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Curcumin Intelligent Packagig

This review discusses the potential of curcumin as a bioactive agent in food packaging systems, highlighting its chemical structure, biological activity, and the properties of curcumin-loaded films. It emphasizes the antimicrobial and antioxidant benefits of curcumin, as well as its role in developing intelligent packaging that can monitor food freshness. The paper also explores the effects of curcumin on the mechanical properties of various film formulations, indicating that while curcumin enhances certain characteristics, high concentrations can negatively impact film integrity.

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0% found this document useful (0 votes)
6 views13 pages

Curcumin Intelligent Packagig

This review discusses the potential of curcumin as a bioactive agent in food packaging systems, highlighting its chemical structure, biological activity, and the properties of curcumin-loaded films. It emphasizes the antimicrobial and antioxidant benefits of curcumin, as well as its role in developing intelligent packaging that can monitor food freshness. The paper also explores the effects of curcumin on the mechanical properties of various film formulations, indicating that while curcumin enhances certain characteristics, high concentrations can negatively impact film integrity.

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thenambika1010
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© © All Rights Reserved
We take content rights seriously. If you suspect this is your content, claim it here.
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Journal of Environmental Chemical Engineering 9 (2021) 105520

Contents lists available at ScienceDirect

Journal of Environmental Chemical Engineering


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

Curcumin: A promising bioactive agent for application in food


packaging systems
Neda Aliabbasi a, Morteza Fathi b, Zahra Emam-Djomeh a, *
a
Transfer Phenomena Laboratory (TPL), Department of Food Science, Technology and Engineering, College of Agriculture and Natural Resources, University of Tehran,
PO Box 4111, Karaj 31587-11167, Iran
b
Health Research Center, Lifestyle Institute, Baqiyatallah University of Medical Sciences, Tehran, Iran

A R T I C L E I N F O A B S T R A C T

Editor: Teik Thye Lim This review paper aimed to provide an insight on (1) the chemical structure and biological activity of curcumin,
(2) physico-mechanical and antimicrobial properties of curcumin-loaded films, (3) the controlled release of
Keywords: curcumin from the films, and (4) the potential applications of the films incorporated by curcumin in food
Antimicrobial activity preservation. It was found that besides the inherent antimicrobial activity of curcumin, the medium in which
Controlled release
curcumin has to execute its function is important. The intelligent packaging system based on curcumin/bio­
Curcumin
polymers can be used as an effective indicator to monitor animal-based protein foods’ freshness. Overall,
Intelligent packaging
Physico-mechanical properties polysaccharide and/or protein composite films loaded with curcumin, as novel kinds of functional films could
find applications in the food packaging industry.

1. Introduction scientific literature. Therefore, for the first time, this article was aimed
to provide an overview of the chemical structure and biological activity
To date, various studies have been carried out on the development of of curcumin. Also, physico-mechanical and antimicrobial properties of
new active packaging systems to play an active role in food preservation. the films incorporated by curcumin were discussed. Additionally, the
The use of bioactive compounds in packaging systems is one of the most release behavior of curcumin from the packaging matrix was reviewed.
effective methods in preserving food quality and further improving food Finally, the potential applications of the films loaded by curcumin in
safety [1]. food quality were explored.
The functional properties of curcumin are mainly associated with its
unique structure. The structure of curcumin is shown in Fig. 1 [2]. 2. Physicochemical properties of curcumin
Curcumin has been recognized as a powerful antioxidant agent, and its
multidimensional healing actions for various chronic diseases have been Curcumin ([1,7-bis (4-hydroxy-3- methoxyphenyl)-1,6-heptadiene-
well demonstrated. Curcumin’s antioxidant activity has been attributed 3,5-dione]), has a molecular weight of 368.385 g/mol and it is solid at
to the existence of the ortho-methoxy groups of curcumin. room temperature. Curcumin has poor water solubility that limits its
At a pH of more than 7, the phenolic hydroxyl groups of curcumin oral administration and decreases its bioavailability. Curcumin is very
react with hydroxyl groups and, as a result, produce phenoxide anion, soluble in polar solvents like ethanol (10 mg/mL), mostly insoluble in
which leads to further alterations in the color of curcumin. water (only 30 nM can be dissolved), and is poorly soluble in hydro­
The incorporation of curcumin into the packaging system improves carbon solvents [3,4]. The melting point of curcumin is 183 ◦ C (361 ◦ F;
the bioavailability and stability of this compound against environmental 456 K). Curcumin undergoes hydrolytic degradation at high tempera­
conditions and enables the packaging to monitor food quality. In this tures. The loss of curcumin content rapidly increased with temperature,
regard, enhancing the active compound’s biological activities through showing its instability at high temperatures. Chen et al. [5] indicated
different strategies has been investigated by several research groups. that the processing temperature of curcumin should not exceed 190 ◦ C.
However, a comprehensive review of the application of curcumin in Different works have been conducted to increase water solubility and
food packaging systems is not currently present in the peer-reviewed thermal stability of curcumin. The entrapment of curcumin into the

* Corresponding author.
E-mail address: [email protected] (Z. Emam-Djomeh).

https://doi.org/10.1016/j.jece.2021.105520
Received 14 February 2021; Received in revised form 6 April 2021; Accepted 15 April 2021
Available online 26 May 2021
2213-3437/© 2021 Elsevier Ltd. All rights reserved.
N. Aliabbasi et al. Journal of Environmental Chemical Engineering 9 (2021) 105520

them, due to the hydrophilic nature of proteins and polysaccharides, the


proteins/polysaccharides-based films become weak under moist condi­
tions and have high water vapor permeability (WVP). WVP is commonly
considered as a critical factor for food packaging and should be as low as
possible [17]. As mentioned above, curcumin is a hydrophobic com­
pound, and thus it is expected that the addition of curcumin to film
formulation results in the decrease of WVP.
Overall, curcumin increases the antimicrobial and antioxidant ac­
tivity of the packaging systems and simultaneously protects foods
Fig. 1. The chemical structure of curcumin.
against deteriorative factors like moisture. Moreover, curcumin-loaded
packaging systems are sensitive to pH changes and can detect food
polymeric matrices is known as one of the most promising approaches to spoilage. Some curcumin actions in active and intelligent packaging are
overcome these issues. depicted in Schematic 1.
Curcumin stability in aqueous solution is pH-dependent, with an
optimum cut-off point ranging from pH 1–6. The color of curcumin
changes to red in the charged form (pH < 1 or pH > 7) [2] and sunlight 3.1. Impact of curcumin on mechanical properties
exposure accelerates curcumin degradation [6]. This property makes
curcumin ideal for developing intelligent packaging systems to monitor 3.1.1. Protein-based films
the quality of seafood like fish and shrimp. Considering the unique The inter- and intra-molecular interactions have a key role in the
physico-chemical properties of curcumin, it is applied as an antioxidant, mechanical characteristics of protein-based films. The interaction of
flavoring agent (warm, bitter taste) and natural colorant (a bright yellow phenolic compounds with proteins can result in changes in the protein
color) in dairy products, beverages, cereals, mustard, food concentrates, structure, consequently affecting the mechanical properties of the
pickles, sausages, confectionery, ice cream, and meat, fish, eggs, and protein-based films and improving the thermal stability of proteins [18,
bakery products [7]. 19]. Both H-bonding and hydrophobic interaction between phenolic
compounds and proteins may occur. The OH groups of the aromatic ring
3. Curcumin: an excellent bioactive compound for film of phenolic compounds such as curcumin provide the binding sites for
fabrication protein-phenols interactions, resulting in improving the mechanical and
water barrier properties of protein films [20]. For instance, Bitencourt
Curcumin accelerates the healing process by acting on the inflam­ et al. [21] added Curcuma ethanol extract (CEE) with different con­
matory, proliferative, and maturation phases of wound healing [8,9]. centrations (0, 0.05, 0.50, 0.10, 0.15, and 0.20 g/g of protein) to gelatin
Therefore, curcumin can be introduced as a promising candidate for film formulation. They found that CEE had 5.5 mg mL− 1 curcumin.
production of packaging systems and/or for biomedical applications (e. Hence, the film formulation’s curcumin concentration was in the range
g., wound healing) [9,10]. of 0.275–11 mg g− 1 of protein. TS and EB increased significantly when
The change in pH is commonly considered as an indicator to recog­ the CEE concentration was increased. As discussed before, this effect
nize bacterial growth. The changes in this factor, as well as carbon di­ may be related to the interaction between phenolic compounds and
oxide and ammonia production during food spoilage, can be detected by gelatin peptides that improves film matrices’ cohesiveness and
curcumin [11]. Therefore, different investigations have been carried out flexibility.
to develop intelligent packaging systems based on curcumin [12–16]. Despite such reports, it is very clear that with the addition of hy­
According to the literature, polysaccharides, proteins, and lipids are drophobic phenolic compounds like curcumin with high concentration
the main polymeric ingredients used to produce edible films. Among levels, the hydrophobicity of the protein matrix increases, and as a
result, the mechanical performance of the protein-based films decreases.

