Journal of Food Process Engineering ISSN 1745–4530

REPLACEMENT OF WHEAT FLOUR BY CHICKPEA FLOUR

IN MUFFIN BATTER: EFFECT ON RHEOLOGICAL PROPERTIES
MARIA DOLORES ALVAREZ1,3, BEATRIZ HERRANZ1, RAUL
 FUENTES1, FRANCISCO JAVIER CUESTA2
1
and WENCESLAO CANET
1
Department of Characterization, Quality and Safety, Institute of Food Science, Technology and Nutrition (ICTAN-CSIC), Jos
e Antonio Novais 10,
28040, Madrid, Spain
2
Department of Products, Institute of Food Science Technology and Nutrition (ICTAN-CSIC), Madrid, Spain

3
Corresponding author. ABSTRACT
TEL: 1 34-91-5492300;
FAX: 1 34-91-5493627; The effect on rheological properties of muffin batter of replacing wheat flour (WF)
EMAIL: [email protected] with chickpea flour (CF) was studied by using viscoelastic and steady-state shear
tests to characterize the physical structure and predict both processing and batter
Received for Publication November 5, 2015
performances. CF was used to replace WF in the batter partially (25, 50, 75% w/w)
Accepted for Publication February 1, 2016
or totally (100% w/w, i.e., CF-based gluten-free muffin batter), and compared with
doi:10.1111/jfpe.12372 a control made only with wheat (100% WF batter). Viscoelasticity and rebuild
time decreased significantly with the increase in the percentage of WF replacement.
Gluten-free muffin batter had the highest viscosity after shearing reflecting a trend
toward a dilatant flow behavior associated with higher intermolecular aggregation
interactions due to higher protein content. Rheological properties of the batters
are dominated by the starch and protein contents present in the formulations.
Replacement of WF by CF also increased the number of air bubbles which were
smaller.

PRACTICAL APPLICATIONS
Gluten-free muffins should resemble those made from WF, overcoming problems
of quality defects and low nutritional value. Potential for use of CF in gluten-free
muffins is related to its high protein content, playing a healthy and functional role.
Formulation of gluten-reduced and gluten-free muffins involves studying batter
rheology and resulting baked product characteristics. Various CF-based muffin
batters were formulated and rheologically characterized under small and large
deformations to attain insights of structural status and mechanical behavior.
Higher WF batter viscoelasticity is related to higher starch content, whereas higher
CF batter viscosity after shearing correlated well with higher protein content. CF
with starch content adjusted to the level of WF could decrease differences in
rheological properties of batters. CF helped to incorporate air into the batter,
which is essential for achieving appropriate final volume and spongy texture.

INTRODUCTION
In turn, baked muffins are characterized by a typical
A muffin batter may well be defined as a “cellular system” alveolar-porous structure and high volume, which give a
(Walstra 2003), in which the continuous semisolid matrix spongy texture. To obtain this final structure, a stable semi-
formed by a complex fat-in-water emulsion could be consid- solid matrix lodging many tiny air bubbles is required
ered a multiphase system containing ungelatinized starch (Martınez-Cervera et al. 2012a,b).
granules, oil droplets, proteins, sucrose, etc. Moreover, those Traditionally, a muffin batter recipe is mainly composed
“cells” are filled with air bubbles as the discontinuous phase. of wheat flour (WF), sucrose, vegetable oil, egg and milk

Journal of Food Process Engineering 2017; 40: e12372; V

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RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER M.D. ALVAREZ ET AL.

(Sanz et al. 2009). For this reason, people with celiac disease TABLE 1. FORMULATIONS OF CONTROL MUFFIN BATTER PREPARED
are unable to consume this type of product. In recent years, WITH 100% OF WHEAT FLOUR (WF) AND BATTERS PREPARED WITH
INCREASING QUANTITIES OF CHICKPEA FLOUR (CF) AS WF REPLACER
there has been extensive research for the development of
gluten-free bakery products. Nevertheless, many gluten-free Ingredients 100% 25% 50% 75% 100%
products available on the market are often of poor technolog- [g/100 g flour] WF CF CF CF CF
ical quality, exhibiting low volume, poor color and crumbling WF 100 75 50 25 0
crumb, as well as great variation in nutrient composition, CF 0 25 50 75 100
with low protein and high fat contents (Martınez-Cervera Whole egg 81 81 81 81 81
Sucrose 100 100 100 100 100
et al. 2011).
Salt 0.75 0.75 0.75 0.75 0.75
Most of gluten-free muffin, cake, or cupcake recipes con-
Milk 50 50 50 50 50
tain rice flour as the principal ingredient (Matos et al. 2014; Oil 46 46 46 46 46
Shevkani et al. 2015). Legumes are rich sources of protein Natural lemon juice 3 3 3 3 3
throughout the world and contain approximately three times Sodium bicarbonate 4 4 4 4 4
more protein than cereals. Chickpea (Cicer arietinum L.) is
one of the top five important legumes on the basis of whole
grain production (Hefnawy et al. 2012). The potential for and to study its effect in the viscoelastic properties (oscilla-
increased use of chickpea is related to its relatively low cost, tory tests) and the flow behavior (steady-state shear tests) of
relatively high protein content (21.9–26.8%), high protein the batter to provide a useful fingerprint of rheological
digestibility (76–78%) and other desirable functionalities (Xu behavior. This prior step would allow establishing and iden-
et al. 2014). Therefore, chickpea flour (CF) could be an excel- tifying correlations between the rheological properties of the
lent choice to improve the nutritional value of gluten-free or batter and the functional properties of the flours and pro-
partially replaced WF in muffin batter. On the other hand, teins and other descriptors of the quality of the baked muf-
the United Nations has declared that 2016 will be the Interna- fin. Optical microscopy of muffin batter was also analyzed,
tional Year of Pulses named as “IYP 2016.” The hope of “IYP and conclusions about the structural features associated with
2016” is to position pulses as primary sources of protein and WF replacement were drawn.
other essential nutrients, leading to dietary uptake.
In addition, the impartation of desirable qualities and MATERIALS AND METHODS
functionalities to food products by the addition of CF
depends largely on the functional properties and characteris- Batter Preparation
tics of the flour (Xu et al. 2014). Functional characteristics,
including water and oil absorption and holding capacities Five muffin formulations (Table 1) were prepared by replac-
and emulsification and foaming abilities, are key to utilizing ing part or all of the WF with CF. Spanish muffin ingredients
and marketing chickpea in a diverse food applications. In were: WF (Triticum spp. with 13.5% moisture and 10.2%
turn, functional properties of WF and composite flours protein content as specified by the supplier) and CF (C. arie-
increased with increase in the incorporation of other flours tinum “Castellano”), both donated by the Garcıa del Valle
with WF (Chandra et al. 2015). flour milling company (Soria, Spain), pasteurized liquid
Chemical composition, physical parameters, functional whole yolk (OvopakV R , Alvarez Camacho S.L., Seville, Spain),

