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To cite this article: Zuzanna Sydow & Krzysztof Bieńczak (2018): The overview on the use
of natural fibers reinforced composites for food packaging, Journal of Natural Fibers, DOI:
10.1080/15440478.2018.1455621
ABSTRACT KEYWORDS
Nowadays global packaging is a very important branch of industry and it is still Food packaging; natural
growing. In the case of food packaging, materials such as polypropylene, fibers; composites; hybrid
polyethylene (PE) and other synthetic polymers have become very popular. composites; biocomposites;
fibers treatment
However, the biggest disadvantage of traditional polymers is their poor biode-
gradability. Alternatives to them are biodegradable polymers, such as starch, 关键词
cellulose, polyhyroxyalkanoate, chitosan, polylactic acid (PLA), however they 食品包装; 天然纤维; 复合
still have some disadvantages, for example in the case of PLA, the prize is very 材料; 混杂复合材料; 生物
high. Very promising materials are natural fibers, which can be used as a filler in 复合材料; 纤维处理
a matrix of biodegradable polymers reducing their cost or non-biodegradable,
increasing their eco-friendliness. Nonwoven based on natural lignocellulosic
fibers are also promising. Therefore, the purpose of this review is to determine
the current state of knowledge about natural fibers used in composites, with
particular reference to new composite materials based on fibers that can be
used in food packaging.
摘要
目前,全球包装是一个非常重要的产业分支,而且还在不断发展。在食品
包装的情况下,聚丙烯、聚乙烯等合成高分子材料已经非常普及。然而,
传统聚合物最大的缺点是生物降解性差。替代他们的是可生物降解的聚合
物,如淀粉、纤维素、聚羟基链烷酸酯、壳聚糖、聚乳酸(PLA),但是
他们仍然有一些缺点,例如在聚乳酸的情况下,这个奖是非常高的。非常
有前途的材料是天然纤维,可作为可生物降解聚合物基质中的填料,降低
其成本或不可生物降解,提高其生态友好性。无纺布基于天然木质纤维素
纤维也有前途的。因此,本次审查的目的是确定使用天然纤维复合材料知
识的当前状态,以纤维,可用于食品包装复合新材料特别参考。
CONTACT Zuzanna Sydow zuzanna.sydow@gmail.com Division of Food Industry and Food Transportation, Poznan
University of Technology, Institute of Machines and Motor Vehicles, Piotrowo 3, Poznań 60-965, Poland.
Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/wjnf.
© 2018 Taylor & Francis
2 Z. SYDOW AND K. BIEŃCZAK
In addition, the topic of innovative intelligent and active packaging has recently been developed
(Realini and Marcos 2014).
According to the latest forecasts by Smithers Pira, the global packaging market, not only related to
food packaging, is going to reach $980 billion in 2020. For comparison, the global packaging market
in 2000 was at the level of $383 billion. Within the six packaging categories: flexible packaging, rigid
plastic, board, glass, metal and others, the biggest impact on the trillion dollars’ achievement are
going to have rigid plastics with the highest annual growth 4.4% year-on-year. This is directly related
to the growing popularity of such polymers as polyethylene terephthalate (PET), as a lighter and
cheaper substitute for metal cans and glass bottles. Still the board is going to be the most popular in
2020 (30.7%), although its share in the total sum is going to systematically decrease in favor of
flexible packaging (paper, plastics and foil laminates) and mainly rigid plastics (22.2% and 22.5%
respectively) (Pira 2017).
The use of synthetic polymers in the packaging industry is associated with such advantages as: low
production costs, convenience in use (low weight), aesthetic appearance, good physical as well as
chemical properties and many others. It is estimated that over 40% of plastics are used for packaging
purposes, while half of them are used for food packaging (Rhim, Park, and Ha 2013) (Figure 1).
