Food and Bioproducts Processing 135 (2022) 190–204

Available online at www.sciencedirect.com

Food and Bioproducts Processing

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

Extrusion of pea snack foods and control of

biopolymer changes aided by rheology and
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simulation
⁎
I. Jebalia, G. Della Valle, M. Kristiawan
INRAE, UR 1268 Biopolymers Interactions and Assemblies (BIA), 44316 Nantes, France

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

Article history: Pea flour and a blend of pea starch and protein isolate with a starch-to-protein ratio close
Received 11 May 2022 to 2/1 were processed using co-rotating twin-screw extruders. Different extruder scales
Received in revised form 2 August operated at a moisture content of 18–35% and a screw speed of 120–700 rpm resulted in
2022 large intervals of melt temperature T (95–165 °C) and specific mechanical energy SME
Accepted 4 August 2022 (150–2000 kJ/kg). With increasing T and SME, starch solubility in water increased due to
Available online 8 August 2022 starch melting and depolymerisation, and protein solubility in SDS decreased due to
formation of protein aggregates linked by disulphide bonds. Extruded foods’ morphology
Keywords: was studied by CLSM. Protein cross-linking increased the median size of protein ag­
Morphology gregates; starch destructuration increased the area of the starch phase to the detriment of
Protein aggregates the protein one. Melt shear viscosity was determined using a pre-shearing capillary rhe­
Starch ometer. The melts exhibited shear-thinning behaviour according to a power-law model,
Solid foams with values close to those of model parameters observed for pea flour and SP 2/1 blend.
1D twin-screw extrusion model The rheological model was implemented in a 1D global extrusion model to simulate pea
Viscosity ingredient extrusion. Satisfactory correlations between predicted extrusion variables (T,
SME) and biopolymer transformation suggested that products with target structure can be
obtained using simulation to tune extrusion conditions.
© 2022 Institution of Chemical Engineers. Published by Elsevier Ltd. All rights reserved.

Extrusion is an efficient, versatile, simple and safe process

1. Introduction
that is widely used to develop various products (Ek and
Ganjyal, 2020). It can be applied to incorporate protein-rich
Pulse crops (pea, lentil, bean, etc.) are an excellent source of
plant ingredients into foods. The extrusion process consists
protein (20–30% dry basis), dietary fibre (10–30%), starch
of a succession of two phenomena: (1) transition from a di­
(40–55%), vitamins and minerals, and they are low in sugar,
vided solid medium (powder) to a deformable continuous
sodium and fat (Boye et al., 2010). Contrary to cereals, pulse
one (melt) due to thermo-mechanical treatment and che­
proteins are high in lysine and low in sulphur-containing
mical action; (2) expansion of continuous medium to a solid
amino acids: cysteine, methionine, and tryptophan. There­
cellular matrix due to a sudden pressure drop at the die exit.
fore, they are good candidates to complement cereals in ex­
The density of products depends on extrusion conditions,
truded foods. The formulation of expanded snacks made
e.g., high feed moisture content and low melt temperature
entirely from pulses is an interesting way to promote the
inside the die results in dense materials (Kristiawan and
consumption of healthy legume-based foods in the young
Della Valle, 2020). The use of physical blowing agents, such
population.
as N2 gas, can increase food expansion accompanied by
small and uniform cells (Luo et al., 2020).
Elevated extrusion temperatures and shear forces in­
⁎
Corresponding author. crease biopolymer transformation such as starch melting
E-mail address: and depolymerisation, protein denaturation and aggregation,
magdalena.kristiawan@inrae.fr (M. Kristiawan).
https://doi.org/10.1016/j.fbp.2022.08.001
0960-3085/© 2022 Institution of Chemical Engineers. Published by Elsevier Ltd. All rights reserved.
 Food and Bioproducts Processing 135 (2022) 190–204 191

