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Polymer Degradation and Stability 91 (2006) 1256e1272

www.elsevier.com/locate/polydegstab

Mechanical behaviour of biodegradable agricultural films


under real field conditions
D. Briassoulis*
Agricultural University of Athens, Department of Agricultural Engineering, Iera Odos 75, 11855 Athens, Greece
Received 7 May 2005; received in revised form 14 August 2005; accepted 6 September 2005
Available online 11 November 2005

Abstract
The mechanical behaviour of various types of biodegradable materials depends on their chemical composition and additives, the processing
characteristics and the application conditions. The environmental conditions during storage and usage of these materials strongly influence their
mechanical properties and behaviour. Ageing and degradation during the useful lifetime of biodegradable agricultural films causes losses in the
mechanical performance of the material, as measured by monitoring the evolution of some of the critical mechanical properties. Such losses may
be comparable to the corresponding losses of the conventional polyethylene agricultural films due to ageing, or they may be more drastic. In the
present paper, the overall mechanical and ageing/degradation behaviour of experimental specially designed and manufactured low-tunnel and
mulching biodegradable films, exposed to full-scale field conditions is analysed. Selected critical mechanical properties of these films manufactured with different grades of Mater-Bi material and additives, different thickness and processing schemes and exposed to real cultivation conditions in four different locations in Europe are investigated in the laboratory and compared against the corresponding behaviour of conventional
agricultural films at various stages of their exposure time.
2005 Elsevier Ltd. All rights reserved.
Keywords: Biodegradable materials; Agricultural films; Degradation of plastic films; Mechanical properties

1. Introduction
An extensive and steadily expanding use of plastic films
(mostly polyethylene) in agriculture and particularly in protected horticulture (mulching, low tunnels, greenhouses) is
reported world-wide over the last decades [1]. The market of
plastics used for these purposes in Europe involves hundreds
of thousands of hectares and thousands of tons of plastic films
per year [2]. The increasing interest in the use of mulching and
low tunnels for protected cultivation aims at elimination of
weeds, conservation of water and fertilisation also providing
a better micro-environment for the plants and protection
against adverse climatic conditions. The conventional agricultural plastic films used today are low density polyethylenes

* Tel.: C30 010 5294011; fax: C30 010 5294026.


E-mail address: briassou@aua.gr
0141-3910/$ - see front matter 2005 Elsevier Ltd. All rights reserved.
doi:10.1016/j.polymdegradstab.2005.09.016

(in some cases HDLE, LLDPE), poly(vinyl chloride), polybutylene or copolymers of ethylene with vinyl acetate.
A major negative consequence of this expanding use of
plastics for protected horticulture is related to handling the
plastic wastes and the associated environmental impact as
only a small percentage of the constantly rising amount of agricultural plastic waste is currently recycled. A large portion of
this is left on the field or burnt uncontrollably by the farmers
releasing harmful substances with the associated obvious negative consequences to the environment. The aesthetic pollution
and landscape degradation of regions of natural beauty is another well-known negative consequence in the Mediterranean
regions of Europe. Furthermore, burying of these materials in
the agricultural land, a practice unfortunately followed by
many farmers in Europe, represents an imminent threat for
an irreversible soil contamination and possibly for the safety
of the food produced in such fields. The reasons for these environmentally dangerous practices are the lack of cost efficient

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

systematic disposal techniques available to the growers and


the high labour cost for the proper collection of the plastic
films following the end of the cultivation. Thus, the use of biodegradable materials appears as a challenging attractive alternative for enhancing sustainable and environmental friendly
agricultural activities related to mulching and low-tunnels cultivation applications.
In an effort to cope up with the severe and continuously
growing agricultural plastic waste problem specific promising
materials have been developed, some of which are already in
the market, even though not widely used yet [3]. Two main
categories of innovative materials, based on two different concepts, are at the moment under development with the support
of intensive research efforts world-wide. In particular, among
the materials developed included are really biodegradable
films but also partially biodegradable films or even films of
controlled photodegradation followed by a questionable fate
in the soil [1]. It should be emphasised that in all the cases
of agricultural biodegradable films, biodegradability is one
of the major design requirements. Unfortunately, in several
cases, biodegradability also represents a major controversial
issue. Thus, it is well known that poly-lactone and poly(vinyl
alcohol) films are readily degraded by soil micro-organisms.
On the other hand, the addition of specialised pro-oxidants
in polyethylene films accelerates the breakdown of polyethylene
but biodegradability of such materials is strongly disputed
[4e11].
The efficient and profitable use of commercial biodegradable films aiming at achieving high performance throughout
their useful lifetime and at reducing pollution through practising environmentally friendly, sustainable agriculture, involves
several crucial technological questions. In particular, biodegradable agricultural films should meet a set of minimum design requirements, including: adequate strength and elongation
at break for mechanical installation, good mechanical properties with regard to ageing during the useful lifetime of the film
and 100% biodegradation in the soil preferably before the next
cultivation season. Specifically for low-tunnel films, the design
requirements also include an adequate mechanical behaviour
of these films to resist various loads and load combinations
(wind, hail, snow loads, etc.) [12]. In addition, special additives may be required aimed at adjusting the physical properties of these films depending on the geographical region, the
particular cultivation needs and the season.
A literature review on the mechanical behaviour of various
types of biodegradable materials [3] reveals that their mechanical properties depend, in general, on their chemical composition [13,14], the processing parameters, storage and
application conditions [15,16] and degradation behaviour.
However, the mechanical behaviour of biodegradable agricultural films has not been the subject of a systematic research yet
as these materials are either at the experimental stage of development or their market share still remains limited. In one case,
carbon-black-filled, biodegradable, copolyester mulch film
(EA) and commercial carbon-black-filled, high-density polyethylene (HDPE) mulch film were exposed for 12 weeks to
commercial vegetable crop growing conditions in the U.S.A.

1257

and the positive results are reported in Ref. [17]. In this case
the biodegradable EA mulch film exhibited higher tensile
and elongation at break than the presently used HDPE mulch
film. It was shown that the mechanical properties, including
the tensile strength of both the EA and HDPE, were sufficiently
preserved from planting to harvest. The changes in the elongation at break of the EA film proved that it possesses the properties needed for the specific agricultural applications.
The present work concerns with the analysis of the mechanical behaviour of the innovative biodegradable mulching and
low-tunnel films developed in the course of a European
project1 aiming at optimising the design of these films. The
biodegradable material selected and used was Mater-Bi, a material
based on starch complexed with biodegradable polyesters. MaterBi was selected among several alternative biodegradable materials considered, with emphasis placed on the applicability of
the selected material for agricultural applications (e.g. biodegradability in soil, no ecotoxicity, acceptable strength of
original films, etc.). Time and cost limitations related to the
full-scale experiments did not allow for testing more materials
in the framework of this project. The series of the full-scale
and laboratory experiments described in this work has been
carried out to investigate, among others, the overall mechanical performance of the new sets of experimental biodegradable
films and optimise their design according to the mechanical
design requirements established in Ref. [12]. The performance
of several experimental biodegradable films made of different
grades of Mater-Bi material and additives, different thickness
and processing parameters exposed in the field under real
cultivation conditions in several locations in Europe, as well
as in the laboratory, is analysed systematically in the following
sections and compared against the performance of the corresponding conventional polyethylene films.
2. Experimental design and materials
2.1. Full-scale experimental design
Three sets of experimental biodegradable low tunnel, direct
cover and mulching films were developed, tested and their design was optimised over a period of three years. The films
were used and tested in full-scale experimental cultivations
in four different European locations, in Italy, Greece, France
and Germany. The biodegradable films were compared against
conventional PE/EVA films used currently in low tunnel,
mulching and direct cover applications. During the field tests
several parameters of the films performance and their effects
in the agronomic productivity, soil characteristics and ecotoxicity were monitored and evaluated continuously. The degradation/ageing process of these materials under real
cultivation conditions (exposure to solar radiation, wind loads,
rain and hail, installation procedures, etc.) was investigated by
means of mechanical, radiometric and other appropriate
1
Bioplastics: Biodegradable plastics for environmentally friendly mulching
and low-tunnel cultivation, QLK5-CT-2000-00044.

