Journal of Food Engineering 78 (2007) 855–860

www.elsevier.com/locate/jfoodeng

Tensile properties of compression-molded whey protein

sheets: Determination of molding condition and glycerol-content
effects and comparison with solution-cast films
a,*
R. Sothornvit , C.W. Olsen b, T.H. McHugh b, J.M. Krochta c,1

a
Faculty of Engineering at Kamphaengsaen, Department of Food Engineering, Kasetsart University, Kamphaengsaen, Nakhonpathom 73140, Thailand
b
USDA, Agricultural Research Service, Western Regional Research Center, 800 Buchanan Street, Albany, CA 94710, United States
c
Department of Biological and Agricultural Engineering, Department of Food Science and Technology, University of California,
Davis, CA 95616, United States

Received 3 November 2004; received in revised form 27 October 2005; accepted 1 December 2005
Available online 19 January 2006

Abstract

Transparent glycerol (Gly)-plasticized whey protein isolate (WPI) sheets could be formed from Gly-WPI mixtures using compression
molding, demonstrating that such mixtures display flowability and fusion behavior under certain conditions. The effects of glycerol con-
tent (GC), molding temperature and molding pressure on the tensile properties of the transparent compression-molded WPI sheets were
studied, and the properties were compared to those of films produced using the solution-casting method. Compression-molding temper-
ature and pressure did not significantly affect sheet stiffness (elastic modulus, EM), strength (tensile strength, TS) or extension (% elon-
gation, %E) (p > 0.05). Increasing the GC of compression-molded sheets decreased EM and TS, but had little effect on %E. The values of
TS and %E of compression-molded WPI sheets with 40–50% GC were greater than those of solution-cast WPI films with 45% GC. These
results indicate the possibility that Gly-WPI mixtures can be extruded into films for formation of edible or biodegradable wraps or heat-
sealed pouches.
 2005 Elsevier Ltd. All rights reserved.

Keywords: Compression molding; Edible films; Whey protein; Glycerol; Tensile properties

1. Introduction vapor permeability (WVP) and solubility results have been

Extrusion is an attractive alternative method for protein
or polysaccharide film formation, because it speeds pro-
cessing and requires less space compared to the traditional
solution-casting method. Generally, compression molding
of sheets is studied as a precursor to extrusion, in order
to demonstrate material flowability and fusion and identify
conditions suitable for extrusion. Production of Glycerol
(Gly)-plasticized whey protein isolate (WPI) sheets by com-
pression molding has been demonstrated and the water
*
Corresponding author. Tel.: +66 19249381; fax: +66 34351404.
E-mail addresses: fengrns@ku.ac.th (R. Sothornvit), jmkrochta@
ucdavis.edu (J.M. Krochta).
1
Tel.: +1 530 752 2164; fax: +1 530 752 4759.
reported (Sothornvit, Olsen, McHugh, & Krochta, 2002).
These Gly-plasticized WPI compression-molded sheets
show promise, but they require further evaluation, includ-
ing testing of tensile properties. Such tensile properties are
important, because they reflect film strength, flexibility,
elongation (stretchability) and toughness (film
strength · elongation at break) when serving as a food
wrap or pouch.
Tensile properties of compression-molded and extruded
soy protein based sheets and films have been investigated
(Cunningham, Ogale, Dawson, & Acton, 2000; Foulk &
Bunn, 2001; Jane & Wang, 1994; Schilling, Babcock,
Wang, & Jane, 1995; Wu & Zhang, 2001; Zhang, Mungara,
& Jane, 2001). However, the tensile properties of compres-
sion-molded WPI sheets have not been reported. We

