natural radioactivity of building materials
TRANSCRIPT
J.RADIOANAL.NUCL.CHEM.,LETTERS 103 /4/ 231-240 /1986/
NATURAL RADIOACTIVITY OF BUILDING MATERIALS
E. Tamez, M.T Olgu[n, N. Segovia, S. Bulbulian, F. Abascal
Instituto Nacional de Investigaciones Nucleares, Agricultura No. 21, Col. Escandon, C.P. 11800,
Mexico D.F., Mexico
Received 6 November 1985 Accepted 12 November 1985
Experiments were designed to measure trace uranium concentration and the rate of radon exhalation from masonry structural materials, both bare and surface finished and coated. LRII5 cellulose nitrate track detectors were used to record the alpha emission from structural material surface. Fission track, neutron activation and fluorometric analysis methods were used to determine the uranium content. Most types of paints studied will reduce alpha contribution and radon emanation from building materials.
INTRODUCTION
It has been known since the beginning of the centu-
ry that uranium is found in trace amounts in most of
the earth substances, including rocks and soils. The
element is relatively scarce in distribution, approximate-
ly 2 ppm /Ref. i/. 222Rn is a noble and alpha radio-
active gas, a member of the natural radioactive ura-
nium series. Building materials are commonly made
from the natural materials /sand, rocks, cement/ which
231 E~ev~r Sequom ~ A., Lausanne Ak~dmmi K ~ 6 , B ~ e s t
TAMEZ et al. : RADIOACTIVITY OF BUILDING MATERIALS
will contain traces of natural radioactive isotopes.
The half life of radon, 3.8 days, is long enough for
part of it to diffuse from the building material to
the inside of the room. The radon gas naturally
arising from the earth below, is added to those ex-
haled from the dwelling materials. The internal wall
decoration used to cover the building materials will
act in such a way as to decrease or increase this
emanation; this depends on whether the material acts as
a sealer against radon emanation or as a source of
radon.
A first mapping of radon in household dwellings in
Mexico City and neighbouring cities showed maximum 2
quantities in houses constructed within volcanic zones
In order to measure the radon contribution arising
from the building materials, an alpha emission survey
was made of the most commonly used masonry structural
materials in Mexico and the surface finishes and coat-
ings.
We report the effects of using different types of
paints, wall paper and plasters on the amount of alpha
contribution and radon emanation from building
materials.
EXPERIMENTAL
Masonry structural materials
Structural materials selected for study were: ordi-
nary kiln-fired bricks, cinder block, hollow compressed
kiln-fired bricks and quarried volcanic rock, both
as purchased from distributors and covered with dif-
ferent kinds of paints, plaster and plastic wall plaper
coating.
232
TAMEZ et al. : RADIOACTIVITY OF BUILDING MATERIALS
The structural materials were studied both coated
and bare except for the volcanic rock samples, which
were not coated since they are commonly used without
such finishes. 66 sample types resulted from varying
the combinations of masonry with surface covering
/5 types of masonry and 12 surface finishings plus
1 volcanic rocks/ as shown in Table i.
Analytical techniques
Track detection, activation analysis and fluoro-
metric techniques were used to determine radon and
uranium in samples.
A Triga Mark III nuclear reactor facility with -2 -i a thermal flux of approximately 1013 n cm .s was
used for uranium determination in masonry samples by
fission track technique and activation analysis.
Radon exhalation sampling by track detection. Measuring
arrangement
Disc-shaped film track detectors /LR!I5 from Kodak-
Pathe/ were utilized for measuring the alpha emission
from the masonry samples. The track detectors, red
dyed cellulose nitrate foils /adhered to a polyester
support i00 ~m thick/ were 12 ~m thick. Two sizes of
can 3 radon capture containers were used:
- The first one was a 32.7 cm 3 can where a detector
was placed upon a 3 mm high PVC supporting ring
which was set upon the surface of each masonry
sample. The internal diameter of the ring was 1.7
cm and the outer 2.7 cm. The sensitive side of the
detector faced downward to record alpha particles
emitted from the sample surface.
