Domanski10.1515 - Pjmpe 2016 0008

Download as pdf or txt
Download as pdf or txt
You are on page 1of 7

Polish Journal of Medical Physics and Engineering 2016;22(2):41-47

doi: 10.1515/pjmpe-2016-0008

Scientific Paper

Experimental investigation on radiation shielding of high performance


concrete for nuclear and radiotherapy facilities
Szymon Domański1,a, Michał A. Gryziński1, Maciej Maciak1, Łukasz Murawski1, Piotr Tulik1, Katarzyna
Tymińska1
1
National Centre for Nuclear Research, 05-400 Otwock-Świerk, Poland
a
E-mail address: [email protected]

Abstract
This paper presents the set of procedures developed in Radiation Protection Measurements Laboratory at National
Centre for Nuclear Research for evaluation of shielding properties of high performance concrete. The purpose of such
procedure is to characterize the material behaviour against gamma and neutron radiation. The range of the densities of
the concrete specimens was from 2300 to 3900 kg/m3. The shielding properties against photons were evaluated using
137
Cs and 60Co sources. The neutron radiation measurements have been performed by measuring the transmitted
radiation from 239PuBe source. Scattered neutron radiation has been evaluated using the shadow cone technique. A set
up of ionization chambers was used during all experiments. The gamma dose was measured using C-CO2 ionization
chamber. The neutron dose was evaluated with recombination chamber of REM-2 type with appropriate recombination
method applied. The method to distinguish gamma and neutron absorbed dose components in mixed radiation fields
using twin detector method was presented. Also, recombination microdosimetric method was applied for the obtained
results. Procedures to establish consecutive half value layers and tenth value layers (HVL and TVL) for gamma and
neutron radiation were presented. Measured HVL and TVL values were linked with concrete density to highlight well
known dependence. Also, influence of specific admixtures to concrete on neutron attenuation properties was studied.
The results confirmed the feasibility of approach for the radiation shielding investigations.

Key words: concrete; radiation shields; recombination chambers.

Introduction aggregate), a “regular” is defined as concrete having a density


in the range of 2000-2600 kg/m3.
Concrete is a cheap, versatile and widely used construction
material. It is associated with its efficiency, flexibility, and
simple manufacturing process. Among the obvious advantages Radiation shields
of concrete are: high strength, good insulation properties, Photon radiation (X and gamma) may interact with matter as a
durability and the ability to take any shape. This material is result of: the photoelectric effect, Compton scattering, or
applied as a radiation shield in radiotherapy centers, isotope creation of electron-positron pairs. All of these effects require
and accelerator laboratories, and especially in nuclear facilities. interaction with the electrons. Therefore the high electron
In this type of industrial projects besides the regular concrete, a density of heavy materials is essential. A typical shielding
special one is also used containing, besides cement, sand, water material used in this case is lead (Z = 82). Concrete used as a
and aggregates (stones, slag, etc.), also different types of shield against gamma radiation should be composed so that the
reinforcements (e.g. steel fibers) and various admixtures (air percentage of “electron-rich” elements is as high as possible.
entraining agents, plasticizers, accelerators, retarders, etc.). A Shielding concrete is prepared on the basis of the heavier
typical concrete mix is prepared from about 25% cement and aggregate so that, compared with other conventional shielding
water, around three quarters of total volume are aggregates [1]. materials, it has a high effective atomic number (12-13). This
The 80% of the concrete is oxygen and silicon, the rest is translates directly to effectiveness in the fields of gamma
calcium, aluminum and small amounts of sodium, potassium radiation and at the same time reduces the space occupied by
and iron [2]. The type and amount of concrete mix ingredients the shield.
result in a qualitatively different shielding properties for In case of neutrons the way they interact with matter varies
different types of ionizing radiation. The density of the regular greatly depending on the kinetic energy of the neutron.
concrete is about 2350 kg/m3, but in practice, due to the Depending on the energy neutrons are divided into two
diversity of the composition (especially quantity of the grain categories: thermal and fast. In experimental practice, the
criterion for the division is specific energy - cadmium cutoff

