Application of Electronic Tongue For Fresh Foods Quality Evaluation A Review

FOOD REVIEWS INTERNATIONAL
2018, VOL. 34, NO. 8, 746–769

https://doi.org/10.1080/87559129.2018.1424184
Application of electronic tongue for fresh foods quality

evaluation: A review
Hongyao Jianga, Min Zhanga,b, Bhesh Bhandaric, and Benu Adhikarid
a
State Key Laboratory of Food Science and Technology, Jiangnan University, Wuxi, Jiangsu, China; bJiangsu
Province Key Laboratory of Advanced Food Manufacturing Equipment and Technology, Jiangnan University,
Wuxi, Jiangsu, China; cSchool of Agriculture and Food Sciences, University of Queensland, Brisbane, QLD,
Australia; dSchool of Applied Sciences, RMIT University, Melbourne, VIC, Australia
ABSTRACT KEYWORDS
Fresh foods occupy an important position in the human diet. A Electronic tongue;
growing number of consumers are attracted by fresh foods due to potentiometry; voltammetry;
their high nutritional value, healthy image, and appealing taste. impedance; sensory indices;
Electronic tongue based on the concept of global selectivity is a safety indices
sensor technology that has developed rapidly since last century
(1998). Compared with human panelists, it has the advantages of
measuring toxic substances, conducting objective analysis and hav-
ing no detection fatigue. In this paper, the principle, types, and
characteristics of electronic tongue are described. The application of
electronic tongue to measure sensory and safety index is discussed.
Finally, the development of miniaturization of electronic tongues is
presented.
Introduction
Fresh foods refer to the unprocessed or preliminarily processed agricultural products
for human consumption including fruits and vegetables, meat, milk, eggs, and
aquatic products. [1] The spoilage of fresh foods takes place frequently because of
the metabolism-related biochemical reactions, infection of putrefactive bacteria, and
substandard storage conditions.[2] To meet consumers’ pursuit for nutrition and
good flavor, a rapid detection technology electronic tongue (e-tongue) has been
investigated in fresh food processing.
The e-tongue is a kind of liquid analytical instrument consisting of three parts including
sensor array, signal acquisition system, and pattern recognition system [3](Figure 1). It was
initially applied to discriminate and analyze five basic tastes. Gradually, it turned into a helpful
tool in the detection of food adulteration, authenticity, and drug residue. Besides e-tongue,
many detection methods such as spectrum analysis, mass spectrometry, electrochemical
analysis, and human panelist have also been explored. Traditional methods are time consum-
ing, expensive, and they are clearly cannot be used for online measurements since discrepan-
cies often occur due to human fatigue or stress.[4] With the advantages of nondestructive
testing, toxic substances analysis and objective evaluation usually without sample pretreat-
ment, the application of e-tongue technology has extended into pharmaceutical industries,[5]
CONTACT Min Zhang min@jiangnan.edu.cn School of Food Science and Technology, Jiangnan University, Wuxi,
Jiangsu Province 214122, China
Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/lfri.
© 2018 Taylor & Francis
FOOD REVIEWS INTERNATIONAL 747
signal Pattern recognition

acquisition
system
Quantitative
analysis
Sensor array Computer
Figure 1. Schematic diagram of basic structural components of an electronic tongue.
environmental monitoring,[6,7] fermentation monitoring,[8,9] and horticultural technique. [10]

However, a disadvantage for the e-tongue systems compared with human is that they are often
affected by the environment factors, for example temperature will cause sensor drift.[11]
This review outlines the advances of e-tongue in the detection of sensory and safety
indices. It also describes the principle and the structure of e-tongues and makes compar-
isons between different taste sensors and updates the current research and development.
Electronic tongue
Sensing technology through a utilization of arrays of nonspecific sensors and pattern recognition
methods (artificial neural networks, principal component analysis, fuzzy logic, etc.) have been
developed since around 1980.[12] Toko et al.[13] firstly applied for a patent of taste sensor in 1989
and developed a taste sensor equipped with the transducer composed of lipid/polymer mem-
branes. The taste sensor with global selectivity showed the capability of transforming informa-
tion of taste substances into an electric signal.[14] In 1995, “Electronic tongue” was put forward as
“an analytical device employing an array of non-selective chemical sensors with partial speci-
ficity to different solution components and an appropriate pattern recognition instrument,
capable of recognizing quantitative and qualitative composition of simple and complex
solutions”.[15] Both e-tongue and taste sensor are essentially the same instruments.[16]
With the features of low selectivity, high cross-selectivity and statistical analysis of the
outputs from multiple sensors, the sensors of an e-tongue are immersed into a sample to
measure its soluble components and global characteristic response signals of the taste
substances. The corresponding signals are sent to a signal processing system to analyze
using pattern recognition. [17]
Common types and working principals of electronic tongue

Sensor array is the core part of the e-tongue system. According to the different working
principles of the sensor array, common e-tongues have the following types: potentiometry,
voltammetry, and impedance spectroscopy. [18]
Potentiometry-based electronic tongue

Potentiometric e-tongue works by measuring and analyzing the different electrode poten-
tial of the samples between outer sensor membrane boundary and reference electrode.[19]
748 H. JIANG ET AL.
There are two types of sensors: one employs multi-channel lipid membrane sensors,
taking Ag/AgCl electrode as reference electrode. The changes of lipid membrane potential,
resulting from electrostatic and hydrophobic effects between the film of taste sensor and
the taste substances, are detected by the output terminal of computer through the signal
acquisition device.[20] Chalcogenide glass sensor uses chalcogenide glass as working
electrode, together with PVC film to realize potential detection. [21]
The e-tongue equipped with potentiometric sensors on the basis of ion-selective
electrodes has certain advantages including rapid response, reproducibility, simple mea-
suring set-up, and possibility of obtaining sensors selective to various species.
Potentiometric sensor arrays may be used for classification and analysis of complex food
samples.[22] However, the main disadvantage of potentiometric measurements is tempera-
ture dependence, and adsorption of solution components easily affect the nature of charge
transfer.[23] The most evident application of potentiometric e-tongue is the quality control
in the foodstuffs industry including taste assessment, evaluation of taste masking effect,
discrimination of liquid food (e.g., beer, honey, and teas) from different brands and types,
and classification of oils. [24–28] Besides, it is also applied in environmental and industrial
analysis, for instance, monitoring of water contamination. [29]
Voltammetry-based electronic tongue

