applied
sciences
Article
Design of a Low-Resolution Gamma-ray Spectrometer for
Monitoring Radioactive Levels of Wastewater
Sangrok Kim 1 , Taeyoon Kim 2 and Hyungjin Yang 3, *
Citation: Kim, S.; Kim, T.; Yang, H.
Design of a Low-Resolution
Gamma-ray Spectrometer for
Monitoring Radioactive Levels of
Wastewater. Appl. Sci. 2022, 12, 5613.
https://doi.org/10.3390/
app12115613
Academic Editor: Francesco Caridi
Received: 18 March 2022
Accepted: 29 May 2022
Published: 1 June 2022
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Copyright: © 2022 by the authors.
Licensee MDPI, Basel, Switzerland.
This article is an open access article
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Attribution (CC BY) license (https://
creativecommons.org/licenses/by/
4.0/).
Appl. Sci. 2022, 12, 5613. https://doi.org/10.3390/app12115613
1 Radiation Safety Section, Korea Institute of Radiation and Medical Sciences, Seoul 01812, Korea;
kim@kirams.re.kr
2 Proton Therapy Center, Research Institute and Hospital, National Cancer Center, Goyang 10408, Korea;
tkkim@ncc.re.kr
3 Department of Physics, Korea University Sejong Campus, Sejong 30019, Korea
* Correspondence: yangh@korea.ac.kr
Abstract: Wastewater containing radioactive materials is stored in decay tanks, which are typically
installed in basements to restrict public access. Specific activity is measured by a gamma spectroscopy
system or a gamma counter for several hours per sample before discharge. To simplify the sample
collection and measurement procedures before draining, the specific activity conversion coefficient
for converting a measured value from a 1.5” NaI (Tl) detector installed on a tank into specific activity
was calculated. The experimental calibration was performed in a test water tank with a volume of
14 L filled with diluted reference source 18 F, which is most commonly used in hospitals. The specific
activity of the test water was measured with a gamma spectroscopy system using a high-purity
germanium detector calibrated with certified reference materials. The change in the conversion
coefficient according to the change in the volume of the water tank was corrected based on a Monte
Carlo calculation. Finally, it was determined whether the minimum detectable activity (MDA) of this
system was lower than that of the draining standard. The counts for the specific activity conversion
factor and MDA were evaluated as 5.5389 × 1010 and 2.09 × 105 for 18 F and for the one-hour count,
respectively. The MDA was lower than the standard value. Thus, this system can be used for
discharge determination.
Keywords: NaI(Tl); MCNP; MC simulation; wastewater; draining; MDA
1. Introduction
Nuclear radiation has a wide range of applications [1,2]. Because radiation is handled
in radiation control zones, people who work and visit these areas are at risk of exposure.
Radiation safety management encompasses all activities that limit radiation exposure to
within acceptable levels [3–5].
Radiation safety management comprises three components: source management,
human management, and area management. Source management focuses on maintaining
the soundness of radiation sources, such as leak tests and radiation surveys. Human
management enforces legal obligations for those entering and exiting radiation-controlled
zones; these obligations include awareness, blood tests, and personal dosimetry. Area
management includes activities that verify whether the legal standards for radiation dose
rates inside and outside the radiation-controlled area are satisfied, whether the area is
contaminated, and whether radioactive materials deviate from the radiation-controlled
area [5–7].
In practice, radiation safety management depends on the type of radiation source.
Radiation sources are classified as radiation generators or radioisotopes, and radioisotopes
are further classified into sealed and unsealed radioisotopes [5].
The use of unsealed radioisotopes for experiments or medical treatments produces
radioactive wastewater. From the perspective of area management in radiation safety
https://www.mdpi.com/journal/applsci
Appl. Sci. 2022, 12, 5613 2 of 11

management, radioactive wastewater should be stored separately in a decay tank and

drained into the general environment only after it has been ascertained that it poses little
risk [4–6]. Because radioactivity decreases with time, the half-life of the radioisotopes must
be considered, and the drainage standards must be satisfied. If the specific activity of the
wastewater sample, including that of the stored radioisotopes, does not meet the criteria,
the storage, sampling, and measurement processes should be repeated until the standards
are satisfied.
The specific activity of wastewater is primarily measured using gamma spectroscopy
systems with a semiconductor detector, which can analyze nuclides and quantities simul-
taneously. Another method is to use a gamma counter, including a proportional counter,
which can only count the amount of radiation emitted by a sample.
The sample collection of radioactive wastewater from decay tanks to analyze the
nuclides and specific activity of radioisotopes is a time-consuming process because decay
tanks are typically installed in basements to restrict public access, and the level of specific
activity that escapes into the natural environment is similar to the minimum detectable
activity (MDA), requiring several hours of measurement time per sample.
To reduce this inconvenience, a regional monitoring system was used in this study
to measure count rates in a fixed place continuously, and the applicability of this system
was evaluated.