41
Domański et al: Concrete radiation shielding Pol J Med Phys Eng 2016;22(2):41-47

energy (about 0.5 eV), neutrons of higher energies are fast a. Linear attenuation factor µ depends on the photon
neutrons [3]. Additionally, in the scope of fast neutrons exist energy and the type of material (effective atomic
the range of intermediate energies from 1 eV to about 0.1 MeV number Z).
- epithermal (or resonance) neutrons. Half Value Layer – HVL - determines the thickness of the
In nuclear matter there are 3 main processes the neutron is material that suppresses the radiation beam so that the initial
undergoing. They are two types of scattering: elastic, when the radiation dose is reduced by half. In a similar manner defined
total kinetic energy of the participants is conserved, and Tenth Layer Value – TVL - is the thickness of the material that
inelastic, when a part of the neutron kinetic energy is suppresses radiation beam tenfold.
transferred to the nucleus, causing its excitation. The nucleus The HVL and TVL values are usually expressed in cm. The
then deexcites emitting a photon. Both kinds of scattering relation between the linear absorption coefficient, and HVL
occur in full range of energies and their result is thermalization and TVL is as follows:
of the neutron. The third process, occurring mostly at low and
resonance energies is neutron capture. In the result a compound HVL = ≅ 0,693 Eq. 2
nucleus is created, usually in unstable excited state. Then it
TVL = ≅ 2,3 Eq. 3
decays emitting alpha, beta and gamma radiation.
The effective neutron radiation shielding materials are the Similar considerations exist for neutron radiation. The
light elements (hydrogen, helium) and the high number of reduction of the intensity of the neutron beam in the material is
nuclei per volume or high density (water, paraffin or the like described by formula:
HDPE and other plastics). From the point of view of neutron
$
shielding the most important is the amount of hydrogen " = · ,# · Eq. 4
contained in the concrete. Overall all the hydrogen contained in For non-collimated radiation beam the build-up factor can be
the concrete is in the form of water, therefore, the higher the described as:
water content, the lower amount of concrete is needed for
,# = 1 − '·# Eq. 5
thermalizing and capturing neutrons.
where parameter β is a constant characteristic for the shielding
Parameters defining the shielding properties material. Knowing the radiation absorption curve we can
determine the macroscopic cross section for neutron absorption
As a result of interactions that cause ionization of matter the
by numerical fit for the equation 4. A frequently used method
intensity of the primary beam of radiation is weakened by
is to determine the estimators of the absorption cross section
interactions, such as the scattering and absorption of radiation
HVLn TVLn defined by analogy with the gamma radiation as a
particles. The probability of interaction with matter particles
shield layer reducing the intensity of the radiation beam to 0.5
with energy E per unit of path traveled by the particle is
and 0.1 of the initial value.
described using the linear absorption coefficient µ(E) in the
Additionally the value of Ln=1/Σ is defined as the mean free
case of gamma radiation or macroscopic cross section Σ(E) in
path of neutrons in the material.
the case of neutron radiation [4].
In the case of photon radiation the intensity of radiation I0
passing through the uniform shield of thickness of x is the Ionizing radiation sources
product of two factors: the beam attenuation e-µ (E) and the As photon radiation sources one can use X-ray units or sealed
buildup parameter B(E, µ(E) x). Both the parameters are radioactive isotope sources. The most commonly used sources
functions of shell thickness, often expressed by the average are 137Cs isotope emitting gamma rays with an energy of 0.662
number of free paths µx travelled by radiation. Generally, this MeV or 60Co emitting two energy lines (1.17 and 1.332 MeV)
dependence is described by the formula: with almost the same intensity and the average energy of 1.25
MeV. Such sources can be found in the form of bars (linear
= · , · Eq. 1 radiation source), or spread evenly on the surface (the plane
The build-up factor B (E,µx) is an amendment showing the source), the most common and simplest are point sources of
increase in the intensity of secondary and scattered radiation. It radiation, of which the transversal dimension is much smaller
depends on: (typically 10 times) compared to the distance to measuring
1. The measured quantity (eg. fluence, dose, detector radiation detector.
response, etc.). As sources of neutron radiation one can use the sealed
2. Geometry radiation sources of proper design. Heavy isotope nucleus (e.g.
235
a. Collimated beam (B = 1) U, 239Pu, 233U) can undergo a fission, by reaction with
b. Wide beam (B > 1) neutron of a suitable energy, into two nuclei of comparable
c. Uniform point source weight. During this process fast neutrons are emitted. For
d. other certain isotopes (e.g. 252Cf, 250Cf, 250Cm) spontaneous fission,
3. The thickness of the shield; expressed by the average with neutron emission, may occur. The neutrons produced in
number of free paths µx this way are also sources of gamma rays resulting from the

