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Trends in Food Science & Technology 93 (2019) 145–157

Contents lists available at ScienceDirect

Trends in Food Science & Technology


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

Review

Intelligent packaging: Trends and applications in food systems T


S. Kalpana, S.R. Priyadarshini, M. Maria Leena, J.A. Moses, C. Anandharamakrishnan ∗

Computational Modeling and Nanoscale Processing Unit, Indian Institute of Food Processing Technology (IIFPT), Ministry of Food Processing Industries, Government of
India, Pudukkottai road, Thanjavur, 613005, India

ARTICLE INFO ABSTRACT

Keywords: Background: In recent years, research on food packaging is gaining momentum, primarily being driven by
Food packaging consumer preferences to food quality and food safety. Also, as food packaging plays a pivotal role in product
Intelligent packaging selection at retail outlets, the interest on developing novel strategies in food packaging is on the rise. One such
Indicators concept with huge potential in the food industry is intelligent packaging.
Sensors
Scope and approach: The focus of this work is to provide an up-to-date information on intelligent tools such as
Radio frequency identification
indicators (thermal indicators, leak indicators, freshness indicators, pH indicators), sensors, radio frequency
Food quality
Smart packaging identification tags and other essential aspects of intelligent packaging systems as reported in literature and those
that have gained commercial value for applications in the food supply chain.
Key findings and conclusions: Emphasizing the potential of intelligent packaging, a range of products, including
muscle-based foods, and fruits and vegetables are discussed. Importantly, this work highlights research needs,
particularly in terms of applications for liquid foods, which are the most perishable commodities.

1. Introduction could otherwise have deteriorative effects on product quality. It also


serves as a preventive tool to ensure that the product is sealed at all
‘Packaging’ is an art, science, and technology, aiming to ensure stages of distribution until it is opened by the end user, ensuring zero
quality, wholesomeness, integrity and safety of a product. It is a co- spillage and checking issues associated with tampering. Importantly,
ordinated system of preparing goods for transport, distribution, storage, food packaging serves as an identification and communication tool
retailing and subsequent end-use. It also serves as a means to ensure between the producer and consumer, presenting details of the product
safe delivery of products to a consumer also including a techno-com- such as nutritional facts, health benefits, direction to use and store,
mercial function aimed to optimize delivery costs whilst maximizing place of manufacture, manufacture date, expiry date/best before date
sales (Coles & Kirwan, 2011; Pal, Devrani, & Hadush, 2019). and other relevant information. Further, an appropriate packaging is a
From the beginning of the era of globalization and urbanization, marketing tool which directly links with an appeal for different classes
consumer preference for safe and high quality foods is on the rise. Food, of consumers who vary with age, gender, culture, and other factors. The
once packaged properly, depending on its composition and a range of packaging is also an optimization tool that helps in the purchase of a
extrinsic factors, can last from few hours to days and even months desired quantity of produce and indirectly helps in waste reduction
depending on its shelf-life. There are chances for a food product to (Biji, Ravishankar, Mohan, & Srinivasa Gopal, 2015; Marsh & Bugusu,
come in contact with physical, chemical and biological agents during 2007; Sohail, Sun, & Zhu, 2018).
handling, preparation or transportation. Packaging facilitates food It is well-known that food packaging mainly focuses on product
products to retain its goodness and freshness. It further avoids the scope safety. But, if the packaging itself is not reliable, food safety becomes a
of contamination that can arise when kept in contact with other food matter of concern. Packaging systems preserve the quality of the pro-
products or material parts at any point of the food supply chain. Thus, duct for extended durations, also contributing to waste reduction.
today's market demands a range of requirements and specifications for Predominant factors that decide the quality, safety and shelf-life of food
food packaging and labeling. products include: temperature, oxygen concentration, carbon dioxide
Food packaging is indispensable component of the food supply concentration, relative humidity and moisture content (Abreu, Cruz, &
chain as it serves as the protection or barrier layer from contamination, Losada, 2012), apart from product attributes. Hence, there is a need for
external environment and mechanical damage during transport, which real-time monitoring of various attributes of a food product that are


Corresponding author.
E-mail address: anandharamakrishnan@iifpt.edu.in (C. Anandharamakrishnan).

https://doi.org/10.1016/j.tifs.2019.09.008
Received 16 October 2018; Received in revised form 8 July 2019; Accepted 8 September 2019
Available online 13 September 2019
0924-2244/ © 2019 Elsevier Ltd. All rights reserved.
S. Kalpana, et al. Trends in Food Science & Technology 93 (2019) 145–157

