Trends in Food Science & Technology xx (2015) 1e20
Review
Advances and
challenges for the use
of engineered
nanoparticles in food
contact materials
Joseph C. Hannona,
Joseph Kerryb,
Malco Cruz-Romerob,
Michael Morrisc and
Enda Cumminsa,*
a such as the cosmetics, food and beverage, textile, medical,
Biosystems Engineering, School of Agriculture, Food
Science and Veterinary Medicine, Agriculture and
Food Science Centre, University College Dublin,
Belfield, Dublin 4, Ireland (Tel.: D353 1 7167476;
e-mail: enda.cummins@ucd.ie)
b
School of Food & Nutritional Sciences, Food
Packaging Group, University College Cork, Cork,
Ireland
c
Department of Chemistry, University College Cork,
Cork, Ireland
The use of nanotechnology in the food industry has great po-
tential, particularly in the area of food packaging. This paper
looks at recent advances and industry challenges in relation
to the use of metal and non-metal engineered nanoparticles
(ENPs) in food packaging to grant active and intelligent prop-
erties. A particular focus will be placed on risk assessment stra-
tegies and policy developments associated with the use of
nanotechnology in food contact materials (FCMs). The
absence of a regulatory framework for NP FCMs has been
highlighted as a drawback for the development of nanoparticle
* Corresponding author.
http://dx.doi.org/10.1016/j.tifs.2015.01.008
0924-2244/Ó 2015 Elsevier Ltd. All rights reserved.
Please cite this article in press as: Hannon, J. C., et al., Advances and challenges for the use of engineered nanoparticles in food contact materials, Trends in
Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
FCMs. To aid the understanding of nanotechnology in the area
of FCMs, a NP specific exposure framework providing prompt
risk assessment could be invaluable to industry, consumers
and regulatory bodies.
Introduction
Currently the world’s population stands at 6.47 billion,
however this is expected to increase to 9.08 billion by
2050 (WPO, 2008). This creates a number of complex
problems, particularly the issue of an adequate food supply.
The world’s food resources are unevenly distributed glob-
ally, resulting in the difficult task of preserving food stuffs
to allow for transportation to a wider geographical area.
Food packaging is a common method of preserving food
stuffs, combined with preservatives, temperature and pres-
sure treatments. The advent of materials containing NPs
in the size range 1e100 nm, granting improved properties,
has proven advantageous in a vast number of industries
electronics and computing, appliances and cooking utensil
industries (Maynard & Michelson, 2014). Emerging food
packaging materials containing ENPs that possess active
and intelligent properties have the potential to alleviate
some of the global food supply issues. These materials
may increase the shelf life of food products, improve
food safety and reduce the amount of food waste due to
spoilage. However, the uptake of novel food packaging ma-
terials containing ENPs has been met with concerns in rela-
tion to the risk posed to humans from consumption of ENPs
which may migrate from NP food packaging into food
(Kanmani & Rhim, 2014b). This issue is exacerbated by
the immense uncertainty which surrounds the field of NP
human oral toxicity. Advancements in the area of in vivo
mouse toxicity (Park, Bae, et al., 2010; Park, Marsh, &
Dawson, 2010) and in vitro human cell studies (Loh,
Saunders, & Lim, 2012) presenting organ damage and in-
flammatory responses in mice, and extensive damage to
intracellular organelles in cells have been challenged by a
recent in vivo human toxicity study showing no clinically
significant effects of engineered silver nanoparticles
(EAgNPs) under acute oral dose conditions (Munger
et al., 2014). EAgNPs are silver NPs which exist as a result
of some size reducing process, whether intentional or unin-
tentional. Additionally, contradictions exist concerning the
toxicity of NPs, mainly surrounding the argument that
2 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
humans are, and have been exposed to quantities of natu-
rally occurring nanoparticles (NONPs) in food and the
environment that would be considered harmful under the
present conservative regulations (Sk, Jaiswal, Paul,
Ghosh, & Chattopadhyay, 2012). A noteworthy distinction
is the disparity between ENPs which are intentionally man-
ufactured to possess enhanced properties and NONPs
which are naturally occurring and unintentional. Currently,
in the literature studies focussing on the presence of
NONPs in food have been limited to a select number of
foods. A study by Sk et al. (2012) confirmed the presence
of carbon NONPs in food products such as bread, jaggery,
corn flakes and biscuits. In their conclusions they noted that
NPs existed in nature long before analytical techniques for
detection of NPs were developed. Similarly, a study by
Yang et al. (2014) found that food grade titanium dioxide
(E171) contained between 17 and 35% nanosized particles.
Another food additive which has been found to contain ag-
gregates with particles <100 nm is silicon dioxide, also
known as synthetic amorphous silica (SAS) or E551 in
the EU (Bouwmeester, Brandhoff, Marvin, Weigel, &
Peters, 2014). It should be noted that although NPs are
naturally and unintentionally present in these foods, the
processes used in their manufacture is a likely cause of
their nano dimensions. Alternatively, the presence of native
casein micelles with a mean diameter of 100 nm in dairy
milk is an example of NONPs that are present in the raw
food material before processing (Trejo, Dokland, Jurat-
Fuentes, & Harte, 2011). According to the United Kingdom
Food Safety Authority (UKFSA) products found to contain
NPs would include; ricotta cheese, homogenised milk and
other nanoemulsion formulations of food, such as co-
enzyme Q10 (UKFSA, n.d.). At present, a lack of suitable
methods to quantify and differentiate between ENPs and
NONPs has resulted in few studies focussing on the pres-
ence of NONPs in drinking water and food (Savolainen
et al., 2010). Although recent developments of nanotech-
nology in the food industry has been great, there are a num-
ber of issues which require attention before nano products
can take the place of existing products. This review will
discuss the recent developments in nanocomposite FCMs,
applications and legislations. It will, more specifically,
focus on the risk associated with human exposure to ENP
FCMs through unintentional oral ingestion of ENPs which
may have migrated from FCMs.
Nanomaterials e synthesis and forms
The definition of nanomaterials is constantly developing
with each region having its own set of nano specific defini-
tions. The most recent definition employed by the European
Commission for a nanomaterial is a “natural, incidental or
manufactured materials containing particles, in an unbound
state or as an aggregate or as an agglomerate and where,
for 50% or more of the particles in the number size distri-
bution, one or more external dimensions is in the size range
1e100 nm” ([EC] European Commission, 2011). Although
Please cite this article in press as: Hannon, J. C., et al., Advances and challenges for the use of engineered nanoparticles in food contact materials, Trends in
Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
the NP upper size limit has been defined as 100 nm, some
authors claim properties of nanomaterials for materials con-
taining particles larger than 100 nm (Busolo, Fernandez,
Ocio, & Lagaron, 2010). Huang et al. (2011) labelled par-
ticles in the size range 100e300 nm as “nano” due to their
novel properties.
Even though nanotechnology is still in its infancy with
regard to research and development, new forms of ENPs
are constantly being uncovered. In industry, emerging NP
technologies are developed for their physicochemical prop-
erties and often gain there name from objects of similar ge-
ometry with the addition of “nano”. Some common types of
NPs include; quantom dots, liposomes, carbon nanotubes,
dendrimers, nanobubbles, nanoclusters, functionalized
NPs (Re, Moresco, & Masserini, 2012), nanoplatelets,
nanocrystals, nanofibres, nanowhiskers (Duncan, 2011),
nanocubes, nanomultifacets, nanowires, nanorods (Chen
& Schluesener, 2008), nanospheres, nanoplates, nanotrian-
gles, fullerenes (Guo, Yuan, Lu, & Li, 2013) and nanocap-
sules (Sato, Quintas, Vincente, & Cunha, 2011).
The synthesis of ENPs is a complex process dominated
by two principal manufacturing categories. Firstly, a ‘Top
down’ method which involves the reduction of larger par-
ticles by some physical or chemical mechanism (Cushen,
Kerry, Morris, Cruz-Romero, & Cummins, 2012). Exam-
ples of the ‘Top down’ method that have been reported
include mechanical milling and homogenisation (Cushen
et al., 2012), laser and vaporisation followed by cooling
(Brody, Bugusu, Han, Sand, & McHugh, 2008), inert-gas
aggregated magnetron sputtering (Cassidy et al., 2013),
etching, electro-explosion and laser ablation (Chaudhry,
Boxall, Aitken, & Hull, 2005). The second known as a
‘Bottom up’ method is more complex, as it influences
the assembly of molecules and ions into NPs. Examples
of ‘Bottom up’ synthesis methods have been reported in
the literature such as the Sol-gel method (Hatat-Fraile,
Mendret, Rivallin, & Brosillon, 2013), biomass reaction
(Gericke & Pinches, 2006), chemical vapour deposition
(Kim, Chung, Youn, & Hwang, 2009), Plasma or flame
spray synthesis (Rudin, Wegner, & Pratsinis, 2013), elec-
tromagnetic levitational gas condensation method
(Kermanpur, Rizi, Vaghayenegar, & Ghasemi Yazdabadi,
2009; Mohammadi & Halali, 2014; Vaghayenegar,
Kermanpur, & Abbasi, 2012), supercritical fluid synthesis
(Daschner de Tercero et al., 2013), spinning (Tai, Wang,
Kuo, Chang, & Liu, 2009), templating (Liu, Tao, &
Zhang, 2012; de Matos & Courrol, 2014), self-assembly
(Zhang & Wang, 2014), atomic layer deposition (Gould
et al., 2013), crystallisation (Kong et al., 2011), solvent
extraction and evaporation (Hung, Teh, Jester, & Lee,
2010), and biosynthesis (Mittal, Bhaumik, Kumar, &
Banerjee, 2014). The list of ENP synthesis methods is
constantly growing, with a shift towards eco-friendly syn-
thesis methods such as the solvent reduction and stabiliza-
tion of Ag colloids using starch and glucose (Cheviron,
Gouanv
e, & Espuche, 2014).
