sensors

Article
Sugar Concentration Measurement System Using
Radiofrequency Sensor
Gerardo Aguila Rodriguez 1 , Nayda Patricia Arias Duque 2 ,
Blanca Estela Gonzalez Sanchez 1 , Oscar Osvaldo Sandoval Gonzalez 1 ,
Oscar Hernan Giraldo Osorio 3 , Citlalli Jessica Trujillo Romero 4 ,
Miriam Andrea Wilches Torres 2 and Jose de Jesus Agustin Flores Cuautle 5, *
1 Tecnológico Nacional de México/I.T. Orizaba, Oriente 9, Emiliano Zapata, 94320 Orizaba, VZ, Mexico;
gerardo_aguila03@yahoo.com.mx (G.A.R.); bgonzalez@ito-depi.edu.mx (B.E.G.S.);
o.sandovalgonzalez@gmail.com (O.O.S.G.)
2 Universidad de Boyacá, Facultad de Ciencias e Ingeniería, Carrera 2ª Este No. 64–169, 15001 Tunja, Boyacá,
Colombia; npariasd@gmail.com (N.P.A.D.); andreawilches@uniboyaca.edu.co (M.A.W.T.)
3 Departamento de Física y Química, Universidad Nacional de Colombia sede Manizales, Cra. 27 N.◦ 64-60,
17001 Manizales, Colombia; ohgiraldoo@unal.edu.co
4 División de investigación en Ingeniería Médica, Instituto Nacional de Rehabilitación-LGII., 14389 Mexico
City, Mexico; cjtrujillo@inr.gob.mx
5 CONACYT-Tecnológico Nacional de México/I.T. Orizaba, Oriente 9, Emiliano Zapata, 94320 Orizaba,
VZ, Mexico
* Correspondence: jflores_cuautle@hotmail.com




Received: 27 March 2019; Accepted: 17 May 2019; Published: 22 May 2019


Abstract: A sugar solution measurement system was developed based on the dielectric properties
of the sucrose molecule. An ac conductivity and tan δ study as a function of the frequency was
performed to find the suitable frequency range for the measuring system. The results indicate that it
is possible to obtain a better response of the sensor using the frequencies as the maxima peak in tan δ
appears. Developed setup for sucrose solution was appropriate to measure in a 0.15 to 1 g/mL range
with an experimental error of about 3%. The proposed system improves the measurement time over
some other methods.

Keywords: sucrose; electromagnetic field; sugar concentration

1. Introduction
Natural sugar (sucrose, α-D-glucopyranosyl β-D-fructofuranoside) is a disaccharide which
contains glucose and fructose joined together by an oxygen bridge; its structure is determined
principally by the hydrogen bonds O-H . . . H [1]. Sucrose is synthesized by plants and can be
assimilated by animals providing an energy source. Sucrose metabolism involves signaling of glucose
and fructose [2]. In cellular metabolism, the glucose plays a role in energy production through
glycolysis reaction involved in the cell respiration into the mitochondria. As it is known, the glycolysis
intermediary pathways involve pyruvate formation, the Krebbs cycle and the release of electrons and
protons to produce adenosine triphosphate (ATP) in ATP-synthase [3]. Additionally, some other sugars
can be assimilated in the human body, as the case of sucrose and fructose, but they are accumulated in
the liver waiting for a drastic decrease in glucose before release [4].
Recently, blood glucose had become one of the leading parameters to take into account as a health
indicator. Several reasons led to blood glucose to become so important; raised blood glucose is an
indicator of diabetes mellitus, which in turn, can lead to several health risks. Recent evidence suggests a
relationship between frequent consumption of sugar-sweetened beverages as a more significant risk of

Sensors 2019, 19, 2354; doi:10.3390/s19102354 www.mdpi.com/journal/sensors

Sensors 2019, 19, 2354 2 of 12

type 2 diabetes [5], sugar consumption is responsible also for weight gain, glycemic load and pancreatic
cancer risk [5–8]. The U.S. Center for Disease Control and Prevention recommends the reduction of
sugar-sweetened beverages consumption in order to prevent and reduce obesity [9]. Nowadays, the
role of sugar-sweetened beverages became more critical than in the past; therefore, governments are
handling this problem in their legislations [10–12]. As part of the efforts to tackle this problem, it is
necessary to research practical ways to measure small variations in sugar concentration in solutions,
such as in beverages [13,14]. In this sense, several methods to measure sugar concentrations have been
developed, namely chromatographic, optical, thermal and radio frequency (RF) methods [14–17].
Among optical methods, different systems to measure sugar concentration are already available;
however, the most important are the polarimeter and the refractometer. In those methods, the
measurement is as follows: First, a calculation of the light rotation degree is done over the interest
substance by using a 1.000 ± 0.002 g/mL sample concentration; this measure is used as a reference.
The sample concentration (p) can be calculated using Equation (1). Those methods are based on light
polarization. Therefore, its use in an industrial environment or those liquids with high absorption
coefficient is not thoroughly recommended.
α
αD = , (1)
pl