properties and microstructural characteristics will determine sucrose (AB Azucarera Iberia S.L., Madrid, Spain), salt
the rheological properties of muffin batters. Viscoelastic (sodium chloride), ultra-high temperature whole milk (Pasc-
properties are very useful in the design and prediction of ual, Burgos, Spain), refined sunflower oil (Koipesol, Madrid,
product stability (Augusto et al. 2013), and they are very sen- Spain), natural lemon juice (cultivar “Primofiori,” Spain)
sitive to chemical composition and physical structure (Van and sodium bicarbonate (Montplet & Esteban, S.A., Madrid,
Bockstaele et al. 2008b, 2008b). Flow and its characterization Spain), in accordance with the method used previously by
during pumping and handling of muffin batters are also Martınez-Cervera et al. (2011, 2012a, 2012b). Mean values
very important because the batter is an intermediate product for proximate composition (g/100 g) of CF, as specified by
that subsequently passes through low (mixing operations) the supplier, were as follows: moisture, 14, crude fiber, 15,
and high (pumping) shear operations. Large deformation crude protein (N 3 6.25), 19.4, fat, 5 and carbohydrate, 55.
measurements seem to be more adequate to evaluate and The batter was prepared in a KPM5 professional mixer
predict batter and end product qualities. Consequently, a (Kitchen Aid, St. Joseph, MI, USA), in which the egg was
complete rheological characterization of food systems entails whisked for 2 min at top rotational speed (10, 220 rpm) and
both viscoelastic and viscosity measurements. the sucrose was added and mixed for 30 s. Then the mixer
The aim of this work was to evaluate the suitability of CF speed was reduced to 4, and lemon juice and half the milk
to replace different percentages of WF in Spanish muffins, were added and mixed for 1 min. The flour, sodium

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M.D. ALVAREZ ET AL. RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER

bicarbonate and sodium chloride were added and the mix- 200 and 300 1/s shear rates, and analyzing the hysteresis
ture was beaten for a further 1 min. Lastly, the mixer speed cycles (data not shown), a previous shearing of 5 min at 300
was increased to 6, the rest of the milk was added and the oil 1/s was selected as the appropriate treatment to obtain a
was gradually dripped in. The mixture was beaten for 3 min reduced hysteresis area. After eliminating the flow time
until it was smooth. Each formulation was prepared at least dependence, sample flow was measured by controlling the
six times (six batches) on different days. Batters were all kept shear rate and recording the shear stress values at shear rates
at 258C for 60 min after preparation before all the from 0.1 to 100 1/s in 5 min and down in 5 min (Abu-Jdayil
determinations. 2003; Tarrega et al. 2004; Alvarez and Canet 2013).

Rheological Properties Three-Step Shear Rate. For viscometry rebuild analysis,

The rheological properties were obtained using a Bohlin samples were subjected to a shear rate of 0.1 1/s for 30 s in
CVR 50 controlled stress rheometer (Bohlin Instruments the first stage. Then, in the second stage, a shear rate of 100
Ltd., Cirencester, UK) and a Kinexus pro rotational rheome- 1/s was applied for 30 s in order to cause the breakdown of
ter (Malvern Instruments Ltd., Worcestershire, UK) using the sample’s structure. In the third stage, the shear rate was
parallel-plate geometry (40 mm diameter and 1 mm gap). again dropped to 0.1 1/s and the viscosity recovery was
Batters were allowed to rest for 15 min before analysis to monitored for 600 s. Then, the percentage of viscosity recov-
ensure both thermal and mechanical equilibrium. Samples ery at the end of the test relative to the original apparent vis-
were covered with a thin film of Vaseline oil (PRS-Codex) to cosity value was calculated from the original (g0) and the
avoid evaporation. Temperature was controlled to within final apparent viscosity (gf ) values as (gf 3 100)/g0. Both the
0.18C by Peltier elements in the lower plates kept at 258C, percentage of viscosity recovery and the time (s) taken in the
except when nonisothermal heating processes were carried third stage to achieve rebuild of the viscosity to 90% of the
out. Three replicates of each test were run with samples pre- original value were considered as reliable measurements of
pared on three different days. Results are means of nine rep- the apparent viscosity time dependence of each batter.
lications from three batches of each formulation.
Other Physical Properties
Small-Amplitude Oscillatory Shear (SAOS) The color of the muffin batter in pots was measured with a
Measurements. Stress, Frequency and Temperature Sweep Hunter-Lab model D25 (Reston, VA, USA) color difference
Tests. To determine the LVE region, stress sweeps were run at meter fitted with a 5-cm-diameter aperture. Results were
1 Hz (6.28 rad/s) with the shear stress (r) of the input signal expressed in accordance with the CIELAB system with refer-
varying from 0.01 to 100 Pa. Frequency sweeps were run ence to illuminant D65 and a visual angle of 10 8. The
subjecting the samples to stress that varied harmonically parameters measured were L* (L* 5 0 [black], L* 5 100
with time at variable frequencies (x) from 0.01 to 10 Hz. [white]), a* (1a* 5 red) and b* (1b* 5 yellow). The total
The strain amplitude was set at c 5 0.1%, within the LVE color difference (DE*) between the control sample and each
range (r was 0.13 Pa for 100% WF, 0.08 Pa for 25% CF, 0.09 of the batters was calculated in accordance with Francis and
Pa for 50% CF, 0.10 Pa for 75% CF and 0.16 Pa for 100% Clydesdale (1975).
CF). Temperature sweep tests were performed from 25 to Specific gravity (SG) of the batter was measured as the
1258C at a linear heating rate (1.68C/min). The oscillation ratio of the weight of a standard container filled with batter
frequency was set at 1 Hz, but maintaining the r signal at to that of the same container filled with water in accordance
the minimum value provided by the Bohlin rheometer for with Martınez-Cervera et al. (2012a, 2012b, 2013). Total
parallel-plate geometry (2.98 Pa). For this stress, the corre- soluble solids (TSS) content [g/100 g (w/w)] as measured by
sponding strain amplitude was higher than 0.1%; therefore, refractive index and the pH of the batters were determined
temperature sweeps were carried out outside the LVE range with an Atago (Itabashi, Tokyo, Japan) dbx-30 refractometer
until starch gelatinization process occurred in order to and a Schott CG pH meter (Model 149 842; Schott-Ger€ate
obtain the gel points (cross-over of elastic modulus, G0 and GmbH, Mainz, Germany), respectively. Moisture (%) was
viscous modulus, G00 ) of the batters. determined by drying samples in a Philips microwave oven
(model M-718, 700 W) with output power at 70%. In all
Steady Shear Rheological Measurements cases, three different batches were employed and each for-
mulation was measured in triplicate.
Flow Behavior. Before analyzing flow behavior, the struc-
Optical Microscopy
ture responsible for flow time dependence was previously
destroyed by shearing (Abu-Jdayil 2003; Tarrega et al. 2004). The batter samples were imaged using an Optiphot SMZ
After testing several shearing conditions, for 5 min at 100, microscope (Nikon, Japan) with a magnification of 10 3 in

