmingdale, NY, USA). A tip of 3.2 mm-diameter vi-
brating at an amplitude of 216 μm was positioned at the center of the
cell to deliver the power level mentioned above. After sonication,
samples were statically cooled without controlling cooling rate by
connecting the crystallization cell to another external water bath (VWR,
model 1160S, Buffalo Grove, IL, USA) that was pre-set at 25 °C. Samples
processed as described before but without HIU application were used as
controls. Immediately after samples reached 25 °C they were stored in
an incubator at 25 °C for 24 h. To evaluate the effect of storage tem-
perature (Ts) on the physical properties of oleogels, samples with 3 and
6 wt% of MG were also stored at 5 °C for 24 h. The physical properties
of oleogels were measured at 25 or 5 °C as described below by taking
the samples from the crystallization cell.
2.2. Quantitation of FFA, MAG, DAG, and TAG
Simultaneous quantification of free fatty acids (FFA), mono-
acylglycerols (MAG), diacylglycerols (DAG), and triacylglylcerols
(TAG), as well as different TAG compounds identification in materials
(MG and HOSO) and oleogel samples was performed by GC according
to Pacheco, Palla, Crapiste, and Carrín (2014).
2.3. Measurement of oleogel physical properties
2.3.1. Melting point (MP) and crystallization temperature (Tc)
Monoglycerides MP was determined by differential scanning ca-
lorimetry (DSC) (TA Instruments DSC, model Q20 1963 with RCS
cooling system, New Castle, DE, USA). Samples (10–15 mg) were her-
metically sealed in aluminum pans, placed in the DSC oven, kept at
25 °C for 1 min, melted at 5 °C/min to 80 °C, kept at 80 °C for 30 min,
and cooled to −20 °C at 5 °C/min to induce crystallization. The analysis
was performed in triplicate. The same procedure was carried out to
determine Tc by measuring the crystallization profile for each molten
oleogel (O3, O4.5, and O6). MP and Tc were determined using TA
Universal Analysis software (TA Instruments, New Castle, DE, USA),
being the first determined as the highest temperature of the melting
peak, and the second obtained from the results of the reduced crystal-
linity (F) calculated from DSC thermograms, according to Palla, de
Vicente, Carrín, & Gálvez Ruiz (2019). High F values were not appro-
priate because it was demonstrated that HIU is more efficient when it is
applied at the onset of crystallization (Wagh et al., 2016). However, a
very low crystallinity at the moment of HIU application could cause loss
of sonication efficiency by melting the crystals that are being formed
(Ye and Martini, 2014). Based on these considerations, an intermediate
F value (48%) was chosen in this work for Tc determination from the
crystallization exothermic peak for each MG concentration.
2.3.2. Melting behavior
Oleogels melting behavior was measured by DSC according to
methodology described above, but using another temperature program.
Samples were heated from Ts to 80 °C at the rate of 5 °C/min. The
thermograms were analyzed to determine the melting onset tempera-
ture (To), melting peak temperature (Tp), and the change in melting
enthalpy (ΔHM) (Giacomozzi et al., 2019).
2.3.3. Polarized light microscopy (PLM)
An aliquot of oleogels was placed on a microscope slide, covered
A. Giacomozzi, et al. Food Research International 134 (2020) 109231

Table 1
Processing conditions tested in oleogels with different monoglycerides (MG) concentration (wt%).
Samples MG concentration (wt%) Cooling rate (°C/min) HIU application Ts (°C)

O3-S-wo HIU 3 0.1 NO 5 / 25 °C

O3-F-wo HIU 3 10 NO 5 / 25 °C
O3-S- with HIU 3 0.1 YES 5 / 25 °C
O3-F- with HIU 3 10 YES 5 / 25 °C
O4.5-S-wo HIU 4.5 0.1 NO 25 °C
O4.5-F-wo HIU 4.5 10 NO 25 °C
O4.5-S- with HIU 4.5 0.1 YES 25 °C
O4.5-F- with HIU 4.5 10 YES 25 °C
O6-S-wo HIU 6 0.1 NO 5 / 25 °C
O6-F-wo HIU 6 10 NO 5 / 25 °C
O6-S-wo HIU 6 0.1 YES 5 / 25 °C
O6-F-with HIU 6 10 YES 5 / 25 °C

HIU: high-intensity ultrasound; Ts: storage temperature; wo HIU: without HIU; with HIU: with high-intensity ultrasound; S: slow; F: fast.

