Molecules: Role of Aunps in Active Food Packaging Improvement: A Review

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molecules

Review
Role of AuNPs in Active Food Packaging Improvement:
A Review
Hamed Ahari 1, * , Mostafa Fakhrabadipour 2 , Saeed Paidari 1 , Gulden Goksen 3 and Baojun Xu 4, *

1 Department of Food Science and Technology, Science and Research Branch, Islamic Azad University,
Tehran 1477893855, Iran
2 Department of Food Science and Technology, Qeshm Branch, Islamic Azad University,
Qeshm 7953163135, Iran
3 Department of Food Technology, Vocational School of Technical Sciences at Mersin Tarsus Organized
Industrial Zone, Tarsus University, Mersin 33100, Turkey
4 Food Science and Technology Program, Department of Life Sciences, BNU-HKBU United International
College, Zhuhai 519087, China
* Correspondence: dr.h.ahari@gmail.com (H.A.); baojunxu@uic.edu.cn (B.X.)

Abstract: There is a worldwide concern about food loss due to reduced shelf life among food science
researchers. Hence, it seems that any techniques contributing to improved food packaging are most
welcome in the food sector. It has been demonstrated that the administration of nanotechnology-based
techniques such as metal-based nanoparticles can fade away the unresolved obstacles in shortened
shelf life and environmental concerns. Along with substantial signs of progress in nanoscience,
there is a great interest in the usage of green synthesis-based methods for gold nanoparticles as the
most advantageous metals, when compared to conventional chemistry-based methods. Interestingly,
those aforementioned methods have significant potential to simplify targeted administration of gold
nanoparticles due to a large surface-volume ratio, and diminished biohazards, aimed at increasing
stability, and induction of anti-microbial or antioxidant properties. However, it is necessary to
Citation: Ahari, H.; Fakhrabadipour,
consider the hazards of gold nanoparticles including migration for food packaging purposes.
M.; Paidari, S.; Goksen, G.; Xu, B.
Role of AuNPs in Active Food
Keywords: antimicrobial effects; food packaging; gold nanoparticles; nanotechnology; shelf life
Packaging Improvement: A Review.
Molecules 2022, 27, 8027. https://
doi.org/10.3390/molecules27228027

Academic Editors: Reshma B 1. Introduction


Nambiar, Rotimi Sadiku Emmanuel
It has been demonstrated that there is a worldwide concern about the growing rate of
and Anand Babu Perumal
food loss related to perishable food [1,2]. Results acquired from those surveys depict that
Received: 2 October 2022 expiring on the shelves of food stores makes problematic challenges leading to food loss [3].
Accepted: 9 November 2022 In other words, food spoilage is accelerated by several microbial activities, and enzymatic
Published: 18 November 2022 activation of oxygen-driving processes [4]. Accordingly, these issues are addressed in
Publisher’s Note: MDPI stays neutral imposing a financial burden on the economy, health system, environment, and even on
with regard to jurisdictional claims in recycling industries [5]. Thereafter, it seems legal to move forward to the establishment of
published maps and institutional affil- any technological approaches aimed at the improvement of food quality.
iations. Proper food packaging (FP), which is traced back to the 18th century, can play an
indispensable role in the prolongation of shelf life of food products [6], and also preserves
nutritional values during various stages such as transport, distribution, and storage [3].
Additionally, reduction of microbial contamination especially during harvesting, process-
Copyright: © 2022 by the authors. ing, slaughtering, and packaging steps in developing countries, is of high practical and
Licensee MDPI, Basel, Switzerland. industrial importance [1,7,8].
This article is an open access article As mentioned earlier, there is an imperative need for signs of progress toward more
distributed under the terms and
efficient biotechnology-based applications in FP. A wide range of technologies including
conditions of the Creative Commons
biomaterials and nanotechnology are utilized in FP [9]. Many researchers have focused on
Attribution (CC BY) license (https://
the employment of nanotechnology for food packaging purposes (Figure 1) [10].
creativecommons.org/licenses/by/
4.0/).

Molecules 2022, 27, 8027. https://doi.org/10.3390/molecules27228027 https://www.mdpi.com/journal/molecules


Molecules 2022, 27, 8027 2 of 23

Molecules 2022, 27, 8027 2 of 22


biomaterials and nanotechnology are utilized in FP [9]. Many researchers have focused
on the employment of nanotechnology for food packaging purposes (Figure 1) [10].

Figure 1. A schematic presentation of nanotechnology applications in daily life.


Figure 1. A schematic presentation of nanotechnology applications in daily life.

Nanotechnology in
Nanotechnology in FP
FP has
has aa wide
widearrayarrayof ofadvantages,
advantages, including
including making
making aa barrier
barrier
between the content of the food and exterior atmosphere [11],
between the content of the food and exterior atmosphere [11], and assuring prevention and assuring prevention of
possible post-contamination of food, aimed at potential production
of possible post-contamination of food, aimed at potential production and processing of and processing of
healthier, safer,
healthier, safer,andandhigh-quality
high-qualityfoods foods[12].[12]. There
There isis aawide
widerange
rangeof ofnanoparticles
nanoparticles thatthat
are extensively
are extensively employed
employed in infood
foodpackaging
packagingsystems systems with
withdistinct purposes
distinct purposes including
includingan-
tibacterial [13],
antibacterial gasgas
[13], scavenging
scavenging [14], antioxidant
[14], antioxidant [15], andand
[15], barrier properties
barrier [16] [16]
properties while con-
while
sidering food
considering quality
food qualitydetectors
detectors as smart
as smart food packaging
food packaging systems
systems[17]. Metal
[17]. nanoparticles
Metal nanoparti-
(e.g., Ag, Au, Cu, CuO, Zn, ZnO, TiO ), nano clay [18], nanoemulsions
cles (e.g., Ag, Au, Cu, CuO, Zn, ZnO, TiO2 ), nano clay [18], nanoemulsions (e.g.,
2 (e.g., essential oil
essential
of of
oil plants
plantssuch
such asasrosemary,
rosemary,ginger)
ginger)metal-organic
metal-organic frameworks (MOF) (MOF) [19]
[19]are known as
are known as
themost
the mostemployed
employednanoparticles
nanoparticlesin inFP
FPsystems
systems[13].
[13].
Amongst the existing nanoparticles,
Amongst nanoparticles,metal-based
metal-basednanoparticles
nanoparticleshave haveattracted
attractedthethe
at-
attention
tention ofofscientists
scientiststotoincorporate
incorporate with with the the biomaterials
biomaterials to makes suitable
suitable packaging.
packaging.
Considering
Consideringmetal-based
metal-based nanoparticles,
nanoparticles, gold gold nanoparticle
nanoparticle (Au)(Au) has
has shown
shown noticeable
noticeable po-
tential
tentialininimproving
improving food food packaging
packaging systems
systems from from the
the viewpoint
viewpoint of antibacterial activity,
activity,
improving
improvingbarrier
barrierproperties,
properties,usingusing asas
biosensors,
biosensors, scavenging
scavenging andand
so on. TheThe
so on. incorporation
incorpora-
of AuNPs
tion of AuNPsinto polymeric
into polymericcomposites playsplays
composites a crucial role inrole
a crucial theinactive packaging
the active of food.
packaging of
Recently, incorporation
food. Recently, of AuNPs
incorporation and grapheme
of AuNPs oxide separately
and grapheme on PVAon
oxide separately (polyvinyl alco-
PVA (polyvi-
hol) composite
nyl alcohol) films on banana
composite films ondemonstrated
banana demonstratedantimicrobial activity against
antimicrobial Escherichia
activity coli.
against Esch-
Banana shelf life was qualitatively enhanced with PVA-glyoxal-AuNPs
erichia coli. Banana shelf life was qualitatively enhanced with PVA-glyoxal-AuNPs nano- nanocomposite for
preserving food, validating its application in food packaging [18]. In another study, AuNPs
conjugated with gallic acid (GA-AuNPs) were examined as an effective and promising
strategy for reducing oxidative damage and physiological degradation of food products.
Molecules 2022, 27, 8027 3 of 22

The potential capacity to scavenge free radicals and green catalytic activity against microor-
ganisms are features of the compound. Results showed that GA-AuNPs is the safest and
most effective food packaging liner in the food business [13].
In this paper, the main aim is to provide a comprehensive review of the role of gold
nanoparticles (AuNPs) in food packaging systems. In this regard, first, a brief discussion
was presented considering the way nanoparticles are employed in FP systems; then, the
synthesis of AuNPs, and their potential in FP systems are discussed.