However, the present overexploitation of synthetic polymers is associated with the problem of
their subsequent disposal. Most polymers used in food packaging are non-degradable and thus
generate environmental problems (Majeed et al. 2013). Therefore, as a substitute for non-biodegrad-
able synthetic polymers, biodegradable synthetic polymers, i.e. decomposable with the participation
of microorganisms, have been used recently. Examples of biodegradable polymers are: poly(lactic
acid) (PLA), poly(lactide-co-glycolide), polycaprolactone, poly(butylene succinate) and many others
(Vroman and Tighzert 2009). However, the main problem associated with this biodegradable
polymers is their high cost. For example, the average cost of using one of the most synthetic
biodegradable polymers PLA is 3–4 €/kg, while for traditional thermoplastic polymers an average
cost is 1.08 euro/kg for polystyrene, 0.80 euro/kg for polypropylene (PP), 0.78 euro/kg for PVC
(Bogoeva-Gaceva et al. 2007).
The use of both non-biodegradable and biodegradable polymers is related to the limitations
mentioned above, hence many scientists have recently paid more attention to suitable fillers to create
composites and consequently eliminate the limitations resulting from the use of the polymer itself.
Examples of the promising fillers that can be used in composite materials for food packaging are
natural fibers, mainly lignocellulosic, like jute, sisal, hemp, cotton, kenaf.
However, in the literature there is still little information about composites with natural fibers used
for food packaging, especially there is a lack of data on the properties of this type of packaging,
including the impact on the quality of stored food.
Therefore, the purpose of this review is to determine the current state of knowledge about natural
fibers used in composites, with particular reference to new composite materials based on fibers that
can be used in food packaging. The article also aims on limitation connected with using natural
fibers in composites and provides solutions to overcome a very common drawback.
Table 1. Properties of selected natural fibers plant origin (Rameshkumar and Mohanraj 2017).
Fiber Density (g/cm3) Moisture content (wt. %) Elongation at break (%) Fracture stress (MPa) Young Modulus (GPa)
Jute 1.3 12.6 1.5 393 26.5
Flax 1.5 10.0 2.7 345 27.6
Hemp – 10.8 1.6 690 –
Sisal 1.5 11.0 2.0 511 9.4
Coir 1.2 8.0 30.0 175 4.0
Bamboo 0.8 – – 391 48
Pineapple – 11.8 1.6 413 34.5
Ramie 1.5 8.0 3.6 400 61.4
Banana – – 2.5–3.7 700–800 27–32
4 Z. SYDOW AND K. BIEŃCZAK
involves the preparation of sheets made of a thermoplastic polymer, and then stalking them with the
layers of natural fibers forming sandwich system with more than two layers. Between the sheets of
the fiber layers, a polymer can be placed in the form of powder. Composite boards are obtained by
pressing at high temperatures (Cierpucha 2013).
The use of natural fibers as a filler in composites has a number of advantages, such as low cost
(compared to synthetic fibers like carbon, steel, glass), which is especially important when using
fibers in composites with the matrix made of biodegradable polymer; low weight due to low density
(the half weigh of glass fibers), wide availability, good mechanical, thermal and acoustic insulating
properties, non-harmful processing. Moreover, natural fibers are a renewable source in opposite to
fossil-fuels based plastics, which make them a sustainable resource (Faruk et al. 2014; Sanjay et al.
2018). Table 2 The improvement of biodegradation rate of composites with natural fibers is also
crucial. Due to the fact that the use of food packaging with the addition of natural fibers is not yet
widespread, there is no biodegradation research of this type of packages in the literature, but their
biodegradability will definitely depend on the nature of the filling and matrix, as well as the
proportions in which they occur in composites. It can therefore be assumed that their biodegrad-
ability will be comparable to the biodegradability of composites for other applications. For example,
Ali et al. (2017) investigated that in the case of composite composed of pineapple peel fiber and low-
density polyethylene (LDPE), the increase in fiber content lead to increasing in biodegradation rate.
The highest biodegradation of composite was obtained for the fiber content 50% and polymer
content 35%.