with a cover-slide, and placed in a polarized light microscope (Olympus
BX 41, Tokyo, Japan) equipped with an Infinity 2 digital camera
(Lumenera Scientific, Infinity 2, Ottawa, ON, Canada). The micro-
structure of MG crystals in the oleogels was evaluated using a 10X
magnification objective. Five images of each sample were recorded for
each independent experiment. Particle size distribution analysis was
performed using the Image Pro-Plus software 7.0 (National Institutes of
Health, Bethesda, MD, USA) and the mean crystals length (Lc) and the
Span (S) were reported (Palla, de Vicente, Carrín, & Ruiz, 2019). Lc was
considered as the individual needle-like crystals, even in the case of
spherulitic clusters formed by the aggregation of these elongated
crystals. Moreover, the box-counting fractal dimension (D) of the mi-
croscopy images was determined following the methodology described
by Palla et al. (2019).
2.3.4. Solid fat content (SFC)
SFC of oleogels was measured by transferring a sample aliquot to
NMR tubes (180 × 10 mm). Tubes were placed in a pulsed nuclear
magnetic resonance (p-NMR) instrument (Bruker mq 20 Minispec) with
a 0.47-T magnetic field operating at a resonance frequency of 20 MHz
(Rincón‐Cardona et al., 2015).
2.3.5. X-ray analysis
After storage for 24 h, an aliquot of oleogels was placed into a
Büchner funnel and filtered using glass microfiber filters (Whatman
CAT N°1823-047, pore diameter 0.7 µm). Crystals retained in the filter
were collected in a beaker and used to determine polymorphism.
Diffraction peaks in the scattering angle (2θ) region of 3–30° were
obtained using a X'pert Pro-Diffractometer 3040 MPD (PANalytical,
Almelo, The Netherlands) which had a single goniometer PW 3050/60
(θ/2–θ, voltage 45 kV, current 40 mA) using a Cu Anode X-ray tube (Ye
et al., 2011). The polymorphic form of the crystals was identified as α
with a short spacing at 4.15 Å, as β' with short spacings at 3.8 and 4.2 Å,
and as β if the peaks do not satisfy the conditions for α and β', and has a
strong short spacing at 4.6 Å (Kadamne & Martini, 2018).
2.3.6. Textural properties
Texture profile analysis (TPA) was performed in a texture analyzer
(TMS-Pro, Food Technology Corporation, Sterling, VA) equipped with a
50 N load cell and a 6 mm diameter cylindrical probe following a two
penetration cycles procedure (Giacomozzi et al., 2019). Measurements
were performed immediately after removing samples from the storage
at Ts. The textural parameters (hardness-HA, adhesiveness-AD, and
cohesiveness-CO) were calculated from TPA curves (Palla et al., 2017).
2.3.7. Elastic (G') and loss (G'') moduli
G' and G'' were measured using a rheometer (TA Instruments, model
AR-G2, New Castle, DE, USA) controlled with the Rheology Advantage
Instrument Control software (TA Instruments, New Castle, DE, USA).
Samples were placed between a parallel plate geometry (diameter
40 mm, gap 1000 µm). Oscillatory strain sweep tests were performed at
Ts from 8.0x10-4 to 10% strain range at 1 Hz (Giacomozzi et al., 2019).
G' and G'' recorded a strain of 0.01% (within the linear viscoelastic
region) and tan δ (G''/G') were used for comparison purpose.
2.3.8. Oil binding capacity (OBC)
Oleogels' OBC was measured by weighing approximately 1 g of
sample in a pre-weighed Eppendorf tube and centrifuged at 11,500 g for
15 min at Ts using a Sorval Legend Micro 17 microcentrifuge (Thermo
Fisher ScientificTM, Waltham, Massachusetts, USA). After centrifuga-
tion, the Eppendorf tube was turned over to drain the released oil from
the sample for 3 min. OBC was calculated as function of percentage of
oil released from the sample after centrifugation (Giacomozzi et al.,
2019).
2.4. Statistical analysis
Results are reported as mean values and standard deviations of three
independent experiments. GraphPad Prism software (Prism 8.0.0;
GraphPad Software Inc., La Jolla, California, USA) was employed to
perform two-way ANOVA and Tukey's post-hoc tests (α = 0.05). Mean
values were compared as follows: within each cooling rate and Ts, mean
values with the same lowercase letters among concentrations and so-
nication conditions are not significantly different (p > 0.05). Means
represented by the same uppercase letters among cooling rate for each
MG concentration and Ts indicate that the samples are not statistically
different (p > 0.05). Means represented by the same Greek letter
among Ts = 5 and 25 °C for each cooling rate and MG concentration
indicate that the samples are not statistically different (p > 0.05).
3. Results and discussion
Table 2 presents the FFA, MAG, DAG, and TAG composition of MG,
HOSO, and the sonicated and non-sonicated O6-F samples. HOSO is
mainly composed of TAG, being the predominant species OOO, fol-
lowed by POO, OOL, POL, and StOO, whereas Myverol is based on MAG
(95.64 ± 1.33%). It is important to point out that both MG and HOSO
are composed of minority compounds (FFA and DAG, in the case of
Myverol, and FFA, MAG and DAG, in the case of HOSO), which could
contribute to the oleogel final structure, even though they are present in
a low proportion. It was found that HIU application did not change
significantly the chemical composition of oleogels (p > 0.05), which
was an expected result since we recorded temperature increments of
about 2–5 °C during sonication. However, it is important to mention
that temperature increments could modify the MG crystallization pro-
cess. Therefore, the effects reported in this paper as “with HIU” include
both pressure and temperature changes during HIU application.

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A. Giacomozzi, et al. Food Research International 134 (2020) 109231

Table 2
Mean composition of monoglycerides (MG), high oleic sunflower oil (HOSO) and oleogels formulated with 6 wt% of MG produced at fast cooling rate (F: fast, 10 °C/
min) without (wo) high intensity ultrasound (HIU) and with HIU.
Componentα MG HOSO Oleogels

O6-F-wo HIU O6-F-with HIU

FFA 2.70 ± 0.05 2.88 ± 0.19 5.28 ± 0.60a 4.64 ± 0.81a

MAG 95.64 ± 1.33 0.56 ± 0.12 6.31 ± 0.37a 5.00 ± 0.69a
DAG 1.66 ± 0.15 1.78 ± 0.19 1.88 ± 0.11a 1.64 ± 0.05a
TAG 0.00 ± 0.00 94.78 ± 0.50 86.54 ± 0.11a 88.72 ± 1.54a

Data are expressed as mean values ± standard deviations. Means represented by the same lowercase letters within each row indicate that the samples are not
statistically different (p > 0.05).
α
FFA: free fatty acids, MAG: monoacylglycerols, DAG: diacylglycerols, TAG: triacylglycerols.