2. Search Method
Data of this review study were collected through an online literature review (in the
English language) in Scopus, PubMed, Cochrane, Science Direct, and Google Scholar
databases/search engines by 8 keywords (including 5 main keywords: (Gold nanoparticle,
Au nanoparticle, AND Food Packaging, AND Food Safety), and 3 complimentary keywords
(Anti-bacterial, Anti-oxidant, Shelf life)) commencing from January 2011 until June 2021
time intervals.

3. Synthesis of AuNPs
The modern era of AuNPs synthesis began over 150 years ago with the work of
Michael Faraday, who was possibly the first to observe that colloidal gold solutions have
properties that differ from bulk gold. Among the several forms of NPS created by biological
systems, the gold ones are recognized as being the most compatible and non-toxic to the
human body. Based on their particular characteristics and distinct surface functions, AuNPs
have been used in food packaging. The simplicity of AuNP operation and functionalization
results in a multi-platform in food packaging systems for antibacterial, gas scavenging,
preventing biofilm formation, inhibiting gas permeability, and other purposes [19].
Along with tremendous development in the usage of AuNPs-based approaches in
a variety of FP systems, there are growing concerns about the commercialization of con-
ventional synthesis methods due to environmental or clinical hazards [20]. Over the past
few decades, a wide range of solution-based approaches is employed to control size [21],
shape [22], and surface functionality [23].
However, so far there is no available report regarding the nano-toxicity of biologically
produced gold NPs (AuNPs) in vitro and in vivo. There are several reports regarding the
synthesis of AuNPs via different chemical agents. For instance, citrate and gold salt are two
famous components to produce gold nanoparticles (Equation (1)) [24]. Scientists showed
that environmental condition including temperature affects the AuNPs dimension and their
life cycle. It was reported that citrate and oxidation by-products (e.g., ACDC2− (acetone
dicarboxylate)) promote gathering and bridging Au(III) ions around the AuNPs seeds in
the initial growth step [24].
Equation (1)

2AuCI4 − +3Ctr3− → 2Au + 3ACDC2− +3CO2 ↑ +8CI− +3H+ (1)

ACDC2− can be converted to acetone at 100 ◦ C according to Equation (2). However,


past studies approved that the products from the Equation (2) can react with auric chloride
and cause complete conversion to produce Au0 (Equation (3)) [24,25].
Equation (2)

100 ◦ C
ACDC2− +2H2 O → acetone + 2CO2 ↑ +2OH− (2)

Equation (3)

100 ◦ C
4 AuCI4 − + 6H2 O + 3 acetone → 4Au + 9CH2 O + 12H+ +16CI− (3)

Summing up Equations (1)–(3), the following equation is obtained in which the effect
of temperature ACDC2− degradation is not considered:
Molecules 2022, 27, 8027 4 of 22

Equation (4)

100 ◦ C
2AuCI4 − +Ctr3− +2H2 O → 2Au + 3CH2 O + 3CO2 ↑ +8CI− +3H+ (4)

In another study, Equation (5) has been speculated at room temperature [26]:
Equation (5)
Room temp
6ACDC2− +22AuCI4 − +24H2 O → 22Au + 6CH2 O + 3HCOOH + 21CO2 +88CI− +54H+ (5)

In another research, it was shown that the polarity of the solvent affects the AuNPs
production and their size [26,27]. It was shown that the smaller size of AuNPs was
synthesized in the high polarity index of the ethanol/water solvent as the reaction medium,
while the bigger size of AuNPs was synthesized in the low polarity index. Polarity can be
calculated from Equation (6) [28].
P0 = ∑ pi0 φi (6)
In which:
pi0 : the polarity index of solvent i in the mixture;
φi : the volume fraction of solvent i in the mixture.
It is mandatory to diminish concerns about by-products as toxic chemicals and in-
crease the stability of AuNPs. It has been demonstrated that it is necessary to consider safe
and cost-effective methods and pave the path for the brisk emergence of green synthesis of
AuNPs [29–31]. There is a relationship between the functions of AuNPs and life cycle eval-
uation on their environmentally friendly nature. It seems that employing green synthesis
of AuNPs is of great prominence due to sustainable and renewable suppliers of chemical
energy [32]. There are several benefits in green biosynthesis procedures to synthesize
AuNPs, when compared with classical chemistry methods. Those aforesaid biological
resources act as nano-factories with less reaction time, size-controlled capability, and high
acceptability [33]. Among the types of NP production techniques, the biological method
is widely accepted because the use of the living organisms in the production pathway is
safer than other methods. In the rest, two techniques (using microbial strains and using
leaf extract) for the green synthesis of AuNPs are discussed.
The aqueous reduction of gold salts with sodium citrate is one of the most typical
techniques for the production of AuNPs [34], compared to the shape-controlled synthesis of
AuNPs [35]. It has been demonstrated that reagents acting as reducing and stabilizing ones
such as chitosan [36] or alginate can serve as the most efficient reagents for the fabrication
of AuNPs in situ [37,38].
As a prime study conducted by Irshad A. Wani et al., they tried to evaluate the size
and shape-dependent anti-fungal activity of various AuNPs [39].
Those recruited AuNPs were different in their reducing agents affecting particle
size, morphology, and properties of nanoparticles under similar ultrasonic frequency
circumstances and without using any stabilizer [40]. Accordingly, two types of AuNPs,
including gold nanodiscs of the average diameter of 25 nm (tinchloride as reducing agent),
and polyhedral (nanocrystal) structure of the average size of 30 nm (sodium borohydride
as reducing agent), were used in this study. Gold nano-discs reveal a much higher surface
area and stronger fungicidal activity through inhibition of H+-ATPase against Candida
albicans (C. albicans) [41].

3.1. Biosynthesis of AuNPs Using Microbial Strains


Researchers have a strong interest in the use of microbial strains, such as bacterial,
due to their manageability and cost-effectiveness [41], actinomycete [42,43], fungal [44],
algal [45], and yeast strains [46], for development of AuNPs for food packaging purposes.
As it was pointed out before, in addition to the existence of phytochemicals in plants,
there are other co-chemical substances synergized with phytochemicals agents such as
Molecules 2022, 27, 8027 5 of 22

citrate or cetyltrimethyl ammonium bromide (CTAB), being affected by photomutagenicity