 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
Nanotechnology in the food industry
Nanotechnology has the potential to penetrate every
aspect of food production. At the farm level, targeted pes-
ticides may increase crop yield and controlled release phar-
maceuticals could improve animal health, whilst reducing
the risk of disease. The efficiency of the food processing
line has the potential to be revolutionised by self-cleaning
antimicrobial machines and faster fluid transport systems
with super hydrophobic coatings. In addition, the product
packaging stage will be shortened due to container adhe-
sives that will set quicker and at lower temperatures than
conventional adhesives (Maynard & Michelson, 2014).
Food contained in nano-packaging with antimicrobial abil-
ity may require less refrigeration during transport and will
stay fresh over longer journeys (Rhim, Park, & Ha, 2013).
In a retail outlet, nanosensor labels on packaging could
inform the consumer if the product has been subject to tem-
perature abuse during transport or if it contains an unsafe
level of bacteria. When the consumer has finished with
the product, waste packaging could be placed in a compost
bin where it would degrade into eco-friendly constituents
over a short period of time. To date, the application of
ENPs in the food industry has mainly centred around four
areas which include; processing food ingredients to form
nanostructures, using ENPs for sensory properties and
food processing, exploitation of “active” and “intelligent”
properties and the direct addition of ENPs in food for sup-
plement or nano-encapsulation (Chaudhry et al., 2008).
Although there have been reports of nanotechnology being
applied in the food industry in countries such as the United
States and Korea (Maynard & Michelson, 2014), due to a
lack of nano specific regulation it is difficult to approximate
its overall use worldwide (Coles & Frewer, 2013). It is
apparent from the rising number of original research papers
that there has been an increased interest in the area of ENP
food packaging.
Nanoparticles in food packaging
Due to the added and improved functions and proper-
ties of food packaging incorporating ENPs, three cate-
gories of ENP packaging can be emphasized which
are “Improved”, “Active” and “Intelligent” packaging
(Chaudhry et al., 2008; Silvestre, Duraccio, & Cimmino,
2011). These three categories indicate what applications
the packaging material is used for. However, the use of
ENPs in FCMs for active and intelligent properties in
the European Union is disallowed, with the exception of
certain products, such as titanium nitride (TiN) in plastic
bottles (Echegoyen & Ner
ın, 2013; Simon, Chaudhry, &
Bakos, 2008).
Metal and non-metal nanoparticles
All metals can exist in NP form. However only a small
number of metals and metal-based composites have been
reduced to NP form and exploited in the food industry to
improve the properties of food packaging (see Table 1).
Please cite this article in press as: Hannon, J. C., et al., Advances and challenges for the use of engineered nanoparticles in food contact materials, Trends in
Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
3
These include silver (Ag), gold (Au), iron (Fe), iridium
(Ir), zinc oxide (ZnO), silicon dioxide (SiO2), titanium di-
oxide (TiO2), titanium nitride (TiN), alumina (Al2O3),
iron oxide (Fe3O4, Fe2O3) (Chaudhry et al., 2008; FSAI,
2008), copper (Cu), copper oxide (CuO) and palladium
(Pd) (Llorens, Lloret, Picouet, Trbojevich, & Fernandez,
2012). Other metals exist which have the potential to be
reduced to nanoscale and be incorporated into food pack-
aging, but are overlooked as a result of lower antimicrobial
potential. Gallium (Ga) is a good example of a rare metal
element which has been overlooked as an alternative to
commonly used metals in nano-particulate form (Kamat,
Guin, Pillai, & Aggarwal, 2011; Youssef, Kamel, & El-
Samahy, 2013). Similar to Ag, Ga shows strong antimicro-
bial effects against a number of pathogenic bacteria and
fungi (Kelson, Carnevali, & Truong-Le, 2013). Notably,
Ga is analogous to Fe and can therefore be used to starve
bacteria of Fe by disrupting the bacterial Fe uptake mecha-
nism which is necessary for bacteria to survive (Kelson
et al., 2013). Ga has been considered for use in cancer med-
icines (Xie et al., 2014). However, due to its toxicity it has
not yet been considered for use in FCMs.
ENPs can also be derived from non-metals such as clays
and organic materials such as protein, polymers (FSAI,
2008), chitosan and poly-lactic acid (Dev et al., 2010).
Nanoclay is composed of fine-grained minerals of naturally
occurring aluminium silicate having a layered sheet like ge-
ometry with sheet thicknesses <100 nm. Nanoclays such as
nanoscale montmorillinite (MMT), also known as
bentonite, have been incorporated in polymers with aims
to increase the gas barrier properties, but have been found
to also increase polymeric strength, heat resistance and
thermal stability (Majeed et al., 2013). In recent years,
both industry and academia have taken great interest in
nanoclays for use in food packaging to combat some of
these long standing issues. In addition to inorganic ENPs,
ENPs are also synthesised from organic sources such as
chitosan. Chitosan is a material derived from deacetylated
chitin which has been shown to exhibit improved antimi-
crobial effects when reduced to the nanoscale (Hajipour
et al., 2012). Bulk chitosan has been identified as a possible
carrier matrix for antimicrobials (Ouattara et al., 2000), as
an incorporated antimicrobial in polymer food packaging
(Park, Marsh, et al., 2010) and as a film to be coated to sur-
faces (Coma, Deschamps, & Martial-Gros, 2003). Howev-
er, few studies have considered the incorporation of ENP
chitosan into polymer food packaging, despite its well es-
tablished strong antimicrobial properties (Cruz-Romero,
Murphy, Morris, Cummins, & Kerry, 2013; Kong, Chen,
Xing, & Park, 2010). Although chitosan can be derived
from fungi and insects, it is more commonly synthesised
from food compatible sources.
Food grade nanoparticles
Food grade NPs are particles which exist naturally or
have been manufactured in the nano size range from food
 4
Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
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Table 1. Applications of metal and non-metal nanoparticles in industry.

NP type Nanomaterial product Manufacturer Country Stage NP size Function Reference

Ag Nano-silver salad bowl Changmin Chemicals Korea on market not disclosed Antimicrobial (Maynard & Michelson, 2014)
Nano silver baby mug cup & Baby DreamÒ Co., Ltd. Korea on market not disclosed Antimicrobial (Bouwmeester et al., 2007)

J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
nurser
Fresh BoxÒ food storage BlueMoonGoodsÔ USA on market not disclosed Antimicrobial (Maynard & Michelson, 2014)
containers
FresherLongerÔ containers & SharperImageÒ USA on market 25 nm & 1e100 nm Antimicrobial (von Goetz et al., 2013)
bags
Nano-silver storage box Quan Zhou Hu Zeng Nano China on market not disclosed Antimicrobial (Maynard & Michelson, 2014)
TechnologyÒ Co., Ltd.
Plastic food containers & water A-Do Global Korea on market not disclosed Antibacterial (Bouwmeester et al., 2007)
bottle
Fresh food containers Oso Fresh USA on market 40-60 nm Antimicrobial (Echegoyen & Ner
ın, 2013)
Smartwist food Storage with Kinetic Go Green USA on market 10-20 nm Antimicrobial (Echegoyen & Ner
ın, 2013)
nano-silver
Au Nanorama - gold tootpaste Lexon, Inc. USA on market not disclosed Antmicrobial (Maynard & Michelson, 2014)
ZnO Nano plastic wrap SongSing Nano Technology., Taiwan on market not disclosed Barrier & antimicrobial (Bouwmeester et al., 2007)
Ltd.
