Food Packaging and Shelf Life 17 (2018) 150–161

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Food Packaging and Shelf Life

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

Antimicrobial poly(lactic acid)/cellulose bionanocomposite for food T

packaging application: A review
⁎
Ivy Gan, W.S. Chow
School of Materials and Mineral Resources Engineering, Engineering Campus, Universiti Sains Malaysia, Nibong Tebal, 14300 Penang, Malaysia

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

Keywords: Conventional food packaging materials are derived from nonrenewable fossil resources and face difficulties in
Poly(lactic acid) disposal and recycling. The development of green and ecologically balanced food packaging materials has re-
Nanocellulose ceived much attention as a prospective solution that can partially substitute for the imperishable fossil fuel-
Antimicrobial derived plastic. Polylactic acid (PLA) is known as a promising biopolymer, and the incorporation of nano-
Packaging
cellulose can further enhance the properties of this biopolymer. The combination of PLA and nanocellulose
enables the development of a sustainable eco-friendly food packaging as PLA can be obtained from agricultural
resources and nanocellulose can be extracted from agricultural waste. This critical review demonstrates the
current developments, and the advantages of PLA and nanocellulose for the purpose of food packaging are
introduced. The nanocellulose produced from agricultural waste is summarized along with specific references to
food packaging applications. In addition, the antimicrobial agents used in PLA/nanocellulose-based packaging
are discussed. Overall, greener food packaging with enhanced antimicrobial properties with a suitable combi-
nation of bio-based nanocellulose is highlighted in this review.

1. Introduction have D-glycopyranoside as their building block or repeating unit (e.g.,

The huge consumption of fossil fuel-derived plastic material has
created consistent waste production issues that cause environmental
pollution (Han, Yu, & Wang, 2017). In 2015, the global plastic market
reached 322 M tons, and approximately 49 M tons of plastics are uti-
lized for packaging purposes. Owing to the inappropriate disposal and
nonbiodegradability of these petroleum plastics, 4.8–12.7 M tons of
plastics ended up in ocean in the year of 2010, and more than 30% of
the plastic waste was land-filled in the year 2014. Consequently, the
recycling of plastic has become an encouraging option to abate the
accumulation of plastic waste in our environment. However, this re-
cycling system does not work on food packaging systems because of the
contamination of organic substances that is found on the food packa-
ging plastics (Ingrao, Gigli, & Siracusa, 2017). Hence, food packaging
producers should not only consider the factor of maintaining the ef-
fectiveness of the quality of food but also the environmental impact
with regards to the disposal of packaging materials. For this reason,
biopolymers have received widespread attention due to their biode-
gradability, and the biopolymers are able to replace the fossil fuel-based
plastic materials and address the waste disposal problem (Adilah,
Jamilah, Noranizan, & Hanani, 2018; Rhim, Park, & Ha, 2013).
Biopolymers can be divided into four categories: [i] polymers that
starches, cellulosic and ligno-cellulosic); [ii] polymers acquired through
microbial sources (e.g., polyhydroxyalkanoates (PHAs) that include the
polymer of poly(hydroxybutyrate) (PHB) and polyglycolic acid (PGA));
[iii] polymers that are chemically synthesized from agroresources (e.g.,
polylactic acid (PLA)) and [iv] polymers that are chemically synthe-
sized from fossil fuel resources (e.g., polycaprolactones (PCLs) and poly
(butylene succinate adipate) (PBAT)) (Elsawy, Kim, Park, & Deep,
2017; Souza & Fernando, 2016).
Among all these biopolymers, poly(lactic acid) (PLA) has been
employed for packaging purposes attributable to the ability of this
aliphatic polyester to be derived from renewable agricultural resources
in the way that its monomer can be generated by the fermentation of
agricultural resources (Tiimob et al., 2018). The bio-based character of
PLA would contribute to the diminution of ecological impacts corre-
lating with the extensive utilization of conventional plastics derived
from nonrenewable fuel sources (Lizundia et al., 2016).
2. Food packaging application
2.1. PLA for food packaging applications
The life cycle production of PLA begins with starch that is extracted

⁎
Corresponding author.
E-mail address: shyang@usm.my (W.S. Chow).