In contrast with potentiometric techniques, the electrode potential in voltammetric instru-
ments is used to drive an electron transfer reaction, and the resulting current is measured.
The simplest measurement set-up employs three electrodes: reference electrodes, working
electrodes, and auxiliary electrodes. Working electrode usually uses a metal bare electrode
or a modified electrode composed of copper, nickel, palladium, silver, tin, titanium,
zirconium, gold, platinum, and rhodium.[30] The basic principle is that by means of
electrochemical voltammetry, the multi-sensor array is placed in the solution to be
measured, the step-potential is added to the working electrode, and the polarization
current of different solutions is measured to analyze the features of the samples qualita-
tively and quantitatively. The step-potential added to voltammetry e-tongue (VE-tongue)
mainly include cycle, conventional large pulse, and multi-frequency pulse. [31]
The VE-tongue can be used for multi-component measurement with high sensitivity
and selectivity, high signal-to-noise ratio and low detection limit. However, this technique
is only applicable to samples where oxidation-reduction reactions occur. Fouling of the
electrode surfaces (e.g., measurements in complex media including milk and process
water) will cause drift and loss of sensitivity, and eventually cause great damage to the
sensors.[32] The simple construction of the VE-tongue makes it suitable in many different
industrial applications including pulp and paper industry,[33], dairy industry (e.g., dis-
crimination of milk adulteration and classification of milk brands),[34] and fermentation
industry (e.g., monitoring the fermentation, post-ripeness and storage processes of set
yogurt, and detection of the optimum fermentation time of black tea). [35,36]
Impedance spectroscopy-based electronic tongue

Based on electrochemical impedance spectroscopy, the impedance-sensing units made
from ultrathin films physically interact with the sample in solution according to their
electrical nature, providing a fingerprint of the solution. [3] Cabral et al. utilized a compact
impedance e-tongue to perform rapid analysis of liquids, and these sensing units were
composed of several ultrathin membranes made from different materials deposited on

interdigitated electrodes.[37]
The impedance e-tongues are advantageous in comparison to potentiometry and
especially voltammetry, owing to the potential experimental simplicity and the reduction
of the response time. [38] They have been applied to qualitative discrimination of mineral
water, tea, coffee, and red wine. [39–41]
Pattern recognition methods

Pattern recognition is the study of how machines can observe the environment, learn
to distinguish patterns of interest from their background, and make sound and
reasonable decisions about the categories of the patterns. [42] The taste information
of samples was acquired by the sensors of e-tongue system and converted into an
electronic signal to be analyzed. To show the response of the e-tongue, electrochemical
responses are used to form databases that were subjected to unsupervised and super-
vised multivariate data analysis methods. [43] Routines include principal component
analysis (PCA),[44] linear discriminate analysis (LDA),[45] partial least squares (PLS),[46]
hierarchical cluster analysis (HCA),[47], learning vector quantization (LVQ),[48] fuzzy
c-means (FCM),[49] artificial neural network (ANN) such as probabilistic neural net-
work (PNN). [50] Among these techniques, PCA is mostly used in identification/
classification for qualitative purpose, and PLS is mainly used in multidetermination
for quantitative purpose. PCA, PLS, LDA, and HCA are based on a linear approach
while FCM, ANN, and PNN are regarded as nonlinear methods. Different recognition
methods have different applicability, and usually a variety of pattern recognition
algorithms are used in a study.
For example, after merging and preprocessing all the sensors data, PCA is used for extracting
information from a dataset by a lower number of variables called principal components (PCs).
Hence, PCA allows the reduction of multidimensional data to a lower dimensional approxima-
tion, while simplifying the interpretation of the data by the first two or three PCs (PC1, PC2, and
PC3) in two or three dimensions and preserving most of the variance in the data. HCA is the
unsupervised classification of patterns (feature vectors) into groups (clusters). Individuals within
the same group are more similar to each other than those belonging to different groups, so that
the distance between two objects in the dendrograms is measured to determine the similarity in
the objects in terms of each of its attributes. Multi-linear regression (MLR), back propagation
artificial neural network (BPANN) and support vector machine (SVM) calibration methods
have demonstrated their use for modeling. The performance of the final model is evaluated by
the samples in calibration set and tested by the independent samples in prediction set.
Correlation coefficient of calibration set (Rc), root mean square error of calibration (RMSEC),
correlation coefficient of prediction (Rp) and root mean square error of prediction (RMSEP) are
used to evaluate models. Good models should have higher Rc and Rp, lower RMSEC and
RMSEP, but small difference between Rc and Rp, or between RMSEC and RMSEP. [51]
Detection of food sensory index

Food sensory indices are the most intuitive indicators for describing and judging food
quality, and they are linked to consumer demand and choice for fresh food. One way
750 H. JIANG ET AL.
of obtaining a detection and evaluation system is to employ human sensory panel. One
drawback of this technique is that evaluating rotted food or drugs may be harmful to
the health of panelists, and sometimes the daily medicine taken by panelists (e.g., anti-
infective drugs, cardiovascular drugs and endocrine system drugs) will cause abnormal
taste that disrupts the result of sensory evaluation. [52] E-tongues have shown their
capability in the detection of food sensory index, including the discrimination between
basic taste properties and detection of taste masking effect. The e-tongue appears to be
a useful tool for the profiling of foods; however, it does not measure the release and
persistence of compounds during eating just like many analytical techniques.
Detection of basic taste