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RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER M.D. ALVAREZ ET AL.

TABLE 2. EFFECT OF WHEAT FLOUR REPLACEMENT ON RHEOLOGICAL PROPERTIES AND KINETICS PARAMETERS FROM OSCILLATORY TESTS OF
THE MUFFIN BATTERS

Rheological parameters 100% WF 25% CF 50% CF 75% CF 100% CF

d b c c,d
rmax [Pa] 0.642 6 0.01 0.646 6 0.01 0.644 6 0.01 0.643 6 0.01 0.808 6 0.00a
cmax [%] 0.63 6 0.03c 0.96 6 0.06a 0.81 6 0.08a,b 0.76 6 0.11b,c 0.84 6 0.03a,b
Gmax [Pa] 102.0 6 5.3a 67.7 6 4.2c 80.2 6 8.0b,c 86.0 6 11.8a,b 95.8 6 3.3a,b
tan d [–] 0.86 6 0.05b 1.05 6 0.06a 1.06 6 0.15a 1.03 6 0.08a,b 1.09 6 0.03a
Tgel [C] 74.5 6 4.9a,b 79.0 6 2.0a 79.4 6 2.9a 78.0 6 2.3a,b 69.5 6 1.4b
Reaction order [n] 0.19 0.94 0.71 0.70 21.73
lnk0 [k0 in Pa(12n)/s] 36.5 47.1 44.3 47.4 66.9
Ea [kJ/mol] 113.4 144.7 135.6 145.3 204.4

Values are given as mean (n 5 9) 6 standard deviation.

a-d
Different letters in the same row mean significant differences (P < 0.05) among samples according to Bonferroni multiple range test.
WF, wheat flour; CF, chickpea flour; rmax, shear amplitude; cmax, strain amplitude; Gmax , complex modulus; tan d, loss tangent 5 G00 /G0 ; Tgel, start-
ing gel point temperature (G0 2 G00 cross-over); n, reaction order; k0, frequency factor and Ea, activation energy.

clear field mode, and micrographs were taken with a Nikon WF batter had a more developed structure (higher viscoelas-
Digital Coolpix 5000 color digital camera. Each formulation ticity) than the batters containing CF.
was prepared twice, on different days, and four replicates of The frequency dependence of G0 and G00 in the linear
each batter were photographed. region at 258C for both 100% WF and 100% CF batters is
shown in Fig. 1. In the 100% WF batter (Fig. 1A), the G0
Statistical Analysis value was greater than the G00 value in the frequency range
For each property or parameter evaluated, one-way analysis studied, showing a predominantly elastic behavior, corrobo-
of variance (ANOVA) was carried out by using the SPSSV R rating previous findings in muffin batters (Martınez-Cervera
Statistics 19.0 computer program (SPSS Inc., Chicago, IL, et al. 2013; Matos et al. 2014). On the other hand, for the
USA). Bonferroni’s multiple comparison procedure was 100% WF batter, differences between moduli decreased at
used to assess significant differences (P < 0.05) among bat- both lower and higher frequencies.
ters that might allow discrimination between them. In turn, 100% CF (Fig. 1B) and 75% CF batters (results
not shown) had two cross-over points in the frequency range
studied, reflecting that the behavior was predominantly
RESULTS AND DISCUSSION more viscous at low and high frequencies. According to Dol-
let and Raufaste (2014), as low frequency, this is a signature
SAOS Measurements of the influence of coarsening on foam rheology. For batters
Table 2 shows the influence of WF replacement within the containing the lower CF levels (25% CF and 50% CF), the
limits of the LVE range. Critical (maximum) stress (rmax) behavior was also predominantly more elastic at intermedi-
and strain (cmax) amplitudes, complex modulus (Gmax ) and ate and high frequency, but tan d was also more than 1 at
loss factor (tan d 5 G00 /G0 ) were used to limit the LVE range. low frequency (results not shown). Therefore, 100% WF bat-
Critical rmax and cmax values were obtained by defining the ter can be characterized as a soft or weak gel, while samples
range of tolerable deviation as 10% (Campo-Dea~ no and with partial and total WF replacement presented a structure
Tovar 2009). After total WF replacement (100% CF), there between those of a concentrated biopolymer and of a weak
was a significant increase in rmax with respect to the control gel, behave like viscous fluids at low and high frequencies,
batter (100% WF), whereas cmax was similar to the rest of which may be associated with their foaming properties (Xu
the samples with added CF. Therefore, batter with CF at et al. 2014). This result evidences that more deformation
100% level had a higher critical stress (up to 0.808 Pa) than energy can be stored in the 100% WF batter than in the rest
the other batters. In turn, batters prepared with increasing of the samples with added CF, again indicating a more solid
quantities of CF replacing WF had higher cmax values than behavior. Nevertheless, there were no significant differences
the 100% WF sample, reflecting that these systems can with- between the moisture contents of the 100% WF and 100%
stand higher overall strain when the stress was applied with- CF batters, as showed below.
out undergoing irreversible modifications (Navarro et al. Muffin batters themselves make up a combined system
1997). Nevertheless, batters containing CF at any level had where each component has its particular complex structural
lower critical Gmax and tan d values > 1, evidencing a more functionality. Consequently, complex chemical properties
fluid-like character of the systems with added CF within the due to composite interactions between all batter components
limits of the LVE domain. As a result, it seems that the 100% and with water would influence the rheological properties of

