Industrial Crops & Products 144 (2020) 112061

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Industrial Crops & Products

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

Blends of PBAT with plasticized starch for packaging applications: T

Mechanical properties, rheological behaviour and biodegradability
Mohamed Dammaka, Yesmine Fouratia, Quim Tarrésb, Marc Delgado-Aguilarb, Peré Mutjéb,
Sami Boufia,*
a
University of Sfax-Faculty of Science-LMSE BP, 802-3018, Sfax, Tunisia
b
LEPAMAP Research Group, University of Girona, C/ Maria Aurèlia Capmany, 61 – 17003, Girona, Spain

A R T I C LE I N FO A B S T R A C T

Keywords: Poly(butylene adipate-Co-terephthalate) (PBAT) is a completely biodegradable aliphatic-aromatic copolyester

Thermoplastic starch with competitive mechanical properties in comparison to commodity plastic, although it is about three times
Blends more expensive than low-density polyethylene (LDPE). The blending of PBAT with plasticized starch is an ef-
PBAT fective way to develop more accessible PBAT-based bioplastics for wide application in packaging, but the ad-
Rheology
dition of an appropriate compatibilizer is recommended. Here, we investigate the effect of maleated PBAT
Biodegradation
(PBATg-MA) and maleic anhydride (MA) coupling agents, on the mechanical properties, morphology, melt
rheology and biodegradability of PBAT/TPS blends. It was found that PBATg-MA is an effective reactive com-
patibilizer promoting the interfacial adhesion between TPS and PBAT phases with a beneficial effect on the
tensile strength as well as the elongation at break. The morphology and continuity index change considerably
according to the compatibilizer. The biodegradation kinetics was also affected by the presence of compati-
bilizers, with a decrease in the degradation rate noted when PBATg-MA was used as compatibilizer.

1. Introduction conventional non-biodegradable commodity plastics, the widespread

use of PBAT in packaging materials is still low to be considered as bulk
Poly (butylene adipate-Co-terephthalate) (PBAT), also known under material, making its biodegradability advantageous only when it is
the trade name of Ecoflex, has attracted great interest as potential decisively required. One promising alternative to made PBAT-based
substitute of high density polyethylene (HDPE), especially for packa- plastic more cost-effective is to blend plasticized starch with PBAT at an
ging materials such as lawn waste bags, food containers or film wraps, appropriate ratio ranging between 20–30 wt.%. (Ivanič et al., 2019,
among others (Vroman and Tighzert, 2009). Apart from its biode- Muthuraj et al., 2018; Olivato et al., 2011).
gradability, PBAT offers attractive physical properties, including high Starch is a biopolymer obtained from renewable resources, such as
flexibility, high strength and good tear resistance, and it is approved for wheat and potato, among others. The formation of TPS requires the
food contact applications (Fereira et al., 2019; Moustafa et al., 2019; disruption of starch granules and dissociation of complexes, as well as
Siracusa et al., 2015). In addition, it has short molding cycles and ex- melting its crystals due to the addition of water and any other plasti-
cellent sealing performance, while it is easy to process at high extrusion cizers, such is the case of glycerol (Schwach and Averous, 2004). Even
speeds (Herrera et al., 2002). though TPS is a cost-effective polymer, it cannot meet all the applica-
Driven by consumer preference towards eco-friendly packaging, tion requirements in terms of processability, mechanical properties and
along with the stringent government policies for non-biodegradable durability due to its strong inherent sensitivity to moisture, high visc-
plastics, the demand for PBAT is expected to steadily grow. For in- osity and high tendency to biodegradation (Niazi et al., 2017). For this
stance, in 2018, the PBAT market accounted for a 1.5 % share of the reason, to counteract these limitations, TPS needs to be blended with
overall bioplastic market, which is estimated to about 2 million tons hydrophobic polymers such as polyesters (Nafchi et al., 2013). Un-
and its production is expected to be tripled by 2020 (European fortunately, the notable difference in the surface properties between
Bioplastics, 2019). TPS and PBAT (i.e. the former is hydrophilic while the latter is hy-
However, mainly due to its high selling price compared to drophobic) leads to poor interfacial adhesion between the two phases,

⁎
Corresponding author.
E-mail address: sami.boufi@fss.rnu.tn (S. Boufi).

