Food Chemistry 236 (2017) 101–108

Contents lists available at ScienceDirect

Food Chemistry
journal homepage: www.elsevier.com/locate/foodchem

Effect of added ingredients on water status and physico-chemical

properties of tomato sauce
Agoura Diantom a, Elena Curti a,b,⇑, Eleonora Carini a, Elena Vittadini a
a
Department of Food Science, University of Parma, Parco Area delle Scienze 47/A, 43124 Parma, Italy
b
Siteia.Parma Interdepartmental Centre, University of Parma, Parco Area delle Scienze, 181/A, 43124 Parma, Italy

a r t i c l e i n f o a b s t r a c t

Article history: Different ingredients (guar, xanthan, carboxy methyl cellulose, locust bean gums, potato fiber, milk,
Received 9 December 2016 potato and soy proteins) were added to tomato sauce to investigate their effect on its physico-
Received in revised form 30 January 2017 chemical properties. The products were characterized in terms of colour, rheological properties
Accepted 31 January 2017
(Bostwick consistency, flow behavior and consistency coefficient), water status (water activity, moisture
Available online 7 February 2017
content) and molecular mobility by 1H Nuclear Magnetic Resonance (NMR).
Water activity was significantly decreased only by the addition of potato fiber. Xanthan, locust bean,
Keywords:
guar and carboxy methyl cellulose significantly enhanced Bostwick consistency and consistency coeffi-
Tomato sauce
Hydrocolloids
cient. Type of ingredient and concentration significantly affected 1H NMR mobility indicators. Principal
Fiber component analysis (PCA) indicated that only 1H NMR mobility parameters were able to differentiate
Water status the effect of milk protein, xanthan and potato fiber on tomato sauce properties. The information collected
Rheological properties in this work provides information to intelligently modulate tomato sauce attributes and tailor its prop-
Molecular mobility erties for specific applications.
Ó 2017 Elsevier Ltd. All rights reserved.

1. Introduction The use of additional ingredients, with specific functionality,

Tomatoes are consumed worldwide, and represent an impor-
tant part of the human diet and a rich source of b-carotene, folate,
potassium, vitamin C, vitamin E, flavonoids, and lycopene
(Hernández, Rodríguez, & Díaz, 2007). Tomatoes can be consumed
fresh, but important quantities are processed to obtain different
products, including tomato juice, paste, puree, ketchup, and sauces.
These products can be sold either as individual products or be
included as ingredients in more complex multi-component food
products (e.g. ready to eat pasta meals, Carini, Curti, Littardi,
Luzzini, & Vittadini, 2013). To meet consumers quality require-
ments, some quality parameters of tomato sauce based-products
are to be considered very important, such as rheological and
appearance indicators (i.e. consistency and colour). It was reported
that tomato based products characterized by a high viscosity and a
red colour are preferred by consumers (Hayes, Smith, & Morris,
1998; Torbica et al., 2016).
⇑ Corresponding author at: Department of Food Science, University of Parma,
Parco Area delle Scienze 47/A, 43124 Parma, Italy.
E-mail addresses: josephagouradiantom@gmail.com (A. Diantom), elena.curti@
unipr.it (E. Curti), eleonora.carini@unipr.it (E. Carini), elena.vittadini@unipr.it
(E. Vittadini).
may, therefore, help in modulating tomato sauce properties, sen-
sory attributes, stability as well as to produce tailor made products
for specific applications (e.g. multicomponent, complex products).
Different ingredients (e.g. additives) are allowed to be included
in tomato sauce and have been reported to affect on multiple prop-
erties of tomato sauce. Citric acid and sodium chloride were
reported to enhance colour stability in tomato sauce, due to inhibi-
tion of enzymes responsible for the browning of tomato sauce
(Plaza, Muñoz, De Ancos, & Cano, 2003). Salt can enhance the col-
our of tomato sauce, while gelatin and flour increase its consis-
tency and viscosity (Carini, Curti, Mora, Luzzini, & Vittadini,
2015). Moreover, these ingredients can also modulate water status
at molecular and macroscopic levels, reducing water activity (salt,
also in combination with flour and gelatin), or increasing (gelatin)
proton molecular mobility (Carini et al., 2015).
Long chain polymers, such as hydrocolloids (polysaccharides
and proteins), are extensively used by the food industry in different
systems as soups, beverages, desserts, ketchups, sauces, or salad
dressings, due to their functionality as thickening (Alexander,
1999; Casas, Mohedano, & García-Ochoa, 2000; Dunstan, Chen,
Liao, Salvatore, Boger, & Prica, 2001; Gibiński et al., 2006;
Koocheki, Ghandi, Razavi, Mortazavi, & Vasiljevic, 2009; Kulicke
et al., 1996; Murray, 2000; Philips & Williams, 2000; Saha &
Bhattacharya, 2010; Sahin & Ozdemir, 2004; Sikora, Kowalski,

http://dx.doi.org/10.1016/j.foodchem.2017.01.160
0308-8146/Ó 2017 Elsevier Ltd. All rights reserved.
102 A. Diantom et al. / Food Chemistry 236 (2017) 101–108

Tomasik, & Sady, 2007; Wang, Ellis, & Ross-Murphy, 2000), gelling
(Oakenfull and Glicksman, 1987; Philips & Williams, 2000; Saha &
Bhattacharya, 2010; Williams, 2006), emulsifying and stabilizing
(Milani & Maleki, 2012) agents. The investigation of the effect of
different ingredients on tomato sauce properties may help in the
selection of ingredients to design products for specific applications
(e.g. ready to eat pasta meals).
This study aims, therefore, to explore the effect of different
ingredients on the physico-chemical properties of tomato sauce,
in terms of colour, macroscopic water status indicators, rheological
properties, as well as proton molecular mobility.
2.2.3. Colour
The colour parameters L⁄ (Lightness), a⁄ (degree of redness) and
b⁄ (degree of yellowness) were measured with a CIELAB colorime-
ter (CM 2600d, Minolta Co., Osaka, Japan) equipped with D65 at
10° position of the standard observer. The a⁄/b⁄ ratio was used to
describe tomato sauces redness (Barreiro, Milano, & Sandoval,
1997; Batu, 2004). Differences of colour between samples (STD⁄
vs STD; samples with added to hydrocolloids vs STD) were evalu-
ated using the DE value, that was calculated with the following
equation
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
 2
ðDL Þ þ ðDa Þ2 þ ðDb Þ
2
DE ¼ ð1Þ