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M.D. ALVAREZ ET AL. RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER

FIG. 1. MECHANICAL SPECTRA DATA OF

MUFFIN CONTROL BATTER AND CHICKPEA
FLOUR-BASED GLUTEN-FREE MUFFIN BATTER
Mean values of nine
measurements 6 standard deviation.

these mixtures. At constant ingredients levels, no more than viscoelastic properties of corn starch-based gluten-free bat-
reducing WF by increasing the CF level, the different con- ters were strengthened following the addition of kidney
tents of the main components of both flours (starch and bean, field pea and amaranth protein isolates. Therefore,
protein) determined the rheological properties of the batters most likely the different proportions of wheat and chickpea
at 258C. proteins present in the cellular system modified the viscoe-
As indicated above, protein contents provided by the sup- lasticity of the CF-based muffin batter, inducing a softening
plier were 10.2 and 19.4% for WF and CF, respectively. In effect by increasing the WF replacement level. Differences
turn, according to the supplier, the total carbohydrate con- observed in the viscoelastic behavior of the batters made
tent of CF is 55% w/w, whereas lower starch content ranging without flour mixtures can also be attributed to the different
between 34.9 and 42.9% w/w has been reported for CF (Xu protein source. Chickpea seed protein consists of globulins
et al. 2014). On the other hand, higher both carbohydrate (56.0%), glutelins (18.1%), albumins (12.0%), prolamin
(85% w/w) and starch (78.8% w/w) contents have been (2.8%) and residual proteins (Chang et al. 2012). This rela-
reported for WF (Abebe et al. 2015). As a result, in the raw tively high glutelin content of chickpea could be responsible
batters, viscoelasticity showed a positive relationship with for the lower batter density as the WF is increasingly
starch content and an inverse relationship with protein con- replaced by CF. However, in addition to albumins and glob-
tent. In contrast, Shevkani et al. (2015) reported that the ulins, wheat protein mainly consists of gluten (85%)

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RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER M.D. ALVAREZ ET AL.

FIG. 2. STORAGE MODULUS (G0 ) AND LOSS

MODULUS (G00 ) (A) AND LOSS TANGENT
(TAN d) (B) AS A FUNCTION OF INCREASING
TEMPERATURE IN THE MUFFIN CONTROL
BATTER AND BATTERS WITH WHEAT FLOUR
(WF) REPLACED BY DIFFERENT PERCENTAGES
OF CHICKPEA FLOUR (CF)
Mean values of nine
measurements 6 standard deviation.

composed of monomeric gliadins and polymeric glutenins lus during heating. In turn, Fig. 2B shows the loss tangent as
(Van Bockstaele 2008a). Moreover, the differences observed a function of increasing temperature for the same batters.
could also be attributed to the different functional properties Similar heating patterns were observed in the 25% CF and
of the two types of flour (Chandra et al. 2015). 75% CF batters (results not shown). Reduction of WF
To understand the structural changes that take place in decreased the initial G0 values and the viscoelasticity (values
the different muffin batters during heating, the viscoelastic of tan d became higher), meaning that the presence of only
properties were studied from 25 to 1258C, trying to simulate WF also increased the nonlinear dynamic properties of the
the batter’s behavior in the oven. In addition to the proper- batter system. At 258C, tan d was 1.1 for the control sample
ties of the muffin batter, the structural changes that occur (100% WF), 1.5 for 25% CF, 1.6 for both 50% CF and 75%
during baking are also determining factors in bubble forma- CF and 1.7 for 100% CF.
tion and evolution and in the final baked product structure The presence of either chickpea starch or proteins pro-
and texture (Martınez-Cervera et al. 2012a,b). As indicated duced changes in the shape of the heating curves that have
above, at the beginning, the nonisothermal heating tests been associated with both starch gelatinization and protein
were carried out in the nonlinear viscoelastic range. coagulation processes in different muffin batter formulas
The effect of reducing WF (at 0, 50 and 100% reduction (Martınez-Cervera et al. 2012a,b; Matos et al. 2014). In all
levels) can be seen in Fig. 2A, which shows the elastic modu- the batters, the initial increase in temperature produced a