Nomenclature flour or %), and gain in WSIsolids of extruded

product (%).
α water plasticisation coefficient (di­ WSIstarch, ΔWSIstarch WSI of starch (in kg/kg dry starch
mensionless). in flour or %), and gain in WSIstarch of extruded
C, D, n0, ai parameters in fitting equations. product (%).
ANOVA analysis of variance.
aMC moisture content-based shift factor (di­
mensionless).
aT temperature-based shift factor (di­ and product browning (Ek et al., 2020; Kristiawan and Della
mensionless). Valle, 2020). The melting dataset is widely available for
CSLM confocal laser scanning microscopy. starches but there is no equivalent entity for proteins. The
DTE dithioerythritol. knowledge of starch melting temperature at various
DSC differential scanning calorimetry. moisture contents is primordial for setting extrusion condi­
D50 median protein aggregate size (μm). tions to obtain fully melting matrices adapted for texturing.
E activation energy (J/mol). Increasing dissipated heat promotes molecular changes in
η viscosity (Pa.s). proteins that take place in several steps: association, dis­
ηG superposed viscosity after time-temperature sociation and aggregation of subunits by non-covalent (hy­
translation and time-moisture content drophobic, ionic, H) and covalent (disulphide, isopeptide)
translation (Pa.s). bonds (Camire, 1991; Day and Swanson, 2013; Stanley, 1989).
, app true and apparent shear rates (1/s). Moreover, increasing shear energy promotes protein un­
Ii starch-protein interface index (di­ folding, resulting in protein re-association, which means that
mensionless). protein unfolding and cross-linking occur simultaneously
K, K0 flow consistency index (Pa.sn) and its value during extrusion (Della Valle et al., 1994; Fang et al., 2013).
at reference temperature T0 and reference These structural changes of biopolymers affect melt
moisture content MC0. rheology, which in turn influences the process itself and melt
L/D length-to-diameter ratio. expansion and, thus, the final structure of the food (Beck
LSD leas significant different test. et al., 2017; Kristiawan et al., 2018, 2020; Kristiawan and Della
MC, MC0 moisture content and its reference value (% Valle, 2020; Xie et al., 2012). In addition, an intense protein
in wet basis). cross-linking can lead to extruded products with the ap­
N screw speed (rpm). pearance of surface irregularities and breakup (Pommet
Nu Nusselt number. et al., 2003). The structure of expanded solid foods can be
n flow behaviour index (dimensionless). described at various structural levels by density, cellular
P pressure (Pa), measured at die entrance of structure and morphology, or the starch-protein organisation
extruder and Rheoplast®. in the cell walls of these foods (Guessasma et al., 2011). The
PAR protein area ratio. cell wall material can be considered as a composite of starch
PF pea flour. and protein whose morphology depends on composition,
PPI pea protein isolate. extrusion conditions and biopolymer transformation
P_DTE, ΔP_DTE protein solubility in DTE (%) and gain in (Habeych et al., 2008; Jebalia et al., 2019; Kristiawan et al.,
protein solubility in DTE (%). 2018). In turn, the structure of extruded foods, expanded or
P_SDS, ΔP_SDS protein solubility in SDS (%) and loss of not, controls their texture and end-use properties, including
protein solubility in SDS (%). nutritional ones (Brennan et al., 2013; Carbonaro et al., 2012;
QF mass flow rate of powdery raw material and Laleg et al., 2016; Philipp et al., 2017, 2018).
water (kg/h). Most of the research on the extrusion of pulse legumes
QV volumetric flow rate of the material (mm3/s), has focused on experimental studies that link operating
R gas constant (J/mol.K). conditions and recipes to extrusion variables, food structure
Ri radius of the capillary (mm). and functional properties using statistical modelling (Beck
S cross-section of the central piston (mm2). et al., 2018; Berrios et al., 2008; Della Valle et al., 1994; Félix-
SDS sodium dodecyl sulphate. Medina et al., 2020; Rangira et al., 2020; Sumargo et al., 2016).
SE-HPLC size-exclusion high-performance liquid Since extrusion trials are laborious and time-consuming, the
chromatography. challenges in extrusion optimisation, scale-up and trouble­
SP 2/1 blend of pea starch and pea protein isolate shooting can be tackled using extrusion modelling. A 1D
with starch-to-protein ratio = 2 /1. global model that calculates the changes in the main ther­
SME, SME_mes, SME_com specific mechanical energy, momechanical parameters such as dissipated energy, tem­
retrieved experimentally and predicted (kJ/kg). perature, viscosity and pressure has been proposed by Della
τw wall shear stress (Pa). Valle et al. (1993) and Vergnes et al. (1998). Knowledge of the
T, T0 melt temperature and its reference viscous behaviour of molten starchy products obtained in
value (°C). extrusion conditions is pivotal for modelling the material
T_mes, T_com measured and predicted melt tem­ flow in an extruder. However, this data is currently lacking in
perature at die entrance (°C). the industrial field, mainly because classical rheometers are
Td, Tb imposed die and last barrel temperature (°C). not relevant and measurements are difficult. Using an off-
Tm melting temperature of starch (°C). line pre-shearing capillary rheometer (Rheoplast®) and spe­
w.b. wet basis. cific in-line slit die rheometers, not widely available, makes it
WSIsolids, ΔWSIsolids WSI of total solids (in kg/kg dry possible to produce structural changes in starch and proteins
192 Food and Bioproducts Processing 135 (2022) 190–204
Table 1 – Chemical composition of raw material (% dry basis).
Raw material Proteins Starch
c c
Pea flour (PF) 24 ± 0.2 46 ± 0.3
Pea starch 0.5 ± 0.04d 98 ± 2a
Pea protein isolates (PPI) 88 ± 0.5a 0.4 ± 0.01d
SP 2/1 32 ± 0.4b 63 ± 0.4b
*Fibre and other components, determined by difference method. ng: not determined. Means with the different superscripts within a column
are significantly different (significance level of 0.05).
before rheological measurement (Horvat et al., 2013; Vergnes
and Villemaire, 1987; Xie et al., 2012).
There is still a lack of knowledge and data, particularly in
relation to melt rheology, necessary to foresee the structural
changes of the biopolymeric components that govern snack
features. Consequently, to date, the design of pulse based-
extruded products at the industrial level is still based on a
trial-and-error approach. Given this context, this work firstly
aims to ascertain the effect of extrusion variables such as
temperature and specific mechanical energy on starch and
protein structural changes of snacks and composite mate­
rials, represented as snack cell walls, and the impact of
biopolymer transformation on composite morphology. In
contrast with “pea snacks” (Kristiawan et al. 2018), the da­
taset of the impact of measured extrusion variables on starch
and protein structural change of “pea composites” and, in
turn, composites morphology has not been published before.
Then, by determining the viscosity of molten pea ingredients
under extrusion conditions, our second goal is to predict
structural changes using extrusion modelling. For this pur­
pose, we will use extrusion data available from the literature
and the present work that focuses on two raw materials: pea
flour and a blend of pea starch and pea protein isolate (SP 2/1)
with a starch-to-protein ratio of 2/1 (dry basis). This work is
original because the determination of viscous behaviour of
pulses-based ingredients and the design of pulse-based ex­
truded foods and composites using rheology-based process
simulation never be accomplished anywhere.
2. Materials and methods
2.1. Raw materials
Pea starch (median particle diameter: D50 = 27 µm) and pea
protein isolates (PPI; D50 = 72 µm) were supplied by Roquette
(France). Pea flour (D50 = 480 µm) was purchased from
Sotexpro (France). A blend with a starch/protein ratio of 2/1
(weight/weight, dry basis), called SP 2/1, was obtained by
mixing pea starch and PPI using a Kenwood mixer. The pea
flour had a starch-to-protein ratio similar to that of SP 2/1
(1.92/1). The chemical composition of the raw materials was
determined by standard enzymatic and Kjeldahl methods,
described in detail elsewhere (Kristiawan et al., 2018). All
measurements were conducted in triplicate. The composi­
tions are presented in Table 1. The reported values are the
average values with a standard deviation. All raw materials
were significantly different at the significance level of 0.05
regarding the content of starch, protein and other con­
stituents such as fibre.
The melting temperature (Tm) of hydrated pea in­
gredients was retrieved from previous works (Jebalia et al.,
2019; Kristiawan et al., 2018). It was measured using a DSC
apparatus following the method of Logié et al. (2017) and was
Ash Lipid Sugar Others*
b
2 ± 0.04 2 ± 0.02 ng 26 ± 0.3a
0.1 ± 0.01c – ng 1.4 ± 0.05d
4 ± 0.09a – ng 7.6 ± 0.04b
2 ± 0.04b – ng 3 ± 0.05c
defined as the maximum temperature of the melting en­
dothermic peak. Some results are reported in Table 2.
2.2. Extrusion experiments
The extrusion trials for manufacturing dense composites
from pea flour and SP 2/1 were conducted using a laboratory-
scale co-rotating twin-screw extruder (Thermo Scientific™
Process 11, Germany), as described in detail by Jebalia et al.
(2019). The screw diameter was 11 mm, and the length-to-
diameter (L/D) ratio was 24.5. The screw profile was com­
posed of right-handed screw (conveying) elements with a
pitch of 11 mm, followed by a block of four kneading discs
with a staggering angle of 90 ° and a total length of 11 mm,
and one left-handed screw element of 5.5 mm (supplemen­
tary material, Fig. S.1a). The design of the experiments was
described as follows (Table 2). For all materials, the flow rate
of powder (QF) was kept constant at 0.24 kg/h, and the die
temperature was regulated at 95 °C to avoid expansion and to
be thus able to process dense composites. The moisture
content (MC) of feed was varied at three levels: 25%, 30%, and
35%. For each value of MC, the rotation speed (N) was
changed at three levels: 120, 300, and 500 rpm. For each N,
the last barrel temperature (Tb) was set at Tm–20, Tm and
Tm+20 °C, where Tm is the melting temperature of the feed.
The setting of operating conditions (MC, N, Tb) led to a wide
interval of measured extrusion variables, which can generate
the composites with a wide range of structural changes. For
further analysis, three representative composites of pea flour
and SP 2/1, extruded at similar three SME levels (≈ 200, 1000,
2000 kJ/g), were selected. Only extrusion trials that generated
the chosen samples were performed in triplicate. For the
selected trials, the reported values of measured SME
(SME_mes), melt temperature (T_mes) and die entrance
pressure (P) were the average values with a standard devia­
tion. These trials were significantly different in terms of ex­
trusion variables at the significance level of 0.05 (Table 2).
The name of selected samples was given in Table 2 and
supplementary material (Table S1). The sample names in­
dicate the SME level (L, M, H) and the formulation (PF: pea
flour, SP 2/1: starch-protein blend).
Expanded snacks (“solid foams”) from pea flour were
processed using a pre-pilot co-rotating twin-screw extruder
(Coperion Werner & Pfleiderer ZSK 26Mc) with a screw dia­
meter of 25.5 mm and a L/D of 29, as formerly indicated by
Kristiawan et al. (2018). All trials were performed using the
same last barrel temperature: Tb = 90 °C. Several die geome­
tries were used: (1) a circular die with a diameter of 3 mm and
a length of 15 mm was directly attached to the extruder die
head; and (2) a multi-step slit die rheometer combined with a
circular die (D = 3 mm, with three length options L: 5, 10,
15 mm) mounted in the extruder die head. The geometry of
the slit die was described elsewhere (Horvat et al., 2013). The
 Food and Bioproducts Processing 135 (2022) 190–204 193

Table 2 – Design of experiments for manufacturing of SP 2/1-based composites.