where α is the observed rotation (◦ ), p sample concentration (g/mL), l sample volume (dL), and αD is
the specific rotation.
Thermal properties have also been used to measure the glucose concentration with high resolution,
photothermal methods like infrared (IR) spectroscopy, deflectometry, and photopyroelectric method are
used for getting glucose thermal parameters, even though the required time to perform measurements
can reach up to hours, and the sample temperature stability is crucial in these kind of measurements.
Table 1 shows a comparison among some methods used for measuring glucose concentration [18–20].

Table 1. Glucose concentration measurement methods.

Range Sensitivity Working

Method Ref.
(g/mL) (g/mL) Frequency
Electromagnetic 0.78–6.25 0.3 40 kHz [15]
Near-infrared Raman
1.8–21.62 0.65 - [17]
spectroscopy
Photopyroelectric 1.3–3.1 0.3 1–100 Hz [18]
Photothermal radiometry 0.21–4.0 0.37 - [19]
Reflected terahertz
5 × 10−4 –2 × 10−3 - THz [20]
radiation
Terahertz time-domain
7.5 × 102 –1.1 × 103 - THz [21]
spectroscopy
Attenuated total
5 × 10−3 –4.3 × 10−1 - THz [22]
reflectance terahertz
This work 0.15–1 0.05 10 kHz

On the other hand, it is known that the RF can affect polar organic molecules. This effect depends
on the electromagnetic properties of the molecule under study, RF wavelength, sample size, geometry
and orientation respect to the radiation, among others. By choosing a suitable RF frequency range, the
interaction between the polar molecule and the RF field becomes detectable. Therefore, it is possible to
obtain information regarding sample electromagnetic properties and concentration [15,23,24].
In this paper, an RF measurement system is proposed for measuring sucrose concentration. The
RF measurement system is based on the dielectric properties of sucrose. Because the sucrose molecule
is a polar molecule and it is susceptible to react to the electromagnetic fields, it was possible to
measure its concentration. The advantage of using RF as a sensing method is contactless; therefore,
sample contamination is avoided. There are available studies using a variation of RF technique for
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determining glucose concentration [20–22]. With frequencies in the THz domain, these techniques
of Fourier-transform
have infrared samples
the capability of measuring (FT-IR),in THz
the 5 ×time-domain
10−4 up to 2 ×spectroscopy
10−3 g/mL; as (THz-TDS),
the drawback,and the
the use
knowledge
of of independent
Fourier-transform infraredmeasurement
(FT-IR), THz of other components
time-domain are necessary.
spectroscopy (THz-TDS), and the knowledge
of independent measurement of other components are necessary.
2. Materials and Methods
2. Materials and Methods
2.1. Sample Preparation
2.1. Sample Preparation
Sucrose (Merck 99%, Darmstadt, Germany) and distilled deionized water were used. An
Sucrose quantity
appropriate (Merckof99%,sucroseDarmstadt,
was added to Germany) and
the distilled distilled
water deionized water
to give concentrations rangedwere
fromused.
0.010
An appropriate
± 0.002 g/mL toquantity of sucrose
1.000 ± 0.002 g/mLwas withadded
0.010to the distilled
± 0.002 water A
g/mL steps. to magnetic
give concentrations
stirrer wasranged from
used for 10
0.010
min to ± 0.002
ensureg/mL to 1.000
a total ± 0.002 All
dissolution. g/mLsamples were±prepared
with 0.010 0.002 g/mLandsteps. A magnetic
measured stirrer was used
at a temperature of 25
for
°C.10 min toand
Before ensure
aftera each
total dissolution.
measurement, Allthe
samples
sample were prepared
holder and measured
was washed at a temperature
using distilled water and of
25 ◦ C. Before and after each measurement, the sample holder was washed using distilled water and
dried with air to avoid measurement errors associated with additional sample dilution.
driedAfter
with air to avoid
solution measurement
preparation, errors
a total associated
of 100 differentwith additional
samples of sugarsample dilution.
solution were measured by
After solution
impedance preparation,
spectroscopy and 50 asamples
total of for
100radio
different samples
frequency of sensor
(RF) sugar solution were measured by
measurements.
impedance spectroscopy and 50 samples for radio frequency (RF) sensor measurements.
2.2. Sample Concentration Cross-Validation
2.2. Sample Concentration Cross-Validation
Nicolet iS5 UV-VIS spectrometer (Thermo Scientific™ Waltham, MA, USA) was used to ensure
Nicolet iS5 UV-VIS spectrometer
the correct concentration (Thermo
of sugar solution usedScientific™ Waltham,
in this study, and a MA, USA) was
calibration curveused
wastodetermined
ensure the
correct concentration of sugar solution used in this study, and a calibration
using standard samples. The absorbance lectures were recorded at 197 nm. Figure 1 showscurve was determined using
the
standard
obtained samples. The
results; the absorbance
obtained lectures
equation waswere recorded
y = 1.934 at 197where
+ 0.175X, nm. Figure 1 shows the
y is absorbance andobtained
X is the
results; the obtained
concentration equation was y = 1.934 + 0.175X, where y is absorbance and X is the concentration
in g/mL.
in g/mL.