42
Domański et al: Concrete radiation shielding Pol J Med Phys Eng 2016;22(2):41-47

decay products, inelastic scattering, the neutron capture recombination chambers are used. Measurement of RQF
reaction or activation of stable isotopes from the environment. involves the determination of changes in the efficiency of ions
The most common source of this type is a source containing collection f(U) at two suitably selected voltage polarizing, the
252
Cf. Its advantage is that the neutrons spectrum is similar to reference voltage, US, and a voltage recombination UR in
the one of neutrons generated in a fission reactor core. relation to the same difference in the reference radiation, i.e.
A very popular neutron source is a nuclear reaction of type one for which Q = 1, according to the formula:
(α, n) induced in certain isotopes using alpha particles coming + ,- + ,.
from alpha decay of the other isotopes. Such sources, contain RQF = Eq. 6
+/01 ,- +/01 ,.
isotopic converters (9Be, 10B, 11B, 18O or 19F) with alpha As a reference gamma radiation is meant radiation of 137
Cs
emitters, mainly actinides (uranium, plutonium, americium).
isotope.
The most common sources of this type are 239PuBe and
241
AmBe. The emitted neutrons have average energies higher
Radiation properties after shield passage
than the average energy of neutrons produced in the fission
reaction. For example, the 239PuBe source emits the neutrons The best accuracy in gamma and X beams provides
from reaction 9Be(α, n)12C. The neutrons have the energy range spectrometric measurement (e.g. a NaI crystal with a
of 0.5-11.5 MeV with the average of about 4.4 MeV. Specific photomultiplier cooperating with multichannel analyzer). As a
for this source are also gammas with an energy of 4.438 MeV, result we observe the reduction of intensity of gamma lines of
accompanying each neutron emission. different radiation energies. However, in the case of
Another type of source used for shielding materials tests are monoenergetic gamma sources displayed in a collimated beam
sources of photoneutron from reaction (γ, n). The great geometry, giving the at measurements of HVL and TVL
advantage of such sources is that they are the source of uniformity coefficient beam h≈1, we can simplify the
monoenergetic neutron beam. Unfortunately, production of measurement using less demanding radiation detectors such as
gamma radiation with sufficiently high energy (typically above Geiger-Muller or ionization chambers.
2.5 MeV) requires costly accelerator installation. The main problem that we encounter performing the
Parameters describing the radiation beam or field formed by measurements in the neutron fields dose is to separate the dose
source are: component derived from gamma radiation. The classic solution
Uniformity coefficient h – defined by the ratio of the is to two-detector method of determining the dose components.
thickness of the first half value layer to the thickness of the This method uses two detectors with different relative neutron
second half value layer. Its change indicates the changes in the and gamma sensitivity - detector of neutron sensitivity similar
radiation spectrum after undergoing successive layers of to the gamma sensitivity, denoted T, and detector "insensitive
shielding. When 1.HVL=2.HVL=3.HVL etc. the beam is to neutrons", that is low relative sensitivity of neutron, denoted
monoenergetic. U. The absorbed dose rate in the mixed radiation is obtained by
Radiation quality factor, Q – allows to determine the value solving the simultaneous equations:
of the absorbed dose equivalent H or energy deposited by 23 = 4 3 5ℎ 3 7 + 9 3 73 : Eq. 7
radiation in living matter (tissue, organ), taking into account
the biological effects caused by different types of radiation. Its 2, = 4, 5ℎ, 7 + 9, 73 : Eq. 8
formal unit (often overlooked) is Sv/Gy. where R is the detector response (depending on the type of
In accordance with the recommendations of the ICRP [5] for detector it may be a current, charge, quantity or pulse rate); hT
gamma radiation Qγ equals to 1, for neutron Qn value depends HU - the relative sensitivity of detectors T and U to gamma
on the neutron energy and is between 5 and 20 Sv/Gy. The radiation in the investigated field, ie. the ratio of detectors
factor of neutron radiation depends on the linear energy response (sensitivity) to the absorbed dose rate (or more
transfer LET. In the case of the continuous radiation spectrum precisely the tissue kerma rate) of gamma radiation in the field
the sufficient information is the spectrum. to the response in calibration field (137Cs); kT, kU - relative
The spectra of isotopic sources are well known, so the neutron sensitivity of detectors T and U, i.e. the ratio of
determination of the quality factor for such radiation is response to the neutron absorbed dose rate in the test field to
relatively easy. Unfortunately, the radiation spectrum behind the response to the absorbed dose rate of gamma radiation
the shield changes (h≠1). In such a case, the numerical D*(10) in the calibration field. The next possible step is to
modeling of the neutron transport through the shielding or calculate the dose equivalent H*(10). For this purpose we use
experimental determination of neutron spectra becomes the formula:
necessary. The alternative is a direct measurement of the
; ∗ 10 = 7 ∗ 10 · = + 7"∗ 10 · =" Eq. 9
radiation LET with recombination chamber or proportional
counter filled with tissue equivalent gas. where D with respective index means absorbed dose rate
Recombination Quality Factor of radiation (RQF or Q4) is components determined by us, and the Q coefficients
used as a measurable indicator of numerical values similar to correspond to the quality coefficients of gamma and neutron
the radiation quality factor [6]. To determine the RQF radiation. For the measurement of the neutron dose one can use