known to impact food quality, organoleptic properties, and overall food microbial contaminations and adulterations are tested during produc-
safety. Innovative packaging continues to drive the growth of the tion and processing, lack of technologies to monitor food safety in
packaging industry and has led to meet the development of various distribution contribute to major food losses. Intelligent packaging can
novel packaging techniques and advanced inter-disciplinary applica- overcome this concern as it can help in monitoring the status and
tions. quality of a product directly from the package, in-turn helping in re-
Among various emerging approaches, intelligent packaging in- ducing the food wastage and spoilage (Müller & Schmid, 2019). How-
tegrates an intelligent function (communication) with conventional ever, materials used for intelligent packaging including indicators and
packaging systems. It provides information to a consumer based on the legislative constraints may increase the cost of the package, challenging
ability to sense, detect, or record external or internal changes in the cost-benefit analysis. There are also issues when test models get
product (Vaikousi, Biliaderis, & Koutsoumanis, 2008). Packaging aims transformed to commercial packaging applications, particularly in
to protect food quality, but it is not appreciable when it has a negative terms of performance efficiencies of the materials used (Dainelli,
impact on natural resources, waste disposal and on other pressing Gontard, Spyropoulos, den Beuken, & Tobback, 2008).
problems of the present era. This work highlights the essential and key It is a matter of food safety concern when intelligent packaging
concepts of intelligent packaging and techniques involved to attain materials come in direct contact with the food. This also raises issue of
economically viable and feasible intelligent packaging systems. The particle migration into the food material, challenging its commercial
need and commercial scope of various intelligent packaging systems for utilization. The European Food Safety Agency (EFSA) had explained
a range of food products as described in recently published works have aspects on safety concerns associated with intelligent and active
been reviewed and summarized. This work aims to be an up-to-date packaging (Restuccia et al., 2010). In an interesting study conducted to
status report on the science of intelligent packaging for academicians, overcome the problem of dye migration into foods having high water
researchers, and manufacturers. With emerging global interests in this contents, bromothymol blue-tetrabutylammonium ion pair dye was
field, such knowledge database envisages projecting research needs and incorporated into a multilayered packaging material as a CO2 sensor in
bottlenecks in the commercial adoption of such approaches. kimchi packages (Lyu et al., 2019).
Similarly, technological advancements in nanotechnology show
2. Definitions proven potential in combating cost-benefit challenges (Fuertes et al.,
2016). For example, nanomaterials could be designed in such a way
The concept of intelligent packaging has been a topic of interest in that they allow enhanced mechanical and barrier properties, and cost
the food packaging sector, intending to improve food quality and value reduction through the production of lightweight materials (Wyser et al.,
by performing one or more intelligent functions such as monitoring 2016). In a recent study, gold nanoparticles immobilized on a glass
quality/safety of the product in its environment, tracing product surface showed prolonged antioxidant property, highlighting its ap-
movement across the supply chain, and sensing and recording relevant plicability in intelligent packaging (Beurton et al., 2019). Further, food
product information (Yam, Takhistov, & Miltz, 2005). safety and food authenticity can be ensured by adopting nano barcode
Several researchers have defined the concept in different ways, technology in which batch information is encrypted into the packaging
considering underlying concepts and applications. In general, in- material so that batch owners can check the supply chain without the
telligent packaging is defined as a system which can make decisions to need to share company information to distributors (Neethirajan & S
increase the shelf life, notify information, improve quality and report Jayas, 2011; Smolander & Chaudhry, 2010).
harms/spoilage by utilization of various intelligent techniques (Yam
et al., 2005). An associate terminology is smart packaging, as it utilizes 3. Indicators
smart devices/data carriers such as barcodes and Radio Frequency
Identification Tags (RFID) which give detailed information about a An indicator is a devices that conveys information to a consumer
product to the consumer. Jang & Won, 2014 defined intelligent regarding microbial activity, food quality, and/or other properties. It
packaging as “the packaging system that senses, communicates and works based on specific characteristics like the presence or absence of a
monitors the conditions of packaged food to give information about target chemical or biological substance, the extent of reaction(s) be-
food quality, safety and the history of a product during transport and tween two or more substances, or the difference in concentration of
storage”. This explains the six-fold functions of intelligent packaging: chemicals present in food as evident through irreversible and visible
monitoring, detecting, sensing, recording, tracking and communicating. color change or movement of color frontiers. In the broader senses,
To achieve real-time monitoring of a product throughout the supply indicators may be categorized as external and internal indicators. The
chain various indicators, data carriers and sensors have been explored. former includes indicators which are generally placed outside the
Most indicators are intended for temperature, freshness, leakage and pH package and the latter includes indicators which are physically present
based applications; data carriers include bar codes and RFID tags. In the inside the package (Pavelková, 2013).
context of sensors for quality evaluation, gas sensors and biosensors are
the broadest application categories. 3.1. Temperature indicators

2.1. Technological gap These are the category of indicators which function based on tem-
perature changes of the product itself or the package containing the
A characteristic issue in several low-income countries is the con- product. Such indicators or integrators measure and display tempera-
siderable losses that occur during the early and mid-stages of food ture and are generally eco-friendly and cost-effective. Based on their
production (i.e., before it reaches the consumer). Though some coun- functions, they are further classified as critical temperature indicators,
tries are self-sufficient in food production, food wastage/spoilage has critical temperature/time integrators and time-temperature indicators
significant implications on the socio-economic status of these countries (Barska & Wyrwa, 2017).
(Nicoletti & Serrone, 2017). According to the Food and Agriculture
Organization (FAO, United Nations) estimation, approximately 1.3 3.1.1. Critical temperature indicators
billion tonnes of food, accounting to one-third of all food produced This type of temperature indicator indicates deterioration and
globally is wasted every year. Category wise food loss is predicted as changes in organoleptic properties of the food when exposed to ab-
20% in dairy products, 35% in seafood, 45% in fruits and vegetables, normal temperature ranges (below or above the critical temperature of
and 20% in meat; losses being predominant at processing, distribution storage) for more than a specified time interval by irreversible but
and consumption stages (FAO, SAVE FOOD initiative). Though visible changes in the color of the indicator. Accordingly, the indicator

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S. Kalpana, et al. Trends in Food Science & Technology 93 (2019) 145–157