2. Materials and Methods

To the best of our knowledge, no study has continuously measured the radioactivity of
radioactive wastewater decay tanks, and the continuous detection system proposed in this
article is similar to underwater radiation monitoring systems that measure radioactivity
in seawater or groundwater using NaI(Tl), LaBr3 :Ce, Ce:GAGG, or CeBr3 detectors [8–14]
and in lakes using NaI(Tl) detectors [15–18]. A scintillation detector capable of examining
radionuclides by analyzing the gamma radiation energy was used in all these studies.
Considering the field characteristics—a semiconductor detector that requires cooling cannot
be used—a scintillation detector is the best choice in situations that require direct installation
in the field. High-purity germanium (HPGe) radiation detectors are not suitable for in situ
monitoring because of their high cost and high consumption requirements [19].
In addition, because water is a good shielding material, the efficiency decreases as
the distance increases. If the distance exceeds a certain limit, measurement is not possible.
In other words, a virtual sphere around the detector in water affects the detector. Owing
to this shielding effect, the detection efficiency of the detector in water is extremely low.
Therefore, the measurement error value increases, and the reliability of the measurement
data decreases. Thus, it is necessary to increase the measurement time [16]. Fortunately,
because radioactive wastewater in a decay tank is stored for weeks or months to reduce
radioactivity owing to the decay of radionuclides, there is no practical limitation on the
measurement time when a detector is installed on top of the tank.

2.1. System Description

In this study, a 38-mm-diameter and 38-mm-height NaI(Tl) scintillation detector (GS-
1515-NaI, Bee Research Pty, Ltd., Mascot, Australia) connected to a photomultiplier tube,
preamplifier, and power supplier was used to measure the amount of radiation. The output
of the preamplifier was connected to a shaping amplifier in a multichannel analyzer (MCA;
GS-USB-PRO, Bee Research Pty, Ltd., Mascot, Australia).
Free gamma spectroscopy software PRA 24.0.2.0 (Marek Dolleiser, Sydney University,
Sydney, Australia) [19] was used as a data logger for Windows 10 (Microsoft Ltd., Raymond,
WA, USA). This software controls an analog-to-digital converter (ADC), including an MCA,
through the USB communication interface, analyzes pulses received from the shaping
amplifier, and records them in real time.
The specifications of the continuous radioactivity monitoring system for the radioac-
tive wastewater decay tank are listed in Table 1.
Appl. Sci. 2022, 12, 5613 3 of 11

Table 1. Specifications of the monitoring system.

Parameters Details
Scintillation crystal 1.5” × 1.5” NaI(Tl)
Enclosure Aluminum case with cylinder shape
Resolution 6.5% to 8% at 660 keV
Gamma efficiency Approx. 60% at 662 keV
Input power +5 V, USB 2.0
Current draw <150 mA
ADC sample rate and bit rate 48 kHz, 16 bit
Pulse length Adjustable
Signal-to-noise ratio 73.97 dB
High-voltage connector SHV
Signal in connector BNC

2.2. Experimental Calibration

The experimental efficiency calibration was performed in a test water tank with a
volume of 14 L, filled with water and reference source 18 F, which is most commonly used
in positron emission tomography/computed tomography. It has a half-life of only 110 min
and emits two 511 keV gamma rays.
The absolute detection efficiency (ε) for 18 F was obtained using the following equation
from previous research [19,20]:
ε = N/(A·Iγ ·T), (1)
where N denotes the net count. Here, A denotes the specific activity of the specific radionu-
clide obtained using a gamma spectroscopy system including an MCA (DSA-1000 Digital
Spectrum Analyzer, Canberra Industries, Meriden, CT, USA), analyzing software (Genie
2000, Miron technologies, Atlanta, GA, USA) [21], and a high-purity germanium detector
(GEM25P-PLUS, Canberra Industries, Atlanta, GA, USA) calibrated by the certified refer-
ence materials in a cylinder-type source (Table 2) certified by the Korea Research Institute
of Standards and Science (KRISS), in units of Bq·m−3 . In addition, Iγ denotes the emission
probability of the gamma ray, and T denotes the live time of measurement.

Table 2. Specifications of certified reference materials in cylinder-type source, certified by KRISS.