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D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

physical tests, soil analyses, etc. Also, the biodegradation behaviour of the biodegradable films after they were rototilled in
the soil, along with the plant remains, was evaluated systematically. Furthermore, the possible release of harmful substances
in the soil due to the biodegradation process of the material
was investigated by means of ecotoxicity tests carried out during the field tests and for a period of three years following the
first experimental season. The optimisation of the design and
manufacturing of each new set of films was based on the systematic evaluation of the overall performance of the previous
set of the films as well as on analytical approaches [12]. Work
is in progress on elaborating, evaluating and eventually publishing the results of these extensive investigations [18e20].
In the present work the mechanical behaviour of the biodegradable films exposed in the four experimental cultivations in
Athens, Montpellier, Bari and Hannover, is analysed. Three
different experimental biodegradable materials were developed and tested within each set of full-scale experiments
(one set a year). Apart from the biodegradable films (denoted
by the codes M1, M2 and M3 for the mulching films and L1,
L2 and L3 for the low-tunnel films), PE conventional films
(denoted by the codes M0 for the mulching film and L0 for
the low-tunnel film) were used as controls.
The low-tunnel field trials in Greece started late in April
with watermelon cultivation. Mulching cultivation without
covering started later, in May. The experimental field shown
in Fig. 1 is located in the region of Spata northeast of Athens.
Mulching films for both covered and uncovered cultivation
were installed by manual work and watermelon plants were
transplanted at one row. The low-tunnel films were installed
by manual work as well (over the mulching and the transplants). The low-tunnel films were stretched over plastic
arches approximately 50 cm high and 60 cm wide (Fig. 1) (installation of low tunnels: April 22, 2002; May 13, 2003; April
6, 2004. Installation of mulching films: April 22, 2002; May 9,
2003; May 4, 2004; low-tunnel films removal: May 20, 2002;
June 27, 2003; May 25, 2004). During the warm days of May,
openings were made on the tunnel films, for ventilation reasons. The low-tunnel films were dismantled late in May or
in June, while the harvesting was performed during the

Fig. 1. The experimental field (watermelon cultivation) of AUA at Spata,


Attiki.

summer period. Analogous full-scale experiments were designed in the other locations [18e20].
During the three experimental cultivation periods samples
were periodically cut out of the exposed biodegradable and
conventional films in all four locations following a strict
schedule, more frequently during the first period, in order to
assess the evolution of their mechanical properties with time
during their exposure under real field conditions. One of the
main targets of this work was to investigate the effects of
the processing parameters, various stabilisers and the film
thickness on the degradation of the biodegradable agricultural
films with the exposure time, aimed at developing optimised
films. It appears that it is in fact possible to develop optimised
thin biodegradable agricultural films based on Mater-Bi that
can perform adequately for the specific applications (on-going
research work).
2.2. Critical material characteristics
As shown in Table 1 three different sets of agricultural biodegradable films were developed, one set each year, over the
three year-period, each set optimised with the development
of thinner films following the evaluation of the performance
of the corresponding previous set of films. All films were especially designed and optimised for the corresponding agricultural applications. Concerning the mechanical performance of
both the mulching and low-tunnel biodegradable films, the
most critical parameters investigated, for the given grades of
Mater-Bi material, are (a) material and additives, (b) film
thickness, and (c) processing parameters.
2.2.1. Materials
The materials finally selected and used in this work for the
experimental films development are various grades of MaterBi, a starch based complexed with biodegradable polyesters
biodegradable material that differ in terms of lifespan under
real cultivation conditions, ranging from 3 to 9 months. Mater-Bi materials are suitable for film cover with a very wide
range of properties in terms of processability, mechanical
properties, transparency, permeability to water, and biodegradation rate. They are both biodegradable and compostable according to the present European standard CEN EN13432 (also
DIN 54900 and UNI 10785 standards). Mater-Bi was selected
among several alternative biodegradable materials suitable for
the production of experimental agricultural films based on criteria related to the particular agricultural films applications: to
be biodegradable in soil, to exhibit acceptable initial strength,
to be free of ecotoxic effects in soil, etc. The number of the
parameters under investigation in the effort to optimise the
film processing and design and the cost and time limitations
associated with the full-scale experiments did not allow for
more biodegradable materials to be studied in this particular
project. The selection made by no means excludes the possibility that other innovative biodegradable materials may be
developed, that could be better suited for the particular applications (this is an open topic of research work). The

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

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Table 1
Material characteristics of low-tunnel and mulching films exposed in full-scale experiments in Athens
Material code

Film material

Processing scheme

Mulching film material


Experimental set of 2002
M1-NF 803/PeA-20b-02/A
M2-NF 803/PeA-25b-02/A
M3-NF x66eA-18b-02/B
M0-LLDPEeA-25b-02/B

Mater-Bi material: NF 803/P e 20 mm; plus 3.6% carbon blacka


Mater-Bi material: NF 803/P e 25 mm; plus 2.8% carbon blacka
Mater-Bi material: NF x66 e 18 mm; plus 5% carbon blackf
LLDPE material e 25 mm; plus 5% carbon blackf

A
A
B
B

Experimental set of 2003


M1-NF 803/PeA-20b-03/A
M2-NF 803/PeA-15b-03/A
M3-NF 803/PeA-15b-03/B
M0-LLDPEeA-25b-03/B

Mater-Bi material: NF 803/P e 20 mm; plus 3.6% carbon blacka


Mater-Bi material: NF 803/P e 15 mm; plus 4.8% carbon blacka
Mater-Bi material: NF 803/P e 15 mm; plus 7% carbon blackf
LLDPE material e 25 mm; plus 5% carbon blackf

A
A
B
B

Experimental set of 2004


M1-NF 803/PeA-15b-04/A
M2-NF 803/PeA-12b-04/A
M3-NF 803/PeA-20c-04/B
M0-LLDPEeA-25b-04/B

Mater-Bi material: NF 803/P e 15 mm; plus 4.8% carbon blacka


Mater-Bi material: NF 803/P e 12 mm; plus 6.0% carbon blacka
Mater-Bi material: NF 803/P e 20 mm; plus 3.7% green coloure
LLDPE material e 25 mm; plus 5% carbon blackf

A
A
B
B

Low-tunnel film material


Experimental set of 2002
L1-NF 803eA-60-02/B
L2-NF 803eA-60s-02/B
L3-NF 803eA-60s-02/A
L0-LDPEeA-60-02/B

Mater-Bi material: NF 803 e 60 mm;


Mater-Bi material: NF 803 e 60 mm; plus 1% UV stabiliserc
Mater-Bi material: NF 803 e 60 mm; plus 0.2% Triazineb
LDPE material e 60 mm; no stabiliser

B
B
A
B

Experimental set of 2003


L1-NF 803eA-40-03/B
L2-NF 803eA-40s-03/B
L3-NF 803eA-30s-03/A
L0-LDPEeA-60-03/B

Mater-Bi material: NF 803 e 40 mm; no stabiliser


Mater-Bi material: NF 803 e 40 mm; plus 1% UV stabiliserc
Mater-Bi material: NF 803 e 30 mm; plus 0.2% Triazineb
LLDPE material e 60 m; no stabiliser