Fig. 1. Effect of high intensity ultrasound (HIU) application on the melting profiles of O3 (grey lines) and O6 (black lines) monoglycerides oleogels under different
processing conditions: without HIU (wo HIU) and with HIU and storage at two different temperatures (Ts). (A) 0.1 °C/min- Ts = 25 °C, (B) 10 °C/min- Ts = 25 °C, (C)
0.1 °C/min- Ts = 5 °C, (D) 10 °C/min- Ts = 5 °C. Please refer to Table 1 for samples’ nomenclature.

3.1. Tc and melting behavior
MG used in this work had a MP of 68.9 ± 0.2 °C. Tc values, cor-
responding to a 48% of crystallization, were 38.3 ± 0.6, 41.4 ± 0.6,
and 45.0 ± 0.4 °C for the O3, O4.5, and O6 samples, respectively.
All melting thermograms showed a single endothermic peak (Fig. 1)
corresponding to the melting of monoglycerides as previously reported
(Giacomozzi et al., 2019). ΔHM represents the energy absorbed during
melting, being dependent on the amount of crystalline material in the
sample and on the structural order of the crystalline network
(Toro‐Vazquez et al., 2007). No significant changes were observed in
ΔHM values as a function of sonication (Fig. 2), in accordance with our
previous work (Giacomozzi et al., 2019), except for O6 crystallized at
both cooling rates and stored at 25 °C. Even though SFC of O6 sonicated
samples was not significantly different from the non-sonicated one
(section 3.3), ΔHM decreased by using HIU. A lower ΔHM means that
less energy is needed to melt the same amount of crystals (same SFC)
suggesting that a weaker crystalline network was formed. Moreover,
lower To was obtained in O6 samples due to sonication (Table 3). A
decrease in To means that the sample starts melting at lower tempera-
tures suggesting that either molecular entities with lower melting
points are being melted or that the crystalline network is weaker. Based
on the fact that sonicated O6 oleogels showed smaller Lc (section 3.2),
which resulted in a stronger crystalline network (higher HA and higher
G', sections 3.5 and 3.6) compared to the correspondent non-sonicated
samples, it is likely that lower melting point compounds either from the
oil (FFA, MAG and/or DAG or even minor TAG such as SOO or POO) or
from the MG (specially FFA) were incorporated in the oleogels network.
da Silva, Cooper, Lee, Gibon, and Martini (2020) also reported changes
in physical properties of an interesterified soybean oil due to HIU

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A. Giacomozzi, et al. Food Research International 134 (2020) 109231

Fig. 2. Effect of high intensity ultrasound (HIU) application on the melting enthalpy (ΔHM) of oleogels with different monoglyceride concentrations (MG (wt%))
measured at two storage temperatures (Ts). White and black bars represent samples obtained without HIU (wo HIU) and with HIU, respectively. Different processing
conditions were tested: Ts = 25 °C, at (A) 0.1 °C/min and (B) 10 °C/min, and Ts = 5 °C at (C) 0.1 °C/min and (D) 10 °C/min. For statistical comparisons please refer to
section 2.4.

Table 3
Peak (Tp) and onset (To) temperatures of the oleogels obtained under different processing conditions at different storage temperatures (Ts, 5 and 25 °C).
Sample Tp (°C) To (°C)

5 °C 25 °C 5 °C 25 °C

bAα dAα bAα

O3-S-wo HIU 59.9 ± 0.9 58.3 ± 0.6 44.7 ± 1.8 43.2 ± 0.3cAα
O3-F-wo HIU 59.0 ± 0.2cAα 57.7 ± 1.4bAα 42.0 ± 1.3bABα 42.5 ± 0.4cAα
O3-S-with HIU 56.8 ± 1.1bBα 56.3 ± 0.5eAα 41.4 ± 1.0bABβ 44.6 ± 0.1cAα
O3-F-with HIU 57.1 ± 0.8dAα 56.7 ± 0.1bAα 40.6 ± 1.1bBβ 44.5 ± 1.2bcAα
O4.5-S-wo HIU nd 62.2 ± 0.6bA nd 43.8 ± 0.6cA
O4.5-F-wo HIU nd 60.0 ± 1.2abB nd 45.1 ± 1.0bA
O4.5-S- with HIU nd 59.8 ± 0.2cA nd 45.4 ± 2.6cA
O4.5-F- with HIU nd 59.9 ± 0.9abA nd 47.4 ± 2.1bA
O6-S-wo HIU 63.3 ± 0.6aAα 63.7 ± 0.4aAα 50.6 ± 1.6aAα 54.4 ± 1.3aBα
O6-F-wo HIU 62.2 ± 0.4aAα 62.3 ± 0.7aBα 49.0 ± 0.4aAβ 57.8 ± 0.1aAα
O6-S-with HIU 61.8 ± 1.2aAα 60.7 ± 0.2cAα 49.2 ± 0.3aAα 49.9 ± 0.4bAα
O6-F-with HIU 60.8 ± 0.4bBα 61.7 ± 0.4aAα 50.8 ± 0.5aAα 49.4 ± 1.0bAα

