Journal of

Environmental Radioactivity 50 (2000) 253}261

Radionuclide content of building materials
and associated gamma dose rates in
Egyptian dwellings
R.H. Higgy*, M.S. El-Tahawy, A.T. Abdel-Fattah',
U.A. Al-Akabawy'
National Centre for Nuclear Safety and Radiation Control, 3 Ahmed El-Zomor Street, Nasr City, 11762,
P.O. Box 7551, Cairo, Egypt
'Nuclear Research Centre of Inshass, AEA, 3 Ahmed El-Zomor Street, Nasr City, 11762 P.O. Box 7551,
Cairo, Egypt
Received 7 September 1999; received in revised form 29 December 1999; accepted 11 January 2000
Abstract
Studies have been carried out to determine the natural radioactivity in some building
materials (bricks, tiles, marble and ceramics) and their associated radiation hazard. The
radioactivity concentrations of ``"Ra, ```Th and ""K were measured using a gamma spectrom-
eter with a Hp}Ge detector. The activities of ```U and ``"U were measured using an
alpha-spectrometer with a surface barrier detector after applying a radiochemical procedure.
The ``"U/```U isotopic ratios were calculated. The radium equivalent activities and the
radiation hazard index associated with the natural radionuclides were calculated. A computer
program was developed and applied to calculate the dose rate a person will receive from the
walls of a room constructed from the studied building materials. 2000 Elsevier Science Ltd.
All rights reserved.
Keywords: Radioactivity; Uranium; Thorium; Radium; Potassium; Buildings; Bricks; Marble; Ceramics;
Gamma dose
* Corresponding author.
E-mail address: ruranda@yahoo.com (R. H. Higgy).
0265-931X/00/$- see front matter 2000 Elsevier Science Ltd. All rights reserved.
PII: S 0 2 6 5 - 9 3 1 X ( 0 0 ) 0 0 0 1 7 - 5
1. Introduction
Exposure to ionizing radiation is generally regarded as undesirable at all
levels, although no harmful e!ects are known to follow very low-level exposures
(UNSCEAR, 1993). Recently, considerable attention has been given to low-level
exposure arising from naturally occurring radionuclides, particularly ```U, ```Th and
""K. The reason for current interest is due to the fact that external radiation exposures
from naturally occurring radionuclides contribute, on average, about 10% of
the average annual dose to the human body from all radiation sources (UNSCEAR,
1993). It has been observed (Bruzzi, Mele & Padoani, 1992; Tufail, Mirza &
Khan, 1992; Hassib, Hussein, Amer & Piesch, 1993; Malanca, Pessina & Dallar, 1993;
El-Tahawy et al., 1995; El-Tahawy & Higgy, 1995; Ibrahim, 1999) that naturally
occurring radionuclides are present in building materials which constitute a lived-in
radioactive environment. This study was carried out to measure the radioactivity
of some Egyptian building materials used in construction of walls and #oors. The
external dose calculations help to make a proper assessment of radiation exposure to
the population (Koblinger, 1977; Stranden, 1979; Mustonen, 1984).
2. Experimental techniques
2.1. Sampling and sample preparation
Ten "nal product building materials (four types of bricks, three types of tiles,
two types of ceramic and one type of marble) were collected from di!erent highly
productive commercial companies in the Cairo region. The samples were crushed to a
"ne powder, sieved through a 1 mm mesh, then dried at 1003C for 24 h to constant
weight.
2.2. Gamma spectrometric measurements
A constant volume of 200 cm` of each sample was packed, weighed in radon-
impermeable identical plastic vessels and sealed for four weeks to reach secular
equilibrium between ``"Ra (of the ```U series) and ```Th and their progenies.
The absolute e$ciency of the detection system was determined through a series of
measurements using a group of standards obtained from the IAEA, namely RGU.1,
RGTh., RGK.1 and Soil 6.
The determination of ```U activity concentrations was based upon the 63.3 KeV
-ray line emitted by ``"Th. The determination of ``"Ra (of the ```U series) activity
concentrations was based upon the 295.2, 351.9 KeV (`"Pb) and 609.3, 1764.5 KeV
(`"Bi) -ray lines. To determine the activity concentrations of ```Th, the -ray lines
338.4, 911.1 KeV (```Ac), 2614.7 KeV (`"`Tl) were used. To determine the activity
concentration of ""K, the 1460 KeV -ray line was used.
254 R. H. Higgy et al. / J. Environ. Radioactivity 50 (2000) 253}261
2.3. Alpha spectrometry measurements
For uranium analysis, a portion of the dried samples was ashed at 5003C. Five
grams of each ashed samples was taken, spiked with ```U tracer to calculate the
chemical recovery and dissolved using mineral acids (HNO
`
, HF and HCl). The
uranium was extracted with trioctylphosphinoxide in cyclohexane, back-extracted
with NH
"
F/HCl solution, then coprecipitated with La(NO
`
)
`
and puri"ed by passing
through anion exchange column. Uranium was then electroplated on a stainless-steel
disk from oxalate-chloride solution. The prepared samples were measured using alpha
spectrometers with surface barrier detectors (Pimpl, Yoo & Yordanova, 1992). Silicon
surface barrier detectors were used for the measurements because of their excellent
resolution, high permissible counting rates, low background and excellent stability.
Also there is no signi"cant variation of the detector e$ciency in the energy interval
2.5}8.8 MeV. This makes the quantitative evaluation of -particle spectra much
simpler than in the case of -ray spectra (De Regge & Boden, 1984; Holm, 1984).
2.4. Mathematical modeling and calculation
In this work, a computer program was developed and applied to calculate the dose
rate a person will receive from the walls of a room constructed of di!erent building
materials. This program is written in Pascal according to a model in which the gamma
lines of the ``"Ra and ```Th series and ""K are used. Also the attenuation factors of
the wall materials and air are taken into consideration. The program can run for
di!erent room dimensions and di!erent radionuclide concentrations. A #ow chart of
the program is shown in Fig. 1. Although the method developed in this work is
applicable to any shape, it can only be tested for regularly shaped volume sources
since analytical expressions only exist for such geometries. It is also assumed in the
model that the gamma ray source is distributed uniformly in a certain wall thickness.
To calculate the exposure at any point, the wall plane subdivision shown in Fig. 2 is
considered. The marked areas in this "gure are calculated once and the total dose
from the whole wall is then
D"4D