Schematic 1. Curcumin action in active and intelligent packaging.

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N. Aliabbasi et al. Journal of Environmental Chemical Engineering 9 (2021) 105520

In this regard, the effects of curcumin addition (400 mg − 1 of protein) on mechanical performance of the films.
the mechanical characteristics of the bovine gelatin-based films have
been investigated by Musso et al. [19] and demonstrated that the values 3.1.3. Polysaccharide-based films
of TS, EB, and YM for gelatin films incorporated with curcumin were Due to chitosan’s excellent film-forming properties and high bio­
lower than those of control film. The same observations have been re­ logical activity, this cationic biopolymer is broadly used to produce eco-
ported by other scientists investigating the effect of curcumin on the friendly packaging systems [34–37]. Incorporating curcumin
mechanical properties of protein-based films. Said and Sarbon [22] (10 mg g− 1 of polysaccharides) into chitosan film resulted in an increase
found that the use of curcumin with different concentrations (these and a decrease in TS and EB, respectively, and improvement of me­
concentrations were not provided by authors in their publication) in the chanical resistance. As presented in Fig. 2, the increase of TS with the
formulation of chicken skin gelatin/rice starch composite films resulted addition of curcumin is related to H-bonding between OH groups of
in a decrease in TS. Due to curcumin’s hydrophobic nature, this bioac­ curcumin and NH2 groups of chitosan macromolecules. Furthermore,
tive compound interrupts the protein-protein interactions in the film the increase of TS after curcumin incorporation may be due to good
network and reduces the film’s structural integrity, and consequently compatibility between chitosan and curcumin, confirmed by SEM
decreases the tensile strength of the films [23]. The decrease of EB with analysis. The reducing effect of curcumin on EB has been attributed to
the incorporation of curcumin to the formulation of protein-based films the smaller molecular length of curcumin than chitosan, which restricts
has been attributed to the chemical structure of curcumin molecules the blend film’s extensibility [38].
composed of aromatic and aliphatic rings, which substantially possessed In another study [39], the effects of glycerol as a plasticizer and
low rigidity, relatively small elongation, and brittle [24]. The same re­ curcumin on the mechanical characteristics of chitosan film were
sults have been reported by Wang et al. [25], who developed curcumin investigated. While the curcumin concentration was increased from 0%
(100 mg g− 1 of proteins) loaded caseinate/zein nanocomposite film, to 0.5%, TS showed an increasing trend, which can be correlated with
confirming the undesirable effect of curcumin at high concentration on H-bond interaction between OH groups of curcumin and NH2 groups of
mechanical properties of protein-based films. chitosan [39] (Fig. 2). Further increasing curcumin concentration
At a temperature above 35 ◦ C, the physical structure of gelatin resulted in a decrease in TS. This observation is well consistent with
changes, and thus the mechanical performance of gelatin-based films those observed by Roy and Rhim [40], who revealed that the intro­
weakens. Accordingly, several studies have been carried out on duction of curcumin with a high concentration to chitosan film led to a
improving the stability of gelatin against temperature [26–29]. Manna decrease in TS. Based on SEM analysis, neat chitosan films were smooth,
et al. [30] modified gelatin by grafting the gelatin molecules with car­ homogeneous, and compact. However, the film containing high curcu­
boxymethylated guar gum and investigated the impacts of curcumin on min concentration showed some irregularities. It seems that the decrease
mechanical characteristics of the film based-carboxymethylated guar in TS is due to the non-uniform distribution of curcumin and the for­
gum grafted gelatin (CGG). Surprisingly, the developed films’ TS and mation of the aggregated complex at high curcumin concentration
YM values were 41.64 MPa and 358.53%, respectively. The TS of CGG which was confirmed by SEM analysis. A similar observation was re­
films incorporated with curcumin was greater than most of the synthetic ported for EB when the curcumin concentration increased.
polymers-based films such as low-density polyethylene (11.8 MPa), Different studies have also used anionic polysaccharides to fabricate
ethylene-vinyl acetate (13.8 MPa), high-density polyethylene biodegradable films. k-carrageenan, as a natural biological macromol­
(17.3–34.6 MPa), equal to that of cast polypropylene (41.5 MPa), pol­ ecule, has excellent film-forming ability. In a recent study [41], curcu­
yvinylidene chloride (48.4–138 MPa), and lower than corresponded min with various concentrations (50, 150, 250, and 350 mg g− 1of
values for cellulose acetate (48.5–82.7 MPa), polyester (178 MPa) [31]. polysaccharide) was added to the k-carrageenan-based film formulation
to modify its mechanical properties. According to their findings, with
3.1.2. Protein/polysaccharide films the increase of curcumin concentration up to a certain point
The addition of polysaccharides is a promising method to improve (150 mg g− 1of polysaccharides), TS and YM were increased, but with
the mechanical properties of protein-based films. In this context, Wu further increase in curcumin concentration, these parameters showed a
et al. [32] developed a biodegradable film based on a combination of decreasing trend. This decreasing effect in TS and YM at high curcumin
fish gelatin and β-cyclodextrin. The effects of curcumin content on the concentration is related to poor dispersion of agglomerated curcumin.
mechanical performance of the films were investigated. According to On the other hand, Roy and Rhim [40] reported that the addition of
their findings, with an increase in curcumin concentration from 100 to curcumin up to a concentration of 10 mg g− 1of polysaccharides did not
250 (mg g− 1 of protein), TS and EB increased, but with further increase affect the carrageenan’s mechanical characteristics film.
in curcumin concentration, these parameters showed a decreasing trend. Cellulose is broadly used to manufacture fibers, textiles, paper, films,
The mechanical characteristics of films are mainly dependent on etc. Luo et al. [42] improved edible cellulose films’ mechanical perfor­
microstructural properties and intramolecular forces [33]. The decrease mance and functionality by incorporating curcumin into cellulose film
of TS and EB at high curcumin concentration is due to interfering in the formulation. 1-allyl-3-methylimidazolium chloride (AmimCl) is an ionic
interaction between gelatin molecules, which leads to the decrease of liquid known as the most effective solvent for cellulose. It has been

Fig. 2. H-bonding interaction between chitosan macromolecules and curcumin [38].