Data are expressed as mean values ± standard deviations of three replicates. nd: Not determined. Please refer to Table 1 for samples’ nomenclature and to section
2.4 for statistical comparisons nomenclature.

application, which promoted the crystallization of low melting TAG
such as monosaturated-diunsaturated TAG.
ΔHM was not different between fast and slowed cooled samples nor
between samples stored at 5 and 25 °C, except for O6 sonicated sam-
ples. The increment in ΔHM in these samples as Ts decreased could be
related to an increment in SFC and G' as will be discussed below.
HIU significantly lowered Tp values in oleogels obtained at 0.1 °C/
min and stored at 25 °C, but remained unchanged in fast-cooled samples
(Table 3). This is an expected result since samples that have been cooled
slowly had more time to allow for molecular arrangement during
cooling and HIU might have helped in the incorporation in the crys-
talline network of lower melting point compounds present in the MG
commercial mixture or even in the oil source. A decrease in Tp due to
sonication was also previously reported by Jana and Martini (2014).
Moreover, a decrease in To for O6 at 25 °C was observed at both cooling
rates due to HIU application, and no significant differences were found

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A. Giacomozzi, et al. Food Research International 134 (2020) 109231

Fig. 3. Polarized light microscopy images and visual appearance of oleogels (O3, O4.5, O6) stored for 24 h at 25 °C as a function of cooling rate (0.1 and 10 °C/min)
and high-intensity ultrasound (HIU) application: without HIU (wo HIU) and with HIU. Images were taken at 10X magnification. Lc (crystals length) and S (span) are
the parameters used to describe the crystal size distribution. For samples' nomenclature please refer to Table 1.

in To for O3 and O4.5. It seems possible that these results are related to
the promotion of crystallization of low-melting point components from
HOSO (as it was discussed above) that were incorporated in the crys-
talline matrix during crystallization and/or from MG such as FFA
(Table 2) at the highest concentration (higher saturation level) which
do not crystallize without HIU (Ye & Martini, 2014).
In general, neither Tp nor To were affected by cooling rate and Ts.
Some exceptions were found in non-sonicated samples: the increment in
cooling rate significantly increased To in O6 and decreased Tp in O4.5
and O6, and in sonicated samples: To decreased as Ts decreased in O3 at
both cooling rates. Storage at lower Ts may induce the co-crystallization
of lower melting point compounds present in the oil, which may be
favored by sonication.
3.2. Microstructure and visual appearance
HIU reduced Lc for all MG concentrations at both Ts, and mainly in
slow-cooled samples (Figs. 3 and 4). A lesser effect of HIU on Lc was
observed for O3 cooled at 10 °C/min. For samples stored at 25 °C, HIU
formed a visually stronger network compared to non-sonicated samples
avoiding flow of the sample when it is inverted, particularly in those
formulated at 0.1 °C/min. This finding was in accordance with fractal
dimension results. Higher D values were obtained as consequence of
HIU application at the slow cooling rate. This parameter significantly

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A. Giacomozzi, et al. Food Research International 134 (2020) 109231

Fig. 4. Polarized light microscopy images and visual appearance of oleogels (O3, O6) stored for 24 h at 5 °C as a function of cooling rate (0.1 and 10 °C/min) and
high-intensity ultrasound (HIU) application: without HIU (wo HIU) and with HIU. Images were taken at 10X magnification. Lc (crystals length) and S (span) are the
parameters used to describe the crystal size distribution. For samples' nomenclature please refer to Table 1.

increased due to sonication from 2.36 ± 0.01 to 2.67 ± 0.0,
2.62 ± 0.01 to 2.67 ± 0.01, and 2.64 ± 0.02 to 2.70 ± 0.01, in O3,
O4.5, and O6, respectively. Thus, the sonicated samples showed smaller
Lc and more homogenous distribution in accordance with a higher
fractal dimension, allowing the formation of a material that has a
stronger network (Blake & Marangoni, 2014).
MG formed irregular elongated needle‐like crystals similar to the
ones observed in MG/olive oils oleogels (Kesselman & Shimoni, 2007).
Non-sonicated samples showed spherulitic clusters formed by the ag-
gregation of the needle-like crystals that were not present in sonicated