#8D
`
#4D
`
. (1)
Only the absolutely necessary elements are calculated and the others are just identical
by point symmetry, and that is why this program is so fast. Of course, integration over
wall depth is performed, and some other `speeding-up tricksa are used. The emission
rate of photons N is given by
dN"dm A, (2)
where A is the activity concentration in Bq/kg, is the emission probability, dm is the
mass of the in"nitesimal volume element d< of the wall material in kg.
The #uence rate of primary photons unattenuated at distance r from the source is
given by
d

d< AeIJ/4r`, (3)

R. H. Higgy et al. / J. Environ. Radioactivity 50 (2000) 253}261 255
Fig. 1. Flow chart of the program.
where is the density of the wall material in kg/m`, l is the attenuation path in m, is
the attenuation linear coe$cient of the wall material.
The #uence rate of primary photons from the whole wall is given by:
"(1/4)A

T
(1/r`)eIJ d< (4)
It is worth noting that the integral over volume is in fact a triple integral in cartesian
space (x, y, z).
The #uence rate of primary photons, over the range of radionuclides and their
gamma lines, is given by
"(/4)
G
A
G

H
[
GH

T
(1/r`)eIGHJ d<]. (5)
256 R. H. Higgy et al. / J. Environ. Radioactivity 50 (2000) 253}261
Fig. 2. Wall plane showing the subdivisions considered.
The summation in the last equation extends over the contribution to the #uence rate
fromall gamma lines of the radionuclides of interest (i is the radionuclide index and j is
the energy line index).
To calculate the dose equivalent rate, two additional functions of energy are
applied. One of them, the build-up factor, accounts for scattered radiation in the wall
material. The other is the exposition-to-dose conversion factor. The dose equivalent
rate, H is expressed by the following formula:
H"(/4)
G
A
G

H
[
GH
C
GH
B
GH

T
(1/r`)eIGHJ d<], (6)
where B is the exposition build-up factor, B"B(E, l) and C is the exposition-to-dose
conversion factor, C"C(E).
In our geometrical modeling, we assumed that the room is rectangular, the thick-
ness of the wall is the same for the three pairs of opposite sides, the walls are
homogeneous, there are no windows or doors, and the point of detection may be
speci"ed arbitrarily. In the calculation of the exposure dose rate, the values of mass
energy absorption coe$cients in air, dose build-up factors and photon mass attenu-
ation coe$cients for concrete obtained by Trubey (1991) were used. The attenuation
coe$cients for materials other than concrete may be written as
"(
"
)/(
"
), (7)
where ,
"
, ,
"
are the attenuation coe$cient and density for the material and
concrete, respectively (Mustonen, 1984). Since the densities of the building materials
are very nearly the same as for concrete, we assume in our case that
/
"
"1. (8)
Thus we have used the attenuation coe$cients of concrete. A nuclide library contain-
ing the relevant energies and emission probabilities is also used (IAEA, 1989) and this
R. H. Higgy et al. / J. Environ. Radioactivity 50 (2000) 253}261 257
Table 1
Activity concentrations, radium equivalent activities and representative level index values
Sample description ``"Ra (Bq/kg) ```Th (Bq/kg) ""K (Bq/kg) Ra