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M.D. ALVAREZ ET AL. RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER

decrease in the G0 values (Fig. 2A) associated with an the presence of a mixture of both flours with different pro-
increase in the tan d values (Fig. 2B). In the 100% WF and tein fractions and starches. This finding may be associated
100% CF samples, the G0 values decreased with temperature with a possible thermodynamic incompatibility between
until approximately 50 and 458C, respectively. In the case of polysaccharides, proteins, or both occurring in batters for-
the batters containing both types of flour, the G0 values mulated with mixtures of both flours. It was found that
decreased considerably between 25 and approximately 608C. many proteins are thermodynamically incompatible in aque-
Initially, this decrease could be associated with the effect of ous solutions (Tolstoguzov 1997). During mixing of flour
increasing temperature. Matos et al. (2014) explained that with water, albumins, globulins, water-soluble starch (from
gluten proteins show a progressive loss of strength due to damaged starch granules) and pentosans form a liquid aque-
protein unfolding, resulting in a decrease of the elastic mod- ous phase. This is immiscible with glutelins and gliadins,
ulus and undergoes a thermal transition around 608C. How- which form a separate gluten phase. Moreover, the increase
ever, it has also been stated that at a temperature in Tgel values in the presence of both flours might also be
approximately of 458C, the decrease in G0 and G00 values may attributable to the fact that either starch granules or proteins
be associated with CO2 formation in the batter, diffusion need more time for swelling and unfolding, respectively,
into occluded air cells, and expansion, reducing the density because of water competition. Lower starch content is related
of the batter (Martınez-Cervera et al. 2012a,b). Conse- to lower Tgel. The results suggest that not only the level of
quently, in comparison to the control batter, total absence of starch but also their properties (swelling capacity, water
gluten could have a negative effect on air retention capacity. absorption and holding capacities and gelation capacity)
In contrast, presence of both WF and CF would indicate a would influence the Tgel values of the batters.
higher capacity of the batter to incorporate air bubbles. After gel point, the G0 and G00 of the samples continued
Following the G0 modulus of all the batters started to increasing until a maximum value were reached; this period
increase gradually with increasing temperature (Fig. 2A), is associated with complete starch gelatinization and/or pro-
and the cross-over of G0 and G00 was reached (data not tein denaturation or coagulation. Note that the behavior pat-
shown), which was also associated with increased viscoelas- tern of G0 and G00 between the Tgel and the final heating
ticity (values of tan d inferior to 1; Fig. 2B). Gel point, most temperature was fairly similar in all the batters, with close
commonly defined as the time at which G0 and G00 intersect, maximum values of the two moduli. At this stage, the behav-
generally occurs as a result of the early stage of starch gelati- ior of the batter is probably dominated by the presence of a
nization (Ahmed et al. 2008); this stage corresponds to when protein network. At the end of the temperature sweep, the
starch granules swell and melt. Effect of replacing WF on the increase in temperature also reduced the values of tan d (val-
starting gel point temperatures (Tgel) of the batters is shown ues closer to 0) in a similar fashion (Fig. 2B). The different
in Table 2. There were nonsignificant differences between the evolution of the tan d throughout the temperature sweep
Tgel values of the 100% WF batter and the gluten-free muffin could be indicating the effect of the distinct protein fractions
batter, whereas the presence of both flours increased the present in the batters, since they have different structures,
starch gelatinization temperature of the batter. Note that in molecular properties, and different functional properties.
the 25% CF, 50% CF and 75% CF batters, the delay in the The nonisothermal kinetic relation based on the experi-
temperature of initial increase of both moduli correlated mental data and regression analysis was determined follow-
well with the delay in the Tgel. Analogously, in the 100% CF ing the steps described by Rhim et al. (1989) for a linearly
batter, the early increase of both moduli resulted in the low- increasing temperature system. In this study, the tempera-
est Tgel. In addition, the advance and the delay in tempera- ture range selected for the kinetic analysis was the range
tures in comparison to the control batter were always of from the starting gel point temperature (Tgel: cross-over of
58C. G0 and G00 ) up to 1008C, which was therefore considered as
During heating, the conformational changes experi- the temperature where G0 achieved its maximum value. Data
mented by the wheat and chickpea starches and proteins from 100 to 1258C were discarded because of their high dis-
were largely responsible for the predominant elastic behavior persion, which is related to sample desiccation occurring at
of the batters. The delay in starch gelatinization in the sam- higher temperatures.
ples containing either WF or CF could be crucial to avoid The general form for nonisothermal kinetics combining
earlier thermosetting and give enough time for appropriate reaction rate, time–temperature profile and Arrhenius rela-
air and vapor expansion during baking (Martınez-Cervera tionship was described elsewhere (Rhim et al. 1989; Ahmed
et al. 2012a,b). However, the early thermosetting associated et al. 2008; Alvarez et al. 2014). The authors just cited
with the lack of gluten of the 100% CF batter could cause showed that the kinetic relation can be used for gelatiniza-
inadequate expansion of individual air cells. In turn, the tion kinetics and converted to Eq. (1), and the concentration
delay in the starch gelatinization process in the 75, 50 and (C) and change in concentration (dC) can be replaced by G0
25%WF replacements with CF could be attributed merely to and dG0 . The negative sign of kinetic equation is substituted

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RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER M.D. ALVAREZ ET AL.