Taste is comprised of five basic gustatory feelings: sourness, saltiness, sweetness, bitterness
and umami. These five tastes are produced by the corresponding chemical components,
acids (e.g., HCl, acetic acid, and citric acid) with hydrogen ions generating sour, some
types of inorganic salts (e.g., NaCl, KCl, and NaNO3) producing saltiness, saccharides
(e.g., sucrose and glucose) developing sweetness, certain alkaloids and glycosides (e.g.,
quinine and caffeine) producing bitterness, some of the amino acids and their salts (e.g.,
monosodium glutamate(MSG) in seaweeds, disodium inosinate (IMP) in meat and fish
and disodium guanylate (GMP) in mushrooms) producing umami. [53,54]
E-tongues generally recognize the five basic tastes based on the construction of a
mathematic model that describes imitation of the human taste system. [55] When the sensor
membrane interacts with the taste substance, the molecular information is classified accord-
ing to taste intensity and quality. There are two opposing views of how taste qualities are
encoded in the periphery — the labeled-line model and the ‘across-fiber pattern’ model.[56]
In the first model, receptor cells are tuned to respond to single taste modalities and are
ennervated by individually-tuned nerve fibers. In this case, each taste quality is specified
by the activity of non-overlapping cells and fibers. For example, TS-5000Z potentiometric
e-tongue was invented based on this theory. It employs seven lipid membrane sensors and
three corresponding reference electrodes, with each sensor indicating a gustatory feeling
(e.g., sensor SB2AAE detects umami taste, sensor SB2CT0 detects saltiness and sensor
SB2CA0 detects sourness) (Table 1) [57,58]
In the second model, individual taste-receptor cells are tuned to multiple taste qualities,
and consequently the same afferent fiber carries information for more than one taste
modality.[56] Based on this theory, another potentiometric e-tongue — the α-Astree e-ton-
gue came out. It is equipped with a seven-sensor probe that can differ in composition of
Table 1. Sensors of the Insent taste sensing system TS-5000Z.

Sensor type Sensor name Corresponding taste
SB2AAE Umami sensor Umami
SB2CT0 Saltiness sensor Saltiness
SB2CA0 Sourness sensor Sourness
SB2AE1 Astringency sensor Astringency
SB2AC0 Bitterness sensor 1 Bitterness of cationic substances
SB2AN0 Bitterness sensor 2 Bitterness of cationic and neutral substances
SB2C00 Bitterness sensor 3 Bitterness of anionic substances
Reference electrode —
different sensors. There are three types of available sensor sets, and one of them is used for
food fields (sensors ZZ, BA, BB, CA, GA, HA, JB). The sensors work in a cross-selective way
with each taste assigned to these seven sensors, and the limits of detection for different
representative taste substances by each sensor are much lower than the human threshold
perception (Table 2).[59,60] These chemically modified field effect transistor technology
(ChemFET) sensors consist of two highly conducting semiconductor regions (a source
and a drain), which are surrounded with an insulator, and a sensitive layer (coated
membrane) is deposited above the insulator between the source and the drain. [5] The
picture α-Astree and TS-5000Z potentiometric e-tongues are shown in Figure 2.[58]
Table 3 lists the recent achievements concerning taste assessment by e-tongue.
Among the three types of e-tongues, the potentiometric e-tongue is the most
frequently used in the application of taste assessment including evaluation and
discrimination of five basic tastes [61–67], astringency quantification [68], and evalua-
tion of binary interactions of basic tastes. [69] In practice, the taste of various food
and beverages, including tea [63], milk [64], mineral water [70], grape juice [71], table
salt [61], mushroom [72], and fish [73], have been measured using e-tongue system. In
light of the present studies, analytical methods based on e-tongue can be a potential
alternative to sensory analysis for screening and selecting the products with better
quality and flavor among a range of potential products.
Table 2. The detection limits of the sensors of AstreeTM electronic tongue (mol/L).
Sensor type and response value
Basic Taste human perception threshold ZZ BA BB CA GA HA JB
Taste substance (×10–4) (×10–7) (×10–7) (×10–7) (×10–7) (×10–7) (×10–7) (×10–7)
+
sour H 1.6 1.0 1.0 1.0 1.0 1.0 1.0 1.0
salt NaCl 10.0 10 100 10 10 1000 1000 100
sweet sugar 6.5 1.0 1000 1.0 1.0 1000 1000 1000
bitter caffeine 5.0 100 1000 1000 100 1000 1000 1000
umami MSG 5.0 100 1000 1000 100 1000 1000 1000
Note: ZZ, BA, BB, CA, GA, HA, JB are the name of sensor arrays
Figure 2. Commercial electronic tongues:a) Taste sensing system TS-5000Z (Insent Inc., Atsugi-shi,
Japan); b) Astree2 (AlphaMOS, Toulouse, France).
752
Table 3. Application of electronic tongue in taste assessment.

Sensor type and materials Applications Data-processing algorithm Ref.
[61,63–66]
Potentiometry Lipidic membranes with active substances such as Five basic taste evaluation, Tea, PCA
H. JIANG ET AL.
trioctylmethylammonium chloride,oleic acid and gallic acid, milk,

etc.
[72]
Ag/AgCl reference Seventeen edible mushrooms
electrode Multichannel lipid/polymer membrane electrodes
[70,71]
ISFET,photocurable polyurethane membranes Mineral waters, grape juice HCA,PCA,PLS
[67]
Ag/AgCl reference Evaluate umami taste and different flavor enhancers PCA
Electrode
[67]
Seven different liquid cross-selective sensors (SRS, GPS, STS, Assess umami taste of fish ANOVA, PCA
UMS, SPS, SWS and BRS)
[140]
Seven liquid sensors Quantify glutamic acid and Na+ PCA, CDA, PLS
[68]
Plasticized polyvinylchloride membranes with sensitivity to Astringency quantification CCSWA
organic anions and chalcogenide glass membranes with red/
ox sensitivity
[141]
Three positively charged lipid membranes,three negatively Assess the intensity of the dominant taste attributes of the ANOVA, HSD, PCA
charged lipid membranes juice (bitterness, astringency, and sourness)
[69]
Ag/AgCl reference Compare the intensities and binary interactions of four basic
electrode taste
[62]
Voltammetry Platinum disks with Five taste PCA
electrodeposition layers properties discrimination
(3-methylthiophene, aniline and pyrrole)
[142]
Lipid/polymer membrane electrode Rapid umami PCA,PLS
taste assessment
[62]
Impedance Polypyrrole Water and taste substances PCA
[143]
Polylactic acid, carbon black, polyvinyl alcohol, Standard taste PCA
Etc. Solutions
Note: Acronyms used: PCA, principal component analysis; HCA, hierachical cluster analysis; ANOVA, analysis of variance; HSD, honest significant difference; PLS, partial least squares
regression; CCSWA, common component and specific weight analysis; CDA, canonical discriminant analysis.
Taste masking effect

