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Food Research International 122 (2019) 129–136

Contents lists available at ScienceDirect

Food Research International


journal homepage: www.elsevier.com/locate/foodres

Using canola oil hydrogels and organogels to reduce saturated animal fat in T
meat batters
Marta Alejandrea, Iciar Astiasarána, Diana Ansorenaa, , Shai Barbutb

a
Department of Nutrition, Food Science and Physiology, Faculty of Pharmacy and Nutrition, University of Navarra, Irunlarrea s/n, 31008, IDISNA – Instituto de
Investigación Sanitaria de Navarra, Pamplona, Spain
b
Food Science Department, University of Guelph, Guelph, Ontario N1G 2W1, Canada

ARTICLE INFO ABSTRACT

Keywords: Conventional canola oil and structured canola oil systems, consisting of oil in water hydrogelled emulsions (with
Carrageenan 1.5% or 3% kappa carrageenan) and ethylcellulose organogels (12%, with 0%, 1.5% or 3% glycerol mono-
Ethylcellulose stearate), were used to replace beef fat in emulsion type meat batters.
Fat replace Replacement with regular canola oil increased hardness and lightness (P < .05) of the reformulated products
Hydrogelled emulsion
as compared to those with beef fat. Structuring the oil resulted in similar color and texture (P > .05), and lower
Meat emulsion
Organogel
oxidation values (P < .05) of meat batters. Reformulated products also gave rise to a healthier fatty acid profile,
evidenced by a decrease in saturated fatty acids (SFA) from 11.8% to ≈ 2% and an increase in polyunsaturated
fatty acids (PUFA) from 0.3% to ≈ 5%. Omega-6 to omega-3 ratio also decreased (16.2 to ≈ 2) when in-
corporating canola oil into meat batters. Batters formulated with organogels showed improved matrix stability
compared to those with hydrogelled emulsions, which showed some coalescence of fat globules and fat losses
during cooking, resulting in a reduction of fat content (P < .05).

1. Introduction Different strategies based on either structured oil systems, inter-


esterification, or encapsulation have been suggested to cope with this
High intake of dietary saturated fat is of particular concern because technological problems (Kılıç & Özer, 2019). Emulsion gels have been
they are correlated with increased risk of cardiovascular diseases (Sacks successfully used to replace/reduce animal fat in comminuted meat
et al., 2017; WHO, 2003). A number of dietary guidelines recommend products (Paglarini, Martini, & Pollonio, 2019; Pintado et al., 2016;
limiting consumption of processed meats due to their high saturated fat Pintado, Herrero, Jiménez-Colmenero, & Ruiz-Capillas, 2016; Wang,
content (Aranceta-Bartrina et al., 2017; USDA, 2015). Thus, replace- Xie, Li, Liu, & Yan, 2018).
ment of saturated fats with unsaturated oils in meat products is one of Oil in water (O/W) emulsions are produced by forming a stable
the most researched options to formulate healthier products. emulsion (oil phase dispersed in a continuous phase) in the presence of
Unsaturated fats in our diet are mainly coming from plant, fish or an emulsifier, followed by emulsion gelation (Jimenez-Colmenero
algae sources. Canola oil, one of the most widely consumed vegetable et al., 2015; McClements, 2010). In the case of kappa carrageenan, this
oils in Canada, has a very low level of saturated fatty acids (SFA) and gelation is based on a conformational transition of the gum from
substantial amounts of monounsaturated fatty acids (MUFA) and random coil to double helix, upon cooling, leading to the formation of
polyunsaturated fatty acids (PUFA). an elastic gel (Stephen & Phillips, 2016). This polysaccharide gum al-
Animal fat plays an important role in formulation of products due to lows wide range of possibilities for incorporating different amounts of
its unique texture (Pehlivanoğlu et al., 2018). Previous studies reported oil (1% - 40%) and kappa carrageenan (1.5% - 3%), making it possible
that simple replacement of animal fat with vegetable oils resulted in to be used for applications such as fat reduction and lipid profile
increased hardness of cooked meat products (Barbut & Marangoni, modification.
2019; Barbut, Wood, & Marangoni, 2016a, 2016c; Youssef & Barbut, Previous studies showed that fresh and cured meat products con-
2009; Zetzl, Marangoni, & Barbut, 2012). Technological problems were taining an O/W hydrogelled emulsion (40% oil and 1.5% kappa car-
also reported by Bloukas, Paneras, and Fournitzis (1997) in dry fer- rageenan) as a partial fat replacer (up to 50%) had improved lipid
mented sausages formulated with olive oil. composition and sensory acceptability (Alejandre, Passarini, Astiasarán,


Corresponding author.
E-mail address: dansorena@unav.es (D. Ansorena).

https://doi.org/10.1016/j.foodres.2019.03.056
Received 18 January 2019; Received in revised form 14 March 2019; Accepted 25 March 2019
Available online 26 March 2019
0963-9969/ © 2019 Elsevier Ltd. All rights reserved.
M. Alejandre, et al. Food Research International 122 (2019) 129–136