https://doi.org/10.1016/j.fpsl.2018.06.012
Received 13 February 2018; Received in revised form 8 June 2018; Accepted 26 June 2018
2214-2894/ © 2018 Elsevier Ltd. All rights reserved.
I. Gan, W.S. Chow
from plants such as corn. During the growth of the corn, the carbon
dioxide is harnessed from the environment for photosynthesis.
Throughout the photosynthesis process, consumption of free energy
originating from solar energy and carbon dioxide will take place in the
corn plant to convert glucose into starch, contributing to chain building
for PLA. Therefore, the benefit of PLA production compared with other
commercial polymers is the ability to reduce carbon dioxide (CO2)
emissions, suggesting that PLA also has the potential to reduce en-
vironmental pollution compared to the other conventional plastics
(Vink, Glassner, Kolstad, Wooley, & O’Connor, 2007).
The building block for PLA is lactic acid, which can be obtained
through the fermentation of maize or other sustainable agricultural raw
resources (Abdulkhani, Hosseinzadeh, Ashori, Dadashi, & Takzare,
2014). A few appealing things about PLA are biocompatibility, pro-
cessability, renewability and less energy consumption (Rasal, Janorkar,
& Hirt, 2010). In comparison with biopolymers such as poly(hydro-
xyalkanoates) (PHAs) and poly(ethylene glycol) (PEG), the good
thermal processability of PLA means it can be manufactured through
various processing methods such as extrusion, film casting and fiber
spinning (Rhim, Mohanty, Singh, & Ng, 2006). Because of the biode-
gradable and biocompatible characteristics of PLA, it received approval
from the Food and Drug Administration (FDA) in the applications with
food contact and became an adequate candidate for the application of
packaging for fresh food or short service life goods, including over-
wrapping, lamination filming and blister packaging (Ingrao et al.,
2017).
PLA can be available in different molecular weights. However, only
PLA with high molecular weight will be selected for use in the packa-
ging industry. There are two main PLA industrial manufacturers, which
are NatureWorks LLC and Corbion, and both of these manufacturers are
using ring opening polymerization to produce PLA. The ring opening
polymerization with rapid reaction time and comparatively mild reac-
tion conditions was able to yield PLA with high molecular weight while
having a smaller molecular weight distribution (Hamdan & Sonomoto,
2011). In 2003, massive production of PLA was recorded under the
tradename of Ingeo. Approximately 150 M tons of PLA (Ingeo) were
manufactured by NatureWorks LLC every year via the process of ring
open polymerization (Ingrao et al., 2017).
According to Lovett and de Bie (2016), the Corbion manufacturer
was employing the highest yielding feedstock locally available to pro-
duce PLA, in such a way that raw sugar originating from cane in Brazil
and Thailand, and raw sugar originating from the sources of sugar beets
in Spain and the Netherlands are used as a feedstock to generate the
monomer of PLA. Instead of using raw sugar, USA is using dextrose
from corn to produce lactic acid. By taking a closer look on the feed-
stock efficiency, PLA can be considered the most efficient biopolymer
because the yield of 1 kg of PLA only required approximately 1.6 kg of
fermentable sugar feedstock. In comparison with the other biopoly-
mers, approximately 2.5–3 times more sugar feedstock was needed to
produce 1 kg of plastic. In addition, by considering the factor of land
use, the land use per ton of bio-based polymer from five crops (i.e.,
maize, wheat, sugar beet, sugarcane and miscanthus) for current agri-
cultural practices was compared in the Lovett and de Bie (2016) study.
PLA produced from either sugarcane or sugar beet is an ideal biopo-
lymer that can be used in food packaging applications as it only occu-
pies approximately 0.12 ha/ton (land use per ton), compared to bio-
based polyethylene (PE), which needs approximately 0.32 ha/ton.
In addition, the unique properties of PLA are comparable to poly-
olefin and poly(ethylene terephthalate) (PET), and these compounds
can be used in a broad range of applications. Overall, the properties of
PLA were almost similar to polystyrene (PS) as PLA has a low value for
elongation at break of approximately 2–5% and a high Young’s
Modulus, which is approximately 3 GPa (Spinella et al., 2015). In
summary, PLA can be recommended as a good candidate for the ap-
plication of food packaging, including in its functional properties, for
example, high transparency, good barrier properties, good sealability,
151
Food Packaging and Shelf Life 17 (2018) 150–161
good oil and grease resistance and excellent organoleptic characteristics
(Gruber, 2001).
2.2. Nanocellulose for food packaging applications
2.2.1. Nanocellulose
Nanocellulose can be depicted as a biodegradable nanomaterial
because cellulose is sustainable, renewable, recyclable, nontoxic and
produces a low carbon footprint (Dufresne, 2017). Cellulose accounts
for approximately 35%–50% of the total composition of natural fibers
and thus significantly influences the chemical properties of natural
plant fibers. Plants produce approximately 75 billion tons of cellulose
per year, making cellulose biopolymers inexhaustible (Feng et al.,
2018). The general formula for cellulose is (C6H10O5)n, and cellulose
represents the major component in vegetable tissue. In nature, cellulose
is seldom available in its pure state. Nonetheless, cellulose is mostly
intimately mingled with coloring matter, fats, gums, hemicellulose,
lignin, tannins, etc. The 1,4-glycosidic bonds linking the cellulose and
β-glucopyranoside residues were used to express the prime structure of
cellulose. The cellulose consists of a linear polymer which is known as
an anhydroglucose unit. The β-glucosidic bond plays an important role
in linking the anhydroglucose units together at carbon atoms one and
four. In general, the degree of polymerization of cellulose depends on
the extraction source and can be very high (up to 20,000 residues
within a chain). Cellobiose residue is recognized as a cellulose repeating
unit rather than glucose residue, as the residues within the cellulose
have a rotation of 180° relative to each other (Candido, Godoy, &
Gonςalves, 2017).
Intramolecular and intermolecular hydrogen bonding is responsible
for the stabilization of the ordering of cellulose chains, which in turn
leads to the formation of compact microfibrils. The hydrogen bonding is
actually responsible for the stabilization of the thermal properties of
cellulose since the existence of this bonding prevents cellulose from
melting before thermal degradation. Moreover, these bonds cause the
cellulose to become insoluble in almost all of the solvents by reason of
considerable tensile strength that is imparted by the bonds on the cel-
lulose. In addition, the cellulose can form thin and long fibrils by
grouping approximately 100 cellulose chains together, and these fibrils
are made up of two parts that are amorphous and crystalline, respec-
tively (de Oliveira, Bras, Pimenta, da Silva Curvelo, & Belgacem, 2016;
Hoi & Martincigh, 2013; Moubarik, Grimi, & Boussetta, 2013). The
connections for both regions of crystalline and amorphous parts execute
important roles as their relationship determines the dimensional char-
acteristics of the crystalline domains as well as the degree of crystal-
linity of the cellulose (Leão, Miléo, Maia, & Luz, 2017).
Three types of nanocellulose have been utilized as key components
for the application of cellulose-derived packaging. These types are
cellulose nanocrystals (CNCs), bacterial nanocellulose (BNC) and na-
nofibrillated cellulose (NFC). Division of these nanocelluloses depends
on their size, synthesis method, function and source. The CNCs are the
archetypal cellulose that has a low aspect ratio, with diameters of ap-
proximately 5 nm and a length of 100–250 nm. The degree of crystal-
linity in CNCs can be high, and sometimes this degree of crystallinity
can achieve 90%. The CNCs mostly can be synthesized by acid hydro-
lysis. Commonly, sulfuric hydrolysis of cellulose results in cellulose
nanocrystals (CNCs) with needle-shaped crystals with diameters within
the range of 10–20 nm and the length of approximately 100 nm. CNF
usually has a higher aspect ratio and a web-like structure. The diameter
of CNF is usually in the range of 5–60 nm, and its synthesis methods
include grinding, high pressure homogenizing, high pressure micro-
fluidization and high intensity ultrasonication. For the preparation of
BNC, the molecule is normally synthesized by microorganisms, re-
sulting in highly crystalline cellulose with a high degree of poly-
merization. However, this kind of synthesis method is usually very
expensive (Feng et al., 2018).
In comparison with CNFs, CNCs tends to offer better elongation
I. Gan, W.S. Chow Food Packaging and Shelf Life 17 (2018) 150–161

