Innovative Food Science and Emerging Technologies 19 (2013) 173–180

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Innovative Food Science and Emerging Technologies

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

Effectiveness of a novel insect-repellent food packaging incorporating essential oils

against the red flour beetle (Tribolium castaneum)
F. Licciardello a, G. Muratore a, P. Suma b, A. Russo b, C. Nerín c,⁎
a
Department of Agricultural and Food Productions (DiSPA), University of Catania, via Santa Sofia 98, Catania 95123, Italy
b
Department of Agri-food and Environmental Systems Management (DiGESA), University of Catania, via Santa Sofia 100, Catania 95123, Italy
c
Department of Analytical Chemistry I3A, GUIA group, EINA, University of Zaragoza, Campus Rio Ebro, María de Luna 3, Zaragoza 50018, Spain

a r t i c l e i n f o a b s t r a c t

Article history: Packaging represents a critical step in the food quality preservation and the ultimate defence against insect
Received 19 July 2012 pests. Cereal-based foods may be infested by insects even during their packed life, i.e. during distribution,
Accepted 5 May 2013 transportation and storage in warehouses or in retail stores. Many studies in the last years have concerned
the development of active packaging with antioxidant and antimicrobial action, but very few studies have
Editor Proof Receive Date 06 June 2013
addressed insect-repellent packaging materials for foods. This work aimed at assessing the repellent efficacy
Keywords:
of novel functional packaging materials containing three essential oils: citronella, oregano and rosemary. Re-
Active packaging pellent films were chemically characterized by MHS-SPME-GC-MS. The results obtained from area tests run
Essential oils in Petri dishes indicated that essential oils at concentrations higher than 0.005 μL/cm2 showed potential in
Insects repellents terms of repellent activities against the red flour beetle, Tribolium castaneum. Assays performed with coated
Repellent packaging packages containing wheat semolina showed repellency results ranging from 53 to 87% for citronella and
Tribolium castaneum rosemary, respectively.
Industrial Relevance: The paper deals with the study carried out of several Essential Oils as repellent for in-
sects in packaged food. Rejection of packaged food caused by insect pests is a great problem that affects
the industry worldwide. Without any doubt the prevention of insect attack from the packaging material
without affecting the packaged product is an environmentally friendly and economical advantage. The indus-
try is demanding this type of solutions.
© 2013 Elsevier Ltd. All rights reserved.

1. Introduction worldwide distributed in various climatic conditions (Robertson,

Insect infestations are the main cause of loss of packed foodstuffs
both in terms of direct damages or cost to preserve and package
food (Hanlon, Kelsey, & Forcinio, 1998). The issue of sustainment of
the world population is generally considered in terms of the need to
increase food productions. However measures such as the safeguard
of stored foods from insect contamination could represent a solution
for increasing food products availability.
Cereal-based dry foods such as pasta, flour, cakes, rice and others
may be subject to insect infestations. The attack to packaged foods
can occur during the production phases or in the following steps of
the distribution, such as transportation and storage in warehouses
or in retail stores. In any case, consumers frequently blame the man-
ufacturers for any occurring insect contamination, independently
from their real involvement, and the consequences on the image of
the company can be severe (Hou, Field, & Taylor, 2004).
The most destructive insect pests of stored products are included in
the orders of Coleoptera (beetles) and Lepidoptera (moths), which are
⁎ Corresponding author. Tel.: +34 976 761873; fax: +34 976 762388.
E-mail address: cnerin@unizar.es (C. Nerín).
2006). The search for tools to prevent infestations is crucial and current
solutions involve the spraying of insecticides such as pyrethins and py-
rethroids (e.g. resmethrin, sumithrin, tetramethrin, permethrin) in the
environment where dry food is processed and packaged, after removing
all food and utensils for food contact. Stored products safeguard has
long relied on the employment of synthetic insecticidal molecules
such as methyl bromide (MB) and phosphine as fumigants but whose
use has been restricted lately due to adverse effects on the environment
(e.g. ozone depletion caused by MB) and to pest resistance develop-
ment of certain species with reiterated phosphine treatments (Shaaya,
Kostjukovsky, Eilberg, & Sukprakarn, 1997).
The theme of the interaction between insect pests and packaged
foods has been handled by several authors, who pointed out on the abil-
ity of insects to penetrate into packages (Essig, Hoskins, Linsley,
Michelbacher, & Smith, 1943; Gerhardt & Lindgren, 1954; Gerhardt &
Lindgren, 1955; Batth, 1970; Cline, 1978; Langbridge, 1970) and on
the resistance of various packaging materials to insect attacks
(Dominichini & Forti, 1975; Licciardello, Cocuzza, Russo, & Muratore,
2010; Sreenathan, Iyengar, Narasimhan, & Majumder, 1960).
Being consolidated that packaging represents a critical point in the
food quality preservation and the ultimate defence against insect