Trial Operating conditions Extrusion variables Sample

MC (%) N (rpm) Tb Tm (°C) T_mes (°C) SME_mes (kJ/kg) P (MPa) code*

1 35% 500 Tm–20 112 97 978 0.9

2 Tm 99 913 0.6
3 Tm ± 20 104 963 0.6
4 300 Tm–20 100 470 0.3
5 Tm 96 520 0.4
6 Tm ± 20 101 590 0.6
7 120 Tm–20 93 ± 2c 192 ± 13c 1.8 ± 0.3c SP 2/1_L
8 Tm 97 210 2.4
9 Tm ± 20 100 285 1.2
10 30% 500 Tm–20 122 101 1295 1
11 Tm 103 1051 0.5
12 Tm ± 20 111 1198 0.8
13 300 Tm–20 105 628 1.2
14 Tm 105 736 1.4
15 Tm ± 20 108 595 0.6
16 120 Tm–20 103 305 1.8
17 Tm 100 287 3.3
18 Tm ± 20 104 288 2.3
19 25% 500 Tm–20 134 122 ± 5b 1914 ± 284a 2.6 ± 0.2b SP 2/1_H
20 Tm 118 1866 1.1
21 Tm ± 20 124 1561 1.3
22 300 Tm–20 116 953 1
23 Tm 113 933 1.8
24 Tm ± 20 135 ± 5a 990 ± 59b 3.7 ± 0.4a SP 2/1_M
25 120 Tm–20 110 361 1.4
26 Tm 106 790 3
27 Tm ± 20 113 427 3.3

*Selected samples for further analysis. Means with the different superscripts within a column, for the selected samples, are significantly
different (significance level of 0.05).

temperature of the slit die was set at 130 °C and 150 °C, while
the circular one was not regulated. The screw profile was
different from that used for dense composite extrusion:
conveying elements with decreasing pitch followed by three
kneading discs staggered at 45 °, three left-handed screw
elements followed by the last conveying elements (supple­
mentary material, Fig. S.1b).
For both extrusion systems, the raw material was fed by a
gravimetrically controlled feeder and water was added to the
second barrel by a volumetric pump to obtain feed with the
desired moisture contents. Both extruders operated at sev­
eral levels of moisture content MC (18–35% w.b.) and screw
speed (120–700 rpm).
2.3.2. WSI of total solids (WSIsolids)
The extruded products were ground (< 250 µm) and dispersed
in deionized water (30 °C, 30 min), and then centrifuged. The
supernatant was dried overnight in a Chopin oven at 105 °C.
WSIsolids was determined as the percentage of the mass of
supernatant dry solid in the original dry sample.
2.3.3. WSI of starch (WSIstarch)
The ground samples first underwent the same extraction and
centrifugation procedure as described above. Thereafter, the
amount of soluble starch in the supernatant was determined
by titration of the supernatant with orcinol in an automatic
spectrocolorimeter.

2.3.4. Protein solubility

2.3. Extruded product analysis
Protein solubility was determined by triplicate measure­
ments using the method of Kristiawan et al. (2018). The
The experimental database of pea snack features was re­
ground extruded products (< 250 µm) underwent two suc­
trieved from the literature (Kristiawan et al., 2018). Con­
cessive protein extractions. The first step consisted in ex­
cerning pea composite characteristics, the structural
tracting the proteins held by weak interactions (non-covalent
changes of starch and protein were determined in this study,
bonds) in a buffer containing sodium dodecyl sulphate (SDS).
whereas their morphological features were analysed in a
In the second step, the proteins insoluble in SDS were ex­
previous study (Jebalia et al., 2019). The methods used for the
tracted at 60 °C under sonication in a buffer containing an
physical-chemical characterisation were described else­
agent that reduces disulphide (S-S) bonds such as dithioer­
where, so this section recalls them briefly. The data of
ythritol (DTE). Both SDS and DTE extracts were analysed by a
composite features is summarized in Table 3. The reported
high-performance size exclusion chromatography (SE-HPLC)
values were the average values with a standard deviation.
apparatus to determine the molar mass distribution of so­
luble protein aggregates. Protein solubility either in SDS
2.3.1. Water solubility index (WSI) (P_SDS) or DTE (P_DTE) was then expressed as a percentage
The measurements of WSI were carried out in triplicate fol­ of the integrated chromatographic area relative to all ex­
lowing the method of Kristiawan et al. (2018). tractable proteins.
194 Food and Bioproducts Processing 135 (2022) 190–204

Table 3 – Solubility of biopolymers and morphological features of composites samples.

Samples WSIsolids WSIstarch Protein solubility (%) Morphological features*

(%) (%) in SDS in DTE D50 of protein Protein area

aggregates ratio

(µm)
e e a f
Native flour 15.0 ± 0.5 7.50 ± 0.6 92.0 ± 2.7 8.00 ± 0.5
Native PPI 17.5 ± 0.6d 6.00 ± 0.7ef 76.0 ± 1.5c 24.0 ± 0.5c
Native starch 2.00 ± 0.5 g 2.50 ± 0.7 g
PF_L 17.1 ± 0.6d 23.7 ± 1.0b 87.0 ± 1.8b 9.00 ± 0.9f 11.0 ± 1.0c 0.31 ± 0.035a
PF_M 21.0 ± 1.0c 17.3 ± 0.9c 78.0 ± 1.1c 16.4 ± 1.0e 16.5 ± 3.0bc 0.24 ± 0.020ab
PF_H 38.6 ± 1.0a 30.7 ± 1.1a 71.0 ± 2.1d 21.0 ± 0.8d 15.0 ± 2.0bc 0.19 ± 0.020b
SP2/1_L 6.56 ± 0.5 f 4.11 ± 0.6fg 69.0 ± 0.9d 29.0 ± 0.9b 35.0 ± 10a 0.31 ± 0.065a
SP2/1_M 15.4 ± 0.6de 13.8 ± 0.7d 56.0 ± 0.9e 39.0 ± 0.9a 40.0 ± 4.0a 0.24 ± 0.035ab
SP2/1_H 25.8 ± 1.0b 17.9 ± 1.4c 58.0 ± 0.8e 29.0 ± 0.8b 27.0 ± 4.0ab 0.17 ± 0.035b

*Data was retrieved from a previous study (Jebalia et al., 2019). Means with the different superscripts within a column are significantly
different (significance level of 0.05).