0260-8774/$ - see front matter  2005 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jfoodeng.2005.12.002
856 R. Sothornvit et al. / Journal of Food Engineering 78 (2007) 855–860
hypothesized that both the WPI-Gly mixture composition
and the compression molding conditions would affect
resulting molded sheet tensile properties.
The objective of this study was to investigate the effects
of glycerol content (GC), molding temperature and mold-
ing pressure on tensile properties of compression-molded
sheets (i.e., transparent films >0.1 mm). We also compared
the tensile properties of the compression-molded sheets
obtained to published tensile properties of solution-cast
WPI films, as well as compression-molded and extruded
soy protein sheets and films.
2. Materials and methods
2.1. Materials
BiPro WPI (97.7% protein dry basis (db)) supplied
by Davisco Foods International (Le Sueur, MN, USA)
was used. Gly was purchased from Starwest-Botanicals
(Rancho Cordova, CA, USA) and used as a plasticizer.
A saturated salt solution of magnesium nitrate from Fisher
Scientific Inc. (Fair Lawn, NJ, USA) was used to equili-
brate films at 50 ± 5% RH in an environmental chamber
prior to thickness measurement and tensile testing.
2.2. Sheet formation
Mixtures of WPI powder and Gly (30%, 40% and 50%
of the total combined weight of WPI powder and Gly) were
thoroughly blended in a Kitchen Aid mixer (St. Joseph,
MI, USA) at room temperature (RT) and low speed for
10, 20 and 30 min, respectively. Blended Gly-WPI mixtures
were stored in a polyethylene bag at 5 C overnight to
equilibrate all components. Samples of 10–15 g were placed
between two 12 · 12 in stainless steel plates preheated to
the temperature studied. The plates were then inserted into
the compression compartment of a Carver Press Machine
(Carver Inc., Wabash, IN, USA), model 2518 with 25 ton
capacity and equipped with heated platens.
From our previous study (Sothornvit et al., 2002), the
feasible temperature range for compression molding of
Gly-WPI sheets was determined to be 104–140 C. A min-
imum temperature of 104 C was necessary for sheet for-
mation. Above 140 C, sheet formation could not be
achieved without degradation at both the minimum
(0.81 MPa) and maximum (2.25 MPa) pressures studied.
Thus, for the study of tensile properties in the present
study, the compression temperature range selected for
sheet formation was 113–140 C. The compression-mold-
ing time selected for the present study was 2 min, since
earlier results showed that at less than 2 min no continu-
ous, transparent sheet was formed and at more than
2 min film degradation was found at high temperature.
The Carver Press was used in the programmable mode.
A hydraulic pump compressed the sample for 2 min
between the stainless steel plates at 113, 127 or
140 ± 5 C, with pressures of 0.81 or 2.25 MPa at each
temperature for each sheet formulation. Sheets were
formed and then removed from the press. Since the sheets
tended to curl upon cooling, they were held between the
metal plates to keep them flat. The tensile properties were
determined from three sheet-formation replications that
were each cut further into 2–4 pieces for testing (described
later).
2.3. Sheet thickness
Sheet thickness was measured, after equilibration at
23 ± 2 C and 50% RH for at least 48 h, with a micrometer
(No. 7326, Mitutoyo Manufacturing Co., Ltd., Tokyo,
Japan) to the nearest 0.0001 in (0.00254 mm) at four ran-
dom positions within the test piece area of 100 mm2. An
average of the four values of thickness was used to deter-
mine tensile properties for each sheet replicate. The average
thicknesses of sheets with 30%, 40% and 50% GC were
1.32 ± 0.27, 0.92 ± 0.21 and 0.57 ± 0.1 mm, respectively.
2.4. Tensile tests
An Instron Universal Testing Machine (Model 5500R-
1122, Instron Corp., Canton, MA) with IX Series (Version
8.09.00) and Merlin Software (Version 4.06) was used to
determine tensile strength (TS), elastic modulus (EM or
Young’s modulus) and % elongation (%E) according to
the ASTM standard method D882 (ASTM, 2002). Maxi-
mum TS is the largest stress (force/area) that a film or sheet
is able to sustain before break. EM, calculated from the
slope of the initial linear region of the force–deformation
curve, reflects stiffness (Steffe, 1996). The %E is the maxi-
mum % change in length before breaking.
2.4.1. Preconditioning
The sheets were preconditioned in a chamber at 100%
RH for 15–20 min to facilitate cutting. A striking die was
used to cut the sheets (The Right Image, Sacramento,
CA). The cut shape looked like a dog bone with a rectan-
gular center, 8 mm wide by 50 mm long, flaring to
12.50 mm by 17.50 mm grip area on both ends. Cut sheets
were then equilibrated at 23 ± 2 C and 50 ± 5% RH in an
airtight cabinet containing saturated magnesium nitrate
solution for at least 48 h prior to tensile testing.
2.4.2. Tensile test conditions
The Instron Universal Testing Machine was operated
with a 500 kg load cell and with self-alignment grips
(Model 2712-002, Instron Corp., Canton, MA) in a room
controlled to 23 ± 2 C and 50 ± 5% RH. Self-alignment
grips consist of one fixed end and one movable end to pro-
vide perfect alignment when load is applied. The grips are
lined with thin rubber faces to prevent sample slippage and
they are air-actuated to prevent sample breakage. The ini-
tial gauge separation was fixed at 58 mm and crosshead
speeds were 2.54 mm/min for 30% GC Gly-WPI sheets
and 50 mm/min for 40–50% GC Gly-WPI sheets.
 R. Sothornvit et al. / Journal of Food Engineering 78 (2007) 855–860 857