3
N. Aliabbasi et al. Journal of Environmental Chemical Engineering 9 (2021) 105520

reported that AmimCl is also a useful solvent for dissolving curcumin. curcumin on chitosan films’ mechanical characteristics were examined.
Thus, Luo et al. [42] fabricated cellulose/curcumin composite films When the nanocrystals concentration was increased, TS increased
using AmimCl as the solvent of curcumin. Curcumin with different significantly, and a slight decrease was observed in EB. A similar trend
concentrations was added to the film formulation. The TS and EB values was reported when curcumin concentration was increased. The positive
for neat cellulose films were 130 ± 7 MPa and 9.1 ± 1.3%, respectively, effect of curcumin on TS of chitosan film is associated with the hydrogen
demonstrating the composite films’ brittle nature. With the addition of band between chitosan and curcumin and useful external load transfer
curcumin, a slight decrease in TS was reported even at high curcumin by the well-dispersed curcumin molecules [38].
concentration, indicating excellent compatibility and interfacial inter­ Varaprasad et al. [51] also formulated nanocomposites based on
action between cellulose and curcumin. It also was found that the EB of sodium carboxymethyl cellulose/silver nanoparticles/curcumin. The TS
the neat cellulose films improved slightly when the curcumin was and EB for the nanocomposites were found to be 15.86 MPa and 2.16%,
incorporated into the films. In another study, Coscia et al. [43] devel­ respectively. It seems that these nanocomposites are brittle due to the
oped a new technique to fabricate cellulose fibers modified with cur­ low value of EB. Incorporating plasticizers such as glycerol and sorbitol
cumin. The cellulose/curcumin composite fibers were obtained by into the film formulation leads to further improvements in the film’s
electrospinning of cellulose/curcumin solution dissolved in 1-ethyl-3-­ extensibility. Other studies in the future are needed regarding the effects
methylimidazolium chloride (EMIN Ac). The value of TS in the manu­ of plasticizer addition on carboxymethyl cellulose/silver nano­
factured cellulose/curcumin composite fibers was 223–336 MPa, which particles/curcumin nanocomposites’ mechanical performance. The
was considerably higher than those reported by other researchers who mechanical parameters of the chitosan/MMT/curcumin nano­
produced cellulose/curcumin composite films [42]. Thus, the developed composites were also determined by Thakur et al. [52]. The TS of the
technique can be introduced as a promising approach to improve cel­ developed nanocomposite was 54.11 MPa, which is higher than most of
lulose/curcumin composite film’s mechanical performance. the synthetic films [31].
In order to increase the compatibility of hydrophobic compounds
and natural polymers such as carbohydrates and proteins, the water 3.1.4. Synthetic films
solubility of these hydrophobic compounds should be improved. The Since the synthetic polymers-based films have good mechanical
antisolvent precipitation technique can enhance the water solubility and performance, the use of a combination of synthetic and natural polymers
dissolution rate of curcumin [44]. In a recent study, curcumin was can be considered as an effective way to produce biodegradable films
treated using the antisolvent precipitation technique and then used to with desirable mechanical properties. In a study by Vimala et al. [53],
formulate hydroxypropyl methylcellulose films [45]. The authors the mechanical characteristics of chitosan-Poly vinyl alcohol (PVA)/­
observed that the addition of native and treated curcumin had no silver/curcumin nanocomposite were investigated. The values of TS and
obvious effect on the films’ mechanical properties and suggested that EB for the developed nanocomposites were, on average, 33.27 MPa and
this observation is due to more rigidity of hydroxypropyl methylcellu­ 5.46%, respectively.
lose structure than curcumin. But, it also may be related to the low Ma et al. [54] applied curcumin with various concentrations (10, 30,
content of curcumin loaded in the films. Further investigation should be and 50 mg g− 1 of polymer) in Tara gum/polyvinyl alcohol films. Con­
conducted to explore the effect of treated curcumin with high concen­ trary to the past research, the authors found that following an increase in
tration on hydroxypropyl methylcellulose films’ mechanical character­ curcumin concentration, the film’s extensibility improved. This effect
istics. In a recent study by Taghinia et al. [46], it was observed that with has been attributed to the formation of phenolic oxygen anions arisen
addition of curcumin in Lallemantia iberica seed gum films, TS increased from the interaction between OH groups of curcumin and OH- groups of
significantly, but, EB showed a decreasing trend. PVA. Phenolic oxygen anions weaken the interaction between polymer
As mentioned before, the encapsulation of hydrophobic compounds and PVA. Furthermore, it may be attributed to the increase of free vol­
like curcumin can result in improvement of their water solubility, and as ume with the addition of curcumin, which was confirmed by SEM
a result, enhancement of the affinity between polymeric matrix and analysis. TS of the films decreased when curcumin was introduced to the
hydrophobic compounds. Wu et al. [47] encapsulated curcumin into films. Curcumin is a small molecule and can reduce the tensile strength
mesoporous silica nanoparticles and then introduced them into of films as plasticizers. In another work, these authors evaluated the
chitosan-based films. They observed that the nanocomposites had high influence of higher curcumin concentrations (100, 150, 200, 250, 300,
TS and plasticity. The desirable mechanical performance of and 500 mg g− 1 of polymer) on Tara gum/polyvinyl alcohol films’ me­
chitosan/curcumin-loaded mesoporous silica nanoparticles can be chanical performance. They found that with an increase in curcumin
related to the increased stiffness of silica that can prevent the collapsing concentration from 0.5% to 5%, TS decreased from 44.22 MPa to
structure of the material, in turn, reinforce the mechanical properties of 25.10 MPa. In comparison, with increasing curcumin concentration
the films [48]. The authors also indicated that incorporating curcumin from 0% to 1%, EB increased, but further increasing curcumin concen­
into chitosan/curcumin-loaded mesoporous silica nanoparticles films tration resulted in a decrease in EB. Conversely, in a recent study, it was
resulted in the increase of TS value from 17.56 to 19.87 MPa. This also found that the addition of curcumin decreased the TS of the
finding could be due to the partial migration of curcumin from SBA-15 PVA-based films [55] (Table 1).
and hydrogen bonds forming with the CS chain during film formation.
However, with curcumin’s addition to film formulation, EB decreased, 3.2. Impact of curcumin on water solubility (WS) and water vapor
which may be attributed to the increasing compactness of chitosan permeability (WVP)
structure. Additionally, the reducing effect of curcumin on EB has also
been attributed to the smaller molecular length of curcumin than chi­ Water solubility indicates the film’s hydrophilicity. The determina­
tosan, which restricts the extensibility of the blend film [38]. tion of WS is useful for choosing a film for specific applications [56]. For
Various efforts have been carried out to improve the mechanical instance, low WS is required to protect food from moisture absorption.
properties of curcumin-loaded nanocomposites. In one of them, ac­ However, in other cases, like the encapsulation of phytochemicals, WS’s
cording to Bajpai et al. [49], the mechanical performance of the chito­ high value may be preferred [57].
san/curcumin films showed a significant improvement after cellulose As mentioned before, biodegradable films are commonly classified
microcrystal addition. The EB values decreased as the cellulose micro­ based on their structural matrix: proteins, polysaccharides, and lipids.
crystal concentration increased. While the TS of the films containing Proteins form the films with high WS and WVP. Combining proteins and
curcumin increased when the cellulose microcrystal concentration polysaccharides is a practical approach to decrease WS and improve the
increased from 0% to 20% and then showed a decreasing trend. In barrier properties [58]. Moreover, different approaches have been pro­
another study [50], the impacts of oxidized chitin nanocrystals and posed to reduce the WS and WVP of protein-based films. Hydrophobic

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N. Aliabbasi et al. Journal of Environmental Chemical Engineering 9 (2021) 105520