In food processing, masking agents such as sweeteners and flavoring agents are often
required to mask undesirable flavors in order to make the product palatable.[74]
Traditionally, the only adopted method for sensory evaluation of taste masking effect
is to employ a group of trained tasters to perform sensory analysis. The high expense
of training panels, the difficulty to assess huge amounts of samples, and subjectivity
inherent in human subjects have promoted the development of alternative electronic
methods.
A calibrated e-tongue was successfully used to predict bitterness intensity of binary
mixtures with a sweetener in terms of the different quinine content. The experiment
further proved an e-tongue had the capability of differentiating between formulations with
different levels of sweetener and/or flavor added, and the result was consistent with the
masking effect as perceived by human panelists. [75] As the further development of
e-tongue technique, the application of taste masking effect has also extended into the
optimizing of medicinal products.
Detection of food safety index

Since microbial contamination, food additives, drug residues, food adulteration and other
issues are important factors affecting food safety, food safety indices are the key indicators that
measure whether the sample can reach national or international standards. E-tongues play an
important role in the qualitative and quantitative analysis of food safety index. Since conven-
tional analytical methods such as chromatography and spectrophotometry are limited by the
various disadvantages (e.g., time consuming, high expense, tedious pre-treatment as well as
the impossibility to conduct on-line detection), an e-tongue shows obvious advantages. [76]
Dairy products
Adulteration, doping, drug residues and other issues in dairy products seriously endanger
the health of consumers. E-tongue can quantitatively monitor these situations with low
detection limit and high sensitivity. [77,78] The limits of detection of the hazardous
substance in dairy products measured by e-tongues and conventional analytical methods
are shown in Table 4 and Table 5. Compared to e-tongues, the quantitative methods of
GS-MS, HPLC and liquid chromatography have the advantage of lower detection limits.
Table 4. The limits of detection of dairy products by electronic tongue.

Types Index The lowest detection limits Data-processing algorithm Ref.
[91]
Voltammetry Melamine 0.95mmol/L PCA,HCA
[92]
Melamine 85.0 mg/L f-PCA
[91]
Urea 4.16 mmol/L(249.8 mg/L) PCA,HCA
[92]
Urea 121.4 mg/L f-PCA
[91]
Formaldehyde 10.0 mmol/L PCA,HCA
[99]
Antibiotic MRLs level PCA,DFA
[93]
Potentiometry Urea 2.5 × 10-5 mol/L
Impedance tetracycline 1–300 μg/L PCA [101]
Note: Acronyms used: PCA, principal component analysis; HCA, hierachical cluster analysis; f-PCA, functional principal
component analysis; DFA, discriminant function analysis.
754 H. JIANG ET AL.
Table 5. The limits of detection of dairy products by conventional analytical instruments.

Methods Index Limits of detection Ref.
[81]
mixed-mode solid phase extraction and GC-MS Melamine 0.01 mg/kg
[74]
SB-ATR-Fourier transform infrared spectroscopy Melamine 2.5 ppm
[82]
GC-MS with coupled column separation Melamine 0.01 mg/kg
[83]
HPLC-DAD and HPLC-ESI-MS Melamine 10 mg/kg, 0.5 mg/kg
[85]
HPLC Melamine 0.08 mgl/L
Spectrophotometric and conductometric detection Urea 2.6 × 10–4 [84]
and 2.8 × 10−5 mol/L

[80]
ATR-FTIR spectroscopy Urea 100 ppm
[80]
HPLC Formaldehyde 5 mg/kg
HPLC with post-column derivatization and fluorescence detection Tetracycline 5 ng/mL [79]
Note: Acronyms used: GC-MS, gas chromatography/mass spectrometry; SB-ATR, single bounce attenuated total reflectance;
HPLC-DAD, high performance liquid chromatography-diode array detection; HPLC-ESI-MS, high performance liquid
chromatography-electrospray ionization tandem mass spectrometry;
However, these conventional techniques are generally time consuming, require expensive
instrumentation and a pre-treatment step. In addition, these techniques cannot be min-
iaturized or allow rapid analysis [74,79–85]
Detection of adulteration
Melamine (C3H6N6) and urea (CN2H4O) are illegally added in milk to cause false
appearance of high-protein content.[86] The World Health Organization (WHO) [87]
proposed a limit of 1 mg/kg for milk power and and infant formula to provide a sufficient
margin of safety for young children. Similarly, the allowed amount of urea in milk is
11.547 mmol/L. [88] Food protein content is normally estimated by total nitrogen quanti-
fication using the Kjeldahl method. Since this method cannot distinguish between nitro-
gen from protein and nonprotein sources, compounds as urea or melamine cannot be
detected. [89] E-tongues are relatively easy to operate and enable quantification and
discrimination between samples in a short time. [90]
To carry out the quantitative analysis of adulterants, a VE-tongue employing three
working electrodes composed of platinum, gold, and copper was used for the detection
and discrimination of harmful substances intentionally added to milk. The instrument
extracted the information from cyclic voltammograms recorded in unadulterated and
adulterated milk The extracted data were analyzed using unsupervised pattern recognition
methods (PCA and HCA), and the results showed that minimum concentration of urea
and melamine that can be well distinguished was 4.16 and 0.95 mmol/L, respectively.[91]
Hilding-Ohlsson et al. [92]proposed a VE-tongue employing a standard three electrode
system including Ag/AgCl reference electrode, a stainless steel helicoidally electrode as
counter electrode, and Au working electrode to detect melamine and urea adulteration in
milk. The voltammetric data and their first derivative were subjected to functional
principal component analysis (f-PCA) and correctly classified by the KNN classifier. The
results showed that the limits of detection in milk samples adulterated with urea and
melamine were 121.4 mg/L (2 mmol/L) and 85 mg/L(0.7 mmol/L), respectively. To
decrease the limits of detection, Trivedi et al. [93] invented a potentiometric urea sensitive
biosensor, employing a NH4+ ion sensitive electrode in double matrix membrane (DMM)
technology as the transducer, presenting a detection limit of 2.5 × 10−5 mol/L for urea.
The urea biosensor had been developed by immobilizing the urease enzyme onto the ion-
sensitive membrane using a polymer matrix of poly (carbamoylsulphonate) (PCS) and
polyethyleneimine (PEI). The biosensor responded rapidly and in a stable manner to the
changes of urea concentrations.
To complete the qualitative analysis of discrimination between milk adulterated with
urea and pure milk, another method using a VE-tongue based on multi-way principal
component analysis (MPCA) and multi-way partial least squares discriminant analysis
(NPLS-DA) was developed. The NPLS-DA model was developed using the first five PCs
according to the distribution of PCs computed by MPCA, and the correct classification
rate for calibration set and prediction set were 100% and 88.9%, respectively. [94]
The VE-tongue is usually used to classify adulterated milk samples for two reasons.
One reason is passivation of the electrode surface by adulterant, and the other is that
different addition of urea or melamine will change the conductivity of samples accord-
ingly. [95] However, voltammetric sensors generate numerous data that make their analysis
extremely difficult. To avoid redundancy in input data and to obtain better discrimination
ability, more applicable pattern recognition methods should be developed.
Detection of drug residues