by a positive sign because of the increase G0 during heating protein coagulation occurring at higher temperatures.
(positive dG0 ). According to Ahmed et al. (2008), the significant increase in
     Ea values of 100% CF batter might also be attributable to the
1 dG0 Ea 1 fact that the starch granules cannot swell to their equilibrium
ln 5lnk 0 2 (1)
G0 n dt R T volume because of limited availability of water. In the 100%
CF batter, the higher protein content could also compete
where G0 (Pa) and dG0 /dt (Pa/s) denote the elastic modulus with starch for water influencing and increasing its Ea value.
and the derivative of G0 with respect to time t, respectively,
k0 the pre-exponential or frequency factor (Pa(12n)/s), n is Steady-State Shear Measurements
the reaction order, Ea is the activation energy (J/mol), T is
After reducing the flow time dependence, the flow behavior
the absolute temperature (K) and R is the universal gas con-
was also measured in the muffin batters. Reference to the
stant (8.314 J/molK).
classification of time-independent flow behavior of fluid
In this study, derivatives of experimental data were calcu-
foods shows that all the batters exhibited non-Newtonian
lated by sixth-order polynomial fits approximating the
shear-thinning behavior, which is a curvature downward on
change of G0 versus t (for all the cases, the corresponding
the shear rate axis (Alvarez and Canet 2013). Data obtained
mean R2 value was 0.999 6 0.002) from 25 to 1008C. A mul-
were fitted to the Casson and Herschel–Bulkley models (Rao
tiple linear regression was then used with the muffin batter
1999). The yield stress value used in the Herschel–Bulkley
kinetic data set to determine the order of the reaction (n)
model was that obtained by fitting the experimental data to
after changing the above equation into the following linear
the Casson model, as described by Tarrega et al. (2004). All
form:
batters gave a satisfactory goodness of fit to the Casson
 0    model (Table 3), with R2 values ranging between 0.997 and
dG Ea 1
ln 5lnk0 1nlnG0 2 (2) 0.999. The yield stress values were high—higher than 4 Pa at
dt R T
100% WF and higher than 12 Pa at 100% CF—indicating
The reaction orders obtained from the above equation for plastic behavior. The high yield stress value obtained at the
muffin batters are shown in Table 2. The values of the kinetic highest replacement level shows that the 100% CF sample
parameters were derived from the mean curves obtained for had a significantly higher initial resistance to flow, as well as
each batter. The 100% WF sample showed a reaction order a significantly higher Casson plastic viscosity, indicating the
very close to zero, whereas the calculated n values were closer existence of a more entangled structure in absence of gluten.
to one for the muffin batters made with mixtures of both Higher particle size of CF can affect the muffin batter viscos-
flours. In turn, the n of the above Eq. (2) was found to be ity (Singh et al. 2015). Nevertheless, experimental data fitted
negative for the 100% CF batter. However, the reaction order better to the Herschel–Bulkley model, with R2 values ranging
was further verified by considering n 5 0 and n 5 1, in Eq. between 0.999 and 1.000. At 258C, n was significantly lower
(1), which confirmed a better fit for zero-order reaction and K was much higher in 100% CF than in the other bat-
kinetics in the batters made without mixtures (100% WF ters, again indicating greater pseudoplasticity and consis-
and 100% CF), as well as a better fit for first-order reactions tency of the gluten-free batter under large deformations.
in the case of the batters containing both types of flour. For Batter consistency is an important physical property as it
the zero-order reactions, the R2 values were higher than is closely related to the final quality of an aerated baked
0.990, except for the 100% CF batter (0.954). However, the product. Air incorporation and retention, bubble stability
applicability of first-order reaction kinetics for 100% WF and the generation of convection currents in the batter dur-
and 100% CF batters decreased the goodness of the fits ing baking are dependent on the initial batter viscosity and
(0.950 and 0.946, respectively). Consequently, zero-order on the evolution of bulk viscosity during heating (Martınez-
reaction kinetics was considered in all five batters in order to Cervera et al. 2012a,b). During baking, the velocity gradient
compare the values of the kinetic parameters obtained. in the batter as a whole will induce convection current at a
Zero-order reaction kinetics has also been reported for CF given moment that depends on its viscosity, with low batter
slurries in a wide moisture range from 1:5 to 1:2 flour-to- viscosity resulting in more convection flow (Martınez-Cer-
water ratios (Alvarez et al. 2014). vera et al. 2011). According to the authors just cited, the
There was an increase in both the ln k0 and the Ea values increasing viscosity as CF levels rose could be an unfavorable
of the muffin batters with the increase in the percentage of factor for the quality of the final baked product. Moreover,
WF replacement. The magnitude of Ea was 113.4 and 204.4 an excessive increase in viscosity could lead to problems in
kJ/mol for the 100% WF and 100% CF batters, respectively. handling the batter, in mould filling (metering) and in clean-
The lower Ea when there was no CF in the batter implies ing the machinery, or to greater energy expenditure on
that it was more favorable for starch gelatinization and/or pumping. Negative effects of replacing WF with CF could be

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M.D. ALVAREZ ET AL. RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER

TABLE 3. EFFECT OF WHEAT FLOUR REPLACEMENT ON RHEOLOGICAL PROPERTIES FROM STEADY-STATE SHEAR TESTS AND OTHER PHYSICAL
PROPERTIES OF THE MUFFIN BATTERS

Rheological parameters 100% WF 25% CF 50% CF 75% CF 100% CF

b b b b
r0 [Pa] 4.2 6 0.5 4.5 6 1.6 3.2 6 0.3 4.9 6 0.7 12.6 6 0.8a
gC [Pa s] 2.3 6 0.3c 2.5 6 0.1b,c 3.0 6 0.1b,c 3.2 6 0.4b 4.4 6 0.5a
K [Pa sn] 8.6 6 0.6b 8.6 6 1.8b 8.7 6 0.3b 10.0 6 1.3b 19.9 6 2.0a
n 0.76 6 0.01b,c 0.78 6 0.03a,b 0.80 6 0.01a 0.79 6 0.02a,b 0.73 6 0.01c
go [Pa s] 51.7 6 1.6a 38.2 6 2.4c 34.5 6 1.6c 35.3 6 0.2c 45.4 6 0.9b
gf [Pa s] 43.2 6 0.1b,c 40.7 6 1.5b,c 40.2 6 1.1c 43.6 6 1.2b 66.3 6 0.7a
Viscosity recovery [%] 83.6 6 2.4d 106.8 6 6.5c 111.9 6 3.3b,c 123.5 6 3.3b 146.0 6 4.0a
Time to recover 90% of go [s] >600 121 6 25a 52 6 3b 26 6 11b,c 10 6 1c
Multiplicative constant, a 1.30 0.78 0.93 0.84 0.83
Power index, b 1.19 1.34 1.31 1.48 1.24
L* 66.9 6 0.1a 66.6 6 0.2b 62. 7 6 0.2d 63.2 6 0.2c 62.5 6 0.2d
a* 1.5 6 0.06d 2.0 6 0.25c 2.8 6 0.08b 2.9 6 0.15b 3.3 6 0.23a
b* 14.5 6 0.1e 19.3 6 0.3d 23.1 6 0.3c 24.2 6 0.6b 25.3 6 0.3a
€
AE* 0.0 4.8 6 0.3d 9.7 6 0.2c 10.5 6 0.5b 11.8 6 0.3a
SG [g/L] 0.97 6 0.00b 0.97 6 0.01b 1.01 6 0.01a 0.98 6 0.01b 0.94 6 0.01c
TSS (g/100 g [w/w]) 22 6 0.2c 21 6 0.3c 25 6 0.2b 24 6 0.3b 27 6 0.5a
pH 7.8 6 0.02b 7.7 6 0.01c 7.5 6 0.02d 7.5 6 0.02d 7.9 6 0.01a
Moisture [%] 13.3 6 0.8b 16.2 6 0.8a 14.8 6 0.8a,b 17.4 6 0.6a 13.4 6 0.8b