& Ansorena, 2017; Alejandre, Poyato, Ansorena, & Astiasarán, 2016). Canada). Kappa carrageenan (GENU® texturizer type MB-151F) was
In addition, organogels have recently been used as another lipid provided by CP Kelco, Atlanta, (GA, USA). Polysorbate 80 was pur-
delivery system. They are formed by combining an organic liquid and chased from Sigma-Aldrich Chemical, (MO, USA). Ethylcellulose
an organogelator at specific shearing conditions, resulting in a three- (ETHOCEL Std.10 Premium) was provided by Dow Chemical, Midland,
dimensional cooled networked structure with thermo-reversible prop- (MI, USA), BHT was obtained from Thermo Fisher Scientific, (NH, USA)
erties (Jimenez-Colmenero et al., 2015; Stortz, Zetzl, Barbut, and GMS was purchased from HallStar, Bedford Park, (IL, USA).
Cattaruzza, & Marangoni, 2012).
Ethylcellulose (EC), a semi-crystalline cellulose polymer derivative, 2.3. Oil in water (O/W) hydrogelled emulsions and organogels preparation
consisting of a cellulose backbone with ethoxyl substitutions at the
hydroxyl groups, has been used as an organogelator (Koch, 1937). The two systems were formulated to supply equal amount of fat to
Texture and plasticity of vegetable oil based EC oleogels can be all the meat batter formulations. O/W hydrogelled emulsions (HG)
modulated by the addition of surfactants. Glycerol monostearate were prepared according to the method described by Poyato, Ansorena,
(GMS), for instance, is able to structure oil resulting in the formation of Berasategi, Navarro-Blasco, and Astiasaran (2014) in Pyrex beakers
a secondary network due to crystallization (Davidovich-Pinhas, Barbut, (300 g). Briefly, the oil phase containing canola oil (40%), polysorbate
& Marangoni, 2015). This surfactant has been successfully incorporated 80 (0.05%; 0.003 oil: surfactant ratio), BHT (0.01%), and the aqueous
into vegetable oil-based EC oleogels with a moderate plasticizing effect phase containing kappa carrageenan (1.5% or 3%), and deionized
(Davidovich-Pinhas, Barbut, & Marangoni, 2016). water (up to 100%) were separately heated at 80 °C. After the homo-
In comminuted meat products, ethylcellulose based organogels have genization of both phases, part of the molten gel was kept in Pyrex
shown promising results as an oil structuring agent (Barbut et al., beakers to be incorporated in the meat batters, other part split into ten
2016a, 2016c; Barbut, Wood, & Marangoni, 2016b; Zetzl et al., 2012). aliquots of 35 mL in 50 mL polypropylene centrifuge tubes (height:
However, the use of surfactants in organogels and how they affect meat 9.0 cm, diameter: 2.7 cm diameter) for the back extrusion test and sy-
products has not been investigated in depth. Overall, only the addition neresis, and the rest poured into cylindrical glass tubes (height:
of the sorbitan monostearate (SMS) surfactant has been tested in meat 14.5 cm, inside diameter:1.9 cm) lined with an aluminum foil (Gravelle,
products (frankfurters and breakfast sausages) showing similar texture Barbut, & Marangoni, 2013) for texture profile analysis. All parts of the
to full animal fat control products (Barbut et al., 2016a, 2016b). Thus, molten gels were cooled at room temperature for 2 h and stored at 4 °C
as GMS has pretty similar properties to SMS, it can be hypothesized that overnight.
GMS may also be of interest in meat products reformulation strategies. Organogels (OG) were prepared with 12% ethylcellulose (viscosity
The objective of this research was to investigate the effect of total of 10 cP), glycerol monostearate (GMS at 0%, 1.5% or 3%), 0.01%
animal fat replacement in meat batters, using two structured oil sys- butylated hydroxytoluene (BHT; to control oxidation) and canola oil
tems, namely O/W hydrogelled emulsions and organogels. In addition, (88%, 86.5% or 85%, depending on the GMS concentration) and
the effect of different amounts of carrageenan in the O/W hydrogelled heating in an oven to 140 °C according to Gravelle, Barbut, and
emulsions and GMS in the organogels were evaluated with respect to Marangoni (2012). The molten gels were split in the same proportions
the physicochemical, textural and nutritional properties of the re- as the hydrogelled emulsions into Pyrex beakers, the 50 mL poly-
formulated products. propylene tubes, and the cylindrical glass tubes. Organogels were kept
in the oven at 100 °C for 1 h, cooled at room temperature for 2 h and
2. Material and methods stored at 4 °C overnight.

2.1. Meat ingredients 2.4. Meat batters preparation

Lean beef leg muscles (semitendinosus and biceps femoris) and beef fat Seven treatments were prepared: beef fat control (BF control); ca-
trimming were obtained from the University of Guelph meat laboratory. nola oil control (CO control); two meat batters containing oil in water
The lean beef meat (72.55 ± 0.24% moisture, 24.43 ± 0.52% pro- (O/W) hydrogelled emulsions with 1.5% or 3% carrageenan (CA)
tein, and 2.08 ± 0.02% fat) and beef fat (74.82 ± 0.19% fat, (HGM-1.5% CA and HGM-3% CA); and three meat batters containing
19.34 ± 0.62% moisture and 5.04 ± 0.52% protein; AOAC, 2002a) organogels with different glycerol monostearate (GMS) concentrations
were separately chopped in a bowl chopper (Schneidmeister SMK 40, (OGM-no GMS, OGM-1.5% GMS, and OGM-3% GMS). Formulations of
Berlin, Germany) at the low speed setting for 1 min, to obtain a meat batters are shown in Table 1.
homogenous mass, and then frozen (−20 °C) in individual polyethylene Meat batters (1.5 kg batches) were formulated to contain 11%
bags (1 kg per bag) and used within 3 months. protein and 21% fat/oil. The lean meat supplied 2.08% of the fat in the
overall meat batter formulation, and the remainder (18.92%) of the
2.2. Gel systems ingredients 21% was provided by either added beef fat, liquid canola oil, a canola
oil based ethylcellulose organogel, or a canola oil based O/W carra-
Canola oil was obtained from Saporito Foods Inc., Markham, (ON, geenan hydrogelled emulsion. Meat and fat were thawed (5 °C)