1466-8564/$ – see front matter © 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.ifset.2013.05.002
174 F. Licciardello et al. / Innovative Food Science and Emerging Technologies 19 (2013) 173–180
pests, efforts should be paid not only towards the design of effective
systems which may retard the food quality decay, but also for the
development of insect-proof packages, able to resist to insects pene-
tration and/or to repel their presence from the food packages
environment.
During the last 10 years, new technologies for food packaging have
emerged and among them “active packaging” is one of the most prom-
ising innovation. It consists of incorporating into the packaging material
active compounds useful for the food protection in terms of antioxidant
and/or antimicrobial effect. Several papers have been published dealing
with different proposals of active packaging (Goñi et al., 2009;
Gutiérrez, Escudero, Batlle, & Nerín, 2009; Gutiérrez, Sánchez, Batlle,
López, & Nerín, 2009; López, Sánchez, Batlle, & Nerín, 2007a, 2007b;
Rodríguez, Batlle, & Nerín, 2007, 2008) but only a few commercial solu-
tions are available. Few papers in literature have dealt with the develop-
ment of insect-repellent packaging systems. Highland & Merritt, 1973;
Highland, Simonaitis, & Boatright, 1984; Highland & Cline, 1986) pub-
lished the first attempts to reduce insects infestations by the use of
repellent-treated packaging materials. More recently, Hou et al. (Hou
et al., 2004) proposed the use of DEET and Neem contained in paper,
Wong et al. (Wong, Signal, Campion, & Motion, 2005) addressed the
use of citronella essential oil in a coating for carton packages, whereas
Germinara et al. (Germinara, Conte, Lecce, Di Palma, & Del Nobile,
2010) embedded propionic acid into corn zein and policaprolactone.
Apart from the mentioned papers, an in-depth survey only gave back
a chapter on a book dedicated to active packaging (Navarro, Zehavi,
Angel, & Finkelman, 2007) another chapter focused on essential oils in
active packaging (Nerín, 2012) and a few US patents concerning the de-
velopment of slow-release repellent systems (Calton, Siemer, & Wood,
2001; Domb, 1993; Tucci & Dry, 2000) while two patents are known
to describe the incorporation of insect repellents into paper-based
packaging (Radwan & Allin, 1997; Whalon & Malloy, 1998). The use of
natural plant extracts in this application could facilitate acceptance by
food regulators as well as the general public.
The aim of the present work was to evaluate the repellent efficacy
of citronella, oregano and rosemary essential oils against one of the
most common stored food pests, Tribolium castaneum (Herbst) (Cole-
optera, Tenebrionidae), and to assess the effectiveness of a novel
functional active plastic material with repellent action containing
the three essential oils.
2. Materials and methods
2.1. Essential oils and repellent films
Citronella (Cymbopogon nardus), oregano (Origanum vulgare) and
rosemary (Rosmarinus officinalis) essential oils (EO) were purchased
from Gutiérrez SAS Matières Premières Essentielles (Grasse Cedex,
France). Such oils are GRAS (Generally Recognized as Safe) according
to FDA (21CFR182.20). In the following the gross composition of test-
ed essential oils is reported:
Citronella oil. FDA: 182.20. Citronellal 35 ÷ 40%; geraniol
25 ÷ 30%; citronellol 15 ÷ 20%, D-limonene 5 ÷ 10%; linalool
0 ÷ 5%; farnesol 0 ÷ 5%
Origanum oil. Carvacrol 75 ÷ 80%; linalool 5 ÷ 10%; thymol
5 ÷ 10%; D-limonene 0 ÷ 5%
Rosemary oil. Beta pinene 10 ÷ 15%; camphor 10 ÷ 15%; camphene
5 ÷ 10%. D-Limonene 0 ÷ 5%; terpineol 0 ÷ 5%; linalool 0 ÷ 5%.
The formulations were suitably diluted for the bioassays described
hereafter.
Repellent films were prepared by Artibal (Sabiñánigo, Spain) from
corona-treated polypropylene (30 μm thickness), following a patent-
ed procedure (European Patent EP1657181). The coating included 4%
(w/w) of the above-mentioned essential oils. Each film was analysed
for the volatile composition and tested for the repellent effectiveness
in the bioassays described in the following after one-month storage in
aluminium-polyethylene hermetically sealed bags.
2.2. Insects
The unsexed adults of T. castaneum used in the experiments were
2–4 weeks post-eclosion and were obtained from laboratory cultures
maintained in incubators at 30 ± 1 °C and 70 ± 5% r.h. in the dark.
The colonies had been cultured in laboratory for over four years on
wheat flour mixed with 5% brewer's yeast.
2.3. Volatile composition of repellent films
A quantitative Multiple Headspace (MHS) SPME analysis was
performed according to the method described by Ezquerro et al.
(Ezquerro, Pons, & Tena, 2003), which is based on the multiple head-
space extraction (MHE) method developed by Kolb (1982). This meth-
od was previously applied for the study of the diffusion of volatile
compounds in plastic films (Licciardello, Del Nobile, Spagna &