properties because CNFs is more susceptible to fiber agglomeration due
to its larger aspect ratio which causes it to be more prone to en-
tanglements. The smaller size of CNCs has less of an effect on the
transparency, and this could be one of the advantages for the applica-
tion to food packaging in which transparency is one of the important
criteria (Azeredo, Rosa, & Mattoso, 2017; Ferrer, Pal, & Hubbe, 2017).
The gas dissolution and diffusion rate will affect the permeability of
gas through the film of nanocellulose. The dense network structure of
the nanofibrils within the nanocellulose contributes to its good oxygen
barrier properties. Among those three types of nanocellulose, CNCs has
the highest degree of crystallinity due to the production method which
involves the strong acid hydrolysis that is capable of hydrolyzing dis-
ordered and amorphous cellulose. The remaining ordered crystalline
region of cellulose will then be responsible for forming the gas molecule
barrier. Despite the crystalline regions of cellulose being impermeable
to most molecules, this characteristic enhances the effective flow path
within the cellulose regardless of gas, air or water molecules. The extent
of the tortuosity of nanocellulose for the reduction of the permeability
of gas molecules through biocomposite films is a topic that is worthy of
further studies (Ferrer et al., 2017).
Table 1 shows different sources of extraction of CNCs that is utilized
in food packaging. Based on Table 1, there are two types of waste ca-
tegories for the classification of these cellulose sources. The lig-
nocellulosic residues obtained directly from agriculture will be cate-
gorized as nonprocessed waste whereas the waste produced through
industrial activities will be known as processed waste (García, Gandini,
Labidi, Belgacem, & Bras, 2016). Table 2 offers the overview of the
extraction of nanocellulose from different plant sources that are em-
ployed in food packaging. The properties (e.g., mechanical, thermal,
optical, barrier) of polymer/nanocellulose composites are controlled by
several factors, including (i) the types of nanocellulose extracted from
different resources (sugarcane bagasse, empty fruit bunches, sweet
potato, mulberry, seaweed, rice straw, wheat straw, corn cob, etc.), (ii)
the loading of the nanocellulose (appropriate and optimum loading give
significant improvement in the properties, while excessive loading leads
to agglomeration and diminishes the properties of enhancement), and
(iii) suitable “blending” of polymer and nanocellulose (polymers with
good miscibility and compatibility with nanocellulose will always ex-
hibit good thermal and mechanical properties). Furthermore, a suitable
amount of nanocellulose being placed into the selected polymer (PLA,
PVA, starch-chitosan film) is important to ensure that the optical
properties (i.e., clarity and transparency) of the polymer/nanocellulose
biocomposites could be maintained, to fulfill some of the packaging
requirements.
2.2.2. Nanocellulose from agricultural waste
Recently, agricultural residue or waste emerged as a good candidate
for the extraction of nanocellulose. The annual global production on the
dry mass basis of the biomass is approximately 220 billion tonnes, and
approximately 10–13 tonnes of dry biomass per hectare per annum
were harvested. Despite the easy availability of this agricultural re-
sidue, most of the agricultural residues were used to direct combustion,
which causes a serious burden to the environment. The gases produced
during the direct combustion of biomass were estimated to be ap-
proximately 5.6 kg of hydrocarbon, 9.2 kg of methane, 111.3 kg of
carbon monoxide, 1599 kg of carbon dioxide and 4.8 kg of particulate
matter per tonne of dry biomass combustion. Thus, a better way to
utilize this residue is convert this biomass into beneficial products such
as nanocellulose (Islam, Kao, Bhattacharya, Gupta, & Choi, 2017).
The worldwide forestry and agricultural activities and abundant
availability of agricultural residue or waste could be a promising
feedstock to synthesize nanocellulose. Using lignocellulosic biomass
originating from the source of agricultural residues to synthesize na-
nocellulose not only ameliorates the disposal issues in the environment
but also provides profits in terms of waste treatment or residue man-
agement (García et al., 2016).
Based on the information provided in the work of Bentsen, Felby,
and Thorsen (2014) and in accordance with the database provided by
the Food and Agriculture Organization of the United Nations (FAO),
globally important agricultural crops in terms of production quantities
are made up of 6 types, which include sugarcane, wheat, barley, rice
and soybeans. The world’s arable land is approximately 1411 million
ha. The harvested area for all these crops occupies up to 702 million ha,
which covers almost half of the arable land in the world. Their studies
also found that approximately 3.7 Pg of dry matter per year of residues
are produced from these crops globally. Hence, agricultural residues
can become a promising renewable resource used to synthesize nano-
cellulose due to the enormous production volume.
2.2.2.1. Sugarcane bagasse nanocellulose. The reduction in
nonrenewable natural resources following widespread attention to
pollution concerns has inspired researchers to develop new materials
employing natural polymers, resulting in bio-based materials that can
be synthesized from lignocellulosic materials gradually taking over

Table 1
Cellulose nanocrystals (CNCs) utilized in food packaging from various sources of extraction.
Waste Category Cellulosic Isolation Technique Reference

Processed waste Cotton Acid Hydrolysis (H2SO4) Thambiraj and Shankaran (2017)
Sugarcane Bagasse Acid Hydrolysis (H2SO4) El-Samahy, Mohamed, Rehim, and Mohram (2017), El Alchaby et al.
(2017) and El Miri et al. (2016)
Empty fruit bunch Acid Hydrolysis (H2SO4) Salehudin, Salleh, Mamat, and Muhammad (2014)
Ramie Acid Hydrolysis (H2SO4) Li, Chen, and Wang (2015)
Sweet potato Acid Hydrolysis (H2SO4) Lu, Gui, Zheng, and Liu (2013) and Ma et al. (2017)
Coffee Silverskin Acid Hydrolysis (H2SO4) Sung, Chang, and Ham (2017)
Red algae waste Acid Hydrolysis (H2SO4) El Achaby, Kassab, Aboulkas, Gaillard, and Barakat (2018)
Seaweed Acid Hydrolysis (H2SO4) Singh, Gaikwad, and Lee (2018)
Bleached kraft bagasse pulp, softwood Acid Hydrolysis (H2SO4) El-Wakil, Hassan, Abou-Zeid, and Dufresne (2015) and Zhang, Jung,
kraft pulp and Zhao (2017)
Wheat Straw Acid Hydrolysis (H2SO4) Oun and Rhim (2016) and Pereira et al. (2017)
Banana peels; Banana pseudostem Acid Hydrolysis (H2SO4); Tempo- de Oliveira et al. (2017) and Faradilla et al. (2017)
mediated oxidation
Phormium tenax (flax), Flax (Linus Acid Hydrolysis (H2SO4); Acid Fortunati, Puglia et al. (2013), Fortunati, Luzi et al. (2014), and
usitatissimum) Hydrolysis (HCl) Mujtaba et al. (2017)
Mulberry Acid Hydrolysis (H2SO4) Reddy and Rhim (2014) and Wang, Shanker, and Rhim (2017)

Non-processed waste Actinidia deliciosa pruning residue Acid Hydrolysis (H2SO4) Luzi, Fortunati, Giovanale et al. (2017)
Rice husk Acid Hydrolysis (H2SO4) Kargarzadeh et al. (2017)
Barley straw and husk Acid Hydrolysis (H2SO4) Fortunati et al. (2016)
Oat husk Acid Hydrolysis (H2SO4) Qazanfarzadeh and Kadivar (2016)

152
 Table 2
Examples of nanocellulose isolated from various plant sources that are applied for application of food packaging.
Sources of isolated cellulose nanocrystals Matrix Loading Properties Reference
(CNCs)
I. Gan, W.S. Chow

Sugarcane Bagasse Starch film 3% There are reduction in surface hydrophilicity and improvement in water vapour barrier Slavutsky and Bertuzzi (2014)
properties with the introduction of CNCs.
Sugarcane Bagasse Polyvinyl alcohol/ carboxymethyl 0.5–10 wt % 5 wt % CNCs showed increased in tensile modulus and strength. Showed positive effect in El Alchaby et al. (2017)
cellulose (PVA/CMC) water vapour permeability.
Sugarcane Bagasse (linear or crosslinked) PVA 0–10 wt% Remarkable improvement in tensile strength, elongation at break, yield force and Mandal and Chakrabarty (2014)
toughness. Enhanced thermal stability and barrier property was observed.
Sugarcane Bagasse / GON (graphene PVA 5wt % Young modulus, tensile strength and toughness was enhanced. Tg, Tm and moisture El Miri et al. (2016)
oxide) (hybrid nanofiller) sorption was also showing improvement.
Sugarcane Bagasse CMC/Starch 0.5–5.0 wt % Exhibited good optical transparency, reduced water vapour permeability and enhanced El Miri et al. (2015)
tensile properties.
Empty fruit bunches Starch-Chitosan 2–10% The tensile strength of starch-chitosan film increased 32.5% by adding 2% CNC. Salehudin et al. (2014)
Phormium tenax leaves PLA 1–3 wt% The addition of CNCs enhanced the thermal stability of PLA and does not affect the Fortunati, Luzi et al. (2014)
transparency of the PLA.
Linus usitatissimum Chitosan 5, 10, 20 and 30% The CNCs incorporation does not show improvement in the thermal stability and water Mujtaba et al. (2017)
vapour permeability of chitosan film but affect the transparency of film by turning
yellowness when the content of CNCs increased.
Ramie PVA/Chitosan 5, 10, 15, 20 and 25% Improvement of mechanical properties, oxygen barrier properties and antimicrobial Li et al. (2015)
activities was observed.
Sweet Potato Cassava starch 2,4,6,8 and 10 wt% Carboxymethyl cellulose nanocrystals (N-CMCs) were produced and N-CMCs/cassava Ma et al. (2017)
starch film with 0.4 g/100 mL shown enhancement in tensile strength and elongation at
break as compared to untreated CNCs/cassava starch film. Better water vapour
permeability and moisture absorption of the N-CMCs/ cassava starch film was also
observed.
Mulberry Agar 1, 3, 5 and 10 wt% The mechanical and water vapour barrier properties of the agar/CNC composite showed Reddy and Rhim (2014)