https://doi.org/10.1016/j.indcrop.2019.112061
Received 31 May 2019; Received in revised form 15 December 2019; Accepted 16 December 2019
0926-6690/ © 2019 Elsevier B.V. All rights reserved.
M. Dammak, et al. Industrial Crops & Products 144 (2020) 112061

limiting the maximum TPS content in the blend to approximately using the same twin screw extruder with a temperature profile of 140/
20–30 wt% (Imre et al., 2019). The addition of a reactive coupling 135/135/135/140 °C from the feed throat to the die, and the screw
agent or a compatibilizer is prerequisite to alleviate the deficient in- speed was kept constant at 120 rpm. A 10 cm width flat die was set at
terfacial adhesion between the two phases and increase the content of the end of the extruder to obtain the materials in the form of film with a
TPS, while maintaining an acceptable balance between strength, stiff- thickness ranging between 0.2 and 0.3 mm.
ness and elongation at break. Several reactive coupling agents have The blends were labeled as PBAT/TPS-X-Y, where X is the weight
been reported in the literature, including maleic anhydride and citric content of TPS in the blend and y the compatibilizer used (MA or
acid, maleated TPS (MTPS) (Raquez et al., 2008a, 2008b), maleated PBATg-MA).
PBAT (Nabar et al., 2005; Mohanty and Nayak, 2009a, 2009b) epoxy
additive (Wei et al., 2015a, 2015b), maleic acid (Fahrngruber et al., 2.3. Maleated PBAT (PBATg-MA)
2017) and tartaric acid (Olivato et al., 2013) are typical compatibilizers
used in PBAT/TPS blends. In all of these compatibilizers, apparently, The grafted PBAT with MA (PBATg-MA) was produced by radical
the anhydride group of maleic anhydride, the epoxy group of GMA, the grafting following the method described in the literature (Nabar et al.,
carboxyl group of acrylic acid and citric acid are efficient to improve 2005) and in our previous work (Fourati et al., 2018). In brief, 45 g of
the mechanical properties of PBAT/TPS blends by enhancing the in- PBAT, 1 g of MA and 0.5 g of BP were fed into a Brabender Plastograph
terfacial adhesion between the two phases. mixer at 140 °C, and the reaction was pursued for 20 min at a screw
In mleated TPS, the addition of maleic anhydride (MA) was found to speed of 50 rpm. Then, the PBATg-MA was cooled and pelletized and
promote the glycerol grafting onto the starch backbone, as well as the used without further purification. The degree of maleation was found to
coupling of PBAT with starch through transesterification reactions be around 1.5 % as evaluated by acid titration according to the pro-
(Raquez et al., 2008a,b). When MA grafted PBAT was used as a com- cedure outlined in the literature (Nabar et al., 2005).
patibilizer, it was hypothesized that grafted MA reacted with the hy-
droxyl groups of the starch forming ester bonds improving the inter- 2.4. Mechanical properties
facial adhesion with better control of the size of the dispersed TPS
phase, as in the case of polypropylene and polyethylene with their re- Tensile tests were performed in a universal testing machine Instron
spective maleated coupling agents (Mutjé et al. 2006). The beneficial 1122 equipped with a 2.5 kN load cell. The strain rate was set at
effect of reactive compatibilizer in improving the homogenous disper- 50 mm/min and the distance between the clamping jaws, at 150 mm.
sion of TPS in continuous PBAT phase was also demonstrated by the use Tensile test was performed in accordance with ISO 527-3 and samples
of compatibilizer bearing epoxy and anhydride group (Wei et al., were conditioned at 23 °C and 50 % of relative humidity for 72 h before
2015a, 2015b). However, these coupling agents failed to improve the testing.Ten specimens were tested for each composition.
tensile strength when the content of TPS exceeded 40 %.
In our previous work, the effect of maleic anhydride (MA), citric
2.5. Rheological measurements
acid (CA) and maleated PBAT (PBATg-MA) on the properties of PBAT/
TPS blends was investigated (Fourati et al., 2018). It was found that the
Rheological properties were investigated by a controlled rate dy-
presence of MA and PBATg-MA strongly affected the mechanical,
namic-mechanical rheometer (Pro + Kinexus from Malvern) with a
morphological and rheological properties of the blend. Both in the neat
plate geometry. The storage modulus, the loss modulus and the complex
blends and those containing PBATg-MA, the PBAT was found to be the
viscosity of blend systems were measured as a function of frequency
continuous phase albeit of representing only the 40 wt% of the total
within the range of 0.01−100 rad/s at 150 °C. Prior to each measure-
weight of the blend, while the TPS became the continuous phase in the
ment, the linear viscoelastic region was determined by an amplitude
presence of MA.
sweep in the deformation range of 0.1–100 %, at frequencies of 1 and
For all the above, in the present work, we pursue our investigation
50 rad/s. Subsequently, the deformation during the frequency sweeps
concerning the effect of MA and PBATg-MA on the mechanical, rheo-
was set to be within the linear viscoelastic region.
logical and biodegradability of PBAT/TPS blend with a content in TPS
ranging from 40 to 60 %.
2.6. Continuity analysis
2. Experimental
A gravimetric method was used to calculate the extent of the con-
tinuity of the phase after selective solvent extraction of the continuous
2.1. Materials
phase.
The TPS phase was extracted by placing the film in a solution of HCl
Native starch from potato was provided by Progial S.L. (El Mas Aliu,
2 N at 50 °C for 2 days. PBAT extraction was performed by immersing
Spain), glycerol was obtained from Quimivita, S.A. (SantAdrià del
the film in chloroform at room temperature for 2 days and the re-
Besòs, Spain), maleic anhydride (MA) and benzoyle peroxide (BP) was
maining film was dried and weighed. When the samples were not self-
acquired from Sigma–Aldrich (Barcelona, Spain). Poly (butylene adi-
supporting after extraction, the extracted phase was arbitrarily con-
pate-co-terephthalate) PBAT (Ecoflex F blend C1200) was purchased
sidered as continuous.
from BASF Chemical Company.
Winit − Wfin ⎞
2.2. Blends preparation %Continuity = ⎛⎜ ⎟ × 100
⎝ Winit ⎠ (1)