processes in AuNPs [47].
Results from the microbial study show that biosynthesis of AuNPs using microbial
strains (such as Shewanella oneidensis) can be considered as highly efficient bio-reduction-
based fabrication approaches [48].
It was reported that Bacillus subtilis could reduce Au3+ ions to AuNPs. The AuNPs
size was reported between 5 and 25 nm inside the cell walls [49]. In an experimental study,
Baker Syed et al. [50] investigated the synthesis of AuNPs from endophytic Pseudomonas
fluorescence 417 inhabiting Coffea arabica L., and the assessment of their biological (anti-
microbial) activities against clinically significant pathogens. AuNPs were confirmed by
hyphenated techniques such as ultra violet (UV)-visible spectrophotometry (changing color
of reaction from yellow to ruby red within 5 min of incubation), XRD, TEM, and FTIR
(majorly in a spherical shape) [50]. Those AuNPs showed the most antibacterial properties
against P. aeruginosa (MTCC 7903), E. coli (MTCC 7410), S. aureus (MTCC7443), B. subtilis
(MTCC 121), and Klebsiella pneumoniae (K. pneumoniae) (MTCC 7407), respectively (results
confirmed by colony forming unit (CFU) method and antibiogram tests). According to
the results acquired from this study, the authors introduced such methods as efficient
alternatives for the treatment of MDR strains [50].
In another study, Pourali and her colleagues employed two microorganisms (Bacillus
cereus and Fusarium oxysporum) for the biosynthesis of AuNPs and compare their nanotoxic-
ity under in vitro assays [51]. In this study, the authors added 100 microliters of HAuCl4 to
the 100 mL of the separated microbial supernatant and incubated shaker incubator for 24 h
at 37 ◦ C and 200 rpm. Both strains showed success in AuNP synthesis. Results revealed
that the AuNPs produced by both strains were hexagonal, spherical, and octagonal with
sizes of around 20–50 nm and irregular contours.
Singh and his colleagues reported AuNPs production using Rhodopseudomonas capsulata
and Pseudomonas aeruginosa bacteria [52] under pH values from 4 to 7. They reported that
pH value was the important parameter to control the shape and size of AuNPs. The
produced AuNPs had a spherical shape and a diameter between 20 and 80 nm at pH 6.5.
They also reported that the spherical AuNPs with the size of 10–20 nm were produced at
pH = 7 while many nanoplates were detected at pH = 4. Shewanella algae were found to
reduce Au3+ ions forming 10–20 nm AuNPs extracellularly with the assistance of hydrogen
gas [52,53]. On the other hand, the AuNPs have been prepared on the surface of bacteria as
a result of incubation of the cells with Au3+ ions [54].
Fungi were capable of reducing the metal ions such as gold salt into their correspond-
ing nanometals i.e., nanogold either in the intracellular or extracellular state depending
on the position of the reduction enzymes. In other words, the nanoparticles were formed
extra-cellular when the cell wall’s reduction enzymes were responsible for metal ions
reduction and the reduction enzymes are secreted extra-cellular [55]. Sastry and coworkers
have reported the extracellular synthesis of AuNPs by fungus Fusarium oxysporum and
actinomycete Thermomonospora sp., respectively [56].

3.2. Biosynthesis of AuNPs Using Leaf Extract


According to the mentioned advantages for green biosynthesis of AuNPs, there is a
growing trend in the usage of eco-friendly, cost-effective, non-hazardous, and sustainable
methods for the synthesis of AuNPs [57]. As far as a wide arrow of studies is being devoted
to green biosynthesis of nanoparticles, some of them believe that usage of several biopoly-
mers as starch, chitosan, cyclodextrins, or even bacterial biomass [58], or environmental-
based material such as olive-mill wastewater can be incorporated for reduction of AuNPs
by phenolic compounds [59]. There are different industrial and laboratory approaches for
the synthesis of leaf (or other parts of plants such as bark, root, or fruit) extract aimed at
the usage for the biosynthesis of AuNPs [40,60]. They include (a) solvent-based extraction,
(b) microwave-assisted extraction, (c) maceration extraction, and (d) ultrasound-assisted
extraction [40]. In this part, several recently conducted studies aimed at the investigation on
Molecules 2022, 27, 8027 6 of 22

the green biosynthesis of AuNPs by leaf extract or marine algae, are summarized: Rajathi
et al., aimed at investigation of anti-bacterial effects of AuNPs produced by Stoechospermum
marginatum (kützing) as a brown alga in their experimental study [61]. Their results from
transmission electron microscopy (TEM) indicated the presence of majorly spherical shapes
in the nanoparticles with (photoluminescent features) and 45.92% elemental gold. Interest-
ingly, hydroxyl groups were recognized as reduction agents (present in the diterpenoids of
the brown seaweed), effectively acting against bacterial pathogens [61].
In another study by Chidambaram Jayaseelan et al. [62], anti-fungal properties of
AuNPs produced by seed aqueous extract of Abelmoschus esculentus (green biosynthesis of
AuNPs with crystalline nature), was investigated. Puccinia graminis critic, A. flavus, A. niger,
and C. albicans were the fungal strains that were tested. The authors reported that all of the
nanoparticles were spherical with a narrow size range of 45–75 nm. Anti-fungal activities
were observed among all of the fungal strains, especially C. albicans, and Puccinia graminis
with the most inhibition zone (18, and 17 mm, respectively.). The authors concluded that
as this approach is a low-cost, and user-friendly approach (done at room temperature), it
also leads to better control over their nanostructures. This approach could be significantly
considered in nanomedicine, and food packaging industries (as nano-preservative agents).
Marjan Shariari et al. [63], designed their study aimed at biosynthesis, and character-
ization of anti-AuNPs produced by Allium noeanum Reut. ex Regel leaves. The authors
declared that antioxidant compounds in fresh leaves can be responsible for reducing
agents (and forming monodisperse particles), confirmed by Fourier-transform infrared
spectroscopy (FTIR) techniques. Based on the results, not only synthesized AuNPs de-
picted excellent antioxidant potential against 1,1-diphenyl-2-picryl-hydrazyl (DPPH) and
improved solubility, but they also revealed significant non-toxicity properties against
human umbilical vein endothelial cells.
Additionally, it is of high prominence to mention that those synthesized AuNPs in-
dicated antibacterial activities against a wide array of Gram-negative or Gram-positive
pathogens (Streptococcus pneumoniae (S. pneumoniae), Bacillus subtilis (B. subtilis), Staphylococ-
cus aureus (S. aureus), Staphylococcus saprophyticus (S. saprophyticus), Salmonella typhimurium
(S. typhimurium), Pseudomonas aeruginosa (P. aeruginosa), Shigella flexneri, and E. coli O157:H7).
They introduced that leaves extract incubated with aqueous gold ions can be considered as
the most reproducible and biocompatible methods [63].
Jayanta Kumar Patra et al. [64] in their experimental study aimed at the synthesis
of AuNPs from aqueous extract of dried outer onion peel (onion peel as food waste
materials), and assessment of their biological activities. It was reported that various water-
soluble phenolic compounds and cysteine derivatives were responsible for the reduction
of nanoparticles (45.42 nm in diameter). Promisingly, synergistic anti-bacterial (against
five different foodborne pathogenic bacteria), anti-oxidant, and proteasome inhibitory
potentials were reported. They declared that this aforesaid approach can be an eco-friendly,
and nontoxic procedure being able to be conducted in one step.
Annamalai et al. [65] in their experimental study, aimed at the synthesis of AuNPs
from Euphorbia hirta L. leaf extract, and assessment of their biological (anti-microbial) activi-
ties. They recruited surface plasmon resonance (SPR) for characterization and confirmation
of synthesized AuNPs through changing the color of the extract from pale yellow to purple
(nanoparticles with the size varying from 6 nm to 71 nm). Promisingly, anti-bacterial
properties of those synthesized nanoparticles against several bacterial strains of E. coli,
P. aeruginosa, and K. pneumoniae were reported at very low concentrations (tested concentra-
tions varying from 1.25 to 200 g/mL) of nanopowders used for nanoparticles. Interestingly,
complete inhibition on bacterial growth was reported at the highest concentration, and the
most inhibited bacterial growth was reported for K. pneumoniae (94%). They declared that
this aforesaid approach (especially with the usage of combinative aqueous and methanolic
extracts of Euphorbia hirta L. leaf) can be an eco-friendly, a rapidly conducted, and efficient
procedure (due to synergized agents), being potentiated for usage in a wide range of
industries or clinical applications [65].
Molecules 2022, 27, 8027 7 of 22