153
improvement when the CNCs content was below 5 wt%.
Mulberry Alginate 2,4 and 6 wt% The water vapour permeability of the resulted composite was enhanced however the Wang et al. (2017)
mechanical properties of the film improved only up to 4 wt% loading of mulberry CNCs.
Actinidia deliciosa pruning residue PVA/ Chitosan 3 wt% The incorporation of CNCs does not affect the transparency of both PVA and PVA/ Luzi, Fortunati, Giovanale et al.
Chitosan film but enhanced the mechanical properties of the composite film. (2017)
Coffee Silverskin PLA 1, 3 and 5 wt% All the nanocomposites film showed excellent oxygen barrier. The Young’s modulus and Sung et al. (2017)
tensile strength of nanocomposite film was enhanced with the incorporation of 1% and
3% CNCs. The water vapour permeability showed improvement up to 3% of CNCs.
Red algae waste PVA 1, 3, 5 and 8 wt% The 8 wt % of CNCs enhanced the PLA composite film with Young’s modulus by 215%, El Achaby et al. (2018)
tensile strength by 150% and toughness by 45%.
Seaweed PVA 5% (w/v) The introduction of 5% CNCs to PVA showed improvement in tensile strength, water Singh et al. (2018)
vapour permeability and thermal stability.
Bleached kraft bagasse pulp Wheat gluten 2.5,5, 7.5,10 and The optimal loading of CNCs and TiO2 was found to be 7.5% and 0.6%. The wheat gluten El-Wakil et al. (2015)
12.5% composite with these loading was having significant improvement in tensile strength and
water resistance.
Softwood kraft pulp poly(3-hydroxybutyrate-co-3- 10 wt% The CNCs acts as heterogeneous nucleation agent in PNBV that promote crystallization Zhang et al. (2017)
hydroxyvalerate) (PHBV) rate. The CNCs had improved the tensile strength by 51.7%, and Young’s modulus by
97.9% whereas the elongation at break was showing reduction to 2.0%.
Wheat straw Carboxymethyl cellulose 5 wt% The 5 wt% of CNCs increased the tensile strength of the composite by 25.2% and reduced Oun and Rhim (2016)
the water vapour permeability by 19.1%.
Wheat straw Wheat straw hemicelluloses 0–8 wt% The studies show the optimal loading of CNCs and citric acid in the composite is 5.9 wt% Pereira et al. (2017)
and 30 wt% respectively in which having the least water sensitivity and permeability,
enhanced modulus, water resistance and elongation.
Rice straw Carboxymethyl cellulose 5 wt% The 5 wt % of CNCs increased the tensile strength of the composite by 45.7% and reduced Kargarzadeh, Johar, and
the water vapour permeability by 26.3%. Ahmad, 2017
Rice husk Starch 2%, 4%, 6%, 8%, and The CNCs had enhanced the thermal stability, tensile properties, storage modulus and Kargarzadeh et al. (2017)
10% reduced the water uptake of the starch biocomposite.
Banana peels Pectin 0, 2.5, 5, 7.5, and de Oliveira et al. (2017)
10 wt%
(continued on next page)
Food Packaging and Shelf Life 17 (2018) 150–161
I. Gan, W.S. Chow Food Packaging and Shelf Life 17 (2018) 150–161

some of the fossil fuel-derived products and growing into ideal

resources for natural cellulosic products. These lignocellulosic

Qazanfarzadeh and Kadivar

Thambiraj and Shankaran

materials are available in abundance as they can be obtained

Fortunati et al. (2016)

Silvério et al. (2013a)

effortlessly from agricultural residues, can be substituted in a shorter
time and are biodegradable. Reports show that the worldwide
agricultural by-products from dominant commodity crops such as
sugarcane, soybean and rice has reached approximately over 2
Reference

(2016)

(2017)
thousand million tons or more per year (Abdel-Halim, 2014).
In addition, these lignocellulosic materials can be great sources for
the replacement of the traditional synthetic fibers with respect to its
of CNCs. The optimal loading of oat husk isolated CNCs was found to be 5 wt% by having

permeability had reduced to 28% with the addition of CNCs. The transparency of the film

had yield about 45% which is suitable for industrial scale up process. The CNCs does not
was not affected by the addition of CNCs and no significant change in tensile strength of

The isolated CNCs was having high aspect ratio and the synthesis method in this research

affect the transparency of the film and had resulted a high transparency and flexible PVA
properties, water vapour and water resistance properties. However, the resulted film still

The film transparency and water vapour permeability were reduced with the introduction
The transparency of the film was reduced by chitosan. The enzymatic treatment extraction

cost, specific properties, density, minimal health hazards, advantageous

The ultimate tensile strength of the film had enhanced up to 140% and water vapour
Chitosan/CNC ternary system showed inhibition on the development of bacterial and
consider having quite high water solubility which made the film more applicable in

aspect ratio, less resulting machine wear and flexibility during pro-
The composite film with 5 wt% of CNCs was found to have improvement in tensile

of CNCs was improving the optical, mechanical and thermal properties. The PVA/

cessing (Mulinari, Voorwald, Cioffi, da Silva, & Luz, 2009; Cerqueira,

Baptista, & Mulinari, 2011). Lignocellulosic materials have distinct
the highest Young’s modulus, tensile strength and lowest moisture content.

origins such as wood, bark, cotton, bamboo, bagasse, rice straw, etc.
(Agunsoye & Aigbodion, 2013; Leão et al., 2017)
secondary packaging that does not require high water resistance.

According to Ng et al. (2015), various types of tropically grown

plants require washing pretreatment before the fiber can be subjected
to prealkaline treatment. Sugarcane and cotton are examples of fibers
that do not require any washing pretreatment, making the extraction of
composite film which is suitable for food packaging.

nanocellulose from both of these fibers more preferable compared with

other fibers. The washing pretreatment is an important procedure as it
can remove dirt and waxy substances on the fiber. These impurities
would restrict the contact between the cellulose fiber and the alkaline
solution, eventually leading to inefficient delignification and chemical
treatment on the fibers.
Sugarcane bagasse (SCB) can be used as an economical industrial
feedstock as SCB can serve as a viable material in manufacturing bio-
the film was observed.

based products (de Oliveira et al., 2016). The difference between su-
garcane bagasse and other agricultural crops is that the plantations of
sugarcane are popular for their volume of production and enormous
Properties

amounts of residues. In the country of Brazil, the sector for sugarcane

fungal.

has increased in production since the year 2000. In addition, in com-

parison with the other countries, Brazil is ranked in the first place with
regard to the greatest production of sugarcane as approximately 632
million tons were manufactured in the 2014/2015 season. Meanwhile,
2.5, 5 and 7.5 wt%

in the country of Thailand, the yield of both sugarcane and bagasse was
3, 6 & 9 wt%

reported as 94 million tonnes and 26 million tonnes during 2015/2016,

1 & 3 wt %

respectively. The total annual production of bagasse around the world

Loading

5 wt%

was approximately 54 million dry tons. However, bagasse is re-

generated to become fuel for sugar factories most of the time. Almost
more than half of the weight of bagasse is cellulose, which is currently
considered a valuable renewable material (Lam, Chollakup,
Poly(vinyl alcohol) (PVA) blended with

Smitthipong, Nimchua, & Sukyai, 2017; Mulinari et al., 2009).

