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Internal Dosimetry Monitoring Detection Limits for a Selected Set of Radionuclides

and Their Translation Into Committed Effective Dose

A. Brandl, E. Hrnecek, F. Steger

Health Physics Division, ARC Seibersdorf research, 2444 Seibersdorf, Austria.


E-mail: alexander.brandl@arcs.ac.at

Abstract. To harmonize the practice of internal dosimetry monitoring across the country, the Austrian Standards
Institute is currently drafting a new set of standards which are concerned with occupational incorporation
monitoring of individuals handling non-sealed radioactive material. This set of standards is expected to consist
of three parts discussing the general necessity and frequency, the requirements for monitoring institutions, and
the determination and rigorous calculation of committed effective dose after incorporation of radioactive
material, respectively. Considerations of the requirements for routine monitoring laboratories have led to an
evaluation of the detection limits for routine monitoring equipment. For a selected set of radionuclides, these
detection limits are investigated in detail. The main emphasis is placed on the decay chains of naturally
occurring radionuclides showing some significant potential for being out of equilibrium due to chemical
processes in certain mining industries. The radionuclides considered in this paper are 226Ra, 228Ra, 228Th, 232Th,
234
U, 235U, and 238U. Given the routine monitoring intervals of the Austrian Standard, these detection limits are
translated into information on committed effective dose. This paper investigates whether routine monitoring
equipment is sufficient to ensure compliance with EC directive 96/29/Euratom for this selected set of
radionuclides.

1. Introduction

To harmonize the practice of internal dosimetry monitoring across the country, the Austrian Standards
Institute is currently drafting a new set of standards which are concerned with occupational
incorporation monitoring of individuals handling non-sealed radioactive material [1]. This set of
standards is expected to consist of three parts: Part 1: General necessity and frequency, Part 2:
Requirements for monitoring institutions, and Part 3: Determination and rigorous calculation of
committed effective doses after incorporation of radioactive material.

Upon completion of Part 2, considerations of the requirements for routine monitoring laboratories
have led to an evaluation of the detection limits for routine monitoring equipment. For a selected set of
radionuclides, mainly in the decay chains of naturally occurring radionuclides, which show some
significant potential for being out of equilibrium due to chemical processes in certain mining
industries, these detection limits are investigated in detail. Given the routine monitoring intervals
specified in Part 1 of the Austrian Standard [2], these detection limits are translated into information
on committed effective dose. The radionuclides under investigation are 226Ra, 228Ra, 228Th, 232Th, 234U,
235
U, and 238U. Future considerations are expected to extend this selection to also include additional
natural radionuclides, e.g., 227Ac and 231Pa.

This paper investigates whether routine monitoring equipment is sufficient to ensure compliance with
EU directive 96/29/Euratom [3] for this selected set of radionuclides. It determines whether the
monitoring suggested in the Austrian Standard for these radionuclides is sufficient to ensure that
workers in industries handling materials containing these naturally occurring nuclides can
unequivocally be classified to belong to Category A or Category B for occupational exposure, or
whether they can be considered members of the general public. This implies that the committed
effective dose at the detection limit must not exceed 1 mSv.

2. Methods and Materials

The routine monitoring intervals and methods recommended in the Austrian Standard are used as the
basis for the investigation of 226Ra, 228Ra, 228Th, 232Th, 234U, 235U, and 238U detection limits, expressed
in committed effective dose for these radionuclides, rather than in activity body or organ burden or in

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excreted activity concentration. The recommendations given in part 1 of the standard are shown in
Table I.

Table I. Monitoring intervals and methods, as recommended by the Austrian Standard.


Radionuclide Monitoring Interval (d) Monitoring Method
226
Ra 180 whole body counter, urine
228
Ra 180 whole body counter, urine
228
Th 90 urine
232
Th 90 urine
234
U 180 urine
235
U 180 urine, faeces
238
U 180 urine, faeces

Predicted values for their retention or excretion for the specific monitoring interval, taken from ICRP
78 [4], serve to compute the expected intake, considering their various absorption types. From the
intake, using the relevant dose coefficients [4,5], the committed effective dose is estimated for a
routine measurement result at the detection limit.

Typical detection limits for various measurement systems or methods and commonly used monitoring
equipment are given in Table II. The detection limits for whole body counter measurements for Ra are
the detection limits encountered at the whole body counting facility are the Austrian Research Centers
Seibersdorf, as are detection limits for alpha and gamma spectrometric measurements. Data on the
detection limits using inductively coupled plasma mass spectrometry, ICP-MS, are taken from the
literature [6-8].

Table II. Typical detection limits for commonly used monitoring equipment.
Radionuclide Monitoring Method Detection Limit
226 whole body counter 400 Bq
Ra
urine 0.5 mBq/d ( spectrometry)

228 whole body counter 600 Bq


Ra
urine 0.7 Bq/d ( spectrometry)
228
Th urine 0.5 mBq/d ( spectrometry)

232 0.5 mBq/d ( spectrometry),


Th urine
0.3 mBq/d (ICP-MS)
234
U urine 0.5 mBq/d ( spectrometry)

235 urine 0.5 mBq/d ( spectrometry)


U
faeces 2 mBq/d ( spectrometry)

0.5 mBq/d ( spectrometry)


238 urine
U 0.2 mBq/d (ICP-MS)
faeces 2 mBq/d ( spectrometry)

3. Results and Discussion

The committed effective dose at the detection limit for the various radionuclides, considering the
different absorption types and the monitoring intervals and methods given in the Austrian Standard,
are summarized in Table III. It is assumed that the incorporation of the radionuclide consisted of an
inhalation at a point in time at half the monitoring interval.