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A. Giacomozzi, et al.
Fig. 5. Effect of high-intensity ultrasound (HIU) application on the solid fat content (SFC) of oleogels with different monoglyceride concentrations (MG (wt%)) stored
at two different temperatures (Ts). White and black bars represent samples obtained without HIU (wo HIU) and with HIU, respectively. Different processing
conditions were tested: Ts = 25 °C, at (A) 0.1 °C/min and (B) 10 °C/min, and Ts = 5 °C (C) at 0.1 °C/min and (D) 10 °C/min. For statistical comparisons please refer to
section 2.4.
samples. Similar results were reported by Bin Sintang, Rimaux, Van de
Walle, Dewettinck, and Patel (2017) in MG/phytosterols oleogels. For
non-sonicated samples, the increase in cooling rate produced a decrease
in Lc, in accordance with many gel systems (Toro-Vazquez et al., 2013).
For sonicated samples, the behavior changed: bigger crystals were
formed as cooling rate increased for O3 samples suggesting that HIU
was less efficient at reducing crystal size under these conditions. No
changes in Lc were found in O4.5 and O6 samples due to increasing
cooling rate. Previous studies performed in triacylglycerols have shown
that HIU is more efficient at inducing crystallization and changing
physical properties in samples with a slow crystallization kinetics
(Kadamne, Ifeduba, Akoh, & Martini, 2017). Slower crystallization ki-
netics can be obtained, for example, by either working at a low driving
force, or by using slow cooling rates. In our work, the lowest MG
concentration and the slow cooling rate in O3-S samples allowed a more
effective HIU application.
Regarding to S values, since this parameter is an indicator of the
width of a particle size distribution, the results showed all oleogel
samples exhibited narrow distributions (Rattes & Oliveira, 2007).
Storage at a lower temperature decreased Lc, except for O6-F soni-
cated and non-sonicated samples where bigger crystals were obtained.
Visual inspection of samples was in accordance with these results.
Oleogels stored at 25 °C appeared to be less structured with greasy
aspect, showing a shiny gloss when compared to the ones stored at 5 °C.
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Food Research International 134 (2020) 109231
3.3. Solid fat content (SFC)
HIU significantly increased SFC of only the O3 samples obtained at
10 °C/min and stored at 25 °C (Fig. 5) suggesting that sonication pro-
moted crystallization in these conditions. Similar interpretation has
been previously reported (Suzuki, Lee, Padilla, & Martini, 2010).
However, no significant differences were observed between SFC of the
remaining fast-cooled sonicated and non-sonicated samples nor in O3
and O6 slow-cooled samples as also reported da Silva et al. (2019) for
similar conditions. Surprisingly, a lower SFC was observed due to HIU
in O4.5 crystallized at 0.1 °C/min and stored at 25 °C. It is unclear why
HIU resulted in a lower SFC in these samples: possibly, the acoustic
waves dissolved some of the crystals in the samples instead of inducing
their crystallization. Even though SFC was lower in these sonicated
samples, a significant effect due to HIU application on Lc and mor-
phology was observed (Fig. 3). In general, no significant differences
were found in SFC among samples crystallized at 0.1 and 10 °C/min and
stored at 25 °C, except for O3 and O4.5 non-sonicated samples, where
SFC decreased as cooling rate increased. This result may be related to
the time in which molecular organization took place prior to formation
of nuclei. At 0.1 °C/min, molecules might have more time to interact
and form more crystals, compared with the crystallization at 10 °C/min.
Ts modified SFC in O3 fast-cooled samples and in O6. For O3-F, HIU
induced crystallization at Ts = 25 °C but the low supercooling in the
A. Giacomozzi, et al. Food Research International 134 (2020) 109231

Table 4 system did not allow for further crystallization to occur (Ye et al.,
Short d-spacings identified from XRD measurements of the oleogels with dif- 2011). Interestingly, a higher level of SFC can be obtained at 25 °C in
ferent monoglyceride concentration (O3, O6) under different processing con- the sonicated sample compared to the samples stored at 5 °C. For both
ditions: without (wo) high intensity ultrasound (HIU), and with HIU. Two cooling rates and sonication conditions, storage of O6 at 5 °C caused an
cooling rates (S: slow, 0.1 °C/min and F: fast, 10 °C/min) and two storage
increase in SFC compared to Ts = 25 °C suggesting that these samples
temperatures (Ts, 5 and 25 °C) were tested.
continued to crystallize at lower Ts due to a higher driving force. This
Samples d (Å) Polymorphic Form effect was also observed in ΔHM.
Ts = 25 °C
O3-S-wo HIU 3.74–3.93–4.31 β'
O3-F-wo HIU 3.75–3.94–4.28 β' 3.4. X-ray analysis
O3-S-with HIU 3.85–4.34 β'
O3-F-with HIU 3.72–3.91–4.29 β' Non-sonicated samples showed a β' polymorph with characteristic
O6-S-wo HIU 3.73–3.90–4.29 β'
peaks at 3.8 and 4.2 Å (Table 4). Similar findings were reported in MG/
O6-F-wo HIU 3.73–3.91–4.31 β'
O6-S-with HIU 3.89–4.31–4.55 β' - β cod liver oil oleogels (Da Pieve et al., 2011). The texture of a β' crystal
O6-F-with HIU 3.89–4.33–4.52 β'-β gives the smooth structure of margarines, and thus is the desired
Ts = 5 °C polymorphism in oleogels obtained for shortening replacement pur-
O3-S-wo HIU 3.45–3.74–4.29 β' poses (Ferro, Okuro, Badan, & Lopes Cunha, 2019). HIU did not change
O3-F-wo HIU 3.74–3.94–4.28 β'
the polymorphism in O3. At the highest MG concentration sonication
O3-S-with HIU 3.58–3.72–3.90 β'
O3-F-with HIU 3.33–3.73–3.93–4.30 β' promoted the formation of the β form (d = 4.5 Å) and the coexistence
O6-S-wo HIU 3.73–3.92 β' of β' and β forms. Since no fractionation was observed in the melting
O6-F-wo HIU 3.74–3.92–4.28 β' profiles (Fig. 1) it is likely that β' was the predominant form in all
O6-S-with HIU 3.94–4.54 β' samples as confirmed by the lower Tp values observed in sonicated
O6-F-with HIU 3.75–3.94–4.28–4.55 β' - β
samples processed at 0.1 °C/min.
Please refer to Table 1 for samples’ nomenclature and to section 2.4 for sta- No changes in polymorphism were observed due to cooling rate and
tistical comparisons nomenclature. Ts, in accordance with Da Pieve et al. (2011).