γ-ray Emission
Half-Life (day) Activity (Bq) γ-ray
Probability (%)
Nuclide Energy
(keV)
Half-Life Uncert. Activity Uncert. Prob. Uncert.
241 Am 158,004 219 1844 74 59.54 35.92 0.17
109 Cd 461.9 0.4 10,257 410 88.03 3.66 0.05

57 Co 122.06 85.49 0.14

271.81 0.04 489 20
136.47 10.71 0.15
139 Ce 137.641 0.020 594 24 165.86 79.90 0.04
51 Cr 27.704 0.004 63,635 2600 320.08 9.89 0.02
113 Sn 115.09 0.03 1515 61 391.70 64.97 0.17
85 Sr 64.850 0.007 2009 81 514.00 98.5 0.4
137 Cs 10,976 29 909 37 661.66 84.99 0.20

60 Co 1173.23 99.85 0.03

1925.23 0.29 1251 50
1332.49 99.9826 0.0006

88 Y 898.04 93.7 0.3

106.63 0.05 3156 130
1836.05 99.346 0.025
 1173.23 99.85 0.03
60 Co 1925.23 0.29 1251 50
1332.49 99.9826 0.0006
898.04 93.7 0.3
88 Y 12, 5613
Appl. Sci. 2022, 106.63 0.05 3156 130 4 of 11
1836.05 99.346 0.025

2.3. Monte Carlo Simulation

2.3. Monte Carlo
In this Simulation
study, the activity conversion factor (ACF) was applied to convert the counts
In this by
measured study, the activity
the detector intoconversion factor (ACF)
specific activity. wasthe
Although applied
ACF to
hasconvert
the samethephysical
counts
measured
meaning asbydetection
the detector into specific
efficiency, it wasactivity.
used to Although the ACF has
clearly distinguish the sameofphysical
the purpose use.
meaning as detection
Because the ACFefficiency, it wasusing
is determined used totheclearly distinguish
intrinsic the purpose
characteristics of the of use.
scintillation
Because
detector and the
MCA, ACF is determined
it cannot be obtainedusing theby
only intrinsic characteristics
simulation; therefore, of the scintillation
it must be obtained
detector and MCA, itorcannot
only experimentally be obtained
calculated only byand
by experiments simulation; therefore,
simulations it must depart-
[15]. Different be ob-
tained only experimentally or calculated by experiments and simulations
ments use different isotopes in hospitals. The F has been commonly used for nuclear
18 [15]. Different
departments use different
medicine outpatients due to isotopes
its shortinhalf-life
hospitals. The 18 F hasconvenience
and production been commonly among used for
proton-
nuclear
emittingmedicine
nuclides.outpatients
In our study, due 18toF its
wasshort
used,half-life
and the and production
sample convenience
was placed among
in the tank, as
proton-emitting 18 was used, and the sample was placed in the
shown in Figurenuclides.
1b. The countIn our study,
rates of the Fsample and background count rates were meas-
tank,
ured as shown
using in Figure
a NaI(Tl) 1b. The
detector for count ratesunder
one hour of thethesample
same and background
experimental count rates
conditions. The
were measured using a NaI(Tl) detector for one hour under the same
ACF was calculated by comparing the simulation results obtained under the same condi- experimental con-
tions. The ACF was calculated by comparing the simulation results obtained under the
ditions.
same conditions.

3.5 cm
(b)
13 cm

Polyethylene bottle

NaI(Tl)
H

detector

Radioactive
Radioactive
wastewater
wastewater

(a) (b)

Figure1.1.Outline
Figure Outlineofofreal
realwastewater
wastewatertank
tank(a)
(a)and
andcalculation
calculationmodel
model(b).
(b).