B
B
A
B

Experimental set of 2004


L1-NF 803/PeA-30-04/B
L2-NF 803/PeA-30s-04/B
L3-NF 803/PeA-30s-04/A
L0-LDPEeA-60-04/B

Mater-Bi material: NF 803/P e 30 mm; no stabiliser


Mater-Bi material: NF 803/P e 30 mm; plus 1% stabiliserd
Mater-Bi material: NF 803/P e 30 mm; plus 0.2% Triazineb
Material PE 1010 e 60 mm; no stabiliser

B
B
A
B

VIBA Carbon Black 99545 is a master-batch based on Mater-Bi carrier with 40% of carbon black.
Cyatec UV1164: CYATEC UV1164 is a UV adsorber characterised by a very low migration rate, and suitable for very low thicknesses.
c
UV master-batch KRITILEN UV 20H (high molecular weight polymeric HALS with a small quantity of processing stabiliser) in LDPE carrier resin produced
using raw materials which comply to the food packaging regulations.
d
UV master-batch KRITILEN UV 22H (mixture of two high molecular weight polymeric HALS with a small quantity of processing stabiliser) in LDPE carrier
resin produced using raw materials which comply to the food packaging regulations.
e
Green master-batch KRITILEN GREEN 51670 in LLDPE carrier resin produced using raw materials which comply to the BGA food packaging regulations.
f
Black master-batch KRITILEN BLACK 438 in LDPE or LLDPE carrier resin produced using raw materials which comply to the food packaging regulations.
b

characteristics of the experimental biodegradable and conventional black mulching and low-tunnel film materials tested in
Athens are presented in Table 1. The conventional mulching
film material used in these experiments is LLDPE while
EVA films were also used and tested as control mulching
film in some other locations. Conventional LDPE films were
used for the low tunnels, without stabilisers. In the case of biodegradable mulching films, two grades of Mater-Bi materials
were tested: NF 803/P and NF x66 (the second one was tested
only during the first experimental set). In the case of biodegradable low-tunnel films, two grades of Mater-Bi materials
were tested: NF 803 (first and second experimental sets) and
NF 803/P (the same NF 803/P material was used for both,
the low-tunnel and the mulching films during the last-third experimental period). Grade NF 803/P was found to be best
suited for thin agricultural films.

2.2.2. Additives
As far as the biodegradable mulching films are concerned,
carbon black was used in most cases (carbon black masterbatch based on Mater-Bi for the processing scheme A or
carbon black master-batch based on polyethylene for the processing scheme B). Any possible stabilising effects of carbon
black on the degradation of Mater-Bi based biodegradable
films are yet unknown (carbon black is known, however, to
act as a strong stabiliser for the conventional film during its
useful lifetime). In some other cases of biodegradable mulching films, special additives that might be of interest for specific
cultivations like colours (especially green) or stabilisers for
transparent mulching films were tested. As far as the biodegradable low-tunnel films are concerned, the effect of the
UV stabilisers belonging to two main groups was investigated,
as shown in Table 1: (a) HALS based UV stabilisers and (b)

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D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

UV adsorber characterised by a very low migration rate, suitable for films of very small thickness.

Table 2
Technical characteristics of the two processing schemes used in the corresponding production lines of agricultural biodegradable films

2.2.3. Thickness
The design of the biodegradable films aimed, among others,
at establishing a minimum possible thickness for the film so
that the price can be reduced and the biodegradability rate
can be enhanced, retaining, however, a satisfactory performance. As shown in Table 1 it was possible to reduce gradually the design thickness of the biodegradable films from the
first to the last experimental set, based on the feedback and
the experience gained from the previous experimental test results and following laboratory tests and processing trials and,
specifically for low-tunnel films, the engineering design approach introduced in Ref. [12]. It should be noticed, however,
that the thickness values of the films shown in Table 1, actually
represent the nominal thickness of the manufactured films.
The measured film thickness was in fact found to deviate
from the nominal one, to a variable degree depending on the
processing conditions.

Processing
parameter

Technical characteristics of the processing schemes


A and B
Case A

Case B

Diameter of
extruder (mm)
Diameter of
head (mm)
L/D of extruder
Die gap of
head (mm)
Cooling ring
System used

80

100/150/100

300

800

25
1.2

30
2.1

2.2.4. Processing parameters


Two different commercial processing schemes were employed in manufacturing the experimental biodegradable films
within each set, as shown in Table 2. The processing parameters pertaining to the two schemes differ significantly. A major
difference concerns the size of the commercial extruder used
(a rather large machine was used with Scheme B).
3. Critical mechanical properties of biodegradable
agricultural films
3.1. Mechanical design requirements of biodegradable
agricultural films
Concerning the design requirements for agricultural films,
a brief overview is presented in Ref. [12]. As it is explained
in Ref. [12] the recent European Standard on plastics e
mulching thermoplastic films for use in agriculture and horticulture [21] and the Standard covering thermoplastic films
for use in agriculture and horticulture [22] require that agricultural films should meet specific minimum values of selected
mechanical properties, without, however, relating those predetermined values with the conditions to which the films will be
exposed to and the installation and supporting systems. Some
critical design requirements for biodegradable agricultural
low-tunnel films are derived in Ref. [12] as a result of a systematic analytical and experimental research work.
3.2. Laboratory assessment of the mechanical behaviour
of biodegradable agricultural films
A complete list of standard methods, pertaining to plastics and
plastic films in general, which can be used for assessing the mechanical properties of LDPE films used in protected cultivation
was presented in earlier works [23]. A sub-set of selected critical

Cooling ring: one outlet


Simple outside cooling
(no IBC)
Screw RPM
23e44 rpm; most of
production 35e44 rpm
depending upon the
flow rate required to
meet both film width
and thickness specification
Screw
130, 140, 145, 145, in one
temperature
case of Mater-Bi NF
profile (  C)
x66 C Mb
Black (12%): 115,
130, 130, 135
Blow die
145, 145, 145, 145, in
temperature
one case of Mater-Bi
profile (  C)
NF x66 C Mb Black
(12%): 140, 140,
145, 145
BUR (blow up ratio) 2.97e4.24
(for film production)
Winder speed
6.2 (60 mm film)e29
(m/min)a
(15 mm film)
Bubble radius
According to film width

Pressure inside
the bubble
Tensile force
from the wind up

Two outlets
IBC
21/31/21 rpm

110e120  C

110e120  C

1.6e2.2
65e80

Not available

According to
film width
Not available

Not available

Not available

Wider speed and screw RPM values may vary according the characteristics of
raw material lot, ambient conditions during extrusion, and melt homogeneousness coming out from the die gap.
a
Winder speed is adjusted in order to obtain the requested thickness.

standard testing methods is introduced in the European Standards


prEN 13655:2001 [21] and prEN 13206:1998 [22]. Testing
methods for mechanical properties of agricultural films that
have been harmonised at a European level2 were employed in
the course of the present work as follows.

3.2.1. Tensile properties


The tensile properties of agricultural films were measured
following the EN ISO 527-3 [24] or its equivalent ASTM D
882 [25]. The basic procedure of this method, with appropriate
adjustments for agricultural films is described in Ref. [26].
2
SMT project: New testing methods for plastic films used as greenhouse
covering materials; contract no. SMT4-CT97-2154 (DG 12).