finds its application in frozen food products as its property irreversibly TTIs. For example, poultry based products in which chicken with
changes after exceeding threshold temperatures (Taoukis & Labuza, spoilage bacteria Pseudomonas spp. were characterized using
2003). Arrhenius equation. The activation energy of spoilage bacteria with a
particular TTI was optimized (Moore & Sheldon, 2003) simulations for
3.1.2. Critical temperature/time integrators the selection of TTI was done to monitor the quality of modified
These indicators show a response above a reference critical tem- atmospheric packaged gilthead seabream fillets at various temperature
perature which can be translated in terms of equivalent exposure time conditions based on Arrhenius equation considering the activation
at that critical temperature. The quality and safety of the product can be energy. In this case, a photochemical based TTI and UV activated TTI
identified using critical temperature/time integrators (CTTIs) above the were modeled to predict spoilage using the kinetics of growth of the
critical temperature as a function of exposure time (Taoukis & Labuza, spoilage bacteria (Tsironi, Stamatiou, Giannoglou, Velliou, & Taoukis,
2003). 2011). A similar mathematical model based on square root function in
addition to the Arrhenius model was studied for three different micro-
3.1.3. Time-temperature indicators organisms considering a colorimetric-based TTI for its responses to
Time and temperature indicators (TTIs) are simple and economic- microbial spoilage. Another study by TRACEO® biological TTIs
ally feasible devices which record the temperature history of a food attempted to provide predictions on lactic acid bacterial growth using
package throughout the entire time period across packaging, storage, pH changes in the medium by providing a time-temperature correlation
distribution, and retailing (Taoukis & Labuza, 1989). Data is recorded (Ellouze et al., 2008).
in terms of irreversible changes that explain food safety and quality to
consumers. TTIs are further classified into two sub-types: full history 3.2. Freshness indicators
indicators and partial history indicators (Robertson, 2005). These in-
dicators find application majorly for temperature-sensitive foods such Freshness indicators, unlike temperature indicators, are direct in-
as chilled and frozen products (Dutra Resem Brizio, 2016). dicators of food quality, analyzing chemical reactions by target micro-
Temperature plays a vital role in the quality of perishable food organisms and their metabolites that cause food spoilage. The under-
items. The quality of several fish species have been evaluated with lying concept is that the target micro-organisms which grows cause
enzymatic TTIs. The advantages, limitations, and difficulties in an ap- irreversible changes such as variation in pH (which indirectly result in a
plication for real-time monitoring of fish quality have been detailed by color change) ensuring a direct indication of the quality of the food
Giannakourou, Koutsoumanis, Nychas, and Taoukis (2005). Several product within the package (Dutra Resem Brizio, 2016). These in-
studies have proved that TTIs significantly help in monitoring changes dicators find applications in various products including fresh foods,
in food attributes (Yan et al., 2008). Though several TTIs have been fruits, and seafood.
developed for dairy products, fish products and other sea foods, frozen In fishes, the quantity of total volatile basic nitrogen (TVB-N) is used
foods and chilled meat by monitoring shelf-life and storage properties as a critical factor of identification of spoilage. Traditional method of
to effectively employ them in intelligent packaging techniques, there analysis of TVB-N levels involve a time-consuming procedure of de-
are limited research works in intelligent packaging of liquid foods. tecting chemical reactions between perchloric acid and volatile amine
Lu, Zheng, Lv, and Tang (2013) reported the use of an enzymatic group, and an additional examination by acid-acid titration method
TTI based on alkaline lipase diffusion though PVA gel substrate to (Commission Decision 95/149/EC of 8 March 1995). Hence, the need
monitor freshness of milk. Cumulative effect of time and temperature for freshness indicators is realistic and freshness indicators as intelligent
was monitored through the diffusion length of the color band. Hetro- methods have been employed using various techniques for detecting
epitaxial growth of plasmonic nanocrystals (silver as the shell on gold food spoilage. In most cases, they function based on pH-sensitive dyes,
nanorods), gave sharp, contrast chronochromics from red to green, with colorimetric approaches or biofilms. Freshness indicators working
tunable temporal duration of color change from minutes to months. based on colorimetric approaches detect an increase in pH caused by
This was made possible by simple adjustment of reaction parameters spoilage, corresponding to total volatile amines. Natural-dye based food
and was developed as a kinetically programmable plasmonic TTI for freshness indicators using curcumin, grape peel and beetroot extracts
highly perishable foods like milk (Yan et al., 2013). In studies on de- have also been explored for detecting ageing of cod flesh. It has been
veloping a bio-polymer based TTI functioning on pH changes, natural proved that natural bio-based extracts as dyes in pH based food fresh-
extracts of Brassica oleracea (red cabbage) was incorporated with bio- ness indicators can be effectively used in intelligent packaging systems
polymer chitosan and synthetic polymer poly-vinyl alcohol. This TTI as they can conveniently function based on total color difference values
actively sensed pH changes in pasteurized milk and provided a visual (Tichoniuk, Radomska, & Cierpiszewski, 2017).
indication by color change, and proved its efficacy for intelligent Similar works on fresh fruits and cut-vegetables have experimented
packaging of liquid foods. (Pereira, de Arruda, & Stefani, 2015). and it is understood that a combination of bromothymol blue and
In spite of well-established technological advancement in TTI, rapid methyl red in the ratio of 2:3 can be used as a real-time freshness in-
activation by UV or temperature necessitate special storage and hand- dicator for green bell pepper stored at 7 ± 1 °C. These freshness in-
ling requirements prior to being used for commercial food packaging dicators have been used in the form of labels that can show an intense
applications. To overcome these issues, recently, room temperature color change from yellow-green to orange (Fig. 1) with an increase in
storable air activated TTI have been developed and investigated for CO2 concentration (Chen, Zhang, Bhandari, & Guo, 2018). Almost all
shelf-life monitoring of sandwich stored at 5 °C for 63 h (Lee, Kim, Jung, developed freshness indicators belong to indirect contact types. A real-
& Lee, 2019). This TTI works based on a redox reaction between col- time monitoring system for freshness indication of direct-contact type
orimetric material (leuco methylene blue) and redox reaction repressor for chicken breasts based on pH variations has also been developed,
(a mixture of L-ascorbic acid and L-cysteine; AC), in the presence of O2 consisting of bromocresol purple immobilized with polyvinyl alcohol
from the environment. Selected commercially available time-tempera- on high absorbance pad. This can be used as both: freshness indicator
ture indicators and their features are presented in Table 1. Apart from and as a shelf-life determination tool with high sensitivity (Kim, Lee,
being used as intelligent tools for recording temperature history, TTIs Lee, Baek, & Seo, 2017).
also finds its application in chill management systems (Tsironi, Gogou, A ripe sensor is another intelligent tool which can indicate the
Velliou, & Taoukis, 2008), quality indicators (Bobelyn, Hertog, & quality and freshness of foods. Here, the term freshness related to the
Nicolaï, 2006), and, shelf life indicators (Taoukis & Labuza, 1989). ripeness of a specific fruit. One such commercially available system is
Ripesense® developed by Plant & Food Research, Auckland, which was
3.1.3.1. Simulations in TTI. Various simulations have been done in the world's first intelligent label sensor that could indicate fruit ripeness

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Table 1
Selected commercial TTIs system used in food packaging applications.
S. Kalpana, et al.