The final results of WSIsolids, WSIstarch and protein solu­
bility were presented either as their original value or as the
gain or loss in solubility: ΔWSIsolids, ΔWSIstarch, ΔP_SDS,
ΔP_DTE, computed as the difference between the solubility of
extruded products and that of native material. The untreated
flour and PPI were taken as reference for extruded flour and
SP 2/1, respectively. As shown in Table 3, the properties of
extruded composites were significantly different from those
of native materials (significance level of 0.05).
2.3.5. Starch-protein morphology
The microstructure of pea composites was observed using
confocal laser scanning microscopy (CLSM) and quantified by
image analysis following the method established by Jebalia
et al. (2019).
Specimen slices with a thickness of 20 µm were obtained
by cutting the extruded sample perpendicularly to the ex­
trusion flow using a cryotome at − 20 °C. For protein labelling,
one part (by mass) of 0.01% (weight volume/volume) fuchsine
acid in 1% (volume/volume) acetic acid was mixed with one
part of Kaiser’s glycerol/gelatine solution at 40 °C.
The slices were investigated using a CLSM apparatus
(Nikon A1, Germany) in the epifluorescence mode excited by
a green laser beam at 561 nm. A long-pass filter selected the
emitted light at 570–620 nm. Thereafter, image analysis was
done using Matlab software for at least three plane projec­
tion CLSM images of three spots in the composites. The CLSM
images were digitized to obtain binary images. Each finite
particle in the image was labelled and the following features
were determined: the median protein aggregate size (D50)
and the protein area fraction. The variation of the digitiza­
tion threshold ( ± 10%) induced uncertainty in the particle
area values of about 15%.
2.4. Determination of viscous behaviour
2.4.1. Measurements
Rheological measurements were performed using a pre-
shearing rheometer (Rheoplast®), as described elsewhere
(Vergnes & Villemaire, 1987). It combines the features of a
Couette rotational system and a capillary rheometer. Starch
and protein transformation took place in the Couette cell due
to shearing, imposed by the rotation of a central piston and
the heating by heating collars. The domain of measurement
conditions is moisture content (MC) between 20% and 35%
wet basis, temperature (T) between 85 and 175 °C, and spe­
cific mechanical energy (SME) up to 250 kJ/kg, modulated by
the rotational speed of the central piston (50 or 200 rpm).
The raw materials were mixed with water using a
Kenwood mixer to obtain selected moisture contents. The
mixture was then maintained at 4 °C for 24 h for moisture
equilibration, before measuring the final moisture content.
For each run, about 15 g of raw material were processed in
the Rheoplast®. After the material was pre-sheared in the
Couette cell by piston rotation for 20 s at a controlled tem­
perature (T), the piston was moved downward to push the
molten material through the capillary at decreasing velocity,
so that the apparent shear rate in the capillary varied from
256 to 0.5 s–1. The sample temperature (T) was measured
before the capillary die. The pressure upstream of the ca­
pillary was recorded during measurements for each shear
rate. Capillaries of the same diameter (2 mm) but different
lengths (0.1, 8, 16 and 32 mm) were used. Each pressure
profile was then measured for four L/D ratios (0.05, 4, 8, 16),
with three repetitions leading to a measurement error of up
to 15%.
2.4.2. Data treatment
Data analysis was carried out according to the basic princi­
ples of capillary rheometry, including the Bagley correction.
The apparent shear rate ( app ) was computed from the
displacement speed of the central piston (injection speed) as
follows:
4Q v 4VS
app = = (1)
Ri3 Ri3
where Q v is the volumetric flow rate of the material (mm3/s),
Ri is the radius of the capillary (mm), V is the downward
speed of the piston (mm/s), and S is the cross-section of the
central piston (mm2).
The pressure drop variation against the L/D capillary ratio
was then plotted for each apparent shear rate and fitted by
linear functions (R2 > 0.95) to obtain Bagley plots (supple­
mentary material, Fig. S.2a).
The variation of wall shear stress ( w) against true shear
rate was then plotted (Fig. S.2b). On the basis of knowledge
about Bagley plots, w can be computed as follows:
 Food and Bioproducts Processing 135 (2022) 190–204 195

P exponential functions. C and D are model parameters, and

w =
4(L / D)
In a more approximate approach, disregarding the en­
trance effect, w was computed from the slope of a straight
line passing through the pressure at L / D = 16 and the co­
ordinate origin (0, 0).
The flow behaviour index (dimensionless), n, is then de­
fined by:
d (log w )
n=
d (log app )
The true wall shear rate ( ), for each measurement con­
dition (MC, T) was determined using the Rabinowitch cor­
rection:
3n + 1
= app
4n
The shear viscosity ( ) is then equal to:
w
= (5)
Finally, flow curves expressing shear viscosity=f (true wall
shear rate) were built (Fig. S.2c) and fitted with a power
function (R2 > 0.95), indicating that the viscous behaviour can
be represented by a power law model.
2.4.3. Development of viscosity model
It was checked that the Ostwald-de Waele power-law model
could be used to determine starchy melt viscous behaviour in
shear flow:
=K n 1
where K is the consistency index and n is the flow behaviour
index.
According to Xie et al. (2012), K and n depend on the
temperature (T ) and moisture content (MC):
E 1 1 For all simulations, Nu was set to 20. Other extrusion para­
K = K 0exp (MC MC0 )
R T T0
n = n0 + a1 T + a2 MC + a3 T MC
where T is the melt temperature in K (Eq. 7a) and °C (Eq. 7b); E
is the activation energy (J.mol–1); R is the gas constant
(J.mol–1. K–1); K0 is the consistency (Pa.sn) at the reference
temperature (T0 =80 °C = 353.15 K) and the reference moisture
content (MC0 = 0.1); α is the water plasticization coefficient;
and n0 and ai are the flow index parameters.
The parameters of Eq. 6, K and n can be derived from the
viscosity master curve using time-temperature and time-
plasticizer superposition approaches (Krauklis et al., 2019).
The master curve, which includes both effects of tempera­
ture and moisture content, can be calculated as follows:
= f (aT aMC )
G (8)
(2)
the products of these parameters can result in parameter K0
of Eq. 7a.
2.5. Extrusion simulation
The twin-screw extrusion of pea ingredients was simulated
using Ludovic® software. This simulating software was based
on a 1D global model developed by Della Valle et al. (1993)
(3)
and Vergnes et al. (1998). This model uses an iterative
method to compute the energy balance and the flow rate/
pressure relationship. Both drag flow and pressure-driven
flow are considered, involving a non-Newtonian viscosity
model of melt. Computation of various parameters is carried
out separately for each type of screw element and for the die
(4)
components. The elementary models are linked together to
obtain a global description of the flow field, such as melt
temperature, SME, viscosity, pressure and filling ratio along
the extruder. Melting is assumed to be instantaneous and
takes place before the first restrictive screw element, such as
the left-handed screw element and kneading blocks, in­
dicated by T > Tm. Afterwards, it is assumed that the ma­
terial is fully molten and that it fills the screw channel,
according to local geometry and flow conditions. Since the
final product temperature is unknown and the screws are
starve-fed, the filling ratio of the system is not known. Thus,
the computation starts from the die and proceeds backwards
towards the hopper and follows an iterative procedure.
In addition to a viscosity model, the input data include the
thermal and physical properties of feeds (Choi and Okos,
(6)
1986; Della Valle and Vergnes, 1994; Vergnes et al., 1998), the
heat transfer coefficient between melt and equipment de­
fined using the Nusselt number (Nu), the extruder config­
uration, screw profile and extruder operating conditions
(screw speed, flow rate, barrel and die temperature profile).
(7a)
meters were set according to an experimental extrusion da­
tabase of composites and snacks (Section 2.2).
(7b) The workflow of predicting food features using extrusion
simulation is as follows. First, the calculated extrusion vari­
ables such as melt temperature (T_com) and specific me­
chanical energy (SME_com) are compared to the measured
ones to confirm the validity of extrusion simulation. Then, in
a second step, the measured structural changes of starch and
proteins are linked to the calculated extrusion variables. On
the basis of these relationships, sets of extrusion variables
(T_com, SME_com) and extrusion parameters such as screw
speed, flow rate and barrel temperature profile that lead to
targeted product structure are defined.
2.6. Statistical analysis