Furthermore, sugarcane is considered the largest harvested crop in
the world as sugarcane is planted in more than 100 countries, making
Whey protein isolate (WPI)

sugarcane a potential feedstock as it can be grown and harvested

natural chitosan (CH)

throughout the year, and its bagasse can also be stored and stacked for a
long period of time (Phinichka & Kaenthong, 2018). The recent fall in
the worldwide price for sugar in the year 2012 and the issue of a surfeit
supply and stockpiling in Brazil has also created another reason to make
sugarcane bagasse into a sustainable material (Candido et al., 2017; Hoi
Matrix

PVA

PVA

& Martincigh, 2013). In the matter of continuous development, su-

garcane bagasse has received much attention due to its bountiful
Sources of isolated cellulose nanocrystals

availability and strong interest in inexhaustible sources for the synth-

esis of polymer composites with excellent mechanical properties. In-
deed, considerable enthusiasm for the generation of new composite
materials from sugarcane bagasse fibers with enhanced properties can
be found in major industries involving packaging.
Industrial waste cotton
Barley straw and husk

Sugarcane bagasse (SCB) is a cellulose-rich solid waste that is gen-

Table 2 (continued)

erated during sugar production. The bagasse can be obtained from su-
garcane stems after the juice has been extracted (Candido et al., 2017;
Lam et al., 2017). Sugarcane bagasse comprises three components
Corn corb
Oat husk

(cellulose, lignin and hemicellulose), which amalgamate in a composite

(CNCs)

tissue (de Oliveira et al., 2016). The glucose polymer cellulose con-
tributes approximately 40–50% of the bagasse, mainly in a crystalline