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Table III. Committed effective dose at the detection limit.
Radionuclide Monitoring Method Absorption Type Committed Effective Dose (mSv)
226 whole body counter M 29
Ra
urine M 0.24

228 whole body counter M 35


Ra
urine M 280

228 M 0.55
Th urine
S 33

232 M 0.66 ( spectrometry), 0.40 (ICP-MS)


Th urine
S 12 ( spectrometry), 7.2 (ICP-MS)

F 0.0027
234
U urine M 0.0088
S 0.79

F 0.0025
M 0.0075
urine
235 S 0.71
U
faeces S 0.11

F 0.0024 ( spectrometry), 0.00097 (ICP-MS)


M 0.0067 ( spectrometry), 0.0027 (ICP-MS)
238 urine
U S 0.66 ( spectrometry), 0.27 (ICP-MS)

faeces S 0.21

The monitoring programs suggested in the Austrian Standard are sufficient to unequivocally detect
committed effective doses below 1 mSv for the uranium isotopes 234U, 235U, and 238U. Whole body
counter measurements for 226Ra and 228Ra are not sufficiently sensitive for that determination.
However, 226Ra excretion measurements in urine can successfully be employed to that end. Excretion
measurements for 228Ra will not comply with the desired end point. For absorption type M, the
suggested measurement methods for 228Th and 232Th can distinguish between occupational exposure
and exposure for members of the general public. The methods investigated in this paper cannot
achieve a detection limit below 1 mSv for absorption type S for 228Th and 232Th.

The monitoring intervals suggested in the Austrian Standard for 234U, 235U, and 238U are not
recommended by ICRP 78 for absorption type F since the potential underestimate of the committed
effective dose for inhalation at the beginning of the monitoring interval is larger than a factor of 3. In
this study, given the monitoring interval suggested, the potential underestimate for uranium isotopes
with absorption type F is determined to amount to a factor of 4 if an inhalation at the beginning of the
monitoring interval is assumed. All other potential underestimates for the selected radionuclides and
absorption types have been verified to be smaller than the factor of 3 recommended by ICRP 78. The
potential overestimates due to inhalation towards the end of the monitoring interval range from a
factor of approximately 3 for 228Th and 232Th with absorption type S to a factor of approximately 34
for 228Ra. For the radionuclides and absorption types not recommended by ICRP 78 for the given
monitoring intervals, mainly the uranium isotopes with absorption type F, these potential
overestimates are higher still.

The use of sector field inductively coupled mass spectrometry for the determination of 235U and 238U or
232
Th in urine could lower the detection limit by at least a factor of 10 [8,9] compared to conventional
ICP-MS measurements. Under these circumstances, the suggested monitoring intervals and methods
for 232Th with absorption type S appear to become sufficient.

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4. Conclusion

For a selected set of naturally occurring radionulcides, 226Ra, 228Ra, 228Th, 232Th, 234U, 235U, and 238U,
the detection limits of commonly used routine internal dosimetry monitoring equipment together with
the routine monitoring intervals and methods suggested in an Austrian Standard are evaluated in terms
of committed effective dose. Compliance with EC directive 96/29/Euratom to determine whether
workers in certain industries handling materials containing naturally occurring nuclides have to be
classified as occupationally exposed personnel is investigated.

The monitoring programs suggested in the Austrian Standard are sufficient to unequivocally detect
committed effective doses below 1 mSv in most cases. The uranium isotopes 234U, 235U, and 238U can
be monitored by excretion measurements of urine or faeces, where applicable depending on the
absorption type. Whole body counter measurements for 226Ra and 228Ra are not sufficiently sensitive.
Excretion measurements of 226Ra in urine can successfully be employed. Excretion measurements for
228
Ra will not comply with the desired end point. For absorption type M, the suggested measurement
methods for 228Th and 232Th can are sufficient while the methods investigated cannot achieve a
detection limit below 1 mSv for absorption type S for these radionuclides.

The use of sector field inductively coupled mass spectrometry for 232Th determination in urine could
lower the detection limit compared to conventional ICP-MS measurements which appears to render
the suggested monitoring intervals and methods for absorption type S sufficient also.

Future considerations are expected to extend the selection of the currently investigated radionuclides
to also include additional natural radionuclides, e.g., 227Ac and 231Pa.

References

1. Austrian Standards Institute, NORM S 5220, Monitoring of Persons with Regard to Incorporated
Radioactive Materials, NORM, Vienna (2002).
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W., Holzmannhofer, J., Knig, F., Mandl, H., Msl, P., Mller, D., Plantusar, E., and F.
Schnhofer, NORM S 5220 - 1: Monitoring of Persons with regard to Incorporated Radioactive
Materials, Part 1: General necessity and frequency. A Regulation in Austria to protect Workers
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3. Council Directive 96/29/Euratom of 13 May 1996, Official Journal of the European Communities
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