TTI commercial name Developer Operational principle Features/scope Food applications References

3M™ MonitorMark® 3M Molecular diffusion of coloured dye-based ester into Partial history indicator with a pressure sensitive Bakery, beverage, confectionary Kour et al. (2013)
viscous material matrix adhesive backing and wrick; temperature scale to and meat products
indicate time dependent temperature history.
Fresh-Check® Temptime Central part of the label is the most active/reactive Self-adhesive device also serving as a freshness Mushroom Nuin et al. (2008)
Temperature Corporation part; on reaction (i.e. at higher temperature), darkens indicator as it records full temperature history
Intelligence™ irreversibly at an accelerated rate
Insignia Deli Intelligent Insignia Colour change accelerates with fluctuation or change Monitors freshness based on accurate description of Chilled products Yusufu, Wang, & Mills, 2018;
Labels™ Technologies in pre-calibrated temperature ranges time and temperature Mohebi & Marquez, 2015
OnVu™ EVIGENCE Activated with UV light source, the dark colour of TTI Tailored for specific shelf-life and optimum Meat, fish and dairy products Mohebi & Marquez, 2015
SENSORS™ progressively becomes lighter with change in temperature ranges; provid consumers with detailed
temperature; colour fading and activation energies of information on transport and storage of product
spiropyran crystals correspond to characteristic
change in bacterial growth
Coolvu™ EVIGENCE Temperature dependent aluminium layer is coated Provides real-time and visual information about the Dairy products, baked goods and Ghaani, Cozzolino, Castelli, and
SENSORS™ with a reactive layer which triggers a chemical product (rather than mere information on use by beverages Farris (2016)
process as the food spoils; respective colour date/expiry date)
changesserve as indicator
Smart dot EVIGENCE Indicator changes colour from green to red when Automatically activated and applied on high speed Bakery and frozen food products https://evigence.com/time-
SENSORS™ exposed to temperature production lines; not affected by UV or light; can be temperature-indicators/, Accessed 1
read visually and digitally via smartphones July 2019
WarmMark® DeltaTrak A blotter paper pad saturated with a red-dyed Visual pass/fail confirmation of exposure to Temperature monitoring during https://www.deltatrak.com/
chemical is specially formulated to melt at the tag's temperature excursions; processing, storage and warmmark-labels,
response temperature Irreversible colour change indicates duration above transportation Accessed 1 July 2019
threshold

148
FlashLink® mini electronic DeltaTrak Electronic time temperature indicator provides visual Alarm triggered after 4 h of accumulated Temperature monitoring during https://www.deltatrak.com/
time-temperature detection of temperature abuse during transportation temperature abusel mounted on high-visibility transportation flashlink-electronic-time-and-
indicator locator card; temperature-indicator,
post-trip evaluation service is also available Accessed 1 July 2019
Cold Chain iToken™ DeltaTrak Smart barcode system tracks cumulative temperature Simple pull-tab activation provides positive ‘ON’ Cold chain management https://www.deltatrak.com/cold-
above threshold value; irreversible barcode change reading; can be scanned with barcode readers or chain-itoken,
provides discrete temperature data Smart phones (iPhone, Android) Accessed 1 July 2019
TempDot® DeltaTrak Indicates cumulative exposure above temperature Indicator window confirms activation; labels can be Shipping, storage and https://www.deltatrak.com/
threshold shipped and stored under any temperature distribution of seafood and meat tempdot-plus-labels,
Accessed 3 July 2019
Freshtag Vitsab The indicator has two separate compartments: When the indicator is not activated, dot appears Meat, fish, and dairy products Tsironi, Ronnow, Giannoglou, and
/Check point ® International AB enzyme solution compartment and substrate solution white. Upon manual or online automated rupture of (eg. Growth of Vibrio spp. during Taoukis (2017)
compartment and pH indicator; controlled lipolytic the inter compartment seal, colour changes from transportation of oysters)
hydrolysis of substrate by enzymes triggers pH green to red based on time- temperature exposure
reduction and colour changes of the indicator
OliTec™ Oli-Tec Multi-layer label in which the base layer comprises of Can monitor degradation profiles of food products Fresh produce and processed https://www.oli-tec.com/, Accessed
Open life multiple ‘reservoirs’, each containing different fluids; at specific storage conditions foods 2 July 2019
packaging middle layer contains multiple ‘conduits’ or capillaries
of differing lengths filled with high viscosity media,
connecting into the reservoirs below to allow the
fluids to react with each other; the top layer acts as
the ‘start mechanism’ for the label when partially or
peelably removed at the point of packaging also has
surface decoration and a viewing window
(continued on next page)
Trends in Food Science & Technology 93 (2019) 145–157
S. Kalpana, et al. Trends in Food Science & Technology 93 (2019) 145–157

by color changes on the packaging material. The onset of ripening in

Louvet, Thuault, and Vaillant (2005)


fruits produces a characteristic aroma. This has been used in some

http://cryolog.com/en/topcryo/,
cases; the sensor element reacts with these aroma compounds and this
results in a change in its color. Initially the color of the label is red and
gradually changes to orange during ripening, finally turning yellow). At
Accessed 2 July 2019

present, this sensor label is available for only pears and research is
being done for other fruits such as kiwi, mango, melon, avocado and
stone fruit (http://ripesense.com/, accessed 19 June 2019). Ripe sensor
References

embedded on the surface of apples also work on the same principle and
follows the same mechanism (Fig. 2) (Kim et al., 2018).
Japanese design agency To-Genkyo proposed a non-scannable and
non-purchasable patterned barcode as a freshness indicator that can
Real-time quality monitoring of

change its color upon reaction upon interaction with ammonia released
by foods during spoilage. This is designed in the form of an hourglass
packed foods in cold chain

and the change in color indicates the onset of spoilage. This can work
Real-time monitoring

well for animal products (https://www.packagingoftheworld.com/


Food applications

2010/06/fresh-label.html, accessed 19 June 2019). The dual on-


package sensor was designed using methyl red and bromocresol purple,
and this pH indicator helps in detection of freshness in beef products
(Kuswandi & Nurfawaidi, 2017). While most of these sensing mechan-
isms are based on color chaning dyes, penetration of the dyes can im-
pact organoleptic property of the packed food. To prevent this, Lee,
Can monitor cold chain compliance; available over