(Bq/kg) I
A'
Clay brick 31.5$2.9 25.5$4.0 298$25 90.8$3.3 0.664
Sand brick 15.1$1.9 5.0$1.7 48.9$10.1 26.0$2.1 0.184
Light-weight brick 26.3$1.4 8.0$1.2 26.9$3.9 39.8$1.5 0.273
Cement brick 11.0$1.2 2.8$0.6 19.6$2.7 16.5$1.2 0.114
Cement tile 19.2$2.2 7.5$2.1 45.8$9.9 33.4$2.2 0.234
Mozaic tile 15.2$1.1 6.3$0.7 46.7$3.7 27.8$1.4 0.196
Marble tile 11.8$1.0 4.5$0.6 18.8$2.6 19.7$1.2 0.136
Natural marble 4.4$0.7 * * * *
Ceramic (wall) 81.6$5.0 55.0$3.4 254$14 180$3 1.263
Ceramic (#oor) 77.3$4.5 64.3$3.3 569$19 213$3 1.538
nuclide library can be varied for any purpose. The input data we have to enter to our
program are the wall dimensions (length, breadth, height, thickness, density) and the
wall material activity concentrations (``"Ra, ```Th and ""K) in Bq/kg. The program
can run for each wall alone, or to calculate the maximum dose for the three walls (big
wall, small wall and #oor/ceiling).
3. Results and discussion
The activity concentrations (C
"
, C
'"
and C
'
) of ``"Ra, ```Th and ""K in the
studied building materials are given in Table 1. The activity concentrations of
C
"
range from 4.4 to 81.6 Bq/kg dry weight. The activity concentrations of C
'"
range
from 2.8 to 64.3 Bq/kg dry weight. The activity concentrations of C
'
range from
18.8 to 569 Bq/kg dry weight. All the values of the activity per unit mass are in the
ranges of the corresponding typical world values (NEA-OECD, 1979; UNSCEAR,
1993) which are 50, 50 and 500 Bq/kg for C
"
, C
'"
and C
'
, respectively; except for
the wall ceramic tiles (C
"
"81.6 Bq/kg, C
'"
"55.0 Bq/kg) and the #oor ceramic
tiles (C
"
"77.3 Bq/kg, C
'"
"64.3 Bq/kg, C
'
"569 Bq/kg). Wall and #oor ceramic
tiles, commonly used in bathrooms, toilets and kitchens get their sanitary white
appearance from zircon added to the glassy (glaze) matrix. Zircon, a zirconium silicate
(ZrSiO
"
), is a mineral that usually contains approximately 400}1000 ppm by mass of
the thorium and uranium oxides. Although the amount of zircon used in the glaze
(10}15% by weight) is low, it may still pose a radiological problem, as glazed tiles are
used in domestic buildings and may cover large areas in places like commercial
kitchens and public toilets (O'Brien, Aral & Peggie, 1998).
To assess the radiological hazard of the building materials used, it is useful to
calculate an index called the radium equivalent activity, Ra

, de"ned according to
the estimation that 1 Bq/kg of ``"Ra, 0.7 Bq/kg of ```U and 13 Bq/kg of ""K produce
the same -ray dose (Malanca et al., 1993). This index Ra