TPS was prepared by mixing starch with glycerol at a ratio of 80/ Where, Winit corresponds to the weight of PBAT or TPS before the
20 wt.% with addition of 10 % water. Then, the starch–glycerol mixture solvent-extraction step and Wfin is the weight remaining after extrac-
was extruded in a twin screw extruder (Letsritz 18 MAXX) with a screw tion. Three replicates were used for each composition.
diameter (D) of 18.5 mm and a screw length of 32D equipped with a
conical volumetric feeder. The screw speed was 100 rpm and the tem- 2.7. Moisture absorption
perature profile was set at 130/130/130/130/135 °C in the five-heating
zones. The TPS blend was then pelletized in-line and dried for 1 h at Water sorption kinetics was determined by placing samples in a
70 °C. The TPS, the PBAT granules and the compatibilizer (either MA or climatic chamber at constant relative humidity (RH) and temperature.
PBATg-MA) were fed by means of a volumetric feeder and extruded The weight of the samples was monitored at regular intervals and

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M. Dammak, et al. Industrial Crops & Products 144 (2020) 112061

recorded until achieving a steady state. For each composition, three The third and last region showed a strain hardening behavior with
previously dried films (square sample 4 × 4 cm and thickness of about continuous increase in the tensile stress until the rupture of the sample.
200 μm) were used. The comparative values for the tensile strength and elongation at break
of the different compositions are reported in Fig. 1b. The PBAT/TPS
2.8. Morphology blends at three TPS contents (40, 50 and 60 %) in the presence of MA,
PBATg and without any additives. Neat PBAT and TPS possess a tensile
The micrograph of the blends was examined using a scanning strength of 52 and 6 MPa, respectively and an elongation at break of
electron microscope (SEM) operating at 10 KV. Cross-sections of the 750 and 36 %, which means that PBAT is a highly ductile soft polymer
extruded samples were obtained after fracturing the films in presence of with a satisfactory strength while TPS has poor mechanical properties.
liquid nitrogen and the fractured surfaces were sputtered with gold. To As the TPS content decreases (from 60 to 40% by weight), and both in
better observe the shape and size of the dispersed phase, the surfaces of the presence and in the absence of PBATg-MA, the tensile strength as
the extruded and cryofractured section were etched either in chloro- well as the elongation at break of the mixture have been improved. On
form to remove the PBAT phase or in HCl solution (2 M) to remove the the other hand, when MA was used, the tensile strength and elongation
TPS phase. The etching treatment was carried out by immersion of the at the break accounted for similar values to neat TPS, remaining almost
sample in chloroform or 2 N HCl solution for 2 h. constant at different TPS contents. For instance, for the blend with 50 %
TPS, the tensile strength and elongation at break attained 12.8 MPa and
2.9. Biodegradation test 205 % in the absence of any additive, while it reached respectively
15.1 MPa and 614 % when PBATg was used as a compatibilizer. These
Biodegradation tests were carried out in a laboratory scale compost values decreased to 6.5 MPa and 36 %, respectively, when the blend
experiment according to ISO 14855-2:2018. In each test, a series of was processed in the presence of 2 % MA, which indicates a poor
vessels (each in duplicate) containing compost and the polymeric ma- compatibilization effect of MA.
terial were prepared along with a control (compost without the poly- The enhancement of the tensile strength as well as the elongation at
meric films). The amount of CO2 produced was measured periodically break, when PBAT/TPS blend was processed in the presence of PBATg-
by measuring the weights of an absorption column for carbon dioxide MA, confirmed the efficiency of this reactive compatibilizer to promote
(soda lime) and an absorption column for water (CaCl2). The biode- the interfacial adhesion between both phases. This was presumably due
gradation tests were performed at 58 °C at a 10 mL/min air (CO2-free) to the ester linkage between the grafted MA onto PBAT and TPS, as