Baek, Kim, & Seo, (2019) developed triple layer freshness indicator,
Can monitor temperature exposure on packaged

with a nonwoven high-density polyethylene (HDPE) sheet (Tyvek®,


with excellent water resistant and good air and vapor permiability) as a
base lyer (in contact with food), bromocresol green (pH sensitive dye)
temperature range from 2 to 12 °C

immobilized with the binding polymer as the colorchanging layer, and


a low-density polyethylene film as the outer layer. This indicator ef-
fectively sense checken spoilage corelated with chang in volatile basic
nitrogen, CO2 and bacterial count (Fig. 3), with no dye migration from
sensing layer, which offers safe, simple and reliable, packaing solution
with digital image processing via a smartphone for quality check.
Features/scope

3.3. Leak indicators


foods

Modified atmosphere packaging involves altering the atmosphere


(i.e. gas concentration levels) inside the package with the focus on
sensitive microbiological label changes its colour from

change in pH is sensed as colour change from green to


Time and temperature cause microorganism growth,
which in turn produces lactic acid and reduces pH;
Based on time/temperature exposure, temperature

extending product shelf-life. However, leaks or distortion in the in-


tegrity of the package can pose concerns. Defects in the package can
also result in variations in optimal concentration of gases, and such
variation in concentrations have drastic effects on the quality of foods.
This can have implications on taste, nutrition, texture, and overall
product acceptability. Hence, to maintain and monitor integrity of
packages, leak indicators find excellent applications (Daş, Gürakan, &
Bayindirli, 2006).
Operational principle

An oxygen indicator was designed based on UV activation with al-


ginate as the coating polymer. The idea behind UV based indicator ink
is the problem of leaching of dyes and solubility of the coating with
green to red

food, which could even result in undesirable quality changes. Results


showed that alginate based UV activated oxygen indicator can serve as
red

a good water-resistant coating as evident from decrease in thionine


leakage (Vu & Won, 2013). Another research group reported a similar
oxygen indicator made up of nanoparticles of P25TiO₂ (semiconductor
photo catalyst) coating of methylene blue (MB) as redox dye and DL-
Developer

threitol (as sacrificial electron donor). This was humidity independent


Cryolog

Cryolog

on low temperatures of around 5 °C. The performance was evaluated


with a study on pork PET packaging, at different time intervals under
refrigeration temperature (5 °C). Characterization was done with a
spectrophotometer for color properties, photo activity and oxygen
sensitivity (Mills et al., 2012).
TTI commercial name
Table 1 (continued)

Apart from conventional oxygen indicators, a pressure operated


Traceo® and eO®

compartmented oxygen indicator was designed and studied at different


combinations of MB, glucose, and NaOH at atmospheric conditions for a
TOPCRYO

time period of 12 h. One of the three combinations used alkaline NaOH


separated from the other compartment consisting of an aqueous mix-
ture of MB and glucose by a fragile barrier. This showed higher stability

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S. Kalpana, et al. Trends in Food Science & Technology 93 (2019) 145–157

Fig. 1. Color changes of fresh-cut vegetables indicated by freshness indicator. Source: Chen et al., 2018. (For interpretation of the references to color in this figure
legend, the reader is referred to the Web version of this article.)

Fig. 2. (A) Ripe sensor embedded on the surface of apple. (B) Graph depicting color change of label during ripening process. Source: Kim et al., 2018. (For
interpretation of the references to color in this figure legend, the reader is referred to the Web version of this article.)

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S. Kalpana, et al. Trends in Food Science & Technology 93 (2019) 145–157

Fig. 3. Triple layered freshness indicator, preventing dye migration from sensing element and easy read via smartphone for food quality check. Source: Lee, Baek,
Kim, & Seo, 2019.

even under aerobic conditions and proved to be a colorimetric oxygen strength. While being a pH indicator showing visible color change in
indicator which could indicate by change of color in proportion with acidic and alkaline conditions for intelligent packaging applications,
the concentration of oxygen. Thus, it was concluded by the research this film also has the potential to actively prevent packed fish spoilage
group that it can be used as an intelligent tool to detect leaks in mod- (Jamroz, Kulawik, Krzysciak, Talaga-cwiertnia, & Juszczak, 2019). For
ified atmosphere packaging (Jang & Won, 2014). intelligent packaging of liquid foods, a colorimetric film based on κ-
As variations in oxygen concentration lead to quality deterioration, carrageenan incorporated with Lycium ruthenicum Murr. extract was
variation in carbon dioxide also leads to microbial spoilage. Thus, a CO2 investigated as in contact pH indicator for milk freshness. This indicator
indicator can be used as a leakage indicator for certain applications. gives reversible color change over the pH range of 2–10 with pink to
Like oxygen indicators, colorimetric CO2 indicator from natural extracts colorless over pH range of 2–6 and blue purple yellow over pH of 7–10.
have been designed with a mixture of lysine, ԑ-polylysine, and antho- The film was also found to be suitable for freshness indication of
cyanin from natural sources to determine variations in pH. The un- aquatic food products (Liu et al., 2019). Examples of pH indicators for
derlying mechanism on which this integrity indicator works is the different food products have been discussed in Table 2.
formation of carbonic acid derivatives through an irreversible reaction.
Researchers have analyzed both aqueous type and label type indicators 4. Data carriers
with different CO2 concentrations and observed the visible color change
from azure to intense purple in an experiment with poultry meat (Saliu Traceability is the “ability to follow the movement of a feed or food
& Della Pergola, 2018). through specified stage(s) of production, processing, and distribution”
(ISO, 2007). Traceability helps in improving food safety (R. S. Chen,
3.4. pH indicators Chen, Yeh, Chen, & Kuo, 2008) and in achieving a better market for
consumers as the total history of the package can be easily accessed
This type of indicator is not essentially the one in which variations with bar codes and Radio Frequency Identification (RFID) tags.
in pH have been used to monitor food freshness and quality. Instead, it
refers to a category of indicators as it just conveys pH variations which 4.1. Barcode
can be further used to develop various other tools.
A colorimetric based pH indicator was developed using agar. Potato A barcode is a machine-readable storage database working on the
starch was used as immobilizer for natural dye (anthocyanin). optical phenomenon of bars spaced at regular width and thickness.
Variations in pH were directly related to spoilage in meat. The devel- Barcodes are of two types: 1D and 2D (Chen et al., 2008); 1D barcode is
oped indicator was tested in pork samples with different buffers. The a simple linear arrangement of white and black bars positioned alter-
pH indicator showed the final point of spoilage at pH value 7.42 from natively, and is used for storing information and data. For the same
an initial spoilage indication at a pH value of 6.28 (where the fresh and function, 2D barcodes employ two-dimensional geometric patterns (Lin
semi-fresh pork samples were at pH values between 5.18 and 6.16). & Lin, 2013). The information stored is collected using an optical reader
This was indicated by a visible color change from red to green. The which scans the arrangement of bars and directs the received content to
indicator was effectively used in intelligent packaging n of pork. a unique identification consisting of alphanumeric (Mahalik & Kim,
Further, research can be done to improve the same for other meat 2016). As an intelligent tool, barcodes can be used to monitor inventory
products (Choi, Lee, Lacroix, & Han, 2017). In another application, a control for assessing individual identification numbers and thus can be
film made up of natural chitosan and anthocyanin as both pH and utilized to trace product history. Universal Product Code (UPC) was the
colorimetric indicators capable of showing an intense and visible color first commercialized barcode, appearing as a pattern of spaces and
variation from pink to bluish-green to yellow, at acidic, neutral and lines, even in use till date. Reduced Space Symbology is another form of
basic conditions, respectively, has also been developed (Yoshida, barcode which emerged later to meet demands for reduced space usage
Maciel, Mendonça, & Franco, 2014). in packages. Similarly, there is a range of other forms of linear sym-
Moreover, the inclusion of these natural polyphenolic compounds as bology with patterns and symbols containing embedded information
pH indicators also offer added advantages like antioxidant and anti- regarding the product (Manthou & Vlachopoulou, 2001; Yam et al.,
microbial properties, showing multifunctional applications (X. Zhang 2005). Different barcodes have been shown in Fig. 4 (Fang, Zhao,
et al., 2019). For example, incorporation of Pu-erh (fermented) and Warner, & Johnson, 2017).
green (unfermented) tea extracts in furcellaran and gelatin biofilm A color based sensor array fabricated in silica beads has been de-
show antioxidant and antimicrobial properties with increased tensile veloped and further modified as a barcode with help of three dyes: Nile