2. Materials and methods
2.1. Materials
Tomato sauce (Siccagno di Valledolmo, Soc. Coop. Rinascita s.r.
l., Palermo, Italy) from the same production lot was purchased
from a local supermarket. Xanthan (Xan), Guar (G), Locust bean
gum (LBG) and Carboxy Methyl Cellulose (CMC) gums were pro-
vided from Chimab S.p.a (Campodaresego, Italy), soy proteins
(SP; Procon 2100 IP) from Solae Belgium N.V (Ieper, Belgium),
potato proteins (PP; SolanicÒ) from Avebe (Veendam, The Nether-
lands), milk proteins (80% of whey protein) (MP) from Reire s.r.l.
(Reggio Emilia, Italy) and potato fiber (PF) from HI-FOOD S.p.a (Col-
lecchio, Parma, Italy). Characteristics of each ingredient are
reported in Table 1.
Tomato sauce added with 0.5, 1 and 1.5% of the hydrocolloids
were mixed using an OsterizerÒ blender (Sunbeam, USA) for
2 min at low speed (2). 400 g of the mixed tomato sauces were
inserted in sealed glass jars, placed into a water bath at 100 °C
for 30 min. The jars were then cooled at room temperature for
12 h before analysis. Tomato sauce without added ingredient was
also subjected to heating and was considered as the control sample
(STD). Tomato sauce without added ingredients was analysed prior
to heating and was considered an unheated control (STD⁄). Two
batches (each batch included two bottles of tomato sauce) were
produced for each formulation.
2.2. Methods
2.2.1. Moisture content
Moisture content (MC,% g water/100 g product) of tomato
sauces was determined by weight loss by drying in a forced-air
oven (ISCO NSV 9035, ISCO, Milan, Italy) at 80 °C to constant
weight. At least triplicate tomato sauce samples were analysed.
2.2.2. Water activity
Water activity of tomato sauces were measured at 25 °C with an
Aqualab 4TE (Decagon Devices, Inc. WA, USA). At least triplicate
tomato sauce samples were analysed.
Based on the resulting DE value, it can be evaluated if the differ-
ent colour is perceivable by the human eye; the higher the value,
the higher the differences between samples due to heating or addi-
tion of ingredients and the reference (STD) (Limbo & Piergiovanni,
2006). At least twelve measurements were taken for each tomato
sauce sample.
2.2.4. Bostwick consistency
Bostwick consistency was measured with a Bostwick Consis-
tometer (LS 100, Laboscientifica, Parma, Italy). The Bostwick con-
sistometer sample chamber was filled with 100 ml of tomato
sauce, and then the gate of the chamber was released to allow
tomato sauce flowing. The distance (cm) travelled by the sample
was recorded after 30 s (Barringer, Azam, Heskitt, & Sastry,
1998). At least three measurements were taken for each tomato
sauce sample.
2.2.5. Apparent viscosity
Tomato sauces apparent viscosity was measured at 25 °C with
an ARES rheometer (Ta Instruments, New Castle, DE, USA), using
the concentric cylinder geometry (Couette geometry). The charac-
teristic dimensions of the geometry were the following: cup diam-
eter 34 mm, bob diameter 32 mm and height 33 mm. About 8 ml of
the sample were placed into the cup and a rate sweep test (1–
1750 s1, 5 points for decade) was used to obtain shear stress (s)
and viscosity. Shear rate (c) and shear stress curves were fitted
with a non-Newtonian model (Eq. (2)) to extrapolate flow index
(n), and the consistency coefficient (K).
s ¼ K  cn ð2Þ
2.2.6. Protons Nuclear Magnetic Resonance (1H NMR)
A low resolution (20 MHz) 1H NMR spectrometer (the MiniSpec,
Bruker Biospin, Milano, Italy) operating at 25.0 ± 0.1 °C was used.
About 4 grams of tomato pulp (10 mm high) were placed into a
10 mm (diameter) NMR tube that was then sealed with ParafilmÒ
to prevent moisture loss during the NMR experiment. 1H FIDs were
acquired using a single 90° pulse, followed by a dwell time of 7 ls,
a recycle delay of 5 s and a 8 ms acquisition window. 1H FIDs were
analysed only in the time range 7–100 ls, where the homogeneity

Table 1
Composition of tomato sauce and ingredients.1

STD* Xan G LBG CMC SP PP MP PF

Humidity – max. 13% max. 13% max. 12% max. 10% max. 7.5% 5.3% <5% –
Ashes – max. 13% max. 1,2% max. 1.2% max. 24% max. 7.5% 1.6% <4% –
Galactomannans – – 80–85% – – – – – –
Proteins (Nx6,25) 1.6 g max. 5% max. 5% max. 7% – min. 68% 94% min. 80% –
Carbohydrates 4.4 g 0 g (0–0,1) – – 7 ± 2% (lactose) 2%
Fat 0.1 g max. 1% max. 1% 1 g (0.5–1.5) – max. 1.5% 0.03% <2%
Fibre 1.5 g 83 g (82–84) 73 g 0.3% – 97%
1 *
Tomato sauce (STD ), Xan – Xanthan Gum, G – Guar, LBG – Locust bean gum, CMC – Carboxy Methyl Cellulose, SP – soy proteins, PP – potato proteins, MP – milk proteins,
PF – potato fiber.
 A. Diantom et al. / Food Chemistry 236 (2017) 101–108 103