Ó
TiO2 Trident White chewing gum Mondelez International USA on market 110 nm Colouring (E171) (Weir, Westerhoff, Fabricius,
(E171) Hristovski, & von Goetz, 2012)
TiN PET bottles (up to 20 mg/kg) Colormatrix USA not disclosed not disclosed Barrier (EFSA, 2012)
MMT NanolokÔ InMatÒ Inc. USA on market not disclosed Barrier (Joshi, Banerjee, Prasanth, &
Thakare, 2006)
SiO2 NanoceuticalsÔ Slim Shake RBC’s USA on market not disclosed Nanoencapsulation (Bouwmeester et al., 2007)
Chocolate
Clay Durethan KU2-2601 film (SiO2) Bayer USA on market 1 nm - 1 mm Barrier (Cushen et al., 2012)
AegisÒ OX Honeyells USA on market not disclosed Oxygen scavenging (Bouwmeester et al., 2007)
Beer bottles (ImpermÔ) NanocorÒ (distributed by USA on market not disclosed Barrier (Bouwmeester et al., 2007)
Colormatrix)
Micelle Nano-encapsulated CoQ-10 Aqua Nova Germany on market 30 nm Nanoencapsulation (Bouwmeester et al., 2007)
(NovasolÒ)
Liposome Nano (gluco, greens, reds, etc.) Biopharma USA on market not disclosed Encapsulation (Biopharma., 2012)
Corn starch Eco PlasticÔ Plantic Technologies Ltd. Australia on market not disclosed Biodegradability (Han, Yu, Li, & Wang, 2011)
 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
compatible sources (Cruz-Romero et al., 2013; Sato et al.,
2011). The use of food grade NPs is a solution to the
inherent toxicity associated with metal and metal oxide
ENPs. There should be a greater public acceptance towards
food grade NPs when compared to metal ENPs due to the
fact that they are more natural, whilst having a diminished
toxicity (Coles & Frewer, 2013). However, concerns persist
regarding the increased bioavailability and accumulation of
different ENPs in the human body. As a result, there is still
a need for specific human exposure assessment. Alcoholic
lecithin and sodium caseinate are both food derived sub-
stances which have been reduced to nanoscale and added
to chitosan for use as nanocapsules in the food sector
(Sato et al., 2011). Similarly, curcumin and ascorbyl dipal-
mitate which are derivatives from the spice turmeric and
vitamin C have been incorporated into cellulose-based
packaging films as a nanoscale additive to provide antibac-
terial function (Sonkaew, Sane, & Suppakul, 2012). A fruit
extract paprika oleoresin has been reduced to the nanoscale
to improve the marinating performance and sensory proper-
ties of poultry meat (Yusop et al., 2012). There are
numerous different food and plant extracts which possess
antimicrobial characteristics and have the potential to be
incorporated into food packaging. Spice essential oils
such as oregano, garlic and rosemary are proven active an-
timicrobials against a range of bacteria when used in pack-
aging films (Rhim et al., 2013; Seydim & Sarikus, 2006;
Sung et al., 2013). Remarkably, none of these potential an-
timicrobials have been investigated at the nanoscale for use
in food packaging.
Incorporation and attachment in food packaging
In regions that permit the use of ENP FCMs (see Table 1),
two main categories of ENP incorporation exist. Indepen-
dent pads or similar ENP contact materials can be included
in the existing packaging or the ENPs can be immobilized
within or at the surface of the packaging (de Azeredo,
2013). The addition of independent ENP FCMs in packaging
has its advantages and disadvantages. A particular benefit is
the increased active properties due to the close contact that
can be established between the foodstuff and independent
Table 2. Non-exhaustive list of studies reporting nanocomposite manufacturing methods.
Manufacturing method Function NP type
Electrospinning Antimicrobial ZnO
Solution casting Improved properties TiO2 15-30 nm
Solvent evaporation Antimicrobial CNT Not stated
Twin screw extrusion Barrier and migration CNC & Ag 5-10 nm & 20e80 nm PLA film
Spray coating Antimicrobial Ag 10-20 nm
Immersion/reaction Barrier and antibacterial 3-polylysine 100-230 nm
Reactive magnetron Antimicrobial Ag & Ag doped ZnO 50-100 nm
sputtering
Automatic spreading Improved properties MMT
(CNT ¼ Carbon nanotubes, CNC ¼ Cellulose nanocrystals and MMT ¼ Montmorillonite).
Please cite this article in press as: Hannon, J. C., et al., Advances and challenges for the use of engineered nanoparticles in food contact materials, Trends in
Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
5
material. However, this benefit is overshadowed by the addi-
tional manufacturing processes and potential for signifi-
cantly greater migration, which could possibly shift the
food industries preference towards ENP polymer composite
packaging.
The method employed to produce ENP polymer com-
posites is greatly influenced by the function of the pack-
aging in a specific application. There are two key
approaches for producing ENP packaging which include;
ENP surface coatings or inclusion of ENPs within the poly-
mer packaging. Table 2 includes a non-exhaustive list of
some of the methods used to manufacture ENP composites.
Due to superior ENP immobilization, direct addition of
ENPs into polymer packaging has been subject to more
research than ENP coating methods. Only two studies
have dealt with the attachment mechanisms of ENPs to
the surface of food packaging (Nobile et al., 2004;
Smirnova et al., 2012). As a result, substantial gaps in
knowledge exists regarding the use of surface coatings in
food packaging and the associated human risk assessment.
Due to the existing popularity of polymers for use in
food packaging applications, polymers make a suitable sub-
strate for the incorporation of ENPs. Moreover, polymers
offer a means of ENP immobilization, preventing aggrega-
tion and uncontrollable release (Guo et al., 2013). The ma-
terial properties, low cost and ease of manufacture of
certain polymers make them increasingly popular for food
packaging applications. Polyolefins are popular food pack-
aging materials which include polypropylene (PP), polyeth-
ylene (PE), polyethylene terephthalate (PET), polystyrene
(PS) and polyvinyl chloride (PVC) (Duncan, 2011). Adding
NPs to these polymers as well as bio-polymers such as pol-
ylactic acid (PLA) has been a focus of many studies (see
Table 3), with an aim of assisting the uptake of ENP food
packaging on the global food market. Although research
focus has mainly centred on the incorporation of ENPs
into biodegradable packaging, it is important that poly-
olefin nanocomposites are not ignored based on their envi-
ronmental impact. Incorporating ENPs into polyolefin
packaging has the potential to minimize the material
required for the packaging to perform successfully in use,
Size Matrix Author(s)
30 nm Chitosan film
(Y. Wang, Zhang, Zhang,
& Li, 2012)
Soy protein film (Z. Wang et al., 2014)
Cellulose film (Dias et al., 2013)
(Fortunati et al., 2012)
PE (Smirnova et al., 2012)
Cellulose (Gao et al., 2014)
PET (Carvalho et al., 2014)
Not stated Gelatin film (Vanin et al.)
 6
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Table 3. Nanoparticle migration studies.

NPs Packaging matrix Detection method Food simulant Parameters tested Reference
Ag/s-CNC PLA ICP-MS Analytical-balance 10% ethanolIsooctane Storage time Storage temperature (Fortunati et al., 2014)

J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
% Fill rate
Ag/Zeolite PE ICP-AES TEM Hach lange 3% acetic acid Distilled water Food simulant % Fill rate (Cushen, Kerry, Morris, Cruz-
Romero, & Cummins, 2014b)
Cu & Ag PE ICP-MS SEM Chicken breast Storage time Storage temperature (Cushen et al., 2014a)
Ag/ZnO LDPE ICP-MS 10% ethanol 3% acetic acid Storage time Storage temperature (Panea et al., 2014)
Distilled water Olive oil
Ag/s-CNC PLA ICP-MS Analytical-balance 10% ethanol Isooctane Storage time Storage temperature (Fortunati et al., 2013)
% Fill rate
Ag PVC ICP-MS SEM Chicken breast Storage time Storage temperature (Cushen et al., 2013)
% Fill rate Particle diameter
Ag PE ICP-MS 10% ethanol 3% acetic acid Storage time Storage temperature (von Goetz et al., 2013)
Distilled water Olive oil
Ag LDPE PP ICP-MS SEM 50% ethanol 3% acetic acid Storage time Storage temperature (Echegoyen & Ner
ın, 2013)
Ag PE ICP-MS TEM AFM Distilled water Alcohol/ No. of coatings (Smirnova et al., 2012) (Ag
ethanolSunflower oil coatings)
Ag PE ICP-MS RSD 95% ethanol 3% acetic acid Storage time Storage temperature (Song et al., 2011)
Ag PE AAS SEM (EDX capabilities) 95% ethanol 4% acetic acid Ultra Storage temperature (Huang et al., 2011)
pure water Hexane
Ag PP ICP-MS Tap water Deionized water 5% Storage time Storage temperature (Hauri & Niece, 2011)
acetic acid
Ag/MMT PLA Strip- Voltammetry EDX-RF Water/HNO3 Storage time % Fill rate (Busolo et al., 2010)
MMT Starch based biopolymers AAS Analytical-balance Lettuce Spinach (Avella et al., 2005)
Ag PP HDPE AF4-ICP-MS SEM Distilled water 3% acetic acid Storage time Storage temperature (Artiaga, Ramos, Ramos, C
amara,
& G
omez-G
omez, )
Ag & Zn LDPE TEM AAS Orange juice % Fill rate (Emamifar, Kadivar, Shahedi, &
Soleimanian-Zad, 2010, 2011)
Al & Si PET TEM XRD ICP-MS 3% acetic acid Storage time Storage temperature (Farhoodi et al., 2014)
Cu PLA-acetone ET-AAS Saline solution Storage time% Fill rate (Conte et al., 2013)
 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
due to the improved structural and thermal properties im-
parted by the ENPs (Silvestre et al., 2011).