2.30

2.25

2.20

2.15
absorbance (a.u.)

2.10

2.05

2.00

1.95

1.90
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
sugar solution concentration (g/mL)

Figure 1. Calibration curve for sucrose solutions; squares represent the experimental data, and the
Figure 1. Calibration curve for sucrose solutions; squares represent the experimental data, and the
solid line is used as a reference for the eye.
solid line is used as a reference for the eye.
2.3. Alternating Current (ac) Conductivity and Loss Tangent (Tand δ) Measurements.
2.3. Alternating Current (ac) Conductivity and Loss Tangent (Tand δ) Measurements.
The complex conductivity is a nondestructive method to elucidate the charge carriers and the
The mechanism.
transport complex conductivity
The complexis aconductivity
nondestructive
canmethod to elucidate
be represented as the charge carriers and the
transport mechanism. The complex conductivity can be represented as
σ𝜎∗ ∗== σ0𝜎+ 00
’ jσ ´´
+ 𝑗𝜎 (2)
(2)
whereσσ´
where 0 is
isthe
thereal
realcomponent andσ”
componentand σ´´isisthe
theimaginary
imaginarycomponent
componentofofthe
theconductivity.
conductivity.
The real component of the conductivity as a function of frequency can generally be described as
frequency-independent conductivity (σdc), and a strongly frequency-dependent components (𝐴𝜔 ). In
this sense, Jonscher describes the real component of the conductivity by the following equation
Sensors 2019, 19, 2354 4 of 12

The real component of the conductivity as a function of frequency can generally be described as
frequency-independent conductivity (σdc ), and a strongly frequency-dependent components (Aωs ).
In this sense, Jonscher describes the real component of the conductivity by the following equation

σ0 = σdc + Aωs , (3)

where σdc is a dc conductivity, A is a pre-exponential term, ω = 2πf is the angular frequency, and s is
the “power law” exponent, 0 < s < 1 [25]. Therefore, it is possible to identify the species that interacts
with the electromagnetic field.
The experimental value of the real component of the complex conductivity can be extracted from
impedance following Equation (4)

d −Z00
σ0 = ( ) (4)
A (Z0 )2 + (Z00 )2

where Z0 and Z” are the real and imaginary component of the complex impedance, respectively.
On the other hand, other relevant parameters to study in this system are the loss tangent (tan δ)
and the relaxation time (τ). The loss tangent is correlated to the energy absorption by the condensed
matter [25] and is described by Equation (5)

ε00 Z00
tan δ = = 0 (5)
ε 0 Z
The relaxation time (τ), describes the time between the state in which molecules undergo a
rotational diffusion as it is oriented in the direction of the electromagnetic field, and its state to return
to the equilibrium position [26]. On the other hand, relaxation time gives us information regarding the
frequency at which the response of the interest molecule is higher over the study frequency range.
This parameter can be extracted from the frequency in which the maxima peak in tan δ occurs
through the following Equation (6):
1
τ= (6)
2π f
where f is frequency in Hz and τ is in seconds
In this study, the range of concentration of tested sugar solution was 0.000–1.000 ± 0.002 g/mL
in steps of 0.100 ± 0.002 g/mL. A total of 100 samples were tested using 5.000 ± 0.002 mL of sucrose
solution and submitted to electrical analysis in a SOLARTRON 1260 coupled with a dielectric interphase
SOLARTRON 1296A with the 12964 A cell sample holder (Solartron Analytical, Farnborough, UK.). The
distance between the reference to the working electrode was about 50 ± 0.001 mm. The measurements
were made by duplicate at 100 mV root mean square (RMS) amplitude and between frequencies from
10 MHz to 0.1 Hz. The experiments were performed from high to low frequency to avoid overloading
of the equipment and to preserve the sample from possible Joule effect at low frequency. With the
experimental data of impedance, conductivity and loss tangent were obtained.