43
Domański et al: Concrete radiation shielding Pol J Med Phys Eng 2016;22(2):41-47

dosimeters of the Leake or Brown type [3], in which the radiation (60Co, 137Cs) and neutron radiation (239PuBe) under
detector is proportional counter with a working gas containing controlled conditions.
3
He or BF3 with a natural content of 10B. The distinctive feature Gamma sources were exposed with Tema Synergie
of these detectors is a thick layer of polyethylene moderator (in irradiator. The device produces collimated beam directed
the shape of a sphere for Leake or cylinder for the Brown type) through a bench for precise positioning of radiation detectors.
surrounding the counter. These devices are designed to be Plutonium-Berylium source was exposed in free field
absolutely insensitive to gamma radiation. For gamma geometry, directly from the specially designed container for
measurements a G-M counter, not sensitive to neutron storing high activity isotopic sources. During the exposition
radiation, can be used. source were placed in the axis of calibration bench, 100 cm
over the floor. Additionally, the laboratory is equipped with
Microdosimetric recombination method two kinds of neutron sources: 241AmBe and 252Cf,
Method RMM consists of examining the current-voltage recommended by international standards [8] as reference
characteristic shape of the recombination chamber [7]. This standards for neutron dosimeter calibrations.
analysis will provide information on energy loss distribution in To estimate parameters of neutron radiation passing through
the gas filling recombination chamber and thus the concrete, two recombination chambers REM-2 and GW2 were
determination of quality factors for the individual components used alternatively. REM-2 № 8 chamber [9] is a high pressure
of the radiation dose in a volume of the detector. recombination chamber, filled with tissue equivalent gas
This method can be used in radiation fields of unknown containing 11% of hydrogen. It has a similar sensitivity for
components and spectrum in a relatively wide range of dose neutron and gamma radiation. Second chamber, GW2 has a
rates. Measurements are based on determination of current- similar construction [10], but it is filled with CO2. Hydrogen
voltage characteristics of the chamber in the studied radiation free filling assures weak sensitivity for neutron radiation.
fields and in a standard field of gamma radiation of 137Cs
isotope. An illustrative series of characteristics for a set of
concrete slabs is shown in the figure 1.
The result is graphs (figure 2) showing the contribution of
individual fractions of radiation with different LET created by
ionizing radiation in the gas of recombination chamber. Here
we can observe the change of individual components of the
dose with a change in the thickness of the concrete shielding.
The first interval corresponds to the percentage part of the
gamma component. The next three columns can be interpreted
as the interaction of neutrons with the molecules of the gas
filling the recombination chamber. Observing the change in the
composition of the radiation after passing through each layer,
you can see the growth of scattered gamma radiation coming
from non-elastic collisions of neutrons with the gas filling the
chamber. We can also observe a decreasing number and energy
of recoil protons, indicating the gradual slowing of neutrons
down to intermediate energy. Passing through the last three Figure 1. Series of ion collection efficiency curves measured in
layers, the proportions of the bars practically do not change, reference field of 137Cs and 239PuBe ionizing radiation and behind
concrete slabs.
which means a total domination of the radiation composition
by the scattered radiation.
The undoubted disadvantage of measurements performed
using this method is the relatively long time it takes to make
one complete characterization of the chamber (at least 5h). In
return, however, we get full information about the quality of
the measured radiation field. Among the advantages one can
include no need for a second radiation detector measuring
gamma radiation only.