The
Thedecay
decaytanks
tanksused
usedin inthe
thefield
fieldstore
storetens
tenstotohundreds
hundredsofoftons
tonsof ofwastewater.
wastewater.In Inthe
the
experiment,
experiment,the theperiphery
periphery of of
thethe
detector, as shown
detector, as shownin Figure 1b, was
in Figure 1b, constructed and used
was constructed and
instead of thatofinthat
used instead Figure 1a, and1a,the
in Figure detector
and was installed
the detector at the at
was installed topthe
of top
an actual-sized
of an actual-
decay tank. A NaI(Tl) detector was installed inside a polyethylene
sized decay tank. A NaI(Tl) detector was installed inside a polyethylene bottle bottle to prevent the
to prevent
detector
the detectorfromfrom
beingbeing
immersed.
immersed.
TheACF
The ACFwaswascalculated
calculatedby bycomparing
comparingthe thecounters
countersininthe
thefull
fullenergy
energypeak
peakmeasured
measured
with
withaaNaI(Tl)
NaI(Tl)detector,
detector,and
andthethe
specific activity
specific activitywas measured
was measured with a gamma
with a gamma spectrometry
spectrom-
system using using
diluted 18 F as 18
radioactive wastewater. A gamma spectrometry systemsystem
using
etry system diluted F as radioactive wastewater. A gamma spectrometry
ausing
semiconductor detector was calibrated using a radioactive certified standard
a semiconductor detector was calibrated using a radioactive certified standard ma- material.
The ACF
terial. Thewas
ACF calculated using the
was calculated usingfollowing equation,
the following and the
equation, andcounts measured
the counts by the
measured by
NaI(Tl) detector were converted to specific activities measured by a gamma
the NaI(Tl) detector were converted to specific activities measured by a gamma spectros- spectroscopy
system
copy systemwith an HPGe
with an detector. In this In
HPGe detector. equation, the units
this equation, ACF,of
theofunits NNaI , and
ACF, C,HPGe
NNaI andwere
CHPGe
Bq · s · m −3 ·counts−1 , counts·s−1 , and Bq·m−3 , respectively:
were Bq·s·m ·counts , counts·s , and Bq·m , respectively:
−3 −1 −1 −3

ACF = CHPGe /NNaI(Tl) , (2)

The radius (R) and height (H) of the water tank used in the experiment were 12.5
and 29.5 cm, respectively, and 14 L of radioactive wastewater was used in the experiment.
Because practical water tanks are usually much larger, the ACF was calculated using a
Monte Carlo simulation.
Appl. Sci. 2022, 12, 5613 5 of 11

Because water is a good shielding material, its efficiency varies according to the
measurement radius [15]. Thus, by changing the radius (R) and height (H) of the water
tank, as shown in Table 1, the change in ACF was calculated by the MCNP 6.2 (Los Alamos,
NM, USA) with the Monte Carlo code using the F8 tally with the GEB option [22].
In this simulation, the geometry of the scintillation detector was designed based on
the drawing provided by the manufacturer, and the density of the NaI(Tl) detector was
3.667 g·cm−3 [23]. In this case, the volume of radioactive wastewater used in the calculation
ranged from 14 to 56.1 L.

2.4. Calculation of MDA in Water

The MDA is the minimum detectable activity that can be distinguished from the back-
ground radioactivity and is calculated using Equation (3), called “Currie’s method” [24,25]:

MDA = LD/(ε·Iγ·T), (3)

where ε denotes the absolute detection efficiency, Iγ denotes the gamma-ray emission
probability, and T denotes the live measurement time. Here, LD is the detection limit in
counts with a 95% confidence level, and it is calculated as:

LD = 2.71 + 4.653 σB , (4)

where σB denotes the standard deviation of background radioactivity [24–26].

3. Results
3.1. Full Energy Peak Efficiency
The count of the full energy peak for one hour, N, was measured, using a NaI(Tl)
detector, to be 3318, and the count of 18 F in the sample was calculated by MCNP 6.2 to be
7.5372 × 107 . Using Equation (1), the efficiency value ε was calculated to be 4.402 × 10−5 .

3.2. Determination of 18 F ACF in Water

In this study, the count rates of wastewater stored in a decay tank were measured
using a NaI(Tl) scintillation detector and then converted into specific activity. To this end,
a radioactive wastewater sample containing 18 F radioisotopes was prepared. Because
our experimental data were used to determine whether radioactive wastewater could be
discharged safely, the specific activity of test water containing 18 F should be less than
1 × 107 Bq·m−3 , which is the discharge standard for radioactive wastewater provided
by law.
The count rates measured for the sample including 18 F and the background count rates
are shown in Figure 2a,b, respectively. Figure 2a confirms that the 511 keV gamma rays are
emitted by 18 F. Because the background count rate was only approximately 5.2% around the
511 keV peak, that of the sample including 18 F, the graph subtracting the background count
rate from Figure 2a was almost the same as in Figure 2a; therefore, it was not separately
indicated in the graph.
To estimate the ACF that can change the count rates (counts·s−1 ) of the 18 F sam-
ple measured with a NaI(Tl) detector to the specific activity (Bq·m−3 ), 500 mL of the
wastewater sample used in the above experiment was selected. It was measured using a
gamma spectroscopy system for one hour. The results are shown in Figure 3. The gamma
spectroscopy system used in this measurement was calibrated using a certified reference
material (Table 2); thus, the background radioactivity was automatically removed.
 4
F-18 source (a)

rates (counts·s−1)
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2
4
F-18 source (a)