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Table 2
pH indicators for different food products.
Materials/chemicals Working pH range Food References

Polyvinyl alcohol, chitosan nanoparticles & mulberry 1–3 Fish Ma, Liang, Cao, and Wang
extracts (2018)
Polylactic acid, poly (ethylene oxide) & phycocyanin 3.6–4 Citrus fruits Moreira, Terra, Costa, and
5.6–6.2 Meat Morais (2018)
Agro industrial waste cassava starch & blueberry All pH Corn oil, chicken meat, Luchese, Abdalla, Spada, and
residue orange juice Tessaro (2018)
Tamarind seed polysaccharide & litmus lichen 4–10 Milk Liang and Wang (2017)
Chitosan, blueberry and blackberry pomace 4–7 Meat Kurek et al. (2018)
Corn starch, glycerol, black bean seed coat and red 5–8 Meat Prietto et al. (2017)
cabbage
Purple potato extraction, chitosan and surface- 1–14 Can be used for foods that Li et al. (2019)
deactylated chitin nanofibers undergo rapid oxidation
Black rice bran anthocyanins, oxidized-chitin 1–12 Seafood Wu et al. (2019)
nanocrystals and chitosan matrix
Anthraquinone and azo chromophores on cellulose 1- 12 (pH 6-12- colour change from 460 nm to Cooked crabs H. Zhang, Hou, Xie, & Gao,
fiber with printed patterns 520 nm; pH 1–4 colour change from 502 nm to 2019
420 nm)
Alizarin (1,2-dihydroxy anthraquinone) in a starch- 2–11 Rainbow trout fillets Ezati, Tajik, Moradi, and
cellulose paper Molaei (2019)

packaging applications (Bibi, Guillaume, Gontard, & Sorli, 2017). An


antenna acts as the intermediate electromagnetic wave medium and
severs as a pathway for transmission of information between a tag and
the reader (Chen et al., 2008). The reader is a small component whose
primary function is to serve as a platform for analyzing and receiving
information from the tag for further processing. Electronic chips are
used for encoding information in the form of bits in the Electronic
Product Code (Bibi et al., 2017). RFID middleware, as the vital part,
performs several functions like filtering, integrating of data, coordina-
tion of reader and proper management of scheduled processes(Chen
et al., 2008).
RFID tags have found several applications in horticultural produces,
meat and fishery products, dairy and bakery products, beverages and
other foods (Costa et al., 2013). In case of fish, RFID tags include a
printable smart RFID tag for detection and examination of spoilage by
understanding humidity and volatile amine levels. Anisotropic con-
ductive adhesives (ACA) have also been used as integrated chips. Low
power consuming MSP430G microprocessors have been used and the
developed RFID system was quantified with a study of codfish at a
temperature of 5 °C for an interval of 2 min. It was concluded that the
developed RFID was independent of the type and quantity of fish, but
depends on freshness indicating factors (Smits et al., 2012). Similar
works in chilled fish products have been conducted to monitor fresh-
ness in cold chain and traceability using smart RFID tags working at
high-frequency ranges and capable of detecting fluctuations in relative
Fig. 4. Barcodes used in food packaging. Source: Fang et al., 2017. humidity and temperature (Abad et al., 2009).

