DOI: 10.1007/s10967-007-0710-3 Journal of Radioanalytical and Nuclear Chemistry, Vol. 273, No.

1 (2007) 55–58

Evaluation of the radioactivity in concrete from accelerator facilities

Q. B. Wang,1 K. Masumoto,2 K. Bessho,2 H. Matsumura,2 T. Miura,2 T. Shibata2
1 Institute of High Energy Physics (IHEP), The Chinese Academy of Sciences, Beijing 100039, P.R. China
2 High Energy Accelerator Research Organization (KEK), Tokyo, Japan

(Received June 30, 2006)

For evaluation of radioactivity induced in the concrete samples from accelerator facilities, the residual radioactivity in concrete sample, collected
from seven accelerator facilities, was determined by γ-ray spectrometry. The tritium was extracted by the heating method using an IR furnace, and
measured with a liquid scintillation counter. It was found that the major radioisotopes activated mainly by neutrons in the concrete samples were
152Eu, 60Co, 134Cs and 3H. The concentrations of radioactivities induced by thermal neutron capture are the highest at a depth of 10 cm in the

concrete wall. The correlation between tritium, 60Co and 152Eu activity was investigated by measuring many concrete samples for seven accelerator
facilities. The results indicate that their activities are strongly correlated with each other. So it would also be concluded that the total activity in
shielding concrete could be estimated on the basis of the activities of 60Co and 152Eu.

Introduction Experimental

During operation of an accelerator, its buildings and
shielding are activated by secondary particles, such as
neutrons, which are produced by nuclear reaction at a
target or beam loss points during acceleration and
transportation of particles. Although the specific activity
of radioisotopes induced in surrounding materials is low,
their amounts of activated materials are quite large.
Therefore, how to evaluate residual radioactivity is one
of important radiation safety issues in releasing the
materials to the environment in case of
decommissioning and decontamination of accelerator
facilities.1–3 In order to provide the clearance level of
each radioisotope, we have developed an analytical
method for induced radioisotopes, such as γ-emitters and
β-emitters.
Beta-ray emitters, such as tritium, induced by
thermal neutron capture reaction, are difficult to
determine nondestructively because of its decay emitting
only low-energy ȕ-rays. Concrete samples were
collected from seven accelerator facilities. We tried to
use the heating method with an IR furnace to extract
tritium from concrete samples, and the tritium activity
was measured with a liquid scintillation counter. The
activities of major γ-ray emitters were also measured by
an automatic γ-ray spectrometer. The correlation
between tritium, 60Co and 152Eu activity was
investigated by measuring many concrete samples for
seven accelerator facilities. As the results, a strong
correlation between tritium activity and the activities of
other radionuclides, such as 60Co and 152Eu, was
obtained, which can be easily measured by using a Ge
detector.
Sampling and sample treatment
We collected concrete samples from seven
accelerator facilities: (1) SF-cyclotron, Center for
Nuclear Study, University of Tokyo, (2) 1.3-GeV
Electron Synchrotron (ES), Tanashi Branch, KEK, (3)
300-MeV Electron Linear Accelerator, Laboratory of
Nuclear Science, Tohoku University, (4) AVF
Cyclotron, Research Center for Nuclear Physics, Osaka
University, (5) Ring Cyclotron, Research Center for
Nuclear Physics, Osaka University, (6) Cyclotron,
Nishina Memorial Cyclotron Center, and (7) 45-MeV
Electron Linear Accelerator, Hokkaido University.
Concrete samples were obtained by boring the
concrete walls or floors of several selected points of each
facility into 500 mm depths. Each sample was sliced to
20 mm thick and pulverized to powder by a stamp mill.
Powdered samples of 60 to 110 g were weighed, and put
into plastic bottles (50 mm∅×55 mm H).
Gamma-ray measurement
The γ-ray measurement of concrete samples was
performed by an automatic γ-ray spectrometer. An
empty plastic bottle was also measured to subtract the
background spectrum. Counting time was set to 40,000
seconds. The data acquisition and analysis package
“Gamma-studio” provided by SEIKO EG&G was used
for the γ-ray measurement. This package consists of a
set of complete algorithms for nuclide identification,
background subtraction, efficiency corrections and
determination of radioactivity for each radionuclide. A
standard source containing several nuclides was
prepared for the efficiency and energy calibrations.