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

3.2.2. Tear resistance


Tear resistance of plastic films is a complex function of its
ultimate resistance to rupture. However, the European Standards prEN 13655:2001 [21] and prEN 13206:1998 [22] do
not include this property among the properties to be tested
and reported. As shown in Ref. [26] standard testing methods
have been devised to test two different values of tear resistance: (a) the force required to initiate the tear and (b) the
force required to propagate the tear. Both properties are important for agricultural films even though it might occasionally be
impossible to prevent a film from tearing and so resistance to
tear propagation becomes of special interest. On the other
hand, it is important for a thin film to resist initiation of tear
since resistance to tear propagation is expected to be much
lower. The method used for initial tear resistance is ASTM
D 1004-90 [27] (also ISO 34-1 [28]; using Graves angle test
piece with nick). In fact, this testing procedure measures the
total force required for both, initiation and propagation of
tear [27]. Tear propagation resistance can be measured by
the trouser tear method ISO 6383/1 [29]. The standard Elmedorf method ISO 6383/2 [30] is a method designed to test
mainly packaging materials and is more suitable for highly extensible films, because it employs very high speeds of tearing
(7.6e46 m/min), when compared to the trouser tear method
which employs low speeds of tearing (250 mm/min). During
a preliminary phase of the present work, the thin biodegradable films under investigation were also tested with the trouser
tear method and were found to exhibit rather low tear propagation resistance values, within the error range of the smaller
load cell available, and so it was decided to employ only the
initial tear resistance method [27] for simultaneously measuring initiation and propagation of tear. Of course, the mechanism of pure tear propagation [29,31] is different from the
combined tear initiation and propagation mechanism [28]
and the results should be interpreted accordingly.
3.2.3. Impact resistance
According to the new prEN 13206:1998 standard [22] the
impact resistance shall be measured with the ISO 7765-1,
method A [31] (or ASTM D 1709 [32]). The impact resistance
of the experimental biodegradable films exposed to real field
conditions was not tested because of the limitations imposed
by the large number of samples needed for this test.
4. Mechanical behaviour of biodegradable
agricultural films
In the following sections, the results of the mechanical tests
performed on the samples taken at pre-defined time intervals
from the low-tunnel and mulching films exposed during the
three full-scale field experiments in Athens and in the other
three experimental locations are presented. Cleaning of the
samples exposed to the field conditions was proven to be
a rather difficult to accomplish, but also a very important
task, related to the efficiency of the mechanical testing as it affects the thickness measurements and also, in some cases, the
condition (degradation) of the samples received.

1261

4.1. Mechanical behaviour of original biodegradable


agricultural films
The experimental Mater-Bi based biodegradable films of
the first full-scale experiment in Italy (University of Bari)
were designed and manufactured for a nine-month strawberry
cultivation. The mechanical performance of these original
films (before exposure) is analysed in this section and compared to the corresponding behaviour of the conventional
polyethylene (or EVA) films (this behaviour was briefly presented in Ref. [3]). The reason for choosing this particular first
set original Mater-Bi based biodegradable films for the comparative studies is that the thickness of these films was comparable to the one of the conventional films as they are designed
for a strawberry cultivation that requires a good mechanical
performance over a longer cultivation period (note that the
full-scale experiments in the other locations or in the next
two experiments in Bari were designed for watermelon, melon
and lettuce that require only one to three months covering period by low-tunnel films and so thinner biodegradable films
were used in those cases).
The following samples of original films were examined: (a)
samples of thin biodegradable films suitable for covering low
tunnels (denoted by L) and (b) samples of thin biodegradable
mulching films (denoted by M). The nominal thickness of
the low-tunnel films was 60 mm whereas the measured thickness was found to vary in the range of 45e75 mm. The
nominal thickness of the mulching films was 60 mm for the
conventional film and 25 mm, 30 mm and 60 mm for the biodegradable films; the measured thickness was found to vary significantly though. The conventional films tested were LDPE
(denoted by L0-B and M0-A) and three-layer LLDPEeEVA
films (denoted by L0-A) and LLPPE (M0-B). The mechanical
properties were determined at the Laboratory of Strength of
Materials of the Agricultural University of Athens in machine
in parallel (P) and in transverse (T) directions according to the
procedure described in Ref. [26].
4.1.1. Tensile strength of low-tunnel films
The behaviour of the original (before exposure) thin lowtunnel biodegradable films shown in Fig. 2 suggests a rather
good mechanical behaviour that is comparable to the corresponding behaviour of the conventional low-tunnel films.
Elongation at break is higher in the transverse direction while
strain hardening in the parallel direction is characterised by
a higher tangent modulus. Elongation at break does not vary
so much as with the mulching films. Variability in the thickness was found to be significant.
4.1.2. Tensile strength of mulching films
The behaviour of the original very thin mulching biodegradable films shown in Fig. 3 is comparable to the one experienced by the corresponding PE mulching films in the parallel
direction while in the transverse direction the elongation at
break is lower [3]. The elongation at break is again higher
in the transverse direction but this property was found to be
rather sensitive. Another characteristic of the thin

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

stress (MPa)

(a)

(b)

parallel direction
20
18
16
14
12
10
8
6
4
2
0

L3NF803B-67
L0-LDPEB-55
L0-EVAA-45
L1NF803A-67

100

200

300

400

500

stress (MPa)

1262

transverse direction
20
18
16
14
12
10
8
6
4
2
0

L1NF803A-65
L3NF803B-67
L0-LDPEB-45
L0-EVAA-47

600

200

strain (%)

400

600

strain (%)

Fig. 2. Typical tensile stressestrain curves for thin biodegradable agricultural film in parallel (a) and transverse (b) direction (5 cm specimens) (two-digit numbers:
thickness in mm) [3].

(b)

parallel direction

transverse direction

16

16

14

14

12
M3NFx66B-30
M1NFx66A-52
M0-LDPEA-55
M0-LLDPEB-22

10
8
6
4

stress (MPa)

stress (MPa)

(a)

12
10

M3NFx66B-32

M1NFx66A-59
M0-LDPEA-52

M0-LLDPEB-24

4
2

2
0

0
0

100

200

300

400

500

100

strain (%)

200

300

400

500

strain (%)

Fig. 3. Typical tensile stressestrain curves for very thin biodegradable mulching film in parallel (a) and transverse (b) direction (10 cm specimens) (2-digit
numbers: thickness in mm) [3].

(b)

parallel direction
140

transverse direction
140

120
100

L1NF803A-62

80

L3NF803B-73

60

L0-LDPEB-50

40

L0-EVAA-49

20

initial tear resistance


(N/mm)

initial tear resistance


(N/mm)

(a)

120
100

L1NF803A-61

80

L3NF803B-75

60

L0-LDPEB-50

40

L0-EVAA-50

20
0

0
0

20

40

60

80

10

displacement (mm)

20

30

40

50

60

displacement (mm)

Fig. 4. Typical initial tear resistance curves for thin biodegradable low tunnel films in parallel (a) and transverse (b) direction (two-digit numbers: thickness
in mm) [3].

(a)

(b)

parallel direction

transverse direction
140

120
100
M1NFx66A-54

80

M3NFx66B-26

60

M0-LDPEB-50

40
20
0

initial tear resistance


(N/mm)

initial tear direction


(N/mm)

140

120
100
M3NFx66B-27

80

M2NFx66A-35

60

M0-LDPEA-49

40
20
0

10

20

30

displacement (mm)

40

10

20

30

40

50

60

displacement (mm)

Fig. 5. Typical initial tear resistance curves for thin biodegradable mulching films in parallel (a) and transverse (b) direction (two-digit numbers: thickness
in mm) [3].