Table 1
Mechanical characteristics of curcumin-loaded films.
Film formulation Test conditions Curcumin conc in film Method TS (MPa) EB (%) References
− 1
Gelatin (FG)/curcumin film Film area: 90 mm × 6 mm, Crosshead 400 mg g of protein ASTM 1.9–3.4 144.3–198.6 [19]
speed 0.4 mm s− 1 At 20 ºC D882-02
− 1
Gelatin/curcuma ethanol extract Film area: 120 mm × 25.4 mm, 0.275–11 mg g of protein ASTM 28.8–35.1 25.0–36.5 [21]
Crosshead speed 50 mm s− 1 D882-10
Chicken skin gelatin/rice starch/ Film area: 70 mm × 6 mm, Crosshead – – 2.29–8.41 228.77–348.07 [22]
curcumin film speed 1 mm s− 1
1
Fish gelatin/curcumin/ Film area: 60 mm × 20 mm, Crosshead 100–500 mg g− of protein ASTM 12.18 267.56 [32]
β-cyclodextrin speed 10 mm min− 1 At room temperature D638
− 1
Caseinate/zein/curcumin Film area: 80 mm × 25 mm, Crosshead 100 mg g of proteins ASTM ≈3.7–6.4 ≈25–50 [25]
speed 50 mm min− 1 D882
Carboxymethylated guar gum Film area: 20 mm × 5 mm, Crosshead – – 41.64 – [30]
grafted gelatin/curcumin film speed 5 mm min− 1 At 25 ºC
Chitosan/curcumin film Film area: 50 mm × 10 mm, Crosshead 10 mg g− 1of polysaccharide UNI ISO 11.82 39.41 [38]
speed 5 mm min− 1 At room temperature 517-1
Chitosan/curcumin film Film area: 120 mm × 25 mm, Crosshead 0.5–1% (wt) ASTM D- 13.2–43.3 2.1–20.6 [39]
speed 0.2 mm s− 1 At 25 ºC 88291
Chitosan/curcumin film Film area: 150 mm × 25.4 mm, 1.0 (wt%) ASTM D 39.8 ± 0.3 13.8 ± 1.4 [40]
Crosshead speed 50 mm min− 1 88-88
1
Chitosan/cellulose crystal Film area: 39 mm × 5.8 mm, Crosshead 0.45 mg g− of film – ~2.5–13 ~5.5–14 [49]
curcumin speed 40 and 200 mm min− 1 At 23 ºC
Chitosan/MMT/nanoparticles/ Crosshead speed 50 and 50 mm min− 1 At 11.76 mg g− 1
of polysaccharide ASTM 17.39–21.01 36.17–39.26 [52]
curcumin room temperature D882-91
Chitosan/curcumin-loaded Film area: 50 mm × 10 mm – ASTM 19.87 25.46 [47]
mesoporous silica nanoparticles
− 1
Curcumin encapsulated chitosan- Film area: 100 mm × 10 mm, Crosshead 0.01 mg g of polymer – 33.27 5.46 [53]
PVA-silver nanoparticle film speed 5 mm min− 1
1
Chitosan/oxidized chitin Film area: 30 mm × 10 mm 10 mg g− of polymer ASTM 23-35 22-28 [50]
nanocrystal/curcumin D882-09
Cellulose/curcumin film Film area: 50 mm × 10 mm, Crosshead 1–5 (wt%) – 6.0–6.7 9.1–10.1 [42]
speed 2 mm min− 1
Cellulose/curcumin composite Crosshead speed 2 mm min− 1 At 20 ºC 10–100 mg g of − 1
– 223–336 8.5–12.8 [43]
fiber polysaccharide
Sodium carboxymethyl Cellulose/ Film area: 100 mm × 10 mm, Crosshead 0.01 mg g− 1 of polysaccharide – 15.86 2.16 [51]
As NP/curcumin speed 5 mm min− 1
1
Hydroxypropyl methylcellulose Film area: 90 mm × 25 mm, Crosshead 0.01 mg g− of polymers ASTM D – – [45]
film speed 0.7 mm s− 1 At 25 ºC 882-12
k-carrageenan/curcumin Film area: 100 mm × 10 mm, Crosshead 500, 1500, 2500 and ASTM – – [41]
speed 0.5 mm s− 1 3500 mg g-1of polysaccharide D882-91
k-carrageenan/curcumin film Film area: 150 mm × 25.4 mm, 10 mg g− 1of polysaccharide ASTM D 42.4 ± 1.1 2.51 ± 0.0 [40]
Crosshead speed 50 mm min− 1 882–88
Agar/curcumin film Film area: 150 mm × 25.4 mm, 10 mg g− 1of polysaccharide ASTM D 50.1 ± 1.0 1.72 ± 0.1 [40]
Crosshead speed 50 mm min− 1 882-88
Lallemantia iberica seed gum film Film area: 100 mm × 10 mm, Crosshead 0.2–0.6% ASTM 17.11–23.21 56.32–98.14 [46]
speed 0.5 mm s− 1 D882-91
− 1
Tara gum/PVA/curcumin films Film area: 80 mm × 15 mm, Crosshead 10, 30 and 50 mg g of – 38.42–44.22 6.07–20.8 [54]
speed 300 mm min− 1 polysaccharide
Tara gum/PVA/curcumin films Film area: 80 mm × 15 mm, Crosshead 100, 150, 200, 250, 300 and – 25.10–40.91 11.24–20.8 [68]
speed 300 mm min− 1 500 mg g− 1of polysaccharide
Low-density polyethylene film Film area: 50 mm × 10 mm – ASTM 11.8 600 [31]
Poly(vinyl alcohol) film Film area: 150 mm × 25.4 mm, – ASTM D 28.6–40.6 72.0–158.0 [55]
Crosshead speed 50 mm min− 1 882-88

bioactive compounds such as curcumin in film formulation are among curcumin and proteins. But, the authors claimed that the change in pH of
the most effective techniques to solve this problem. the film-forming solutions did not affect WS and WVP of gelatin film
with incorporated curcumin or not. Likewise, Said and Sarbon [22]
3.2.1. Protein-based films observed that the WVP of curcumin-loaded chicken skin gelatin/rice
Gelatin is an inexpensive, biocompatible, biodegradable, and readily starch films was significantly lower than that without curcumin. Several
available biopolymer with excellent film-forming properties [59]. parameters affect films’ barrier properties, such as the hydro­
However, it is highly water-soluble, and thus searching for new methods phobic/hydrophilic balance of film components, the crystallinity of
to decrease the WS and WVP of the gelatin-based film has attracted films, pathway tortuosity, and structural defects [60]. Curcumin is a
researchers’ attention. The effect of pH, two solvents (water and hydrophobic compound comprised of the long carbon chain and ben­
ethanol-water mixture), and curcumin addition on gelatin films’ phys­ zene ring (See Fig. 1). Such a structure prolongs the penetration of water
ical characteristics were investigated by Musso et al. [19]. The addition molecules through the composites [41]. Moreover, the hydrogen
of curcumin with a concentration of 400 (mg g− 1 of protein) signifi­ bonding and/or hydrophobic interactions between curcumin and func­
cantly increased the hydrophobic character of gelatin films, and as a tional groups present in gelatin structure decrease the number of polar
result, reduced the WVP of the films. However, the gelatin films loaded groups and reduce the films’ water permeability [61]. A similar effect
with curcumin had similar WS to pure films. This observation may be has been reported for curcumin’s impact on the values of WVP in
related to the morphological properties and compactness of film struc­ caseinate/zein nanocomposite films [25].
ture. An SEM analysis is suggested to elucidate the structural changes In another study, Wu et al. [32] developed an eco-friendly film based
that occurred after introducing curcumin to the gelatin film. The change on the gelatin of silver crap skin/β-cyclodextrin (GL-βCD-film). First,
in pH of the film-forming solution affects the interaction between curcumin was loaded to β-cyclodextrin, and then the encapsulated