Table 1
Formulations (%) of meat batters prepared with beef fat (BF); canola oil (CO); hydrogelled emulsions (HG) with different carrageenan (CA) concentrations (1.5% or
3%); and organogels (OG) with different glycerol monostearate (GMS) concentrations (1.5% or 3%).
Treatment Treatment identification Lean beef meat Beef fat Liquid canola oil Organogel (OG) Hydrogelled emulsion (HG) Ice

1 BF control 39.00 28.00 – – – 29.75


2 CO control 45.45 – 20.56 – – 30.74
3 HGM-1.5% CA 45.45 – – – 51.30 –
4 HGM-3% CA 45.45 – – – 51.30 –
5 OGM- no GMS 45.45 – – 22.84 – 28.46
6 OGM-1.5% GMS 45.45 – – 23.23 – 28.07
7 OGM-3% GMS 45.45 – – 23.63 – 27.67

All formulated with 2% salt, 1% modified starch and 0.25% sodium tripolyphosphate.

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M. Alejandre, et al. Food Research International 122 (2019) 129–136

overnight. A common procedure (Youssef & Barbut, 2009) was used to cut into 2-mm cubes and fit into a slot of the E7449 universal specimen
prepare the meat batters in three separate trials. Briefly, lean meat was stub (Quorum Technologies, Lewes, UK). A formulation of water so-
chopped in the bowl chopper (Schneidmeister SMK 40, Berlin, Ger- luble glycols and resins (Tissue-Tek O.C.T., Canempco Supplies, St.
many) at the low speed setting for 30 s, followed by the addition of Laurent, QC, Canada) was used to provide convenient specimen matrix
2.0% NaCl, 0.25% sodium tripolyphosphate and 1% modified waxy for cryostat sectioning. In both cases, the stub was placed in a cryogenic
maize starch (FIRM-TEX®; Ingredion, Westchester, IL, USA), and preparation system (Emitech K1250X, Ashford, Kent, UK) and then
chopping at high speed for 30 s. This was followed by a 1.5 min break plugged into a liquid nitrogen-slush bath at −210 °C to rapidly freeze
(allowing time for protein extraction). The fat source was then added the sample, followed by transfer to the cryogenic preparation system
and chopped at the high speed setting for 1 min, followed by ice ad- under vacuum. Samples were fractured with a razor blade and the
dition, and chopping at the high speed for 5 min. Final batter tem- frozen phase was sublimed for 5 min (OG samples) or for 30 min (HG
peratures, for all treatments, did not exceed 12 °C. Each batter was samples) at −90 °C, depending on sample composition. Samples were
vacuum-packed (150 Torr, Multivac Model A300/16, Sepp Haggen- then sputter coated with 30 nm of platinum and then transferred to the
meuller KG, Wolfertschwenden, Germany) to remove trapped air, and SEM unit (Quanta FEG 250, FEI, Hillsboro, OR, USA) to be viewed at
then nine 35-g samples were stuffed into 50 mL polypropylene tubes acceleration voltage of 10 kV and a temperature no higher than −
(height: 9 cm, diameter: 2.7 cm diameter) which were centrifuged (Fi- 120 °C.
scher Scientific, Model 225, Pittsburgh, PA) at the low speed setting for
30 s to remove any remaining small air bubbles. The tubes were cooked
2.6. Analyses of meat batters
in a water- bath set to 80 °C (Haake W-26, Berlin, Germany) from 25 °C
to 72 °C within 1.5 h. A thermocouple unit (Fluke Corporation, Model
2.6.1. Cooking loss and proximate composition
52, Everett, WA, USA) was used to monitor the core temperature of the
Cooking loss was determined as the fluid collected after heating and
samples. Samples cooked in the polypropylene tubes were kept at 4 °C
brief cooling of the polypropylene tubes (cold water for 5 min), ex-
until further analyses (cooking loss, proximate composition, TPA, back
pressed as percentage water and fat loss from the raw batter. Liquids
extrusion, color and TBARS).
were kept at 4 °C overnight, so fat/oil floated to the top, and measured
the next day.
2.5. Analyses of hydrogelled emulsions and organogels
Proximate analyses were performed on fresh meat and on cooked
meat batters according to the Official Method of Analysis AOAC
2.5.1. Texture profile analysis (TPA) and back extrusion tests
International (AOAC, 2002a; AOAC, 2002b; AOAC, 2002c; AOAC,
The mechanical properties were evaluated using two large de-
2002d).
formation techniques: texture profile analysis (TPA) and the back ex-
trusion test. Both tests were performed using a texture analyzer
(TA.TXT2, Stable Micro Systems, Texture Technologies Corporation, 2.6.2. Fatty acid profile and thiobarbituric acid-reactive-substances
Scardsdale, NY, USA). (TBARS)
For gels, samples were prepared in the cylindrical glass tubes. Fatty acid profile was determined on the lipid extracts by gas
Samples kept at 4 °C were compressed twice to 30% of their original chromatography, after initial derivatization to form fatty acid methyl
height, at a crosshead speed of 1.5 mm/s with a cylindrical probe (TA- esters (FAME), following the method of Alejandre et al. (2017).
30A, 7.6 cm diameter, 1.0 cm tall). The following parameters were re- TBARS were determined on the extracted fat of cooked meat batters
corded: hardness, springiness, cohesiveness, chewiness, gumminess, according to Maqsood and Benjakul (2010) with slight modifications
and resilience (Bourne, 1978). Nine samples per treatment were mea- reported in Poyato, Ansorena, Navarro-Blasco, and Astiasaran (2014).
sured in each of the three separate trials. The two hydrogelled emulsion
treatments were also analyzed after 10 days of storage at 4 °C to eval- 2.6.3. Texture profile analysis (TPA) and back extrusion
uate their stability. Nine cores (16 mm diameter, 10 mm high) taken from samples
Back extrusion samples were prepared in the 50 mL polypropylene cooked in the 50 mL polypropylene tubes the day before were used for
centrifuge tubes and evaluated 24 h after preparation (Zetzl et al., the TPA. Cores were compressed twice to 75% of their original height at
2012). A stainless steel probe with a cylindrical shaft (height 9.8 cm, a crosshead speed of 1.5 mm/s.
diameter 1.8 cm) and a truncated spherical tip (height 1.3 cm, diameter The back extrusion test (see conditions above) was performed on
2.0 cm) was used to penetrate 30 mm into each sample. Parameters samples cooked in the 50 mL polypropylene tubes the day before.
collected were: Young's modulus (ratio of the compressive stress to the Results were recorded as described by Gravelle, Barbut, Quinton, and
longitudinal strain; MPa) and force at maximum penetration (30 mm; Marangoni (2014).
N). Five tubes per treatment were measured in two separate trials.