Several researchs are dedicated to the improvement of the antimicrobial effects of


metal-based nanoparticles, as well as considerable indicators of success in the case of
the combinational use of AuNPs with others. Exemplary examples of these studies are
collected. One comparative experimental study conducted by Priyanka Singh et al. [66]
was aimed at the evaluation of anti-inflammatory properties of spherical silver nanoparti-
cles, and monodisperse hexagonal AuNPs. Those nanoparticles were produced by green
biosynthesis from fruit extract of Prunus serrulata at 80 ◦ C. In their study, nanoparticles
were confirmed and characterized through visual observation (with the appearance of color
change in reaction for silver, and AuNPs, including from ruby red to brown within 50 min,
and from light ruby red to deep purple color within 30 s, respectively), UV-VIS FETEM,
EDX, elemental mapping, FTIR, XRD, and DLS. Criteria for anti-inflammatory effects of
both nanoparticles were inhibition of downstream NF-kB activation in macrophages [66].
Results of MTT assay from this study reported a significantly attenuated expression of
inflammatory mediators such as nitric oxide (NO), prostaglandin E2 (PEG2), inducible
nitric oxide synthase (iNOS), cyclooxygenase-2 (COX-2), and LPS-induced activation of
NF-kB signaling pathway in LPS-induced RAW264.7 cells line as in vitro model. According
to the results acquired from this study, the authors introduce the mentioned approach as an
eco-friendly synthesis with biocompatible nature, being used as novel therapeutics for the
prevention and cure of inflammation [66].
In another comparative experimental study done by R Geethalakshmi et al. [67],
synthesis of gold and silver nanoparticles from Trianthema decandra L. root extract, and
assessment of their biological (anti-microbial) activities were investigated. The shape of
AuNPs was confirmed through FESEM (with the size for gold, and silver nanoparticles
varying from 33 to 65 nm, and 36–74 nm, respectively), and the presence of metallic
gold and silver in the nanoparticles was approved by EDX and FTIR. Phytochemical
constituents were responsible for reducing agents. Both nanoparticles showed significant
anti-bacterial/anti-fungal activities against S. aureus (MTCC 29213), Streptococcus faecalis
(S. faecalis) (MTCC 0459), Enterococcus faecalis (E. faecalis) (MTCC 2729), E. coli (MTCC
443), P. aeruginosa (MTCC 1035), Proteus vulgaris (P. vulgaris) (MTCC 1771), B. subtilis
(MTCC 121), Yersinia enterocolitica (Y. enterocolitica) (MTCC 840), and C. albicans (MTCC 183),
especially in Gram-negative bacteria. Comparatively, the anti-bacterial properties of silver
nanoparticles were more than AuNPs. But both of those fabricated nanoparticles showed
notable anti-bacterial effects on Y. enterocolitica, P. vulgaris, E. coli, S. aureus, and S. faecalis.
They declared that due to the smaller size of AuNPs (varying from 37.7 nm to 79.9 nm)
compared to bacteria, adherence to the bacterial cell wall is simplified and accelerated,
leading to bacterial cell death [67].
In another study conducted by S. Lokina et al. [68], promising results from an investi-
gation on biological (anti-microbial) properties of AuNPs produced from Punica granatum
fruit (pomegranate) extract, were reported. For characterization and confirmation of
AuNPs (with the size ranging from ranges from 5 nm to 17 nm), UV-Vis, fluorescence,
high-resolution AuNPs (HRTEM), XRD, FTIR, selected area electron diffraction (SAED),
and thermogravimetric analysis (TGA), were used. Through SPR, it was found that auric
chloride (chloroauric acid or AuCl4) is the responsible agent for the bio-reduction of AuNPs
(through observing the color change from yellow to black in the reaction mixture) [68].
According to the minimum inhibitory concentration (MIC) assay, they reported an excellent
anti-microbial activity of synthesized AuNPs against C. albicans (ATCC 90028), A. flavus
(ATCC 10124), S. aureus (ATCC 25175), Salmonella typhi (ATCC 14028), and Vibrio cholerae
(ATCC 14033). Additionally, according to the MTT assay, they reported excellent cytotoxic
activity of synthesized AuNPs against HeLa cancer cell lines at different concentrations.
Interestingly, the percentage of cancerous cell death was 98.9% in the presence of the high-
est dose of AuNPs (1000 µg/mL). They introduced the aforementioned green synthesis
method as low cost, non-toxic, and eco-friendly [68]. Table 1 shows a wide range of studies,
aimed at the investigation of green synthesis of AuNPs from plant sources.
Molecules 2022, 27, 8027 8 of 22

Table 1. Several recent studies evaluating on the usage AuNPs from plant sources.

Reducing Microorganisms Wavelength NP Size Year


Plant Source Agents Biological Effects (nm) Shape (nm) (Ref)
prunus
cerasifera Anti-microbial and E. coli, S. aureus, B. Spherical 2021
pissardii extract anti-fungal subtillis, P. aeruginosa, 535 20 [69]
properties and C. albicans. (20 nm)
nigra leaf
Bacillus subtilis,
Staphylococcus aureus, 2021
extract Antimicrobial and Escherichia coli, 517 53.7
licorice root anticancer Spherical [70]
Pseudomonas aeruginosa,
and Salmonella typhi
oplopanone,
γ-eudesmol, Vibrio parahaemolyticus
Turnera hydroquinone- antimicrobial and Aeromonas multiple shapes, 2021
diffusa Willd properties and 540 24 [71]
β-d-glucoside hydrophila mostly spherical
immune response Longfin yellowtail
(arbutin) and
inositol
antibacterial activity
banana pith Alkaloids, Bacillus subtilis, E. coli, 530–560 470 2021
extract Flavonoids and catalytic Pseudomonas aeruginosa spherical [72]
reduction
alkaloids, Bacillus cereus, Klebsiella
Ricinus terpenoids, 550 100 2021
antibacterial activity pneumonia, Pseudomonas spherical [73]
communis L. aeruginosa, B. cereus
steroids
Mentha
Longifolia anti-human breast breast carcinoma (Hs spherical shape 2021
- 512 36 [74]
carcinoma 578Bst) particles
leaf
antimicrobial,
Curcuma pseu- antioxidant, and Pseudomonas aeruginosa,
domontana anti-inflammatory Staphylococcus aureus, spherical shape 2021
curcumin 542 20 [75]
isolated activities, antioxidant Bacillus subtilis and particles
curcumin and radical Escherichia coli
scavenging activities.
sing Pimenta Photocatalyst, spherical shape 2021
dioica extract antioxidant, and S. aureus and E. coli 517 11 [76]
Leaves antibacterial particles

Staphylococcus
Garcinia kola epidermidis, Bacillus spherical shape 2021
extract Antibacterial activity 564 18–38 [77]
Pulp subtilis, Staphylococcus particles
aureus, Escherichia coli

Kaempferia antimicrobial, spherical


extract antioxidant, and Escherichia coli, 540 structure with 20–60 2021
parviflora catalytic degradation Staphylococcus aureus [78]
high crystal in
rhizome agent nature
B. subtilis, S. aureus,
Clerodendrum extract Antimicrobial, and Klebsiella, and E. coli, A. 520 5 2020
inerme antioxidant activities niger, T. harzianum, and spherical [79]
A. flavus
antibacterial, spherical shape
antioxidant, S. epidermidis, B. subtilis, mostly spherical
Nigella flavonoids, cytotoxicity against in shape and less
S. aureus, E. coli, Serratia 546 3–37 2017
arvensis leaf alkaloids, and marcescens, and P. [80]
proteins H1299 and MCF-7 triangle,
extract cancer cell lines, and aeruginosa pentagon and
catalytic activities hexagon shapes
Aqueous phenols,
Extract of flavonoids, 540–550 spherical shape 2016
Garcinia benzophe- - - (UV-vis) 32 [81]
mangostana particles
nones, and
Fruit Peels anthocyanins
a moderate cytotoxic
effect at 24 and 48 h
deprotonation was found
of hydroxyl Cytotoxicity on
Mimosa groups present HUVEC cells using maximum
tenuiflora in 280 nm and 20–200 2019
in MTT, Cellular uptake, multiple shapes [82]
Bark Extract polyphenolic and catalysis broad of 50 nm
molecules of 12.5 mg/L of
extract Mt extract, we
obtained a 50%
inhibition (L50),
Molecules 2022, 27, 8027 9 of 22

Table 1. Cont.