5
N. Aliabbasi et al. Journal of Environmental Chemical Engineering 9 (2021) 105520

curcumin was incorporated into gelatin films (GL-βCD-CUR film). It was properties was investigated in a recent study [41]. They used a wide
observed that the encapsulation of curcumin significantly increased the range of curcumin concentrations (500, 1500, 2500, and 3500 mg g− 1of
WS of curcumin. Furthermore, the homogeneity of the particles also polysaccharides). WVP decreased as the curcumin concentration
improved after encapsulation. Following an increase in encapsulated increased from 500 to 1500 (mg g− 1of polysaccharide). This fact is to be
curcumin content from 0 to 100 (mg g− 1 of protein), the WS of the film expected since curcumin is a strongly hydrophobic compound. Simi­
increased from 21.22% to 54.48%. According to the authors of this larly, Taghinia et al. [46] showed that with addition of curcumin to
article, curcumin molecules entrap into the cavities and holes of βCD, Lallemantia iberica seed gum-based film, WVP and WS decreased. In
their water solubility increase, so the films’ WS increases. Accordingly, another study, Salarbashi et al. [65] also found that when the curcumin
the gelatin film introduced by encapsulated curcumin had higher WS was incorporated into soluble soybean polysaccharide films, WVP and
values compared with those containing free curcumin. WS decreased.
On the other hand, with the increase in curcumin concentration from
100 to 250 (mg g− 1 of protein), the WS decreased; however, a further 3.2.3. Synthetic films
increase in curcumin concentration led to an increase in WS. The In synthetic polymers, LDPE is commonly used to fabricate pack­
permeability and WS of films depend on their structural and morpho­ aging systems due to its excellent physico-mechanical properties. Zia
logical properties. Based on SEM analysis, the GL-βCD-CUR film struc­ et al. [66] showed that the addition of curcumin to LDPE film formu­
ture containing 250 (mg g− 1 of protein) curcumin had a higher density lation improved its water vapor barrier performance. As mentioned
than the film incorporated by 100 or 500 (mg g− 1 of protein) curcumin. before, this observation is related to the hydrophobic nature of curcu­
WVP of the GL-βCD-films was 2.38 × 10− 10 (g m− 1 Pa− 1 s− 1). With the min. The authors also stated that this effect might be due to the decrease
increase of curcumin concentration, the WVP of the film slightly in the distance between the chains of polymer macromolecules that
decreased, which has been attributed to the hydrophobic nature of hinders water molecules’ diffusion through the films. Likewise,
curcumin. It was expected that hydrophobic compounds’ presence acts Abazović et al. [67] developed an intelligent film based on PVA/­
as an obstacle for hydrogen interactions, and it causes a decrease in curcumin and showed that with increasing curcumin concentration,
WVP. However, as mentioned above, the curcumin loaded into βCD had WVP decreased significantly.
a higher value of WS. Hence, the reduction in WVP with the increase of Ma et al. [68], in two separate studies, indicated that introducing
curcumin content might be due to the higher compaction structure of the curcumin to Tara/PVA film formulation led to increasing in WS and
GL-βCD-CUR than a neat GL film. WVP values. The authors suggested that phenolic oxygen anions in
curcumin structure act as an obstacle for intermolecular interactions
3.2.2. Polysaccharide-based films between Tara and PVA macromolecules, weakened the compatibility of
The presence of hydrophilic functional groups in the backbone of these polymers, and as results increase WVP and WS of the Tara/PVA
polysaccharides facilitates hydrogen bonding between polysaccharides film.
and water molecules, which in turn increases WS and WVP of
polysaccharides-based films. To date, several attempts have been carried 3.3. The antimicrobial, anti-mold, and anti-yeast activity
out to reduce the wettability and WVP of polysaccharides-based films.
As mentioned before, the addition of curcumin to film formulation could Different works have been published on the antimicrobial activity of
reduce WS and WVP of protein-based films. However, Liu et al. [38] curcumin loaded biopolymers-based films (Table 2). At this point of the
showed that incorporating curcumin had no considerable effect on study, we have reviewed the effectiveness of fabricated packaging sys­
chitosan films’ barrier properties, which may be associated with too low tems loaded with curcumin for imparting antimicrobial activity.
curcumin concentration used in this study (10 mg g− 1of poly­
saccharides). Chitosan has both hydroxyl and carboxyl groups, and thus 3.3.1. Polysaccharide-based films
it can easily interact with water. Accordingly, a high level of curcumin Liu et al. [38] fabricated an active packaging system based on chi­
should be added to the chitosan film to reduce the WVP. The effect of tosan (molecular weight, 110 kD) and curcumin and tested the films’
curcumin addition to chitosan-based film formulation on WS and WVP antimicrobial activity. For this purpose, two microorganisms, Staphylo­
was also investigated among other research [39]. As expected, the coccus aureus, a common food poisoning bacteria, and Rhizoctonia solani,
addition of curcumin reduced the WVP of the chitosan films. The pres­ a pathogenic fungus, were tested. A clear inhibition zone (12 mm and
ence of curcumin crystals on the film surface can act as a barrier and 20.8 mm for S. aureus and R. solani, respectively) for the chitosan film
decrease water diffusion. Likewise, Pereira and Andrade [62] demon­ incorporated with curcumin (10 mg g− 1of polysaccharides) was re­
strated that the use of curcumin in chitosan film formulation led to a ported. The chitosan film’s antimicrobial effect against these microor­
decrease in the values of WS and WVP. The same results have been re­ ganisms was also examined to determine chitosan film’s antimicrobial
ported by Roy and Rhim [40] and Wu et al. [50], who evaluated the activity without curcumin. The inhibition zone diameter against
effect of curcumin WVP of several carbohydrate-based films. S. aureus for both pure chitosan and curcumin-loaded chitosan films was
Rostami and Esfahani [63] used a new polysaccharide source ob­ 10 mm and 12 mm, respectively, showing the inhibitory effect of the
tained from Melissa officinalis seeds (MOSG) to form an intelligent film. chitosan/curcumin film is mainly related to chitosan [69]. In positively
In this regard, Na+-montmorillonite (MMT) nanoparticles were used to charged polymers (eg, chitosan), when the pH of the polymers disper­
improve the physico-mechanical characteristics of the films, and then sion reduces up to acid dissociation constant (pKa) (for chitosan is 6.3),
curcumin was loaded into the films. Considering their findings, the WS the amino groups present in the structure of cationic polysaccharides
and WVP values of MOSG /MMT/curcumin were significantly lower will be largely dissociated, and then, making it positively charged [70].
than MOSG films with or without MMT. SEM images revealed a ho­ The antimicrobial effect of chitosan has been attributed to amino
mogenous and continuous structure for the developed films, indicating groups’ reaction and negatively charged microbial cell membranes,
excellent compatibility between MOSG and curcumin. The reason for leading to the leakage of proteinaceous and other intracellular constit­
that may be associated with the presence of tween 80 as an emulsifier in uents of the cell [71]. The antifungal activity of curcumin against a
the film formulation. Emulsifiers are commonly employed to avoid broad spectrum of fungus has also been well documented in an excellent
precipitation and improve the stability of emulsions [64]. In the absence review [72]. R. solani causes several diseases in some vegetables (to­
of emulsifier, plenty of curcumin molecules precipitates after ethanol mato, sugar-beet, and watermelon). Thus, the developed film can be
removal. Hence, emulsifiers in the formulation of the polysaccharide­ introduced as a promising packaging for vegetables. Similarly, Roy and
s/proteins based films incorporated with curcumin were suggested. The Rhim [40] observed that chitosan/film inhibited the growth of E. coli
effect of curcumin concentration on the k-carrageenan film’s barrier and L. monocytogenes.

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Table 2
Antimicrobial activity of curcumin loaded polymer-based films.
Microorganisms Film formulation Zone inhibition (mm) References

Bacteria Gram-negative
E.coli Guar gum grafted gelatin/curcumin 16.0 [30]
Chitosan/curcumin-loaded silica nanoparticles ~8.5 [47]
Gelatin/curcumin 0 [19]
Chitosan/cellulose crystal/curcumin 40.0 [49]
Curcumin encapsulated chitosan-PVA 18.0 [53]
Curcumin encapsulated by carboxyl methylcellulose 6.0 [49]
Polyacrylonitrile/curcumin 8–10 [83]
Hydrogel-silver nanoparticle-curcumin composites 90% inhibition growth [51]
Chitosan/curcumin – [40]
Agar/curcumin – [40]
Carrageenan/curcumin – [40]
Cellulose/curcumin 7–23 [42]
E. aerogenes Guar gum grafted gelatin/curcumin 16.0 [30]
V. vulnificus Guar gum grafted gelatin/curcumin 16.0 [30]
P. aeruginosa Guar gum grafted gelatin/curcumin 12.0 [30]
Curcumin encapsulated by chitosan-PVA 10.0 [53]
S. Enteritidis Gelatin/curcumin 0 [19]
S. pseudomona Curcumin encapsulated chitosan-PVA 19.0 [53]
k. pneumonia Polyacrylonitrile/curcumin 8–10 [83]
Gram-positive
B. cereus Guar gum grafted gelatin/curcumin 16.0 [30]
Gelatin/curcumin 0 [19]
B. subtilis Guar gum grafted gelatin/curcumin 17.0 [30]
Polyacrylonitrile/curcumin 8–10 [83]
Micrococcus Curcumin encapsulated chitosan-PVA 17.0 [53]
Lysinibacillus Guar gum grafted gelatin/curcumin 15.0 [30]
S. aureus Guar gum grafted gelatin/curcumin 15.0 [30]
Gelatin/curcumin 0 [19]
Chitosan/curcumin-loaded silica nanoparticles ~ 10.5 [47]
Chitosan/curcumin 12.0 [38]
Polyacrylonitrile/curcumin 8–10 [83]
L. monocytogenes Chitosan/curcumin – [40]
Agar/curcumin – [40]
Carrageenan/curcumin – [40]
Yeast C. albicans Chitosan/cellulose crystal/curcumin 30.0–35.0 [49]
Curcumin encapsulated chitosan-PVA film 11.0 [53]
C. parapsilosis Chitosan/cellulose crystal/curcumin 30–35.0 [49]
Fungus R. solani Chitosan/curcumin 20.8 [38]
P. expansum Lallemantia iberica seed gum 13.66 [46]