red, zinc tetraphenylporphyrin and methyl red in three different geo- 5. Sensors
metric shapes, to detect spoilage in chicken. Detection is based on the
separation of red, blue, green dyes and can be read out by a built-in app Sensors are electronic devices that detect and convert one form of
devised in a smartphone. The approach is cost effective and the fabri- signal to other form using a transducer. Based on the working type of
cation process is simple (Chen et al., 2017). If pathogenic bacteria grow the transducer, sensors can be classified into active and passive types.
inside the package during the storage period, it can be sensed by the Chemical and biosensors have been used as intelligent packaging tools
barcode, thereby undergoing changes in color, thereby making the for common analytes like pH, humidity, color and biological species
barcode unreadable. (Mahalik & Nambiar, 2010). The edible sensor is another new concept
which is poised to make a great pathway in the field of food packaging
4.2. Radio frequency identification as it is a non-destructive method of spoilage detection. Pectin based
edible sensor with a combination of the principle of colorimetric
RFID is a technology which is usually available as a chip made up of changes of anthocyanins (red cabbage extract) and variations in total
tags which are mainly used to store data. They are basically of two volatile basic nitrogen with spoilage of meat-based products were de-
types; active and passive, classified based on battery requirement. veloped (Dudnyk, Janeček, Vaucher-Joset, & Stellacci, 2018). Based on
Active types use the battery as power sources and passive type generate a similar concept, membrane film sensor was developed and char-
power from signals received. Generally, low frequency (125 kHz–134 acterized for golden pomfret fillet freshness by inkjet assisted layer-by-
kHz) and high frequency (13.56 MHz) ranges are used in food layer and polyelectrolyte multilayer film fabrication method. The idea

152
S. Kalpana, et al. Trends in Food Science & Technology 93 (2019) 145–157

Fig. 5. Electrochemical pattern writing on red radish anthocyanins incorporated gelatin-gellan gum film (A) under different current; (B) patterning in different
structure; (C) its response to acid and ammonia gas; (D) intelligent sensing of milk and crap freshness. Reprinted with permission from (Zhai et al., 2018). Copyright
(2019) American Chemical Society. (For interpretation of the references to color in this figure legend, the reader is referred to the Web version of this article.)

was to detect spoilage of fish fluids due to variations in pH represented types and grouping similar ones, as well as the possibility of monitoring
via a fluorescent sensitive dye. This approach is non-toxic and can be the aging process as a function of the storage conditions (Medeiros,
potentially effectively used for food packaging applications (Kiryukhin Gregório, Martinez, & Mattoso, 2009). Wen et al. (2015) developed
et al., 2018). Based on ammonia and biogenic amines detection, solid-state polyaniline (PANI)/polyamide 66 (PA66) nanofiber sensor
covalent immobilization of pH sensitive dyes into food grade silicone based on reversible non-redox acid/base doping process to detect L-
matrix for the development of optical colorimetric sensor have been ascorbic acid (L-AA). Such superior and inexpensive sensing films can
developed for freshness evaluation. However, the toxicity of in- detect L-AA and indicate visible color changes even at a low con-
corporation of sensors into food and the cost-factor limit its commer- centration of up to 50 ppb, which can be automatically read out via an
cialization (Schaude, Meindl, Fröhlich, Attard, & Mohr, 2017). iPhone. All these film based sensor have potential to be incorporated in
intelligent packaging.
5.1. Chemical sensors
5.1.1. Gas sensors
Sensors undergo chemical interactions between substrate and ana- Gas sensors are intended to detect and indicate the presence of
lyte molecules, which are in turn used for detection/sensing applica- gaseous or volatile compounds like carbon dioxide, oxygen, volatile
tions. Ramon-Marquez, Medina-Castillo, Fernandez-Gutierrez, and amines, and other specific gases. Carbon dioxide sensor based on for-
Fernandez-Sanchez (2016) developed highly selective optical sensors ester resonance energy transfer mechanism which is a solid-state
based on covalent interaction between active vinyl groups and trypta- polymeric optochemical sensor has been used for detecting accurate
mine molecule to detect biogenic amines in beer. Covalently bound levels of carbon dioxide with the help of an indicator dye (phosphor-
amines give luminescence signals due to its intrinsic phosphorescence escent Pt-porphyrin) and α-naphtholphthalein. The developed sensor
nature. The high concentration of active vinyl groups (330 μmol/g) was also characterized and examined for toxicity due to migration of
incorporated in nanofibers (300 nm diameter, 150 μm thick membrane) dyes (Pereira et al., 2015). Based on the same principle, with a different
could detect tryptamine in ten different varieties of beers, with a de- pH indicator dye (Sudan III co-immobilized in the sol-gel matrix-ru-
tection limit of 6 ng/ml. Nitrite in foods samples like sausage and pickle thenium polypyridyl complex), the CO2 sensor was able to detect even
could be sensed electrochemically using N-doped graphene quantum low concentrations of CO2 (up to 0.06%) with accuracy and rapidity.
dots decorated N-doped carbon nanofibers membrane. Incorporation of Though both sensors exhibit cross-sensitivity with O2 detection, it can
N-doped graphene quantum dots increases the electron transfer rate be overcome through suitable modifications (Von Bültzingslöwen,
and N-doped carbon nanofibers provide higher electrical conductivity McEvoy, McDonagh, & MacCraith, 2003).
and large electroactive area and free-standing film structure, making Aydogdu et al. (2011) used ion pair formation between fluorescent
the composite appropriate for the electrochemical sensor. This quantum dye 8-hydroxypyrene-1,3,6-trisulfonic acid trisodium salt (HPTS)
dots based nanofiber sensor displays superior performance for nitrite (sensitive to pH and CO2) and room temperature ionic liquid (RTIL) to
sensing with low detection limit of up to 3 μM, a wide range of linearity, sense CO2. RTIL was incorporated in poly methyl methacrylate or ethyl
high selectivity and excellent reproducibility (Li, Liu, Wang, Mao, & cellulose and formed as nanofiber (∼370–527 nm diameter) based
You, 2017). optical sensor which show 24 to 120-fold higher sensitivity towards
Taste sensor array for classification of eight different types of orange CO2 with shorter response time than thin film based sensors and has
juices was developed using polyaniline nanofiber. Through capacitance potential to be incorporated in intelligent packaging. Zhai et al. (2018)
measurements, the nanofiber sensors were able to detect changes in developed pH based gas sensing edible film from gelatin, gellan gum,
citric acid concentration in aqueous solutions of orange juices up to and red radish anthocyanin extract, showing an orange red-to-yellow
values as low as 2 ppm, proving its efficacy for separating different color change in the pH range of 2–12 (Fig. 5). Multicolored patterns

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S. Kalpana, et al. Trends in Food Science & Technology 93 (2019) 145–157

were successfully written by electrochemical writing and were used for

Chun, Min, & Hong, 2014; Lv et al., 2019;


Banerjee, Kelly, Kerry, & Papkovsky, 2016
real-time sensing of milk and fish spoilage. This film indicates the

Borchert, Kerry, and Papkovsky (2013)


freshness of milk by sensing the gas produced by anaerobic bacteria in
milk. Similarly, this film could indicate the freshness of black carp by

Von Bültzingslöwen et al., 2003


changing the color of the film, induced by volatile basic gases like
ammonia, trimethylamine, and dimethylamine generated by decom-
position of proteins by bacteria and enzymes.