Adding formaldehyde into milk can extend the shelf life of the product. The standard
contents of formaldehyde in fresh milk and commercial milk products are no more than
0.027 mg/kg and 0.164 mg/kg, respectively. [96]
With the purpose of detecting and discriminating the different levels of formaldehyde, a
special VE-tongue was fabricated that was equipped with three working electrodes including
custom-made copper, commercial gold and platinum electrodes, an Ag/AgCl reference
electrode, and an auxiliary electrode made of platinum or gold wire. The three working
electrodes were polished using an alumina suspension (1 µm, Alfa Aesar, MA, USA) with a
microcloth polishing pad. The result of PCA and HCA showed that detection limit of
adulterant that induced an apparent discrimination was 10.0 mmol/L for formaldehyde.[91]
Antibiotic residues result from the improper medication of lactating dairy cows or inade-
quate time to stop collecting milk after treatment, especially the cow conducting breast
perfusion in the treatment of mastitis.[97] The Council Regulation (EC) regulates the max-
imum levels of antibiotic residues (maximum residue limits (MRLs)) in dairy products. [98]
Tan et al. [97] used the self-developed VE-tongue combined with PLS analysis to
recognize the different types of antibiotics (chlortetracycline, spectinomycin, erythromy-
cin, lincomycin, neomycin, and gentamicin) and the different concentration of neomycin.
The e-tongue employed working electrodes made of Pt, Au, Pd, Wu, Ti and Ag electrode,
a Ag/AgCl reference electrode, and a Pt auxiliary electrode. The optimum detection range
of neomycin was in the range of 300–1100 μg/L. In another study, a VE-tongue combined
with PCA and DFA was developed to detect six antibiotics (Chloramphenicol,
Erythromycin, Kanamycin sulfate, Neomycin sulfate, Streptomycin sulfate, and
Tetracycline HCl) spiked at four different concentration levels (0.5, 1, 1.5, and 2 MRLs)
in bovine milk. At the MRLs, the six antibiotics could not be completely separated from
bovine milk using PCA, but were clearly demarcated by DFA.[99]
Nanomaterial science greatly contributes to the development of novel and portable chemical
sensors in the application of food industry, because the high specific surface area and large
porosity make electrospun nanofibers attractive to design ultrasensitive sensors.[100] To further
obtain more accurate detection limits, an impedimetric e-tongue based on gold interdigitated
microelectrodes (IDEs) modified with polyamide 6/polyaniline electrospun nanofibers was
756 H. JIANG ET AL.
developed to detect tetracycline (TC) residue in whole and skimmed milk samples. After
analyzing the electrical resistance data collected by the e-tongue with PCA analysis, the
e-tongue was able to identify the presence of tetracycline residues (from 1 to 300 ppb) in
these samples. The results obtained demonstrate the ability of the approach of modifying IDEs
with conducting electrospun nanofibers to be used as sensing units in the e-tongue, aiming to
analyze complex matrices such as milk without any prior pre-treatment. [101]
Detection of freshness
A VE-tongue composed of four working electrodes (e.g., gold, silver, platinum, and
palladium electrode) was developed to monitor the quality and shelf life of unsealed
pasteurized milk. PCA and HCA results indicated that the e-tongue based on multi-
frequency rectangle pulse voltammetry (MRPV) and multi-frequencey staircase pulse
voltammetry (MSPV) could differentiate between the milk samples of different storage
time. Since the mathematic model based on partial least squares regression (PLSR) and
least squares-support vector machines (LS-SVM) successfully predicted the total bacterial
count and viscosity of milk, e-tongue can effectively predict the biochemical and microbial
indicators of food deterioration, achieving the purpose of monitoring freshness.[102]
Meat products
The detection limits of safety indices in meat products and aquatic products are shown
in Table 6.
Key factors affecting the freshness of meat products include volatile basic nitrogen (TVB-N),
total viable count (TVC), nitrite residual, and trimethylamine (TMA). Traditional methods
of microbial detection include plate pouring method, plate coating method, and spiral
inoculation method, but these methods have the disadvantages of being complex and
time-consuming operations as well as requiring related professional knowledge. The e-ton-
gue system enables the rapid assessment of freshness by detecting the changes of taste
substances in the sample or sample solution.[103]
A rapid, nondestructive technique based on the e-tongue system composed of seven
working electrodes was applied to analyze the fingerprint of the electrochemical com-
pounds of three types of minced meat samples (e.g., sheep, goat, and beef), and a support
vector machines (SVM) trained classifier gave perfect discrimination among these three
kinds of meats. [104]
During the process of monitoring the freshness of beef, researchers developed amine-
sensitive voltammetric sensors based on screen-printed electrodes modified with polypyrrole
Table 6. The limits of detection of meat and aquatic products by electronic tongue.
Types Index The lowest detection limits Data-processing algorithm Ref.
Voltammetry Ammonia 1.85 μmol/L PCA, PLS-DA, ANOVA [105]
Putrescine 0.34 μmol/L [105]
Trimethylamine 1.58 × 10−5 mol/L PCA, PLS-DA [114]