2.5. Statistical analyses 50% GC, 127 oC, 2.25 MPa

0.06 50% GC, 140 oC, 2.25 MPa
A split plot experimental design was used to study the

Load at peak (kN)

following factors: (1) 3 levels of molding temperature; (2) 0.04
2 levels of molding pressure and (3) interactions between
temperature and pressure or temperature and GC or pres-
sure and GC. Temperature factor was the main plot, with 0.02
pressure and GC factors as subplots arranged in a com-
pletely randomized design. SAS system software program, 0
release 6.12 (SAS, 1996) was used to calculate analysis 0 20 40 60 80
of variance (ANOVA) using the TEST statement in the % strain
General Linear Models Procedure PROC GLM, and a
Fig. 1. Typical load–% strain curves for compression-molded sheets at
Duncan’s multiple range test was used to determine the
50% GC, 127 or 140 C and 2.25 MPa.
significant treatments at a 95% confidence interval.

3. Results and discussion

350
3.1. Sheet formation
0.81 MPa

Elastic modulus (MPa)

300
2.25 MPa
The 30% GC Gly-WPI mixture used for compression 250
molding had fine granular consistency, the 40% GC Gly-
200
WPI mixture had larger particle size, and the 50% GC
Gly-WPI mixture was a homogeneous viscous mass. 150

Increasing GC enhanced the flowability of Gly-WPI mix- 100

tures and flexibility of molded sheets. A minimum formula
50
concentration of 30% GC was required to produce contin-
uous, transparent compression-molded sheets. At lower 0
113 127 140
GC, the sheets were too brittle to handle and test. Over (A) Molding temperature (o C)
the 30–50% GC range studied, transparent flexible sheets
were formed, indicating that the molding temperatures 200
113 C, 0.81 MPa
and pressures used induced flowability and fusion of the 180
113 C, 2.25 MPa
Gly-WPI mixtures. 160 127 C, 0.81 MPa
Elastic modulus (MPa)