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

biodegradable mulching films is the insignificant strain-hardening effects. The most important observation for the mulching films is the significant variability of the thickness.
Another feature of interest is the significant variation of the
elongation at break, especially in the parallel direction. The
main source of this differentiation was attributed to the thickness of the film (the thinner the film the higher the variability)
and also, to the processing parameters used.
4.1.3. Tear resistance
Finally, the initial tear resistance results, shown in Fig. 4 for four
thin biodegradable low-tunnel films and in Fig. 5 for four thin biodegradable mulching films indicate a satisfactory behaviour,
comparable to that of the corresponding conventional PE films [3].
4.2. Evolution of mechanical properties of mulching films
exposed under real cultivation conditions
The evolution of the elongation at break, the tensile
strength and the initial tear resistance for three sets, each

400

M0LDPEB-40
M1NF803/PB-20

300

M2NF803/PB-12

200

M3NF803/PB-20 (green)

100
0
2

10

500
400

M0LLDPEA-25b
M1NF803/PA-15b
M2NF803/PA-12b
M3NF803/PA-20c

300
200

100
0

12

(d)

parallel direction
600
500
M0LLDPEA-25

400

M1NF803/PA-20

300

M2NF803/PA-15

200

M3NF803/PA-15

100
0

500
M0LDPEA-25

400

M1NF803/PA-20

300

M2NF803/PA-25

200

M3NF866A-18

100
0

time (weeks)

500

MOLDPEC-25

400

M4NF803/PC-25
(transparent)

300

M5NF803/PC-25
(stabilized)

200

M6NF803/PC-25

100
0

10

12

time (weeks)

(f)

parallel direction

transverse direction

All B

600

600

time (weeks)

(e)

time (weeks)

elongation at break (%)

elongation at break (%)

transverse direction
600

time (weeks)

(c)

elongation at break (%)

elongation at break (%)

500

4.2.1. Elongation at break


The evolution of the elongation at break of the biodegradable mulching films in the four full-scale experimental
locations (Fig. 6) confirms that in some cases no major decrease is experienced at least within the first weeks (Fig. 6c:
M1, M2; Fig. 6a: M1) whereas, in other cases, the elongation
at break value of the original biodegradable film is already
very low (e.g. case of M3-film manufactured by processing
scheme B: Fig. 6c,e; M2 thin film (thickness 12 mm; processing scheme A) and M3 film (thickness 20 mm; processing
scheme B): Fig. 6a). A dramatic drop of elongation at break
to zero is confirmed in the transverse direction for the mulching biodegradable films within the first couple of weeks for

(b)

parallel direction
600

consisting of three different mulching films and the conventional polyethylene film, exposed in the experimental field of
AUA (Spata, Attiki) during the years 2002e2004, is presented
in this section. Selected typical cases of films exposed in the
other three locations and tested in AUA, of special interest
for the present analysis, are also analysed in this section.

elongation at break (%)

elonation at break (%)

(a)

1263

transverse direction
600
500
M0LDPEA-25

400

M1NF803/PA-20

300

M2NF803/PA-25

200

M3NF866A-18

100
0

time (weeks)

Fig. 6. Typical elongation at break in parallel (a,c,e) and transverse (b,d,f) direction curves for thin biodegradable mulching films exposed in Athens (b,c,e,f), Bari
(a), and Montpellier (d) (two-digit numbers: nominal thickness in mm) (e,f and c,d and a,b are the corresponding curves of the first and second and third experimental tests, respectively).

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

1264

most of the cases (Fig. 6), unless the initial elongation at break
values is already very low (mostly processing scheme B or
very thin films; M2 thin film 12 mm: Fig. 6b).
The low initial elongation at break values observed in several cases of biodegradable mulching films may be partially
attributed to the processing parameters used for the film extrusion and film blowing that apparently would need further optimisation for the particular Mater-Bi material, especially for
scheme B. Despite this, it should be noticed that it was possible to produce rather thin films (third experimental set) with
performance analogous to that of thicker films (the film thickness was gradually reduced from the first set to the third set;
from 25 mm to 12 mm).
In general, the relatively quick drop of the elongation at
break of the biodegradable mulching films as compared to
the conventional polyethylene films (thicker in most cases) under their exposure to field conditions is directly related to the
degradation of this property under a combination of conditions
(UV, temperature, stress, humidity, etc.), a behaviour that
appears to be inherent to Mater-Bi made very thin films produced with the specific processing schemes. The additive carbon black used with the mulching films does not function as

(a)

a stabiliser in the case of the Mater-Bi based films in the


way it does for polyethylene films.
4.2.2. Tensile strength
The evolution of the tensile strength in most cases of the
biodegradable mulching films experienced in the four locations (Fig. 7) suggests a slight local drop in the tensile strength
especially in the transverse direction, during the first week
followed by a quick recovery right after it. In some cases
the tensile strength in the transverse direction decreases slightly
below the initial stress at yield, a behaviour observed at random time intervals (Fig. 7). In addition, there are also some
cases of biodegradable mulching films that exhibit a strength
that is systematically lower than the corresponding initial
stress at yield values (e.g. very thin films exposed in Athens,
Fig. 7b; it should be noticed that the tensile strength values follow closely and asymptotically the evolution of the corresponding stress at yield values). This low-tensile strength
behaviour may be partially attributed to the processing parameters used, especially for some cases of very thin films, as discussed later on but, most probably, to the higher sensitivity of
the very thin mulching films to degradation, following their

(b)

parallel direction
30
25

M0LDPEB-40

20

M1NF803/PB-20

15

M2NF803/PB-12

10

M3NF803/PB-20 (green)

5
0
0

10

tensile strength (MPa)

tensile strength (MPa)

35

transverse direction

25
20
M0LLDPEA-25b
M1NF803/PA-15b
M2NF803/PA-12b
M3NF803/PA-20c

15
10
5
0
0

12

time (weeks)

(d)

parallel direction
25
20

M0LLDPE-25

15

M1NF803/PA-20

10

M2NF803/PA-15

M3NF803/PA-15

5
0
0

tensile strength (MPa)

tensile strength (MPa)

(c)

M0LDPEA-25
M1NF803/PA-20

10

M2NF803/PA-15
M3NF803/PA-15

5
0
2

15

M1NF803/PA-20

10

M2NF803/PA-25
M3NF866A-18

time (weeks)

tensile strength (MPa)

tensile strength (MPa)

(f)
M0LDPEA-25

10

time (weeks)

20

15

parallel direction

20

25

transverse direction

25

time (weeks)

(e)

time (weeks)

transverse direction

25
20

M0LDPEA-25

15

M1NF803/PA-20

10

M2NF803/PA-25
M3NF866A-18

0
0

time (weeks)

Fig. 7. Typical tensile strength in parallel (a,c,e) and transverse (b,d,f) direction curves for thin biodegradable mulching films exposed in Athens (bef) and Bari (a)
(two-digit numbers: nominal thickness in mm) (e,f; c,d; and a,b are the corresponding curves of the first, second and third experimental tests, respectively).

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

exposure to field conditions. This sensitivity explains the decrease of the tensile strength below the initial stress at yield,
observed in a few cases (note that ageing is in general associated with a slight increase of the stress at yield [33]). Nevertheless, with a few exceptions, the tensile strength of the
biodegradable mulching films in the parallel direction is
shown to remain remarkably stable and above the stress at
yield. Higher sensitivity is observed with the tensile strength
in the transverse direction (as it is also the case with the elongation at break), especially for very thin films, than in the parallel direction suggesting that processing parameters should be
further optimised in order to overcome these problems. In general, the tensile strength of the thinner mulching biodegradable
films of the third and second experimental period may be considered to be as satisfactory as the one of the thicker films of
the first experimental period. This behaviour may be further
improved provided that large deviations from the nominal
(design) thickness and/or premature degradation of the film
are avoided (e.g. during storage, installation, etc.). The initial
stress at yield of well-designed and processed biodegradable
mulching films, following a targeted optimisation and refinement of the processing parameters, may be safely considered
to represent an asymptotic lower limit for the evolution of
the tensile strength (a criterion established already for the
LDPE films in Ref. [33]).