2.6.4. Light microscopy


2.5.2. Syneresis- hydrogelled emulsions
Samples (approximately 2.0 × 2.0 × 0.5 cm) from the 50 mL poly-
Syneresis of carrageenan gels was measured according to Banerjee
propylene tubes were cut from the centers of cooked meat batters,
and Bhattacharya (2011) to evaluate their stability at 4 °C for 48 h. The
which were then treated and fixed following Youssef and Barbut
50 mL polypropylene tubes, containing 30 mL of carrageenan gel, were
(2009), and observed using a microscope (Model BX60, Olympus Op-
weighted (M1) and centrifuged at 5000 rpm (2800 g) for 10 min in a
tical Co, Ltd., Tokyo, Japan). Average size of fat globules was calculated
laboratory model centrifuge (Marathon 21000R, Thermo IEC, Needham
using a micrometer.
Heights, MA, USA). After centrifugation, gels along with the tubes were
weighed again after discarding the separated water (M2). Syneresis of
gel was calculated as (M1– M2)/M1 and expressed as per cent basis. 2.6.5. Color
Three polypropylene tubes per treatment were measured in two sepa- Samples (27 mm diameter, 1.0 cm height) from the 50 mL poly-
rate trials. propylene tubes were used to measure the color. Seven measurements
per treatment were done based on Holman, Collins, Kilgannon, and
2.5.3. Cryo-scanning electron microscopy- hydrogelled emulsions and Hopkins (2018), using a NIX (Nix Pro Color Sensor™, Nix Sensor Ltd.,
organogels ON, Canada) using the CIE L*a*b* system, illuminant D65 and 10°
Organogels (40–60 mg) were placed in a 5-mm high stub with single standard observer settings. Hue [tan−1 (b*/a*)] and Chroma
hole (6 mm diameter x 3 mm deep), and hydrogelled emulsions were [(a*2 + b*2)1/2] were also calculated.

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M. Alejandre, et al. Food Research International 122 (2019) 129–136

Table 2
Texture profile analysis (TPA) and back extrusion parameters of hydrogelled emulsions (HG) with different carrageenan (CA) concentrations (1.5% or 3%); and
organogels (OG) with different glycerol monostearate (GMS) concentrations (1.5% or 3%).
Parameters HG-1.5% CA HG-3% CA OG-no GMS OG-1.5% GMS OG-3% GMS SEM P value

TPA Hardness (N) 6.35 (0.12)a 15.97 (0.39)c Too soft 11.69 (0.63)b 16.43 (0.29)c 0.75 0.001
Springiness (cm) 0.97 (0.00)b 0.95 (0.00)b Too soft 0.74 (0.02)a 0.84 (0.00)ab 0.04 0.001
Cohesiveness (ratio) 0.73 (0.00)b 0.72 (0.00)b Too soft 0.45 (0.02)a 0.57 (0.00)ab 0.04 0.001
Chewiness (N cm) 4.61 (0.06)a 11.41 (0.22)b Too soft 5.19 (0.26)a 9.38 (0.57)b 0.58 0.001
Gumminess (N) 4.45 (0.07)a 10.86 (0.22)b Too soft 3.85 (0.26)a 7.88 (0.09)b 0.51 0.001
Resilience (ratio) 0.44 (0.00)b 0.41 (0.01)b Too soft 0.12 (0.01)a 0.19 (0.00)a 0.03 0.001
Back extrusion Force at maximum penetration (N) 8.95 (1.67)b 20.65 (1.19)c 0.35(0.29)a 6.74 (0.84)b 19.12 (1.5)c 2.31 0.001
Young's modulus (MPa) 1.07 (0.03)ab 1.57 (0.11)c Too soft 0.87 (0.08)a 1.31 (0.35)bc 0.15 0.001

Standard error of the mean (SEM) appear in parentheses. For each parameter, different letters in the same row indicate significant differences (P < .05) based on
post hoc Tukey test. No significant differences (P > .05) were found between trials.