140 127 C, 2.25 MPa

3.2. Tensile properties 140 C, 0.81 MPa
120
140 C, 2.25 MPa
Tensile properties of sheets with 30% GC could not be 100

measured at the desired crosshead speed (50 mm/min), 80

because these sheets were quite strong and slipped out of
the grips. Therefore, the crosshead speed was reduced to
2.54 mm/min for these 30% GC Gly-WPI sheets. Since
tensile properties depend on several factors, including
crosshead speed, sample size and % RH, the 30% GC
Gly-WPI sheets could not be directly compared to the
40% and 50% GC Gly-WPI sheets. Thus, data from the
30% GC Gly-WPI sheets were not included in the statistical
analysis.
Typical load–% strain curves for compression-molded
WPI sheets are shown in Fig. 1. All 50% GC Gly-WPI
sheets at both 127 and 140 C showed flexibility and elon-
gation greater than 30% GC Gly-WPI sheets.
Molding temperature and pressure did not significantly
affect tensile properties (p > 0.05) (Figs. 2–4). However,
GC had a significant effect on sheet TS and EM
(p 6 0.05). Comparing the data for the 40% and 50% GC
Gly-WPI sheets reveals that increasing GC decreased TS
and EM. Furthermore, the 40% and 50% GC Gly-WPI
sheets had lower TS and EM compared to the 30% GC
60
40
20
0
40 50
(B) % Glycerol
Fig. 2. Effect of molding temperature and pressure and film formulation
glycerol content (GC) on Elastic Modulus (EM) of compression-molded
WPI sheets. Error bar shows standard deviation. Fig. 2A is for 30% GC
sheet tested with 2.54 mm/min crosshead speed. Fig. 2B is for 40% and
50% GC sheets tested at 50 mm/min crosshead speed.
Gly-WPI sheets. Since Gly is a plasticizer, it reduces inter-
actions between protein chains, thereby reducing film or
sheet brittleness and increasing flexibility (i.e., reducing
the EM). The effect of a plasticizer also generally includes
reducing strength, as result also seen in the data. However,
comparing data from 40% and 50% GC Gly-WPI sheets
shows that elongation (%E) was not significantly affected
by GC for these formulations (p > 0.05). But, the 40%
858 R. Sothornvit et al. / Journal of Food Engineering 78 (2007) 855–860

12 80
0.81 MPa 0.81 MPa
2.25 MPa 70 2.25 MPa
10
Tensile strength (MPa)

60

% Elongation
8 50
40
6
30

4 20
10
2 0
113 127 140
0 (A) o
Molding temperature ( C)
113 127 140
(A) o
Molding temperature ( C) 113 C, 0.81 MPa
113 C, 2.25 MPa
12 113 C, 0.81 MPa
127 C, 0.81 MPa
113 C, 2.25 MPa
127 C, 2.25 MPa
10 127 C, 0.81 MPa 140 140 C, 0.81 MPa
127 C, 2.25 MPa
Tensile Strength (MPa)

140 C, 2.25 MPa

140 C, 0.81 MPa 120
8
140 C, 2.25 MPa
100

% Elongation
6
80

4 60

40
2
20
0
40 50 0
(B) % Glycerol 40 50
(B) % Glycerol
Fig. 3. Effects of molding temperature and pressure and film formulation Fig. 4. Effects of molding temperature and pressure and film formulation
glycerol content (GC) on Tensile Strength (TS) of compression-molded glycerol content (GC) on Elongation (%E) of compression-molded WPI
WPI sheets. Error bar shows standard deviation. Fig. 3A is for 30% GC sheets. Error bar shows standard deviation. Fig. 4A is for 30% GC sheet
sheet tested with 2.54 mm/min crosshead speed. Fig. 3B is for 40% and tested with 2.54 mm/min crosshead speed. Fig. 4B is for 40% and 50% GC
50% GC sheets tested at 50 mm/min crosshead speed. sheets tested at 50 mm/min crosshead speed.

and 50% GC Gly-WPI sheets had greater %E than the 30% greater cross-linking of protein chains within the protein
GC Gly-WPI sheets. structure resulting from the high heat and pressure applied
Molding temperature and pressure were expected to during the molding process, compared to the heat denatur-
affect tensile properties, since high temperature improves ing that is used before solution casting of WPI films.
matrix flowability and strengthens protein chain networks Increase in TS was also found for heat-cured solution-cast
(Paetau, Chen, & Jane, 1994). However, there was only a
slight, insignificant increase in EM and TS as molding tem-
perature increased, and the %E was not affected by the
Table 1
increase in molding temperature and pressure. These Tensile properties of WPI sheets produced from compression-molding and
results suggest that the protein chain network strength WPI films made from solution casting
was not significantly changed over the range of molding Method % Gly Tensile properties
conditions studied.
EM (MPa) TS (MPa) %E
Compression moldinga 30c 251 ± 18 10 ± 0.3 43 ± 15
3.3. Comparison of compression molding and solution
Compression moldinga 40 144 ± 26 8 ± 0.7 85 ± 15
casting Compression moldinga 50 60 ± 5 4 ± 0.5 94 ± 17
Solution castingb 25 407 ± 51 10 ± 0.9 39 ± 15
In contrast to compression-molded sheets, solution-cast Solution castingb 30 264 ± 24 7 ± 0.3 61 ± 7
films are made from drying aqueous solutions of the WPI Solution castingb 35 144 ± 18 4.4 ± 0.4 74 ± 19
Solution castingb 45 106 ± 18 3 ± 0.4 45 ± 12
and Gly. Average EM of compression-molded WPI sheets
Solution castingb 55 26 ± 3 1.4 ± 0.2 68 ± 18
with 40–50% GC made in this study was similar to EM of a
Data from 140 C molding temperature, averaged from three
solution-cast WPI films with 45% GC reported in the liter-
replications.
ature (Table 1). However, TS of compression-molded WPI b
From Sothornvit and Krochta (2000).
sheets with 40–50% GC was greater than that of solution- c
Crosshead speed at 2.54 mm/min, otherwise crosshead speed at
cast WPI films with 45% GC. This might be attributed to 50 mm/min.
 R. Sothornvit et al. / Journal of Food Engineering 78 (2007) 855–860 859