Count rates (counts·sCount

1

−1)
3 Background (b)
0
0 100 200 300 400 500 600 700 800 900 1000
2
Energy (keV)

1
Figure 2. Count rates of 18F source including background (a) and background (b) obtained by exper-
iment using NaI(Tl) detector.
0
0 100 200 300 400 500 600 700 800 900 1000
To estimate the ACF that can change the count rates (counts·s−1) of the 18F sample
Energy (keV)
measured with a NaI(Tl) detector to the specific activity (Bq·m ), 500 mL of the
−3

wastewater sample used in the above experiment was selected. It was measured using a
Figure
gamma
Figure 2. spectroscopy
2. Count
Countrates
ratesofofsystem
18F
18source including
for
F source one background
hour.
including The (a) and
results
background (a) background
are shown
and (b) obtained
in Figure
background 3. The
(b) by exper-
gamma
obtained by
iment using
spectroscopy NaI(Tl) detector.
system used
experiment using NaI(Tl) detector. in this measurement was calibrated using a certified reference
material (Table 2); thus, the background radioactivity was automatically removed.
To estimate the ACF that can change the count rates (counts·s−1) of the 18F sample
measured with a NaI(Tl) detector to the specific activity (Bq·m−3), 500 mL of the
1
wastewater sample used in the above experiment was selected. It was measured using a
gamma spectroscopy system for one hour. The results are shown in Figure 3. The gamma
rates (counts·s−1)

spectroscopy 0.1system used in this measurement was calibrated using a certified reference
material (Table 2); thus, the background radioactivity was automatically removed.

0.01
1
Count rates (counts·sCount

0.001
−1)

0.1

0.0001
0.01
0 100 200 300 400 500 600
Energy (keV)
0.001
Figure3.3.Count
Figure Countrates
ratesof
of1818FF source
source obtained
obtained by
by experiment
experiment using
using HPGe
HPGedetector.
detector.

0.0001
Thecount
The countrates
ratesof ofthethefull
fullenergy
energypeak peak at at 511
511 keV,
keV,obtained
obtainedby bysubtracting
subtracting the
the back-
back-
0 100 200 300 400 500 600
ground counts
ground counts from the the counts
countsof ofthe
thewastewater
wastewatersample sample measured
measured using thethe
using NaI(Tl) de-
NaI(Tl)
tector, was
detector, was 0.9217
0.9217 counts·s −1 , Energy
counts−1·,sand and
(keV)
the specific
the specific activity of the
activity ofsame sample
the same measured
sample using
measured
the gamma
using spectroscopy
the gamma spectroscopy systemsystem
was 1.15031 × 106 Bq·m
was 1.15031 Bq·m−the
× 10−36. Thus, 3 . Thus, the ACF value
ACF value calculated
Figure 3. Count
usingrates of F4.6415
source 10 − 3 − 1.
calculated
using Equation Equation
(2) was 18
(2) was×obtained
104.6415
10 Bq·s·mby
× experiment
10 Bq·s−1
−3·counts ·m.using HPGe detector.
·counts
To
Todetermine
determine the the change in ACFfor
in ACF forthe
thevariation
variationinintank tank size,
size, a calculation
a calculation waswas
im-
The
implemented count rates
plemented bybya aMonte of the
MonteCarlo full energy
Carlosimulation peak
simulationusing at 511
using MCNP keV,
MCNP 6.2 obtained by subtracting
6.2 with the same geometryback-
the
same geometry and
and
ground
physicalcounts
physical fromas
conditions
conditions asthe counts
ininthe
theabove of the
above wastewater
experiment.
experiment. sample
Figure
Figure 4a measured
4awas
was obtained
obtainedusing
by the NaI(Tl)the
bysubtracting
subtracting de-
the
tector, was
background
backgroundcount0.9217 counts·s
countrates
ratesshown
−1, and the specific activity of the same sample measured using
shownininFigure
Figure2b 2bfrom
fromthe thecount
countrates
ratesofofthe
thewastewater
wastewatersample
sample
the gamma
measured
measured spectroscopy
using
using the
theNaI(Tl)
NaI(Tl) system
detectorwasshown
detector 1.15031
shown inin×Figure
106 Bq·m
Figure 2a. . Thus, the ACF value calculated
2a. −3