Fig. 6. Effect of high-intensity ultrasound (HIU) application on the hardness (HA) of oleogels with different monoglyceride concentrations (MG (wt%)) stored at two
different temperatures (Ts). White and black bars represent samples obtained without HIU (wo HIU) and with HIU, respectively. Different processing conditions were
tested: Ts = 25 °C, at (A) 0.1 °C/min and (B) 10 °C/min, and Ts = 5 °C (C) at 0.1 °C/min and (D) 10 °C/min. For statistical comparisons please refer to section 2.4.

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A. Giacomozzi, et al. Food Research International 134 (2020) 109231

Table 5
Adhesiveness (AD) and cohesiveness (CO) of the oleogels obtained under different processing conditions at different storage temperatures (Ts, 5 and 25 °C).
Sample AD (N.s) CO

5 °C 25 °C 5 °C 25 °C

cAα eBβ abAα

O3-S-wo HIU 1.53 ± 0.21 * 0.40 ± 0.03 *cBβ
O3-F-wo HIU 0.61 ± 0.07cBα 0.24 ± 0.03fAβ 0.40 ± 0.02bAβ 0.50 ± 0.03abAα
O3-S-with HIU 2.05 ± 0.49cAα 0.92 ± 0.10cAβ 0.42 ± 0.03aBβ 0.74 ± 0.04aAα
O3-F-with HIU 2.55 ± 0.17bAα 0.37 ± 0.03eBβ 0.52 ± 0.03aAα 0.55 ± 0.03aBα
O4.5-S-wo HIU nd 0.02 ± 0.01eB nd 0.52 ± 0.05bA
O4.5-F-wo HIU nd 1.66 ± 0.10dA nd 0.51 ± 0.06abA
O4.5-S-with HIU nd 1.60 ± 0.13bB nd 0.47 ± 0.05bA
O4.5-F-with HIU nd 2.66 ± 0.09cA nd 0.50 ± 0.00abA
O6-S-wo HIU 4.29 ± 0.51bAα 0.45 ± 0.03dBβ 0.37 ± 0.01abAβ 0.49 ± 0.06bAα
O6-F-wo HIU 4.80 ± 1.33aAα 3.49 ± 0.18bAα 0.37 ± 0.07bAα 0.42 ± 0.04bcAα
O6-S-with HIU 6.07 ± 0.67aAα 3.69 ± 0.64aBβ 0.30 ± 0.02cAβ 0.44 ± 0.03bAα
O6-F-with HIU 5.32 ± 1.30aBα 4.33 ± 0.21aAα 0.24 ± 0.05cAβ 0.41 ± 0.03cAα

Data are expressed as mean values ± standard deviations. nd: Not determined. Please refer to Table 1 for samples’ nomenclature and to section 2.4 for statistical
comparisons nomenclature. *Samples were too soft to be measured.

Table 6
Tan δ and cross-over point (γG'=G'') of the oleogels with different monoglyceride concentration (O3, O4.5, O6) under different processing conditions: without (wo)
high intensity ultrasound (HIU), and with HIU. Two cooling rates (S: slow, 0.1 °C/min and F: fast, 10 °C/min) and two storage temperatures (Ts, 5 and 25 °C) were
tested.
Samples Tan δ γG'=G''(%)

25 °C 5 °C 25 °C 5 °C

aAα 01bAβ bBβ

O3-S-wo HIU 0.20 ± 0.01 0.15 ± 0. 6.9 ± 0.1 8.9 ± 0.1 bAα
O3-F-wo HIU 0.18 ± 0.03 aAα 0.10 ± 0.00 aBβ 7.8 ± 0.1 aAβ 8.8 ± 0.0 bAα
O3-S-with HIU 0.18 ± 0.00 aAα 0.10 ± 0.01 bAβ * *
O3-F-with HIU 0.19 ± 0.02 aAα 0.08 ± 0.00 aBβ * *
O4.5-S-wo HIU 0.16 ± 0.01 aAα nd 5.5 ± 0.1 cB nd
O4.5-F-wo HIU 0.16 ± 0.02 aAα nd 6.9 ± 0.1 bA nd
O4.5-S-with HIU 0.16 ± 0.01 aAα nd 8.7 ± 0.0 aB nd
O4.5-F-with HIU 0.15 ± 0.02 aAα nd 9.8 ± 0.1 bA nd
O6-S-wo HIU 0.15 ± 0.02 aAα 0.29 ± 0.03 aAβ 2.9 ± 0.1 dAβ 6.5 ± 0.6 cBα
O6-F-wo HIU 0.16 ± 0.01 aAα 0.10 ± 0.00 aBβ 2.5 ± 0.4 cAβ 8.1 ± 0.1 cAα
O6-S-with HIU 0.18 ± 0.01 aAα 0.10 ± 0.01 bAβ 5.6 ± 0.1 cBβ 9.9 ± 0.1 aBα
O6-F-with HIU 0.17 ± 0.01 aAα 0.13 ± 0.01 aBβ 6.7 ± 0.4 bAβ 9.0 ± 0.1 aAα

γ: strain. Data are expressed as mean values ± standard deviations. * absence of a cross-over point. nd: Not determined. Please refer to Table 1 for samples’
nomenclature and to section 2.4 for statistical comparisons nomenclature.