soy protein and whey protein films compared to non-cured The compression-molded 40% GC Gly-WPI sheets had
films, also likely due to increased protein chain crosslinking similar TS but lower %E compared to low density polyeth-
(Gennadios, Ghorpade, Weller, & Hanna, 1996; Miller, ylene (LDPE) films (Table 2). Thus, extruded films made
Chiang, & Krochta, 1997). from synthetic polymer such as LDPE are tougher than
The ability of compression-molded 40–50% GC Gly- protein and starch films and sheets. However, the tensile
WPI sheets to stretch (%E) was also greater than that of properties of Gly- WPI films and sheets appear to be suffi-
heat-denatured solution-cast 45% GC Gly-WPI films. cient to allow uses such as food wraps and pouches.
These results are consistent with the greater %E found by
Perez-Gago and Krochta (1999) with heat-denatured,
4. Conclusion
crosslinked protein films compared to uncrosslinked native
films. Thus, we hypothesized that the potentially even
Gly content was the only factor to significantly affect
greater crosslinking in the compression-molded sheets
tensile properties of compression-molded WPI sheets over
may have resulted in the greater %E. However, these
the range of molding temperature and pressure conditions
results contrast with those from heat-cured solution-cast
investigated in this study. Increasing GC reduced TS and
soy protein and whey protein films, where heating reduced
EM of the molded sheets. TS and %E values for compres-
%E (Gennadios et al., 1996; Miller et al., 1997). This differ-
sion-molded Gly-WPI sheets were greater than those for
ence might be due to the different protein structures result-
solution-cast films with comparable composition, but EM
ing from the different treatment conditions.
values were similar. TS and %E of the compression-molded
40% GC Gly-WPI sheets investigated in this study were
3.4. Comparison among compression-molded protein and
greater and similar, respectively, compared to TS and %E
starch sheets
of compression-molded 40% GC Gly-soy protein sheets
and acetylated soy protein sheets. The TS and %E of the
Compression-molded 40% GC Gly-WPI sheets had
40% GC Gly-WPI sheets were smaller and greater, respec-
greater TS and similar %E compared to values obtained
tively, compared to compression-molded unplasticized soy
with compression-molded 40% GC Gly-soy protein sheets
protein and starch sheets, which were stiffer (higher EM)
(Cunningham et al., 2000) and acetylated soy protein sheets
and stronger (higher TS) but much less stretchy (lower
(Foulk & Bunn, 2001) (Table 2). Compared to compres-
%E). Overall, the GC-plasticized sheets appear to be some-
sion-molded soybean-water sheets without added plasti-
what tougher than compression-molded soy protein and
cizer (Paetau et al., 1994), the compression-molded 40%
potato starch sheets. The results of this study for compres-
GC Gly-WPI sheets had lower TS but much higher %E.
sion-molded sheets indicate that Gly-WPI mixtures can be
Thus, since toughness is related to the product of TS and
extruded into films for formation of edible or biodegrad-
%E, the 40% GC Gly-WPI sheets made in this study had
able wraps or pouches that have useful tensile properties
toughness greater than the glycerol-plasticized, acetylated
for food products.
or unplasticized soy protein sheets in Table 2. Interestingly,
the 40% GC Gly-WPI sheets also had lower TS but much
higher %E compared to compression-molded potato starch References
sheets (van Soest & Kortleve, 1999), again indicating
greater toughness. ASTM (2002). Standard test method for tensile properties of thin plastic