154
I. Gan, W.S. Chow
structure. The hemicellulose that is an amorphous polymer makes up
approximately 25–35% of the bagasse, and this hemicellulose often
comprises arabinose, mannose, glucose, galactose and xylose. The re-
maining components are in small fractions, approximately 2.4% ashes,
mineral and wax. The lower ash content compared to other agricultural
crops suggests that bagasse can be a potential lignocellulosic source for
nanocellulose extraction (Hossain et al., 2014; Moubarik et al., 2013).
The general chemical route for the extraction of nanocellulose from
sugarcane bagasse consists of the following steps: 1) opening the lig-
nocellulosic structure through the pulping process, 2) a pretreatment
process to eliminate hemicellulose and lignin to obtain cellulose, and 3)
strong acid hydrolysis (de Oliveira et al., 2016). After a series of ade-
quate purification processes, the availability of lignin within the ba-
gasse will be reduced to approximately 42%, making sugarcane bagasse
a perfect feedstock to extract nanocellulose (Phinichka & Kaenthong,
2018).
Therefore, the feasibility of undergoing chemical treatment for the
extraction of fiber and cellulose makes SCB a potential ingredient to be
utilized as a reinforcement material to develop green products that
possess desired physical and chemical properties. SCB can show sig-
nificant improvement in mechanical properties after appropriate mod-
ification is applied, showing that SCB can become an ideal candidate to
enhance the properties of green composites. Two factors, which are the
availability of SCB originating from the industry of sugar processing
and the inexpensive pretreatment and chemical extraction process,
have favoured the utilization of SCB in generating green products with
enhanced properties. As the demand for green food packaging is getting
higher, SCB is a good option to be incorporated into biopolymers to
develop a biocomposite suitable for food packaging application, which
satisfies the greening requirement by having the property of biode-
gradability (Loh, Sujan, Rahman, & Das, 2013).
2.2.2.2. Corn nanocellulose. Corn is one of the most famous crops as
most of the cereals produced in the world are produced from maize
(Boufi & Chaker, 2016; Silvério, Neto, Dantas, & Pasquini, 2013a).
Today, the corn yield grows gradually with the aid of agricultural
science and technology (Yang et al., 2017). The annual corn production
in the industrial segment is approximately 12.7 million tons between
the years 2011 and 2012. In 2013, the Food and Agricultural
Organization of the United Nations reported that the world-wide
output for maize has reached approximately 1 trillion tonnes.
According to Liu et al. (2016), the United States Department of
Agriculture reported that more than 900 million metric tons of corn
were produced globally in 2014. Therefore, the increased production of
the corn has led to the abundance of agricultural corn stalks as the by-
product of corn (Cheng, Yang, Liu, Liu, & Chen, 2017).
Generally, the ears of the maize are the important resources for food
production as the maize is used to generate a wide range of industrial
products such as vegetable oils, starch, animal feed and so on. However,
not all parts of the maize plant are fully utilized, and some parts of the
plant remain underutilized (Boufi & Chaker, 2016; Smyth, García,
Rader, Foster, & Bras, 2017). The cultivation of corn produces the by-
product or agricultural residue known as corn stover, which consists of
stalk, leaves and husk. Corn stover is composed of approximately 56%
stalk, 21% leaves, 15% cobs and 8% husk (Mourtzinis, Arriaga,
Balkcom, & Price, 2015). However, this agricultural residue is usually
undervalued and utilized in products such as material for incineration
or animal feed. Furthermore, the reuse of this agricultural residue does
not cause any negative impacts on food supplies but improves the
economy of rural areas as well as solve the issues of waste accumulation
in the environment (Silvério, Neto, & Pasquini, 2013b). Corn is there-
fore a potential biomass that can be converted into high-value bio-
products such as cellulose nanocrystals.
In general, corn stover comprises cellulose in the range of 28–44%,
23–28% of hemicellulose and approximately 12–16% of lignin (Cheng
et al., 2017; Rehman et al., 2014). According to work done by Costa
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Food Packaging and Shelf Life 17 (2018) 150–161
et al. (2015), corn stover is composed of approximately 45.5% cellu-
lose, 27.6% hemicellulose and approximately 6.77% lignin. Costa et al.
(2015) also showed that sulfuric acid can extract the CNCs from corn
stover with a yield of 64% and the resulting CNCs has a 55.04% degree
of crystallinity and aspect ratio (length/diameter = L/D) of 54.7 ± 24.
In addition, there are many parts of the corn stover that can be utilized
as a source to extract nanocellulose, especially its stalks, cobs and
husks. Each of these parts is extensively characterized as each is com-
posed of different percentages of cellulose content.
The agricultural residue corn stalk makes up the major portion of
the corn stover, and forms of underutilization such as burning as
compost have led to haze issues (Cheng et al., 2017). The composition
of untreated corn stalks consists of 33.3% hemicellulose, 29.8% cellu-
lose, 16.65% lignin, 8.5% ash and 11.75% other compounds (Shawky,
Mahmoud, Ghazy, Asker, & Ibrahim, 2011). Mtibe et al. (2015) used
sulfuric acid to isolate both CNFs and CNCs from corn stalk residue to
produce nanopapers. Through their research, CNCs was proven to have
a higher degree of crystallinity compared with CNFs, resulting in CNCs
nanopapers having better transparency than the CNFs nanopapers.
The husks of the maize are usually used in the application of pre-
venting erosion or manufacturing insulating materials or papers.
Cellulose nanocrystal isolated from the maize husks could add value to
this agricultural residue, and thus this application receives great in-
terest from researchers. According to Smyth et al. (2017), the maize
husk is composed of 78.86% hemicellulose, 43.14% α-cellulose, 23%
lignin and 0.76% ash. Smyth et al. (2017) also reported the successful
extraction of CNCs from maize husks by using sulfuric acid. The ex-
tracted CNCs had a length of 940 ± 70 nm, width of 6 ± 2 nm, and a
high aspect ratio of approximately 157.
The corncob is depicted as the central core of the ear of maize, and it
is the place where the kernels grow. This corncob usually will be con-
sidered waste once the kernels have been removed (Silvério et al.,
2013b). The corncob is commonly used as a potential biomass feedstock
and as an energy resource that is applicable in gasification systems for
energy production. Approximately 18 kg of corncob is generated for
every 100 kg of ears of maize. Between 2010 and 2011, Brazil harvested
approximately 58 million tons of maize, resulting in the production of
corncob reaching approximately 10.4 million tons (Costa et al., 2015;
Silvério et al., 2013a). Corncob is composed mainly of 37.2% hemi-
cellulose, 48.1% cellulose and 14.7% lignin (García et al., 2016). The
corncob residue usually would be in a porous structure after the
hemicellulose is hydrolyzed, making corncobs more susceptible to cel-
lulose extraction with the potential to be promoted as a basic material
to synthesize nanocellulose. According to Liu et al. (2016), four dif-
ferent types of approaches have been taken for the isolation of cellulose
nanocrystals from corncobs: pulp refining, TEMPO-mediated oxidation,
sulfuric acid and formic acid hydrolysis. Their studies showed that
formic acid hydrolysis resulted in cellulose nanocrystals that are longer
in length, with better thermal stability and capable of forming crystals
compared to sulfuric acid hydrolysis.
2.2.2.3. Wheat nanocellulose. One of the most widespread crops around
the world is cereal, and its world production reached 2707 million tons
in 2014. Wheat, corn, oats and barley are the main contributors to
cereal production (Espinosa, Sánchez, Otero, Domínguez-Robles, &
Rodríguez, 2017). The latest estimation for the world production is
approximately 2531 million tonnes, and 29% of its production is
accounted for wheat (Domínguez-Robles et al., 2017).
The worldwide statistic for wheat consumption increases gradually
with each subsequent year. Between 2013 and 2014, the worldwide
wheat consumption was recorded at approximately 705 million and in
the year 2015/2016, the record for wheat consumption rose to 710
million tons. The coproduct of a wheat crop is wheat straw and bran,
which are also plentiful. Generally, 1.3 kg of wheat straw will be gen-
erated for every 1 kg of wheat grain produced, and the world produc-
tion of wheat straw is estimated to be approximately 920 million tons
I. Gan, W.S. Chow
annually. The large amounts of wheat straw are usually employed in
paper production, animal feed, discarded as waste or even burned in the
field, which causes air pollution. Thus, this abundant source could be
used to extract nanocellulose to produce green materials (Azeredo
et al., 2015; Pereira et al., 2017; Sánchez, Espinosa, Domínguez-Robles,
Loaiza, & Rodríguez, 2016).
Wheat straw consists mainly of cellulose in the range of 30 to 40%,
approximately 20 to 35% hemicellulose and lignin with 15 to 25%
(Ruiz et al., 2013). According to the studies done by Sun, Xu, Sun,
Fowler, and Baird (2005), the optimum yield of cellulose (40%) can be
isolated from wheat straw by employing pretreatment through steam
explosion followed by post-treatment with alkaline peroxide because
the treatment with steam explosion promotes considerable reduction
for hemicellulose whereas the alkaline peroxide treatment can dissolve
the lignin, which leads to an increase in cellulose crystallinity.
2.2.2.4. Barley nanocellulose. The total grain barley production is
approximately 150 million tons with approximately 10% originating
from Northern America, approximately 20% from Eastern Europe, 40%
from the European Union, and 30% in temperate regions, making
barley the fourth most popular cereal in the world. The grain barley is
used mainly in the application of malting and brewing or as animal
feed. Barley grain is usually husked, and both barley straw and barley
husks become crop residue. Barley straw is generated after the barley
grain is harvested, whereas barley husk is a by-product in brewing
industries. Both these agricultural wastes consist of high amounts of
cellulose and can be a potential source for cellulose or CNCs isolation
(Fortunati et al., 2016).
Furthermore, barley can be a main source of starch as it consists of
approximately 65% starch. However, there is a lack of studies being
done on barley compared to rice, wheat as well as maize, despite barley
being rich in both cellulose fiber and starch. Barley husk is considered
an agricultural residue of barley, and 20% of barley is made up of this
agricultural waste. In addition, the composition of cellulose in barley
husk can be as high as 39% (El Halal et al., 2015). The composition of
barley husk is approximately 20.7% hemicellulose, 31.8% cellulose,
14.9% lignin and 5.8% ash (Espino et al., 2014). Espino et al. (2014)
have successfully isolated the CNCs from barley husk, which has a
length of 329 ± 123 nm, diameter of 10 ± 4 nm with an aspect ratio
of 32. Their study has proven that CNCs isolated from barley husks can
be potential reinforcing fillers in polymer manufacture.
In general, the barley straw is composed of approximately 20–30%
hemicellulose, 35–40% cellulose and 15–25% lignin. Oun and Rhim
(2016) produced CNCs with an aspect ratio of 19, a crystallinity index
of 0.634 and a yield of 69 wt%. Moreover, their work also demonstrated
that the incorporation of 5 wt% of barley straw isolated from CNCs
enhances the tensile strength of the composite by 42.6% along with the
improvement on water vapour permeability to 20.4%.
2.2.2.5. Rice nanocellulose. Approximately 500 million tons of rice are
being harvested globally per year. Nearly 20% of the dry weight of
harvested rice is represented by rice hull (Nascimento, Marim,
Carvalho, & Mali, 2016) and approximately 1–1.5 kg rice straw (Hu,
Gu, Jiang, & Hsieh, 2016) can be obtained per kg of rice grain
harvested. Cellulose isolation from rice husk involves a series of
processes: pretreatment followed by delignification. The main
purpose of these series of processes is to break up the complex lignin-
cellulose-poliosis without causing any damage to the cellulose fibrils.
Nascimento et al. (2016) reported that the bleaching step was able to
reduce lignin content from 7.22% to 4.22% and enhanced the
crystallinity of CNCs up to 70%, resulting in CNCs with better
thermal stability. The cellulose fibers of rice husks have a high degree
of purity of approximately 93% reported by Oliveira et al. (2017). The
studies reported by Johar, Ahmad, and Dufresne (2012) demonstrated
that approximately 25% of rice husks are in the form of silica ash, and