2.4. Sensor
The sensor was handmade using a 5-mm-diameter glass pipe, and two coupled coils separated
10 mm from each other. Those coils are the base of an oscillator; following this principle, and due to
the polar properties of the sucrose molecule, the dielectric properties of a medium between the two
coils change, and as a consequence, resonant frequency changes as sucrose concentration function.
A constant distance (d in Figure 2) between sensing coils was obtained by fixing them to the
sample container as Figure 2 shows. The frequency range was chosen to obtain a maximum response
from the designed sensor. Therefore, a study of the sample electrical conductivity was made.
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Figure 2. The sensing coils arrangement with the sample container.

For designing Figure 2. The sensing

the sensors, there is coils arrangement with thethe
a relationship sample container.
Figure 2. The sensing coils arrangementbetween sensor
with the sample impedance and the sensing
container.
system electronics, the sensor impedance can change in a wide range provided the electronics is
Fordesigning
For designingthe thesensors,
sensors,there
thereisisaarelationship
relationshipbetween
betweenthethesensor
sensorimpedance
impedanceandandthethesensing
sensing
tuned for working in the 1 kHz–10 kHz frequency range. The coils configuration shown in Figure 2,
system
system electronics,
electronics, the sensor
the sensor impedance
impedance can change
can change in a wide range
in a wide range provided the electronics is tuned
is named as the loosely couple coils; under this configuration, only provided
a fractionthe electronics
of the transmittedis
for working
tuned for in the 1inkHz–10
working the 1 kHz frequency
kHz–10 kHz range. The
frequency range.coils
Theconfiguration
coils shown inshown
configuration Figurein2,Figure
is named2,
electromagnetic flux is captured in the receiver, and the transmitted electromagnetic flux depends
isasstrongly
the loosely
named as couple coils;
onthe
theloosely
undercoils;
couple
transmitting
this configuration,
mediumunder between
only a fractiononly
thiscoils.
configuration, of the
Therefore, in this
transmitted
a configuration,
fraction electromagnetic
of the transmitted
the sample has
flux is capturedflux
electromagnetic in theis receiver, and
captured in thereceiver,
the transmitted
and electromagnetic
the transmitted flux depends strongly
electromagnetic flux on the
depends
more influence on the coils system response. The distance between coils was chosen for maximizing
transmitting
strongly on medium
the between
transmitting coils. Therefore,
medium between in this
coils. configuration,
Therefore, in this the sample hasthe
configuration, more influence
sample has
the relationship between the influence of transmitting medium (sample), and the transmitted signal
on
more the coils system response. The distance between coils was chosen for maximizing the relationship
stillinfluence
affects theonsecond
the coils system response. The distance between coils was chosen for maximizing
coil.
between
the the influence
relationship betweenofthe transmitting
influence of medium (sample),
transmitting and the
medium transmitted
(sample), signal
and the still affects
transmitted the
signal
second
still coil.
affects theSystem
second coil.
2.5. Sensing
2.5.Sensing
2.5. Sensing Systemcoils (sensor) were connected to an RF generator. A phase-locked loop was used to
The couple
System
detect
Thethe variations
couple at the reference
coils(sensor)
(sensor) frequency;
wereconnected
connected toanthose
an variations A
RFgenerator.
generator. arephase-locked
changed intoloop an electric
wasused
usedsignal.
to
The
Finally,couple
the coils
obtained data were
were recorded for to
further RF
analysis. The A phase-locked
schematic design loop
is shownwas in Figureto 3.
detect
detect the variations
the variations at the
at the reference
reference frequency;
frequency; those
thosewasvariations
variations are
are changed
changed into
into anan electric signal.
electric signal.
A volume
Finally,the of 10.000
theobtained
obtained ±
data 0.002
were mL of
recordedthe sample
for further poured
analysis. into the
The schematicsensor container at room
Finally,
temperature; an data were
appropriate recorded for further
temperature analysis.
control was The to
used schematic
avoid design isdesign
temperatureshown is
inshown
Figure
variations on
in
3.the
AFigure 3. Aofvolume
volume 10.000of± 10.000
0.002 ±mL0.002
of mL
the of the sample
sample was was poured
poured into into
the the sensor
sensor containeratatroom
container room
recorded
temperature;anmeasurements.
anappropriate Several
appropriatetemperature measurements
temperaturecontrol were
controlwas made
wasused
usedto at each
toavoid concentration
avoidtemperature to obtain
temperaturevariations
variationsonstatistical
onthe
the
temperature;
values about measurement errors.
recordedmeasurements.
recorded measurements.Several
Severalmeasurements
measurementswere weremade
madeatateach
eachconcentration
concentrationto toobtain
obtainstatistical
statistical
values about measurement
values about measurement errors. errors.