[109]
Potentiometry TVC RMSEP was 0.73 log CFU/g
Note: Acronyms used: PCA, principal component analysis; PLS-DA, Partial Least Squares-Discriminant Analysis; ANOVA, one-
way analysis of variance
and bisphthalocyanine. The limits of detection for ammonia and putrescine were 1.85 μmol/
L and 0.34 μmol/L, respectively. [105]
Gil et al. [106] monitored the changes of physico-chemical parameters and microbiolo-
gical indices of fresh pork during cold storage with PCA and artificial neural network,
using the potential e-tongue comprised of six working electrodes (e.g., gold, copper, silver,
lead, zinc, and carbon). Through the use of PLS analysis, a rather good correlation was
found between pH and the potentiometric data. Also, a remarkable correlation was
observed between the measures carried out with the e-tongue and the so-called K-index
that simultaneously measures the variation in the adenosine triphosphate (ATP) degrada-
tion products. The results of PLS prediction models suggest an e-tongue can contribute to
the qualitative or semi-quantitative analysis of meat freshness.
Detection of additives
NaCl, nitrites, and nitrate are often used in the processing of meat products to preserve
meat and protect color. Labrador et al. [107] used a combination e-tongue based on pulse
voltammetry and electrochemical impedance spectroscopy measurements to detect the
concentration of NaCl, nitrites, and sodium chloride. The data management and predic-
tion models based on cross-validation and PLS techniques showed that predicting accu-
racy for the concentration of chloride was high, whereas for nitrate and nitrite it was
considered as moderate. The main advantages of the proposed measuring systems are the
possibility of online measurements, fast and nondestructive methodology, and possibility
of creating portable devices to be used in the processing step.
Based on the above study, Campo et al.[108] used a VE-tongue composed of a group of
noble metal electrodes and a set of common metal electrodes to measure the salt content in
salt water and minced meat. PLS regression analyzed the true concentration of the three
salts and the results showed that there was a good correlation between the two parameters in
the salt water and meat sample; however, the interaction between the complex components
in the minced meat led to a poorer prediction. These studies suggest that the detection of
levels of salt (chloride, nitrate and nitrite) in real, complex samples could be performed via
measurement of the electro-chemical response of a simple set of metallic electrodes, and
such e-tongue device may allow the design of fast and nondestructive methodologies.
Aquatic products
During fish spoilage, the increasing microbial flora will cause serious problems to human health
and food economic value. The detection limit for TVC in food quality testing is 106 cfu/g. The
TVB-N limit of marine fish is 30 mg/100 g, and the TVB-N limit of freshwater fish is 20 mg/
100 g. Above the limit means the requirement is not met. Han et al. [109] used a potentiometric
e-tongue coupled with linear and nonlinear multivariate algorithms to match fish freshness
measured by chemical and microbiological tests (TVC and TVB-N). Fisher LDA and SVM were
applied comparatively to classify the samples stored at different days. The results revealed that
SVM model was better than Fisher LDA model with a higher identification rate of 97.22% in the
prediction set. PLS and SVR were applied comparatively to predict the TVB-N and TVC values.
The models were evaluated by RMSEP and the correlation coefficient in the prediction set
(Rpre). The results revealed that SVR model was superior to PLS model with RMSEP = 5.65 mg/
758 H. JIANG ET AL.
100 g, Rpre = 0.9491 for TVB-N prediction and RMSEP = 0.73 log CFU/g, Rpre = 0.904 for TVC
prediction. This study demonstrated that the e-tongue combined with SVM and SVR has a great
potential for a convenient detection of fish freshness. To build quantitative evaluation models
for fish safety analysis, Han et al.[110] compared three kinds of models, the PLSR, support vector
regression (SVR) and back propagation neural network (BP-NN), to predict the TVC value on
the basis of above study. The BP-NN model showed superior performance with correlation
coefficient and RMSEP of 0.993 and 0.211 logCFU/g, respectively.
In addition, based on the principle of VE-tongue, the difference among 11 kinds of
pathogenic vibrios was studied using different electrode arrays combined with PCA. The
results showed that the 1 Hz frequency segment of the tungsten electrode had the ability to
separate the 11 species of pathogenic vibrios, and the combination of 100 Hz of the silver
electrode and 10 Hz of the tungsten electrode can also discriminate 11 pathogenic vibrios
in the map of principal component analysis. [111]
Amines play an important role in the degradation pathways of amino acids in biological
systems, so the measurement of amines can provide important information about fish
freshness. [112] Voltammetric sensors chemically modified with electroactive materials can
be used for global detection of amines because they are sensitive to the presence of both ions
and electroactive substances. [32] Rodríguez et al. [113] used a VE-tongue modified with
phthalocyanine to determine the content of biogenic amines in fish to deduce fish freshness.
With the purpose of further evaluating the detection limits of biogenic amine compounds, an
innovative e-tongue composed of polypyrrole-modified electrodes doped with several doping
agents was developed, recording the change of voltammetric measurements in solutions with
the increasing amine concentrations to get a calibration curve. The PCA and PLS-DA analysis
showed that the detection limit for trimethylamine was 1.58 × 10−5 mol/L This study showed
that e-tongue could be effectively applied in the analysis of fish freshness as well as the
determination of postmortem time elapse. [114]
As for the evaluation of shelf life of aquatic products, Ruizrico et al. [115]used a VE-tongue to
distinguish between fresh cod (storage days≤1) and spoiled cod (storage days≥4) in cold storage
(4οC). The classification results were in accordance with those measured by the physico-
chemical and microbial methods (moisture content, TVBN, and ATP-related compounds).
This study described the possibility of a VE-tongue to be used as a rapid and nondestructive
method applicable to routine quality control at any stage of the supply chain. As for the
evaluation for fish in frozen storage, an alpha-astree potentiometric electronic tongue combined
with PCA and DFA showed that silver carp samples could be distinguished effectively in
different storage periods. The main signal strength of silver carp freshness difference came
from the sensor JB, HA, GA, and the DFA method was more effective than PCA. [116]
Various sensor technologies have been developed to address the drawbacks of the conven-
tional methods for fish freshness evaluation. Since electronic tongue coupled with linear and
nonlinear multivariate algorithms can quantitatively measure TVC, TVBN, and amines, it has
potential for a convenient and comprehensive detection of fish freshness.
Fruits & vegetables and their processed products

