Radiation Measurements

PERGAMON Radiation Measurements31 (1999) 223-226

or-PARTICLE RADIOACTIVITY FROM LR 115 BY TWO

METHODS OF ANALYSIS
K. AZKOUR*, A. NOURREDDINE*, J.C. ADLOFF**, AND A. PAPE**
* Laboratoire de Physique et Teclmiques Nucldaires, Facult6 des Sciences,
B.P. 20, E1 Jadida, Maroc
** Institut de Recherches Subatomiques, F-67037 Strasbourg Cedex 2, France

ABSTRACT
LRll5 track detectors were exposed to samples of Moroccan phosphate and
phosphogypsmn to measure their c~-particle radioactivity. Then two formalisms were used
for the dosimetry: simulation by a Monte Carlo method and determination of
concentrations from a numerically integrated track registration equation. The results were
compared with those deduced ~'-ray spectrometry.

KEYWORDS
LR 115; Monte Carlo method; detection probability; "/-spectrometry; contact autoradiography.

INTRODUCTION
In general sedimentary phosphates contain appreciable amounts of uranium and its daughters. The
thorium content is usually much lower. In Moroccan phosphates, the uranium concentration varies
between about 75 and 300 ppm, depending on the site (Khalil et al., 1995). While commercial
extraction of uranium from these materials has become less attractive nowadays, surveillance of the
by-products and waste for radioactivity has become an important ecological consideration.
In the present work, we will be interested in quantifying the concentration of cx-particle
emitters in naturally occurring samples of phosphate and phosphogypsum by three methods. From the
number of tracks registered in the solid state nuclear track detector LR115, we use two formalisms of
calculation, both using the degree of radioactive equilibrium deduced by 7-ray spectrometry, which is
the third method used as reference.

EXPERIMENTAL

Contact autoradiography
We have placed 1 x 1 cm ~- squares of L R I I 5 - I I in contact with 50 g samples of phosphate and
phosphogypsum inside 38 cm 3 closed cylindrical polyethyleue bottles (qb = 3.5 cm, h = 4 cm). After 20
days of irradiation, the detectors were etched in 2.5 N NaOH at 60°C for 2 h. The tracks over the
entire detector area were counted manually under a microscope (xl00) and by an automatic track
counting system (Boukhair et al.,1998) obtaining substantially the same numbers. For four detectors
in each of two samples, average track densities D = 0.0054 tracks cm -2 sj (phosphate) and 0.0017
tracks cm -2 s 1 (phosphogypsum) were found (~/D = 2.4 %). No significant differences in D were
observed for measurements made in closed or open bottles, which allows one to suppose that the rate
determining step in the 222Rn loss is its diffusion from the sample material and not leak from the
closed but not necessarily air-tight vials.

1350-4487/99/$ - see front matter © 1999 ElsevierScience Ltd.All rights reserved.

PII: S1350-4487(99)00099-2
224 K. Azkour et al. / Radiation Measurements 31 (1999) 223-226

),-ray spectrometry
The same samples were counted in a lead-shielded cave by a Ge(HP) diode having a FWHM
resolution of 1.75 keV and a peak/Compton ratio of 49 at 1332 keV. For energy and efficiency
calibration of the detector, a certified standard of mixed radionuclides (NG3 multigamma
QCRB4650, Amersham, 91944 Les Ulis, France) was counted in the same type of bottle in the same
geometry as the samples. The intensity of the various T-rays have been corrected empirically for the
apparent densities of p = 1.33 (phosphate) and 0.90 g/cm3 (phosphogypsum), the respective self-
absorption correction factors being 0.81 and 1.07 relative to the standard which consists principally of
H20.

CONCENTRATIONS FROM LRll5 TRACK DENSITY

Me~odl
Neglecting the 2 % radioactivity of the 232Th chain compared to that of the 23SUchain, and assuming
the radioactive equilibrium for members of 23SU chain deduced from the T-ray counting, the track
density D registered by the LR 115 can be obtained from the relation •
8
D = A u P Z RiPi(Er) (1)
i=l

where Au is the o~-particle radioactivity of 238U per unit mass of sample, p the density of the sample,
Ri the range of the cz-particles with Eai in the sample and Pi(Er) the detection probability
corresponding to the residual energy Er at the LR 115 detector surface.

The detection probability P(Er) as a function of o~-particle energy has been determined in other work
(Nourreddine et al., 1999). The residual energies Er for our thick samples were calculated using a
Monte Carlo code that takes into account the energy and angular conditions necessary for an o~-
particle to produce a track in LRI15 (1.4 < Ea _<4.7 MeV and the corresponding critical angles 0c).
In Table 1 are given the Monte Carlo simulated Er and the calculated detection probabilities for the
eight o~-particles emitted by the members of the 23SUseries.

Method11
This calculation (Pape et al., 1998) D is obtained by integration of the equation

A ~lR(E=4'7)ft0c sin0cos 0d0dR

D=2 R(E=14) 0 (2)

where A is the o~-particle activity in Bq/m3 and the energy-critical angle response ofLR 115 is
6
0c =ZcnEn . (3)
n=O

where E is the {x-particle energy in MeV and Co= -183.13, cl = -95.92, c2 = 479.02, c3 = -358.37,
c4 = 117.85, c5 = -18.32, c6 = 1.09. These coefficients were obtained by firing data from Barillon et
al. (1997).
The second degree polynomial

R = aE2 + bE + c (4)
 K. Azkour et al. / Radiation Measurements 31 (1999) 223-226 225

was used to describe the range-energy relationship of the sample material studied. Table 2 gives the
a, b, c coefficients fitted to the R-E results calculated by TRIM (Biersack and Ziegler, 1991). E is in
MeV and these a, b, c must be divided by the density p -- 3200 kg/m 3 for the phosphate and 9 = 2750
kg/m 3 for the phosphogypsum to have a consistent set of units for Eq.(5).
Numerical integration of Eq. (2) gives

D = A (2.518a + 0.413b) (5)

from which the activity of 238Ucan be deduced from a measured track density D as A~j = A/8.