2.6.6. Statistical analysis compromising the texture.


Analysis was done using the STATA/IC 12.1 program (StataCorp LP,
Texas, USA) to evaluate the random block design which included three
independent trials. One-way analysis of variance (ANOVA) was per- 3.2. Meat batters evaluations
formed to evaluate statistical significance (P < .05) among treatments.
Treatments were assigned as fixed effect and trial as a random effect. Testing for cooking loss is essential to assess the ability of a meat
Multiple comparisons of means were done by the Tukey Post Hoc system to hold water and fat during the protein denaturation phase
procedure to evaluate significance (P < .05) among treatments. Values (Tahmasebi, Labbafi, Emam-Djomeh, & Yarmand, 2016). Meat batters
reported are the mean values and standard error of the mean (SEM). A formulated with liquid canola oil (CO control) showed significantly
common SEM and P-value for all means was also calculated. lower water loss (< 1%) compared to beef fat control batters (BF
control; Fig. 2). This reduction by itself could be considered as an ad-
vantage. However, the significant increases (P < .05) in hardness and
3. Results and discussion springiness in products with liquid canola oil compared to BF control
(Table 3), showed some negative effects. These results are in agreement
3.1. Hydrogelled emulsions and organogels characteristics: texture and with previous studies showing that substitution with liquid vegetable
microstructure oil by itself resulted in much firmer comminuted meat products (Barbut
et al., 2016a; Youssef, Barbut, & Smith, 2011; Zetzl et al., 2012).
Both types of oil delivery systems were evaluated to better under- The reduction in fluid loss and the increased hardness of the CO
stand their physical properties. Texture was evaluated by TPA and back control batter can be explained by the oil globules´ size and distribution
extrusion tests in all samples except for organogel without surfactant within the matrix. Fig. 3 shows that the CO control batter (Fig. 3B) had
(OG-no GMS), which was too soft to be measured (Table 2). much smaller fat globules (average size < 50 μm), compared to fat
Addition of carrageenan (3%) and GMS (3%), in their respective oil globules in BF control batter (average size ≈100 μm; Fig. 3A). The
delivery systems, showed a clear dose-effect (P < .05) on hardness, small fat globules are covered with an interfacial protein film (IPF) and
chewiness and gumminess as compared to emulsions with 1.5% carra- hence, provided more surface for fat-protein interactions, which results
geenan or GMS (Table 2). Moreover, back extrusion data showed in- in more resistance to compression and less chance for fluid exudation
creased force and Young's modulus values at the initial state of de- during the cooking process. The same finding was reported in previous
formation, confirming the increased firmness when adding more studies using liquid oil in meat batters (Barbut et al., 2016b; Youssef &
carrageenan or GMS. These results agree with Poyato, Ansorena, Barbut, 2009).
Berasategi, et al. (2014) who pointed out the increased hardness of In order to counteract the higher hardness observed by using canola
hydrogelled emulsions with higher levels of carrageenan, and the re- oil by itself (as compared to the BF control), oil structuring systems
sults of Davidovich-Pinhas et al. (2015) who reported the effect of were employed. The hydrogelled emulsions meat products (HGM)
surfactant addition on organogel firmness. In addition, Lopez-Martínez, showed a decrease in water loss, compared to the BF control (Fig. 2).
Charó-Alonso, Marangoni, and Toro-Vazquez (2015) described a sy- Carrageenan (CA) had a positive effect on water retention. Thus, the
nergistic interaction between ethylcellulose and GMS in canola oil or- higher level of CA (3%) contributed to a 50% lower water loss com-
ganogels. An increase in gel firmness was also reported when SMS pared to 1.5% CA. However, fat was not so well retained in HGM
(surfactant) was added into ethylcellulose oleogels (Gravelle et al., products; i.e., resulting in fat losses of around 5%. Thus, HGM products
2013). In the present study, the hydrogelled emulsions (HG) showed showed higher cooking losses (fat + water) compared to BF control
higher resilience (a parameter related to the elastic recovery of the products.
sample) compared to organogels (OG), which demonstrated kappa The use of the organogel system also showed lower water losses
carrageenan's ability to produce a more elastic gel. compared to the BF control (Fig. 2). The further addition of glycerol
Differences in gel systems microstructure were also visualized monostearate (GMS) surfactant did not affect water and fat loss values.
(Fig. 1). Hydrogelled emulsions with 1.5% carrageenan showed a ty- This agrees with previous studies in which sorbitan monostearate (SMS)
pical honeycomb structure (Fig. 1A, B and C) seen after sublimation of a was added as a surfactant to a finely comminuted meat product (Barbut
high amount of water (60% within the original structure). The orga- et al., 2016a, 2016c).
nogel with 1.5% GMS (Fig. 1D, E and F) showed a rough and waxy Unlike the increased hardness of the CO control, meat batters for-
morphology due to the high oil content in the system. A fairly similar mulated with the structured oil gel systems (OGM and HGM) showed
structure of an organogel was also reported by Laredo, Barbut, and similar hardness, cohesiveness, chewiness, gumminess and resilience as
Marangoni (2011). Only two gel systems were selected since the other the BF control (P > .05; Table 3). This is desirable as it demonstrates
gels showed similar microstructure. These structured oil systems were that vegetable oil can be used, when incorporated into a meat gel
later incorporated into our test meat formulations as total animal fat system, without negatively affecting texture. The back extrusion test
replacers, with the ultimate goal of improving the lipid profile without showed that penetration force was similar in HGM and OGM-no GMS