Muratore, 2009; Licciardello, Muratore, Mercea, Tosa & Nerín, 2013).
MHS-SPME involves various SPME extractions of the same sample,
and the total amount of the analyte can be calculated from the sum of
the areas of the chromatograms relative to each extraction. The total
area can be easily calculated from the following equation:
X
N
A1
AT ¼ Ai ¼ ð1Þ
i−1
1−β
where: AT is the total area relative to multiple extractions, Ai is the
area of the chromatographic peak relative to the i-th SPME extrac-
tion), A1 is the area relative to the first extraction, β is a constant,
and N is the total number of extractions. The latter value can be calcu-
lated from the slope of the plot resulting from the following equation:
lnAi ¼ ði−1Þ lnβ þ lnA1 ð2Þ
The fibre used was a polydimethylsiloxane (PDMS, 100 μm,),
which gave the richest profiles for basil and rosemary essential oils
in a previous work (López, Huerga, Batlle, & Nerín, 2006). A
6.25 cm2 sample of each functional film was incubated into 20-mL
headspace vials at 80 °C for 30 min and extracted at 80 °C for
30 min. Pre-incubation and extraction temperature and times
resulted from preliminary experiments which considered incubation
and extraction temperatures ranging from 60 to 80 °C and extraction
time ranging from 15 to 35 minutes. After extraction, the fibre was
desorbed for 5 min into the GC injector set at 270 °C in splitless
mode, the temperature of the transfer line being set at 280 °C.
GC–MS analyses were performed using an Agilent (Palo Alto, CA, USA)
6890 N GC equipped with a 5975B mass detector, and a HP-5 MS
(30 m × 0.25 mm, 0.25 μm film thickness) 5% phenyl-methylsyloxane
capillary column. The temperature program was as follows: initial tem-
perature 40 °C for 2 min, raised by 10 °C/min to 300 °C and 300 °C for
2 min. The carrier gas was helium, 99.999% purity, supplied by Carburos
Metálicos (Barcelona, Spain). Samples were analyzed in a Combi-Pal
autosampler (CTC Analytics AG, Zwingen, Switzerland) coupled to the
GC-MS, which allowed analytical reproducibility and precision.
Quantification of essential oil components was carried out by ex-
ternal calibration, preparing appropriate solutions of pure standards
in the same organic coating used to encapsulate the essential oils,
and spiking virgin PP with suitable amounts (microliters) of such so-
lutions. The spiked films, having the same size as the active film sam-
ples, were analyzed as above described.
 F. Licciardello et al. / Innovative Food Science and Emerging Technologies 19 (2013) 173–180
2.4. Bioassays for the repellency of essential oils
Preference area assays (Nerio, Olivero-Verbel, & Stashenko, 2010;
Ogendo et al., 2008) were run to evaluate the repellent effect of citro-
nella, oregano and rosemary essential oils against T. castaneum, com-
monly referred to as the red flour beetle.
Filter paper disks (11 cm diameter) were cut in halves, one half was
treated with 0.5 mL of suitable dilutions of the essential oils in acetone
and the other half was impregnated with 0.5 mL of acetone alone (con-
trol). After solvent evaporation, disks were reconstituted in glass plates
(11 cm diameter) by coupling one half treated with the essential oils
and one half of control paper. Ten adults of T. castaneum were placed
in the centre of each plate. Two repellency tests were carried out at
25 °C and 70% RH with the following essential oil concentrations:
Test#1: 0.001 and 0.01 μL/cm2
Test#2: 0.005, 0.01 and 0.02 μL/cm2
For each concentration and for each essential oil, four replicates were
performed. Insects were enumerated after 0.15, 0.30, 1 and 3 h and re-
sults were expressed as percent repellency (R%), calculated as follows:
R% ¼ ðC−T Þ=ðC þ T Þ  100
where:
C number of insects in the control area;
T number of insects in the treated area
2.5. Bioassays for the effectiveness of repellent films
Sachets sized 52.5 × 74.25 mm were prepared with repellent
films, with the coated side as the outer side of packages, and filled
with 25 g durum wheat semolina.
For the preference tests, one sachet made with the control film
and one made with the treated one were positioned at the sides of
rigid polyethylene white boxes (20 × 10 × 7 cm). Twenty adults of
the red flour beetle, unfeeded for 48 hours, were then released in
the centre of the boxes, and maintained in the dark until the end of
the trial, carried out at 25 °C and 70% RH. A control trial was also
performed, consisting of two semolina sachets made with control
film aimed at excluding other factors than the essential oil on the in-
sect behaviour. Each test was carried out in triplicate.
Boxes were checked after 2, 24 and 48 h, and the percentage of re-
pellency (R%) was calculated as aforementioned, with:
C = number of insects on the control package; T = number of in-
sects on the repellent package.
2.6. Statistical analysis
All data were submitted to one-way analysis of variance (ANOVA),
and post-hoc comparison of means was performed by the Tukey test