ENPs are commonly immobilized within polymer pack-
aging using two methods; formation of particles and/or
polymer in situ or attachment of particles and polymer in
their final state (Yang, 2003). In situ methods that involve
incorporation of ENPs into liquid polymers, include spin
coating and casting methods. When the polymer is a solid,
ENPs can be formed by a reduction of ions. An example of
this reduction process may be the formation of EAgNPs us-
ing silver nitrate (AgNO3) as a precursor (Cushen, Kerry,
Morris, Cruz-Romero, & Cummins, 2014a). Attaching the
ENPs and polymer in their solid state is a more complex
process. Nanocomposites can be formed using a combina-
tion of casting followed by solvent evaporation. Alterna-
tively, ENPs in powder form can be added to an extrusion
process. More complex methods of creating nanocompo-
sites include diffusion and synthesis of ENPs and polymer
in situ. The method employed often determines the concen-
tration and distribution of the ENPs within the polymer.
ENP surface coatings for food packaging applications is
an area which has, until recently, been neglected as a result
of intensified ENP migration and the absence of commer-
cially viable manufacturing methods. Nevertheless, due to
the substantial benefits linked to ENP surface coatings, there
needs to be a greater emphasis on research and development
in this area. Applying ENPs to a packaging surface has an
advantage of increasing the antimicrobial function of the
ENPs as there is more reactive surface area in contact with
foodstuff allowing greater Ag ion migration. However, the
ENPs position makes them more susceptible to migration.
Guo et al. (2013) reviewed methods of applying polymer
coatings containing ENPs to surfaces in order to benefit
from antibacterial properties. The inclusion of a polymer
in the coating process highlights the poor attachment charac-
teristics of certain ENPs. Further methods of ENP attach-
ment with improved immobilization exist and have been
considered for other industries such as the biomedical
(Roguska, Pisarek, Andrzejczuk, & Lewandowska, 2014),
energy and electronic industries (Kim, Lee, & Maeng,
2009). Therefore, it would be counter-productive to reject
surface coating methods based on factors such as attachment
which can be improved.
A simple method of creating nanocomposites for antimi-
crobial application is via spray coating. Currently, the only
study which has used spray coatings to coat ENPs to food
packaging was carried out by Smirnova et al. (2012). A
study by Nobile et al. (2004) used a plasma technique to
coat EAgNPs in a polyethylenoxide-like coating on poly-
ethylene food/beverage packaging. Despite this technique
being considered for biomedical applications (Favia et al.,
2000), this is the first time it has been proposed for appli-
cation in food packaging. An emerging technology for
incorporation of ENPs onto surfaces with improved immo-
bilization is by means of a Self-Assembling Block Copol-
ymer. The process involves self-assembly of uniform
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Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
7
nanostructures using an anionic polymerization process.
Once the nanostructure is in place, ENPs which have an af-
finity for the polymer substrate are attached to the nano-
structure in a process called templating. The block
copolymer is then exposed to some chemical reaction
which leaves a nanoscale pattern. A major limiting factor
of the process is the restricted number of organic monomers
which can be used, such as PS, PB, PI and PMMA (Yang,
2003). Furthermore, only certain ENPs have an affinity for
the polymer substrates which can be used for self-
assembling block copolymers. Self-assembling block co-
polymers have been considered for use in the pharmaceu-
tical industry as a means of drug delivery (Vauthier,
Persson, Lindner, & Cabane, 2011), however, no studies
have suggested this mechanism for attachment of ENPs
in food packaging materials. Similarly, the use of Atomic
Layer Deposition (ALD) methods have not been considered
for use in food packaging applications. Unlike other
methods, ALD provides an industrially viable and scalable
method for coating food packaging. The “line-of-site” inde-
pendent nature of ALD allows a pinhole-free film of ENPs
to be coated to any surface that is exposed, including inter-
nal surfaces (King, Liang, & Weimer, 2012). ALD has the
ability to deposit oxides, non-oxides, metals and hybrid-
polymer based materials on surfaces.
Properties of nanoparticle food packaging
For NP packaging to be embraced by the public there
must be a seamless transition from existing packaging to
nanopackaging. Certain functional and aesthetic character-
istics of food packaging materials are generally recognised
as necessary for a food product to be successfully marketed.
Characteristics such as the transparency, structural integrity,
gas barrier, antibacterial, product texture and in the case of
re-usable storage containers washability, could be consid-
ered important. The transparency of food packaging is a
desirable characteristic as it allows the consumer to view
the content of the product before it is purchased. High per-
centages of well distributed fine NPs have been found to
produce relatively transparent polymers (Nazarov,
Khaydukov, Sokolov, Panchenko, & Shkurinov, 2013).
However, small percentages of large size particles can
cause a loss in transparency. Kanmani and Rhim (2014b)
reported the linear decrease in transparency of gelatin films
with increasing EAgNP content. The protein content of
food has been shown to affect the transparency of pack-
aging containing ENPs. Martinez-Abad, Lagaron, and
Ocio (2012) observed varied changes in transparency and
colour of NP packaging in contact with two food media,
chicken and apple. The high protein sample, chicken was
found to cause the greatest loss of transparency in compar-
ison to the apple samples. Considering the most likely
application of nanopackaging is for high value meat prod-
ucts, this is an important finding as loss in transparency
would hinder the marketability of such a high protein prod-
uct. In addition to the basic requirements of conventional
8 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
packaging that nanocomposites must satisfy, there must
also be clear benefits in terms of existing and novel pack-
aging properties. Properties such as; barrier characteristics,
oxygen scavenging, antimicrobial, thermal, biosensing and
material strength. On examination of products that are
commercially available, two areas which have seen
increased interest can be recognised; gas barrier and antimi-
crobial nanocomposites (see Table 1).
Gas and moisture barrier properties
A particularly important function of food packaging is to
maintain the sensory properties of the enclosed food prod-
uct, as well as the freshness through transport and storage.
A barrier to the outside environment should be established
to prevent the movement of moisture and gases through the
walls of the packaging (Simon et al., 2008). Nanoscale ma-
terials having large aspect ratios have the ability to improve
gas barrier properties dramatically when incorporated as a
filler into the walls of packaging. The increased aspect ratio
creates an obstacle for gas and moisture passing through the
packaging walls by increasing the path that the gas/mois-
ture must travel. One particular type of nanomaterial which
has been investigated to provide gas barrier properties to
food packaging is nanoclay. It is evident that industry has
taken an interest in nanoclays due to the range of food
packaging products containing nanoclay which have been
developed (see Table 1). A company called Voridan in as-
sociation with Nanocor has developed a nanocomposite
containing clay nanoparticles called Imperm. Imperm has
been used by a number of companies, such as Honeywell
(AegisÒ), Hite Brewery Co. and Bayer AG (Durethan
KU2-2601) to produce their own nanocomposite packaging
materials having improved material and gas barrier proper-
ties (Handford et al., n.d.). Ever since the pioneering work
by Avella et al. (2005) on MMT ENPs in starch biodegrad-
able films, research in the area of nanoclay composite pack-
aging has evolved and diversified to include alternative
packaging materials in combination with multiple types
of NPs (Busolo et al., 2010; Farhoodi, Mousavi, Sotudeh-
Gharebagh, Emam-Djomeh, & Oromiehie, 2014).
Antibacterial properties
The antimicrobial properties of packaging containing
NPs has been attributed to the ENPs capacity to prevent
the attachment and growth of bacteria at the surface of
packaging (Lichter, VanVliet, & Rubner, 2009), as well
as the release of ions to preserve food against microbial
growth (Fortunati et al., 2014). One factor linked to the
antibacterial efficacy of NPs which has been the subject
of significant debate in the scientific community is the ef-
fect of NP size (Hajipour et al., 2012). The debate sur-
rounds the question of whether NP size has an effect on
antibacterial activity. Small well dispersed ENPs in the
nano scale range of between 1 and 10 nm were shown to
produce improved antimicrobial properties (Fern
andez
et al., 2009). In a study concentrating on the size dependant
Please cite this article in press as: Hannon, J. C., et al., Advances and challenges for the use of engineered nanoparticles in food contact materials, Trends in
Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
antimicrobial activity of Ag colloid NPs it was found that
the smallest particles with a mean size of 25 nm had the
greatest antimicrobial activity (Pan
acek et al., 2006). How-
ever, a recent study by Xiu, Zhang, Puppala, Colvin, and
Alvarez (2012) stipulated that ENP size had an indirect ef-
fect on antibacterial activity. Under strictly anaerobic con-
ditions EAgNPs were found to have a lack of antimicrobial
activity. This implies that Ag ions are the source of antimi-
crobial properties. Therefore, ENP size does not increase
cell toxicity but alternatively increases the reactive surface
area for oxidation of Ag into Ag ions, increasing antimicro-
bial activity. Consequently, ENP aggregation is a factor that
can dramatically reduce the antimicrobial activity of NPs
by reducing the reactive surface area (Zook, Halter,
Cleveland, & Long, 2012). Zook et al. (2012) demonstrated
the effects that polymer coatings had on the agglomeration,
dissolution and toxicity of EAgNPs. The application of
coatings was found to decrease agglomeration and conse-
quently increase toxicity.