132
M. Alejandre, et al. Food Research International 122 (2019) 129–136

Fig. 1. Scanning electron micrographs of hydrogelled emulsion (HG) with 1.5% carrageenan (A, B, C); and organogel (OG) with 1.5% glycerol monostearate (GMS)
(D,E,F), at three magnifications (2000x, 10,000x and 20,000x), respectively.

compared to the force used for the BF control, but lower values were resulted in similar L* values compared to the BF control. Redness and
noticed in organogel batters with GMS. However, as was previously yellowness values (a*, b*) were significantly lower in the CO control as
pointed out, these differences were not noticed in hardness measured compared to the BF control. However, these differences were not no-
by TPA. Barbut et al. (2016b) also reported that the addition of orga- ticed in OGM. Wolfer, Acevedo, Prusa, Sebranek, and Tarté (2018) also
nogels containing a SMS surfactant, to breakfast sausages, did not affect reported lighter and less red frankfurters formulated with soybean oil as
the hardness of the products. replacer of animal fat compared to control, even in treatments where
The similar textural properties of OGM and the BF control product the oil was structured with rice bran wax. As expected, a decrease in fat
may also be explained by looking at microscopy results. Fig. 3E and F globules size was also observed in soybean oil frankfurters.
show the microstructure of organogel meat batters formulated with Despite the similar texture of HGM, compared to BF control, light
0.0% GMS and 1.5% GMS, respectively (3% GMS is not shown; as its micrographs showed some irregular shaped fat globules and some
structure resembles the 1.5% GMS). Increases of fat globules size, coalescence in the CA added treatments (Fig. 3C and D). This helps to
compared with the CO control, gave rise to a lower IPF surrounding the explain the fat losses observed in these treatments. In any case, this fat
globules and hence, lower hardness of these products. morphology did not affect the color of HGM (P > .05; Table 4).
The size of fat globules can also be used to explain the differences A possible explanation for the fat destabilization in these products
observed in lightness among formulations (Table 4). CO control and could be related to the addition of Polysorbate 80, as surfactant, in the
meat batter with organogel (without GMS) showed lighter appearance hydrogelled emulsions. Previous studies reported a protein matrix ag-
as compared to the rest of the products, since more light reflectance is gregation and high cooking losses in meat batters when this surfactant
related to smaller fat globules (Youssef & Barbut, 2010). Meanwhile, was added (Youssef et al., 2011).
increases of fat globules size in meat batters with organogels plus GMS Nevertheless, in order to clarify the potential origin of the instability

Fig. 2. Fat and water losses (%) of meat batters prepared with
beef fat (BF); canola oil (CO); hydrogelled emulsion (HGM)
with different carrageenan (CA) concentrations (1.5% or 3%);
and organogel (OGM) with different glycerol monostearate
(GMS) concentrations (1.5% or 3%). Means (n = 9) related to
fluid loss with same lower case are not significantly different
(P < .05). Means (n = 9) related to fat loss with same capital
letter are not significantly different (P < .05). Error bars
show the standard error of the mean.

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Table 3
Texture profile analysis (TPA) parameters and force of back extrusion of cooked meat batters prepared with beef fat (BF); canola oil (CO); hydrogelled emulsions
(HGM) with different carrageenan (CA) concentrations (1.5% or 3%); and organogels (OGM) with different glycerol monostearate (GMS) concentrations (1.5% or
3%).
Treatment 1 2 3 4 5 6 7

Treatment identification BF control CO control HGM-1.5% CA HGM-3% CA OGM- no GMS OGM-1.5% OGM-3% GMS SEM P value
GMS

TPA Hardness (N) 14.78 (0.54)ab 20.72 (0.98)c 14.55 (0.53)ab 15.77 (1.03)ab 17.61 (0.39)b 13.57 (0.61)a 14.62 (0.62)a 0.35 0.001
Springiness (cm) 0.62 (0.05)a 0.88 (0.01)c 0.82 (0.43)bc 0.77 (0.01)abc 0.75 (0.05)abc 0.68 (0.02)ab 0.71 (0.04)abc 0.02 0.003
Cohesiveness (ratio) 0.22 (0.01)ab 0.28 (0.01)b 0.25 (0.02)ab 0.25 (0.01)ab 0.23 (0.01)ab 0.20 (0.01)a 0.23 (0.02)ab 0.01 0.028
Chewiness (N cm) 2.11 (0.36)a 5.14 (0.37)a 4.43 (1.73)a 3.31 (0.55)a 3.28 (0.58)a 1.75 (0.24)a 2.35 (0.34)a 0.35 0.104
Gumminess (N) 3.36 (0.27)a 5.86 (0.38)a 5.24 (1.79)a 4.26 (0.71)a 4.31 (0.49)a 2.55 (0.30)a 3.22 (0.26)a 0.35 0.104
Resilience (ratio) 0.07 (0.00)ab 0.09 (0.00)b 0.08 (0.01)a 0.07 (0.00)ab 0.07 (0.00)ab 0.06 (0.00)a 0.07 (0.01)ab 0.00 0.059
Back extrusion Force (N) 46.42 (0.89)c 52.81 (1.47)d 43.21 (1.56)c 44.71 (1.55)c 42.53 (1.33)bc 33.27 (0.89)a 36.40 (1.40)ab 1.21 0.000