of magnetic field was assured. The curves were fitted with a two
components model (exponential and gaussian; Le Grand,
Cambert, & Mariette, 2007; sigmaplot, v6, Systat Software Inc.,
USA):
f ¼ y0 þ A  eðTAÞ þ B  eðTBÞ
2
t t
ð3Þ
where y0 is the FID decay offset, A and B are the intensities of each
relaxation component, TA and TB are the apparent relaxation times.
T2 relaxation time was measured with a Carr-Purcell-Meiboom-
Gill (CPMG) pulse sequence with a recycle delay of 3 s (P5 1H T1),
an interpulse spacing of 0.04 ms and 10,000 data points. 1H T2
curves were analysed as quasi-continuous distributions of relax-
ation times using a UPENWin software (Alma Mater Studiorum,
Bologna, Italy). Default values for all UPEN settings parameters
were used with the exception of LoXtrap, that was set to 1 to avoid
extrapolation of relaxation times shorter than the first experimen-
tal point. 1H T2 CPMG relaxation decays were also fitted with a dis-
crete exponential model (Sigmaplot, v.6, Systat Software Inc., USA).
Proton self-diffusion coefficient (1H D) was measured at 25 °C
with a pulsed-field gradient spin echo (PFGSE) pulse sequence at
30% gradient. The instrument was calibrated with water at 25 °C
(D = 2.29 * 109 m2/s).
2.2.7. Statistical analysis
Statistical analysis was carried out with a SPSS software (Ver-
sion 22.0, IBM SPSS Statistics, Armonk, New York, USA). The effect
of formulation and concentration in different samples were veri-
fied by one-way-analysis of variance (ANOVA) with a Tukey-high
and LSD significant difference test (p 6 0.05).
Data were also analysed by factor analysis (FA) and principal
component analysis (PCA) (Statistica, version 8.0; Stat-Soft, Tulsa,
OK, USA). Factor analysis is a statistical method used to reduce
the number of variables of complex multivariate data sets by max-
imising the information presented using a limited number of fac-
tors. FA was carried out with 10 independent variables. Factors
were extracted by means of a regression modelling technique, to
test hypotheses producing error terms. Only parameters with fac-
tor loadings higher than 0.70 were used for the PCA analysis. PCA
has been used as descriptive statistical technique plotting the
selected vectors (by factor analysis) versus all cases (samples).
3. Results and discussion
3.1. Moisture content and water activity
Moisture content of STD and STD⁄ was 91% (g water/100 g pro-
duct), indicating that moisture content was not affected by heating,
as expected, since jars were hermetically sealed. On the contrary,
water activity was significantly reduced by the heating process
(Table 2), possibly for the establishment of stronger interactions
between water and macromolecules (e.g. pectins) during heating.
Moisture content, slightly but significantly, decreased in the pres-
ence of added ingredients (Table 2), as expected, except in CMC
where no changes were observed between 1% and 1.5% of added
CMC, while SP and PP showed changes in moisture content only
at higher concentrations (1.5%). The addition of ingredients did
not affect water activity, unregarding of their nature and concen-
tration, except for potato fiber (PF), which significantly reduced
water activity (in a comparable way at the three levels considered

Table 2
Physico-chemical properties of tomato sauces with different formulations: MC (Moisture Content), aw (Water Activity) and Bostwick consistency.1

Moisture content aw Bostwick distance (cm)

(%, g H20/100 g sample)
STD 90.9 (0.1) A 0.996 (0.001) A 7.3 (0.3) C
STD* 90.9 (0.1) A 0.982 (0.003) B 8.6 (0.3) B
G 0.5% 90.4 (0.1) a/CD 0.997 (0.001) a/A 9.0 (0.1) a/A
1% 90.1 (0.1) b/C 0.996 (0.001) a/A 8.8 (0.3) a/A
1.5% 89.1 (0.1) c/DE 0.996 (0.001) a/A 8.2 (0.3) b/B
LBG 0.5% 89.8 (0.1) a/F 0.992 (0.002) b/A 6.5 (0.1) a/E
1% 89.6 (0.1) b/E 0.995 (0.003) ab/A 5.5 (0.1) b/D
1.5% 89.1 (0.1) c/DE 0.997 (0.001) a/A 5.8 (0.3) b/DE
Xan 0.5% 90.6 (0.1) a/B 0.996 (0.003) a/A 7.1 (0.3) a/D
1% 89.7 (0.1) b/DE 0.999 (0.001) a/A 4.4 (0.3) b/E
1.5% 89.1 (0.1) c/E 0.995 (0.004) a/A 2.5 (0.1) c/G
CMC 0.5% 90.0 (0.1) a/E 0.996 (0.003) a/A 8.9 (0.3) a/A
1% 89.3 (0.1) b/F 0.996 (0.003) a/A 8.3 (0.3) b/A
1.5% 89.2 (0.1) b/CD 0.997 (0.004) a/A 7.1 (0.3) c/C
PP 0.5% 89.9 (0.2) a/EF 0.996 (0.004) a/A 4.5 (0.1) b/F
1% 89.8 (0.1) a/D 0.995 (0.005) a/A 4.9 (0.3) a/E
1.5% 89.2 (0.1) b/CDE 0.998 (0.001) a/A 4.5 (0.1) b/F
MP 0.5% 90.5 (0.1) a/BC 0.997 (0.002) a/A 7.0 (0.1) a/D
1% 90.0 (0.1) b/C 0.996 (0.002) a/A 6.4 (0.3) b/C
1.5% 89.3 (0.1) c/C 0.996 (0.002) a/A 5.5 (0.1) c/E
SP 0.5% 90.3 (0.1) a/D 0.993 (0.002) a/A 6.5 (0.1) b/E
1% 90.3 (0.1) a/B 0.994 (0.002) a/A 7.5 (0.1) a/B
1.5% 89.5 (0.1) b/B 0.994 (0.003) a/A 6.1 (0.3) c/D
PF 0.5% 90.3 (0.1) a/D 0.986 (0.001) a/B 6.7 (0.3) a/E
1% 89.7 (0.1) b/DE 0.986 (0.001) a/B 4.4 (0.3) b/E
1.5% 89.1 (0.1) c/DE 0.985 (0.001) a/B 2.8 (0.3) c/G
1
STD – control tomato sauce heated, STD* control tomato sauce not heated, Xan – Xanthan Gum, G – Guar, LBG – Locust bean gum, CMC – Carboxy Methyl Cellulose, SP –
soy proteins, PP – potato proteins, MP – milk proteins, PF – potato fiber; 0.5%, 1% and 1.5% are the levels of added ingredient; standard deviations are given in parenthesis
following the means values; different letters close to numbers indicate significant difference among samples (p 6 0.05), where the small letters to the difference due to the
concentration and capital letters to the type of hydrocolloids. The ‘‘a” and ‘‘A” letters were assigned to the highest value.
104 A. Diantom et al. / Food Chemistry 236 (2017) 101–108