Improved antimicrobial properties can be exibited by a
number of ENPs such as Ag, ZnO, TiO2 and MMT
(Cushen et al., 2012). However, due to the superior antimi-
crobial properties of EAgNPs, there has been growing in-
terest regarding the incorporation of EAgNPs and EAgNP
hybrids in food packaging. Significantly improved antimi-
crobial properties have been observed for Ag-chitosan
nanocomposites (Rhim, Hong, Park, & Ng, 2006; Sanpui,
Murugadoss, Prasad, Ghosh, & Chattopadhyay, 2008). Ag
ions released from EAgNPs in absorbent pads were found
to be an efficient antimicrobial against Escherichia coli
(E. coli) and Staphylococcus aureus (S. aureus)
(Fern
andez et al., 2009). Similarly, Ghosh et al. (2010)
demonstrated antimicrobial activity for EAgNP/agar nano-
composite thin films in the order C. albicans > E. coli > S.
aureus. Contradictory studies can be found which present
mild inhibition of S. aureus in comparison to the satisfac-
tory inhibition of E. coli using EAgNPs of mean diameter
13.5 nm in an aqueous solution (Kim et al., 2007). When
comparing antimicrobial studies it is important to consider
the media in which the ENPs are restrained. Many antimi-
crobial studies deal with EAgNPs mobilized in aqueous so-
lutions. The antimicrobial activity of ENPs contained in
such a state could be considered a poor representation of
ENPs immobilized in food packaging as the ionisation po-
tential of ENPs is increased in a liquid medium. Thus it is
important that antimicrobial studies be available for NPs
incorporated in food packaging.
Despite the considerable research focus on nanocompo-
sites containing EAgNPs to provide antimicrobial activity,
there has been instances of non-metal, metal-oxide and
metal-hybrids being used to provide antimicrobial function.
In particular, nanoclays such as MMT which would be
conventionally exploited for barrier properties have been
incorporated in food packaging as an antimicrobial. Rhim
et al. (2006) observed greatly improved antimicrobial
activity for four different chitosan-based nanocomposites
 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
containing unmodified MMT, organically modified MMT,
Ag and Ag-zeolite ENPs. In later work, particular attention
was paid to two chitosan/organoclay nanocomposites
(CloisiteÒ 30B and CloisiteÒ 20A) which increased gas
barrier properties in linear low density polyethylene
(LLDPE) and gave antimicrobial properties against gram-
positive bacterium (Hong & Rhim, 2008, 2012). Other
ENPs which have been found to be effective antimicrobials
against food pathogens include ZnO (Akbar & Anal, 2014)
and TiO2 (Bodaghi et al., 2013).
Examples of materials containing natural antibacterial
properties can also be found, which include protective
nanostructured coatings on animals and insects. It has
been shown that insects coat themselves with antibacterial
substances to form a protective coating from predators
and the environment. The surface of Cicada insect wings
possess natural bactericidal characteristics attributed to
their nanopillar surface coating (Hasan, Crawford, &
Ivanova, 2013). A number of naturally occurring antioxi-
dants have been studied for use in food packaging applica-
tions such as a-tocepherol, plant extracts and essential oil
extracts from herbs and spices (Woranuch & Yoksan,
2013).
For NPs to be adopted in industry for use in packaging to
provide antimicrobial properties the benefits must be clear
and substantial. A significantly increased antimicrobial ac-
tivity must be observed for materials containing NPs which
can compete with alternative antimicrobial materials which
are already in use such as chitosan. Chitosan has been
shown to be affective against a wide range of bacteria, is
biodegradable and does not have the same regulatory bar-
riers as nanocomposites due to its non-toxicity (Aider,
2010). The manufacture of nanocomposites such as biode-
gradable food packaging (e.g. chitosan) containing
EAgNPs (Kanmani & Rhim, 2014a) providing synergistic
improvements in terms of mechanical and antimicrobial ac-
tivity could provide an alternative to conventional pack-
aging. More attention is required for applications were
NP combinations in packaging can present synergistic im-
provements and thus tackle some of the world’s current
packaging problems (Busolo et al., 2010).
Risk assessment strategies for nanoparticles in food
packaging
ENPs have the potential to cause harm to humans and
the environment through increased toxicity, mobility and
bioaccumulation. For nanotechnology to be accepted by
consumers, all associated risks should be clearly communi-
cated in such a way that consumers can make an informed
decision. Furthermore, the level of risk posed to humans
should be investigated under the worst case conditions of
exposure. If an unacceptable level of risk is presented, a
risk management strategy should be developed to mitigate
the risk. Risk assessment is a methodology commonly
used to assess the risk posed to humans and the environ-
ment from exposure to a substance or process. When
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Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
9
applied to ENP food packaging, the level of exposure to hu-
mans from ingestion of NPs is determined via migration
studies and in vivo toxicity studies. If an acceptable level
of risk is observed it is then the responsibility of the gov-
erning authority to allow or disallow the use of the product.
A recent success of this process was the acceptance on TiN
ENPs by the European Food Safety Authority (EFSA) for
use in PET bottles in concentrations up to 20 mg/kg
(EFSA, 2012). The function of TiN ENPs is to improve
the oxygen barrier properties of the walls of the PET
container that they are incorporated into. Excellent contain-
ment of the TiN NPs within the walls of the PET containers
may be a unique aspect of the migration mechanism which
is not shared by other NPs which require some level of
migration to carry out their function. NPs such as EAgNPs
must migrate in the form of Ag ions to allow for their anti-
microbial function, while complying with the migration
limits set out by the European Commission (EFSA, 2008;
European Commission, 2011). Therefore a compromise
must be made between the level of migration and antimi-
crobial activity.
Exposure assessment models
Frequently, substances that are considered harmful to
humans may not exist in high enough doses to pose any
real risk to humans. Mathematical exposure models provide
a method for quantifying the risk posed to humans from
NPs. Using the results from NP migration studies as an
input to an exposure model, the associated risk from NPs
can be predicted based on the scenario surrounding their
use. Two common scenarios are often identified for human
exposure to ENPs, the worst case scenario (wcs) and the
most likely scenario (mls) (Cushen, Kerry, Morris, Cruz-
Romero, & Cummins, 2013). The mls is an exposure value
based on the most probable intake of a substance obtained
from migration studies and survey data. The wcs involves
the greatest exposure to ENPs possible, based on exagger-
ated migration and consumption data. To produce a human
exposure model suitable toxicity studies, migration studies
and consumer data must be available. Given the lack of
in vivo toxicity studies for exposure to ENPs, it is necessary
to adapt non-nano rodent oral toxicity studies and apply a
safety factor. Only four human exposure models are
currently available in the literature that quantifies the risk
posed to humans from oral exposure to ENPs which have
migrated from food packaging (Bachler, von Goetz, &
Hungerb€uhler, 2013; Cushen et al., 2013, 2014a; von
Goetz et al., 2013; Smirnova et al., 2012). In each study
a mathematical model is generated to predict the potential
migration and resulting migrant amounts are compared to
actual migration results. The resulting migrant quantities
are then coupled with consumer data to generate a model
that predicts the risk posed to humans from oral exposure.
von Goetz et al. (2013) observed worst case acute exposure
of 4.2 mg EAgNPs caused by storage of 100 ml of food sim-
ulant in an EAgNP food container. Although this could be
10 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
considered a large quantity of migrating particles it was
noted that other potential sources of EAgNPs are present
in nature which can contain comparably large quantities,
such as drinking water (Akaighe et al., 2011). Weaknesses
in the model were attributed to the uncertainties surround-
ing the toxicological effects of EAgNPs and the possibility
of a “Trojan horse mechanism” (Kreuter, 2004). In the
model no link was made to food consumption data and
alternatively it was stated that a given amount of liquid
food would cause worst case acute exposure for humans.