E1 The reported values were the average values with a standard

aT = C exp (9)
RT deviation. Some data, such as chemical composition of raw
materials, composites feature, and flow curves of some
aMC = D exp ( MC) (10) melts, were analyzed using one-way analysis of variance
(ANOVA) followed by the least significant difference test
n = n0 = constant (11) (Fisher LSD) at the significance level of 0.05. One-way
where G is the reduced viscosity, and aT and aMC are ANOVA, Fisher LSD, and correlation tests (Pearson and
temperature and moisture content shift factors, respectively. Spearman) between variables (processing and structural
The data of aT =f(1/T ) and aMC =f(MC) can be fitted by changes) were performed by XLSTAT 2022 (Addinsoft,
196 Food and Bioproducts Processing 135 (2022) 190–204

Fig. 1 – Relationship between extrusion variables and operating parameters.

Extrusion experiments to manufacture pea composites were conducted at different moisture contents: 25% (white), 30%
(grey) and 35% (black), using pea flour (square) and SP 2/1 (circle) as raw material. The pea snack data (crosses) were retrieved
from Kristiawan et al. (2018).

(a) Variation of specific mechanical energy (SME_mes) with filling ratio (Q/N);
(b) Variation of melt temperature (T_mes) with SME_mes.
The solid lines represent data fitting:

(a) Composites: SME_mes= 0.69 × (Q/N)–0.97; R2 = 0.80;

Snacks: SME_mes= 133.9 × (Q/N)–0.51; R2 = 0.87;
(b) Composites (pea flour): T_mes= 0.019 ×SME_mes+ 95.25; R2 = 0.64;
Composites (SP2/1): T_mes= 0.011 ×SME_mes+ 98.72; R2 = 0.36;.
Snacks: T_mes= 27.24 ×SME_mes0.26; R2 = 0.76.

France). Pearson stands for linear correlation while
Spearman for monotonic correlation.
3. Results and discussion
3.1. Extrusion experimental results
3.1.1. Variations of extrusion variables with operating
parameters
Combining two extrusion datasets (composites and ex­
panded snacks) led to a wide range of extrusion variables:
measured SME (SME_mes = 150–2000 kJ/kg) and melt tem­
perature at die entrance (T_mes = 95–165 °C) (Fig. 1a,b), which
leads to a large panel of product transformation and struc­
ture changes.
As indicated in Fig. 1a, good correlations were found be­
tween SME_mes and the ratio of total flow rate to screw
speed (filling ratio: Q/N), meaning that SME can be easily
controlled by tuning the filling ratio of the screw. The cor­
relations were distinct for composites and snacks (R2 =
0.8–0.87) due to the differences in extruder screw profiles.
The use of a more restrictive screw profile resulted in a
higher melt temperature (maximum T_mes: 165 °C vs. 135 °C,
snacks vs. composites, Fig. 1b). Acceptable positive correla­
tions between T_mes and SME_mes were found (R2 =
0.64–0.76) for each product, except for SP 2/1 composites,
regardless of the operating conditions and moisture content.
Pearson correlation analysis result supported that T_mes is
strongly and positively correlated with SME_mes (r = 0.78,
significance level = 0.05, supplementary material, Table S2).
Indeed, an increase in moisture content had a negative im­
pact on T_mes and SME_mes. These results indicated that
heating phenomena in extrusion were dominated by solid
friction and melt viscous dissipation rather than conduction
from the barrel, and that they are enhanced when screw
configuration is more restrictive.
3.1.2. Impact of extrusion on starch structural change
WSIsolids are positively and linearly correlated with WSIstarch,
regardless of raw materials, extrusion systems and condi­
tions (supplementary material, Fig. S.3, R2 = 0.81). The values
of WSIsolids are generally higher than those of WSIstarch be­
cause, in addition to starch, WSIsolids considers the solubility
of other components such as fibres that may be solubilised
during extrusion. Concerning protein aggregates resulting
from the cross-linking of proteins, they are not soluble in
water (Stanley, 1989). Consequently, the greater the WSIsolids
is, the greater is its gain (ΔWSIsolids) compared to the solu­
bility of untreated ingredients. Therefore, the larger the
starch macromolecules depolymerised by extrusion will be.
An increase in specific mechanical energy (SME_mes) in­
creased starch solubility in water (Fig. 2a), with a distinct
correlation observed for each extrusion system (snacks and
composites, R2 = 0.86–0.88). Pearson correlation analysis re­
sult supported that SME_mes is very strongly and positively
correlated with ΔWSIsolids, and thus with starch solubility
(r = 0.94, significance level = 0.05, supplementary material,
Table S2). The difference between the trend observed for the
two materials is probably due to the difference in screw
profile, less restrictive for pea composites and more re­
strictive for pea snacks. The gain in starch solubility of pea
snack systems extruded at higher temperatures (120–165 °C)
abruptly increased from 6.5% to 25% in a narrow SME domain
(450–550 kJ/kg) before it levelled at 30%. Conversely, pea
composite systems extruded at lower temperatures
(95–135 °C) required a much larger SME (up to 2000 kJ/kg) to
 Food and Bioproducts Processing 135 (2022) 190–204 197

Fig. 2 – Impact of measured melt temperature or SME on biopolymer solubilities: gain in WSIsolids (a), loss of protein
solubility in SDS (b), and gain in protein solubility in DTE (c). The curves correspond to the data fitting: (a) Snacks: ΔWSIsolids
= 27/(1 + exp(−0.0237 ×(SME_mes − 483))); R2 = 0.86; (b) Composites: ΔWSIsolids = 0.011 ×SME_mes + 1.58; R2 = 0.88; (c)
ΔP_SDS = 278008/(1 + exp(−0.041 ×(T_mes − 373))); R2 = 0.72; (d) ΔP_DTE = 92965/(1 + exp(−0.0358 ×(T_mes − 387))); R2 = 0.76.