(Table 2), suggesting that potato fiber was able to bind water more
strongly than the other ingredients used in this study.
3.2. Colour
L⁄, a⁄ and b⁄ values were measured with a colorimeter and used
to calculate a⁄/b⁄ ratio (redness index) and DE (Table 3). The a⁄
value was significantly higher in STD⁄ (unheated tomato sauce)
than in STD (heated tomato sauce), while L⁄ and b⁄ were similar
in both samples, indicating that redness of tomato sauce was
reduced by heating as shown also by the higher a⁄/b⁄ for unheated
sample (1.10 ± 0.01 in STD⁄ vs 1.07 ± 0.01 for STD). This might be
due to carotenoids degradation, which induced a formation of
cis-carotenoids isomers, as previously reported in heat treated
canned carrot juice (Chen, Peng, & Chen, 1995).
The presence of added ingredients drastically changed the col-
our of tomato sauce. At 0.5% of ingredients addition, a significant
increase of L⁄, a⁄ and b⁄ was found in all samples, as compared to
STD (Table 3). Colour changes were concentration dependent
(Table 3), except for CMC, LBG and G. In particular, CMC had a com-
parable effect on sauce colour, at the three levels of substitution, G
significantly decreased L⁄, a⁄ and b⁄, while LBG significantly
decreased a⁄ and increased L⁄ and b⁄ with increasing concentration.
The redness index (a⁄/b⁄) was also affected by the different
ingredients (Table 3), with a significantly higher a⁄/b⁄ in all sam-
ples compared to STD, except for MP and PF, which resulted com-
parable to STD. The redness index was not affected by ingredients
concentration, except for G and PP, where a⁄/b⁄ decreased only at
higher concentration (1.5%), while for LBG the redness index signif-
icantly decreased with increasing concentration. Redness index
enhancement might be associated to a limited alteration of lyco-
pene (the most important compound associated to tomato sauce
colour, D’Souza, Singha, & Ingle, 1992) during cooking. Chavan,
Kumar, Basu, Nema, and Nalawade (2015) reported that the pres-
ence of whey proteins in tomato soup powder avoided changes
of the red colour during processing (80° C for 10 min), due to their
capacity to bind lycopene. In this study, MP showed a similar red-
ness index to STD, possibly due to an inefficient whey proteins-
lycopene interaction, due the higher temperature and duration of
the thermal treatment (100 °C for 30 min), that may have altered
whey protein during the heating process. The enhancement in
the redness index of CMC, LBG and G samples might be related
to the capacity of CMC, locust bean gum and guar to bind lycopene,
possibly avoiding its thermal degradation. Tomato sauce colour
influences consumer habits (Garrett, Ammerman, Desrosier,
Fields, 1960), thus it was also necessary to evaluate the effect of
the ingredients on consumers perception. To this aim, the total col-
our difference (DE) was used to evaluate products colour accep-
tance (Table 3). Based on the DE evaluation reported by Limbo
and Piergiovanni (2006), LBG, SP, PF and CMC exhibited only small
differences in tomato sauce colour (DE < 2), Xan and MP a fairly
perceptible difference (2 < DE < 3), PP a perceptible difference
(3 < DE < 6), while a strong colour difference was only observed
in G (6 < DE < 12). DE significantly increased with increasing added
ingredients concentration in all samples, except for G and LBG,
where it decreased and was only slightly affected with increasing
ingredient concentration, respectively.
3.3. Bostwick consistency
Bostwick consistency of tomato sauce samples is reported in
Table 3. A reduced running distance indicates an increase of
tomato sauce consistency. Running distance of heated tomato
sauce (STD) was significantly lower than in STD⁄. This result
indicated an enhanced consistency, possibly associated to a
heat-induced structural modification of its components (e.g. pectin

Table 3
Colour parameters (L*, a*, b*, DE, a*/b*) of tomato sauces with different formulations.1