(p b 0.05) through the statistical package SPSS® Statistics 13.0
(Armonk, NY, USA).
3. Results and discussion
3.1. Volatile composition of coated repellent films
A typical chromatogram of the PP film coated with citronella EO
(film A) is shown in Fig. 1a. The MHS-SPME analysis was able to
quantify 6 major compounds, as shown in Table 1: citronellol, gerani-
ol and their acetates, together with citronellal and eugenol represent
almost 50% of the total chromatographic area. Among the major com-
pounds, elemol and δ-cadinene were not quantified as a commercial
175
standard was not available, while myrcene and trans-β-ocimene did
not follow the linear relationship ln Ai versus i-1.
A typical chromatogram of B-type film B (PP coated with oregano
EO) is shown in Fig. 1b. The MHS-SPME analysis revealed the quanti-
tative composition of linalool, thymol, carvacrol and β-caryophyllene
(Table 1), which represent more than 60% of the total chromato-
graphic area, carvacrol being the major compound characterizing
this EO, as shows Table 1.
A typical chromatogram of film C (PP coated with rosemary EO) is
shown in Fig. 1c. The MHS-SPME analysis could quantify 5 major
compounds (Table 1), which represent almost 40% of the total chro-
matographic area. Among the major compounds, camphor could not
be quantified by the MHS-SPME technique, as it did not follow the lin-
ear relationship ln Ai vs i-1.
3.2. Repellency of essential oils
Preliminary bioassays of the repellent effect of diluted EOs by the
area preference tests (Fig. 2) were carried out as a screening for the ef-
fectiveness of natural substances to be incorporated in functional repel-
lent packaging and for comparative purposes: this method is the most
widely used for the assessment of the repellency of natural substances.
Test#1 (Fig. 3a–c) performed with two EO concentration (0.01 e
0.001 μL/cm2) showed a dose–response effect, with special regards for
citronella. For this oil, the repellency value reached 90 and 100% after
30 min-1 h in the trial performed with the highest concentration, and
values below 50% in the trials at 0.001 μL/cm2. Citronella EO showed
in the first hour of the test significantly higher repellency (p b 0.05)
compared to the other EOs. It has to be noted that the repellency values
decreased after 3 h, and this might be attributed to the loss of the essen-
tial oils from the filter paper by evaporation. Rosemary essential oil also
showed a concentration effect (p b 0.05), however at the lowest dilu-
tion this oil seemed to exert an attractive action, especially at the latest
time intervals, as evidenced by the negative R% values.
Test#2 (Fig. 4a–c) was performed with three EO concentration
(0.005, 0.01 and 0.02 μL/cm2); this test confirmed the effect of concen-
tration on the insect response. As for Test#1, repellency decreased after
3 h, possibly due to the essential oil evaporation from filter paper.
All of the tested essential oils at concentrations 0.005–0.02 μL/cm2
were effective at repelling T. castaneum in preference area tests, while
a lower concentration (0.001 μL/cm2) was not satisfactorily effective
or, in the case of rosemary, it showed an attractive effect.
The evaporation of the EOs from the paper support was expected
due to the fact that such volatiles compounds are not bound but
only absorbed on paper. Also, this is one of the main reasons why a
special formula is needed to incorporate EOs in packaging material,
either in plastic or in paper and board. Thus, the resulting active ma-
terials would act as reservoir of EO and the controlled kinetics of re-
lease is the key point for proposing them as commercial active
materials with repellent properties versus insects.
3.3. Effectiveness of the repellent films against the red flour beetle
Two hours after the start of the trials, most of the insects were found
grouped close to the sachets made with the control film, while only 2 to 5
insects out of 20 were found on the treated sachet. Fig. 5 shows the per-
cent repellency after 2, 24 and 48 h of semolina packages made with
films containing the tested essential oils. Values did not change signifi-
cantly through the duration of the assays for oregano and citronella,
while data referred to rosemary essential oil are slightly higher after 24
and 48 h. Repellency data for the control sachets were always signifi-
cantly different (p b 0.05) from those referring to the coated sachets
and, among test materials, no significant difference (p b 0.05) was ob-
served. Insects tended to locate behind the sachets (this is a typical be-
havioural aspect of the Tenebrionidae family) and in correspondence
with the seal, which are known to be the most vulnerable points of
176 F. Licciardello et al. / Innovative Food Science and Emerging Technologies 19 (2013) 173–180
 F. Licciardello et al. / Innovative Food Science and Emerging Technologies 19 (2013) 173–180 177