this finding was similar to the studies done by Real, Alcala, and Criado
156
Food Packaging and Shelf Life 17 (2018) 150–161
(1996). Overall chemical composition for rice husks consists of 33 wt%
hemicellulose, 35 wt% cellulose, 23 wt% lignin and 25 wt% silica ash.
Rosa, Rehman, de Miranda, Nachtigall, and Bica (2012) extracted
CNCs from rice husk by using totally chlorine-free technologies. Their
work has shown that there were no toxic effluents generated during the
extraction of CNCs from rice husk while also resulting in a yield of
approximately 74%. In addition, the CNCs produced have a crystallinity
of 67%, an aspect ratio of approximately 18, width in the range of
6–14 nm and a length of 100–400 nm. Furthermore, Rezanezhad,
Nazanezhad, and Asadpur (2013) studied how ultrasonic treatment
affected the isolated nanocellulose, and they found that the degradation
behavior of the ultrasonic-treated nanocellulose is similar to the pur-
ified cellulose fibers.
According to Islam, Kao, Bhattacharya, Gupta, and Bhattacharjee
(2017) the production of CNCs on an experimental scale usually results
in a very low yield of less than 30%. Based on their studies, the utili-
zation of low pressure alkaline delignification (LPAD) is consider a good
approach for industrial production of CNCs from rice husk, as this
process increases the yield of production up to more than 95% without
sacrificing the quality of the final product.
The fiber of rice straw can normally be typified by the existence of a
significant percentage of silica. The rice straw fiber has a short fiber
length which is in the range of 0.65–3.48 mm. The diameter of the rice
fiber is approximately 5 to 14 μm. In addition, the hemicellulose of the
rice straw is made up mainly of pentoses, including xylose along with
arabinose sugars whereas the lignin is made up predominantly of syr-
ingyl-guaiacyl units (El-Wakil, Kassem, & Hassan, 2016). The rice straw
is composed of 19–27% hemicellulose, 32–47% cellulose, 11–24%
lignin and 7–20% silica (Hu et al., 2016). The CNCs isolated from rice
straw have an aspect ratio of 18, crystallinity index of 0.663 and yield
of 64%. The incorporation of 5 wt% rice straw isolated from CNCs
produced a composite successfully enhancing the tensile strength by
45.7% and reducing the water vapour permeability by 26.3% (Oun &
Rhim, 2016).
2.3. Antimicrobial agent for food packaging
The outbreak of foodborne diseases has stirred up the awareness of
the public about the importance of the prevention of microorganism
contamination of raw ingredients and of processed food products. The
contaminated food becomes waste, and the consumption of this con-
taminated food would jeopardize the health of the consumer.
Therefore, active packaging with regard to inhibiting the activity of
pathogenic microbials in food has been studied to overcome these is-
sues and provide safer food products (Otoni, Espitia, Avena-Bustillos, &
McHugh, 2016; Sung et al., 2013).
Active food packaging can exercise many kinds of functions such as
antioxidant, oxygen scavenger, flavoring, moisture absorber, ultraviolet
barrier and antimicrobial. However, the active packaging with the
purpose of giving off active biocide substances to food has received high
attention due to the ability to lengthen the service life of food as well as
lessen the presence of foodborne microorganisms. The antimicrobial
action can be accomplished by introducing active biocides directly into
food products or in the space surrounding the food. The main function
of antimicrobial packaging is to lessen and subsequently prevent the
spoilage microorganisms from growing (Ribeiro-Santos, Andrade, &
Sanches-Silva, 2017).
According to Kapetanakou and Skandamis (2016) and Appendini
and Hotchkiss (2002), there are different kinds of approaches where
antimicrobial compounds can be applied in food packaging, and those
approaches can be divided into three main concepts: (1) Without any
contact between antimicrobial compounds and food by incorporating
the antimicrobial compound into separate carriers (which is usually
practiced in meat packaging); (2) Indirect contact between anti-
microbial compounds with food by having a part of the antimicrobial
compound immobilized in the carriers (e.g., encapsulation of
I. Gan, W.S. Chow
Fig. 1. Utilization of antimicrobials in food packaging. No contact between antimicrobial compounds with food (Concept 1). Indirectly contact between antimicrobial
compounds with food (Concept 2). Direct contact of antimicrobial compounds with food (Concept 3).
antimicrobial compound into biopolymer matrices); and (3) Direct
contact of antimicrobial compound with the food by introducing anti-
microbial compounds onto the surface or core of the food. Approaches
to food packaging are presented in Fig. 1.
In general, antimicrobial compounds are made up of two categories
that are either organic or inorganic materials. The organic materials are
organic acids, polymers or enzymes while the inorganic materials are
nanoparticles of metals or metal oxides. The difference between these
two antimicrobial materials is that the thermal stability of organic an-
timicrobial materials is lower compared to inorganic materials, and
thus both metal and metal oxide nanoparticles are more likely to tol-
erate tougher processing conditions (Carbone, Donia, Sabbatela, &
Antiochia, 2016).
Consequently, the incorporation of nanoparticles of antimicrobial
agent has emerged to aid advances in food preservation. Today, na-
notechnology application, particularly in the food sector, has been
dominated by packaging materials (Echegoyen & Nerín, 2013). Nano-
technology-derived food packaging can be classified into two different
categories: improved packaging and active packaging. Improved
packaging can be obtained when the polymer matrix is incorporated by
nanomaterial to enhance barrier properties, whereas active packaging
involves the direct interaction between the nanoparticles with the food
products or the environment to achieve a greater degree of protection of
food products. Since metal nanoparticles are more advantageous in
terms of thermal stability, they can be considered for use as anti-
microbial compounds and be utilized in active packaging. Few metal
nanoparticle antimicrobial agents have been studied, including Cu, Au,
Zn, Ag and Ti. Silver nanoparticles (AgNPs) demonstrated higher an-
timicrobial activity compared to the other metal nanoparticle agents
(Carbone et al., 2016).
The nanosize of AgNPs provides a larger surface area that eases its
interaction with microbial cells and accomplishes a more efficient
157
Food Packaging and Shelf Life 17 (2018) 150–161
antimicrobial activity compared to normal-sized Ag particles (de
Azeredo, 2013; Guo, Yuan, Lu, & Li, 2013). Furthermore, nanosilver
also possesses broad-spectrum antimicrobial properties and is still ac-
tive against antibiotic resistant or multidrug resistant microorganisms
(de Azeredo, 2013; Guo et al., 2013; Huang, Li, & Zhou, 2015; Su, Lin,
Chen, Wu, & Wang, 2017).
Despite many studies being conducted on the antimicrobial beha-
vior of AgNPs, the mechanism of the antimicrobial activity of AgNPs is
not clearly known and remains a subject for research. Basically, a few
types of mechanisms have been suggested: (i) The silver nanoparticle
will accumulate and bind to the cell wall as well as the membrane
proteins, which creates ‘pits’ on the cell and eventually penetrates the
cell, resulting in structural damage to the bacterial cell which causes
cell death (Aderibigbe, 2017; Dakal, Kumar, Majumdar, & Yadav, 2016;
Prabhu & Poulose, 2012;), (ii) The penetration of silver nanoparticles
upsets the stability of the intracellular structures and biomolecules such
as DNA. The interaction of silver nanoparticles with bacterial cells can
be defined as a reaction of a soft acid with a soft base because the cells
are composed mainly of sulfur and phosphorus which act as a soft base
whereas silver can be considered a soft acid. Moreover, the backbone of
DNA is made up of phosphorus atoms, allowing the silver nanoparticles
to react easily with this soft base and eventually destroy the DNA. This
phenomenon triggers a defense mechanism in which the bacteria pro-
tects its DNA from damage and eventually restricts the cells from self-
replicating (Duncan, 2011; Feng et al., 2000; Prabhu & Poulose, 2012),
(iii) Ag+ will disrupt the vital cells by targeting and binding to the thiol
groups (ASH) that contain disulfide or sulfhydryl functional groups on
the enzymes or surfaces of membrane proteins. The binding of Ag (+)
ions to these thiol groups will establish stable SAAg bonds that cause
the deactivation of the protein. This action will tend to inhibit overall
functionality in the microorganism (Duncan, 2011; Dallas, Sharma, &
Zboril, 2011), (iv) Formation of excessive reactive oxygen species
I. Gan, W.S. Chow
Fig. 2. Possible antimicrobial mechanism of nanosilver.
(ROS) from both AgNPs and Ag+ will cause an imbalance of oxidation/
antioxidation that results in oxidation stress, inflammation and sub-
sequent destruction in membranes, proteins and DNA (Guo et al.,
2013), and (v) The silver nanoparticle will also inhibit the signal
transduction and cell growth by altering the phosphotyrosine profile of
bacterial peptides (Aderibigbe, 2017; Dakal et al., 2016). Fig. 2 de-
monstrates the possible antimicrobial mechanism of nanosilver.
The current nanotechnology applications in the food sector are
dominated by nanotechnology-derived food packaging materials. In
addition, as the commercialization of nanomaterials grows and the at-
tention to the environmental effects of plastic continues to rise, en-
vironmentally friendly food packaging materials will become the norm
(Echegoyen & Nerín, 2013; Fortunati, Peltzer, Armentano, Jiménez, &
Kenny, 2013). This nanotechnology-derived food packaging can be
obtained through the combination of bio-based nanocellulose and an-
timicrobial functional agents that can be derived from either natural
resources or metal nanostructures. The combination of these two na-
nomaterials develops a green bionanocomposite with enhanced anti-
microbial behavior. In addition, by using biopolymers such as polylactic
acid (PLA) as a matrix for this green nanocomposite, with the combi-
nation of antimicrobial and cellulose nanocrystals, this nanocomposite
can serve as a good packaging material that not only protects the food
from microorganisms but can also address the issues of the accumula-
tion of agricultural waste and environmental pollution. Table 3 relates
PLA/nanocellulose composites to different types of antimicrobial
agents. Nanosilver (loading in the range of 0.5 wt% to 1 wt%) could
produce antimicrobial effects on Staphylococcus aureus and Escherichia
coli for PLA/nanocellulose biocomposites. In other words, the me-
chanical, thermal and barrier properties of the PLA/nanocellulose are
either enhanced or maintained in the presence of nanosilver. However,
some of the natural antimicrobial agents (e.g., oregano essential oil,
158
Food Packaging and Shelf Life 17 (2018) 150–161
nisin) could demonstrate good antimicrobial activity but at the cost of
strength, modulus and even water vapour barrier properties. Thus, one
should always bear in mind that the development of PLA packaging
materials should achieve a balance in the mechanical, thermal, optical,
and other specific functional properties (e.g., antimicrobial, gas barrier,
water barrier, etc.).
3. Future perspectives and outlook
Bionanocomposites are definitely a good alternative source for the
(partial) substitution of the petroleum-based plastic material in pack-
aged food due to the inability to recycle food packaging plastic film.
Among all the biopolymers, PLA is the most adequate candidate in
terms of its unique mechanical properties comparable to the common
packaging plastic material. The production of PLA by fermentation of
agricultural resources (or waste) can reduce the emission of carbon
dioxide, possibly leading to reduced pollution as well as addressing the
issue of depletion of fossil fuels. In addition, the abundant availability
of agricultural residues can be utilized to produce nanocellulose. The
nanocellulose can be incorporated into biopolymer (e.g., PLA) to de-
velop greener bionanocomposites. There are various forms of PLA
packaging systems available on the market in the form of flexible
packaging film, food trays, containers and bottles. All of these forms of
packaging require different processing techniques, and the most com-
monly applied technique for PLA packaging applications are thermo-
forming and injection molding. Many techniques can be applied to
manufacture a PLA/nanocellulose packaging system, but the selection
of techniques should consider the desired end use of the application, the
intrinsic chemical and physical properties of nanocellulose and the
thermal stability of the nanocellulose. The use of PLA/nanocellulose in
food packaging should be accompanied by the appropriate
I. Gan, W.S. Chow Food Packaging and Shelf Life 17 (2018) 150–161