Banerjee et al. (2016)


Oxygen sensors are based on different principles such as photo-

Zhai et al. (2019)


luminescence quenching, lifetime decay of O2 sensitive dyes, polymeric
host quenching, etc. Phosphorescent solid-state oxygen sensors-

References
OptechTM-O2 and Platinum & Platinum (II)-benzoporphyrin dye based
polypropylene were developed and characterized at two physical con-
ditions with plasma processing. It was concluded that both optochem-
ical sensors can be effectively used as intelligent tools in the packaging

Sensor was optimized by analyzing different chemo-sensitive dyes which respond to


increasing stability with decrease in storage temperature with 1 min response time

The gGellan gum- silver nanoparticles shows colour changes when used as colour
Variations in concentration of O2 is determined by the intensity of luminescence
quenched by the oxygen sensitive phosphorescent dye; sensor responses quickly

sensor for hydrogen sulfide sensor to detect the spoilage ofin chicken and silver
hydroxide as base in methanol and nano beads were spin coated to from sensor
(Pankaj et al., 2016). Optical oxygen sensors for muscle-based products

Sensor was prepared by ion pairing method using cetyltrimethylammonium-


cetylmethylammonium hydroxide as phase transfer agent; sensor showed an
detect spoilage by quantitative measurement of residual oxygen present

Plastic matrix incorporated with PtTFPP as phosphorescent indicator dye,

layers which showed improved response time; resolution of ± 1% to CO2


in the headspace of package. The developed oxygen sensor showed a
decrease in oxygen content, increase in levels of pH, TVB-N and TBA at

naphtholphthalein as colorimetric pH indicator and tetraoctyl or


4 °C for both beef and chicken fillet samples (Sharoba, Morsy, Khalaf, &
El-Tanahi, 2014).
An amine gas sensor system for freshness examination by quanti-
tative measurement of ammonia, dimethyl amine and trimethyl amine
released by fresh fish on comparison with pre-detected results was
developed with organic solid-state semiconductor with a detection

change in pH and thiobarbituric acid levels.


period of 1 min and characterized with three different types of fishes
(Chang et al., 2017). Another ammonia gas sensor for protein-rich food
materials was also developed using polyaniline (a conducting polymer)
by oxidative polymerization and the developed sensor was flexible,
consumed less energy for operation and was more sensitive (Matindoust

and 4 min recovery time


et al., 2017). An additional list of gas sensors with the principle of

and results are reliable


operation/mechanism has been described in Table 3.

concentration.
Description

5.2. Biosensors

carp
The sensor in which a biological analyte plays the role of detection
of a change, further converted into an electric signal using a transducer,

Binding of silver from silver nanoparticles with


is a biosensor. A biosensor based on strong analyte interactions for
Forster Resonance Energy Transfer (FRET)

Colorimetric detection based on array of

quality monitoring of muscle-based products (beef and chicken fillets)

hydrogen sulfide to form silver sulfide


was developed to indicate color changes from green color fresh to red
color after 9 days and 10 days of storage for beef and chicken fillet,
Dual Luminophore Referencing

Photoluminescence quenching

respectively was developed to explain spoilage history (Fang et al.,


chemo-sensitive compounds

2017). In another study, an electrochemical biosensor based on nylon-6


nanofibrous membrane functionalized with glucose oxidase (GOX) en-
zyme was developed to sense glucose in various beverages
(Scampicchio, Arecchi, Lawrence, & Mannino, 2010). GOX was im-
Description of gas sensors with principle of operation/mechanism.

mobilized on electrospun nanofibrous membrane by chemical cross-


Principle

linking via glutaraldehyde and bovine serum albumin. Here, ferrocene


methanol was used as the electron acceptor to replace dioxygen as a
cofactor for GOX enzyme, thus mediating the electrochemical trans-
Hydrogen sulfide

duction process. Upon analysis of different beverage samples such as


Carbon dioxide

Carbon dioxide

digested milk, coke, honey, and energy drinks, GOX immobilized na-
compounds
Element of
Detection

nofiber based biosensor confirmed accurate sensing of glucose (with


Volatile

Oxygen

rsd < 1%) as compared to colorimetric assay (rsd > 8%). Such con-
cepts can be modified for intelligent food packaging applications.
Pesticide detecting acetylcholinesterase biosensor made of nano
gold particles, chitosan, naifon modified nano porous pseudo carbon
Gas sensor-based on colorimetric

Gas sensor-based on colorimetric


Gas Sensor- optochemical sensor

showed a rapid response, acceptable stability and sensitivity to orga-


Gas sensor-based on sol gel

nophosphate and methyl parathion pesticides at low detection limits


(Deng, Liu, Liu, Dong, & Li, 2016). Field effect transistor based bio-
photoluminescence
Gas sensor-based on

sensors with the microfluidic channel in the form of a chip was im-
planted in the epoxy method of fabrication of biosensors. This can be
Type of Sensor

adopted for food packaging applications as it reduces the size of the


sensing

sensing

sensor to a much reduced area and has the potential for high trans-
Table 3

conductance gain (Hsu, Chen, & Wang, 2017).

154
S. Kalpana, et al. Trends in Food Science & Technology 93 (2019) 145–157

6. Conclusion 011.
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The author M. Maria Leena acknowledges Department of Science Ellouze, M., Pichaud, M., Bonaiti, C., Coroller, L., Couvert, O., Thuault, D., et al. (2008).
Modelling pH evolution and lactic acid production in the growth medium of a lactic
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