achieve the same state of final starch destructuration
(ΔWSIsolid ≈ 25%). Both the heat, generated by viscous dis­
sipation, and shear (mechanical energy), contributed to
starch destructuring mechanisms at low moisture (up to
35%), a common trend for extruded starchy products. The
SME itself took thermal and mechanical energy into account.
The heat induced crystallite melting and internal dis­
organisation of the granular structure, whereas mechanical
energy induced granule fragmentation (Barron et al., 2002; Li
et al., 2014; Xie et al., 2012). Combination of thermal and
mechanical energy increased the breakdown and solubilisa­
tion of starch granules and macromolecules to a greater ex­
tent, including insoluble fibres, and subsequently increased
the amount of water-soluble components.
3.1.3. Impact of extrusion on protein structural change
After extrusion, an increase in loss of protein solubility in
SDS (ΔP_SDS), indicating the degree of non-covalent protein-
protein interactions, occurs concomitantly with the increase
in gain in protein solubility in DTE (ΔP_DTE), regardless of
raw material, extrusion conditions and systems
(Supplementary material, Fig. S.4). The very strong and po­
sitive correlation between ΔP_SDS and ΔP_DTE was also
shown by Pearson correlation test (r = 0.82, significance level
= 0.05, supplementary material, Table S2). The ΔP_DTE re­
flects the quantity of protein cross-linked by S-S bonds. This
result therefore confirmed that the protein insolubilisation is
due to protein cross-linking by covalent bonds. Furthermore,
increasing melt temperature (T_mes) from 95° to 165°C in­
creased ΔP_SDS from 5% to 60% (R2 = 0.72), whereas ΔP_DTE
increased from 1.5% to 40% (R2 = 0.76) (Fig. 2b,c). Spearman
correlation analysis result supported that T_mes is strongly
and positively correlated with ΔP_SDS and ΔP_DTE (r = 0.77
and 0.66, respectively, significance level = 0.05, supplemen­
tary material, Table S3). The loss of protein solubility in SDS
started at 137 °C, while the onset of formation of DTE-soluble
proteins occurred at 130 °C, regardless of raw material and
extrusion systems. As specific mechanical energy (SME)
correlated positively with melt temperature (T) (Fig. 1b), the
same trend was found as in the case of T: SME impacted
ΔP_SDS and ΔP_DTE positively (as also shown by Spearman
correlation matrix, supplementary material, Table S3).
However, the temperature was better correlated to protein
solubility changes than SME: R2 0.76 vs. 0.23 for ΔP_DTE of
composites, and R2 0.76 vs. 0.62 for ΔP_DTE of snacks (results
not shown). This result indicates that heat is a dominant
factor in creating S-S bonds during extrusion.
The mechanisms of protein insolubilisation during ex­
trusion can be drawn from our results and the literature.
Increasing heat and shear during extrusion led to the protein
denaturation and creation of SDS-insoluble protein ag­
gregates via protein cross-linking by covalent bonds. This
trend has been reported for the extrusion of soya, legumes
and glutens (Alonso et al., 2000; Camire, 1991; Laleg et al.,
2016; Pommet et al., 2003; Stanley, 1989). However, heat
seems to play a crucial role in forming S-S bonds. On the
198 Food and Bioproducts Processing 135 (2022) 190–204
Fig. 3 – Variations of composite morphological features with starch and protein solubilities. (a) Change of protein area ratio
with the gain in WSIsolids. The curve stands for data fitting: PAR= –0.01 × ΔWSIsolids + 0.34; R2 = 0.95; (b) Variation of median
size of protein aggregates with protein solubility in DTE. The trend is as follows: D50 = 1.04 × P_DTE – 0.57; R2 = 0.88.
other hand, shear can enhance the unfolding of protein ag­
gregates (Della Valle et al., 1994; Fang et al., 2013), after which
the re-association and re-cross-linking of the protein sub-
units occur under heat.
The combination of solubility data set of pea composites
with the one of “pea snacks”, published in Kristiawan et al.
(2018), extends the interval of experimental domain for ex­
trusion variable and product characteristics. The overlapping
of several data points of starch and protein solubility for
snacks and composites (‘snack’s cell wall’) means that the
selected composites can be a representative of the cell wall.
3.1.4. Impact of biopolymer structural changes on composite
morphology
The pea composites had the morphology of protein ag­
gregates dispersed in a continuous and amorphous starch
matrix, regardless of raw material and moisture content
(supplementary material, Fig. S.5, snapshots of CLSM image),
as described by Jebalia et al. (2019). Depending on SME, the
protein aggregates varied greatly in size (D50 = 10–50 µm) and
protein area ratio (0.15–0.30) and exhibited various shapes
(spherical, ellipsoidal, fibrillar) (see Table 3). At the sig­
nificance level of 0.05, protein aggregates of pea flour-based
composites are significantly smaller than SP 2/1-based
composites (D50 11–16.5 vs 27–40 µm). This difference can be
likely explained by different morphologies of native mate­
rials. Indeed, the native SP blends presented assembled
proteins due to the wet process extraction of PPI (Jebalia
et al., 2019), whereas native PF proteins are distributed
around starch granules according to smaller domains. In
contrast to D50, a significant difference in protein area ratio
(PAR) was observed regarding the SME level of composites
manufacturing. At the same SME level, regardless of raw
material, PAR is similar.
These morphological features were correlated with bio­
polymer structural changes, as shown by their correlation
with ΔWSIsolids and protein solubility in DTE (Fig. 3a,b). The
protein area ratio is negatively and linearly correlated with
the gain in WSIsolids (Fig. 3a, R2 =0.95) and, thus, with starch
destructuration. By favouring the swelling of amorphous
starch, the increase of thermo-mechanical energy (T, SME)
could enlarge the volume (surface area on microscopy
images) of the continuous starch phase to the detriment of
that of dispersed protein aggregates. This result is in
agreement with preceding results showing that SME nega­
tively impacted the protein area ratio (R2 = 0.86) (supple­
mentary material, Fig. S.5) (Jebalia et al., 2019). The median
size protein aggregate (D50) is positively correlated with
protein solubility in DTE (R2 = 0.88, Fig. 3b). The protein cross-
linking by covalent bonds (S-S) can lead to the formation of
large protein aggregates. Pearson correlation analysis result
(supplementary material, Table S2) supported that PAR is
very strongly and negatively correlated with ΔWSIsolids
(r = −0.88); in contrast, D50 is positively correlated with P_DTE
(r = 0.94) at the significance level of 0.05.
This work emphasizes that, for the first time, the mor­
phology of composites (‘snack’s cell wall’) can be modulated
by protein structural changes tuned by the variation of pro­
cessing variables. The previous work (Jebalia et al., 2019) fo­
cussed on the impact of morphological features on
composite mechanical properties but did not really deal with
the relations between extrusion processing and morpholo­
gical features.
3.2. Viscous behaviour
Viscosity of pea flour and SP 2/1 decreased with increasing
shear rate, thus manifesting shear-thinning behaviour. The
flow curves can be fitted by the power-law model (Eq. 6),
regardless of T, MC and SME conditions (Fig. 4 and supple­
mentary material, Fig. S.6). The SME had little impact on the
shear viscosity, even under the lowest temperature and
moisture content (see supplementary material, Fig. S.6).
Statistical analysis, conducted at the significance level of
0.05, proved that at the same shear rate, there is no sig­
nificant difference between the viscosity of SP 2/1 melt is­
sued of different SME (supplementary material, Table S4a,b).
This result may appear as surprising regarding the me­
chanical energy sensitivity on molten starch viscosity (Della
Valle et al., 1996). It can be attributed to the protective effect
exerted by other constituents (fibres, protein aggregates) on
starch. Therefore, the rheological model was built without
taking SME into account.
As shown by the flow curves of pea flour processed with a
moisture content of 35%, a noticeable decrease in viscosity
was observed by increasing the temperature from 105° to
145°C, i.e., Tm, Tm+20, Tm+40 °C (Fig. 4a). Viscosity varied
little when the product was heated from 85° to 105°C (Tm–20,
 Food and Bioproducts Processing 135 (2022) 190–204
Fig. 4 – Flow curves of pea flour. (a) Flow curves at different temperatures at constant MC (35%); (b) Master curves for different
MC at T0 = 105 °C; (c) Comparison of pea flour and SP2/1 master curves at MC0 = 30% and T0 = 105 °C; (d) Comparison with pea
starch flow curves (MC = 30%, T = 115 °C).
Table 4 – Parameters of viscosity model (Eq. 7a, 11).
Coefficients Pea ingredients
Pea flour SP 2/1
K0 (Pa.sn) 8.05E+05 1.39E+06
E/R (K) 4 210 4 237
α 11.4 14.6
n0 0.288 0.292
Tm). This result was also observed for other moisture con­
tents. It can be explained by the competition, in the interval
[Tm–20, Tm °C], between the decrease of the volume fraction
of solid particles (fibre, protein aggregates, residual starch
granules) and the increase of molten starch macromolecules
in the continuous phase.
For each moisture content (21 < MC < 35%, on a wet basis),
a master curve was obtained from flow curves measured at
different temperatures. Here, the viscosities (η) were ex­
pressed as a function of the reduced shear rate (aT× ) using
the time-temperature superposition principle (Krauklis et al.,
2019) in order to more accurately determine the parameters
of the viscosity model. This is illustrated for pea flour by the
master curves built at reference temperature (T0 = 105 °C)
(supplementary material, Fig. S.7a). The changes in shift
factor aT with 1/T can be fitted by an exponential function (R2
≈ 0.75, for pea flour and SP 2/1 (Fig. S.7b), leading to a para­
meter called thermal sensitivity E/R.
199
The curves stand for data fitting using the power function.
The sensitivity of the MC effect (21%, 25%, 30%, and 35%)
was therefore studied at the same reference temperature
(105 °C) for pea flour (Fig. 4b). The moisture content had a
negative effect on the viscosity, as expected, and suggested
that water acts as a plasticizer. By adapting the time-tem­
perature superposition principle to the plasticizer (water)
content, the master curves obtained at four MC values were
shifted to build a final master curve at a reference MC of 30%
(Fig. S7b). The fitting yielded the values of the parameters of
the rheological model: K0 and n. The variation of shift factor
aMC with MC followed exponential functions (R2 = 0.77 and
0.86 for SP 2/1 and pea flour, respectively (Fig. S.7b), allowing
us to determine the water plasticizing coefficient α. The va­
lues of the viscosity model parameters (K0, n, α and E/R) for
pea products are reported in Table 4. Pea flour and SP 2/1 in
the molten state had similar values of thermal sensitivity E/R
(4210 K vs. 4240 K), water sensitivity α (11.4 vs. 14.6), and flow
behaviour index n (0.29), respectively, and their final master
curves were very similar to each other (Fig. 4c). Statistical
analysis, conducted at the significance level of 0.05, proved
that at the same shear rate, there is no significant difference
between the viscosity of pea flour and SP 2/1 melts. (sup­
plementary material, Table S5). This result suggests that the
viscous behaviour of these materials depends little on the
protein and fibre content. To obtain more insight into the
effect of ingredients on the viscous behaviour of pulses, the
flow curves of SP 2/1 and pea flour were compared to those of
200 Food and Bioproducts Processing 135 (2022) 190–204