4.2.3. Initial tear resistance and tear propagation


The evolution of the initial tear strength (tear propagation is
simultaneously measured with the corresponding test [28]) follows in general the corresponding behaviour of the elongation

at break as far as the displacement at maximum load is concerned and the tensile strength as far as the tear strength is
concerned, with some variations (Figs. 8 and 9). It should be
noted that the tear resistance is not normalised with respect
to the film thickness (there is a strong relationship between
tear resistance and film thickness; this relationship is not linear
though). Therefore, care should be taken to account for the
film thickness in evaluating the film performance in tear resistance, as presented in Figs. 8 and 9. There are cases, where
tear resistance of biodegradable mulching films is reduced
within the first week or start from a rather low value that
remains inferior to the corresponding behaviour of the conventional film in both directions (taking into account the film
thickness deviation from the nominal thickness). Thus, for example, the biodegradable mulching film M3: NF 803/P A-15b-03
(i.e. 15 mm thick; processing scheme B) exposed in Athens,
exhibits the worst performance in terms of tear resistance in
the transverse direction (Fig. 9b) but also the smallest tear displacement at maximum load in both directions from the beginning of the cultivation period, as compared to the other two
films M1 and M2 (Fig. 8c,d). The low values obtained with
the displacement at maximum load imply that tear propagation
associated with the initiation of tear is faster in these cases.
A similar behaviour is observed with thicker films manufactured with scheme B during the first experimental period
and so this behaviour is considered systematic and it is attributed to the processing of the film by scheme B. The same
lower tear resistance of films manufactured by processing
scheme B as compared to the corresponding resistance of
the conventional films is observed in both directions with films
exposed in all other locations.

(b)

parallel direction
30
25
M0LLDPEA-25

20

M1NF803/PA-15

15

M2NF803/PA-12

10

M3NF803/PA-20

displacement at max
load (mm)

displacement at max
load (mm)

(a)

transverse direction

30
25

M0LLDPEA-25

20

M1NF803/PA-15

15

M2NF803/PA-12

10

M3NF803/PA-20

5
0

2 B

time (weeks)

(d)

parallel direction
30
25
M0LLDPEA-25

20

M1NF803/PA-20

15

M2NF803/PA-15

10

M3NF803/PA-15

5
0
0

time (weeks)

B 5

displacement at max
load (mm)

(c)
displacement at max
load (mm)

1265

6 B 8
time (weeks)

12

transverse direction
30
25
M0LLDPEA-25

20

M1NF803/PA-20

15

M2NF803/PA-15

10

M3NF803/PA-15

5
0

10

B 5

time (weeks)

Fig. 8. Typical displacements at maximum load curves in parallel (a,c) and transverse (b,d) direction, due to initial tear for thin biodegradable mulching films
exposed in Athens (two-digit numbers: nominal thickness in mm) (c,d and a,b are the corresponding curves of the second and third experimental tests, respectively).

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

1266

(a)

(b)

parallel direction

M0LLDPEA-25

M1NF803/PA-15

M2NF803/PA-12

M3NF803/PA-20

1
0

tear resistance
(10-3 kN)

tear resistance
(10-3 kN)

transverse direction

6
5

M0LLDPEA-25

M1NF803/PA-15

M2NF803/PA-12

M3NF803/PA-20

1
0

time (weeks)

(c)

time (weeks)

(d)

parallel direction
7

transverse direction
7

6
M0LDPEB-40

M1NF803/PB-20

M2NF803/PB-15

M3NF803/PB-20
(stabilized)

2
1
0

tear resistance
(10-3 kN)

tear resistance
(10-3 kN)

6B

6
5

M0LLDPEA-25
M1NF803/PA-20

M2NF803/PA-15
M3NF803/PA-15

3
2
1
0

10

15

time (weeks)

time (weeks)

B 5

Fig. 9. Typical initial tear resistance curves in parallel (a,c) and transverse (b,d) direction for thin biodegradable mulching films exposed in Athens (a,b,d) and
Bari (c) (two-digit numbers: nominal thickness in mm) (c,d and a,b are the corresponding curves of the second and third experimental tests, respectively).

4.3. Evolution of mechanical properties of low-tunnel


films exposed under real cultivation conditions
The evolution of the elongation at break, the tensile
strength and the initial tear resistance for three sets, each consisting of three different biodegradable low-tunnel films and
the conventional polyethylene film, exposed in the experimental field of Athens during the years 2002e2004, is presented in
this section. As in the case of mulching films, selected cases of
biodegradable low-tunnel films exposed in the other three locations, of special interest for the present analysis, are also
presented in this section.

4.3.1. Elongation at break


The evolution of the elongation at break of the low-tunnel
films in the full-scale experimental locations (Fig. 10) suggests
a gradual drop of the elongation at break in the parallel direction within the first month of exposure (processing scheme A),
or even a more abrupt drop within the first week for processing
scheme B and for thinner films (Fig. 10a,c,e). A dramatic drop
of elongation at break to zero in the transverse direction is observed for the low-tunnel films exposed in the full-scale experiments within the first week, especially for processing
scheme B (Fig. 10b,f). In the case of very thin direct cover
films (exposed in Hannover; lettuce cultivation), the elongation at break in the transverse direction was shown to drop significantly within the first 1e2 weeks. On the contrary, in
another case, some low-tunnel films exhibited a relatively
good behaviour in the transverse direction (films exposed in
Montpellier; melon cultivation; Fig. 10d). In general, the elongation at break of the low-tunnel films exposed for more than

one month reaches very low values and may go practically to


zero in some cases, especially in the transverse direction.
It is apparent that the performance of the Mater-Bi based
low-tunnel biodegradable films, in terms of the elongation at
break, is dependent to a large extent on the processing parameters (but also on several other factors including thickness, exposure conditions, etc.). A further optimisation of the processing
parameters should aim at improving the performance of the thin
biodegradable films, especially in the transverse direction that
is the weak point in the performance of these films in comparison with the corresponding (thicker) conventional films.
4.3.2. Tensile strength
The evolution of the tensile strength in the parallel direction, of the low-tunnel films exposed in Athens as well as in
the other locations, confirms that the tensile strength of the
films manufactured by processing scheme A remains remarkably stable and above the stress at yield throughout their
exposure period (Fig. 11a,c,e; the typical cases shown are representative of the observations made in all four experimental
locations). In a few cases of films produced by processing
scheme B, the tensile strength was found to decrease to a lower
value than the corresponding initial stress at yield value. An
analogous behaviour to the parallel direction is observed for
the tensile strength in the transverse direction, expect that, in
some cases, films manufactured by processing scheme B experience a more significant, randomly occurring, drop in the value
of the tensile strength, below the initial stress at yield value
(Fig. 11b,d,f). In most cases of samples of biodegradable
low-tunnel films, especially of those produced by processing
scheme A, the tensile strength in the transverse direction
remains close to the initial stress at yield, throughout the

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

(a)

(b)

parallel direction
500
L0LDPEB-40

400

L1NF803/P B-30

300

L2NF803/P B-30
(stabilized)

200

L3NF803/P B-30
(stabilized)

100

elongation at break (%)

elongation at break (%)

600

500
L0LDPEA-60

400

L1NF803/P-A-30

300

L2NF803/P-A-30
(stabilized)

200

L3NF803/P-A-30
(stabilized)

100
0

time (weeks)

500

L0LDPEA-60

400

L1NF803A-40

300

L2NF803A-40
(stabilized)

200

L3NF803A-30
(stabilized)

100

(d)

parallel direction
600

elongation at break (%)

(c)
elongation at break (%)

transverse direction
600

0
0

time (weeks)
transverse direction

600
500

L0EVAC-50

400

L1NF803C-40

300

L2NF803C-40
(stabilized)

200

L3NF803C-30
(stabilized)

100
0

0
2

(e)

(f)

parallel direction
600
500

L1NF803B-60
(stabilized)
L2NF803B-60 (not
stabilized)

400
300

L3NF803B-60
(stabilized)

200

L4NF803B-60 (not
stabilized)

100
0
0

time (weeks)

10

15

20

25

time (weeks)

elongation at break (%)

elongation at break (%)

1267

3
4
A 2
time (weeks)

transverse direction
600
500

L0LDPEA-60

400

L1NF803A-60 (not
stabilized)

300

L2NF803A-60 (not
stabilized)

200

L3NF803A-60
(stabilized)

100
0
0

time (weeks)