usingInEquation
Figure 4a, (2)awas
small 4.6415
peak× appears
10 Bq·s·m
10 −3 ·counts .−1
at approximately 440 keV. This peak might be
To determine
attributed the change
to the difference in ACF
between thefor the variation
Monte in tank size,
Carlo geometry in oura calculation and
was the
im-
plemented
actual geometryby aof Monte Carlo simulation
the material used in ourusing MCNPThis
experiment. 6.2 with the same
is because theregeometry and
was no peak
physical
around conditions
440 keV when asmeasuring
in the above theexperiment.
same sample Figure
using4athe was obtained
gamma by subtracting
spectroscopy the
system,
background
as count rates
shown in Figure 3. shown in Figure 2b from the count rates of the wastewater sample
measured using the NaI(Tl) detector shown in Figure 2a.
Appl.
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3
Measurement (a)

Count rates measured by NaI(Tl)

MCNP (b)
2 Measured full energy peak (c)
Calculated full energy peak (d)

(counts・s-1)
1

0
0 200 400 600 800 1000
Energy (keV)
Figure 4. Specific activities measured by HPGe and count rates measured by NaI(Tl): count rates (a),
Figure
(b) and4.full
Specific activities
energy measured
peaks (c), by HPGe
(d) obtained and countand
by experiment rates measuredrespectively.
calculation, by NaI(Tl): count rates
(a), (b) and full energy peaks (c), (d) obtained by experiment and calculation, respectively.
As shown in Table 3, the ACF calculated in computer simulations continued to increase
andInwas
Figure
fixed4a,at a5.5389
small ×peak
1010appears
Bq·s·m−at3 ·approximately
counts−1 when440 the keV.
volume Thisexceeded
peak might38 L.beIt
attributed to the difference between the Monte Carlo geometry in our calculation
was concluded from those that the larger the water tank, the larger the value measured and the
actual
usinggeometry
the NaI(Tl)of the material
detector, used
and infixed
it is our experiment. This is because
when the volume exceedsthere38 L.was no peak
Because the
around
decay 440
tankkeVforwhen measuring
radioactive the sameused
wastewater samplein using the was
the field gamma spectroscopy
at least 38 L, thesystem,
ACF of
as5.5389
shown× in
10Figure
10 Bq·s·3.m−3 ·counts−1 was suitable as an ACF for wastewater containing 18 F.
As shown in Table 3, the ACF calculated in computer simulations continued to in-
crease
Table and was fixed
3. Activity at 5.5389
conversion × 10
factors 10 Bq·s·m−3·counts−1 when the volume exceeded 38 L. It
(ACFs) for various water tank volumes in Figure 1b.
was concluded from those that the larger the water tank, the larger the value measured
using the NaI(Tl) detector, and it is fixed when the volume Calculated
exceeds 38 L. Because ACFthe decay
R (cm) H (cm) Volume (`) N
tank for radioactive wastewater used in the field was at NaI(Tl) least−38 L, the ACF
(Bq · s · of
m −5.5389 ×−10
3 ·counts 1 ) 10
(counts·s 1 )
Bq·s·m ·counts was suitable as an ACF for wastewater containing F.
−3 −1 18
12.5 29.5 14.0 2.4783 × 104 4.6415 × 1010
Table 3.14.4
Activity conversion
31.4 factors (ACFs) for various water
20.0 tank
2.2132 4
volumes
× 10 in Figure × 1010
5.19751b.
16.0 26.0 NNaI(Tl) 2.1122 × 10
33.0 4 5.4460 × 1010
Calculated ACF
R (cm) H (cm) Volume (ℓ)
17.4 34.2 (counts·s
32.0 −1) 2.0775 × 104(Bq·s·m−3·counts
5.5370 ×−1)1010
12.5 29.5 18.6 14.0 35.4 2.4783
38.0× 10
4
2.0768 × 104 4.6415 5.5389
× 1010 × 1010
14.4 31.4 19.7 20.0 36.5 2.2132
44.0× 10
4
2.0768 × 104
5.1975 5.5389
× 1010 × 1010
16.0 33.0 26.0 2.1122 × 10 4 5.4460 × 1010
20.7 37.5 50.0 2.0768 × 104 5.5389 × 1010
17.4 34.2 32.0 2.0775 × 104 5.5370 × 1010
21.6 38.6 56.1 2.0768 × 104 5.5389 × 1010
18.6 35.4 38.0 2.0768 × 104 5.5389 × 1010
19.7 36.5 44.0 2.0768 × 104 5.5389 × 1010
3.3. Calculation of MDA of 18 F in Water
20.7 37.5 50.0 2.0768 × 10 4 5.5389 × 1010
21.6 38.6 Figure 2b shows the background
56.1 2.0768count
× 10rates
4 measured for one5.5389 hour in× a1014
10 L water tank
containing tap water, and the counts in the full energy peak of 18 F were 186 counts. Using
Equation
3.3. (4), the
Calculation LD for
of MDA of 18the
F inone-hour
Water measurement was calculated as 6.62 × 101 counts.
5 − 3
Then, this value was transferred to 2.09 × 10 Bq·m , the MDA for the same measurement
Figure 2b shows the background count rates measured for one hour in a 14 L water
live time, using Equation (3) with an absolute detection efficiency (ε) of 511 keV. This
tank containing
efficiency was tap water,by
obtained and the counts
dividing the in the full
counts at energy
511 keVpeak of 18F were
in NaI(Tl) by the186counts
counts.at
Using Equation (4), the LD for the one-hour measurement was calculated
511 keV in the gamma spectroscopy system, and it was 4.40 × 10−5 . This value was smaller as 6.62 × 101
counts. Then, this value was transferred to 2.09 × 10 5 Bq·m−3, the MDA for the same meas-
than 1 × 107 Bq·m−3 , which is the amount prescribed by law in Korea, where the public
urement live time,
is predicted to reachusing
theEquation
dose limit(3) owing
with antoabsolute detection
the draining of 18efficiency
F-containing (ε) of 511 keV.
wastewater
This efficiency was obtained by dividing the counts at 511 keV in NaI(Tl)
into the public environment. Using this system, it was possible to determine whether the by the counts at
511 keV in the gamma spectroscopy system, and it was 4.40
18 × 10 −5. This value was smaller
specific activity of radioactive wastewater containing F could be measured for one hour.
than 1The
× 10change
7 Bq·m−3, which is the amount prescribed by law in Korea, where the public is
in MDA at various measurement times and assuming that the background
predicted to
radioactivity reach
wasthe dose limit
constant owingintoTable
is shown the draining
4. When of the
18F-containing wastewater into
measurement time was one
Appl. Sci. 2022, 12, 5613 8 of 11