is given as:
Ra

"C
"
#1.43C
'"
#0.077C
'
, (9)
258 R. H. Higgy et al. / J. Environ. Radioactivity 50 (2000) 253}261
Table 2
Comparison of activity concentrations for uranium obtained with gamma spectrometry and alpha spectro-
metry
Sample description Activity concentrations in Bq/kg dry weight
``"U -spectrometry ```U -spectrometry ```U -spectrometry ``"U/```U
Clay brick 31.3$1.5 31.9$1.6 30.2$6.8 0.981
Sand brick 13.3$0.8 14.4$0.9 14.1$4.1 0.924
Light-weight brick 21.4$1.0 24.0$1.1 26.1$2.9 0.892
Cement brick 11.7$0.7 11.9$0.7 9.4$2.7 0.983
Cement tile 16.8$0.7 17.3$0.7 18.8$4.4 0.971
Mozaic tile 15.9$0.7 16.1$0.7 16.1$2.8 0.988
Marble tile 15.4$0.8 15.1$0.8 10.8$2.9 1.020
Natural marble 5.7$0.7 5.1$0.6 3.6$1.6 1.118
Ceramic (wall) 65.2$2.9 67.5$3.0 80.1$9.9 0.966
Ceramic (#oor) 63.3$3.3 68.5$3.6 72.5$7.9 0.924
where C
"
, C
'"
and C
'
are the activity concentrations in Bq/kg of ``"Ra, ```Th and
""K, respectively. The calculated values of the radium equivalent Ra