Fig. 10. Typical elongation at break in parallel (a) and transverse (b) direction curves for thin biodegradable low-tunnel films exposed in Athens (b,c,f), Bari (a,e)
and Montpellier (d) (two-digit numbers: nominal thickness in mm) (e,f; c,d; and a,b are the corresponding curves of the first, second and third experimental tests,
respectively).

exposure period (e.g. films manufactured by using processing


scheme A and exposed in Montpellier; Fig. 11d).
As it was observed with the mulching films, the performance of the biodegradable low-tunnel films over their useful
lifetime may be comparable to, or in some cases, inferior to
that of the corresponding conventional films in terms of tensile
strength in both directions. The performance of the biodegradable films in the transverse direction is the weak point in this
particular comparison with the specific conventional films. In
most cases though, at the end of the cultivation period, the biodegradable films experiencing the best performance exhibit
behaviour comparable to the behaviour of the conventional
films in terms of tensile strength in both directions tending
to the corresponding initial stress at yield values asymptotically.
This could be used as a criterion of successful processing of
biodegradable films. Therefore, the stress at yield may be considered, in general, as an asymptotic lower limit for the

evolution of the tensile strength for low-tunnel biodegradable


films, as in the case of mulching films. Higher sensitivity is
again observed with the tensile strength in the transverse direction confirming that this behaviour represents a systematic and
difficult to tackle processing optimisation problem for MaterBi based thin films, suggesting also the need for further
optimising the relevant processing parameters. The practical
aim should be to optimise the processing parameters in such
a way that the initial stress at yield may be safely considered
to represent an asymptotic lower limit for the evolution of the
tensile strength for well-designed and processed biodegradable
low-tunnel films in both directions. As far as stabilisation is
considered, it appears that the effect of the particular additivation schemes tested on the performance of the biodegradable
low-tunnel films, in terms of tensile properties, is insignificant.
Processing problems appear to be dominant and also, more
critical and controllable than stabilisation (comparing the

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

1268

(b)

parallel direction
35
30
25

L0LDPEA-60
L1NF803A-30
L2NF803A-30 (stabilized)
L3NF803A-30 (stabilized)

20
15
10
5

tensile strength (MPa)

tensile strength (MPa)

(a)

transverse direction
35
30
L0LDPEA-60

25

L1NF803/P-A-30

20
15

L2NF803/P-A-30
(stabilized)

10

L3NF803/P-A-30
(stabilized)

5
0

0
0

A 2

(c)

(d)

parallel direction

L0EVAC-50

15

L1NF803C-40
L2NF803C-40 (stabilized)

10

L3NF803C-30 (stabilized)

tensile strength (MPa)

tensile strength (MPa)

20

20

L0EVAC-50

15

L1NF803C-40
L2NF803C-40
(stabilized)

10

L3NF803C-30
(stabilized)

A
0

0
0

time (weeks)

(f)

parallel direction
25
20

L0LDPEA-60
L1NF803A-60 (not
stabilized)
L2NF803A-60 (not
stabilized)
L3NF803A-60
(stabilized)

15
10
5

0
0

time (weeks)

time (weeks)

tensile strength (MPa)

(e)
tensile strength (MPa)

transverse direction

25

25

time (weeks)

time (weeks)

transverse direction
25
20

L0LDPEA-60
L1NF803A-60 (not
stabilized)
L2NF803A-60 (not
stabilized)
L3NF803A-60
(stabilized)

15
10

5
0
0

time (weeks)

Fig. 11. Typical tensile strength in parallel (a) and transverse (b) direction curves for thin biodegradable low-tunnel films exposed in Athens (a,b,e,f), Montpellier
(c,d) (two-digit numbers: nominal thickness in mm) (figures e,f; c,d; and a,b are the corresponding curves of the first, second and third experimental tests,
respectively).

stabilisation schemes used against no stabilisation; basic research is needed in the direction of developing new additivation schemes appropriately designed for biodegradable
Mater-Bi films).
4.3.3. Initial tear resistance and tear propagation
The evolution of the initial tear strength of the low-tunnel
biodegradable films follows in general the corresponding behaviour of the elongation at break as far as the displacement
at maximum load is concerned and the tensile strength as far
as the tear strength is concerned (resistance to tear propagation
is simultaneously measured with the corresponding test). As in
the case of the mulching films, a more gradual reduction in
tear resistance is observed with time. The low-tunnel biodegradable films exposed in Athens confirm a systematic difference between processing schemes A and B, in favour of
scheme A (Figs. 12 and 13). It appears that biodegradable

films manufactured with processing scheme A exhibit better


tear resistance and they tear more slowly than the films
manufactured with scheme B. The initial tear resistance of
the low-tunnel biodegradable films (scheme A), if normalised
with respect to the film thickness, is found to be comparable to
the corresponding resistance of the conventional films and
remains relatively stable over most of the exposure period.
An analogous behaviour was observed with the films exposed
in the other locations (e.g. the tear resistance in the transverse
direction of films exposed in Hannover confirms the adequate
behaviour of processing scheme A; Fig. 13f).
The particular stabilisation schemes used with the biodegradable low-tunnel films do not appear to affect the tear resistance of the films and certainly they do not improve the weak
behaviour of the films produced with a processing scheme that
has not been optimised for the specific thin Mater-Bi based
films production.

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

(a)

(b)

parallel direction

L0LDPEA-60

25

L1NF803A-30

20
15

L2NF803A-30
(stabilized)

10

L3NF803A-30
(stabilized)

displacement at max
load (mm)

displacement at max
load (mm)

30

20
L0LDPEA-60

15

L1NF803A-30

10

L2NF803A-30
(stabilized)
L3NF803A-30
(stabilized)

0
2

time (weeks)

(c)

time (weeks)

(d)

parallel direction
30
25

L0LDPEA-60
L1NF803A-40
L2NF803A-40
(stabilized)

20
15
10

L3NF803A-30
(stabilized)

displacement at max
load (mm)

displacement at max
load (mm)

transverse direction

25

35

1269

transverse direction
30
25

L0LDPEA-60
L1NF803A-40
L2NF803A-40
(stabilized)

20
15

L3NF803A-30
(stabilized)

10
5
0

0
0

A
time (weeks)

4 A

time (weeks)

Fig. 12. Typical displacements at maximum load curves due to initial tear for thin biodegradable low-tunnel films exposed in Athens in parallel (a,c) and transverse
(b,d) direction (two-digit numbers: nominal thickness in mm) (c,d and a,b are the corresponding curves of the second and third experimental tests, respectively).

5. Overall evaluation of the mechanical behaviour


of the biodegradable films
5.1. The mechanical behaviour of the biodegradable
films under real field conditions
5.1.1. Low-tunnel films
The overall mechanical performance in the field experiments of the low-tunnel biodegradable films that were (a)
manufactured with an adapted-optimised processing scheme
(e.g. scheme A) and (b) designed in accordance with an appropriate design procedure [12], was found to be satisfactory in
general, comparable to the corresponding tensile strength performance of the conventional films of an analogous thickness
(a further effort for optimisation of the processing parameters
is under way aimed at improving the behaviour with respect to
elongation at break). An illustrative example is shown in
Fig. 14: the mechanical performance of the 30 mm film L3NF 803/PeA-30s-04/A (Table 1) after 50 days of exposure
in the experimental filed of AUA was found to be as good as
the corresponding performance of the 60 mm conventional
LDPE films. Despite the presence of ventilation openings,
the film performed very well and no tear propagation or premature failure due to wind pressure was observed. It may be
concluded therefore that the tensile strength criterion, strongly
associated with the tear resistance of the film, is the major design criterion in the case of the thin low-tunnel biodegradable
films. Improvement of the film behaviour in terms of retaining
a satisfactory percentage of the initial value of the elongation
at break with the time of exposure is desirable, but it appears
that this property is not as critical as the tensile strength for the