Table 1
Quantitative composition, by MHS-SPME-GC-MS, of coated
PP films (film A = citronella EO, 4% w/w; film B = oregano
EO, 4% w/w; film C = rosemary, 4% w/w).

μg/cm2

Film A
Citronellal 134.22
Citronellol 40.78
Geraniol 94.90
Citronellyl acetate 12.74
Eugenol 6.00
Geranyl acetate 15.44
Film B
Linalool 8.88
Thymol 10.65
Carvacrol 174.26
β-caryophyllene 95.58
Film C
1,8 cineole 211.04
Linalool 5.21
α-terpineol 32.29
Carvacrol 3.28
β-caryophyllene 318.92

packages. Insects remained substantially in the same place chosen dur-

ing the first 2 hours throughout the duration of the trials. No attempt
to pierce packages was observed during the tests, however it is possible
that a longer starvation of insects could determine an increased aggres-
siveness towards packages.
Repellency data relative to the control trials were close to zero, as
insects placed themselves randomly and choose one or another pack-
age indifferently. The fact that the histograms for the control are neg- Fig. 2. Detail of a plate during the preference test for the evaluation of repellency. In
ative should be taken as a merely casual result. this case, all of the ten insects are found on the control half and as far a possible
The observed repellency of essential oils in the tests performed on from the essential oil.

filter paper and with treated packages can be attributed to the essen-
tial oils components. It has been demonstrated that terpenoids pos-
sess biological activity against several post-harvest Coleoptera
(Weaver, Dunkel, Ntezurubaza, Jackson, & Stock, 1991). In particular,
citronellol and trans-geraniol, which are key components of the citro-
nella EO, were found to have strong repellent effect on T. castaneum
(Zhang et al., 2011). Also, linalool, which is present in all of the tested
EOs, has been demonstrated to effectively repel T. castaneum in repel-
lency tests carried out in olfactometers (Ukeh & Umoetok, 2011). An-
other study assessed the potential of 1,8 cineole, one of the most
representative terpenoid in rosemary EO, against T. castaneum (Lee,
Annis, Tumaalii, & Choi, 2004). An interesting research by Bekele
and Hassanali (2001) demonstrated that single components of essen-
tial oils do not show comparable toxicity to the EO towards two
stored food insects, but their combinations do provide bioactivity:
the mixtures allowed to select 1,8 cineole, limonene and camphor
among the most powerful components.
Compared to the repellency data obtained in the preliminary bio-
assays conducted with essential oils on filter paper, where the effica-
cy decreased drastically after 3 hours from the beginning of the
experiments, coated films showed a durable efficacy, ranging around
60% for citronella- and oregano-based repellent packaging, and 87%
for the rosemary-based coated film. The retention of effectiveness is
due to the bonding of essential oil to the packaging film by the coating
matrix which, while immobilizing the essential oil preventing its loss
by evaporation, it guarantees a controlled release able to effectively
repel insects. As previous studies demonstrated this coated polymers
are stable for at more than 4 months and in some cases the activity
remains even for more than one year (Nerín, 2012). Further studies
should address the shelf life of repellent packaging by the release ki-
netics: indeed it is required that the effectiveness of such systems is at
least as long as the product shelf life.
Finally, some studies (Huang, Lam, & Ho, 2000; Huang, Tan, Kini, &
Ho, 1997; Rozman, Kalinovic, & Korunic, 2007) demonstrated that T.
castaneum is less sensitive to some essential oils compared to
Sitophilus spp., another frequent stored food pest. Therefore, our
promising results obtained with T. castaneum let hypothesize an
even stronger efficacy of the essential oils object of this research
and of the repellent packaging films on other pest species.
4. Conclusion
Repellency for coated films ranging from 53 to 87% is to be considered
a very promising result and encourage the study and application of repel-
lent packaging materials for the safeguard of packaged foods and the
reduction of packaged food losses due to insect attacks. Data obtained
from the bioessays on filter paper supplied tentative information on
T. castaneum response to citronella, oregano and rosemary essential oils,
which were completed by the results coming from the tests run with
coated films. The development of insect-repellent packaging should
take into account that high doses might be required, with possible effects
on the sensory quality of the produce, hence it is necessary to orient the
diffusion of active components towards the outside of packages. This