* E-mail: qbwang@ihep.ac.cn

0236–5731/USD 20.00 Akadémiai Kiadó, Budapest

© 2007 Akadémiai Kiadó, Budapest Springer, Dordrecht
 Q. B. WANG et al.: EVALUATION OF THE RADIOACTIVITY IN CONCRETE FROM ACCELERATOR FACILITIES
Tritium extraction and measurement
Tritium was extracted by heating using an IR furnace
(UL VAC RHL-410P) and collected in two cold traps
cooled by dry ice/ethanol mixture.4 The sample
temperature and heating time were controlled exactly by
the programmable controller (ULVAC TPC-100062-1).
About 1 g sample was weighed and put on a quartz boat
and inserted into a quartz tube set in the IR furnace. The
appropriate condition of tritium extraction was
determined by heating to a temperature of 800 °C for 30
minutes under Ar-gas flow of 200 ml/min.
Tritium was collected into a vial by washing two
cold traps with 1 ml water and 20 ml liquid scintillator
(INSTA-GEL). Tritium activity was measured for three
times with a liquid scintillation counter (Packard
2000CA/LL). Counting time was set to 30 minutes. A
vial containing 1 ml pure water and 20 ml liquid
scintillator was also prepared and measured for
background subtraction.
Results and discussion
Introduction to seven accelerator facilities
(1) The SF-cyclotron has been used to studies in
nuclear physics and radioisotope production since 1974.
The accelerated energy of protons was 50 MeV and the
beam current was 10 μA. The total operation time was
36,000 hours. This machine was also used as the injector
of both a 1 GeV proton storage ring and a heavy-ion
linear accelerator for an RI-beam. Dismantling of the
beam-transport line and the cyclotron started from the
beginning of January 2000.
(2) In 1961, the 750-MeV electron synchrotron was
first constructed for the research of high-energy physics
in Japan. In 1966, the acceleration energy was raised to
1.3 GeV and the beam current was attained to 0.4 μA.
This machine was also used as injector of the 500-MeV
storage ring (INS-SOR), and has been shut down in Jun.
1999. The concrete block used for shielding the
synchrotron ring was reused at other accelerator
facilities. So for decommissioning and decontamination
of the accelerator facility, the activated area of the
building was only limited to the floor inside of the
accelerator room.
(3) The concrete samples were obtained from the
300-MeV Electron LINAC, Laboratory of Nuclear
Science, Tohoku University. The sampling points were
located under the electron LINAC beam line and were
exposed to secondary particles for 20 years.
(4) The AVF Cyclotron is located at the Research
Center for Nuclear Physics, Osaka University, and
established in 1974, As the injector of the Ring
Cyclotron, the AVF cyclotron accelerates protons,
deuterons, 3H particles, alpha-particles and various
56
light-heavy ions up to 85, 70, 175, 140 and 140 Q2/A
MeV, respectively. The concrete samples were obtained
from the AVF Cyclotron hall, which were exposed to
secondary particles for 18 years.
(5) The Ring Cyclotron is also located at the
Research Center for Nuclear Physics, Osaka University.
The beams extracted from the AVF cyclotron are
transported through one of the beam lines of the nuclear
physics facility and injected into the Ring Cyclotron.
With this accelerator system, beams of protons,
deuterons, 3He, alpha-particles and light-heavy ions are
available in the wide range of energies of up to 400, 200,
510, 400 and 400 Q2/A MeV, respectively. Operation of
the Ring Cyclotron started from 2002.
(6) The Nishina Memorial Cyclotron Center was
established in 1990 for the purpose of contributing to the
development of nuclear medicine. In the center, a small
cyclotron of compact design produces positron emitting
nuclides which can be used for disease diagnosis and
research work.
(7) The 45-MeV Electron Linear Accelerator is sited
in the Hokkaido University. Operation of the Electron
Accelerator started from 1974.
Residual radioactivity in concrete samples
The major radionuclides induced in the concrete of
seven facilities such as 60Co, 152Eu and 134Cs were
detected by an automatic γ-ray spectrometer and 3H was
measured by a liquid scintillation counter, respectively.
These activities took the greater part of the residual
radioactivity because of their large neutron capture cross
sections. Together with these radionuclides, 54Mn
induced via the 54Fe(n,p)54Mn reaction and 22Na
induced via the 23Na(n,2n)22Na reaction were observed
in the surface region of concrete, as these were produced
by fast neutron reaction, the activity was decreased
exponentially from the surface. In case of electron
accelerator, these can be also produced by photonuclear
reactions. The activity of 3H induced in concrete was
about one order higher than other radionuclides because
of 3H produced by the 6Li(n,α)3H reaction with a large
cross section of 945 barn.
Depth profile of the residual radioactivity
Figure 1 shows the depth profiles of major
radionuclides observed in the concrete samples collected
from seven accelerator facilities. The figure clearly
indicates that long-lived radioactivities such as 3H, 60Co
and 152Eu are mainly produced by thermal neutron
capture reactions, and the concentration of
radioactivities are the highest at a depth of 10 cm, then
decrease exponentially to a low level over a depth of
50 cm. On the other hand, the radioactivity of 22Na
induced by fast neutrons are the highest at the concrete
 Q. B. WANG et al.: EVALUATION OF THE RADIOACTIVITY IN CONCRETE FROM ACCELERATOR FACILITIES