Figure 3. A schematic design of the sensing system.

2.6. Statistical Data ProcessingFigure 3. A schematic design of the sensing system.

2.6.With the aim

Statistical Data to Figure 3.
evaluate
Processing A schematic
the statisticaldesign
qualityof the
of sensing system.five measurements at each
the results,
concentration were performed; the standard deviation gives the error magnitude of the sensor
2.6. With the
Statistical Dataaim to evaluate the statistical quality of the results, five measurements at each
Processing
signal. Additionally, the Pearson coefficient was evaluated to obtain the correlation between the sugar
concentration were performed; the standard deviation gives the error magnitude of the sensor signal.
solution
Withconcentration
the aim and response
the sensor data.quality
Finally,of
receiver operating
fivecharacteristic (ROC) curve
Additionally, the to evaluate
Pearson statistical
coefficient was evaluated to the results,
obtain measurements
the correlation between at theeach
sugar
analysis was
concentration applied
were to calculate
performed; the the statistical
standard performance,
deviation gives the such
error as sensitivity
magnitude of and
the specificity
sensor of
signal.
solution concentration and response sensor data. Finally, receiver operating characteristic (ROC)
the sensor. the Pearson coefficient was evaluated to obtain the correlation between the sugar
Additionally,
curve analysis was applied to calculate the statistical performance, such as sensitivity and specificity of
Theconcentration
solution ROC curve is determined
and response by calculating
sensor data. theFinally,
sensitivity and specificity
receiver operating[27] using the confusion
characteristic (ROC)
the sensor.
matrixanalysis
curve shown was in Table
applied2 firstly.
to calculate the statistical performance, such as sensitivity and specificity of
the sensor.
Sensors 2019, 19, 2354 6 of 12

Table 2. The confusion matrix for receiver operating characteristic (ROC) curve

Observed
Y1 Y0
Predicted Y0 1 a b
Y0 0 c d

In Table 2, Y1 and Y0 belong to class Y and does not belong to class Y, respectively. The parameters
a and d represent true positives and true negatives, respectively; b represents false positives (type I
error), and c represents false negatives (type II error) [27].
In this sense, the sensitivity can be calculated as
a
Sensitivity = (7)
a+c

The sensitivity of the model is the proportion of positive sugar concentrations sensed by the RF
sensor correctly predicted (the probability that a sensor response belongs to a particular category is
correctly identified).
This parameter is commonly named “1-sensitivity”, and represents the probabilities of committing
a type II error, or false negative (error of omission).
On the other hand, the specificity can be calculated as Equation (8)

d
Speci f icity = (8)
b+d

The specificity, therefore, is the proportion of negative sugar concentrations sensed by the RF
sensor correctly predicted (the probability that a sensor response belongs to a particular category is
correctly identified). This parameter is commonly named “1-specificity” and means a type I error or
false positive (error of commission).
In this work, the ROC curve with a 95% of confidence was used to evaluate the performance of
the sensor response.