L* a* b* DE a*/b*
STD 42.31 (0.10) F 13.20 (0.21) F 12.31 (0.01) F 1.07 (0.01) D
STD* 42.51 (0.09) EF 13.70 (0.24) E 12.46 (0.01) EF 0.73 (0.15) 1.10 (0.01) C
G 0.5% 51.82 (0.62) a/A 16.42 (0.51) a/A 14.49 (0.21) a/A 10.30 (0.18) a/A 1.14 (0.02) a/C
1% 52.19 (0.43) a/A 16.42 (0.29) a/B 14.36 (0.29) a/C 10.48 (0.19) a/A 1.14 (0.01) a/C
1.5% 42.93 (0.23) b/D 14.28 (0.16) b/D 12.96 (0.12) b/D 1.42 (0.18) b/F 1.10 (0.01) b/CD
LBG 0.5% 43.09 (0.32) b/C 14.87 (0.22) a/D 12.32 (0.10) b/F 1.44 (0.19) a/E 1.21 (0.02) a/D
1% 43.31 (0.19) a/D 14.51 (0.11) b/D 12.36 (0.13) b/E 1.71 (0.14)a/E 1.17 (0.01) b/B
1.5% 43.16 (0.13) ab/B 13.88 (0.21) c/D 13.07 (0.21) a/E 1.55 (0.20) a/EF 1.06 (0.01) c/A
Xan 0.5% 44.25 (0.06) b/C 14.65 (0.25) b/CD 12.93 (0.13) b/D 2.61 (0.18) c/D 1.13 (0.01) a/B
1% 45.06 (0.44) a/D 14.96 (0.35) a/C 13.12 (0.27) b/D 3.35 (0.17) b/D 1.13 (0.01) a/C
1.5% 45.25 (0.22) a/B 15.07 (0.27) a/B 13.38 (0.20) a/C 3.79 (0.15) a/B 1.13 (0.01) a/DE
CMC 0.5% 42.91 (0.30) a/DE 12.52 (0.17) a/D 12.52 (0.11) a/E 1.44 (0.11) b/E 1.15 (0.01) a/A
1% 42.73 (0.33) a/F 14.89 (0.30) a/C 12.39 (0.19) a/E 1.74 (0.17) a/E 1.15 (0.01) a/A
1.5% 42.93 (0.71) a/D 14.41 (0.40) a/C 12.47 (0.15) a/E 1.78 (0.78) a/E 1.16 (0.01) a/C
PP 0.5% 45.14 (0.45) c/B 15.97 (0.25) c/B 13.67 (0.13) c/C 4.23 (0.17) c/B 1.17 (0.01) a/B
1% 46.89 (0.40) b/B 17.32 (0.31) b/A 14.92 (0.14) b/B 6.66 (0.15) b/B 1.17 (0.01) a/B
1.5% 48.90 (0.36) a/A 18.11 (0.22) a/A 16.10 (0.14) a/B 8.93 (0.18) a/A 1.12 (0.01) b/B
MP 0.5% 44.05 (0.13) c/C 14.82 (0.09) c/C 13.90 (0.07) c/B 2.91 (0.18) c/C 1.07 (0.01) a/D
1% 46.14 (0.31) b/C 16.68 (0.18) b/B 15.68 (0.13) b/A 6.33 (0.15) b/C 1.07 (0.01) a/E
1.5% 48.73 (0.62) a/A 18.03 (0.44) a/A 16.79 (0.29) a/A 8.90 (0.20) a/A 1.07 (0.01) a/G
SP 0.5% 42.83 (0.19) c/DE 13.93 (0.16) c/E 12.41 (0.07) c/EF 1.05 (0.09) c/F 1.12 (0.01) a/B
1% 43.38 (0.07) b/E 14.07 (0.10) b/E 31.21 (0.08) b/D 1.67 (0.11) b/E 1.13 (0.01) a/E
1.5% 43.69 (0.08) a/C 15.37 (0.07) a/B 13.64 (0.06) a/C 2.96 (0.12) a/C 1.13 (0.01) a/E
PF 0.5% 43.02 (0.26) c/D 13.76 (0.19) c/E 12.81 (0.09) c/D 1.03 (0.10) c/F 1.07 (0.01) a/D
1% 43.28 (0.17) b/E 14.12 (0.19) b/E 13.27 (0.11) b/D 1.70 (0.14) b/E 1.07 (0.01) a/E
1.5% 43.67 (0.23) a/C 14.61 (0.39) a/C 13.74 (0.27) a/C 2.17 (0.20) a/D 1.07 (0.01) a/G
1
STD – control tomato sauce heated, STD* control tomato sauce not heated, Xan – Xanthan Gum, G – Guar, LBG – Locust bean gum, CMC – Carboxy Methyl Cellulose, SP –
soy proteins, PP – potato proteins, MP – milk proteins, PF – potato fiber; 0.5%, 1% and 1.5% are the levels of added ingredient; standard deviations are given in parenthesis
following the means values; different letters close to numbers indicate significant difference among samples (p 6 0.05), where the small letters to the difference due to the
concentration and capital letters to the type of hydrocolloids. The ‘‘a” and ‘‘A” letters were assigned to the highest value.
 A. Diantom et al. / Food Chemistry 236 (2017) 101–108 105

gelation), that resulted in the formation of a more rigid matrix, Table 4

conferring higher flow resistance to the sample. Consistency coefficient (K) and flow behavior index (n) of tomato sauce with different
formulation.1
Changes in Bostwick running distance were dependent on the
type of added ingredient and concentration. At 0.5% addition, the Consistency coefficient (K) Flow behavior index (n)