Although chitosan as a desirable antimicrobial agent is effective Cu/chitosan. This observation may be due to the sustained release of
against a wide range of microorganisms, Bajpai et al. [49] showed that curcumin from Cu-SBA-chitosan films. Similar observations have been
chitosan (molecular weight, 1463 kDa)/carboxyl methylcellulose reported on the effect of curcumin on antimicrobial activity of some
without curcumin had no inhibition activity against E. coli, C. para­ polysaccharides-based films such as agar, cellulose, carrageenan films
psilosis, and C. albicans. The antibacterial activity of chitosan is molec­ [40,42]. In another study [75], it was found that the maximum release of
ular weight-dependent [73]. Accordingly, the absence of antimicrobial curcumin from cellulose acetate/curcumin membranes was higher than
effect in chitosan (molecular weight, 1463 kDa)/carboxyl methylcellu­ the MIC of curcumin (15.7 mg L− 1) [76], demonstrating the developed
lose without curcumin may be related to chitosan’s molecular weight composites can be employed as an active packaging with desirable
used to fabricate the developed film. On the other hand, the authors antimicrobial activity. Kuswandi et al. [77] also designed a bacterial
showed that incorporating curcumin (0.45 mg mL− 1 of the film) into cellulose based packaging film. The designed films had an excellent
chitosan (molecular weight, 1463 kDa)/carboxyl methylcellulose film antimicrobial effect against Pseudomonas auroginosa bacteria.
effectively inhibits the growth of tested microorganisms. Antibacterial and anti-mold activity of the curcumin-loaded Lalle­
Other findings demonstrated that with the addition of turmeric mantia iberica seed gum films were studied by Taghinia, Abdolshahi,
extract to chitosan (low molecular weight) based film, the antimicrobial Sedaghati and Shokrollahi [46]. The film incorporated with curcumin
effect against two common food poisoning bacteria, S. aureus, and Sal­ showed clear microbial inhibition zones against Escherichia coli O157:
monella, was improved [74]. In contrast, the chitosan film showed H7EDL 933, Bacillus cereus PTCC 1247, Bacillus subtilis PTCC 1023
considerable antibacterial activity against tested microorganisms. (ATCC 6633), and Penicillium expansum. As discussed above, the
Furthermore, the film containing turmeric showed more antibacterial hydrogen-bonding and hydrophobic interactions of curcumin and
activity than pure chitosan film, which is associated with curcumin, membranal proteins of the bacterial cells alter the membranes perme­
curcuminoid, and terpenoids in turmeric extract. ability, consequently, inhibit the bacterial growth.
In another investigation, Wu et al. [47] introduced curcumin loaded
mesoporous silica nanoparticles (Cu-SBA) to chitosan-based film to 3.3.2. Protein-based films
enhance its antimicrobial properties. For evaluating the nano­ The interaction between curcumin and polymeric matrix changes the
composites’ antimicrobial activity, the inhibition zone of two food antibacterial and anti-mold effects of biopolymer-based films. For
pathogens, bacteria, i.e., E. coli and S. aureus, was recorded. Unexpect­ instance, despite the numerous data on the antimicrobial activity of
edly, the antimicrobial effect of Cu-SBA-chitosan was less than curcumin, Musso et al. [19] observed that gelatin/curcumin film had no

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N. Aliabbasi et al. Journal of Environmental Chemical Engineering 9 (2021) 105520

antimicrobial effect against S. Enteritidis, E. coli, B. cereus, and S. aureus. Table 3


This phenomenon has been explained as the low concentration of cur­ Overview migration researches on curcumin loaded into packaging systems.
cumin loaded in gelatin films and the interaction between gelatin and Film formulation Simulant Test conditions References
curcumin [19]. The interactions between phenolic groups, amino acids,
Fish gelatin/curcumin Phosphate-buffered At 22 ºC for [19]
and proteins occur via H-bonding and hydrophobic interactions [78,79]. saline solution 168 h
The hydrogen bonding and hydrophobic interactions of the bacterial Fish gelatin/curcumin/ Phosphate-buffered At 22 ºC for [32]
cells’ phenols and membranal proteins alter the membrane’s perme­ β-cyclodextrin saline solution 168 h
ability and inhibit bacterial growth. As mentioned above, proteins could Cataractous eye protein/ Phosphate-buffered – [80]
curcumin saline solution with
interact with phenolic compounds such as curcumin and block the active two pHs 4.8 and 7.4
sites for the desired reactions. Besides the compounds’ inherent anti­ Carboxymethylated guar Phosphate-buffered At 32 ºC for [30]
microbial activity, the medium in which the antimicrobial agents have gum grafted gelatin/ saline solution 96 h
to execute their function is essential. Likewise, Parveen et al. [80] curcumin film
Chitosan/MMT Phosphate-buffered At 32 ºC for 8 h [52]
showed that curcumin-loaded cataractous eye protein isolate films had
nanoparticles/curcumin saline solution/
no antibacterial activity against S. aureus. On the other hand, Manna ethanol (50:50 v/v)
et al. [30] indicated that curcumin-loaded carboxymethylated guar gum Chitosan/curcumin Water At 37 ºC for 6 h [40]
grafted gelatin film could considerably inhibit the bacteria growth. This Chitosan-PVA/curcumin Phosphate-buffered At room [53]
effect might be due to the interaction between guar gum and curcumin film saline solution temperature
for 6 h
that prevent protein-curcumin interaction. Curcumin encapsulated Phosphate-buffered At room [53]
Wang et al. [81] investigated the antimicrobial activity of curcumin chitosan-PVA-silver saline solution temperature
loaded zein fibers against S.aureus and E. coli. Zein-curcumin fibers nanoparticle film for 6 h
showed better antimicrobial activity against S.aureus than E. coli at the Chitosan/cellulose crystal Physiological fluid At 37 ºC for 1 h [49]
k-carrageenan/curcumin Ethanol At 25 ºC [41]
same curcumin content. This can be explained by the fact that the
k-carrageenan/curcumin Water At 37 ºC for 6 h [40]
peptidoglycan layer present in the cell’s gram-negative bacteria struc­ Agar/curcumin Water At 37 ºC for 6 h [40]
ture is thin that preserves them against different antimicrobial agents Cellulose acetate/ Distilled water/ At room [75]
like curcumin [82]. curcumin Ethanol (80:20) temperature
Hydroxypropyl Ethanol At room [45]
methylcellulose/ temperature
3.3.3. Synthetic films
curcumin
In a study, the antimicrobial activity of polyacrylonitrile films Sodium carboxymethyl Phosphate-buffered At 37 ºC for [51]
incorporated with curcumin was investigated by the agar diffusion cellulose/As NP/ saline solution 6.4 h
technique [83]. The films’ antibacterial capacity was examined against curcumin
Polyacrylonitrile/ Phosphate-buffered For 5 h [83]
both gram-negative (E.coli and k. pneumonia) and gram-positive bacteria
curcumin saline solution
(B. subtilis and S. aureus). Based on the findings, the poly­
acrylonitrile/curcumin combination inhibits these bacteria’s growth
even at a low concentration of curcumin. This study’s curcumin con­ 3.4.1. Polysaccharide-based films
centration was similar to that used in gelatin/curcumin films mentioned Manna et al. [30] also introduced curcumin to carboxymethylated
above [19], confirming the polymer matrix’s vital role in producing guar gum grafted gelatin. The sustained release of curcumin resulted in
packaging films. restricting bacterial growth for a prolonged time. The release rate of
The antimicrobial and anti-mold activities of the nanocomposite curcumin from other protein-based films was also investigated by
films incorporated (chitosan/poly (vinyl alcohol) to encapsulate cur­ Parveen et al. [80].
cumin) with nano encapsulated curcumin have been investigated by In another study, Thakur et al. [52] produced nanocomposite based
Vimala et al. [53]. Three techniques (disc diffusion, viable cell count, chitosan/Montmorillonite (MMT) (1:1, 1:4, and 4:1) incorporated with
and spread plate methods) were employed to test the developed nano­ curcumin. In all of the tested nanocomposites, the strong electrostatic
composites’ antibacterial and antifungal activity. The curcumin loaded interaction between chitosan and MMT led to a sustained release of
nanocomposite films inhibited the growth of E. coli, P. pseudomonas, curcumin. The controlled release of curcumin from k-carrageenan films
Staphylococcus, Micrococcus, P. auroginosa, and C. albicans. Therefore, was tested by Liu et al. [41]. The testing films (1.5 cm × 1.5 cm) were
the developed nanocomposite films can be used as a useful packaging dispersed in 250 mL flasks containing 100 mL ethanol aqueous (95%, as
system to prevent/treat the infection. fatty acids stimulant), and then the flasks were moved to a shaking
The designing of novel metallodrugs-ecofriendly materials with incubator (100 rpm, 25 ◦ C) under dark condition. The authors reported
improved antimicrobial properties has attracted scientists’ attention in that in the first three hours, the release rate was high, which is due to the
recent years. Papadimitriou et al. [84] synthesized [ZnI2 (curcumin)2] as presence of a low amount of curcumin on the surface of the films.
a new complex antimicrobial agent and then investigates this antimi­ Subsequently the release rate of curcumin decreased after 72 h of con­
crobial agent’s dispersion in packaging material based on polystyrene. tact of the film with the PBS solution.
The results revealed that MIC values for curcumin and [ZnI2 (curcu­ Similar results have been reported by Roy and Rhim [40], who
min)2] were 75.3 μg mL− 1 and 125 μg mL− 1, respectively. Hence, it investigated the release of curcumin from different types of
seems that the complex antimicrobial agent such as [ZnI2 (curcumin)2] carbohydrates-based films. However, the authors stated that the release
is a better candidate for the development of new active packaging sys­ properties of curcumin were carbohydrate type-dependent. It seems that
tems than pure curcumin. However, further studies on evaluating the there is a positive correlation between water solubility and the release
toxicity or genotoxicity of this complex should be carried out. rate of curcumin, which is opposite to those observed on the top side.