Due to specific physical and chemical properties, natural fibers acquire the applicable mechanical
properties, which are very important in the aspect of their use in filling composite materials. For
example, the bast fibers are characterized by high stiffness, surface smoothness and resistance to
bending, which makes the fibers more and more often used to reinforce polymer composite
materials (Cierpucha 2013). However, the specific properties of the obtained composite depend on
a number of factors. According to Pickering (Pickering, Aruan Efendy, and Le 2016), during the
production of a fiber/polymer composite, factors such as: fiber selection (type, treatment, harvest
time, method of extraction); fiber content; fiber dispersion and orientation; matrix selection, porosity
as well as composite manufacturing process should be taken into consideration. For example, Bos,
Van Den Oever, and Peters (2002) showed that a higher (by 20%) strength was characterized by flax
fibers extracted manually rather than mechanically by decortication using pilot scale breaking,
scutching and hackling procedure, which is the result of generating in this way cracks of bridges
between microfibrils. Also Shah et al. (2012) determined that minimum and critical fiber volume
fractions for flax and jute-polyester composites were higher than for synthetic fiber composites, e.g.
the critical volume for jute-polyester and carbon-polyester were found 8.1% and 2.4% respectively.
Thanks to many advantages and specific properties, composites containing natural fibers have
found commercial applications widely described in the literature. Fibers of plant origin, in particular
bast and leaf (e.g. flax, hemp, kenaf, sisal), are successfully used in the automotive industries. Door
JOURNAL OF NATURAL FIBERS 5
panels, seat backs, package trays or trunk liners made of natural fiber reinforced composites can be
found e.g. in Audi, BMW, Citroen, Fiat, Opel, Peugeot, Rover, Toyota, Volksvagen, Ford, Volvo,
Honda and many others (Faruk et al. 2014). The use of natural fibers in the automotive industry is
mainly related to the possibility of cost reduction, good electrostatic properties, absorption of
vibrations, thermal insulation and sound damping properties (Cierpucha 2013). Moreover, reduction
of the specific gravity of fiber-reinforced composites compared to traditional polymers reduces the
weight of vehicles, which results in savings in fuel consumption. Composites filled with fibers have
also found application in the aerospace industry, construction, furniture, horticulture and the
production of equipment used in sports and recreation (Cierpucha 2013; Faruk et al. 2014,
Kozłowski and Muzyczek 2017). Also, according to Yang et al. (2006), due to the properties, such
as water absorption biocomposites with lignocellulosic fillers can find applications in many damp
places, such as interior of bathrooms, wood decks and others.
It is also worth mentioning that, except of extracted fibers, there is the possibility of using hurds
(shives) e.g. from hemp for composites, especially for particle boards. Hurds are woody lignocellu-
losic particles with elongated shapes that are obtained in retting mills as a by-product during the
processing of bast fibers such as flax and hemp, and are usually treated as waste material. On the
basis of hemp hurds building and packaging materials are successfully created. Such materials are
characterized by lower costs compared to traditional ones, as well as improvement of thermal
insulation conditions. The technology of using the hurds in construction is widespread in Great
Britain and France, where buildings are put in the lime-and-hurds composite technology. In the
rooms made of these composites the specific microclimate is created ideal for, for example, wine
storage. Hurds can be also successfully used for making composites with thermoplastic polymers.
Composite materials using thermoplasts and hurds grasshoppers are extruded using traditional
methods (Cierpucha 2013).