Standard error of the mean (SEM) appear in parentheses. For each parameter, different letters in the same row indicate significant differences (P < .05) based on
post hoc Tukey test. No significant differences (P > .05) were found between trials.

of meat batters formulated with the hydrogelled system (i.e., with below 5 °C. However, meat batters formulated with hydrogelled emul-
carrageenan) their stability was monitored after 10 days storage at 4 °C sions reached temperatures of 10 °C to 12 °C. This might have affected
(TPA test and syneresis after centrifugation). No significant differences the protein extraction and the emulsification process. In this regard, it
in TPA parameters were found before and after storage at both CA has been indicated that protein extraction is enhanced at temperatures
concentrations (data not shown for the 10th day). Syneresis was low for of 2 °C to 4 °C (Barbut, 2015; Schmidt, 1984). The reason for reaching a
both HG products (2.96% and 1.85% at 1.5% and 3% CA, respectively). higher temperature was that no ice was added to the carrageenan
Consequently, this gel delivery system seemed not to be the cause of treatments as that water was already incorporated during emulsion
instability. These findings suggest that the origin of destabilization is preparation (Table 1).
affected by the manufacturing process and therefore further study is As the goal of the study was to improve the fatty acid composition of
needed. It is also interesting to note that the meat batters with beef fat, meat batters, (i.e., via using canola oil as an animal fat replacer),
canola oil and organogels showed a final end chopping temperature changes in the nutritional profile were also determined (Table 5).

Fig. 3. Light micrographs of cooked meat batters prepared with beef fat (A); canola oil (B); hydrogelled emulsion with 1.5% carrageenan (C); hydrogelled emulsion
with 3% carrageenan (D); organogel without glycerol monostearate (GMS) (E); and organogel with 1.5% GMS (F). Scale bar, 200 μm.

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Table 4
Color parameters of cooked meat batters prepared with beef fat (BF); canola oil (CO); hydrogelled emulsions (HGM) with different carrageenan (CA) concentrations
(1.5% or 3%); and organogels (OGM) with different glycerol monostearate (GMS) concentrations (1.5% or 3%).
Treatment 1 2 3 4 5 6 7

Treatment identification BF control CO control HGM-1.5% CA HGM-3% CA OGM- no GMS OGM-1.5% GMS OGM-3% GMS SEM P value

L* 63.03 (0.04)a 74.28 (0.32)c 68.95 (3.47)abc 64.91 (1.07)a 71.72 (0.45)c 69.22 (0.14)ab 71.10 (0.25)ab 0.92 0.000
a* 7.50 (0.12)b 5.70 (0.05)a 6.88 (0.75)ab 7.15 (0.23)ab 6.78 (0.28)ab 7.20 (0.16)ab 6.95 (0.20)ab 0.16 0.045
b* 10.00 (0.07)b 8.78 (0.18)a 10.18 (0.43)b 10.68 (0.14)b 9.90 (0.05)b 10.05 (0.13)b 10.01 (0.09)b 0.13 0.001
Hue 53.14 (0.39)a 56.98 (0.53)a 56.18 (1.94)a 56.19 (0.91)a 55.60 (0.96)a 54.38 (0.68)a 55.22 (0.94)a 0.42 0.220
Chroma 12.50 (0.11)a 9.55 (1.07)a 11.72 (0.64)a 12.69 (0.30)a 10.95 (0.90)a 11.45 (0.95)a 11.08 (1.06)a 0.33 0.184

Standard error of the mean (SEM) appear in parentheses. For each parameter, different letters in the same row indicate significant differences (P < .05) based on
post hoc Tukey test. No significant differences (P > .05) were found between trials.

Table 5
Proximate composition (%), lipid profile (%) and lipid oxidation (mg MDA/kg product) of cooked meat batters prepared with beef fat (BF); canola oil (CO);
hydrogelled emulsions (HGM) with different carrageenan (CA) concentrations (1.5% or 3%); and organogels (OGM) with different glycerol monostearate (GMS)
concentrations (1.5% or 3%).
Treatment 1 2 3 4 5 6 7

Treatment identification BF control CO control HG-1.5%CA HG-3%CA OG-no GMS OG-1.5%GMS OG-3%GMS SEM P value