3. Results

3.1. Alternating Current (AC) Conductivity

The conductivity was used with the aim to know the transport mechanism in sugar solutions.
Figure 4 shows the ac conductivity of the sample as a function of the frequency for different sucrose
concentrations. There was a decrease in conductivity with an increase of sucrose concentration, and a
low conductivity dispersion below 100 Hz. After that, there was a “plateau” from 100 Hz to 1 MHz,
and the exponential increase of conductivity according to the universal Johnsher law [25,28,29]. The
low-frequency dispersion showed in Figure 4 was assigned to the vehicular mechanism of protonic
transport between water and hydroxyl groups of sucrose [30] (water–sucrose interaction). Meanwhile,
the plateau was assigned to a Grotthus mechanism for the water–water interaction in which there
is water hopping or tunneling of the proton from one molecule to the next as described by Miyake
et al. [31].
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Figure 4. Real component of the sample complex conductivity, in Siemens per cm (S/cm), as a function
Figure
Figure Real component
4. Real
4. component of of the
the sample
sample complex
complex conductivity,
conductivity, in Siemens per
in Siemens cm (S/cm),
per cm (S/cm), as
as aa function
function
of the frequency of different sucrose concentrations.
of the frequency of different sucrose concentrations.
of the frequency of different sucrose concentrations.
The sucrose molecule in solution interacts readily with other sucrose molecules and water
The sucrose molecule in solution interacts readily with other sucrose molecules and water
The sucrose
molecules throughmolecule
hydrogeninbond
solution
because interacts readily with
of its structure (14 Hother
atoms,sucrose molecules
eight OH groups,and and water
three
molecules through hydrogen bond because of its structure (14 H atoms, eight OH groups, and three
molecules through
hydrophilic oxygen hydrogen bond
atoms) [32], as itbecause
can be of its in
seen structure (14 H atoms,
the optimized eightgeometry
molecular OH groups, [33]and
donethree
in
hydrophilic oxygen atoms) [32], as it can be seen in the optimized molecular geometry [33] done in
hydrophilic oxygen atoms) [32], as it can be seen in the optimized molecular geometry
MOPAC software (Figure 5). Additionally, it was reported that three types of molecular interactions [33] done in
MOPAC software (Figure 5). Additionally, it was reported that three types of molecular interactions
MOPAC
occur software
in sugar (Figure
solutions: 5). Additionally,
Water–water, it was reported
sucrose–water that three typesresulting
and sucrose–sucrose, of molecular
in theinteractions
formation
occur in sugar solutions: Water–water, sucrose–water and sucrose–sucrose, resulting in the formation
occur
of in sugar solutions:
intermolecular hydrogenWater–water,
bonds [32–35]. sucrose–water
Then, the acand sucrose–sucrose,
conductivity behaviorresulting in the
of sucrose formation
obeys to the
of intermolecular hydrogen bonds [32–35]. Then, the ac conductivity behavior of sucrose obeys to the
of intermolecular hydrogen bonds [32–35]. Then, the
different mechanism of charge carrier transport explained above. ac conductivity behavior of sucrose obeys to the
different mechanism of charge carrier transport explained above.
different mechanism of charge carrier transport explained above.

Figure 5. An electronic density representation of the molecular structure of sucrose. In this model,
Figure 5. An electronic
sticks represent bondingsdensity
betweenrepresentation of the
carbon, hydrogen andmolecular structure
oxygen atoms. Theof sucrose.
electron In this
clouds model,
is depicted
Figure
sticks 5. An
representelectronic
bondingsdensity representation
between carbon, of the
hydrogen molecular
and
around each atom. Red: Oxygen, white: Hydrogen and blue: Carbon. structure
oxygen atoms.of sucrose.
The In
electron this model,
clouds is
sticks represent bondings between carbon, hydrogen and oxygen
depicted around each atom. Red: Oxygen, white: Hydrogen and blue: Carbon. atoms. The electron clouds is
Tan δ was
depicted calculated
around fromRed:
each atom. dielectric
Oxygen, permittivity and dielectric
white: Hydrogen and blue:losses to elucidate the absorption
Carbon.
Tanfrom
energy δ was calculated from
electromagnetic dielectric
waves permittivity
of sucrose solutionsand dielectric
(see losses
Figure 6). to elucidate
For pure the absorption
water, there was a peak
energyTan
between δ
10was
from calculated
to 10 kHz from
electromagnetic
Hz dielectric
waves
centered permittivity
of sucrose
around and(see
100 solutions
Hz. When dielectric
theFigure losses
sucrose to pure
elucidate
6).concentration
For water,thethere
was absorption
was a
increasing,
energy
peak from
Tan δ between electromagnetic
peak was10 Hz to 10
displaced waves
kHz to
around of sucrose
centered
400 Hz aroundsolutions (see
100 Hz.
as it is shown Figure
When
at 1.000 the sucrose concentrationwas
g/mL. 6). For pure water, there wasa
peak between 10 Hz to 10 kHz centered around 100 Hz. When the
increasing, Tan δ peak was displaced around to 400 Hz as it is shown at 1.000 g/mL. sucrose concentration was
increasing, Tan δ peak was displaced around to 400 Hz as it is shown at 1.000 g/mL.
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Figure 6. Tan δ as a function of frequency for different sucrose concentrations.