water absorption and thickness swelling for composites LDPE matrix were higher than for those with
PP matrix. This is the result of weak interfacial adhesion between the filler and PE chains. The
increase in filler content from 30% to 40% also increased the value of the studied parameters. The
utility of polymer composites reinforced with natural fibers in terms of the creation of food
packaging materials to respiring fresh products has also been noted by Berthet et al. (2015a). The
authors observed an increase in water vapor transmission rate from 11 up to 110 g/(m2*day), for
poly(3-hydroxybutyrate-co-valerate) (PHBV)/wheat straw fibers composites. In addition, using the
natural fiber as a filler reduced the cost of the composite, because the PHBV polymer, although
biodegradable, is expensive. However, it is worth noting that high water absorption is not always
treated as an advantage. Higher hydrophilicity results in lower affinity to the polymer matrix, so it is
difficult to obtain a homogeneous dispersion of fibers in the polymer matrix, which can lead to
decrease of mechanical properties of composite (Essabir et al. 2016)
An additional property that may be important in the context of creating food packaging materials
is thermal stability. Soman, Chacko, and Prasad (2017) indicated that PLA with cellulose-nanofibers
from Areca catechu husk composites were characterized by higher thermal stability compared to
PLA. A similar effect of higher thermal stability for a biocomposite composed of wheat straw and
aromatic copolyester, polybutyleneadipate-co-terephthalate, in comparison to the polymer matrix
itself was observed by Averous and Digabel (2006).
Very important are also UV-blocking properties of natural fibers, which are especially valuable
for the protection of packaged products, in particular colored products. It has been proved that
natural bast fibers such as flax and hemp are rich in Ultraviolet Radiation absorbers, for example
pigments, lignin, waxes and pectin. In the case of textiles made of natural fibers, many factors may
influence the blocking properties, for example structure, density and porosity of fabric as well as type
of dyes covered the fabric. However, it is worth mentioning that due to aggressive treatment during
extraction and processing of fibers, UV-blocking properties can be reduced. This results in need for
improvement of mentioned properties, for example by the treatment with the solution of nanolignin
(Zimniewska and Batog 2012).
The application of the obtained composite is also determined by the mechanical properties of the
material. Although some researchers observe a decreasing of mechanical properties of composites
with natural fibers (Berthet et al. 2015a, b), others indicate their improvement (Fendler et al. 2007;
Julson et al. 2004; Lopez-Gil et al. 2014; Panthapulakkal, Zereshkian, and Sain 2006), which is
understandable due to the use of different matrix and differences in many other factors. According
to Lopez-Gil et al. (2014), one of the methods which can improve the mechanical properties of
starch-based materials is the use of natural fibers as a filling. Starch is a good alternative to
traditional biodegradable polymers such as PLA due to the relatively low cost. However, due to
such disadvantages as poor mechanical properties and high density, their application to food
packaging is limited. Plasticization of starch with glycerol in order to obtain thermoplastic starch
and secondly using barley straw and grape waste as natural fibers filler resulted in the fact that new
materials developed were compered (with reference to mechanical properties) to PP, PET and PLA.
Recently, there is a tendency to create active packages, which are supposed to be the future for the
food packaging industry. Active packages are defined as systems which (as a result of chemical,
physical and biological activities) actively change the conditions inside the packages in order to
extend the shelf-life and preserve the quality and sensory characteristics of food (Han 2005). This
kind of packages can act as absorbers, with the function of absorbing gases with unpleasant smell,
water vapor or oxygen. Moreover, on the other hand, there is also a group of active packages that
play the role of emitters excreting the substances that protect food against spoiling microorganisms.
Therefore, packages with the addition of natural fibers characterized by the possibility of absorbing,
for example, water vapor, can be treated as active packages. Moreover, there is also the possibility to
introduce active substances, create packaging material with antimicrobial activity. The choice of an
antibacterial active agent depends on many factors, including the type of food product, as well as the
expected microorganism that causes food spoilage. However, it should be noted that the introducing
JOURNAL OF NATURAL FIBERS 7
substance must be safe and able to be used in contact with food products. The substances described
in the literature as promising antimicrobial agents for use in food packaging are e.g. essential oils
(like oregano, thyme, cinnamon and tea tree oil), herbs, lysozyme, nisin, natamycin and other. Also
an example of such an active substance is thymol (2-isopropyl-5-methylphenol), which shows
antioxidant and antimicrobial activity against bacteria, fungi, yeast and mold. Tawakkal, Cran, and
Bigger (2017). Tawakkal, Cran, and Bigger (2017) tested the antibacterial effect of thymol introduced
into kenaf fiber/PLA composite packages against E. coli bacteria. It was observed that a significant
addition of thymol provides strong antibacterial effects against E. coli in both solid and liquid media.