running distance was significantly decreased in PP, followed by STD 12.68 (0.62) D 0.251 (0.009) DE
LBG, SP and PF (comparable among each other), Xan and MP (com- STD* 9.01 (0.61) E 0.274 (0.09) BC
parable among each other), while it significantly increased in CMC G 0.5% 11.40 (0.29) c/D 0.285 (0.004) c/B
and G. Bostwick running distance significantly decreased with 1% 12.98 (0.17) b/EF 0.361 (0.002) b/B
increasing ingredient concentration, more markedly in Xan (from 1.5% 20.75 (0.66) a/DE 0.429 (0.006) a/A

7.1 ± 0.3 cm at 0.5% to 2.5 ± 0.1 at 1.5%) and PF (from 6.8 ± 0.3 at LBG 0.5% 23.60 (0.12) c/A 0.241 (0.001) a/E
0.5% to 2.8 ± 0.3 at 1.5%). 1% 38.46 (0.90) b/A 0.267 (0.004) b/DE
1.5% 55.55 (1.46) a/A 0.293 (0.003) c/D
A decreased running distance of tomato sauce has been
reported in the presence of flour and gelatin (Carini et al., 2015) Xan 0.5% 19.08 (0.37) c/A 0.215 (0.008) c/F
1% 33.14 (0.06) b/B 0.192 (0.001) b/F
and hydrocolloids (G, CMC, Xan) (Gujral, Sharma, & Singh, 2002), 1.5% 52.75 (0.82) a/B 0.171 (0.003) a/F
possibly due to the interactions of these ingredients with water,
CMC 0.5% 14.84 (0.28) c/C 0.306 (0.003) c/A
resulting in the formation of a gel-like structure. It was reported 1% 15.64 (0.06) b/D 0.381 (0.002) b/A
that guar (Sandolo, Matricardi, Alhaique, & Coviello, 2009), xan- 1.5% 18.49 (0.20) a/E 0.400 (0.001) a/B
than (Katzbauer, 1998) and locust bean gum solutions PF 0.5% 14.31 (0.36) a/C 0.261 (0.007) c/CD
(Richardson, Willmer, & Foster, 1998) are able to form a gel during 1% 14.05 (0.16) a/DE 0.297 (0.002) b/CD
cooling, due to polymer aggregation by hydrogen bonding. A previ- 1.5% 15.38 (0.86) a/F 0.329 (0.011) a/C
ous study (Sahin & Ozdemir, 2004) observed that ketchup fluidity PP 0.5% 19.10 (0.54) b/B 0.204 (0.003) a/F
was significantly affected by hydrocolloids, depending on the type 1% 22.92 (1.17) a/C 0.190 (0.007) a/F
and concentration: xanthan caused the maximum increase in Bost- 1.5% 23.12 (1.51) a/CD 0.187 (0.010) a/F
wick consistency of ketchup, followed by guar and locust bean gum SP 0.5% 11.49 (0.83) b/D 0.252 (0.011) a/DE
and carboxy methyl cellulose, respectively. This might be associ- 1% 11.49 (0.26) b/F 0.261 (0.003) a/DE
1.5% 13.61 (0.59) a/FG 0.251 (0.005) a/E
ated to the effect of tomato sauce formulation, which affects the
interaction of these ingredients with water. Banerjee and MP 0.5% 15.44 (0.46) c/C 0.214 (0.003) a/F
1% 21.39 (1.38) b/C 0.185 (0.008) b/F
Bhattacharya (2012) reported that acidification can promote
1.5% 24.81 (0.92) a/C 0.181 (0.008) b/F
aggregation of denatured soy protein molecules, and that unfolded
1
whey proteins molecules can aggregate, forming a network. This is STD – control tomato sauce heated, STD* control tomato sauce not heated, Xan –
Xanthan Gum, G – Guar, LBG – Locust bean gum, CMC – Carboxy Methyl Cellulose,
in agreement with the results observed in this study, where
SP – soy proteins, PP – potato proteins, MP – milk proteins, PF – potato fiber; 0.5%,
protein-based ingredients (MP and PP) increased the Bostwick 1% and 1.5% are the levels of added ingredient; standard deviations are given in
consistency. parenthesis following the means values; different letters close to numbers indicate
significant difference among samples (p 6 0.05), where the small letters to the
3.4. Apparent viscosity difference due to the concentration and capital letters to the type of hydrocolloids.
The ‘‘a” and ‘‘A” letters were assigned to the highest value.