flow rate to provide aerobic conditions during the test. The air was pointed out in the literature (Nabar et al., 2005).
bubbled through distilled water to maintain relative moisture content
of at least 50 %. 3.2. Morphology
A biodegradation curve was obtained by plotting released CO2 (%)
versus exposure time. Biodegradation was calculated as the percentage In polymer blends, morphology is a key factor affecting the me-
of polymer carbon mineralized as CO2 according to Eqs. (1) and (2): chanical and rheological properties. In order to understand some of the
properties of polymer blends, analyzing how the minor phase is dis-
(CO2)s − (CO2)c
Biodegradation (% ) = 100 persed within the continuous matrix is crucial.
ThCO2 (1)
SEM observations were performed on cryofractured films that were
Where (CO2)s and (CO2)c were the amounts of CO2 produced in the immersed in a HCl solution to selectively remove TPS phase, which will
sample and in the control, respectively. then appear in the form of holes. Morphological variations were found
depending on the blend composition as well as the compatibilizer used.
44 × Ctotal × Mtotal
ThCO2 = In the blend with a TPS content of 60 wt% without any compatibilizer,
12 (2)
the TPS phase appeared in the form of dispersed elongated droplets
where ThCO2, Ctotal, Mtotal, 44, and 12 are the theoretical carbon di- (5–20 μm in size) with some connections between them. In the presence
oxide, the relative amount of total carbon per total weight, the total of MA (Fig. 2B), the morphology changed to a fiber-like structure where
weight, the molar mass of CO2, and the molar mass of C, respectively. both the PBAT and PBAT/TPS phases were in the fibrillar form, which is
Eventually, the percentage of biodegradation can be obtained by the indicative of a fully continuous structure. When PBATg-MA was used as
ratio of released CO2 per theoretical CO2. a compatibilizer, the TPS phase was dispersed in the form of deformed
droplets with a size of about 2–15 μm and with some interconnections
2.10. Biodegradation of the films in vegetable compost between them.
At 50 wt% PBAT and 50 wt% TPS content (Fig. 2D–F), the starch
Samples cut into pieces of 4 cm × 4 cm were buried at about 4 cm was in the form of dispersed droplets of about 2−10 μm diameter, with
depth of soil composed of vegetable compost at a temperature of 25 °C. a low connection between them. In the presence of MA, a full con-
Water was sprayed once a day to sustain the moisture of the compost. tinuous morphology was observed, where the TPS formed an inter-
Samples were removed at different times and taken in photos for visual connected structure. A change from continous to dispersed morphology
tracking of the film. of the TPS phase is observed when the blend is processed in the pre-
sence of PBATg-MA. When the TPS content decreased to 40 % (Fig. 2G,
3. Results and discussion H), the TPS was well dispersed in the form of discrete spherical droplets
(2−5 μm in diameter) in the PBAT matrix, without any connection
3.1. Mechanical properties between them. The addition of PBATg-MA slightly reduced the diameter
of the TPS droplets with a narrower distribution in size.
Fig. 1A shows the typical tress-strain curves of PBAT/TPS blends From the SEM analysis, the main evolution in the morphology of the
with different TPS contents (40, 50 and 60 wt %) in the presence of MA PBAT/TPS blends was observed for the composition with a TPS content
and PBATg-MA compatibilizers and without. Except for the blends of 60 %, where a transition from co-continuous to a dispersed mor-
prepared in the presence of MA, all samples exhibited three regions in phology occurred in the presence of PBAtg-MA compatibilizer. Below
the tensile-strain plot involving elastic, plastic deformation, and strain 50 % TPS, with the exception of the PBAT/TPS50-MA, the TPS was
hardening behaviour. The first region showed linear stretching with dispersed within the PBAT matrix and was fully encapsulated by the
recoverable deformation, followed by the second region, which re- polyester. The addition of PBATg-MA contributed to reduce the size
vealed plastic deformation after the neck forming for certain samples. distribution of the dispersed TPS phase.