In addition, the authors indicated the antibacterial effect of composite films with thymol in a real
food system – the population of E. coli inoculated on chicken slices was significantly reduced. Thus,
authors stated that kenaf/PLA/thymol composite films are a very promising material for the
production of active packaging systems (Figure 2).
Some types of natural fibers, like kapok, bamboo, hemp and flax are believed to be inherently
antimicrobial. For example, in the case of hemp, essential oils can act as antimicrobial agent and
inhibitory effect depends on variety and sowing time (Borsa 2012).
Figure 2. Fungal growth on the chicken surface stored in contact with PLA composites films at 25°C (Tawakkal, Cran, and Bigger
2017).
8 Z. SYDOW AND K. BIEŃCZAK
composites containing natural fibers as one of the fillers. Nanoclays are defined as nanoparticles of
layered mineral silicates found naturally in the Earth’s crust. The clay group includes montmor-
illonite, bentonite, kaolinite, hectorite and halloysite, and they differ in chemical composition and
nanoparticle morphology (http://www.sigmaaldrich.com 2018).
Najafi et al. (2012) studied the effect of nanoclay on the physical and chemical properties of a
composite based on PP and reed fiber. An increase in tensile modules and strength was observed, and
the biggest improvement of mechanical properties was achieved when the nanoclay was used at 4 phc
(parts per hundred compounds). On the other hand, decrease of water absorption of composites in the
presence of nanoclay was noted, which is consistent with the results obtained by Kord (2012).
Also Kord (2011) applied nanoclay as a second filler for composites based on PE matrix and rice
husk flour as a basic filler. Authors observed that the studied parameters, such as crystallization
temperature, crystallization enthalpy and crystallinity level increased with the increase of nanoclay
content to 2 phc, while above this value, a decreasing trend was observed. The addition of nanoclay
at 2 phc resulted in better dispersion and higher order of intercalation.
Improvement of the mechanical properties of PP/hemp fiber after addition of nanoclay was also
observed by Kord (2012). Authors noted an increase in the value of tensile modulus, tensile strength
and elongation at break with the increase in the content of nanoparticles, but only up to 3%. Further
loading of nanoclay caused a decrease in the value of the tested parameters.
Physical methods mainly include the use of corona or plasma as a source of ionized gas, laser or
steam explosion (Venkatachalam et al. 2016). Enciso, Abenojar, and Martınez (2017) determined the
effect of low-pressure plasma treatment on the adhesion between natural flax fibers and LDPE
matrix. Authors observed that the use of plasmas significantly improves tensile strength and Young’s
modulus. It was determined that the best results for improving the mechanical properties of treated
fibers were obtained for fiber content around 20%. The use of plasma did not change the chemical
composition of fibers, which means that the improvement in adhesion was connected directly to
dehydration and cleaning of the fibers.
The second group of modifications widely described in the literature are chemical modifications.
Their base lies in the fact that natural cellulosic fibers are rich in hydroxyl groups, and most chemical
modifications involve reacting with these groups. Examples of chemical modifications of fibers are
mercerization, acetylation, silanization as well as benzoylation. Mercerization (alkaline treatment)
involves treating the fibers with alkaline solutions such as NaOH at various concentrations and
soaking time. In addition to the removal of lignin, waxes and fatty acids from cell walls, alkaline
treatment increases also the number of reaction centers on the fiber surface as a result of the
hydrogen bonds breaking. Improvement of mechanical properties after applying alkali treatment was
observed by many researchers (Bachtiar, Sapuan, and Hamdan 2008; Ray et al. 2001; Sreekala et al.