Detection of freshness and maturity
Fruit with great flavor and highly desirable taste is consumed in large quantities, either fresh or
as fruit juice. The harvesting date indicators of fruits are determined by parameters such as berry
weight, must density, and the relation between sugar content and total acidity. A VE-tongue
consisting of eight metallic electrodes housed inside a stainless steel cylinder was used as a tool to
monitor grape ripeness in juice. The PCA models that were obtained from the physico-chemical
or electrochemical data showed variation of ripeness with time, and PLS regression was applied
to establish a correlation between the data collected from the e-tongue and total acidity, pH, and
°Brix values. These results suggested the possibility of employing electronic tongues to monitor
grape ripeness and then to evaluate the right time for harvesting. [117]
The freshness and maturity of fresh fruit are affected by storage conditions including
shelf life, storage temperature, waxing, and so on. An e-nose and e-tongue combined with
two-way multivariate analysis of variance (MANOVA) have been used to investigate the
impacts of storage temperature and time on internal quality of citrus (vitamin C, total
soluble solid, and total acid). The e-nose showed a better performance than e-tongue for
the identification of storage condition, and e-nose based on random forest (RF) algorithm
achieved better prediction performance than e-tongue. However, compared with a single
system, the predicting accuracy of a fusion system was higher. This work indicated that
the fusion system composed of e-nose and e-tongue could be used as a rapid and objective
method applicable to routine quality control at any stage of the fruit supply chain. [118]
The procedure of processing fruits into juices makes it hard to identify the freshness of
raw materials. Traditionally, the quality detection methods for fruit juice fall primarily in
four types: instrumental analysis (e.g., GC-MS, texture analyzer, and scanning electron
microscopy),[119] chemical analytical method (e.g., pH, total acidity, and soluble solid),[120]
microbiology testing, and sometimes sensory evaluation. The first three conventional
techniques appear to have some drawbacks: laborious and time-consuming sample pre-
paration, requirements for skilled personnel to operate analytical instruments, and the
final information usually being partial. Sensory evaluation by human is associated with
problems such as the standardization of scoring, the stability and the reproducibility of the
evaluation. E-nose and e-tongue are rapid analytical systems that provide global informa-
tion about the sample instead of information on particular components. [121] Several
studies have proven that the combination of e-nose and e-tongue are effective alternatives
for traditional methods in the analysis of juice freshness. [122–124]
For example, Hong[122] employed e-tongue and e-nose system combined with canonical
discriminant analysis (CDA) and library support vector machines (Lib-SVM) to realize the
discrimination of 100% juices squeezed from cherry tomatoes at different post-harvest
storage time. Tracking and prediction of physicochemical qualities (pH, soluble solids
content (SSC), Vitamin C (VC), and firmness) of the fruit were performed using principle
components regression (PCR). Though quality regression models trained by either e-nose
or e-tongue dataset were not robust enough, the fusion system made it possible to build
more robust prediction models. This study indicates the potential for tracking quality/
freshness of fruit squeezed for juice consumption using the e-nose and e-tongue system,
and that sensor fusion approach would be better than individual utilization only if proper
fusion approaches are used.
Detection of adulteration
Traditional methods to identify juice authenticity such as HPLC, GC, or sensory methods
cost too much time and require well-trained personnel. An e-tongue can be successfully
applied in the identification of different varieties of apples, citrus,[125]and apple
760 H. JIANG ET AL.
juice.[126,127] To further improve the discrimination ability towards fruit juice, e-nose-e-
tongue technology combined with PCA, CA analysis, and fuzzy artmap neural network
(FAMNN) was employed to identify 11 kinds of different flavors of fruit juice.These 11
different flavors were produced by six kinds of fruit (mango, pear, apple, orange, pine-
apple, and multivitamins) with different fruit content varying from 15% to 50%.[128]
In recent years, several papers have been published dealing with cherry tomato juice
adulteration by applying e-nose measurements, e-tongue measurements, and some fusion
approaches. These studies clearly point out that e-tongues combined with principle
component analysis, cluster analysis, and regression methods can be utilized as efficient
tools to classify juice according to their juice contents. [129,130]
Miniaturization of electronic tongue