sheeting. Designation D882-01. In Annual book of ASTM standards.
Philadelphia, PA: American Society for Testing and Materials.
Table 2 Briston, J. H. (1986). Films, plastic. In M. Bakker (Ed.), The Wiley
Comparison of tensile properties of compression-molded protein and encyclopedia of packaging technology (pp. 329–335). New York: John
starch sheets Wiley & Sons, Inc..
Cunningham, P., Ogale, A. A., Dawson, P. L., & Acton, J. C. (2000).
Type of Formation method Tensile properties Tensile properties of soy protein isolate films produced by a thermal
material compaction technique. Journal of Food Science, 65(4), 668–671.
EM (MPa) TS (MPa) %E
Foulk, J. A., & Bunn, J. M. (2001). Properties of compression-molded,
40% Gly-WPI Compression molding 144 8 85
acetylated soy protein films. Industrial Crops and Products, 14(1),
40% Gly-soy Compression molding – 2.6 74.5
11–22.
proteina
Gennadios, A., Ghorpade, V. M., Weller, C. L., & Hanna, M. A. (1996).
Acetylated soy Compression molding – 2.3 105
Heat curing of soy protein films. Transactions of the American Society
proteinb
of Agricultural Engineers, 39(2), 575–579.
Soybean-waterc Compression molding 1250 36 5
Jane, J-L., Wang, S., & Iowa State University Research Foundation, Inc.,
100% Potato Compression molding 90 29 5
assignee. (1994). Soy protein-based thermoplastic composition for
starchd
preparing molded articles. U.S. patent 5,523,293.
LDPEe Extrusion – 8.6–17 500
Miller, K. S., Chiang, M. T., & Krochta, J. M. (1997). Heat curing of
a
Cunningham et al. (2000). whey protein films. Journal of Food Science, 62(6), 1189–1193.
b
Foulk and Bunn (2001). Paetau, I., Chen, C. Z., & Jane, J. L. (1994). Biodegradable plastic made
c
Paetau et al. (1994). from soybean products I: effect of preparation and processing on
d
van Soest and Kortleve (1999). mechanical properties and water absorption. Industrial & Engineering
e
Briston (1986). Chemistry Research, 33(7), 1821–1827.
860 R. Sothornvit et al. / Journal of Food Engineering 78 (2007) 855–860
Perez-Gago, M. B., & Krochta, J. M. (1999). Water vapor permeability,
solubility and tensile properties of heat-denatured versus native whey
protein films. Journal of Food Science, 64(6), 1034–1037.
SAS Institute Inc. (1996) (4th ed.). SAS/STAT Users Guide, Version 6.12
(Vol. 2). Cary, NC: SAS Institute, Inc..
Schilling, C. H., Babcock, T., Wang, S., & Jane, J. (1995). Mechanical
properties of biodegradable soy-protein plastics. Journal of Materials
Research, 10(9), 2197–2202.
Sothornvit, R., & Krochta, J. M. (2000). Oxygen permeability and
mechanical properties of films from hydrolyzed whey protein. Journal
of Agricultural and Food Chemistry, 48(9), 3913–3916.
Sothornvit, R., Olsen, C. W., McHugh, T. H., & Krochta, J. M. (2002).
Formation conditions, water-vapor permeability, and solubility of
compression-molded whey protein films. Journal of Food Science,
68(6), 1985–1989.
Steffe, J. F. (1996). Rheological methods in food process engineering.
Michigan: Freeman Press.
van Soest, J. J. G., & Kortleve, P. M. (1999). The influence of
maltodextrins on the structure and properties of compression-molded
starch plastic sheets. Journal of Applied Polymer Science, 74(9),
2207–2219.
Wu, Q. X., & Zhang, L. N. (2001). Properties and structure of soy protein
isolate-ethylene glycol sheets obtained by compression molding.
Industrial & Engineering Chemistry Research, 40(8), 1879–1883.
Zhang, J., Mungara, P., & Jane, J. (2001). Mechanical and thermal
properties of extruded soy protein sheets. Polymer, 42(6), 2569–2578.