surface and decreased to no detectable amounts over a
depth of 30 cm. The attenuation curves of 3H, 60Co and
152Eu are also close to each other.
Correlation between tritium and γ-ray nuclides
Figure 2a shows the correlation between tritium and
60Co specific activity for many concrete samples
obtained from seven accelerator facilities. Figure 2b
shows the correlation between tritium and 152Eu specific
activity. As seen from these figures, a good agreement
between these three reactions was found. It indicates that
tritium in concrete was produced mainly by thermal
neutron capture reactions on these seven accelerator
facilities, and the tritium in shielding concrete will be
estimated on the basis of the activity of 60Co and 152Eu.

Fig. 1. Depth profiles of major radionuclides induced in concrete for seven accelerator facilities

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 Q. B. WANG et al.: EVALUATION OF THE RADIOACTIVITY IN CONCRETE FROM ACCELERATOR FACILITIES

Fig. 2. Correlation between tritium and 60Co, 152Eu specific activity for seven accelerator facilities;
correlation with 60Co activity (a) and with 152Eu activity

Conclusions *

We observed 3H, 60Co, 152Eu and 134Cs in concrete
samples of seven accelerators facilities. The activity of
3H was ten times higher than that of 60Co and 152Eu.
Their maximum radioactivities were observed at a depth
of 10 cm, then decreased exponentially to an extremely
low level beyond a depth of 50 cm. These isotopes were
produced by thermal neutron capture. The activities of
22Na and 54Mn could be measured in the surface region
of concrete samples. As both of them were produced by
fast neutron reactions, their activities decreased
exponentially from the surface. In the case of electron
accelerator, these radionuclides can be also produced by
photonuclear reactions.
The correlation between tritium, 60Co and 152Eu
activity was investigated by measuring many concrete
samples for seven accelerator facilities. The results
indicate that their activities are strongly correlated with
each other. So, it would also be concluded that the total
activity in shielding concrete could be estimated on the
basis of the activities of 60Co and 152Eu obtained easily
by γ-ray measurement.
This work was supported by Japan Society for the Promotion of
Science. The authors also are grateful to Dr. S. WATANABE, Center for
Nuclear Study, University of Tokyo, Dr. T. OHTSUKI, Laboratory of
Nuclear Science, Tohoku University, and Dr. T. SAITO, Research
Center for Nuclear Physics, Osaka University, and their colleagues for
concrete sampling.
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2. W. P. SWANSON, Radiological Safety Aspects of the Operation of
Electron Linear Accelerators, IAEA Technical Reports Series No.
188, IAEA, Vienna, 1979, p. 101.
3. A. B. PHILLIPS, D. E. PRULL, R. A. RISTINEN, J. J. KRAUSHAAR,
Health Phys., 51 (1986) 337.
4. Q. B. WANG, K. MASUMOTO, K. BESSHO, H. MATSUMURA,
T. MIURA, T. SHIBATA, J. Radioanal. Nucl. Chem., 262 (2004)
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