Table 1. Uranium family or-particle energies E(x, ranges, average residual energy Er of (z-particles
leaving the samples, and Monte Carlo calculated probabilities Pir in LR 115.

Phosphate Phosphogypsum

Radionuclie E~ (MeV) Rmax (~m) Er (MeV) Pir Rmax Otm) Er (MeV) Pir

238U 4.19 12.46 1.82 0.047 13.46 1.80 0.048

234U 4.77 15.00 1.90 0.043 16.19 1.93 0.041
23°Th 4.69 14.64 1.91 0.042 15.80 1.92 0.042
226Ra 4.78 15.05 1.91 0.042 16.24 1.93 0.041
222Rn 5.49 18.49 2.18 0.032 19.87 2.23 0.030
218po 6.00 21.16 2.28 0.029 22.69 2.37 0.026
214po 7.68 31.23 2.90 0.017 33.17 2.88 0.017
21°po 5.30 17.53 2.12 0.033 18.87 2.17 0.032

Table 2. Fits of R = aE2+ bE + c to TRIM-computed ranges (in kg/cm2) for (x-particle energies
Between 1.4 and 4.7 MeV.

a b c

Phosphate (1.269 + 0.005) 10 -7 (1.364 + 0.031) 10 -7 (2.621 ± 0.039) 10 -7

Phosphogypsum (1.063 + 0.007) 107 (3.752 ± 0.041) 10 -7 (2.289 + 0.054) 10 -7

RESULTS AND DISCUSSION

In Table 3 are presented the specific activities of 238U in the phosphate and phosphogypsum
determined by the two methods of analysis of the LR I 15 track density and by y-ray spectrometry.
The LR115 measures the total o~-particle emissions but it does not yield the identity of the precursors.
A measurement (or assumption) of the degree of radioactive equilibrium, and of the absence of 232Th
family activity, was necessary to arrive at the activity of the 238U and consequently of each member of
its chain. While there is not a one-to-one correspondence between o~-emitters and y-emitters in the
radioactive families, it was possible to deduce from the ~/-ray spectrometry that the o~-particle
activities abo,~e and below 22ZRn in the decay series were in their respective radioactive equilibrium
for both materials. Then account was taken in the calculations of the diminished activity of 222Rn and
its daughters.
226 K. Azkour et al. / Radiation Measurements 31 (1999) 223-226

Both methods of analysis used for LRI 15 depend on a knowledge of the R-E curve of the tx-particles
and on the assumption that the o~-particle activity is dispersed in grains small enough to allow
detection by the LR115. The coherence of the 7-ray results, which are not sensitive to grain size, and
the L R l l 5 results lends credence that both the R-E and grain size conditions were fulfilled. One
might mention however that the composition and density of complex natural materials are not always
well known. The use of Eq. (5), which after a one-time numerical integration of the angular part of
Eq.(2) depends only on the R-E curve of the medium to be monitored, is more convenient to use in
practice than the Monte Carlo approach that requires a new calculation for each medium.

Table 3. Specific activities of 238Uobtained by LR 115 track detectors and Ge(HP) 7-ray spectrometry,
/'or phosphate and phosphogypsum.

Analysis Phosphate A~r(Bq/kg) Phosphogypsum Atr(Bq/kg)

LR 115 - Monte Carlo 3339 + 166 1155 + 58

LR 115 - Eq. (5) 3342 + 103 1393 + 43
y - spectrometry 3432 + 222 1140 + 112

CONCLUSION
The methods of o~-particle dosimetry presented in the present work are valid for determining
concentrations of o~-emitters in our samples. This allows making studies of different parameters
(sample composition, granulometry, leaching, radioactive equilibrium) intervening in the phosphates
and their by-products (fertilizers, phosphoric acid, phosphogypsum, etc.) and allows following these
activities throughout the industrial cycle.

Acknowledgments -- The authors wish to tank M. Benjelloual, M.G. Bontemps, A. Boukhair,

A. Haessler, M. Fahad and D. Oster for their help.

REFERENCES

Barillon R., Fromm M., Chambaudet A., Marah H. and Sabir A. (1997) Track etch velocity study in
a radon detector (LR115, cellulose nitrate). Radiat. Meas. 28, 619-628.
Biersack J.P. and Ziegler J.F. (1991) TRIM 91. Pergamon Press, New York.
Boukhair A., Haessler A., Adloff J.C. and Nourreddine A. (1998) Automatic measurements of or-
particle tracks in CR39 and LR115 with a digital CCD camera. This issue.
Khalil A., Membrey F., Fromm M. and Chambaudet A. (1995) A new method for determining
uranium and thorium contents in mineral mining materials. Appl. Radiat. 1sot. 46, 719-720.
Nourreddine A., Azkour K., Benjelloun M., Boukhair A., Fahad M. and Pape A. (1999) Monte Carlo
detection probabilities for SSNTD: application to uranium and thorium analysis in Moroccan
phosphates. J. Env. Rad. 42, 101-107.
Pape A., Adloff J.C., Barillon R., Haessler A., Hoernel A., Nourreddine A., Oster D. and
Weidmann D. (1998) Quantitative or-particle detection in a homogeneous medium with LR 115.
Nucl. lnstr. Meth. B 143, 557-560.