Fig. 1. a–c. Typical chromatograms relative to the MHS-SPME analysis of the coated PP film. (a): film A (citronella EO). 1) Myrcene; 2) α-Pinene; 3) trans-β-Ocimene; 4) Linalool;
5) allo-Ocimene; 6) Citronellal; 7) Isopulegol; 8) Citronellol; 9) Geraniol; 10) Geranial; 11) Thymol; 12) Carvacrol; 13) Citronellyl acetate; 14) Nerol; 15) Eugenol; 16) Geranyl acetate;
17) β-Elemene; 18) δ-Cadinene; 19) Elemol; 20) γ-Eudesmol; 21) t-Cadinol; 22) α-Eudesmol; 23) Germacrene; 24) trans-β-Farnesene; 25) α-Cubebene; 26) cis-α-Bisabolene;
27) β-Cubebene; 28) α-Amorphene; 29) β-Cadinene; 30) 1S,cis-Calamenene; 31) α-Cadinene. (b): film B (oregano EO). 1) Limonene; 2) Camphor; 3) endo-Borneol; 4) α-Terpineol;
5) Thymol; 6) Carvacrol; 7) Camphene; 8) Eugenol 9) β-Caryophyllene; 10) α-Humulene; 11) δ-Cadinene; 12) Caryophyllene oxide; 13) t-Cadinol. (c) film C (rosemary EO).
1) 1,8-Cineole; 2) Linalool; 3) Camphor; 4) Endo-borneol; 5) α-Terpineol; 6) Bornyl acetate; 7) Thymol; 8) Carvacrol; 9) α-Cubebene; 10) α-Ylangene; 11) α-Copaene;
12) Isocaryophyllene; 13) β-Caryophyllene; 14) Aromadendrene; 15) α-Humulene; 16) α-Amorphene; 17) δ-Cadinene; and 18) 1S,cis-Calamenene.
178 F. Licciardello et al. / Innovative Food Science and Emerging Technologies 19 (2013) 173–180

15 min 30 min 60 min 180 min

100

80

60

40
Repellency %

20

-20

-40

-60

-80
0.001 0.01 0.001 0.01 0.001 0.01
Citronella Oregano Rosemary

µL/cm2

Fig. 3. Repellent effect, as repellency %, of citronella (a), oregano (b) and rosemary (c) essential oils, Test#1.