hour, the MDA calculated using Equation (3) was 2.09 × 105 Bq·m−3 ; however, when the
measurement time was increased to 24 h, the MDA decreased to 4.12 × 104 Bq·m−3 . This
means that, by increasing the measurement time from one hour to one day, the measurement
ability was improved by five times.

Table 4. Minimum detectable activity (MDA) for reading time.

Reading Time (h) MDA (Bq·m−3 ) Reading Time (h) MDA (Bq·m−3 )
1 2.09 × 105 13 5.62 × 104
2 1.46 × 105 14 5.41 × 104
3 1.18 × 105 15 5.23 × 104
4 1.02 × 105 16 5.06 × 104
5 9.12 × 104 17 4.91 × 104
6 8.32 × 104 18 7.77 × 104
7 7.69 × 104 19 4.64 × 104
8 7.19 × 104 20 4.52 × 104
9 6.77 × 104 21 4.41 × 104
10 6.42 × 104 22 4.31 × 104
11 6.11 × 104 23 4.21 × 104
12 5.85 × 104 24 4.12 × 104

4. Discussion
Measuring the specific activity before draining radioactive wastewater is a resource-
and time-intensive process. In this study, a method of continuously measuring radioactivity
by installing a detector on a decay tank was used to reduce time and cost.
For this purpose, a NaI(Tl) detector, which is commonly used in studies measuring
radioactivity in seawater, groundwater, or lakes, was used to measure the count rates
in a tank containing radioactive wastewater, and the ACF was calculated. The specific
activities in Bq·m−3 (CHPGe ) were obtained by multiplying the counts per second (NNaI )
measured using a NaI(Tl) detector by the ACF. Using the ACF, a radiation safety manager
can observe the specific activity of wastewater stored in the wastewater tank in real time
and can immediately decide whether to drain the tank or not.
For this experiment, a NaI(Tl) detector with a diameter of 38 mm and a height of 38 mm
was used. It is inexpensive and has low efficiency among the products sold. The ACF to
transfer counts obtained using a NaI(Tl) detector to the specific activity was calculated
using a gamma spectroscopy system with an HPGe detector calibrated with standard
reference materials.
When underwater radioactivity is measured, water acts as a shield and affects the
measurement radius [13]; thus, a change in ACF was observed while increasing the size of
the tank containing radioactive wastewater. The change in the counted value for various
sizes of the tank containing radioactive wastewater was calculated using MCNP 6.2. As a
result of the calculation, when the volume of the tank exceeded 38 L, the ACF was fixed
at 5.5389 × 1010 Bq·s·m−3 ·counts−1 . Because the decay tank for radioactive wastewater
used in the field is at least 38 L, this conversion factor is suitable for radioactive wastewater
containing 18 F.
The MDA is the minimum detectable activity that can be separated from natural
radioactivity. Because the system used in this study must prove that the specific activity of
radioactive wastewater is less than the draining standard, the MDA of this measurement
system must be less than that of radioactive wastewater. Otherwise, this system cannot
determine whether the radioactive wastewater can be drained or not. To prove this, the
MDA of the measurement system was calculated to be 2.09 × 105 Bq·m−3 for one hour
Appl. Sci. 2022, 12, 5613 9 of 11