3.5. Textural properties
HA of sonicated samples stored at 25 °C was significantly higher
than non-sonicated ones and this increment was greater in slow-cooled
samples than in the fast-cooled ones (Fig. 6). This increase in HA can be
attributed to the smaller crystals generated by HIU, which have more
contact area contributing to a harder structure compared to a network
formed by larger crystals. Interestingly, O3-S-wo HIU did not show a
well-structured network and flowed after 24 h of storage at 25 °C
(Fig. 3), whereas the ones obtained under sonication did not flow,
showing a solid-like structure. Moreover, the same level of HA was
obtained in oleogels with 3 wt% MG using HIU compared to a non-
sonicated oleogel with 6 wt% of MG and a higher HA was obtained in
sonicated 4.5 wt% samples compared to non-sonicated 6 wt% (Fig. 6A).
Fast cooling rate enhanced the HA of oleogels obtained without HIU, in
accordance with Ojijo, Neeman, Eger, and Shimoni (2004). For soni-
cated samples, this trend was only found in O3, whereas no significant
differences were found in HA values of O4.5 and O6 due to cooling rate.
This was because HIU increased hardness in the slow-cooled samples in
a higher percentage than in the fast-cooled ones.
HA of oleogels stored at 5 °C was significantly higher than those
stored at 25 °C for all processing conditions tested, suggesting a re-
organization of the crystalline network during storage at 5 °C. Increased
HA at 5 °C could result from stronger non-covalent interactions and
from a higher amount of crystalline material due to an increase in the
driving force for crystallization. However, SFC did not change sig-
nificantly with storage at 5 °C in some of the samples suggesting that
other physical properties, such as crystal microstructure and/or inter-
actions, determines sample hardness.
HIU increased AD for slow- and fast-cooled samples stored at 25 °C,
being this increment greater in samples crystallized at 0.1 °C/min
(Table 5). This result may suggest that HIU generated more inter-
connections between MG crystals (in accordance with rheology results
described below) that could modify the AD of the network.
The increase in cooling rate increased AD for samples stored at
25 °C, which correlates well with HA results, except for O3-with HIU
probably due to a more disordered molecular arrangement with weaker
crystal-crystal interactions generated for the sonication evidenced by
lower elasticity values (section 3.6).
Lower Ts increased AD compared to the ones stored at 25 °C, which
was in agreement with Öǧütcü and Yılmaz (2014) in carnauba wax/
MG/olive oil oleogels. An exception to this behavior was found in O6-F-
wo HIU and O6-F-with HIU samples, which did not show significant
differences in AD due to the decrease in Ts.
In general, at Ts = 25 °C HIU did not affect significantly the CO of
oleogels (Table 5). CO is calculated by the ratio W2/W1, being W1 and
W2 the deformation work obtained during the first and second pene-
tration cycle, respectively. In this study, both parameters increased with
the use of HIU, which means that sonication allowed to strengthen the
network structure. However, since the increment was comparable in

10
A. Giacomozzi, et al.
Fig. 7. Effect of high-intensity ultrasound (HIU) application on the elastic modulus (G') of oleogels with different monoglyceride concentrations (MG (wt%)) stored at
two different temperatures (Ts). White and black bars represent samples obtained without HIU (wo HIU) and with HIU, respectively. Different processing conditions
were tested: Ts = 25 °C, at (A) 0.1 °C/min and (B) 10 °C/min, and Ts = 5 °C (C) at 0.1 °C/min and (D) 10 °C/min. For statistical comparisons please refer to section
2.4.
W1 and in W2, CO was practically not affected. Cooling rate only af-
fected CO in oleogels formulated with the lowest MG concentration. An
increase in CO was observed for O3-F-wo HIU compared to O3-S-wo
HIU stored at 25 °C, whereas the increment in cooling rate decreased
CO in O3 sonicated samples stored at 5 °C.
Contrary to HA, oleogels stored at 5 °C showed, in general, sig-
nificantly lower CO values than the ones at stored at 25 °C. The higher
HA found in fast-cooled sonicated samples and stored at 5 °C could have
accounted for the decrease of CO.
3.6. Elastic modulus (G') and loss modulus (G'')
All samples satisfied the gel definition (tan δ < 1, Table 6),
showing a solid-like behavior (Patel & Dewettinck, 2015).
At Ts = 25 °C, HIU significantly increased G' of oleogels obtained at
both cooling rates for almost all tested MG concentrations, suggesting
that HIU application allows to develop a more elastic crystalline net-
work (Figs. 7 and 2S). The cross-over point was determined for each
sample at the strain value where tan δ = 1. Higher crossover points
were found in sonicated samples (Table 6), indicating the formation of a
stronger gel and a more stable network (Doan, Van de Walle,
Dewettinck, & Patel, 2015) due to HIU application. Moreover, some
samples did not show a cross-over point over the tested strain range (O3
sonicated samples at both cooling rates and Ts), indicating that these
oleogel samples could resist higher deformation forces without
breaking down their structure. Patel, Cludts, Sintang, Lesaffer, and
Dewettinck (2014) also showed the absence of a cross-over point even
at an increased rate of deformation in oleogels from sunflower oil,
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Food Research International 134 (2020) 109231
methylcellulose and xanthan gum, and this finding was related to the
well-structured network of these materials.
These results are consistent with those observed by microscopy: a
reduction in crystal size was obtained in sonicated samples, enhancing
crystal-crystal interactions and hence increasing oleogels’ elasticity; this
was also observed by Toro‐Vazquez et al. (2007). The exception to this
behavior was found for O3 fast-cooled samples, where G' remained
unchanged due to sonication. It is possible that the decrease in Lc ob-
served for this condition was not enough to change the network elas-
ticity. The highest increment in G' due to sonication was observed for
O6 at 25 °C and it could be related to the presence of a small amount of
β crystals (as described above).
G’ increased with cooling rate even though SFC remained un-
changed or decreased. This finding was in accordance with Dibildox-
Alvarado, Rodrigues, Gioielli, Toro-Vazquez, and Marangoni (2004).
Similarly, lowering Ts from 25 to 5 °C increased G' values. For samples
stored at 5 °C, the greatest increment in elasticity due to HIU applica-
tion was obtained for the highest MG concentration by processing at
0.1 °C/min, which was in accordance with the biggest decrease in tan δ
(from 0.29 ± 0.03 for O6-S-wo HIU to 0.10 ± 0.01 for O6-S-with
HIU, Table 6). Moreover, some oleogels stored at 5 °C had tan δ ≤ 0.1
and so, they can then be considered as true gels (Patel, Babaahmadi,
Lesaffer, & Dewettinck, 2015). During storage at 5 °C, the molecular
organization in the O6 oleogels generated a more ordered structure and
a higher amount of solids resulting in an increment in the elasticity of
the network.
A. Giacomozzi, et al. Food Research International 134 (2020) 109231