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M. Dammak, et al. Industrial Crops & Products 144 (2020) 112061

Fig. 1. (A) Tensile stress–strain curves of PBAT/TPS blends, (B) tensile strength, and (C) strain at break according to the TPS content and the additive used during
processing.

Referring to our previous work and based on the viscosity ratio of hand, in the presence of PBATg-MA, the rheological behavior is close to
the individual components the phase inversion composition was found that of PBAT. These evolutions could be explained by the morphology
to be around 60–65 wt% TPS and decrease to about 50 – 55 wt% when of the PBAT/TPS blends. In the presence of MA and at a TPS content of
MA was used as a compatibilizer. This explains the co-continuous 50 and 60 wt%, the morphology is dominated by a co-continuous
structure observed in the blend PBAT/TPS50 processed in the presence structure where both the PBAT and TPS have three-dimensional spatial
of MA (PBAT/TPS50-MA). continuity forming an interpenetrated network structure. Accordingly,
both the TPS and PBAT phases contribute to the viscoelastic property
3.3. Rheology and the influence of the TPS phase, with the highest viscosity, is more
pronounced. This can be seen from Fig. 3C, where the continuity index
The linear viscoelastic behaviour at melt (G' and η* vs frequency) of for TPS was plotted with the corresponding G′ for the different blends
the different blends was also studied at 150 °C. The rheological prop- studied. For the blend processed in presence of PBATg-MA and at TPS
erties of the neat PBAT and TPS as a function of frequency are shown in content of 40 wt%, the morphology is, to a large extent, nodular with
Fig. 3A and B. At 150 °C, the rheological behavior of neat PBAT and TPS PBAT forming the matrix phase and the TPS is dispersed in the form of
is completely different, with TPS exhibiting a rheological behavior ty- nodules with a size ranging from 2–15 μm (Fig. 2G, H). Therefore, the
pical of a gel (G′ nearly frequency-independent, i.e., G′ ≈ ω0.), while viscosity of the blend will be equal to that of the matrix multiplied by a
PBAT is characterized by a liquid-like behavior with G″ being higher constant factor depending on the volume fraction and the particle size.
than G′ and power-low dependence of the frequency. All the blends The viscosity curve of the blend should thus be parallel to that of the
follow a shear thinning behavior intermediate between those of the matrix in a log– log representation.
neat TPS and PBAT component. However, for the same PBAT/TPS ratio, The evolution of G' follows nearly the same trend than that of η*,
the rheological behavior was affected by the compatibilizer, especially with a domination of a gel-like behavior for a composition with a major
when MA was used. At both 50 and 60 wt% TPS, blends processed in co-continuous morphology. The deviation observed in G' at low fre-
the presence of MA displayed a behavior closer to that of the TPS, quencies domains arouses from an additional contribution to G' re-
especially in those blends containing a 60 wt% of TPS. On the other sulting from a shape relaxation of the droplets of the dispersed phase