100 15 min 30 min 60 min 180 min

80

60
Repellency %

40

20

-20
0.005 0.01 0.02 0.005 0.01 0.02 0.005 0.01 0.021

Citronella Oregano Rosemary

µL/cm2
Fig. 4. Repellent effect, as repellency %, of citronella (a), oregano (b) and rosemary (c) essential oils, Test#2.
 F. Licciardello et al. / Innovative Food Science and Emerging Technologies 19 (2013) 173–180
Citronella
100.00
80.00
60.00
% repellency
40.00
20.00
0.00
2 24
-20.00
-40.00
Fig. 5. Repellency of semolina packages made with coated PP films, compared with packages realized with control PP, against Tribolium castaneum, in a preference test carried out
with 20 adult insects.
could be attained by coupling active films, as outer layers, with materials
having barrier properties to volatiles, as inner layers. Moreover, the
breakdown of active components in the repellent films might occur, re-
ducing their effectiveness with time, and innovative techniques of
immobilisation (nanocomposite materials, microencapsulation, use of
beta-cyclodextrins) could extend effectiveness for several years. Finally,
it should be taken into consideration that repellent packages would re-
duce the incidence of exogenous infestations and can only be synergistic
with hygienic prevention measures, since they have no effect on insects
already present in the packaged produce at any life stage. The widespread
of repellent packaging is currently limited by the lack of scientific studies,
therefore this work should encourage further investigation considering
active substances, doses, modes of application and target insects. The
adoption of repellent packaging could reduce the recourse to thick pack-
aging films, which ensure a certain level of prevention against insects at-
tacks to packages, and help fight overpackaging (i.e. the use of higher
volumes of plastic than strictly necessary). The potential of essential oils
could be the answer to the current search for environmental and
health-friendly solutions for the safeguard of foods. If packaging is the
last frontier against insect pests, then repellent packaging might repre-
sent the ultimate weapon for producers and consumers against pests at-
tacks to packages.
Acknowledgement
The authors acknowledge the company Artibal for supplying the
active polymers. Thanks are given to Gobierno de Aragon and Fondo
Social Europeo for the financial help through the GUIA group T-10
References
Batth, S. S. (1970). Insect penetration of aluminium-foil packages. Journal of Economic
Entomology, 63, 653–655.
Bekele, A. J., & Hassanali, A. (2001). Blend effects in the toxicity of the essential oil con-
stituents of Ocimum kilmandscharicum and Ocimum kenyense (Labiateae) on two
Post-harvest insect pests. Phytochemistry, 57, 385–391.
Calton, G. J., Siemer, S. R., & Wood, L. L. (2001). Slow release insect repellents. U.S. Patent
6,180,127.
Cline, L. D. (1978). Penetration of seven common flexible packaging materials by larvae
and adults of eleven species of stored product insects. Journal of Economic Entomology,
71, 726–729.
Domb, A. J. (1993). Sustained release formulations of insect repellent. U.S. Patent
5,221,535.
Dominichini, G., & Forti, D. (1975). Research on packaging materials resistant to the at-
tacks of insects. Presented at 1st Symposium on Control of parasites in the food indus-
try and food protection. Piacenza, Italy, 1972.
179
Oregano Rosemary Control
48
time (h)
Essig, E. O., Hoskins, W. M., Linsley, E. G., Michelbacher, A. E., & Smith, R. F. (1943). A
report on the penetration of packaging materials by insects. Journal of Economic En-
tomology, 36, 822–826.
European Patent EP1657181. Antimicrobial packaging based on the use of natural ex-
tracts and the process to obtain this packaging.
Ezquerro, O., Pons, B., & Tena, M. T. (2003). Multiple headspace solid-phase microextraction
for the quantitative determination of volatile organic compounds in multilayer packag-
ings. Journal of Chromatography. A, 999, 155–164.
FDA. U.S. Food and Drug Administration. Code of Federal Regulations, Title 21, Volume
3, Revised as of April 1, 2012, Sec. 182.20.
Gerhardt, P. D., & Lindgren, D. L. (1954). Penetration of various packaging films by com-
mon stored-product insects. Journal of Economic Entomology, 47, 282–287.
Gerhardt, P. D., & Lindgren, D. L. (1955). Penetration of additional packaging films by
common stored-product insects. Journal of Economic Entomology, 48, 108–109.
Germinara, G. S., Conte, A., Lecce, L., Di Palma, A., & Del Nobile, M. A. (2010). Propionic
acid in bio-based packaging to prevent Sitophilus granarius (L.) (Coleoptera,
Dryophthoridae) infestation in cereal products. Innovative Food Science and Emerg-
ing Technologies, 11(3), 498–502.
Goñi, P., López, P., Sánchez, C., Gómez-Lus, R., Becerril, R., & Nerín, C. (2009). Antimicro-
bial activity in the vapour phase of a combination of cinnamon and clove essential
oils. Food Chemistry, 116, 983–987.
Gutiérrez, L., Escudero, A., Batlle, R., & Nerín, C. (2009). The effect of mixed antimicro-
bial agents and flavours in active packaging films. Journal of Agricultural and Food
Chemistry, 57, 8564–8571.
Gutiérrez, L., Sánchez, C., Batlle, R., López, P., & Nerín, C. (2009). New antimicrobial
active package for bakery products. Trends in Food Science and Technology, 20(2),
92–99.
Hanlon, J. F., Kelsey, R. J., & Forcinio, H. E. (1998). Handbook of package engineering.
EEUU: CRC Press.
Highland, H. A., & Cline, L. D. (1986). Resistance to insect penetration of food pouches
made of untreated polyester or permethrin-treated polypropylene film. Journal of
Economic Entomology, 79, 527–529.
Highland, H. A., & Merritt, P. H. (1973). Synthetic pyrethroids as package treatments to
prevent insect penetration. Journal of Economic Entomology, 66, 540–541.
Highland, H. A., Simonaitis, R. A., & Boatright, R. (1984). Insecticide-treated film wrap
to protect small packages from infestation. Journal of Economic Entomology, 77,
1269–1274.