Fig. 8. Effect of high-intensity ultrasound (HIU) application on the oil binding capacity (OBC) of oleogels with different monoglyceride concentrations (MG (wt%))
stored at two different temperatures (Ts). White and black bars represent samples obtained without HIU (wo HIU) and with HIU, respectively. Different processing
conditions were tested: Ts = 25 °C, at (A) 0.1 °C/min and (B) 10 °C/min, and Ts = 5 °C (C) at 0.1 °C/min and (D) 10 °C/min. For statistical comparisons please refer to
section 2.4.

3.7. Oil binding capacity (OBC) Storage of oleogels at a lower temperature resulted in higher OBC
with the highest change observed for O3-S-wo HIU. The highest OBC of
At Ts = 25 °C, OBC significantly increased with HIU at both cooling samples stored at 5 °C were found for sonicated samples (O3-S-with HIU
rates (Fig. 8), which agreed with Sharifi et al. (2018). The highest in- and O6-F-with HIU).
crement in OBC due to sonication was found in the slow-cooled sam-
ples, and it was greater as MG concentration decreased, being 59.5,
4. Conclusions
47.3, and 32.8% for O3, O4.5, and O6, respectively. These results
suggest a synergism between slow cooling rate and HIU to create a more
HIU modified MG crystallization and reduced Lc for all MG con-
effective network at structuring liquid oil. The slow cooling rate slowed
centrations, being more effective when a slow-cooling process was used
down the crystallization process before sonication in comparison to the
before applying HIU and when samples were stored at 5 °C. The re-
fast one and therefore, a greater effect of sonication was achieved. Si-
duction in crystal size resulted in a stronger crystalline network with
milar values of OBC were obtained in the sonicated O4.5 and O6 slow-
more crystal-crystal interactions and higher HA and G', allowing to
cooled samples which was not possible in our previous work
effectively entrap liquid oil even with the lowest MG concentration.
(Giacomozzi et al., 2019) showing that it could be possible to reduce
HIU favored the packing of MG crystals in a more cohesive structure
the MG amount used in oleogels without losing desired physical prop-
with similar hardness when half MG amount was used at 0.1 °C/min
erties. These results correlate well with the HA, G', and microscopy
compared to non-sonicated oleogels. Moreover, the same OBC was
findings: samples with lower Lc showed higher HA and G' values, and
produced in sonicated oleogels obtained at 0.1 °C/min with 4.5 wt% of
higher OBC.
MG compared to an oleogel with 6 wt% of MG.
In general, at Ts = 25 °C OBC significantly increased with cooling
In conclusion, HIU in combination with cooling rate can be used to
rate in non-sonicated samples. However, fast-cooled sonicated samples
tailor physical properties of monoglycerides oleogels by reducing the
showed lower (O3, O4.5) or no significant different (O6) OBC compared
amount of saturated fats in oleogels while keeping the desired physical
to the slow-cooled ones. Smaller crystals present in sonicated O3-S and
properties. We found an improvement in the hardness and elasticity of
O4.5-S samples (Fig. 3) showed higher OBC due to the higher surface
oleogeles by decreasing MG concentration from 6 to 4.5 wt% and ap-
area available to entrap oil, and to more interactions that lead to a
plying HIU at 0.1 °C/min, without changing the oil binding capacity of
stronger oleogel (Blake & Marangoni, 2015) compared to the larger
the network. These findings provide useful information for the devel-
crystals found in oleogels processed at 10 °C/min, which presented
opment of healthier food products in an attempt to reduce the content
lower OBC. At the highest MG concentration, the slight difference in Lc
of saturated fats of these products while retaining or improving their
seemed not to influence the network OBC.
technological properties. In a future work, it would be extremely

12
A. Giacomozzi, et al.
interesting to evaluate the applicability to industrial scale of the pro-
duction of MG oleogels using HIU.
Acknowledgements
This research was supported by the Utah Agricultural Experiment
Station, Utah State University, and approved as journal paper number
9243. Financial support for this research was provided by CONICET
(PIP 1122015-0100156 CO), ANPCyT (PICT 2016-0520, PICT 2017-
1522), UNS (PGI 24/M132), and Fulbright Commission of Argentina.
Conflict of interest
The authors have no conflict of interest to declare.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.foodres.2020.109231.
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