overall mechanical performance of the films (it is important


when related to tear propagation and possibly to localised failure due to puncture or impact though).
5.1.2. Mulching films
The thin biodegradable mulching films with very low elongation at break values were found to degrade quicker than the
(thicker) conventional films as a result of tear propagation in
the transverse direction along the holes opened for the transplantation (premature failure in cases of using tools with
tooth-like edges) or due to gradual degradation (Fig. 15).
Such problems were not observed with thicker biodegradable
or conventional mulching films (e.g. thickness of 20e
25 mm). Therefore, very thin Mater-Bi based biodegradable
mulching films need to be further improved in terms of their
mechanical behaviour through optimisation of the processing
parameters. Thicker biodegradable films (i.e. at least 15 mm)
may be used safely in replacing conventional mulching films.
5.2. Optimising the processing parameters
The performance of the various biodegradable experimental
mulching and low-tunnel films exposed under different field
conditions (as presented in the previous sections) confirms
that the processing parameters used for the extrusion and
film blowing play a crucial role in the overall mechanical behaviour of these films. It is apparent that some of the processing scheme B parameters used were not appropriate for the
film extrusion and blowing of the particular Mater-Bi material
based thin films. It is also evident that the processing scheme A
parameters may be further optimised to improve the

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

1270

(a)

(b)

parallel direction

L0LDPEA-60

L1NF803A-30

L2NF803A-30
(stabilized)

L3NF803A-30
(stabilized)

tear resistance
(10-3 kN)

tear resistance
(10-3 kN)

transverse direction
7

L1NF803A-30

4
3

L2NF803-30
(stabilized)

L3NF803A-30
(stabilized)

4 A

L0LDPEA-60

4
A
time (weeks)

time (weeks)

(c)

(d)

parallel direction

L0LDPEA-60

L1NF803A-40

L2NF803A-40
(stabilized)
L3NF803A-30
(stabilized)

3
2

tear resistance
(10-3 kN)

tear resistance
(10-3 kN)

transverse direction
7

L0LDPEA-60

L1NF803A-40

L2NF803-40
(stabilized)

L3NF803A-30
(stabilized)

0
0

(e)

(f)

parallel direction

L0PE1010B-40
L1F803B-40

L2F803B-40
(stabilized)

2
1
0
4

time (weeks) AlI B

tear resistance
(10-3 kN)

6
5
4

time (weeks)

A 2

time (weeks)

tear resistance
(10-3 kN)

transverse direction
7
6
5
4
3
2
1
0

D0LDPEH-50
D1NF803H-15
D2NF803H-20
D3NF803H-12

time (weeks) AlI A

Fig. 13. Typical initial tear resistance curves for thin biodegradable low-tunnel films exposed in Athens in parallel (a,c) and transverse (b,d) direction, in Bari (e)
and Hannover (f) (two-digit numbers: nominal thickness in mm) (c,d; e,f; and a,b are the corresponding curves of the second and third experimental tests,
respectively).

mechanical performance of the biodegradable films, even


though satisfactory in most cases. Nevertheless, improvement
is needed especially in the mechanical performance of the thin
and very thin films in the transverse direction. Subsequently,
the parameters of the processing schemes A and B have
been critically evaluated and they are currently under revision/refinement (work in progress).
6. Conclusions
The mechanical performance of several experimental biodegradable films made of different grades of Mater-Bi material
(polymers based on starch complexed with biodegradable
polyesters) and additives, different thickness and processing
parameters are investigated and compared against the corresponding behaviour of conventional agricultural films under
real cultivation conditions. Investigation of selected critical
mechanical properties describing the mechanical behaviour

of these experimental mulching and low-tunnel biodegradable


films, exposed to four different locations across Europe, confirms that a rather good mechanical behaviour is possible for
these films, comparable to the behaviour of conventional agricultural films in terms of strength, inferior, however, to the
conventional films in terms of elongation at break. The most
important points may be summarised as follows:
e The performance of the biodegradable mulching and lowtunnel films over their useful lifetime may be comparable
to that of the conventional (thicker) films in terms of tensile strength in the parallel direction; the tensile strength of
thin biodegradable films may reach values below the initial
stress at yield in the transverse direction.
e The biodegradable mulching and low-tunnel films, especially thin films in the transverse direction, may exhibit
a very low elongation at break values within the first
week of their exposure.

D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

1271

and certainly they do not improve the weak behaviour of


the films produced with processing schemes that have
not been optimised for the specific biodegradable films
production. Processing problems appear to be more critical
and controllable at this moment, than stabilisation. Basic
research is needed though in the direction of developing
new additivation systems, appropriate for biodegradable
Mater-Bi based low-tunnel and mulching films.
e In general, the performance of the thin biodegradable films
in the transverse direction remains the weak point in comparison with the conventional films (thicker films).

Fig. 14. Typical low-tunnel L3-NF 803/PeA-30s-04/A biodegradable film


after 50 days of exposure between low tunnels using conventional
L0-LDPEeA-60-04/B LDPE films.

e The evolution of the initial tear strength of the Mater-Bi


based biodegradable films follows in general the corresponding behaviour of the elongation at break as far as
the displacement at maximum load is concerned and the
tensile strength as far as the tear strength is concerned;
The biodegradable films manufactured with processing
scheme A exhibit a better tear resistance and they tear
more slowly than the films manufactured with scheme B
(large machine) in both directions.
e The stabilisation schemes used with the biodegradable
films do not affect the mechanical performance of these
films. The particular stabilisation schemes used with the
biodegradable films do not appear to affect significantly
the tensile strength and the tear resistance of the films

Concerning low-tunnel films, for first time the design of


low-tunnel films was based on a specific design procedure
and was not done empirically. It appears that it is in fact
possible to develop optimised thin low-tunnel films based on
Mater-Bi that can perform adequately for these specific applications. This can be achieved despite the fact that Mater-Bi
based films degrade faster than the corresponding conventional
films.
The Mater-Bi grade NF 803/P was found to be best suited
for blow extrusion of thin biodegradable agricultural films. It
has been shown that it is possible to develop very thin biodegradable films made of this grade (with a thickness of at
least up to 30 mm for low tunnels and 15 mm for mulching
films) that perform satisfactory for the specific applications
and may replace conventional (thicker) polyethylene films.
A further optimisation of the processing parameters in
blow extrusion of thin biodegradable films is expected to
allow for an improvement of their mechanical behaviour in
the transverse direction, and especially in retaining higher
values of the elongation at break during the useful lifetime
of the films. The practical aim is to optimise the processing
parameters in such a way that the stress at yield may be safely
considered to represent an asymptotic lower limit for the
evolution of the tensile strength for well-designed and processed thin biodegradable low-tunnel films and improve the
elongation at break in the transverse direction for both,
mulching and low-tunnel films. Work along this direction is
in progress.

Acknowledgments

Fig. 15. Typical very thin mulching M2-NF 803/PeA-12b-04/A biodegradable


film after 21 days of exposure.

This work has been carried out in the framework of the


European research project Bioplastics: Biodegradable plastics
for environmentally friendly mulching and low-tunnel cultivation, QLK5-CT-2000-00044, funded by the EU. Special
thanks are due to N. Chronopoulou, O. Thodi and E. Hatzis
for performing the mechanical tests and to Mr. G. Makris
for collecting the samples and supervising the experiments
in the experimental field in Athens. Also, thanks are due to
the partners of the project who provided the samples exposed
to their experimental fields in Hannover (J. Michaelis, B. von
Elsner; University of Hannover), in Montpellier (P. Feuilloley,
V. Judais; Cemagref) and in Bari (G. Vox, E. Schettini, G.
Scarascia; University of Bari).

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D. Briassoulis / Polymer Degradation and Stability 91 (2006) 1256e1272

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