of measurement, which was smaller than the draining standard of 1 × 107 Bq·m−3 as
prescribed by law in Korea, where the public is predicted to reach the dose limit owing to
the draining of 18 F-containing wastewater into the public environment. Thus, it is possible
to use this system to determine whether the specific activity of radioactive wastewater
containing 18 F can be measured for one hour.
However, the following limitations exist when applying the results of this study to
the field. First, 18 F is a nuclide that emits 511 keV gamma rays and has sufficient energy
to pass through the aluminum outer wall of the NaI(Tl) detector. Therefore, radioisotopes
emitting low-energy gamma rays that do not pass through the outer wall of the detector
cannot be analyzed. This is a common problem with general radiation counters, and
this type of radioisotope should be used with a specialized instrument, such as a liquid
scintillation counter.
Another limitation is that the ACF is determined by the measurement system, and the
MDA is determined by the background radioactivity of the measurement environment. In
other words, the ACF should be determined for each measurement system, and the MDA
should be determined by measuring the background level after installation. For a lower
MDA, the shielding of the measurement system can be considered.
Finally, the cause of the peak around 440 keV in Figure 4 could be the difference
between the MCNP geometry in the calculation and the real geometry of the material used
in the experiment. This is because there was no peak at approximately 440 keV when the
same sample was measured using a gamma spectroscopy system with HPGe.
Despite these limitations, 18 F and 131 I, the most commonly used unsealed radioisotopes
in hospitals, emit radiation with sufficient energy to be measured with this system—18 F
used for cancer diagnosis and 131 I used for thyroid cancer treatment emit 511 and 971 keV
gamma rays, respectively. In particular, many hospitals use only 18 F and 131 I; therefore, the
possibility of applying this system is high.
The results of this study indicate that specific activity measurements for the draining
of radioactive wastewater into the public environment can be conducted using a rela-
tively inexpensive NaI(Tl) detector without relying on an expensive HPGe detector or a
gamma counter.
When measuring radioactivity using a NaI(Tl) scintillation detector with a diameter
of 38 mm and height of 38 mm, which is the smallest commercially available detector, the
MDA was found to be smaller than the value that is the draining standard for radioactive
wastewater provided by law. This system can be improved by using a larger scintillation
detector or installing a shield on the detector to reduce background radioactivity, which is
planned for further research. In this system, a detector is fixed on the top of a decay tank
for continuous measurement; therefore, the measurement time can be extended to several
hours or days; in such cases, the MDA decreases. These properties are not applicable to
radioactive wastewater containing 18 F, which has a short half-life. However, it can be
used for wastewater with a long half-life. In addition, this system is very similar to the
underwater, in situ spectrometer system for measuring the radioactivity contained in rivers
or seas, and it has potential applications for measuring radioactivity in ballast tanks or live
fish transport containers because it measures the radioactivity of stored water. We expect
that the proposed monitoring system can be used to monitor the radioactivity of the water
contained in a ship’s ballast tanks [27] and live fish containers. The proposed system can
help identify radioactivity because many people are concerned about the marine pollution
possibility by radioactive materials after the Fukushima nuclear disaster.

Author Contributions: Investigation, T.K.; methodology, T.K. and S.K.; simulation and experiment,
S.K.; writing—original draft, S.K.; writing—review and editing, T.K. and H.Y. All authors have read
and agreed to the published version of the manuscript.
Funding: This study was supported by the Research Foundation of Korea University (K1915361)
and a grant from the Korea Institute of Radiological and Medical Sciences (KIRAMS), funded by the
Ministry of Science and ICT (MSIT), Republic of Korea (No. 50422-2022).
Appl. Sci. 2022, 12, 5613 10 of 11

Institutional Review Board Statement: Not applicable.

Informed Consent Statement: Not applicable.
Data Availability Statement: Not applicable.
Conflicts of Interest: The authors declare no conflict of interest.

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