Shear stress/shear rate curves were fitted with a Power law

model, that properly described the flow behavior of all tomato
sauce samples (R2 > 0.96). Consistency coefficients and flow behav-
ior indexes were calculated and reported in Table 4. The flow
behavior index (n) was <1 in all samples indicating the pseudoplas-
tic nature of all samples.
Heating of tomato sauce (STD) increased the pseudoplastic
behavior of tomato sauce, as compared to STD⁄. Ingredients differ-
ently affected the flow behavior index of tomato pulp: at 0.5% of
addition, a reduction (Xan, PP and MP), an increase (G and CMC),
and no effect (LBG, PF and SP) on n were observed (Table 4). Flow
behavior index was also dependent on ingredient concentration,
except for SP and PP. The presence of Xan significantly decreased
tomato sauce flow index with increasing concentration, while the
other ingredients significantly increased n with increasing ingredi-
ent concentration.
Regarding the consistency coefficient (K, Table 4), STD showed a
higher consistency (12.7 ± 0.6 Pa*s) as compared to the untreated
product STD⁄ (9.0 ± 0.6 Pa*s), indicating an effect of processing on
rheological properties, as similarly observed for Bostwick running
distance. Ingredients addition induced significant changes in K.
At 0.5%, K increased in all samples, except for G and SP, where K
was similar to STD. LBG exhibited the highest consistency coeffi-
cient, followed by Xan and PP, which were higher than CMC, PF
and MP. The consistency coefficient increased with increasing con-
centration in all samples, except for SP where it was approximately
constant. Tomato sauce consistency and flow behavior enhance-
ment and changes were previously reported (Bottiglieri et al.,
1991; Carini et al., 2015; Koocheki et al., 2009; Sahin & Ozdemir,
2004; Sharoba, Senge, El-Mansy, Bahlol, & Blochwitz, 2005), and
associated to the hydrocolloids capacity to bind water, resulting
in the formation of a gel-like network. This was in agreement with
the Bostwick consistency results, although the same ingredients
did not show the same trend at two different dimensional rheolog-
ical scales of analysis (R2 of linear relation between Bostwick con-
sistency and consistency coefficient <0.30).
3.5. Protons Nuclear Magnetic Resonance (1H NMR)
To investigate the effect of added ingredients on water status at
a molecular level, proton mobility was studied with low resolution
1
H NMR (20 MHz) through different parameters: Free Induction
Decay (1H FID), transverse relaxation time (1H T2) and self-
diffusion coefficient (1H D).
1
H FIDs were fitted with a two components model and the two
proton populations were named population A and B (data not
shown). The more rigid protons population (population A) was rep-
resented by 3% of protons and it relaxed at 0.01 ms while pop-
ulation B, the more represented (97%) relaxed at 1.14 ms, for
both standards (STD and STD⁄). The comparable mobility of FID
population of both STD samples indicated that heating did not
affect the more rigid FID protons mobility. The protons observed
in the 1H FIDs window were not affected by hydrocolloids and con-
centration (data not shown), except for PF where relevant changes
in FID mobility were observed at 1.5%. The more rigid proton pop-
ulation A was significantly larger in PF than in the other samples
(49% versus 3%; relaxation time TA 0.01 ms), suggesting a
strongly reduced mobility, possibly associated to the formation of
106 A. Diantom et al. / Food Chemistry 236 (2017) 101–108
a rigid water-potato fiber mediated structure (as indicated also by
the increased Bostwick consistency) occurring only in the presence
of a relatively high amount of potato fiber.
A characteristic 1H T2 distribution of heated tomato sauce is
reported in Fig. 1A. The effect of different ingredients on 1H T2 dis-
tribution is shown in Fig. 1B that provides an expanded section of
the representative distribution for each sample. Two unresolved
populations were observed in all samples, except for Xan which
exhibited three unresolved populations. 1H T2 curves were, there-
fore, fitted with a bi-exponential model for all samples, and tri-
exponential model for Xan (Table 5). 1H T2 populations were
named population C (pop C) and population D (pop D) and their
corresponding relaxation times T2C and T2D, respectively. The addi-
tional population in Xan was named population E (pop E) with the
corresponding relaxation time T2E. 1H T2 populations and relax-
ation times are reported in Table 5.
Fig. 1. Characteristic 1H T2 relaxation time distribution for heated tomato sauce (A)
and expanded section of 1H T2 distributions for STD and added ingredients samples
(B).
The more abundant and more mobile population, pop D, was
significantly larger (93.7 ± 0.1%) in STD as compared to the
untreated sample (88.5 ± 0.1%, STD⁄). Relaxation times, T2C and
T2D, were 99.4 ± 0.1 ms and 303.0 ± 0.1 ms in STD, respectively,
while they were 115.8 ± 1.1 ms and 322.6 ± 0.1 ms in STD⁄, respec-
tively. Similar relaxation times in tomato sauce were reported in a
recent paper (Carini et al., 2015). The corresponding relaxation
times, T2C and T2D were significantly decreased in processed sauce
(STD, Table 5), and this might be associated to the observed struc-
tural changes (i.e. consistency coefficient K and Bostwick consis-
tency). 1H T2 mobility in raw tomato was previously investigated
using a low resolution NMR (at 20 MHz; Musse et al., 2009), and
protons with different mobility were observed, and were attribu-
ted, in relation to cell compartmentalization, to exchangeable
solutes (<100 ms), cell walls (100 ms), cytoplasm (400–600 ms)
and vacuole (900–1600 ms) protons. In the present study, a very
different mobility in heated sauce (STD) was observed, as cell com-
partments were altered by processing in tomato sauce, resulting in
the observation of an ‘‘averaged” mobility originating from all pro-
tons in the tomato pulp matrix, that were no more located in sep-
arated compartments.
Added ingredients significantly affected tomato sauce proton
mobility, in a manner dependent on the ingredient type. At 0.5%
the more abundant population pop D was significantly decreased
in all samples as compared to STD, except for CMC and LGB, where
it was significantly increased (Table 5). Pop C consequently
increased in all samples, except for CMC and LBG where it
decreased. Concerning the mobility of protons belonging to pop
D, the relaxation time T2D significantly decreased in the presence
of added ingredients, except for LGB where it was comparable to
STD. The relaxation time of the less mobile protons (T2C) exhibited
similar trend to T2D, except for guar, where T2C was increased, and
CMC where T2C was comparable to STD. 1H T2 molecular mobility
was generally decreased with the presence of added ingredients,
in a different manner depending on the type of the ingredient.
The concentration increase of added ingredients induced a further
significant decrease of the more mobile protons population (pop
D), except for CMC where this population significantly increased
with increasing concentration. Ingredients concentration generally
decreased protons relaxation times (mainly T2D and T2C) in all
samples.
These changes in protons mobility might be related to the inter-
actions of each specific ingredient with water, that possibly
resulted in a modification of the sauce into a gel-like structure of
lower mobility.
Addition of xanthan affected 1H mobility, differently from the
other ingredients, as three proton populations were detected. A
third population was observed (pop E) and it represented about
22% of total protons at 0.5% of added Xan, resulting to be the more
mobile with a corresponding relaxation time (T2E) about 212.0 ms.
However, T2D resulted to be lower than in the other samples, sug-
gesting structural changes induced by xanthan at a molecular level.
This result was in agreement with Bostwick consistency and con-
sistency coefficient (K) that increased in the presence of xanthan.
This suggested that the addition of Xanthan induced to a formation
of a rigid network, either at molecular and macroscopic levels.
Proton self-diffusion coefficients (1H D) are reported in Table 5.
Both STD samples showed similar D values (1.898 ± 0.003 * 109
m2/s in STD and 1.901 ± 0.004 * 109 m2/s in STD⁄), indicating that
heating did not affect protons translational mobility. The presence
of added ingredients induced changes in 1H D. At 0.5% of added
ingredients, 1H D was significantly decreased in LBG and PP, and
significantly increased in Xan and SP, while it was not significantly
affected in the other samples. 1H D significantly decreased with
increasing ingredients concentration in all samples, except for
LBG and SP. In the case of locust bean gum (LBG), 1H D significantly
 A. Diantom et al. / Food Chemistry 236 (2017) 101–108 107