Reducing Microorganisms Wavelength NP Size Year


Plant Source Agents Biological Effects (nm) Shape (nm) (Ref)
Chenopodium Most of the
phenolic antibacterial 533 8 2018
formosanum groups properties E. coli, and S. aureus. resultant Au NPs [83]
shell extract were spherical
peak in the
range of
Leaf Extract antioxidants, 525–540 nm
of enzymes, and with Majorly spherical
Antimicrobial and E. coli, S. marcescens or 30–50 2018
Ziziphus antifungal activity C. albicans a peak and [84]
phenolic maximum in monodisperse
zizyphus moieties the range of
approximately
527–535 nm
Antimicrobial,
hexane, antifungal,
dichloromethane and anticancer prominent
Brazilian red and ethyl activities S. aureus, E. coli, S. mostly spherical 2021
acetate, peak at a range 8–15 [85]
propolis (dose-dependent mutans, C. albicans shapes
prenylated ben- cytotoxicity activities of 523–541 nm
zophenones in bladder and
prostate cancer cells)
Different
Gram-positive and
Gram-negative bacteria.
reducing Furthermore, the
fresh peel enzymes as biosynthesized GNPs a sharp
(aqueous) well as capping In vitro toxicity
exerted remarkable absorption spherical in 2021
extracts of (antibacterial and in vitro cytotoxicity 22 [86]
agents such as peak at 520 shape
Benincasa anticancer)
secondary against human cervical nm,
hispida
metabolites cancer cell line,
while sparing normal
human primary
osteoblast cells
Platycodon flavonoids,
grandiflo- saponins, antipathogenic
rum leaf alkaloids, activity under E. coli and absorption at spherical in 2020
15 [87]
extract amino acids, optimal B. subtilis 545 nm shape
(Balloon proteins, and conditions
flower plant) carbohydrates
Hibiscus spherical sized 2014
rosa-sinensis alkaloids and - - 520 16–30
flavonoids nanoparticles [88]
extract
spherical with a
Galaxaura
elongata few rods,
E. coli, K. pneumoniae, S. triangular,
(powder or Anti-microbial aureus, and 520 3–77 2017
properties Methicillin-Resistant S. truncated [89]
free triangular, and
ethanolic) aureus
based extract hexagonal
AuNPs
Saponins,
alkaloids,
of phytosterols, B. subtilis, S.
Memecylon phlobatannins, biocompatibility and spherical-shaped
pneumoniae, S. aureus, S. 540 15–20 2018
umbellatum phenolic anti-microbial typhimurium, Klebsiella nanoparticles [90]
leaf extract activities aerogenes, and E. coli
compounds,
phytosterols,
and quinones
strong DPPH radical
Solanum S. saprophyticus, B. spherical-shaped
phenolic and hydroxyl radical 2014
nigrum leaf subtilis, E. coli, and P. 537 nanoparticles 50 [91]
extract compounds scavengers and aeruginosa and crystaline
antibacterial activity

4. Potential Application of AuNPs in Food Packaging


Although the emergence of nano-biotechnology approaches is not a newly introduced
concept in the food or agriculture sectors, there is a recent development in this area with
novel aspects [92,93] Growing competitions and considerations for health concerns lead
to increasing demand for sustainable and cost-effective production of food [94], and the
development of more novel approaches for food packaging, coating, and processing to
Molecules 2022, 27, 8027 10 of 22

meet consumer’s demands [93,95]. In case of the emergence of nanotechnology in food


packaging, as mentioned earlier, it should not be underestimated that targeted delivery of
bioactive compound with reduced side-effects, stability of delivery systems [96,97], easiness
in fabrication, regulation of food processed with nanomaterials, and public acceptance with
affordable prices are highly encouraged to meet consumer’s demands, as well [98].
Manufactured nanomaterials such as thin films, nanotubes, and nanoparticles (made
in one, two, and three-dimensional structures, respectively), have been extensively used
in food sectors [97]. Usage of those aforementioned structures in food industries are
categorized into food supplementations, food ingredients, food additives, food nutrients,
and delivery systems (in the forms of nanoemulsions, nanoparticles, surfactant micelles,
emulsion bilayers, and reverse micelles aimed at improvement in texture, color, and flavor).
These structures are aimed at improving the taste or color of the food, and masking
unpleasant tastes.

4.1. Antibacterial Activities


In addition to the general properties of AuNPs [92,99], significant chemical properties
of gold as a metal with the less corrosive one, and non-toxic effects [100,101], has attracted
the focus of researches toward the usage of AuNPs in material based food industries
(Figure 2). In a recent study, the function of 3-aminopropyltrimethoxysilane (APTMS)
in the chitosan gold nanoparticles system was investigated. The addition of APTMS to
chitosan resulted in a significant reduction in apparent viscosity, which can contribute to the
achievement of higher miscibility in the structure. Additionally, the antimicrobial properties
of a film composed of chitosan, APTMS, and AuNPs was evaluated against the Salmonella
bacterium. The combined antibacterial activity of the three components was enhanced by
their synergistic impact [102]. Anti-cancerous, anti-oxidant, and anti-microbial [103–105]
properties of gold-based compounds, including anti-bacterial (especially against gram-
negative bacteria when compared to Gram-positive bacteria [106]), anti-cancerous [41,107],
anti-biofilm [108], anti-fungal (especially against Aspergillus niger (A. niger) and Fusarium
oxysporum) [35,109–111], (majorly square-planar complexes of AuNPs [61]), anti-malaria,
anti-amoebic, anti-leishmanial, and anti-trypanosomal features play an indispensable role
in achieving success in food packaging, and prolongation of shelf life [16,103,110,112].
Mycelial extracts of the edible wild fungus Cantharellus sp. were used to manufacture
AuNPs. On a variety of microorganisms, the antibacterial and antifungal capabilities of
these NPs were evaluated. Significant antibacterial and antifungal properties were shown
by the NPs [113]. Some studies tend to evaluate the effective ingredients responsible or in
synergistic relations for induction of anti-bacterial effects in AuNPs against some bacterial
strains such as: E. coli, S. epidermidis, and Pseudomonas aeruginosa [114]. Whereas, other
studies recommend administration of other metals recruited as nanoparticles, including
alloying colloidal silver-based nanoparticles with AuNPs.
Results from one experimental study carried out by Yongwen Zhang et al. [115] aimed
at the investigation of anti-bacterial effects of colloid AuNPs, indicated promising findings.
Successful preparation of AuNPs, high dispersion stability, and excellent antimicrobial
efficiency was carried out through an in situ reduction and stabilization of hyperbranched
poly (amidoamine) with terminal dimethylamine groups (HPAMAM-N(CH3)2) in water,
and an adjusted molar ratio of AuNPs (from 10 to 30) in feed [7,115]. HPAMAM-N(CH3)2
was used as an effective reducing and stabilizing agent. Anti-microbial effects of several
strains, including E. coli (ATCC 8739), S. aureus (ATCC 6538), B. subtilis (ATCC 21332),
and Klebsiella mobilis (K. mobilis) (ATCC 13048), A. niger (ATCC 16404), and Penicillium
citrinum (P. citrinum) (ATCC 10499), were assessed by administration of 108 CFU/mL from
each bacterial cell suspension. Smaller particle size and narrower distribution were due to
increased molar ratio and exacerbated anti-microbial effects (increased inhibition ratio up
to ca. 98% at the low content of 2.8 µg/mL for AuNPs [115,116]).
To be more precise, AuNPs show less cytotoxic effects controversially compared with
other metal-based nanoparticles such as silver [100,117]. They, as soluble complexes in
[106]), anti-cancerous [41,107], anti-biofilm [108], anti-fungal (especially against Aspergil-
lus niger (A. niger) and Fusarium oxysporum) [35,109–111], (majorly square-planar com-
plexes of AuNPs [61]), anti-malaria, anti-amoebic, anti-leishmanial, and anti-trypanoso-
Molecules 2022, 27, 8027 11 of 22
mal features play an indispensable role in achieving success in food packaging, and pro-
longation of shelf life [16,103,110,112]. Mycelial extracts of the edible wild fungus Can-
tharellus sp. were used to manufacture AuNPs. On a variety of microorganisms, the anti-
organic solvents, have a strong binding affinity to other biological agents, which makes
bacterial and antifungal capabilities of these NPs were evaluated. Significant antibacterial
them more potentiated in releasing ions, and anti-microbial activities, as well [47,118].
and antifungal properties were
Results shown
from by the NPs [113].
a multidisciplinary studySome studies
conducted bytend to evaluate
Enrique the
Lima et al. [119] aimed
effective ingredients responsible or in synergistic relations for induction of anti-bacterial
at investigating the anti-microbial properties of AuNPs as biocide material against E. coli
effects in AuNPs and
against some typhi
Salmonella bacterial
after strains suchofas:
assessment E. dispersion,
size, coli, S. epidermidis, and Pseudo-
and roughness of AuNPs. Those
monas aeruginosa [114]. Whereas,
properties other studies
were supported recommend
by zeolite. administration
Interestingly, of other
they reported thatmetals
there were anti-
bacterial features
recruited as nanoparticles, by elimination
including alloying of the aforementioned
colloidal silver-based bacteria by Au-faujasite
nanoparticles with dispersed
AuNPs. nanoparticles (particles sized 5 nm at the surface) [119].