Protein (%) 13.32 (0.12)a 13.58 (0.23)a 12.62 (0.23)a 12.12 (0.31)a 13.41 (0.25)a 13.56 (0.33)a 13.27 (0.14)a 0.09 0.478
Moisture (%) 62.13 (0.44)b 63.57 (0.83)bc 66.73 (1.08)c 65.12 (1.26)c 60.87 (0.23)a 59.82 (0.40)a 59.23 (0.48)a 0.45 0.004
Fat (%) 23.29 (1.03)c 21.94 (0.75)c 16.73 (0.89)a 18.28 (1.19)ab 20.82 (0.19)bc 21.39 (0.16)c 21.85 (0.37)c 0.35 0.005
SFA 11.79 (0.10)d 2.37 (0.08)c 1.57 (0.05)a 1.72 (0.04)ab 1.97 (0.03)bc 2.01 (0.07)bc 2.12 (0.02)bc 0.91 0.001
MUFA 9.87 (0.09)a 14.04 (0.10)c 10.48 (0.10)ab 11.77 (0.13)b 13.31 (0.01)c 13.25 (0.20)c 13.74 (0.10)c 0.38 0.001
PUFA 0.31 (0.04)a 5.45 (0.18)b 4.59 (0.03)b 4.72 (0.04)b 5.47 (0.16)b 5.75 (0.24)b 5.93 (0.13)b 0.47 0.001
Omega-3 0.02 (0.00)a 2.29 (0.01)b 1.51 (0.00)b 1.22 (0.04)b 2.00 (0.01)b 1.89 (0.07)b 1.92 (0.00)b 0.18 0.001
Omega-6 0.26 (0.00)a 3.14 (0.16)b 3.08 (0.00)b 3.49 (0.16)bc 3.45 (0.15)bc 3.85 (0.03)c 3.99 (0.04)c 0.31 0.001
Omega-6/omega-3 16.21 (0.33)b 1.37 (0.06)a 2.05 (0.00)a 2.87 (0.10)a 1.73 (0.07)a 2.03 (0.00)a 2.08 (0.00)a 1.46 0.001
PUFA/SFA 0.03 (0.00)a 2.31 (0.16)b 2.92 (0.01)b 2.75 (0.09)b 2.78 (0.12)b 2.85 (0.02)b 2.80 (0.01)b 0.26 0.001
PUFA + MUFA/SFA 0.86 (0.01)a 8.25 (0.33)b 9.57 (0.12)b 9.60 (0.27)b 9.54 (0.15)b 9.42 (0.010)b 9.27 (0.00)b 0.78 0.001
trans 1.31 (0.04)b 0.04 (0.00)a 0.08 (0.00)a 0.07 (0.00)a 0.07 (0.00)a 0.09 (0.00)a 0.11 (0.00)a 0.11 0.001
TBARS (mg MDA/kg product) 0.84 (0.02)b 1.04 (0.12)b 0.37 (0.06)a 0.48 (0.06)a 0.45 (0.03)a 0.38 (0.08)a 0.42 (0.01)a 0.07 0.284

Standard error of the mean (SEM) appear in parentheses. For each parameter, different letters in the same row indicate significant differences (P < .05) based on
post hoc Tukey test. No significant differences (P > .05) were found between trials. SFA = saturated fatty acids; MUFA = monounsaturated fatty acids;
PUFA:polyunsaturated fatty acids; TBARS = thiobarbituric acid reactive substances; MDA:malonhaldeyde.

Saturated fatty acids (SFA) went down from 11.8% (BF control) to 4. Conclusion
≈2% (all reformulated products), whereas PUFA increased from 0.3%
to ≈5%. Thus, higher unsaturated fraction (MUFA+PUFA) was Two promising structured oil gel delivery systems (organogels and
achieved when canola oil was incorporated, mainly due to the high hydrogelled emulsions) prepared with different technological strate-
levels of oleic (omega-9), linoleic (omega-6) and alpha-linolenic gies, showed adequate properties to be used as total fat replacements in
(omega-3) acids (Table S1, Supplementary material). It is also im- comminuted meat batters. Using liquid canola oil by itself (i.e., un-
portant to mention that the addition of alpha-linolenic acid resulted in structured) resulted in undesirable attributes (e.g., texture and color)
decreasing the omega-6/omega-3 ratio (from 16.2 to ≈2). that could be improved by structuring the oil as organogels or hydro-
Fat losses during cooking led to a lower fat content in products gelled emulsions. These gel systems also improved the fatty acid profile
formulated with hydrogelled emulsions (Table 5). However, fat content of meat batters and reduced lipid oxidation. Organogels were more
in treatments 2, 5, 6 and 7 were not significantly different (P > .05) efficiently incorporated into the meat matrix than hydrogelled emul-
compared to the BF control. sions, showing a more uniform microstructure, and without fat losses
Increasing unsaturated fatty acids levels can sometime induce lipid from the cooked meat batters.
oxidation. However, incorporating canola oil did not show an adverse
effect on TBARS values of meat batters (P > .05). Moreover, oil
structuring strategies significantly reduced TBARS values (P < .05; Acknowledgements
Table 5) as compared to the animal fat containing product or to liquid
canola oil addition. This reduction may be explained by the addition of We thank the Ministerio de Economía y Competitividad- Spain
BHT, helping to control lipid oxidation during gel and meat product (AGL2014–52636-P) for the financial support. We are grateful to “Red
preparation. In particular, this may have occurred in the organogels, de Excelencia Consolider” PROCARSE (AGL2014-51742-REDC) and
which were prepared by heating to 140 °C, and where the use of an INPROCARSA (AGL2017-90699-REDC). M. Alejandre is grateful to
antioxidant (BHT) was definitely needed. Gravelle et al. (2012) re- “Asociación de Amigos de la Universidad de Navarra” for the pre-doc-
ported a significant increase in oxidation by products if an antioxidant toral fellowship. Gobierno de Navarra (Departamento de Educación) is
is not added during organogel preparation. Cooked meat products with also acknowledged for the mobility fellowship to M. Alejandre. The
carrageenan have not been reported to show oxidation problems authors would also like to thank A. Gravelle for training M. Alejandre
(Poyato, Ansorena, Berasategi, et al., 2014). on how to prepare organogels.

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