Hou, X., Field, P., & Taylor, W. (2004). The effect of repellents on penetration into pack-
aging by stored-product insects. Journal of Stored Products Research, 40, 47–54.
Huang, Y., Lam, S. L., & Ho, S. H. (2000). Bioactivities of essential oils from Elletaria
cardamomum (L.) to Sitophilus zeamais Motschulsky and Tribolium castaneum
(Herbst). Journal of Stored Products Research, 36, 107–117.
Huang, Y., Tan, J., Kini, R. M., & Ho, S. H. (1997). Toxic and antifeedant action of nutmeg
oil against Tribolium castaneum (Herbst) and Sitophilus zeamais Motsch. Journal of
Stored Products Research, 33, 289–298.
Kolb, B. (1982). Multiple headspace extraction — A procedure for eliminating the influ-
ence of the sample matrix in quantitative headspace gas chromatography.
Chromatographia, 15(9), 587–594.
Langbridge, D. M. (1970). Treatment of paper to protect packaged food from insect at-
tack. Appita Journal, 24, 45–51.
Lee, B. H., Annis, P. C., Tumaalii, F., & Choi, W. S. (2004). Fumigant toxicityof essential
oils from the Myrtaceae family and 1,8-cineole against 3 major stored-grain in-
sects. Journal of Stored Products Research, 40, 553–564.
Licciardello, F., Cocuzza, G. E., Russo, A., & Muratore, G. (2010). Quality maintenance
performance and resistance to Tribolium castaneum and Plodia interpunctella pene-
tration of an alternative packaging material for semolina. Italian Journal of Food Sci-
ence, 22(4), 461–466.
180 F. Licciardello et al. / Innovative Food Science and Emerging Technologies 19 (2013) 173–180
Licciardello, F., Del Nobile, M. A., Spagna, G., & Muratore, G. (2009). Scalping of
ethyloctanoate and linalool from a model wine into plastic films. LWT- Food Science
and Technology, 42, 1065–1069.
Licciardello, F., Muratore, G., Mercea, P., Tosa, V., & Nerín, C. (2013). Diffusional behaviour
of essential oil components in active packaging polypropylene films by Multiple
Head-Space-Solid Phase Microextraction-Gas Chromatography (MHS-SPME-GC-MS).
Packaging Technology and Science, 26, 173–185. http://dx.doi.org/10.1002/pts.1969.
López, P., Huerga, M. A., Batlle, R., & Nerín, C. (2006). Use of solid phase microextraction
in diffusive sampling of the atmosphere generated by different essential oils.
Analytica Chimica Acta, 559, 97–104.
López, P., Sánchez, C., Batlle, R., & Nerín, C. (2007a). Development of flexible antimicro-
bial films using essential oils as active agents. Journal of Agricultural and Food
Chemistry, 55(21), 8814–8824.
López, P., Sánchez, C., Batlle, R., & Nerín, C. (2007b). Vapor-phase activities of cinna-
mon, thyme and oregano essential oils and key constituents against food-borne
microorganisms. Journal of Agricultural and Food Chemistry, 55(11), 4348–4356.
Navarro, S., Zehavi, D., Angel, S., & Finkelman, S. (2007). Natural nontoxic insect repel-
lent packaging materials. Taylor and Francis. In C. L. Wilson (Ed.), Intelligent and
Active Packaging for Fruits and Vegetables (pp. 336). New York, USA: CRC Press.
Nerín, C. (2012). Essential Oils In Active Packaging. Chapter 17 in the book “Essential Oils
as Natural Food Additives: Composition, Applications, Antioxidant and Antimicrobial
Properties. In Luca Valgimigli (Ed.), : Nova Science Inc9781621002413.
Nerio, L. S., Olivero-Verbel, J., & Stashenko, E. E. (2010). Repellent activity of essential
oils: A review. Bioresource Technology, 101, 372–378.
Ogendo, J. O., Kostyukovsky, M., Ravid, U., Matasyoh, J. C., Deng, A. L., Omolo, E. O., et al.
(2008). Bioactivity of Ocimum gratissimum L. oil and two constituents against five insect
pests attacking stored food products. Journal of Stored Products Research, 44, 328–334.
Radwan, M. N., & Allin, G. P. (1997). Controlled-release insect repellent device. U.S. Pat-
ent 5,688,509.
Robertson, G. L. (2006). Food packaging: Principles and practice. Taylor and Francis
Group, Boca Raton, FL, USA: CRC Press.
Rodríguez, A., Batlle, R., & Nerín, C. (2008). The use of cinnamon-based active paper
packaging against Rhizopus stolonifer food spoilage. Journal of Agricultural and
Food Chemistry, 56, 6364–6369.
Rodríguez, A., Battle, R., & Nerín, C. (2007). The use of natural essential oils as antimi-
crobial solutions in paper packaging. Part II. Progress in Organic Coatings, 60, 33–38.
Rozman, V., Kalinovic, I., & Korunic, Z. (2007). Toxicity of naturally occurring com-
pounds of Lamiaceae and Lauraceae to three stored-product insects. Journal of
Stored Products Research, 43, 349–355.
Shaaya, E., Kostjukovsky, M., Eilberg, J., & Sukprakarn, C. (1997). Plant oils as fumigants
and contact insecticides for control of stored-product insects. Journal of Stored
Products Research, 33, 7–15.
Sreenathan, V. R., Iyengar, N. V. R., Narasimhan, K. S., & Majumder, S. K. (1960). Studies
on insect resistance of packaging materials-cellulose and polyethylene films. Food
Science, 9, 199–202.
Tucci, R. J., & Dry, N. M. (2000). Slow-release insect-repellent compositions and uses.
U.S. Patent 6,015,570.
Ukeh, D. A., & Umoetok, S. B. A. (2011). Repellent effects of five monoterpenoid odours
against Tribolium castaneum (Herbst) and Rhyzopertha dominica (F.) in Calabar,
Nigeria. Crop Protection, 30, 1351–1355.
Weaver, D. K., Dunkel, F. V., Ntezurubaza, L., Jackson, L. L., & Stock, D. T. (1991). The
efficacv of linalool, a maior component of freshly milled Ocimum canum Sims
(Lamiaceae) for protection against post-harvest damage by certain stored product
Coleoptera. Journal of Stored Products Research, 27, 213–220.
Whalon, M. E., & Malloy, G. E. (1998). Insect repellent coatings. U.S. Patent 5,843,215.
Wong, K. K. Y., Signal, F. A., Campion, S. H., & Motion, R. L. (2005). Citronella as an insect
repellent in food packaging. Journal of Agricultural and Food Chemistry, 53,
4633–4636.
Zhang, J. S., Zhao, N. N., Liu, Q. Z., Liu, Z. L., Du, S. S., Zhou, L., et al. (2011). Repellent con-
stituents of essential oil of Cymbopogon distans aerial parts against two
stored-product insects. Journal of Agricultural and Food Chemistry, 59(18), 9910–9915.