Figure 2. Functional
Figure 2. Functional properties ofproperties
AuNPs. of AuNPs

Results from one An experimental


experimental studycarried
study conductedout by
by Saima
Yongwen Hameed
Zhanget et
al.al.,
[120] wasaimed
[115] aimed at investi-
at the investigation of anti-bacterial effects of colloid AuNPs, indicated promising in
gating the shape and concentration-dependent anti-microbial properties AuNPs (with
find-
the size varying from 300 to 800 nm) against E. coli, P. aeruginosa, and S. aureus. Consid-
ings. Successful preparation of AuNPs, high dispersion stability, and excellent antimicro-
ered shapes for AuNPs were as following: nanospheres, nanostars, and nanocubes [120].
bial efficiency was carried
UV-vis out through
spectroscopy, XRD, anand
in TEM
situ were
reduction
used forandthestabilization
characterization of hyper-
and confirmation
branched poly (amidoamine) with terminal dimethylamine groups (HPAMAM-N(CH3)2)
of AuNPs. AuNPs in the form of nanocubes depicted full ability in the inactivation of
in water, and an adjusted
foodborne molar ratio(zero
bacteria of AuNPs
survival (from 10 to 30)
percentage inagainst
rate feed [7,115]. HPAMAM-
all bacterial strains). Several
N(CH3)2 was used as anprocedures,
cellular effective reducing
including and stabilizing
cell loss, loosening agent.
of theAnti-microbial
cell wall, loss of effects
flagella, releasing
of several strains,nucleic
including acid E.(orcoli
nucleic
(ATCCacid8739),
leakage), and loss(ATCC
S. aureus of cellular matrix
6538), were reported
B. subtilis (ATCCafter usage
of those AuNPs through visual analysis (at lower concentrations).
21332), and Klebsiella mobilis (K. mobilis) (ATCC 13048), A. niger (ATCC 16404), and Peni- In this study, they con-
cluded
cillium citrinum (P. that despite
citrinum) (ATCC similar surfacewere
10499), areas in those AuNPs,
assessed anti-microbial interactions
by administration of 108 of gold
nanoparticles with the Gram-negative or Gram-positive bacteria at lower concentrations
CFU/mL from each bacterial cell suspension. Smaller particle size and narrower distribu-
will be shape-dependent [120,121].
tion were due to increased
Resultsmolar from aratio and exacerbated
preliminary anti-microbial
interdisciplinary effects
study carried out (increased
by Thirumurugan, A.
al. [122] demonstrated constructive effects of AuNPs exacerbated by )incorporated
inhibition ratio upetto ca. 98% at the low content of 2.8 μg/mL for AuNPs [115,116] . food
To be more precise, AuNPs show
bio-preservatives (suchless cytotoxic
as peptide effects controversially
of bacteriocin compared plantarum
produced by Lactobacillus with strain
other metal-basedATM11,
nanoparticles
and nisin) such as silver
against [100,117].
reduction They,spoilage
of microbial as soluble complexes
(Micrococcus in B. cereus,
luteus,
organic solvents, E. coli, aand
have S. aureus),
strong that makes
binding affinitythem properbiological
to other to be used agents,
aimed atwhich
the prolongation
makes of shelf
life [122].
them more potentiated The most significant
in releasing anti-bacterial activities
ions, and anti-microbial were
activities, asobserved in the combinative
well [47,118].
usage of AuNPs/nisin, and AuNPs/bacteriocin against E. coli. They concluded that
Molecules 2022, 27, 8027 12 of 22

peptide-producing organisms presented more anti-microbial abilities against mentioned


food-borne pathogens. Additionally, the combination of bacteriocins with AuNPs showed
more anti-bacterial properties when compared to AuNPs/nisin [122].
Carlos H. Pagno and his colleagues [123], in their study, aimed at investigating anti-
microbial properties of active biofilms of quinoa (Chenopodium quinoa W.) starch-containing
AuNPs against E. coli (ATCC 25972), and S. aureus (ATCC 1901) [123]. Anionic silsesquiox-
ane containing the 1,4-diazoniabicyclo, octane chloride group (a silica-based hybrid poly-
mer) was used for stabilizing AuNPs [123]. The final product was in the form of AuNPs
dispersed to biofilms of quinoa starch with enhanced tensile strength. The significant anti-
microbial activity was reported as inhibition percentages of 99% against E. coli, and 98%
against S. aureus. In addition to the significant anti-bacterial properties, and increased UV
radiation absorption and a decreased solubility make them more proper for food packaging
applications [123].
Sujan Chowdhury et al. [124] assessed the effects of poly(vinyl) alcohol cross-linked
film containing AuNPs on prolongation in the shelf life of bananas. They compared
acquired results to the incorporation of graphene oxide into poly(vinyl) alcohol cross-linked
film. They reported that improved mechanical and physical properties (such as tensile
strength, Young’s modulus value, water vapor transmission rate, and water solubility)
are beholden to the dispersion of AuNPs and graphene oxide in the PVA cross-linked
composites [124]. In case of advantages for anti-microbial efficacies, graphene oxide
incorporated into poly(vinyl) alcohol showed less inhibition zone on disk diffusion agar
tests against food-borne pathogens. They concluded that poly(vinyl) alcohol cross-linked
film containing AuNPs was more efficient in increasing shelf life for bananas, and this
efficacy in AuNPs was to a greater extent when glyoxal had been used as a cross-linker agent
in poly(vinyl) alcohol cross-linked composite films. Mechanism of action for AuNPs against
E. coli was cell lysis, which is accelerated by ethanol present in the poly(vinyl) alcohol film,
electronic effects due to the changes in local electronic structures of the surfaces and their
smaller sizes (less aggregated form and larger exposed expose a larger available surface
area), as well [124].
Siying Tang et al. [125] designated their comparative study aimed at investigation
of photocatalytic, and anti-microbial properties of gold-TiO2 /Sodium alginate nanocom-
posite films (as a degradable film and adsorber for visible light), which were produced
by hydrothermal and casting method. Mechanical properties of produced film containing
AuNPs, conferred them good shape stability. In the case of assessed anti-bacterial proper-
ties, there was an improved antibacterial activity against S. aureus and E. coli. This activity
is accelerated by synergistic effects SPR of AuNPs, and increased production of reactive
oxygen species [125,126].
Biologically, those useful properties are highly dependent on ligands. Furthermore,
migration of AuNPs due to high surface to volume ratio of AuNPs [51], production of
radical oxygen (scavenging free radical species via catalytic reaction), hydrophobicity [52],
ability to interact with both gram-negative and positive bacteria with adjusted size and
morphology (even optimized concentration) [127–129] have been considered as a merit for
their reaction with food-borne pathogens, making an impressive decrease in the incidence
of bacterial pathogenesis in food, and subsequently in consumers. Figure 3, indicates that
how the chemical synthesis of AuNPs affects their potential applications.
To be more specific, there are several strategies for enhancing the antimicrobial char-
acteristics of AuNPs. These methods may be roughly classified into three groups, includ-
ing chemical reduction, green synthesizing [11], and incorporation of AuNPs with other
nanoparticles. Multiple research suggest that these properties are dependent on chemical
agents bound to the AuNPs surface. Therefore, maximizing the antimicrobial activity of
synthesized AuNPs is a controversial subject.
migration of AuNPs due to high surface to volume ratio of AuNPs [51], production of
radical oxygen (scavenging free radical species via catalytic reaction), hydrophobicity
[52], ability to interact with both gram-negative and positive bacteria with adjusted size
and morphology (even optimized concentration) [127–129] have been considered as a
merit for their reaction with food-borne pathogens, making an impressive decrease in the
Molecules 2022, 27, 8027
incidence of bacterial pathogenesis in food, and subsequently in consumers. Figure133,ofin-
22