3.4.2. Protein-based films


3.4. Control release properties In a study, cataractous eye protein was used as a film matrix, and
curcumin was added to the film formulation. The release of curcumin
Different studies have been investigated in vitro release properties of was monitored in two mediums (buffer systems with pH 7.4 and 4.5).
curcumin from biodegradable films (Table 3):

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N. Aliabbasi et al. Journal of Environmental Chemical Engineering 9 (2021) 105520

The release rate of curcumin into the buffer system with a pH of 4.5 was In a recent study, Baldino et al. [75] used a process assisted by su­
faster when compared to that observed in pH 7.5, which is due to the percritical CO2 to fabricate an active packaging based cellulose aceta­
more solubility of curcumin at lower pH [85]. Alehosseini et al. [86] te/curcumin. The release kinetic of curcumin from the developed film
evaluated the release rate of curcumin from the protein fibers (gelatin into an aqueous solution (80% water and 20% ethanol) was evaluated. It
and zein-based fibers) in two different food simulants, including Ethanol was found that as the cellulose acetate content increased in film
50% and vegetable oil (soybean oil). The release rate of curcumin from formulation, the release rate decreased. This phenomenon is due to the
the gelatin coatings was more than zein fibers, attributed to the swelling more compact structure of the film containing higher cellulose acetate
of gelatin in this medium and the excellent solubility of phosphatidyl­ concentration, confirmed by SEM analysis. Any factor that can change
choline in ethanol. the morphological and microstructural characteristics of films, such as
the fabrication method or the concentration of polymer and bioactive
3.4.3. Polysaccharide/protein films agent, may affect the release behavior of curcumin from the film. The
Wu et al. [32] investigated in vitro release of curcumin from fish effect of curcumin (10% and 20% w/w) and polymer concentration
gelatin (FG)/β-cyclodextrin film. As mentioned above, curcumin has low (12%, 18%, and 24% w/w) and processing conditions on release prop­
water solubility, and thus another simulant, such as phosphate-buffered erties of curcumin from cellulose acetate films was studied by Baldino
saline solution, is commonly used to investigate the in vitro release of et al. [75]. As expected, with an increase in the curcumin concentration
curcumin. The authors used a phosphate-buffered saline solution to from 10% to 20%, curcumin’s release rate increased considerably.
investigate the release behavior of curcumin from FG/β-cyclodextrin Moreover, an increase in process temperature was accompanied by a
films. They found that the release rate of curcumin from FG film (92.8%) slight increase in the release of curcumin. In another study, the release
was considerably higher than FG/β-cyclodextrin film (63.67%). This properties of curcumin from Polyvinylidene fluoride-hexafluoro
observation has been attributed to the tubular structure of β-cyclodex­ propylene porous structures incorporated with 3% w/w curcumin,
trin, which provides cavities for the entrapment of hydrophobic com­ constructed by supercritical assisted technique, was investigated. The
pounds [87]. Curcumin molecules may be entrapped into the inner maximum release of curcumin was prolonged up to 44 h for 12% w/w
cavities, bonded with hydrophobic groups of β-cyclodextrin, and coated PVDF-HFP aerogel. Kosmeyer-Peppas model could describe the curcu­
by β-cyclodextrin macromolecules. Thus, curcumin remains in the min release experimental data for PVDF-HFP-curcumin membranes and
package for a longer time. aerogels [10].
The release properties of curcumin from k-carrageenan film have
3.4.4. Synthetic films been described in a recent study [41]. The Peppas model’s release
The migration of curcumin from a synthetic packaging system exponent was 0.49, which was near to the value that corresponded to the
fabricated from LDPE/curcumin (5 wt%) to ethanol was tested by Zia Fickian diffusion mechanism. Hence, the release of curcumin from the
et al. [66]. They found that in the first 6 h of the release process, the k-carrageenan film obeys Fickian’s mechanism.
release rate was high, and subsequently, the release rate of curcumin
decreased considerably. Considering the sustained release of curcumin 4. Films and coatings with the incorporation of curcumin:
from LDPE/curcumin films, it is expected that this packaging system can Applications
be used for inhibiting the oxidation of foods.
Diverse biological activities and sensitivity against pH change make
3.4.5. Mathematical modeling curcumin ideal for application in intelligent packaging systems. The
Different models, including zero-order diffusion, first-order diffu­ films containing curcumin can inform consumers that the product is
sion, Higuchi’s diffusion, Korsmeyer’s Peppas, and Hixson-Crowell suitable for consumption or not. To date, various studies have been
models, are commonly employed to describe the release profile of conducted to fabricate intelligent packaging systems incorporated with
bioactive compounds: curcumin (Table 4). In a recent study, the color stability and variability
In the following, an overview of recent advances in mathematical of curcumin, betanin, and anthocyanin solutions under various com­
modeling of the curcumin release will be presented together with a mercial food storage conditions and pHs were studied. It was found that
discussion of the corresponding observations. curcumin was a more powerful colorant, but lost its stability over stor­
Thakur et al. [52] used different models, including Higuchi’s diffu­ age period [90]. Similarly, Yang et al. [91] observed that cellulo­
sion and Korsmeyer’s Peppas, zero order, first order, and Hixson Crowell se/chitin films changed their colors from yellow to reddish brown as pH
models, to describe the release profile curcumin from chitosan/MMT increase from 1.0 to 13.0. In another study, a pH-sensitive film, based on
nanocomposites. The release exponent value obtained from Korsmeyer’s chitosan and curcumin, was successfully fabricated by Pereira and
Peppas model was between 0.46 and 0.62, demonstrating an anomalous Andrade [62]. As expected, in aqueous environments, the films showed
or non-Fickian transport release behavior [88,89]. excellent responses to pH changes, mainly for pHs higher than 8.
Varaprasad et al. [51] developed a bionanocomposite based sodium Etxabide et al. [92] also reported that the incorporation of curcumin
carboxymethyl cellulose/As NP/curcumin and investigate the release into gelatin films provided films with the capacity to sense pH changes
profile of curcumin. The authors modeled the release data to determine before and after immersion in a fatty food simulant. Thus, they are
the release mechanism of curcumin-loaded films. The modeling pa­ suitable for intelligent fatty food packaging applications.
rameters, including n and k, were found to be 1.62 and 2.37, respec­ In most animal-based protein foods such as fish, pork, and shrimp,
tively, which indicate super Case II release kinetic. In another study, the microorganisms produce volatile compounds known as total volatile
release of curcumin from polyacrylonitrile based films was analyzed base nitrogen (TVBN). TVBN is commonly used as an indicator to
[83]. They used two models, including Higuchi’s diffusion and Kors­ monitor the freshness of the seafood. The conventional techniques to
meyer’s Peppas models, to fit the release data. It was found that Higu­ determine TVBN are steam distillation, followed by the titration of
chi’s diffusion model was better for describing the release of curcumin amines with HCL, photometric method, and chromatography analysis
from the developed film. with solid-phase microextraction [95,96]. Unfortunately, these methods
Bajpai et al. [49] loaded curcumin into chitosan/cellulose crystal are time-consuming and expensive. Therefore, it is essential to introduce
film and analyzed its release into the physiological fluid. It was found a rapid and inexpensive technique to monitor the spoilage of seafood. In
that with the increase of cellulose crystal concentration, the release rate basic spoilage, the phenolic hydroxyl groups of curcumin can react with
of curcumin decreased, indicating cellulose crystal particles act as a OH and form phenoxide anion that changes curcumin color.
hindrance for releasing curcumin from the films. They used Higuchi’s The color-changing of the films fabricated by curcumin/gelatin
diffusion model to fit release data. exposing liquid, semisolid, and gaseous media with various pH were