The relaxationFiguretime wasδextracted

6. Tan as a functionfrom the maxima
of frequency for peak showed
different inconcentrations.
sucrose tan δ (Figure 7). The increase
Figure 6. Tan δ as a function of frequency for different sucrose concentrations.
in tan δ obeys to the change of transport mechanism in sucrose molecules as it can be seen in the real
componentThe
The relaxation
relaxation time
timewas
of conductivity was extracted
extracted
(Figure from
4) andfrom the
themaxima
maxima
impedance peak
peakshowed
diagrams showed inintan
(not shown δ(Figure
tanδhere).
(Figure 7).
From7). The
The increase
increase
the Pearson
in
in tan
tan δδ obeys
correlation obeys to
to the
the change
coefficient change of
r = 0.896,of transport
there wasmechanism
transport mechanism in
in sucrose
a direct relation sucrose
to sugarmolecules
molecules as
as itit can
can be
be seen
concentration–relaxation seen in the
the real
intime real
(τ),
component
component
as it was shown of
of conductivity
in the fitting(Figure
conductivity (Figure
of Figure 4)
4) and
and
6. impedance
The equation diagrams
impedance diagrams
that (not
(notshown
represents shown
the best here).
here). From
From the
adjustment the Pearson
Pearson
of the data
correlation
correlation
was coefficient
τ = (8.412 × 10−7) × rSC
coefficient r== +0.896,
5.157there
× 10−7was a direct
, where relation tothe
SC represents sugar concentration–relaxation
sucrose concentration. Solution time (τ),
with
as
as itit was
high was shown
shown
sucrose in
in the
the fitting
concentration fitting of
had Figure
Figure 6.
of highest 6. The equation
equation
relaxation times, that
so represents
that the dipolesthe
represents the best
bestaadjustment
suffer adjustment of
of the
delay to return todata
the data
the
was
was ττ =
= (8.412 ×
× 10
10 −7 ) × SC + 5.157 ×−710−7 , where SC represents the sucrose concentration. Solution
−7 ) × SC + 5.157 × 10 , where SC represents the
equilibrium position and absorb electromagnetic energy in a high proportion as the sucrose sucrose concentration. Solution with
with
high high
concentration sucrose
sucrose concentration
concentration
increase. Therefore, had
had highest highest
frequencies relaxation
relaxation times,
among times,
so theso
1 kHz–10 the range
dipoles
kHz dipoles
suffer
aresuffer a delay
a suitable
delay toto to return
return
use tothe
in the
to the equilibrium
equilibrium
proposed position
sensor. position
and andabsorb absorb electromagnetic
electromagnetic energy
energy in in
a ahigh
highproportion
proportionas as the sucrose
sucrose
concentration
concentration increase.
increase. Therefore, frequencies among 1 kHz–10 kHz–10 kHz kHz range
range areare suitable
suitable to
to use
use in in the
the
proposed
proposedsensor.sensor.

-0.1 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1
-6 -6
1.6x10 1.6x10
-6 -6
1.4x10 -0.1 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.4x10
1.1
-6 -6
1.6x10-6
1.2x10 1.6x10-6
1.2x10
-6 -6
1.4x10-6 1.4x10
-6
10 10
-6 -6
1.2x10 1.2x10
-7 -7
8x10 -6 8x10
-6
10 10
τ (s)

-7 -7
8x10-7
6x10 8x10-7
6x10
τ (s)

-7 -7
6x10 6x10
-7 -7
4x10 4x10

-7 -7
4x10 4x10
-0.1 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1
sugar solution concentration (g/mL)
-0.1 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1
Figure 7. Relaxation time (τ) as a function of concentration from maxima peak in tan δ.
sugar solution concentration (g/mL)
Figure 7. Relaxation time (τ) as a function of concentration from maxima peak in tan δ.

Figure 7. Relaxation time (τ) as a function of concentration from maxima peak in tan δ.
Sensors 2019, 19, 2354 9 of 12
Sensors 2019, 19, x FOR PEER REVIEW 9 of 12

3.2.3.2. Sensor
Sensor Response
Response
The
The results
results ofofthe
thelinear
linearregression
regressionperformed
performed for for sensor
sensor response
responseagainst
againstsucrose
sucroseconcentration
concentrationis is
presented in Figure 8. The performed test of linearity indicated a linear response (p-value <
presented in Figure 8. The performed test of linearity indicated a linear response (p-value < 0.001) with0.001) with an
an intercept
interceptofof1.425
1.425andand slope of 0.680. Samples with sucrose concentrations under 0.150 ± 0.002 g/mL gave
slope of 0.680. Samples with sucrose concentrations under 0.150 ± 0.002 g/mL
error values that can be compared with the measurement value. Therefore, it was not possible to obtain
gave error values that can be compared with the measurement value. Therefore, it was not possible to
reliable information in this range. The sensor presented a linear response in the range from 0.150 ±
obtain reliable information in this range. The sensor presented a linear response in the range from 0.150
0.002 to 1.000 ± 0.002 g/mL with a standard deviation around 1% and sensitivity in the measurement
± 0.002 to 1.000 ± 0.002 g/mL with a standard deviation around 1% and sensitivity in the measurement
range of 0.05 g/mL, as it can be seen on error bars in Figure 7. The correlation factor is 1.
range of 0.05 g/mL, as it can be seen on error bars in Figure 7. The correlation factor is 1.
2.2