dicates that how the chemical synthesis of AuNPs affects their potential applications.

Figure 3. Chemical synthesis of AuNPs loading with different agents.


Figure 3. Chemical synthesis of AuNPs loading with different agents.

To be Properties
4.2. Barrier more specific, there are several strategies for enhancing the antimicrobial char-
acteristics of AuNPs.
Permeability Thesevapor,
of water methods
gasesmay beCO
(e.g., roughly classified into three groups, includ-
2 , O2 , and N2 ), aroma chemicals, and light
ingbarrier
are chemical reduction,
properties. Thegreen synthesizing
presence [11],inand
of moisture food incorporation of AuNPs
promotes microbial with other
development
nanoparticles. Multiple research suggest that these properties
and rapid food deterioration. Therefore, packaged food goods may have a muchare dependent on chemical
longer
agents bound to the AuNPs surface. Therefore, maximizing the antimicrobial
shelf life if they are wrapped in a film with enhanced barrier qualities (WVTR) [130]. Not activity of
synthesized AuNPs is a controversial subject.
only anti-microbial properties of AuNPs are of food packaging systems, but gas barrier
properties also make them a proper choice. In general, there are not enough studies
4.2. Barrier the
discussing Properties
effect of AuNPs on barrier properties. However, similar to other metal
nanoparticles, AuNPs depicted a notable improvement in barrier properties.
In a research by Pagno et al., it was reported that the presence of AuNPs does not
negatively affect the water vapor permeability of quinoa starch film (p > 0.05). They also
reported the improvement of permeability of oxygen and carbon dioxide after AuNPs
were embedded within the biofilm (p < 0.01). The presence of AuNPs in the biofilms
can significantly reduce the permeability of gases (p < 0.01), so that AuNPs, like other
metal nanoparticles, are considered an additional barrier to the penetration of gases and
consequently, due to the elongation and complication of the path within the film matrix, the
penetration of gases leads to a delay in oxygen transfer. They also reported that increasing
the AuNPs concentration from 2.5% to 5% did not change the permeability significantly
(p > 0.05). In another study, AuNPs were embedded with a poly(vinyl) alcohol-based
film [124]. It was reported that the addition of AuNPs enhanced the molecular structure
tortuosity (p < 0.05), thus the water molecules are unable to pass through [45].
Barrier properties are reduced when a high concentration of AuNps are employed
which the reason turns back to the agglomeration of AuNPs at higher concentration. It
was shown that AuNPs can own distinct sizes (Table 2) and shapes which shows different
behavior in agglomeration [131]. So, it is important to optimize the AuNPs concentration
within the film matrix to reach the best barrier properties. Furthermore, the shape of AuNPs
may affect the diffusion pathway which may result in better or worst barrier properties.
Molecules 2022, 27, 8027 14 of 22

Table 2. AuNP dimension, weights, and volume.

Average Size (nm)


AuNPs mAuNP (10−18 g) Volume (10−25 m3 )
(Diameter)
Citrate AuNS 12.5 19.7 10.2
Tryptophan AuNS 8.4 5.9 3.1
Tyrosine AuNS 9.9 9.8 5.1
CTAB/citrate AuNS 8.9 7.1 3.7
AuNS (CTAB) 77.9 4800 2475.2
58.8 (length)
AuNR (CTAB) 270 137.6
15.3 width
AuNPr (CTAB) 94.7 (side length) 1900 970.8
AuNC (CTAB) 47.5 (side length) 2100 1071.7
Cetyltrimethylammonium bromide (CTAB), spherical AuNP (AuNS), cubic AuNPs (AuNC), rod-shaped (AuNR),
prismatic AuNPs (AuNPr).

4.3. Antioxidant Properties


Metal and metal oxide NPs, carbon nanotubes (CNT), and different types of polymeric
antioxidant NPs loaded with antioxidants demonstrated notable antioxidant properties.
AuNPs as well as other common metal NPs own antioxidant potential. AuNPs are ca-
pable of interacting with both stable and unstable free radicals [132]. However, it was
reported that AuNP’s potential as an antioxidant agent can be varied in a dose-dependent
manner [133].
In a study, J. Beurton et al. [112], aimed to investigate the presser ing of controlled an-
tioxidant properties (DPPH% and 2,2-azino-di(3-ethylbenzathiazolin-6-sulfinate) (ABTS•+ )
in the well-individualized I mobilized AuNPs on glass support (conducted through elec-
trostatic interactions). As there was not any other peak except a localized SPR at 514
nm, no aggregation was reported. Promising results indicated a long-lasting antioxidant
capacity characterized by a different kinetic (than colloidal AuNPs), and with the same
efficiency. They designated the ability for prevention from the degradation of molecules
(containing a thiol function) as a criterion for adaptable support of immobilized AuNPs.
They represented that a ten-fold increase in the half-life of N-acetylcysteine, proved the
efficacy of immobilized AuNPs for food packaging purposes with an adoptable covered
surface, and the number of deposited AuNPs [112].
It has been reported that the high surface area to volume ratio of nanoparticles plays
a vital role in their ability to scavenge free radicals [134]. Functionalized NPs attracted
scientist’s attention in food packaging systems because of benefits such as unique and local-
ization interactions of NPs with the bio components from the foods. In research carried out
by Patra and his colleagues [64], AuNPs were synthesized by green synthesis using onion
peel extract and named OP-AuNPs. Antioxidant activity was one of the main parameters
under study. Based on the results, they reported that OP-AuNPs showed a notable DPPH
scavenging capacity of 14.44%/100 µg/mL in comparison with 36.54%/100 µg/mL by
butylated hydroxytoluene as a commercial antioxidant. OP-AuNPs also demonstrated
higher radical scavenging compared to butylated hydroxytoluene. It was reported that the
main reason turns back to the secondary metabolites, aromatic phenolic, and flavone groups
in the onion peel extract and high surface area to volume ratio of nanoparticles [126,135].