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M. Dammak, et al. Industrial Crops & Products 144 (2020) 112061

Fig. 2. SEM Micrographs of PBAT/TPS blends : A), PBAT/TPS-60, B)PBAT/TPS-60-MA, C) PBAT/TPS60-PBATg, D)PBAT/TPS50, E)PBAT/TPS50-MA, F) PBAT/
TPS50-PBATg, G) PBAT/TPS-40, H) PBATTPS-40-PBATg. (The cross-section of the film was etched by HCl solution after cryofracturing).

driven by the interfacial tension. acceptable levels of mechanical properties.

Moisture absorption at 50 %of RH of the PBAT/TPS blends with
different TPS contents and as function of time is shown in Fig. 4(a and
3.4. Moisture absorption b, respectively). The moisture absorption increased rapidly during the
first 20 h and then gradually slowed down until a saturation plateau
Moisture absorption is one of the main shortcomings that restrict was reached after about 48 h, depending on the TPS content. Neat TPS
the application of starch-based materials. One of the objectives of and PBAT have a very different intrinsic water uptake at 50 % of RH,
blending TPS with hydrophobic polyester is to reduce the water ab- attaining about 10 % and less than 1 % for TPS and PBAT, respectively.
sorption of the film to meet the requirements for maintaining

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M. Dammak, et al. Industrial Crops & Products 144 (2020) 112061

Fig. 4. Moisture uptake at equilibrium and continuity index as a function of the

TPS content and the compatibilizer used during processing.

This is expected, given the difference in their surface properties: the

former is highly hydrophilic while the latter is a hydrophobic polymer.
As expected, the moisture absorption at equilibrium increased as the
TPS content increased, attaining in the absence of any compatibilizer,
3.3, 4.3 and 4.8 % at TPS content of 40, 50 and 60 wt%, respectively. At
a given TPS content, the moisture absorption did not change sig-
nificantly in the presence of PBATg-MA compatibilizer. However, when
MA was used, higher levels of moisture absorption were reached for the
blend with a TPS content of 40 % as well as 50 % attaining respectively
5.0 and 6.3 %.
This higher water absorption could be explained by the higher
continuity in TPS when MA was used as a compatibilizer. The full
continuity in TPS made the completely hydrophilic TPS phase acces-
sible to water by diffusion from the surface through the network paths
of the TPS phase. In the presence of PBATg-MA, the TPS phase became
dispersed and encapsulated by the PBAT matrix, especially below a TPS
Fig. 3. (a) The complex viscosity and (b) the storage modulus as functions of content of 50 %. This morphology limited the accessibility of water to
frequencies and (c) the continuity index for TPS, for PBAT/TPS blends at 150 °C TPS, thus reducing the water absorption of the PBAT/TPS blend.
at different TPS content and compatibilizer.

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M. Dammak, et al. Industrial Crops & Products 144 (2020) 112061