Instrumentation
Tests were performed on 40 cm × 40 cm × 5 cm slabs with Figure 2. RMM graphs: a) histogram for bare 239PuBe source. b) -
g) histograms for consecutive thickness of 5 cm, 10 cm, 15 cm,
density approx. 3000 kg/m3. Units were exposed to gamma
20 cm, 25 cm, 30 cm of portland concrete slabs.

44
Domański et al: Concrete radiation shielding Pol J Med Phys Eng 2016;22(2):41-47

Recombination chamber REM-2 operates with the


recombination voltage UR = 60 V and saturation voltage
US = 1000 V. Ionization chamber GW2 operates with the
voltage US = ±30 V. The setup of twin chambers allows for
determination of particular dose components 7"∗ 10 and
7 ∗ 10 . If additional recombination techniques are applied it is
possible to estimate the ambient dose equivalent ; ∗ 10 .
The measurements were conducted for various thickness of
each concrete. The slabs were set on a steel frame, strong
enough to carry at least ten concrete plates with a total mass up
to 300 kg. The distance between the source and the detector Figure 3. Gamma and neutron dose rate from 239PuBe source
was set to 132.8 cm. The scattered fraction of neutrons was measured behind portland concrete slabs. Absorbed dose from
measured using shadow cone and estimated as direct and in scattered neutrons determined with shadow cone
7"∗ 10 >?@ABC@B> =8.73±8.7 µGy/h. The value was used as a technique.
shift correction of neutron dose rate 7"∗ 10 DEDF according to
the formula:
7"∗ 10 = 7"∗ 10 DEDF − 7"∗ 10 >?@ABC@B> Eq. 10
Using obtained measurement results, one can plot the functions
describing beam attenuation versus increasing shield layer
thickness. Exemplary plot is shown on the figure 3.
To determine the absorption of radiation from gamma
sources only GW2 chamber was employed. One can easily read
out HVL and TVL values or determine linear attenuation Figure 4. Transmission of gamma radiation from 137
Cs source
coefficients using equations 1 or 4. thru concrete slabs of different density.
To determine the RMM histogram for selected types of
concrete chamber REM-2 № 8 was used. The current voltage
characteristics, which later appointed curves of ions collection
effectiveness, was measured in the voltage range from ±5 to
±1000 V. Deconvolution of ions collection effectiveness
function to the form of histograms-LET spectrum estimation
was performed according to the algorithm RMM [7]
implemented for this purpose in R language [11], and using the
non-negative least squares NNLS model [12].

Measurement data analysis


The final result of the study for each concrete, are the values of Figure 5. Variation of HVL and TVL values, gamma attenuation
HVL and TVL determined on the basis of attenuation curves. estimators, as a function of the density of different concretes for
The resulting values are presented on the figure 5. We can 137
Cs source.
clearly state that the density of the shield is an important factor
in attenuation. Hence reduction of high specific gravity
enhance the attenuation performance of concretes.
In opposition to the previous figure is an attempt to search a
similar dependence for neutron radiation. As one can see in the
graph in figure 6, for this particular problem, it is hard to find a
simple relation between the applied aggregate and shielding
parameters studied concrete mixtures. The accuracy of the
designated half value layers due to the uncertainty of the source
position, the measurement technique and the data extrapolation
is at the level of 5.5% for gamma radiation and 16% for
neutron radiation. Measured results do not show any
correlation to concrete density. Figure 6. Measured values of 1.HVLn (circles) and
1.HVLn+2.HVLn (triangles) for various types of high performance
concretes.