Fig. 5 – Comparison of extrusion simulation results with measured ones for SME (a) and melt temperature at die entrance (b).
For composites, the melt temperature was studied at three levels of last barrel temperature (Tb): Tm–20 °C (□,○), Tm °C ( , )
and Tm+ 20 °C (■, •), where rectangular and circle symbols stand for pea flour and SP 2/1, respectively. The grey dashed lines
indicate the equity between measured and predicted variables, while the solid lines stand for the linear correlation between
them: (a) SME_com= 0.657 ×SME_mes; R2 = 0.87; (b) Snacks: T_com= 1.031 ×T_mes; R2 = 0.90; Composites (pea flour):
Tb= Tm–20; T_com= 0.57 ×T_mes+ 49.3; R2 = 0.41; TbTm; T_com= 0.79 ×T_mes+ 31.8; ]R2 = 0.92; TbTm+ 20;
T_com= 0.69 ×T_mes+ 50; ]R2 = 0.96. Composites (SP 2/1): Tb= Tm–20; T_com= 1.46 ×T_mes–39.9; R2 = 0.80; TbTm;
T_com= 1.58 ×T_mes–43.4; ]R2 = 0.92; TbTm+ 20; T_com= 1.27 ×T_mes–7.23; ]R2 = 0.99.

pea starch found in the literature (Barron et al., 2002; Logié,
2017). Pea starch viscosity, measured using the same rhe­
ometer (Rheoplast®) at similar conditions (MC = 30%,
T = 115 °C, SME < 250 kJ/kg), is only slightly higher than that of
pea flour and SP 2/1 (Fig. 4d). Statistical analysis, conducted
at the significance level of 0.05, proved that there is no sig­
nificant difference between the viscosity of pea starch, pea
flour, and SP 2/1 melts at a shear rate higher than 95 1/s
(supplementary material, Table S5). These results are in
agreement with the finding of Chanvrier et al. (2015),
showing that molten maize flour, starch/zein blend (85/15%)
and maize starch exhibited shear viscosities very similar to
each other. However, the pea starch processed at higher SME
(1000 kJ/kg) exhibited lower viscosity than pea ingredients
processed at lower SME (< 250 kJ/kg) (Fig. 4d). For the whole
shear rate, the viscosity of this ultra-processed pea starch is
significantly different from other materials at the sig­
nificance level of 0.05 (supplementary material, Table S5).
Higher starch depolymerisation can lower system viscosity
(Della Valle et al., 1996).
In conclusion, regardless of the minor fractions (lipids,
proteins, fibre), the shear viscosity of pulses and their bio­
polymer blends in the molten state is governed by the be­
haviour of the starch phase and its transformation.
3.3. Extrusion simulation
First, the predicted extrusion variables were compared with
values measured during experiments. A good and unique
correlation between predicted and measured SME was ob­
tained (R2 = 0.87), regardless of extrusion system, formula­
tion and operating conditions, although the computed SME
was slightly underestimated (Fig. 5a). This slight difference is
probably because the Ludovic® flow model only considers the
melting and viscous dissipation energies, and neglects fric­
tion (inter-particle, particle-metal, metal-metal).
For most simulations of composite extrusion, the predicted
temperature at die entrance correlates well with the mea­
sured temperature, regardless of moisture content for each
material and each barrel temperature (Tb) (R2 > 0.80, except
for pea flour at Tb = Tm–20 °C) (Fig. 5b). For snack extrusion
simulation, a good agreement between the computed and
measured melt temperature was found regardless of extru­
sion conditions and die geometry (R2 = 0.90, Fig. 5b). Contrary
to composites, the snack extrusion simulations revealed a
unique correlation between T_com and T_mes because all
trials were performed using the same barrel temperature
(Tb). The predicted temperature, in most cases, is slightly
overestimated, which may be partly due to the inaccuracy of
the measurements. Indeed, using a temperature sensor
flush-mounted at the wall of the die entrance may result in a
temperature that is different from the actual temperature in
the product core. The results for the legume case confirm the
proven capacity of a 1D global extrusion model (Ludovic®) to
simulate extrusion processing of starchy products (Berzin
et al., 2010; Della Valle et al., 1993; Robin et al., 2010).
The variations in structural changes of biopolymers were
then correlated with the melt temperature and SME. They
were calculated using the extrusion model (Fig. 6), in agree­
ment with experimental results (Fig. 2). Regarding starch
transformation, an acceptable correlation was obtained be­
tween the gain in the water solubility index of solids
(ΔWSIsolids) and the predicted SME: R2 = 0.77 and 0.82, for
composites and snacks, respectively (Fig. 6a). Similar to ex­
perimental results, ΔWSIsolids was better correlated to pre­
dicted SME than predicted temperature (results not shown).
It should be kept in mind that the intensity of starch de­
structuration, assessed by WSIstarch can be deduced from
WSIsolids through the strong correlation between them (sup­
plementary material, Fig. S.3).
Concerning protein transformation, the gain in DTE-so­
luble proteins (ΔP_DTE) was positively correlated with the
 Food and Bioproducts Processing 135 (2022) 190–204 201