2009b). However, the rate of produced CO2 differs depending on the

composition of the blend and the compatibilizer added. For PBAT/TPS
blends, with TPS content between 40–60%, without any compatibilizer,
the biodegradation profile is quite similar with biodegradation rate
between 82–87% after 90days. However, in the presence of PBATg-MA,
the extent of mineralization decreased in the range of 72–74 % sug-
gesting a decrease in the rate of CO2 production with the addition of the
PBATg-MA coupling agent. The tendency changed when MA was used,
with a degradation profile close to that of cellulose and PBAT, though
only a composition with 60 wt% TPS was tested. Two hypotheses might
explain the change in the biodegradation profile depending on the
compatibilizer used. Firstly, the decrease in the continuity index of TPS
in the presence of PBATg-MA meaning that TPS is more encapsulated by
PBAT phase and less accessible by the external medium. Secondly, the
addition of PBATg-MA will create a chemical continuity between the
Fig. 5. Biodegradation test of PBAT/TPS blends based on the emission of PBAT and the TPS phase, generating an interfacial domain harder to
CO2monitoring at 58 °C according to ISO 14855-2 standard method. degrade by bacteria and enzymes to hydrolyze starch. In the presence of
MA, the acceleration of the rate of degradation might be explained by
the morphology of the blend exhibiting higher continuity index for the
3.5. Biodegradation of materials
TPS phase than that processed in the presence of PBATg (Fig. 4B). The
higher hydrophilic property along with the strong biodegradability of
Results of biodegradation test by mineralization of carbon of the
TPS might explain this effect.
different compositions and of standard cellulose are shown in Fig. 5. All
The macroscopic change of the films as a function of the time of
samples (except cellulose) were used in the same form of a thin film
burial in vegetable compost for two months at 25 °C is shown in Fig. 6.
(about 300 μm thickness) cut into of 5 × 7 cm and duplicate com-
All samples were gradually degraded with progressive fragmentation
posting tests showed a good reproducibility with no more than 3 %
and after two months, only a small amount of residual debris remained.
deviation. For all samples, the amount of CO2 produced by miner-
In addition, it can be seen that the colour of film rapidly turned to
alization steadily increased, without induction period, which is in
yellow starting from the first week of soil burying and became brownish
agreement with the biodegradable properties of TPS and PBAT. For
after one month. However, no meaningful difference in the biode-
TPS, PBAT and cellulose, the degree of biodegradation reached more
gradation process among the different compositions could be noted
than 90 % after 90 days indicating a fully biodegradable material,
under these conditions.
which is in agreement with literature data (Mohanty and Nayak, 2009a,

Fig. 6. Macroscopic appearance of biodegradation in soil at different burying time.

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M. Dammak, et al. Industrial Crops & Products 144 (2020) 112061

4. Conclusions References

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gradability of PBAT/TPS blends with different TPS contents has been Fereira, F.V., Cividanes, L.S., Gouveia, R.F., Lona, L.M.F., 2019. An overview on prop-
investigated. erties and applications of poly(butylene adipate-co-terephthalate)–PBAT based
composites (review). Polym. Eng. Sci. 59, 7–15.
The evolution of the mechanical properties was affected by the Fourati, Y., Tarrés, Q., Mutjé, P., Boufi, S., 2018. PBAT/thermoplastic starch blends: effect
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to 60%, the tensile strength and elongation at break was the highest in Carbohydr. Polym. 199, 51–57.
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both 50 and 60 wt% TPS, blends processed in the presence of MA dis- bioplastics/materials/.
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Mohamed Dammak: All blend of PBAT and TPS.
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Sami Boufi: Write the paper; Supervised the work. maleated thermoplastic starch/polyester melt blends by reactive extrusion. Polym.
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Declaration of Competing Interest Maleated thermoplastic starch by reactive extrusion. Carbohydr. Polym. 74 (2),
159–169.
Schwach, E., Averous, L., 2004. Starch-based biodegradable blends: morphology and
We wish to confirm that there are no known conflicts of interest interface properties. Polym. Int. 53 (12), 2115–2124.
associated with this publication and there has been no significant fi- Siracusa, V., Lotti, N., Munari, A., Dalla Rosa, M., 2015. Poly (butylene succinate) and
nancial support for this work that could have influenced its outcome. poly (butylene succinate-co-adipate) for food packaging applications: gas barrier
properties after stressed treatments. Polym. Degrad. Stab. 119, 35–45.
We confirm that the manuscript has been read and approved by all
Vroman, I., Tighzert, L., 2009. Biodegradable polymers. Materials 2 (2), 307–344.
named authors and that there are no other persons who satisfied the Wei, D., Wang, H., Xiao, H., Zheng, A., Yang, Y., 2015a. Morphology and mechanical
criteria for authorship but are not listed. We further confirm that the properties of poly (butylene adipate-co-terephthalate)/potato starch blends in the
presence of synthesized reactive compatibilizer or modified poly (butylene adipate-co
order of authors listed in the manuscript has been approved by all of us.
terephthalate). Carbohydr. Polym. 123, 275–282.
Wei, D., Wang, H., Xiao, H., Zheng, A., Yang, Y., 2015b. Morphology and mechanical
Acknowledgement properties of poly (butylene adipate-co-terephthalate)/potato starch blends in the
presence of synthesized reactive compatibilizer or modified poly (butylene adipate-
co-terephthalate). Carbohydr. Polym. 123, 275–282.
The authors gratefully acknowledge financial support from the
Ministry of Tunisia industry through PNRI project.