45
Domański et al: Concrete radiation shielding Pol J Med Phys Eng 2016;22(2):41-47

Figure 7. Measured enhancement of neutron radiation attenuation


Figure 8. Attenuation factor for ionizing radiation for portland
(HVLn decrease) related to Hydrogen (left) and Gadolinium (right
concrete of density G = HIJJ KL/NO .
graph) contents. Circles represent 1.HVLn values and triangles
represent sum of 1.HVLn and 2.HVLn.

In the case of neutron radiation the type of designed concrete Summary


shielding should be considered individually, carefully choosing
During the measurements of neutron fields parameters created
its elemental composition. In fact, already rough comparison of
by neutron sources carried out so far, we stated that at the
the HVLn changes to the content of serpentine aggregate
calibration hall one can determine the exact value of ambient
(3MgO·2SiO2·2H2O) used in the mixture, so tied hydrogen
dose equivalent after passing through the concrete shielding
content in the material, can be seen to improve the properties of
smaller of thickness than about 30 cm. For thicker layers, high
the shielding (figure 7).
contribution of scattered radiation makes it impossible to
Obtained from measurement data attenuation curves shown
perform measurements without the use of sophisticated
previously in figure 3 and 4 can be converted to the
measurement techniques. Moreover the authors skip details of
nomograms allowing for the determination of the attenuation
the procedure for radiation fields with high fluxes of neutrons
coefficients in the radiation field. Example nomograms
in which gamma generation in n-g reactions become
presents figure 8.
significant. Regarding the results of gamma, one can measure
the thickness of the shielding material of more than 140 g/cm2.
Determination of HVL and TVL parameters (shielding
properties of various materials, various concretes mixtures) in
such fields is much more complicated and also will be
presented in another publication. In spite of all described above
disadvantages presented technique is good enough to make
rough quantitative and qualitative comparison of different
materials e.g. samples of different concrete mixtures.

References
[1] Neville AM. Concrete properties. Krakow: Polish Cement Association; 2000.
[2] Kaplan MF. Concrete radiation shielding. New York: John Willey & Sons; 1989.
[3] Knoll GF. Radiation Detection and Measurement. New York: John Wiley & Sons; 2000.
[4] Shultis J, Faw R. Handbook of Nuclear Engineering. in: Radiation Shielding and Radiological Protection. Springer, p. 1313-1448.
2010
[5] ICRP. 1990 Recommendations of the International Commission on Radiological Protection. ICRP Publication 60. Ann ICRP.
1991;21(1-3):1-201.
[6] Zielczyński M, Golnik N, Makarewicz M, Sullivan AH. Definition of radiation quality by initial recombination of ions. In: Proc 7th
Symp Microdosimetry; 1980 Sep 8-12; Oxford, UK. p. 853-862.
[7] Golnik N. Microdosimetry Using A Recombination Chamber: Method and Applications. Radiat Prot Dosim. 1995;61(1-3):125-128.
[8] Reference neutron radiations – Part 1: Characteristics and methods of production. ISO 8529-1:2001. Geneva, Switzerland:
International Organization for Standardization; 2001.
[9] Zielczyński M, Golnik N. Rekombinacyjne komory jonizacyjne. Seria monografie IEA, Otwock-Świerk. 2000.

46
Domański et al: Concrete radiation shielding Pol J Med Phys Eng 2016;22(2):41-47

[10] Golnik N, Pliszczynski T, Wysocka A, Zielczynski M. Determination of Dose Components in Mixed Radiation Fields by means of
Recombination Chambers. 5th Symp Neutr Dosim; 1985 Sep 17-21; Munich; Germany. Luxembourg: Commission of the European
Communities, p. 717-725.
[11] R Core Team. R: A language and environment for statistical computing. R Foundation for Statistical Computing, Vienna, Austria:
2015.
[12] Lawson CL, Hanson RJ. Solving Least Squares Problems. Classics in Applied Mathematics. Philadelphia: SIAM. 1995.

47

You might also like