Most electronic tongue systems reported now for food quality detection are laboratory
versions that are equipped with large-sized sensors and data collection equipment, and this
situation limits the application of e-tongue in daily use for consumers.[131] Since small-sized
detecting instruments bring remarkable improvements in convenience and a dramatic reduc-
tion of sample consumption, a hot area of research has been the realization of miniaturized
electronic tongue. Sensor miniaturization of e-tongue can be realized by two possible
approaches: to miniaturize single sensors, or to develop integrated sensor arrays. [132]
The miniaturization of the potentiometric sensors and the design of solid-state electro-
des are connected with the elimination of the internal electrolyte or the immobilization of
this solution on planar electrode structure.[133] Ciosek and Wroblewski [134]developed an
e-tongue based on miniaturized solid-state potentiometric sensors to discriminate between
different brands of beer. The membrane solution casting on the surface of the planar Au
transducers was applied for the preparation of classical ion-selective and partially selective
microelectrodes. 69.7% of corrected classifications were obtained using PLS regression,
however the combination of PLS and ANN analysis enabled the correctness of the
recognition of beer to 83%. This study indicates that miniaturized electronic tongue
systems based on the proper choice of solid-state polymer membrane sensors can be
developed for the quality control in foodstuff industry.
Silicon technology [135] and thin-film techniques including electron beam (e-beam)
evaporation, thermal vacuum deposition, and pulsed laser deposition can be used in the
development of sensor arrays.[136] Winquist et al. [137] made a miniaturized VE-tongue by
inserting three types of wires functioning as working electrodes (gold, platinum, and
rhodium; diameter 0.25 mm) into a counter electrode made of a platinum tube (diameter
2 mm; length 4 mm). The simple setup was connected to a potentiostat controlled by a
computer, and was quite convenient without a reference electrode.
Verrelli et al. [135] realized the integration of potentiometric sensors combined with
silicon technology that allows the construction of micro-sized sensors with different
geometries in deposition area. The developed sensors were firstly tested toward the
detection of membrane selectivity performances, and then applied for the identification
of wine polluting agents such as SO2, H2S, and acetic acid. The developed e-tongue system
showed good responses in solutions containing different ions, and it was able to distin-
guish these polluting agents in a concentration range from 10–6 to 10–1 mol/L.
Another miniaturized potentiometric electronic tongue combined with PLS-DA analy-

sis exhibited perfect classification abilities toward milks originating from various diaries.
This e-tongue was equipped with integrated array of microelectrodes made from epoxy-
glass laminate and PVC membranes functioning as chemosensitive layers. Moreover, the
comparison of milk classification results obtained with the use of commercial Ag/AgCl
electrode and miniaturized reference electrode based on ionic liquid (1-dodecyl-3-methyl-
imidazolium chloride) showed that it is possible to integrate the miniature reference
electrode with ion-selective electrodes on the same substrate, which can be advantageous
for future constructions. [138]
Giménezgómez et al. [139] fabricated a portable e-tongue to classify 78 cava wine
samples according to the ageing time. The array of microsensors was formed by one
conductivity sensor, one redox potential (ORP) sensor, and two amperometric gold
microelectrodes, which were measured with the multisensor meter. The sensors based
on a platinum four-electrode configuration were employed as the conductivity sensors and
ORP sensors. Two conventional thin-film gold electrodes, which were fabricated with
standard photolithographic techniques, were employed to perform chronoamperometric
measurements. The amperometric cell contained the working electrode, a platinum
electrode as a counter electrode, and an Ag/AgCl/10% (w/v) KNO3 reference electrode.
The size of the system was 21 cm×10 cm×3 cm. [139]
Compared to the technology of miniaturizing single sensors, the methods to realize
integration of sensor arrays seem more effective. As e-tongue is suitable for nonexpert
users and applicable to detect the quality of various fresh foods in daily life, new
fabrication technology is necessary to decrease its bulky size.
Concluding remarks
e-tongue is emerging as a promising supplemental technique to conventional analytical
methods due to its high sensitivity, rapid testing speed and low detection limit of food
sensory and safety index. This paper has presented the main application of electronic tongue
in fresh food field including discrimination between basic taste properties, taste masking
effect, detection of adulteration and drug residue, evaluation of freshness and storage time,
and food processing monitoring. The foods mentioned in this review vary widely, including
dairy products, meat products, aquatic products, and fruit and vegetables.
Electronic tongues combined with other detection technologies can be used for more
accurate monitoring and optimization of the production process. As the volume of
e-tongues limits the promotion in daily usage, different types of sensors can be combined
to create a common small portable electronic tongue in the future. A portable electronic
tongue may have broad application in the food industry.
Funding
This work was financially supported by China Key Research Programs (Contracts No.
2017YFD0400901 and No. 2017YFD0400501), Jiangsu Province (China) Agricultural Innovation
Project(Contract No. CX(17)2017), Jiangsu Province (China) Key Project in Agriculture (Contract
No. BE2016362), and Jiangsu Province (China) Infrastructure Project (Contract No. BM2014051).
762 H. JIANG ET AL.
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FOOD REVIEWS INTERNATIONAL

2018, VOL. 34, NO. 8, 746–769

Application of electronic tongue for fresh foods quality

signal Pattern recognition

Figure 1. Schematic diagram of basic structural components of an electronic tongue.

environmental monitoring,[6,7] fermentation monitoring,[8,9] and horticultural technique. [10]

Common types and working principals of electronic tongue

Potentiometry-based electronic tongue

Voltammetry-based electronic tongue

Impedance spectroscopy-based electronic tongue

composed of several ultrathin membranes made from diﬀerent materials deposited on

Pattern recognition methods

Detection of food sensory index

Detection of basic taste

Table 1. Sensors of the Insent taste sensing system TS-5000Z.

Table 3. Application of electronic tongue in taste assessment.

trioctylmethylammonium chloride,oleic acid and gallic acid, milk,

Taste masking eﬀect

Detection of food safety index

Table 4. The limits of detection of dairy products by electronic tongue.

Table 5. The limits of detection of dairy products by conventional analytical instruments.

and 2.8 × 10−5 mol/L

Detection of drug residues

Putrescine 0.34 μmol/L [105]

Trimethylamine 1.58 × 10−5 mol/L PCA, PLS-DA [114]

Fruits & vegetables and their processed products

Miniaturization of electronic tongue

Another miniaturized potentiometric electronic tongue combined with PLS-DA analy-

[137] Fredrik Winquist, C.K.R.; Lundström, I. A Miniaturized Voltammetric Electronic Tongue.

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