Values are given as mean (n 5 9) 6 standard deviation.

a–d
Different letters in the same row mean significant differences (P < 0.05) among samples according to Bonferroni multiple range test.
WF, wheat flour; CF, chickpea flour; r0, Casson yield stress; gC, Casson viscosity; K, Herschel–Bulkley consistency index; n, Herschel–Bulkley flow
behavior index; go, original apparent viscosity; gf, final apparent viscosity after 600 s of recovery; a, b, power model coefficients from modified
Cox–Merz rule; L*, luminescence; a*, red color; b*, yellow color; AE*,€ total color difference; SG, specific gravity and TSS, total soluble solids.

because of the higher protein, and/or lower starch contents tent could induce and reinforce new intermolecular attrac-
in CF, corroborating previous findings (Singh et al. 2015). tions resulting in a dilatant system.
For each batter, three-step shear rate tests were carried Different functional properties of both flours could
out. Table 3 shows the values of the parameters derived from explain the differences observed. Foam capacity of protein
the tests. The original apparent viscosity (g0) value was high- refers to the amount of interfacial area that can be created by
est in the 100% WF batter, agreeing with the more solid-like the protein, whereas foam stability refers to the ability of
(elastic) response at small deformations. In turn, the 100% protein to stabilize against gravitational and mechanical
CF batter had an intermediate g0 value. In contrast, the final stresses (Chandra et al. 2015). These authors obtained, for
apparent viscosity (gf ) value after restructuring for 600 s was WF, foam capacity and stability values of 12.9 and 1.9%,
significantly (P < 0.05) higher for the 100% CF batter (Table respectively, but both functional properties increased with
3). As a result, the percentage of viscosity recovery calculated decreasing in the proportions of WF up to 55%. In turn,
with respect to the g0 value was 83.6% for the 100% WF foam capacities of different CFs varied from 9.6 to 11.5%
sample. This percentage increased significantly as the level of (Xu et al. 2014). It is likely that the CF used in this study had
WF replacement increased, being 146.0% for the full amount much higher foam capacity and stability than the WF, which
of replacement. Therefore, the time required to recover 90% could justify the different rheological behavior of both 100%
of g0 after structure breakdown, it could not be obtained for WF and 100% CF batters before and after shearing under
100% WF batter, being higher than >600 s. However, this large deformations. A positive relationship between foam
time decreased significantly with increasing percentage of capacity and foam stability was also observed by Chandra
WF replacement, and the lowest value corresponded to the et al. (2015). On the other hand, according to the author
100% CF sample. just cited, emulsion stability can also be greatly increased
In the CF-based muffin batters shearing increased the final when highly cohesive films are formed by the absorption of
viscosity (Table 3), reflecting atypical structural reinforce- rigid globular protein molecules that are more resistant to
ment probably because of further intermolecular aggregation mechanical deformation.
of the protein. Consequently, from three-step shear rate tests, The three-step shear rate test also provides information
it seems that as reducing WF by increasing the CF level, the on the degree of structural stability. The highest value of
systems tend to have a shear-thickening flow behavior. In time to recover was obtained for 100% WF sample, which
the 100% CF sample, it is possible that greater protein con- was the most stable batter to the applied shear strain. Most

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RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER M.D. ALVAREZ ET AL.