sensor response
2.1

2.0
sensor response (a.u.)

1.9

1.8

1.7

1.6

1.5

1.4
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
sugar solution concentration (g/mL)

Figure
Figure 8. 8. Sucrosesensor
Sucrose sensorresponse.
response. The
The squares represent
represent the
theexperimental
experimentaldata
dataand
andthe solid
the line
solid thethe
line
best
best fitting
fitting ofof a linetotothe
a line theexperimental
experimentalpoints.
points.

TheTheROCROC analysisofofthe
analysis thesensor
sensorresponse
response can be seen
seen in
in Figure
Figure9.9.The
Theresults
resultsshowed
showedthethe
right
right
measurement
measurement of of separability
separability in
in both
both
Sensors 2019, 19, x FOR PEER REVIEW 1-sensitivity
1-sensitivity and
and 1-specificity
1-specificity indicating
indicatingthat the
that sensor
the response
sensor response
10 of 12
hashas statistical
statistical significance.
significance.
0.0 0.5 1.0

1.0 1.0
1-Sensitivity

0.5 sucrose concentration 0.5

sensor response

0.0 0.0

0.0 0.5 1.0

1-Specificity
Figure 9. Sensitivity and specificity test for sensor response.
Figure 9. Sensitivity and specificity test for sensor response.

The proposed sensor achieves a sensibility of 0.05 g/mL which improves the sensibility of the
existing sensors (see Table 1); the working frequency helps in avoiding a possible destructive
interaction with the sample under study, and the electronics is simpler.

4. Conclusion
Sensors 2019, 19, 2354 10 of 12

The proposed sensor achieves a sensibility of 0.05 g/mL which improves the sensibility of the
existing sensors (see Table 1); the working frequency helps in avoiding a possible destructive interaction
with the sample under study, and the electronics is simpler.

4. Conclusions
The first approach to measure sugar solution concentration using RF system was reached. By using
low-frequency electromagnetic fields, a measurement system able to measure sugar concentration in
a water-based solution was developed. The proposed system is a contactless measurement method
and avoids the interaction between the sample under study and the measurement system. The coils
used in the system are homemade and not precise construction since the coils are similar, and the
electronics provide the working frequency in the range where the sample has a peak in the dielectric
response. Due to the electromagnetic nature of the sensor, it is possible measuring not only sugar
concentrations, but also other polar molecules. A measurement is achieved within seconds which can
be considered real-time when is compared with photothermal or spectroscopy techniques and accuracy
is comparable with mentioned methods. The sensor range is from 0.150 ± 0.002 to 1.000 ± 0.002 g/mL.
The influence of other standard components of sugar-sweetened beverages must be studied for getting
more information about the application of the system in control of this type of beverages. The sensor
sensibility is improved with the available methods using RF techniques as shown in Table 1. With this
improvement the possibility for further applications on polar samples is opened.

Author Contributions: Sensor conceptualization, G.A.R. and J.d.J.A.F.C.; methodology, J.d.J.A.F.C., O.H.G.O.,
N.P.A.D. and O.O.S.G.; MOPAC software, O.H.G.O. and N.P.A.D.; validation, C.J.T.R. and B.E.G.S.; formal analysis,
N.P.A.D. and J.d.J.A.F.C.; investigation and data curation M.A.W.T., C.J.T.R. and O.O.S.G.; writing J.d.J.A.F.C. and
N.P.A.D.; all authors reviewed and approved the manuscript.
Funding: This research received no external funding.
Acknowledgments: The authors want to thank the help of G. Lara Hernandez from ESIME-IPN. Also, N.P. Arias
and A. Wilches-Torres thanks to Vicerrectoría de Investigación, Ciencia y Tecnología Universidad de Boyacá for
the financial support, O. Giraldo thanks to Dirección de Laboratorios de sede, Universidad Nacional de Colombia
Sede Manizales.
Conflicts of Interest: The authors declare no conflicts of interest.

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