Fig. 6 – Variations of structural characteristics of starch: ΔWSIsolids (a) and proteins: ΔP_DTE (b), with computed temperature
and SME. The curves correspond to the data fitting: (a) Pea snacks: ΔWSIsolids = 27/(1 + exp(−0.0359 ×(SME_com − 294))); R2
= 0.82; Pea composites: ΔWSIsolids = 0.015 ×SME_com+ 2.53; R2 = 0.77. (b) ΔP_DTE = 101/(1 + exp(−0.0373 × (T_com − 194)));
R2 = 0.81.

Fig. 7 – 2D contour plots of extruder operating chart. Study case: Manufacturing of pea snacks using a Coperion Werner &
Pfleiderer ZSK 26Mc extruder equipped with a circular die. Pea flour was extruded at MC = 21% and Q = 20 kg/h. The hatched
area indicates the range of extrusion conditions (N, Tb) leading to predicted melt temperature (155 < T_com < 162.5 °C) and
specific mechanical energy (425 < SME_com < 625 kJ/kg) in order to achieve the goals: ΔP_DTE= 20 ± 5% and ΔWSIsolids
= 27.5 ± 2.5%.

computed temperature (R2 = 0.81, Fig. 6b), in accordance with predicted by temperature than SME (result not shown).
the experimental results. Indeed, ΔP_DTE, indicating the Hence, extrusion can be simulated for predicting extruded
amount of protein cross-linked by S-S bonds, was better product structure from the knowledge of extrusion variables.
202 Food and Bioproducts Processing 135 (2022) 190–204
In the last step, a sensitivity study of the effects of ex­
trusion conditions (screw speed, flow rate, barrel tempera­
ture) on predicted processing variables was conducted
through extrusion simulation. As an example of a study case,
pea flour was processed using a pre-pilot extruder equipped
with a circular die at MC = 21% and Q = 20 kg/h. It resulted in
2D contour plots, expressing computed extrusion variables,
i.e., melt temperature at die entrance T_com and specific
mechanical energy SME_com, as a function of two extrusion
operating parameters (i.e., screw speed N and last barrel
temperature Tb). The product temperature at die entrance
(T_com) increased from 130° to 178°C and SME_com from 448
to 624 kJ/kg when barrel temperature and screw speed in­
creased from 90° to 145°C and 200–700 rpm, respectively. The
higher value of T_com compared to Tb was indicative of the
importance of viscous dissipation (Fig. 7). As an example of
these plot applications, let us consider the manufacturing of
expanded pea snacks with the following characteristics:
maximum ΔWSIsolids (27.5 ± 2.5%) and an average gain in
protein solubility in DTE = 20 ± 5%. Note that, in turn, this
gain in protein solubility in DTE can lead to a composite (cell
wall) with a morphology characterised by an average of D50
of protein aggregates of ≈ 20 µm (Fig. 3b). On the basis of the
correlations between extrusion variables (T_com, SME_com)
and transformation (Fig. 6), it follows that this product can be
obtained by processing pea flour at T_com = 155–162.5 °C and
SME_com = 425–625 kJ/kg. The hatched area in Fig. 7 gives the
particular combinations of N and Tb leading to desired melt
temperature and SME. The same rationale can be applied to
other extrusion parameters (MC, Q) to deliver a complete set
of operating conditions.
Using the present extrusion database with an appropriate
viscosity model of the feeds, the extrusion simulation can
help us to predict the transformation of biopolymers and the
structure of extruded foods.
4. Conclusions
This study has shown that rheology and process simulation
could help to design pulse-based extruded foods. The struc­
tural changes in pea biopolymers, e.g., starch depolymer­
isation and protein aggregation that occur during the
extrusion process, were assessed by solubility indices. These
changes govern the morphological features of pea-based
starch-protein composites, such as protein area ratio and
median width of protein aggregates. These results suggest
that thermal and shear energies work synergistically to
perform starch transformation, whereas thermal energy
probably controls protein cross-linking by forming S-S bonds.
These structural changes can therefore be tuned by the
proper setting of extrusion variables such as melt tempera­
ture (T) and SME. These extrusion variables can be predicted
by a 1D global model of co-rotating twin-screw extrusion
implemented in simulation software (Ludovic®). One of the
model inputs, the viscous behaviour of pea flour and starch/
protein blend, was determined using a capillary pre-shearing
rheometer under conditions similar to extrusion. The visc­
osity of the molten hydrated protein-starch blend and pea
flour was governed by the starch viscosity, regardless of the
minority fraction (proteins, fibres) present. The extrusion
simulations allowed a fair prediction of extrusion variables (T
and SME) from extrusion parameters (feed rate, screw speed,
barrel temperature). This study reveals how extrusion si­
mulation empowered with a rheological model can be used
as a tool in designing extruded foods with targeted struc­
tures, and opens the way for the prediction of the structural
features of extruded pulse crops. In the future, a mechanistic
model for predicting the variation of melt microstructure
along the extruder screw and die will be established through
an in-depth study of the local interfacial stress and local
structural changes of starch and proteins along the screws
and die. Complete characterisations of extruded products
issued of dead-stop operation will be performed. Further
improvements involve determining the cellular structure of
expanded snacks from the knowledge of morphology, rheo­
logical behaviour and extrusion variables to predict their
texture.
Declaration of Competing Interest
The authors declare that they have no known competing fi­
nancial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgements
We are thankful to Joëlle Bonicel and Valérie Micard (INRAE-
IATE) for protein SE-HPLC analysis and protein solubility
determination, and to Mathieu Bretesche (INAE-BIA) for
rheological measurements. We are grateful to Azad Emin
(KIT) for pea snack extrusion, and to the Pays de La Loire
Region (France) for financially supporting Imen Jebalia’s PhD
thesis.
Appendix A. Supporting information
Supplementary data associated with this article can be found
in the online version at doi:10.1016/j.fbp.2022.08.001.
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