likely, during shearing, the emulsifying activity of CF was the human eye (Bodart et al. 2008). Similar results were
higher than that of WF. Proteins act as emulsifier mainly obtained by Martınez-Cervera et al. (2012a) when a study
because of their surface active properties which are in turn was made of the color of low-sucrose muffins in which the
related to their structural and surface characteristics. Pro- sucrose had been totally or partially replaced by a sucralose:-
teins from CF were possibly more active due to their great polydextrose mixture. Analogously, the protein content of
proportion of vicilins and legumins which were reported to navy bean flour had a significant effect on the color of the
possess high emulsifying properties (Shevkani et al. 2015). cakes (Singh et al. 2015).
The surface activity of CF proteins could be associated with The retention of air in batters is reflected by the specific
the formation of interfacial layer causing a higher viscosity gravity (SG) values (Martınez-Cervera et al. 2013). The effect
(Chandra et al. 2015). on SG of WF replacement with CF can be seen in Table 3.
In contrast, under SAOS measurements 100% WF batter For the replacement levels of 25% and 75%, the SG values
had higher viscoelasticity (Table 2) and also more time sta- were not significantly different from those of the control bat-
bility, exhibiting more elasticity. Recovery time of non- ter. A significant increase in SG was found for the 50% CF
Newtonian fluids depends on both particle orientation and sample, whereas a significant decrease in SG was observed
collision effects during structure rebuilding. It is obvious for the 100% WF replacement. Lower SG is associated with
that the 100% CF sample exhibited the fastest rate of struc- higher aeration of the batter (Khalil 1998), indicating a
ture rebuilding. The results show that the reduction or total higher capacity to incorporate air bubbles during beating
absence of WF in the batter, i.e., of gluten, significantly accel- and retain them (Bath et al. 1992). SG has also been found
erates the recovery rate when the viscosity function is con- to decrease in sponge cakes on replacing sucrose with wheat
sidered alone, without taking the elastic component into starch, sorbitol and aspartame (Baeva et al. 2003), as well as
account. Bubbles deformed at high shear rates can either in muffin batter on replacing either sucrose with sucralose:-
break or coalesce due to the interaction with the flow (Dollet polydextrose mixtures (Martınez-Cervera et al. 2012a) or fat
and Raufaste 2014). with Nutriose (Martınez-Cervera et al. 2013). The authors
Applicability of the Cox–Merz rule was tested. For all the just cited reported that the volume of the muffins is deter-
batters, the complex viscosity (g*) magnitudes in the LVE mined by the air trapped in the batter, the capacity of the
range were always higher than the apparent viscosity (gapp) batter to retain this air and the moment at which starch
magnitudes. Therefore, a power (Eq. 3) modified Cox–Merz gelatinization occurs. In this study, the gluten-free batter
rule was used for evaluation of the rheological properties showed an advance in starch gelatinization (Table 2), which
(Augusto et al. 2013). it could reflect a lower gas retention capacity during heating.
Gas retention depends on the viscosity of the batter (or,
gx5a½gapp ð_c Þb x5_c
(3) rather, the liquid between the bubbles) at temperatures at
which gas is generated (Martınez-Cervera et al. 2013). Muf-
The values of parameters a and b are shown in Table 3, fin batter in presence of egg white protein also had the low-
with R2 higher than 0.997 for the 100% WF, 25% CF and est SG, which showed that more air was incorporated and
50% CF batters. Both 75% CF and 100% CF batters exhib- retained during mixing (Matos et al. 2014).
ited lower R2 (0.967 and 0.980, respectively). The difference The TSS content of the muffin batter increased signifi-
between viscosities was highest for 100% WF (highest value cantly as a result of increasing the percentage of WF replace-
of a). The power indices ranged from 1.19 for 100% WF to ment (Table 3), which could be ascribed to higher protein
1.48 for 75% CF, indicating that the relationship between the content. The 100% CF batter also had the highest pH. In
viscosities was clearly nonlinear (b values are not close to 1). comparison with the 100% WF and 100% CF samples, bat-
ters made with 25, 50 and 75% WF reduction levels showed
Other Physical Properties of Muffin Batter
significantly (P < 0.05) lower pH and higher moisture.
An increase in WF substitution produced a decrease in the Higher moisture can be associated with higher water absorp-
lightness of the batter and an increase in the redness and yel- tion due to the presence in these batters of two distinct sour-
lowness values (Table 3), that is to say, the batter acquired a ces of protein and starch. However, there were no significant
more saturated yellowish color. The a* and b* values were differences in the moisture determined in the batters pre-
significantly (P < 0.05) higher in the formulations with a pared with the 0 and 100% WF reduction levels. The pH val-
higher degree of WF substitution with CF, reflecting that the ues of the flours in water suspension are important because
reduced-WF muffin batters had a more orangey color than some functional properties (mainly related to protein) such
the 100% WF control. In addition, the DE* values were in as nitrogen solubility and emulsion properties are highly
excess of 3 units for all the batters when compared with the affected by pH changes. The particle size and protein content
control; therefore, these differences are clearly appreciated by both affected the pH of the cake batter elaborated with navy

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M.D. ALVAREZ ET AL. RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER

FIG. 3. OPTICAL
MICROSCOPY IMAGES FOR
THE CONTROL BATTER (100%
WF) AND BATTERS PREPARED
WITH INCREASING QUANTITIES
OF CHICKPEA FLOUR (CF)
REPLACING WHEAT FLOUR
(WF) (25% CF, 50% CF, 75%
CF AND 100% CF) (310)

bean flour, but higher protein contents lowered the pH could be the consequence of the lower elasticity of the WF-
(Singh et al. 2015). reduced batters, favoring bubble buoyancy (Martınez-Cer-
vera et al. 2012a). As the beating energy provided to all the
Microscopy Images of Muffin Batter batter formulations was the same, a lower elasticity may
have allowed the larger air cells to coalesce and escape while
Micrographs obtained for the control batter, and for the 25, retaining the small ones. Nevertheless, during baking, a sec-
50, 75 and 100% WF-replaced batters are shown in Fig. 3. ond step takes place: the air cells are expanded by CO2 and
When WF was replaced by increasing quantities of CF, a the vapor pressure generated, resulting in the formation of
change in air bubble size and quantity was observed: the the final gas cells, which influence the texture of the finished
number of larger-diameter air bubbles tended to decrease, product (Matos et al. 2014). In principle, a larger number of
and generally the number of air bubbles present in the bat- small gas nuclei in the batter is a positive factor for final
ters seemed to increase. In 50% CF and 75% CF batters, an quality, as it will favor the formation of tiny air cells that can
intermediate size of air bubbles was found. As the percentage enlarge during baking, which in turn favors height and vol-
of WF substitution increased until 100%, an increase in the ume gain (Martınez-Cervera et al. 2012a,b). One explana-
amount of air in the 100% CF batter was observed, in agree- tion for the greater number of air bubbles found in the
ment with its lower SG value. This reduction in bubble size gluten-free muffins is that the early starch gelatinization

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RHEOLOGICAL PROPERTIES OF CHICKPEA MUFFIN BATTER M.D. ALVAREZ ET AL.

advanced batter thermosetting, which favoured bubble ALVAREZ, M.D. and CANET, W. 2013. Time-independent and
retention. More research is needed to get an understanding time-dependent rheological characterization of vegetable-based
of the influence of this higher number of small air bubbles infant purees. J. Food Eng. 114, 449–464.
in the batter on the final quality of the baked muffin. ALVAREZ, M.D., FUENTES, R., OLIVARES, M.D., CUESTA, F.J.
and CANET, W. 2014. Thermorheological characteristics of
chickpea flour slurry as affected by moisture content. J. Food
CONCLUSIONS Eng. 136, 9–18.
SAOS measurements indicated that the CF-based muffin AUGUSTO, P.E.D., IBARZ, A. and CRISTIANINI, M. 2013. Effect
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batters had greater conformational stability when the stress
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was applied and higher tan d values (>1), but lower critical
Cox–Merz rule. J. Food Eng. 114, 57–63.
Gmax values than the 100% WF control batter, reflecting
BAEVA, M.R., TERZIEVA, V.V. and PANCHEV, I.N. 2003. Struc-
their lower degree of viscoelasticity. During heating, zero-
tural development of sucrose-sweetened and sucrose-free
order reaction kinetics described the batter gelatinization
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The authors wish to thank the Spanish Ministry of Economy Food Res. J. 19, 521–525.
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