A particular strength of the exposure model formulated
by Cushen et al. (2013) was the use of chicken consump-
tion data from an Irish survey to predict the exposure to
an individual consuming the average quantity of chicken
per day. In addition, when determining the toxicity of
ENPs to humans the surface area of the dosage was consid-
ered alongside the weight of the dose when calculating the
Provisional Ingestion Limit (PIL) which was adapted from
O’Brien and Cummins (2010). It was found that the worst
case conditions would cause migration of 8.85 mg/kg of
EAgNPs, considerably lower than the conservative
60 mg/kg overall migration limit allowed by the European
Union (European Commission (EU), 2002). This value far
exceeds the specific migration limit of 0.01 mg/kg for un-
authorized substances outlined in Directive 10/2011/EEC
(European Commission (EU), 2011). Migration limits
have been set by the European Commission for products
that are used in applications involving particularly suscep-
tible persons, such as infants (Commission Regulation
(EU), 2009). Given the number of applications for nano-
composites in the infant food storage industry it is surpris-
ing that few studies have specialized in the area.
In a recent study by Bachler et al. (2013) a physiologi-
cally based pharmacokinetic model was generated for ionic
and NP silver for five exposure scenarios. Oral exposure
was quantified for EAgNPs from two sources; dietary
intake and from food which has been stored in ENP food
storage boxes. The pharmacokinetic model was validated
by comparing simulated organ concentrations to those ob-
tained from in vivo experimental studies. It was demon-
strated that for EAgNPs size and coating did not show a
significant effect on biodistribution. Furthermore, in vivo
studies suggested that EAgNPs are more likely to be stored
as insoluble salt particles than dissolve into silver ions.
Interestingly, in all exposure scenarios the Ag levels in
most organs were below or around the background levels
of dietary intake and lower than levels which would cause
adverse effects in vitro. The results indicate that outside of
an occupational setting, the level of risk to adults from
exposure to nanosilver consumer products is low.
O’Brien and Cummins (2011) presented a risk assess-
ment framework on three nanomaterials; EAgNPs, cerium
oxide NPs and TiO2 NPs which have the potential to accu-
mulate in surface and waste water in the environment
(O’Brien & Cummins, 2011). The framework utilized un-
certainty and variability principles, alongside qualitative
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Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
risk assessment principles to generate a ranking system
for metallic NP concentration, transport and persistence
in aquatic environments. Nanomaterial characteristics as
well as aquatic environmental characteristics were
compiled to rank risk of exposure under three scenarios.
The study highlights were data critical to NP exposure
are lacking and suggests research needs in order to populate
the qualitative framework with quantitative exposure data.
Although, the risk assessment of human exposure to
ENPs was not featured in the study, the structure of the
framework was very applicable to food packaging risk as-
sessments. Such a qualitative risk ranking framework for
human exposure to nano FCMs would give a preliminary
indication of human exposure and help prioritise quantita-
tive exposure assessments to populate a nano food pack-
aging exposure model.
The NanoRelease Food Additives Expert Group (Nano-
Release Food Additives Expert Group, 2015) has focused
on the uptake of ENPs in the alimentary tract (Alger,
Momcilovic, Carlander, & Duncan, 2014), characterisation
methods and related risk management aspects. The expert
group have published a number of papers, particularly in
the area of characterisation of NPs released from FCMs
(Noonan, Whelton, Carlander, & Duncan, 2014) and the
use of gastro intestinal models to assess the digestion and
absorption of ENPs release from FCMs (Lefebvre et al.,
2014). A particular strength of the review carried out by
Lefebvre et al. (2014) is the presence of an example
approach for the assessment of the uptake of NMs in the
human gastro intestinal tract (GIT). The model accounts
for In vivo animal models, Ex vivo tissue models, In vitro
cell culture models, In vitro non-cellular fluid models and
In silico computational models. Each of these elements
can be used to strengthen an overall methodology for the
assessment of NP release from FCMs and subsequent hu-
man exposure.
A comprehensive human exposure framework for fla-
vours, additives and FCMs has recently been published un-
der the FACET project (European Commission (EU),
2012). The framework combines European consumer sur-
veys with toxicity studies to allow for the risk assessment
of existing and emerging materials. A major downfall of
the framework is the exclusion of nanomaterials in the
list of contaminants. However, the project has the potential
to be used as a methodology for the human risk assessment
of nanomaterials. There is a growing need for a framework
dealing with human exposure to NPs in FCMs. Barriers to
such a framework being established include; gaps in knowl-
edge related to ENP migration, ENP physicochemical prop-
erties, human toxicity and the fate of ENPs in the GIT.
Fate of nanoparticles in the GIT
In the human body there are three main routes of exposure
from ENPs, these are dermal contact, inhalation and inges-
tion. Other uncommon routes of exposure which have
recently become applicable, due to emerging ENP medicines
 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
and hygiene products, are through rectal administration,
through the female genital tract and by direct administration
into the blood by injection (Chen & Schluesener, 2008).
There are numerous scenarios in which humans can be
exposed to NPs through any of aforementioned routes. For
example, a study on the levels of vinyl chloride from PVC
in a domestic water supply found that the vinyl chloride
could be ingested and also inhaled from shower water due
to the formation of aerosols (Lee et al., 2002). In this review
the principal focus is on ENP exposure via the oral route of
exposure. It should be noted that although the possible risk to
humans from oral exposure to ENPs are great, studies that
focus on oral exposure and the fate of ENPs in the GIT are
limited (Silvestre et al., 2011). At present there are no
in vivo studies related to the toxicity of ENPs to the human
body through the ingestion route. Therefore, the toxicity of
ENPs in the GIT has been investigated by means of in vivo
studies of rodents (Kim et al., 2008; Park, Bae, et al.,
2010; Park, Marsh, et al., 2010), in vitro studies on represen-
tative human GIT cells (Aueviriyavit, Phummiratch, &
Maniratanachote, 2014) and in vitro studies of ENPs when
exposed to a synthetic human stomach (Rogers et al.,
2012). Each independent study has the potential to contribute
to a broader investigation into the toxicity of ENPs for hu-
mans. However, few studies have linked the numerous frag-
mented studies to build a general human exposure model for
ENPs in food packaging materials.
The ambiguous nature of ENP fate in the GIT has not
aided the acceptance of ENPs in food packaging applica-
tions. Recent studies presenting data on important GIT
mechanisms have shown similarities concerning ENP
behaviour. Rogers et al. (2012) carried out in vitro studies
on the exposure of EAgNPs to a synthetic human stomach
and the effects of synthetic human stomach fluid on the
agglomeration of NPs (Rogers et al., 2012). Following a
1 h exposure period it was noted that EAgNPs agglomer-
ated and reacted with the synthetic stomach fluid to form
silver chloride (AgCl). It was noted that the results may
not have been representative of a human stomachs expo-
sure to NPs due to the effects of some of the coating com-
pounds used during the preparation of the EAgNPs.
Similarly, Mwilu et al. (2013) carried out an in vitro study
on the influence of synthetic stomach fluid on EAgNPs
with different sizes and capping agents. Significant aggre-
gation was noticed, particularly in relation to the smaller
ENPs (<10 nm) in comparison to the larger particles
(75 nm). A significant difference was also observed be-
tween the agglomeration of EAgNPs prepared in house
(pvp-stabilized) to those obtained from a commercial
source.
Another important factor influencing the uptake of NPs
into the GIT is the transit time of food after ingestion. In a
review of different models of the human gastric and small
intestinal digestion system, Guerra et al. (2012) gives a
detailed break-down of the time required for food to
pass through the GIT. When food passes into the stomach
Please cite this article in press as: Hannon, J. C., et al., Advances and challenges for the use of engineered nanoparticles in food contact materials, Trends in
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11
it is exposed to hydrochloric acid (HCL), pepsin and
gastric lipase at a pH of between 1 and 5 for approximately
15 min to 3 h. It is then discharged to the small intestines
where it is exposed to a higher pH of between 6 and 7.5 for
2 to 5 h. Lastly it is passed to the colon were it is exposed
to a pH of 5e7 for 12e24 h before being removed from
the body (Guerra et al., 2012). Both the time and pH
that the food is exposed to while passing through the
GIT generates a number of questions in relation to the
fate of ENPs passing through the GIT. Time, ionic
strength, pH and increased temperature are known to cause
aggregation of ENPs as well as increased aggregate diam-
eters (Liu, Surawanvijit, Rallo, Orkoulas, & Cohen, 2011;
Majedi, Kelly, & Lee, 2014). This could possibly affect the
toxicity or even migration of ENPs within the human body.
Furthermore, it was suggested that the digestion of food-
stuffs may take place in the nanoscale implicating that
the human body has the potential to process such ENP sub-
stances (Chaudhry et al., 2008). Regardless of the ability
of ENPs to aggregate and cause harm within the GIT, there
are further worries in relation to the fate of NPs in the GIT
such as the ability of ENPs to penetrate the natural barrier
in the GIT and accumulate in organs potentially forming
harmful doses. Fr€ohlich and Roblegg (2012) presented a
review of human exposure to ENPs from consumer prod-
ucts through oral ingestion, with a focus on models
demonstrating the ability of NPs to penetrate the natural
barrier within the GIT. Most notably, ENP size is investi-
gated as a major factor influencing the permeation of nat-
ural mucus layers in the GIT. From existing studies, it can
be deduced that the toxicity to humans from exposure to
ENPs will remain the subject of scepticism until In vivo
studies are available. Another aspect which effects the
toxicity of ENPs to humans is the ability or inability of
ENPs to migrate from food packaging to food.