for the studied

building materials are given in Table 1. Another radiation hazard index, the represen-
tative level index, I
A'
, used to estimate the level of -radiation hazard associated with
the natural radionuclides in speci"c building materials, is de"ned as (NEA-OECD,
1979)
I
A'
"(C
"
/150)(C
'"
/100)#(C
'
/1500), (10)
where C
"
, C
'"
and C
'
are the activity concentrations in Bq/kg of ``"Ra, ```Th and
""K, respectively. The values of I
A'
for the studied samples are given in Table 1. It is
clear that all the studied building materials do not exceed the upper limit for the
representative level which is unity, except the ceramic samples which have values of
1.3 and 1.5.
In Table 2, the ```U activities obtained both by -spectrometry and -spectrometry
are compared. The results of these two techniques are in good agreement within the
experimental accuracy. The activity ratios ``"U/```U are between 0.9 and 1.1. Within
the reported experimental errors, the samples show similar values for ``"U and ```U,
thus suggesting maintenance of equilibrium between the two isotopes, which is in
agreement with the results obtained by Holm and Bojanowski (1989) for uranium of
natural origin.
To estimate the radiation hazard due to the natural radioactivity from the building
materials, especially bricks, the dose rate of a room constructed from four walls is
calculated using the program developed. The results of these calculations are given in
Table 3. The dose rates in the middle of a room of dimensions 5.0;4.0;2.8 m` for
wall thicknesses 25 and 35 cm constructed of di!erent kinds of bricks are given in
Table 3. The values range from 0.0065 to 0.0370 Sv/h for a wall thickness of 25 cm
and range from 0.0072 to 0.0413 Sv/h for a wall thickness of 35 cm. It is clear from
R. H. Higgy et al. / J. Environ. Radioactivity 50 (2000) 253}261 259
Table 3
Exposure dose rate in the middle of a 4.0;5.0;2.8 m` model room for di!erent brick and ceramic
materials
Type of wall material Wall thickness Dose in Sv/h
Clay brick 25 0.0370
35 0.0413
Sand brick 25 0.0103
35 0.0115
Light-weight brick 25 0.0154
35 0.0171
Cement brick 25 0.0065
35 0.0072
Ceramic (wall) 2 0.0091
4 0.0178
Table 4
Exposure dose rate in the middle of a 12.0;6.0;2.5 m` room made of brick materials
Activity concentration in Bq/kg
dry weight
Exposure rate in Sv/h
Sample descriptionDensity (g/cm`) ``"Ra ```Th ""K Mustonen
(1984)
This work
Clay brick 1.6 23 21 620 0.0201 0.0190
White brick 1.6 80 62 990 0.0493 0.0431
the results that the dose obtained in a room constructed of clay brick is about 576%
higher than for cement brick and about 360% higher than sand brick and about 242%
higher than light-weight brick. Also the exposure rates due to radioactive nuclides in
2 cm and 4 cm thick ceramic coverings on the internal walls of a kitchen or bathroom
were calculated using the proposed program. The dose rate due to the ceramic cover is
0.0091 Sv/h for a thickness of 2 cm and 0.0178 Sv/h for a thickness of 4 cm.
Neglecting the absorption of the radiation from the wall material, we obtain values of
the total dose rate for a wall thickness of 35 cm constructed from clay brick and
covered with ceramic of thickness 4 cm of 0.0590 Sv/h. The method used for dose
calculation using the proposed program was tested against the results obtained by
Mustonen (1984), for a model room of dimensions 12.0;6.0;2.5 m` constructed of
four brick walls. The results are shown in Table 4.
From our study we can conclude that the wide usage of ceramic walls and ceramic
tiles as coverings for the entire surfaces of bathrooms and kitchens should be done
with caution as they show high radiological hazard indices in comparison to other
kinds of building materials. But still no regulations and restrictions against the usage
of any building material are needed as the radiation level lies su$ciently below that of
natural radiation. When constructing some buildings, e.g. nuclear medicine and
260 R. H. Higgy et al. / J. Environ. Radioactivity 50 (2000) 253}261
research laboratories for low level counting techniques, building materials of the
lowest activity concentrations must be chosen carefully.
Acknowledgements
The authors are greatly indebted to Dr. M. Makarewicz, Expert in the IAEA
Laboratories in Seibersdorf, Austria, for his support and help. The authors wish to
express deep gratitude for help and support to Dr. D.E. Mahfouz, Professor of
Radiation Physics in Monou"a University.
References
Bruzzi, L., Mele, R., & Padoani, F. (1992). Evaluation of gamma and alpha dose due to natural radioactivity
of building materials. Journal of Radiology Protection, 12, 67}76.
De Regge, P., & Boden, R. (1984). Review of chemical separation techniques applicable to alpha spectro-
metric measurements. Nuclear Instruments and Methods in Physics Research, 223, 181.
El-Tahawy, M. S., & Higgy, R. H. (1995). Natural radioactivity in di!erent types of bricks fabricated and
used in the Cairo region. Applied Radiation Isotopes, 46, 1401}1406.
El-Tahawy, M. S., Farouk, M. A., Higgy, R. H., & Ibrahiem, N. M. (1995). Radioactive analysis of building
materials in central region of Egypt. Nuclear Science Journal, 32, 322}329.
Hassib, G. M., Hussein, M. I., Amer, H. A., & Piesch, E. (1993). Assessment of radon concentration in
Egyptian dwellings by using a passive technique. Nuclear Tracks Radiation Measurements, 22, 341}344.
Holm, E. (1984). Review of alpha-particle spectrometric measurements of actinides. International Applied
Radiation Isotopes, 35, 285.
Holm, E., & Bojanowski, R. (1989). Natural activity in the Baltic sea. In: The Radioecology of Natural and
Arti"cial Radionuclides, Proceeding of the XVRegional Congress of IRPA, Visy, Sweden. IRPA(pp. 49}54).
Ibrahim, N. M. (1999). Natural activities of ```U, ```Th and ""K in building materials. Journal of
Environmental Radioactivity, 43, 255}258.
IAEA, International Atomic Energy Agency (1989). Measurement of radionuclides in food and the environ-
ment. A Guide Book, Technical Reports series No. 295, Vienna.
Koblinger, L. (1977). Calculation of exposure rates from gamma sources in walls of dwelling rooms. Health
Physics, 34, 459}463.
Malanca, A., Pessina, V., & Dallar, G. (1993). Radionuclide content of building materials and gamma dose
rates in dwellings of Rio Grande Do Norte, Brazil. Radiation Protection Dosimetry, 48, 199}203.
Mustonen, R. (1984). Methods for evaluation of radiation from building materials. Radiation Protection
Dosimetry, 7, 235}238.
NEA-OECD, Nuclear Energy Agency (1979). Exposure to radiation from natural radioactivity in building
materials. Report by NEA Group of Expert, OECD, Paris.
O'Brien, R. S., Aral, H., & Peggie, J. R. (1998). Radon exhalation rates and gamma doses from ceramic tiles.
Health Physics, 75, 630}639.
Pimpl, M., Yoo, B., & Yordanova, I. (1992). Optimization of a radioanalytical procedure for the determina-
tion of uranium isotopes in the environmental samples. Journal of Radioanalytical Nuclear Chemisry
Articles, 161, 181.
Trubey, D. K. (1991). New gamma-ray buildup factor data for point Kernal calcultations. ANS-6.4.3.
Standard Reference Data.
Tufail, M., Mirza, S. M., & Khan, H. A. (1992). Natural radioactivity from building materials used in
Islamabad and Rawalpindi, Pakistan. The Science of the Total Environment, 121, 283}291.
Stranden, E. (1979). Radioactivity in building materials and the gamma radiation in dwellings. Physics and
Medical Biology, 24, 921}930.
UNSCEAR. (1993). Exposures from natural sources of radiation. Forty-second session of United Nations
scienti"c committee on the e!ects of atomic radiation, Vienna, 12}28 May.
R. H. Higgy et al. / J. Environ. Radioactivity 50 (2000) 253}261 261