4.4. Biosensing
One of the main concerns of customers is food quality and safety. Therefore, exploring
fast, accurate, and efficient techniques to detect food quality is significantly important
for human health. Biosensors depict a cutting-edge frontier in food packaging manage-
ment [19], and nanomaterial such as AuNPs have been employed in the food contamination
detection field to monitor, assess, and control food quality [136].
The intrinsic properties of AuNPs such as high stability, easy to control size and
shape of the NPs, large surface-to-volume ratio, and excellent biocompatibility, offer them-
selves various benefits as sensors to make smart food packaging. For instance, a high
Molecules 2022, 27, 8027 15 of 22

surface/volume ratio provides high sensitivity and rapid responses. AuNPs also can be
considered as multiple detection platforms [137]. Colorimetric sensors are one of the most
common AuNPs-based sensors. AuNPs have shown their detecting potential in food
contamination monitoring [137]. However, there are a few reports about employing AuNPs
in food packaging systems.
M.R. Bindhu et al. [138] aimed to assess biosensory capabilities of gold and silver
nanoparticles by a green approach (using Solanum lycopersicum extract). Carboxylic acid
groups in the mentioned extract were recognized as reducing agents. UV-vis, FTIR, TEM,
and energy dispersive spectroscopy (EDS) techniques were used for the characterization
and confirmation of metal-based nanoparticles. Results of this study for monodispersed
spherical gold, and silver nanoparticles showed significant SPR peaks at 546 nm and 445 nm,
average size of 14 nm, and 12 nm, respectively. In addition to significant anti-microbial
activity against S. aureus and P. aeruginosa existed in water samples, they were able to sense
ions of heavy metals such as Fe3+ and Cu4+ in water by an SPR optical sensor, being efficient
in water purification [131]. Results of this study were in agreement with other studies
carried out by Govindhan Maduraiveeran et al. [132] indicating successes in the usage of
AuNPs for sensitive detection of multi-target analytes with food safety and environmental
monitoring purposes.
One innovative experimental study done by Cheuk-Fai Chow [139], was aimed at
the investigation of correlations between the sensitivity of a colorimetric probe based on
AuNPs (as a nano detector) to detection of microbial spoilage in meat products (stored at
4 ◦ C), and volatile biogenic markers (such as dimethyl sulfide and histamine,). The ability
of detection in the colorimetric probe is beholden to the ability in the transformation of the
non-aggregated form of AuNPs to its aggregated form, after binding to aforesaid biomark-
ers. Of note, 0.5 and 0.035 µg/mL of AuNPs could detect dimethyl sulfide, and histamine
biomarkers, respectively [139]. Additionally, they demonstrated that the constitution of
AuNPs in the 2:1 H2 O/DMSO mixture confers them to high stability to show the selective
colorimetric response for mentioned biomarkers. In the case of microbial assessments, sens-
ing signals of AuNPs for detection of mentioned volatile biogenic markers on 12 different
raw meat samples were estimated. CFUs of 107 were recognized as an alarm for the level of
spoilage. For raw meat, preserved raw meat, raw fish, and raw crustaceans, UV-vis signals
(at 520 nm) of 0.15, 0.1, 0.45, and 0.35 were reported alarm values, indicating harmful levels
of food spoilage (CFUs of 107 ).
The development of nanotechnology offers several industries, particularly the food
packaging industry, significant prospects. As functional additives, several nanoparticles
(such as nanoclay and metallic nanoparticles) have recently been incorporated to food
packaging. Their beneficial impacts on modern packaging materials have been widely
reported. According to the findings, the introduction of nanoscale fillers into the poly-
mer matrix will alleviate packaging material difficulties while also enhancing functional
properties [140]. These polymers incorporating nanocomposites have enhanced barrier
characteristics, thermal properties such as melting temperature and glass transition, and
altered functions such as surface properties and hydrophobicity. Inorganic nanoparticles
have the ability to inhibit bacterial development inside packaging. By adding nanoscale
components into biopolymer-based packaging composites, packaging-related waste may
be decreased.
The migration behavior of nanomaterials from packaging may vary from that of
conventional materials, and migrating nanoparticles may be more reactive and have a
distinct toxicological profile. Thus, certain nanomaterials are prohibited in the EU due to
insufficient toxicity data [141].
Multiple factors, such as temperature, time, the concentration of nanoparticles in
polymer matrix, polymer characteristics, placement of the nanoparticles in the packaging
material, interaction between the nanoparticles and the materials, sample selection type of
material, contact type of material, and the nature of the food/food simulants, have been
shown to influence the migration of nanomaterials from food packaging substance into
Molecules 2022, 27, 8027 16 of 22

food or food simulants. In general, nanoparticles have the ability to migrate into food,
particularly when exposed to more acidic chemicals [142].

5. Hazard
Allergies and the release of heavy metals as the migration phenomenon are the two
main safety concerns of nanoparticles. AuNPs depict a good safety profile. Considering
AuNPs, as well as other metal nanoparticles have the potential of toxicity. AuNPs are
capable of migration from packaging to food matrix and finally, they will be released in the
human body after food consumption which is a toxin for different cells and tissues [138].
Currently, AuNPs are employed in active and smart food packaging systems at a
relatively faster rate without desired knowledge and regulations, which can affect health
and the environment. There is a likelihood of interacting between AuNPs and food
molecules which leads to unwanted and toxic products. This issue is also important
in smart food packaging systems which may result in false-positive detection [143].
Nevertheless, experimental use of AuNPs presented possible medical hazards as the
surface to volume ratio causes catalytic properties and can make particles very reactive.
Furthermore, nanoparticles easily pass cell membranes and can interact with intracellular
metabolism [139]. Environmentally, AuNPs can be released into the ecosystem along
with the nanocomposite. However, they are benign to the ecosystem if no accumulation
happens in the environment. For instance, there is a report considering the non-toxicity
of AuNps to zebrafish As at nano-scale gold-particles may exhibit size-related properties
that differ significantly from the known properties of non-nano-scaled gold-particles, one
cannot predict reliably the nature of AuNPs and a biologic system and interactions between
AuNPs and living cells. Moreover, AuNPs showed different shapes with different charge
and surface-chemistry and each one may have distinct behavior [144].

6. Future Prospective
To improve nano-packaging systems via AuNPs, it is necessary to consider all aspects
including hazards. AuNPs as well as other common NPs, can migrate from packaging into
the food matrix. However, AuNPs due to having various shapes can be a good candidate
to modify a film structure with desired features.
Surface modification of the inner surface of the polymeric films (the surface which
touches the food) can decrease the NPs diffusion by limiting the micro-channels. Creating
a bilayered film, in which the inner layer is responsible for controlling NPs migration,
can be a good solution. By the way, it is dictated that increasing the layers may consume
more materials which can be considered as a hazard to the environment, so modifying the
thickness of the layers is recommended.
As another recommendation, NPs modification can be another recommendation to
decrease the rate of migration. Chemically, connection of NPs to the inner structure of the
films can lower the migration phenomenon. It is also recommended that this connection,
based on the various factors, can be permanent or temporary. Considering the previous
point, AuNPs are known as good carriers. When AuNPs are loaded with an antibacterial
agent, it is predicted to improve both barrier properties and migration rate.
As the final recommendation, AuNPs and ionic gold can show different activities
against a range of microorganisms. It can be recommended for future studies to evaluate
the level of improvement by employing both types of gold.

7. Conclusions
Food packaging is one of the most important challenges which has a direct effect on
human health. In this regard, it is mandatory to engineer a packaging system that not only
can increase foods shelf life but also can provide online information about food quality.
Nanotechnology plays a vital role in this area of science. Metal NPs showed their potential
in improving food packaging systems.
Molecules 2022, 27, 8027 17 of 22

AuNPs with their unique potential demonstrated that can be integrated with other
technologies in food packaging to achieve an active and smart food packaging system with
suitable antibacterial, antioxidant, and scavenging properties while providing appropriate
information about food quality. AuNPs have the potential to migrate from the film or
coating packaging to the food matrix. Thereby, the way of polymeric film manufacturing,
the concentration of AuNPs, employed agents, used biomaterial, type of food, and storage
condition can affect AuNPs activity as antibacterial/antioxidant/biosensor agents.

Author Contributions: Conceptualization, H.A.; methodology, S.P. and M.F.; investigation, M.F. and
G.G.; writing—original draft preparation, H.A. and M.F.; writing—review and editing, G.G. and B.X.;
visualization, S.P.; supervision, H.A. and B.X.; project administration, H.A.; funding acquisition, B.X.
All authors have read and agreed to the published version of the manuscript.
Funding: This study is supported by a research grant R202107 from BNU-HKBU United International
College, China.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Not applicable.
Conflicts of Interest: The authors declare no conflict of interest.

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