2000). However, it is very important to use the optimal concentration and soaking time, since it is
possible to deteriorate the mechanical properties using not appropriate conditions. For example,
Mohd et al. (2011) showed that increasing soaking time from 12 to 24 h decreased the value of
tensile strength. Acetylation involves introducing acetyl group, in the form of, for instance, acetic
anhydride. This causes substitution of hydroxyl groups to acetyl groups and results in plasticization
of fibers, increased adhesiveness as well as reduced hydroscopicity. Many researchers proved the
positive influence of acetylation on mechanical properties of composites with natural fibers (Edith
M. Cadena et al. 2017; Milan, Christopher, and Winowlin Jappes 2018). Silane treatment involves the
reaction of functional groups of fibers with functional groups of organic silicon compounds. Due to
bifunctional groups, which can react with two phases (polymer matrix and fiber filler), forming of a
bridge between them is possible (Xie et al. 2010). Sepe et al. (2018) compared alkaline and silane
treatment on mechanical properties of hemp fiber-reinforced composites. Authors indicated that
hemp-reinforced composites with silane treatment resulted with a greater tensile modulus than
without pretreatment and alkali treatment and the properties. The optimal concentration to improve
mechanical properties was 1% of silane. Benzoylation involves treating the fiber with benzoyl
chloride, which results in replacing hydroxyl groups of the fibers in benzoyl groups. This increases
the hydrophobic properties and improves adhesion of fibers to the matrix. Aside from methods
mentioned above, there are much more techniques described in detail by e.g. Kabir et al. (2012).
The limitation in the case of using natural fiber composites with functionalization during
production process is the fact that material will have a direct contact with food, so in the case of
food packaging it is necessary to choose the appropriate modification method so that it does not
affect the stored food. The suggested modification methods are therefore the physical modifications
previously described that are completely safe for stored food. However, permitted additives for the
production of food packaging and the maximum migration limits are listed in the European
Directive COMMISSION REGULATION (EU) No 10/2011of 14 January 2011on plastic materials
and articles intended to come into contact with food.
Conclusions
Food packaging made of natural fibers/matrix composites are certainly more environmentally
friendly not only due to the introduction of a biodegradable factor, but also due to their specific
properties that allow for a longer shelf-life of the product. Composites based on biodegradable,
renewable raw materials are an attractive alternative to fossil-fuel based plastics, which are
widely used in the packaging industry. The use of fibers in composites for food packaging is
10 Z. SYDOW AND K. BIEŃCZAK
associated with such advantages as, improving gas barrier properties, increasing thermal stability
and in some cases also improving mechanical properties. Due to the hydrophilic properties,
fibers also contribute to the increase of the thickness of the swelling and water absorption,
which is particularly desirable in the case of packaging for high respiring food. On the other
hand, hydrophilic properties reduce their affinity to the hydrophobic polymer matrix, which
involves the need to modify them by chemical or physical methods. Interesting materials that
can be used in the food packaging industry are hybrid materials, such as, nanoclay/natural fibers
filled composites with polymeric matrix. This kind of composite is usually characterized by
combining the advantages of components with the elimination of their disadvantages. Thus, in
addition to ecofriendly benefits and cost reduction, materials with very satisfying mechanical
properties with high barriers properties are obtained, which is desirable not only for food
packaging production, but also in many other applications. Certainly, in the near future,
particular attention should be paid to the necessity to replace fossil-fuel based materials with
biodegradable materials that will significantly contribute to the reduction of environmental
pollution.
List of abbreviations
HDPE high-density polyethylene
LDPE low-density polyethylene
PBS poly(butylene succinate)
PCL polycaprolactone
PE polyethylene
PET polyethylene terephthalate
PHBV poly(3-hydroxybutyrate-co-valerate)
phc parts per hundred compounds
PLA polylactic acid
PLGA poly(lactide-co-glycolide)
PP polypropylene
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