- The second container was a 103.7 cm 3 can. Detectors
were placed at the top of the can facing the mason-
233
TAMEZ et al.: RADIOACTIVITY OF BUILDING MATERIALS
g-4
0 o
u]
u~ 0
0 -,-I 0 ~h
o m o
-,-I
o
01
0 4J t~
~d
o o
r g~
0
o
t~ 0
n~
O
m �9 ,'4 ~ ]
�9 ~.t 0
, ~ 0
I
1
a
c6 0
0 -,.-t
~ 0 ~ m m 0
14
0 m
0
0 0
O
m t~
�9 ,-I 4-J
m ~ 0 -,~ 4J ",'~ o
-,~ �9 -,'~ -~
�9 -,-I O o ~ ~r
~ ~ 0 - ~ 0 ~ ~ ~ ~ ~.,-~
0 ~
O 0 0 ,-q m
O~
0 ~ -,~ �9 0 -~ -~
O~ t~ m Cl O~ 0 ~; �9 ~ Z o
0 ~ ~ ~l ~l o 0 .~ .,-~ 0
r o t~
�9 ,4 ~ ~ 4~ ~ ~ �9
D.~ ~ ml .,-4 .,..4 ~ -,-4 ~
�9 ,-4 -,~ ,.-4 -~ ~ ,-4
0 Z~ 4~ ~ .~ O ~ 0 -,~ 4J ,--I o m �9 �9 m 0 4J D~ 4J ~ m . ,-.I 0 ~ �9 Z~ ~ ~ -,--I .,..-I ~ ml: �9 ~ ~ ,-..-I ,...-4 ,.-.I ..~ ~ ..~ ~ ,-I-,
LO ~0 P" CO O~ 0 ,--I C~ rO ,--~ ~ ,--I
oo ~ ~-~ ~ ~-I r 0 0 ~-~
0 0 �9 ,-I -~ I I
�9 ,~ -~ 0
�9 oJ h h ~ n3h 0
-4 ,4 0 ~ �9 ,.c:l -,-4
0 -,q 0 -4
~ ~ H ~ 3 h .,4
,4 o -,.~ �9 , - - 4 0 ,-.4 �9 q21 1.4
1.4 >~ ~ ~ O- -4 O - ' 4 -,4 O ~ O E ~ ~ q - 4 ~ q . 4 rJ C~
Z ~ 0 0 ~" ~ 0
E~ ~ ~ Ea
2 3 4
TAMEZ et al. : RADIOACTIVITY OF BUILDING MATERIALS
40
I" 2.8 ,
e
Dimens ions in cm
�9 containers: A/ 32.7 cm can. B/ Fig. 1 Radon capture 3
103.7 cm ~ can. a - radon capture containers, b - PVC rings, c - track detectors, d - sensitive side, e - masonry structural material
ry. 222Rn and daughters alpha particles were re-
corded in this assemblage. Both sizes of can were
sealed to the surface of each masonry sample /Fig. i./.
The detectors were left for exposure for 55 days.
After this period all cans were removed at the
same time.
Track etching and track c0untin q
After exposure, to enlarge the alpha tracks the
detectors were immersed in an etching solution of
2.5N NaOH at 56~2 ~ for 3 h. The newly-etched
detectors were then stripped from the support layer
and the tracks counted with a spark counter 4. A
uniform residual thickness of the detectors had to
be achieved in all etched detectors for consistency
of results.
235
TAMEZ et al. : RADIOACTIVITY OF BUILDING MATERIALS
The results of track counting of the detectors are 2
reported in number of tracks per cm per week.
Uranium determination
Uranium content in the samples was determined by
fission track, neutron activation and fluorometric tech-
niques.
Fission track technique
Powdered brick samples of 250 mg were~pressed into
pellets and placed in an irradiation container in contact
with policarbonate detector for fission track recording.
The samples and detectors were irradiated in the nuclear
reactor for 15 min. After irradiation the detectors were
etched for 60 min in a 2.5N NaOH solution at 56+2 ~
and the etched tracks microscope counted. Calibration
of the method was performed with NBS glass standards
with uranium contents of 0.02 and 1 ppm.
Neutron activation and fluorometric techniques
Uranium was chemically separated from the masonry
samples. They were crushed and powdered and uranium
extracted by a leaching out method previously reported 5.
After separation the uranium fraction was used for
analysis by neutron activation and fluorometry techniques.
RESULTS AND DISCUSSION
The results of the alpha track survey experiments
from bare masonry samples and from the 12 combinations
of surface finishings and coatings are summarized in Figs
2. and 3. Figure 2. shows results from track detectors
placed at 3 mm upon the surface of each masonry sample.