antimicrobial properties, so the selection of antimicrobial agents should

Fortunati, Rinaldi et al. (2014)

Pal, Dubey, Gopinath, and Pal

Luzi, Fortunati, Jiménez et al.
be considered. For example, according to the European Food Safety

Yu, Yang, Lu, Chen, and Yao

Fortunati, Armentano, Zhou,

Fortunati, Armentano, Zhou,

Authority (EFSA), the upper limit for silver migration in food packaging

Yalcinkaya et al. (2017)

Salmieri et al. (2014b)

Salmieri et al. (2014a)
Iannoni et al. (2012) cannot go beyond 0.05 mg/L in water and 0.05 mg/kg in food.

Puglia et al. (2012)

Yang et al. (2016)

Therefore, the generated bionanocomposites should be considered for
the migration phenomenon. Thus, more attention should be focused on
researching antimicrobial as well as migration behavior of anti-
Reference

microbial agents (e.g., nanosilver) in the future by the virtue of having

(2017)

(2016)

(2017)
maximum use of PLA/nanocellulose bionanocomposites in different
types of antimicrobial packaging applications.
The antibacterial activity of the composite was greater on E. coli compared to S. aureus

water vapour permeability. However, there was no significant antimicrobial activities

The antibacterial activity for both Staphylococcus aureus and Escherichia coli cells was

The incorporation of CNC and silver showed improvement in barrier properties of the

The PLA-CNC-nisin films only showed total inhibition of L. monocytogenes from day 3.
properties. The ternary nanocomposite film does not showed migration level beyond
films. The migration level of the nano-biocomposites films was below the permitted

The utilization of CNC and ZnO showed improvement in mechanical properties and

The nisin release of the film had increased continuously and up to 21% at day 14.
The AgNPs and CNF improved the mechanical, thermal, barrier and antibacterial
Acknowledgments

Xanthomonas axonopodis pv. vesicatoria and Xanthomonas arboricola pv. Pruni.

The introduction of oregano essential oil enhanced antimicrobial activity.

The resulted film showed an effective antibacterial activities against both

We gratefully acknowledge the financial support provided by the
Antibacterial activities for both E. coli and S. aureus were observed.
Research University grant (1001/PBAHAN/8014024) from Universiti
Sains Malaysia.
The PLA/1 CNC/ 0.5 Ag displayed best antibacterial activity.

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