Nanoparticle migration
Migration refers to the release of a substance from one
medium to another. Following Fick’s first law of diffusion,
the substance will migrate due to a concentration gradient
between both mediums (Simon et al., 2008). If there are
no ENPs present in the food, any ENPs that are loosely
bound in the food packaging will migrate from the pack-
aging to the food. This occurs due to the lower concentra-
tion of ENPs in the food which drives migration. Factors
that affect migration include temperature, time, concentra-
tion gradient, material properties, migrant position in the
material and the interaction between the migrant and mate-
rial. The migration potential and diffusion mechanisms for
ENPs from food packaging materials is an area of nano-
technology which has not received the same attention as
such areas as nano-aerosols (Savolainen et al., 2010),
nano-fluids (Mohammed, Al-aswadi, Shuaib, & Saidur,
2011) and nano-medicines (Lehner, Wang, Marsch, &
Hunziker, 2013).
12 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
Experimental migration studies
Until recently, numerous nanocomposite food packaging
related articles (de Azeredo, 2013; Echegoyen & Ner
ın,
2013; Rhim et al., 2013) have been unsuccessful in high-
lighting the increasing number of ENP migration studies
(see Table 3). Several studies are present in the literature as-
sessing the migration of ENPs from polymer food pack-
aging to real food matrices and simulants. For example,
the migration of EAgNPs and Ag-based ENP combinations
are the most widely studied from packaging materials such
as PVC (Cushen et al., 2013), PE (Huang et al., 2011;
Song, Li, Lin, Wu, & Chen, 2011; von Goetz et al.,
2013), low density polyethylene (LDPE) (Echegoyen &
Ner
ın, 2013; Panea, Ripoll, Gonz
alez, Fern
andez-Cuello,
& Albert
ı, 2014), PP (Echegoyen & Ner
ın, 2013; Hauri
& Niece, 2011) and also biodegradable materials such as
modified PLA (Busolo et al., 2010; Fortunati, Peltzer,
Armentano, Jim
enez, & Kenny, 2013; Fortunati et al.,
2014) and starch based biopolymers (Avella et al., 2005).
The majority of studies have concentrated on the incorpora-
tion of ENPs into food packaging materials to avail of
improved antimicrobial effects. In contrast, Avella et al.
(2005) focussed on the improved biodegradability of starch
based polymers containing MMT ENPs and Fortunati et al.
(2013) examined the improved oxygen barrier properties of
PLA containing pristine s-CNC and EAgNPs. Although the
focus of migration studies is to assess the risk posed to hu-
mans through unintentional ingestion of ENPs from FCMs,
two of the studies (Huang et al., 2011; Song et al., 2011)
don’t compare the low levels of migration observed, to
migration limits set by the European Commission
(European Commission (EU), 2011) or another regulatory
body. Furthermore, only four of the studies (Cushen
et al., 2013, 2014a; von Goetz et al., 2013; Smirnova
et al., 2012) included models for human exposure to ENPs.
Even though different approaches were employed for
each migration study certain aspects are similar. The use of
food simulants is a commonality between almost all of the
migration studies. A major benefit of using food simulants
is that they cover a wide range of food types which allows
for a comprehensive human exposure assessment when
coupled with consumption data. Additionally, increased
migration from using fatty or acidic food simulants produces
a worst case scenario, adding a safety factor to human expo-
sure assessment. Real food matrices such as chicken and
turkey meat have been used to test the antimicrobial effect
of active packaging (Contini et al., 2012; Cushen et al.,
2013), however, it was pointed out by Contini et al. (2012)
that the lower fat content of the turkey meat reduces the
diffusion of antioxidants into the meat. In a migration study
both chicken and turkey meat would not be a model food
matrices for testing, as reduced diffusion could possibly
cause the overall migration to be underestimated. A benefit
of pairing real food matrices with the packaging in which
they are sold, is that a human exposure assessment can be
carried out for that particular food application.
Please cite this article in press as: Hannon, J. C., et al., Advances and challenges for the use of engineered nanoparticles in food contact materials, Trends in
Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
Depending on the desired outcome of the study, migra-
tion can be determined in terms of an overall migration
limit (OML) or a specific migration limit (SML). An over-
all migration study is used to clarify that no packaging ad-
ditive or contaminant migrates from the packaging to food.
Specific migration studies involve the analysis of a partic-
ular migrant from packaging. With a focus on presenting
a worst case migration scenario as well as a most likely sce-
nario, multiple packaging and environmental factors have
been investigated; mainly storage time, storage tempera-
ture, ENP percentage fill and ENP size. Natural light has
the potential to degrade polymers via photo-oxidation and
increase migration of substances from those polymers in
applications involving long term exposure (Kumar,
Depan, Singh Tomer, & Singh, 2009). However, due to
the short exposure period for food packaging in service it
is unlikely that natural light will cause significant deteriora-
tion and have any effect on migration. Few studies have
considered the increased migration from packaging in sce-
narios of repeated use (von Goetz et al., 2013). This is sur-
prising given the number of studies which have determined
the migration from reusable food storage containers such as
lunch boxes and re-sealable bags. Directive 10/2011/EEC
(European Commission (EU), 2011) states that for articles
destined for repeated use, three repeated migration tests
should be carried out using a fresh food simulant sample af-
ter each repetition. Disregarding such conditions could
potentially lead to underestimated migration levels.
The use of combinations of ENPs in packaging films has
been found to affect the migratability of substances. In
studies on PLA modified with pristine CNC and including
EAgNPs, it was found that the migration of Ag was faster
in the samples that had been modified with the CNC nano-
crystals (Fortunati et al., 2013). The inclusion of the modi-
fied nanofiller with a high affinity for PLA consequently
resulted in higher Ag ion mobility and increased migration.
Studies are also available which focus on the detection of
Ag ion migration specifically and not ENP migration
(Kumar, Howdle, & M€unstedt, 2005; Mart
ınez-Abad,
Ocio, Lagar
on, & S
anchez, 2013; Fernandez, Soriano,
Hernandez-Munoz, & Gavara, 2010). Given the number
of migration studies to date, it is remarkable that no frame-
work has been generated to deal with the migration of
ENPs from food packaging materials. This could be attrib-
uted to a lack of applicable numerical models or the rapid
development of ENP polymer composites for food pack-
aging applications.
Mathematical migration models
In terms of migration modelling, a mathematical model
provides an analytical formula containing a compact rela-
tionship between relevant variables in a system. Numerical
models are applied in situations where mathematical
models cannot be solved analytically and involve an itera-
tive computational procedure (Barnes & Chu, 2010). Math-
ematical and numerical models can be highly beneficial
 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
when used for ENP migration modelling as they can pro-
duce comparable migration results, for a range of different
system conditions. There is the potential for mathematical
and numerical models to be used as an alternative for costly
and time consuming migration studies. Currently there is
only one mathematical model (Simon et al., 2008) which
focusses specifically on ENP migration from polymer
food packaging to food. Simon et al. (2008) presented gen-
eral equations for the migratability, diffusion rate and
amount of migrating particles. The type of ENP was not ac-
counted for. Instead the size of the ENP and the viscous
properties of the polymer were used. The interphase be-
tween the packaging and food was assumed to present no
obstacle to the migration of ENPs. The wide-ranging appli-
cations of the mathematical model are a significant advan-
tage, giving an insight into the probability of ENPs
migrating from popular polyolefin packaging materials.
However, neglecting specific characteristics of ENPs on a
case-by-case basis has the potential to cause errors in the
results. There are a number of mathematical models which
deal with migrants which are of nanoscale dimensions such
as monomers (Helmroth, Rijik, Dekker, & Jongen, 2002;
Lickly, Rainey, Burgert, Breder, & Borodinsky, 1997).
Helmroth et al. (2002) presents a critical review of existing
migration models for regulatory purposes. ENPs are not
specifically mentioned in the review, however, certain poly-
mer monomers are listed as possible migrants which are of
nanoscale size. Deterministic, stochastic and worst case
mathematical models were critically reviewed on the basis
of migration prediction. They concluded that although
mathematical models allowed for cost and time saving
when compared to experimental migration studies, it is still
necessary to confirm migration quantities with experi-
mental studies. Similarly, Lickly et al. (1997) examines
the limitations of mathematical models dealing with the
migration of acrylonitrile and styrene monomers from
food packaging materials (Lickly et al., 1997). From the
migration predictions an estimate of US consumer exposure
to both monomers was created. Assuming that ENPs follow
the laws of Fickian diffusion, models generally dealing
with the diffusion of additives and contaminants could be
applied to ENP diffusion. Mathematical models have
been used to model the migration of phenolic antioxidants
from polypropylene (Hamdani, Feigenbaum, & Vergnaud,
1997) and general food additives and contaminants from
food packaging films (Chung, Papadakis, & Yam, 2002).