236
TAMEZ et al. : RADIOACTIVITY OF BUILDING MATERIALS
1 2 3 4 5 6 7 8 9 10 11 12 13 Codes
Fig. 2. Alpha record /tracks cm-2.week/ from masonry
structural materials and coatings in bottom track detectors. Masonry and coatings are codified as sDecified in Table i. a - TRN; b - TRH; c - TRC; d - TOC; e - T; f - L
-~ 250
200
~ 150
lie
I 2 3 4 5 6 7 8 9 10 11 12 13
Codes
Fig. 3. Alpha record /tracks cm-2.week/ from masonry structural materials and coatings in top track detectors. Masonry and coatings are codified as specified in Table i. a - TRN; b - TRH; c - TRC; d- TOC; e - T
3 237
TAMEZ et al. : RADIOACTIVITY OF BUILDING MATERIALS
In this figure the ordinate is the number of tracks -2
cm .week while the abscissa corresponds to the codes
defined in Table 1 for the superposition of plasters,
paints, varnish and plastic wall paper coatings on
the ordinary kiln-fired brick, cinder block and hol-
low compressed kiln-fired brick structural materials
/except volcanic rock that appears uncoated/. The high-
est alpha contribution values are observed for uncoat-
ed hollow compressed kiln-fired bricks /code 1/I \
Comparing the effects of different types of paints
with that of alternative covers on the alpha measure-
ment it appears that yellow, green and blue enamel
paints are most efficient in reducing the alpha emission.
Generally paints /codes 4-9/ reduced the alpha emission
to at least one fourth of the bare brick values, while
the white vinyl base paint reduced it only to one half
in the hollow compressed kiln-fired bricks /TRC and
TOC! and did not reduce alpha emission for the other
structural materials. The likely speculation is that white
paint contains enough natural alpha active materials
which compensate for the alpha absorption from structural
materials. Using varnish and plastic wall paper cuts
the alpha contribution in a similar way as the coloured
paints showing only a slight alpha contribution.
Figure 3. shows the results in the detectors exposed
at 5 cm upon the surface of each masonry sample. This
analysis indicates a reduction in radon emanation when
masonly samples are covered.
Theoretical estimation of the LRII5 des
response using the relations reported by Somogyi et al 6 .
indicates that for the 103.7 cm 3 can, a record of 29.82 -3
tracks cm .30 days, corresponds to a radon concentra-
tion of 1 pCi i-i; therefore the maximum radon concentra-
tion /for the TRC structural material/ is approximately
2 3 8
TAMEZ et al. : RADIOACTIVITY OF BUILDING MATERIALS
-i 32 pCi 1 . The study of the uranium content in the
masonry materials showed that uranium concentration for
TRC and TOC samples were found to be at least two times
higher /in average 1.6 and 1.2 ppm, respectively/ than
the other structural materials /which had in average
0.6 ppm/. From the previous observations, the more like-
ly explanation for the effect of paint on reducing ra-
don emanation from the bricks is that it acts as a
sealer to the pores between the grains, thus reducing
the gas emanation.
Figure 3. shows that TRC, the material with higher
uranium content, produces higher radon emission; those
structural materials which have lower uranium content
favour the radon emission, particularly TRN ordinary
kiln-fired bricks, probably as an effect of the high
porosity of the material Comparison of Figs 2. and 3.
indicates that the number of tracks registered in the
bottom detectors is a measure of 238U, 234U and other
alpha emitting elements of the natural radioactive
chains, including 222Rn, present in the upper layer of
the masonry materials while the top detectors show the
measurements of the 222Rn gas liberated from the mason-
ry materials and the coatings.
ONCLUSIONS
Building materials studied showed an alpha contri-
bution that depends on the uranium content of the
samples. Coatings reduced the alpha emission except
in finishes that contribute by themselves to the alpha
emission. In general radon emission depends on the
uranium content of masonry but porosity of the ordi-
nary kiln-fired bricks favours the radon emission
~* 239
TAMEZ et al. : RADIOACTIVITY OF BUILDING MATERIALS
compensating in this way the effect of low uranium
content. Coatings reduce the radon emission.
Results obtained in the present work show that
contribution of radon in household dwellings as re-
ported in Ref. 2 can be partially explained by the
emission from building materials.
x
The authors wish to thank the Triga Reactor staff,
from the Nuclear Center of M~xico for their colla-
boration in irradiation and activation analysis sup-
port; Dr. C. Collins for her relevant suggestions
and C. Martlnez for technical assistance.
REFERENCES
i. D.K. Evans, Health Physics, 17 /1969/ 229.
2. N. Segovia, J. Cejudo, Nucl. Tracks Rad. Meas., 8 /1984/ 407.
3. F. Abu Jarad, H. Fremlin, Health Physics, 44 /1983/ 243.
4. L. Maldonado, R. Linares, T. Morales, N. Segovia, Technical Report, ININ AII-82-19, 1982.
5. J. Korkisch, F. Abascal, C. Aguilar, Rev. Lat. Am. Quim., 4 /1973/ 165.
6. G. Somogyi, B. Parip~s, Z. Varga, Nucl. Tracks Rad. Meas., 8 /1984/ 423.
240