Table 5
1
H T2 relaxation times and populations of tomato sauce with different formulations.1

T2C (ms) Pop C (%) T2D (ms) Pop D (%) T2E (ms) Pop E(%) Self-diffusion coefficient D (10-9 m2/s)
STD 93.4 (0.6) C 6.3 (0.1) E 303.0 (0.1) B 93.7 (0.1) B – – 1.898 (0.003) BC
STD* 115.8 (1.1) A 11.5 (0.1) A 322.6 (0.1) A 88.5 (0.1) F – – 1.901 (0.004) B
G 0.50% 97.8 (1.8) a/B 9.5 (0.3) c/B 294.1 (4.5) a/C 90.5 (0.3) a/E – – 1.894 (0.002) a/BC
1% 85.4 (0.8) b/E 12.6 (0.3) b/A 250.0 (0.1) c/E 87.4 (0.3) b/F – – 1.848 (0.004) b/G
1.50% 96.7 (1.4) a/C 13.7 (0.5) a/C 270.3 (0.1) b/D 86.3 (0.5) c/F – – 1.825 (0.004) c/F
LBG 0.50% 84.1 (0.9) a/E 5.4 (0.1) b/F 301.8 (3.4) a/B 94.3 (0.1) a/A – – 1.850 (0.005) a/E
1% 76.0 (0.5) c/G 5.8 (0.1) b/F 268.2 (3.5) b/C 94.2 (0.1) a/A – – 1.831 (0.003) b/E
1.50% 80.7 (0.5) b/F 8.1 (0.2) a/F 270.3 (0.1) b/D 91.9 (0.2) b/C – – 1.834 (0.003) b/E
Xan 0.50% 18.4 (1.0) b 0.9 (0.1) c 128.0 (4.2) a 76.8 (1.6) b 212.0 (1.8) a 22.3 (2.6) b 1.919 (0.005) a/A
1% 22.5 (1.0) b 1.3 (0.1) b 127.4 (1.7) a 64.5 (3.5) c 194.2 (3.2) c 34.2 (3.4) a 1.898 (0.005) b/B
1.50% 21.6 (0.4) a 1.5 (0.1) a 116.8 (1.8) b 84.8 (1.8) a 207.5 (3.6) a 13.8 (1.8) c 1.880 (0.003) c/B
CMC 0.50% 83.7 (2.0) a/C 6.0 (0.3) a/F 277.8 (0.1) a/E 94.1 (0.3) b/A – – 1.894 (0.004) a/BC
1% 72.0 (0. 6) c/H 6.0 (0.1) a/F 250.0 (0.2) c/E 94.0 (0.1) b/A – – 1.839 (0.002) b/F
1.50% 73.8 (0.6) b/G 5.4 (0.1) b/H 270.3 (2.4) b/D 94.6 (0.1) a/A – – 1.831 (0.004) c/EF
PP 0.50% 91.1 (1.0) a/D 11.8 (0.2) c/A 238.1 (0.1) a/F 88.2 (0.2) a/F – – 1.882 (0.003) a/D
1% 79.7 (0.6) c/F 10.9 (0.2) b/C 197.1 (2.0) b/F 89.1 (0.2) a/D – – 1.869 (0.002) b/D
1.50% 86.3 (2.1) b/E 15.9 (1.3) a/B 183.2 (1.8) c/F 84.1 (1.3) b/G – – 1.855 (0.004) c/D
MP 0.50% 90.8 (1.0) c/D 7.7 (0.1) c/C 285.7 (0.1) a/D 92.4 (0.1) a/D – – 1.893 (0.002) a/C
1% 88.2 (0.8) b/D 9.0 (0.2) b/D 263.2 (0.1) b/D 91.0 (0.3) b/C – – 1.879 (0.002) b/C
1.50% 148.4 (1.2) a/A 48.5 (0.1) a/A 285.7 (0.1) a/C 51.5 (0.1) c/H – – 1.852 (0.002) c/D
SP 0.50% 85.6 (1.3) a/E 7.0 (0.1) b/D 277.8 (0.1) a/E 93.0 (0.1) b/C – – 1.923 (0.003) a/A
1% 76.5 (0.7) b/G 5.9 (0.1) c/F 270.3 (0.1) b/C 94.1 (0.1) a/A – – 1.926 (0.003) a/A
1.50% 68.0 (0.4) c/H 7.4 (0.1) a/F 232.6 (0.1) c/G 92.6 (0.1) c/C – – 1.903 (0.004) b/B
PF 0.50% 90.3 (1.9) a/D 8.9 (0.3) c/B 285.7 (0.1) a/D 91.1 (0.3) a/E – – 1.891 (0.002) a/C
1% 89.9 (1.1) a/C 11.2 (0.2) a/C 270.3 (0.1)b/C 88.8 (0.2) c/D – – 1.883 (0.001) b/C
1.50% 80.3 (1.0) c/F 10.5 (0.2) b/E 263.2 (0.1) c/E 89.5 (0.2) b/D – – 1.872 (0.002) b/C
1
STD – control tomato sauce heated, STD* control tomato sauce not heated, Xan – Xanthan Gum, G – Guar, LBG – Locust bean gum, CMC – Carboxy Methyl Cellulose, SP –
soy proteins, PP – potato proteins, MP – milk proteins, PF – potato fiber; 0.5%, 1% and 1.5% are the levels of added ingredient; standard deviations are given in parenthesis
following the means values; different letters close to numbers indicate significant difference among samples (p 6 0.05), where the small letters to the difference due to the
concentration and capital letters to the type of hydrocolloids. The ‘‘a” and ‘‘A” letters were assigned to the highest value.

Fig. 2. Projection of the variables on the factor plane (1  2) (A); Projection of the cases on the factor plane (1  2) (B); L (LBG), X (Xan), G (G), C (CMC), M (MP), S (SP), P (PP)
and F (PF); 0.5, 1, and 1.5 represent the level of each added ingredient.

decreased at 1% and then remained constant, while it significantly
increased in soy protein (SP), only at higher concentration (1.5%).
The changes observed in proton self-diffusion coefficient might
be associated to interactions between the added ingredients and
water that hindered protons translational mobility, possibly due
to the development of a gel-like structure. Carini et al. (2015)
reported that the addition of salt, flour and gelatin reduced the
translational mobility, due to the high amount of solid (salt) or
to the formation of a viscous gel matrix (gelatin and flour).
PCA was performed with the aim to better evaluate which
parameters were more significant in discriminating tomato sauces.
Among the ten variables considered in this work, only four were
selected for PCA from factor analysis, with factor loadings higher
than 0.70 for the first two principal components (PC1 and PC2)
(Fig. 2A).
Fig. 2A shows the projection of the variables on the factor plane
that explained 87% of the total variance. Among the variables, pop
D-T2 and FID-pop A exhibited high positive loadings on PC1 and
PC2, respectively, while T2C the higher negative loadings on PC1.
Concerning PC2, FID – Pop A. Fig. 2B shows the projection of the
cases on factor plane defined by the two factors. PC1 clearly dis-
criminated samples with added xanthan (0.5, 1 and 1.5%) and
108 A. Diantom et al. / Food Chemistry 236 (2017) 101–108
1.5% of milk proteins from the other samples from the other sam-
ples. PC2 discriminated the sample with the highest amount of
potato fiber (1.5%) from the other samples. These results might
suggest that the addition of ingredients (in particular milk protein,
xanthan and potato fiber) importantly affected proton molecular
mobility of tomato.
Molecular mobility parameters were generally in agreement
with macroscopic indicators (smaller amount of the more mobile
protons, i.e. pop D, reduced 1H D and higher Bostwick consistency
and K), except for G, which showed a lower Bostwick consistency
and a reduced molecular mobility (smaller pop D). The disagree-
ment between the molecular and macroscopic indicators in G sam-
ples might suggest that changes at molecular and macroscopic
levels occurring at the different time-scale levels were not related.
4. Conclusions
The effect of heating and addition of ingredients on physico-
chemical properties of tomato sauce was explored at different
time-space levels. Different ingredients affected colour, macro-
scopic water status indicators (water activity), rheological attri-
butes (Bostwick consistency and consistency coefficient), and
molecular mobility parameters. Moisture content decreased with
increasing amount of added ingredient, as expected. Water activity
was affected only in the presence of potato fiber. Xanthan, locust
bean, guar and CMC gums induced stronger changes in rheological
properties (Bostwick consistency and consistency coefficient) and
molecular mobility indicators (1H T2) than other ingredients.
These results suggested that the addition of ingredients had the
ability to affect physico-chemical properties of tomato sauce for-
mulation, at different time-space levels. The effect of each ingredi-
ent should be, therefore, carefully considered during the
production of tomato sauce, especially when more than one ingre-
dient is envisaged or when used in multi-component complex
food.
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