Fortunati et al. (2013) calculated the diffusion coefficients
for PLA modified with s-CNC nanocrystals with nanosilver
using the migration model described by Chung et al. (2002)
showing the broad applicability of the model.
Numerical migration models
Numerical models dealing with ENP migration from
packaging to food are lacking. To date, a numerical model
presented by von Goetz et al. (2013) is the only model
which deals with ENP migration from food packaging.
Please cite this article in press as: Hannon, J. C., et al., Advances and challenges for the use of engineered nanoparticles in food contact materials, Trends in
Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
13
The numerical model is a 2D Lagrangian Particle
Tracking Model (LPTM) which was adapted from a model
predicting the “Influence of Dead-Water Zones on the
Dispersive Mass Transport in Rivers” (Weitbrecht, 2004).
The model assumes Fickian diffusion and takes account
of the ENP diffusion from within the polymer to the plas-
tic/liquid interphase. What occurs beyond the interface as
well as leaching effects of liquid food matrices are
excluded from the model. The affect that the penetration
of food has on migration of particles from food packaging
is a major factor that has been intentionally neglected in
all the aforementioned migration models (Hamdani
et al., 1997).
Regulation due to possible migration
Due to uncertainties in relation to ENP migration, a
number of regulatory bodies have placed strict regulation
on the use of ENPs in FCMs. In each region, regulatory au-
thorities have taken their own approach to manage the com-
mercialisation of ENP FCMs, whether it is in the form of a
guidance document, specific FCM regulation or amend-
ment to existing FCM regulations. Regions such as
Australia, New Zealand, United States of America, Euro-
pean Union and Canada have made amendments to current
FCM legislation and have provided general guidance docu-
ments for nanomaterials. For countries such as Brazil,
Argentina, China, Japan and Mexico there has been limited
regulation related to nanomaterials. None of the aforemen-
tioned countries have established regulations specific to
ENPs in FCMs (Magnuson et al., 2013). In Australia and
New Zealand the Food Standards Australia New Zealand
has amended its Application Handbook (Food Standards
Australia New Zealand [FSANZ], 2013) to include FCMs
containing substances in the nanoscale. Health Canada
has provided a guidance document for nanomaterials in
general (Health Canada [HC], 2011). Prior to 2004, Euro-
pean Union regulations related to the application of nano-
materials in FCMs were limited. Regulation No. 1935/
2004 of the European Parliament was the first regulation
to deal with active and intelligent materials intended to
come into contact with foodstuff. ENPs were not mentioned
specifically, but were instead accounted for under the terms
‘active’ and ‘intelligent’ materials. European Commission
Regulation No. 10/2011 (European Commission (EU),
2011) was brought about amending and consolidating EU
Directive 82/711/EEC (European Commission (EU),
1982) and 85/572/EEC dealing with migration studies and
food simulants. In Regulation No. 10/2011 it is stated
that any substance which can migrate from food packaging
to food must not exceed the limit of 10 mg/dm2 of the
FCM. Included among the list of substances for use in
FCMs are active and intelligent materials which includes
nanomaterials (European Commission (EU), 2011). The
limit of migration for a specific substance can be altered
in the event that a risk assessment is carried out which
shows a higher overall level of migration. The current status
14 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20

of NP FCM regulation is outlined in Fig. 1. The United
States Food and Drug Administration (USFDA) regulate
the use of nanomaterials in FCMs in the United States of
America. According to the USFDA in a recent guidance
document (United States Food and Drugs Association
[USFDA], 2014), for a new FCM to be made commercially
available the product manufacturer must provide a safety
assessment which includes studies on humans and animals
evaluating its safety under the worst case conditions of use.
Furthermore, studies must also distinguish the food sub-
stances identity, stability, purity, potency, performance
and usefulness. Throughout the document it is stressed
that the reduction of any substance to the nanoscale is
considered a significant deviation from conventional
manufacturing processes and consequently merits partic-
ular examination. In such cases, safety evaluations should
be accompanied by toxicity studies specific to the substance
and should not use data extrapolated from conventionally
manufactured substances. An important point is that the
USFDA states that it does not make generalisations related
to the harmfulness of all products containing nanotech-
nology but instead encourages industry to provide specific
risk assessment so that products can be assessed on a
case-by-case basis.
When dealing with polymer food packaging including
nanomaterials, an important argument is that although
agglomeration of ENPs during synthesis can be problem-
atic, once the polymer has been formed the ENPs are prac-
tically immobilized (Yang, 2003). This characteristic can
be beneficial in terms of reducing the risk to humans
from exposure to NPs which have migrated from food
packaging to foodstuffs (Savolainen et al., 2010). Immobi-
lization can also hinder the antimicrobial properties that are
migration dependant. It is the basis for the recent accep-
tance of TiN ENPs for use in PET bottles up to 20 mg/kg
by the European Food Safety Authority (EFSA). This is

Fig. 1. Schematic illustration of the current status of food contact material legislation in the European Union.

Please cite this article in press as: Hannon, J. C., et al., Advances and challenges for the use of engineered nanoparticles in food contact materials, Trends in
Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
 J.C. Hannon et al. / Trends in Food Science & Technology xx (2015) 1e20
as a result of a specific risk assessment on the novel food
packaging material conducted by ColorMatrix group
(EFSA, 2012). The study found that TiN ENPs did not
migrate from PET bottles in any harmful amount under a
range of time and temperature conditions. As a result of
the positive outlook from the risk assessment, TiN ENPs
were added to the EFSA 21st list of substances for FCMs
(EFSA, 2008). The acceptance of TiN ENPs in PET bottles
shows promise for the acceptance of other nanomaterials
for food contact applications in the future.
Conclusion
In recent years, ENP food packaging technologies have
been the focus of attention due to their associated benefits.
Development has increased exponentially with industry,
academia and regulatory bodies contributing to the uptake
of the technology in the food industry. However, the
increased use of ENP food packaging is being impeded by
uncertainty surrounding ENP toxicity and bioaccumulation.
For society to accept ENP technologies human risk assess-
ment must indicate an acceptable level of risk for the tech-
nology in question under the worst case scenario of use.
The level of risk should then be clearly communicated to
regulatory bodies and the consumer to allow them to make
an informed decision on the use of the product. In light of
the increasing numbers of ENP migration studies, only three
studies have presented human exposure assessment models
for unintentional uptake of ENPs from active food pack-
aging (Cushen et al., 2013, 2014a; von Goetz et al., 2013;
Smirnova et al., 2012). Given the uneven ratio of migration
studies (19) to human exposure assessments (4) it can be
seen that more emphasis needs to be placed on presenting
comprehensive exposure data that could be informative to
regulatory bodies and the consumer.
In the area of ENP food packaging, developments have
materialized at a relentless rate. Methodologies for ENP syn-
thesis are emerging with higher yields, greater size control,
decreased environmental impact and improved industrial
viability. Additionally, novel antimicrobial nanocomposites
are being developed using bioavailable materials from food
and plant extracts which eliminate some of the toxic and reg-
ulatory issues related to metal and metal oxide nanocompo-
sites. New sources of NPs from food and plants are being
investigated which are readily available in large quantities
and may not have the same public perception and toxicity
as metal derived ENPs. There is presently no migration study
or human risk assessment that deal with food and plant
derived ENPs incorporated into food packaging.
In the literature, knowledge gaps are present in a number
of areas. The majority of studies have had an undeviating
focus on packaging with ENPs incorporated within poly-
mer substrates. Presently, only two studies have assessed
the migration of ENPs from antimicrobial food packaging
coatings (Nobile et al., 2004; Smirnova et al., 2012). Given
the clear benefits of using surface coatings it is surprising
that limited studies are available. Currently there are no
Please cite this article in press as: Hannon, J. C., et al., Advances and challenges for the use of engineered nanoparticles in food contact materials, Trends in
Food Science & Technology (2015), http://dx.doi.org/10.1016/j.tifs.2015.01.008
15
mathematical or numerical models for NP migration pre-
diction from the surface of packaging. Similarly, no human
exposure models or frameworks exists for packaging ENP
surface coatings. Although the European Commission
have imposed strict regulations on the migration of unau-
thorized contaminants from FCMs in applications involving
particularly susceptible persons, no studies have focused on
applications such as infant FCMs.
Following the recent release of the FACET exposure tool
it has become apparent that a similar framework specific to
ENPs would be highly beneficial to industry, consumers
and regulatory bodies. A framework would allow for the
amalgamation of data from the multiple fragmented migra-
tion and toxicity studies, establishing a footing for the safe
uptake of ENP polymer composites in the food packaging
industry.
Acknowledgements
This work was funded under the Food Institutional
Research Measure (FIRM) as administered by the Irish
Department of Agriculture, Food and the Marine (Project
no. 11/F/038).
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