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N. Aliabbasi et al. Journal of Environmental Chemical Engineering 9 (2021) 105520

Table 4 stages, the films with PDADMAC on the top are more appropriate than
Recent studies on determining the freshness of foods. those of PSS.
Film/ Film/coating solution Food application References In order to monitor the bacterial spoilage of shrimp, Kuswandi et al.
coating formulation [77] fabricated a real-time monitoring system based on bacterial cellu­
Film Gelatin/ (a) Protecting apple juice [32] lose membrane/curcumin that could accurately detect the onset of
β-cyclodextrin/ against browning; (b) spoilage in shrimp. As shown in Fig. 3, when the shrimp’s storage time
curcumin Preserving polyphenols against increased from 0 to 18 h, the concentration of TVBN formed by micro­
oxidation bial spoilage increased, and then, the sensor response increased. In
Film Gelatin/curcumin Sensing pH change of liquid, [19]
semisolid and gaseous media
another study, a pH sensing indicator was developed by Liu et al. [41] to
Film Gelatin/curcumin Sensing pH change before and [90] evaluate pork and shrimp’s freshness. This indicator was fabricated by
after immersion in a fatty food curcumin/k-carrageenan. A good linear relationship was observed be­
simulant tween the levels of TVBN in both tested foods and the value of a* over
Film k-carrageenan/ Determining the freshness of [41]
storage time. The authors suggested that the intelligent packaging sys­
curcumin shrimp and pork
Film Bacterial cellulose Detecting the onset of shrimp [77] tem based on curcumin/k-carrageenan can be introduced as a useful
membrane/curcumin spoilage indicator to monitor animal-based protein foods’ freshness.
Film PDADMAC/curcumin Sensing pH change at pH 7.5 [93] In another study, Ezati and Rhim [97] developed a pH-sensitive
Film Chitosan/oxidized Determining the freshness of [47] pectin-based films by adding curcumin and sulfur nanoparticles (SNP).
chitin nanocrystals/ pomfrets meat and shrimp
curcumin
When these films were applied for shrimp packaging, they exhibited a
Film Starch/PVA/ Indicating three different [99] pH-responsive highly distinctive color change from yellow to orange as
curcumin/ colors corresponding to the quality of the shrimp changed. A pH sensing indicator was developed
anthocyanins freshness, medium freshness, by Taghinia et al. [46] to monitor the freshness of shrimp. As expected,
and spoilage.
the authors reported that TVBN content of the shrimp samples increased
Film Lallemantia iberica Determining the freshness of [46]
seed gum/curcumin shrimp over storage time. They also found that a* value of LISG/curcumin film
Film Pectin/Curcumin/ Determining the freshness of [97] increased significantly when the storage time increased to 5 days,
Sulfur nanoparticles shrimp indicating the developed smart packaging system could successfully
Coating Encapsulated Preserving the quality of the [94] detect the shrimp spoilage. Likewise, Salarbashi et al. [65] showed that
curcumin in gelatin tested foods over the storage
there is a strong positive correlation between TVBN content of shrimp
and starch period (72 h).
and a* values of the soluble soybean polysaccharide films during storage
time (Pearson’s correlation = 0.985).
investigated by Musso et al. [19] and indicated that the films could sense Zhang et al. [98] constructed an intelligent hydrogel using chitosan,
pH change in all the tested media. The color-changing of the films was bacterial cellulose, and curcumin to monitor the freshness of shrimp.
more visually clear when they were exposed to liquid and gaseous The curcumin film gradually changed from yellow to orange-red with
media. Overall, it is expected that curcumin/gelatin films can be used to the decrease of the sample’s freshness. The curcumin film indicated a
detect the pH changes resulting from the spoilage of liquid, semisolid, clear color changes which the ΔE values were increased to 36.5 at 60 h.
and canned foods. It should be noted that the sensor’s sensitivity A positive correlation was reported between the changed color and the
incorporated with curcumin is dependent on the fabricating method. For TVB-N level with a coefficient of 0.97.
instance, Saikeaw et al. [93] fabricated intelligent films using the The value of a* (redness) as a function of storage time is presented in
layer-by-layer deposition of Poly(diallyldimethylammonium chloride) Fig. 3. It can be observed that a* value of LISG/curcumin film increased
(PDADMAC) and poly(sodium 4-styrene sulfonate) (PSS). For this pur­ from 5.7 to 9.9 when the storage time increased to 5 days. Corre­
pose, polyelectrolyte multilayers (PEM) films were coated by dipping spondingly, the color of the films changed from yellow to red during
into a polyelectrolyte solution of PDADMAC (10 mM) and PSS layers storage period.
with NaCl (1 M) for 2 min. Then, the coated samples were immersed into The packaging system incorporated with curcumin has also been
a curcumin solution (1 g L− 1) for 2 h. Surprisingly, they observed that employed to preserve some juicy fruit like apples. Wu et al. [32]
when PDADMAC was used as the top layer, the changing color occurred developed an intelligent package based on gelatin/β-cyclodex­
at pH 7.5, while when using PSS as the top layer, the change was trin/curcumin to protect apple juice against deteriorative conditions.
detected at pH 9.5. Therefore, to detecting seafood spoilage in the first The apple juice’s total phenol content and color attribute were evaluated

Fig. 3. TVBN values of shrimp samples and the sensor response at ambient (A) and chiller (B) conditions [77].

10
N. Aliabbasi et al. Journal of Environmental Chemical Engineering 9 (2021) 105520

over the storage period (0, 12, and 24 h). It was observed that the film concentration and packaging materials, and thus these factors should
incorporated with curcumin could preserve apple juice against brown­ take into account in designing this type of intelligent packaging system.
ing. Furthermore, the authors reported that the films containing cur­ Further investigations should be conducted to improve the pH-
cumin could effectively protect polyphenols against oxidation. sensitivity of curcumin-loaded films. More evaluations are required to
Surprisingly, the film containing 2.5 mg curcumin was more effective confirm the safety and possible side effects of curcumin-loaded pack­
than containing 5 mg to protect polyphenols. The reason for that has aging systems before their application in the industrial scale.
been associated with the more compact structure of the films at lower
curcumin concentrations, making the films a better barrier against ox­ Authors’ contribution
ygen [32]. As a suggestion for a future study, microbiological stability
and safety of apple juice packed by gelatin/β-cyclodextrin/curcumin Authors N. Aliabbasi and M. Fathi critically reviewed previous data
should be considered. and prepared the first draft of the paper. Author Z. Emam-Djomeh
Wang et al. [94] coated tofu, bread, and cooked pork using a participated in the study design and critically reviewed the manuscript
dispersion containing curcumin microencapsulated by gelatin/porous draft.
starch. It was found that when the curcumin concentration was higher
than 0.035%, the quality of the tested foods was preserved over the Conflict of Interest
storage period (72 h). High temperatures can lead to degradation of
heat-sensitive ingredients like curcumin. Wang et al. [94] tested the Authors declare that they are free of any conflicts of interest.
encapsulated curcumin’s heating stability by cooking coated tofu, bread,
and cooked pork. Interestingly, the authors observed that there was still References
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