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Critical remarks on gross alpha/beta activity

analysis in drinking waters: Conclusions from a
European interlaboratory comparison
ARTICLE in APPLIED RADIATION AND ISOTOPES: INCLUDING DATA, INSTRUMENTATION AND METHODS FOR USE
IN AGRICULTURE, INDUSTRY AND MEDICINE DECEMBER 2013
Impact Factor: 1.23 DOI: 10.1016/j.apradiso.2013.11.073 Source: PubMed

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Applied Radiation and Isotopes 87 (2014) 429434

Contents lists available at ScienceDirect

Applied Radiation and Isotopes

journal homepage: www.elsevier.com/locate/apradiso

Critical remarks on gross alpha/beta activity analysis in drinking

waters: Conclusions from a European interlaboratory comparison
V. Jobbgy n, J. Mereov, U. Wtjen
European Commission, Joint Research Centre, Institute for Reference Materials and Measurements, Retieseweg 111, B-2440 Geel, Belgium

H I G H L I G H T S

Gross alpha/beta standard methods for drinking water analysis are discussed.
Large spread of results (up to 2 orders of magnitude) observed in comparisons.
Sources of interferences are reviewed.
We propose to use true standardized methods to obtain better measurement results.

art ic l e i nf o

a b s t r a c t

Available online 1 December 2013

The most common gross alpha/beta standard methods used for drinking water analysis are discussed,
and sources of interferences are reviewed from a metrological point of view. Our study reveals serious
drawbacks of gross methods on the basis of an interlaboratory comparison analyzing commercial mineral
water samples with the participation of 71 laboratories. A proposal is made to obtain comparable
measurement results using true standardized methods.
& 2013 Elsevier Ltd. All rights reserved.

Keywords:
Gross alpha/beta activity
Drinking water
Interlaboratory comparison
Radioactivity
Limits of gross methods

1. Introduction
Gross alpha/beta activity measurement is applied widely as a
screening technique in the eld of radioecology, environmental
monitoring and industrial applications. Water intended for drinking purposes has to be analyzed rst for gross alpha/beta activity
content according to many different national and international
standards and recommendations. Anticipating the new European
Union (EU) Drinking Water Directive (EC, 2012) which incorporates gross alpha/beta activity screening levels, the Institute for
Reference Materials and Measurements (IRMM) organized an
interlaboratory comparison (ILC) to check the tness for purpose
of this method and the performance of European monitoring
laboratories. On the basis of the reported values from the 71
participating laboratories, we review some of the most inuential
parameters on gross measurements.
The claimed main advantages of the gross alpha/beta methods
are the relatively low costs, rapidity and simplicity. Although it is
one of the simplest, it is also one of the most disputed radioanalytical
methods because the determination of gross alpha and beta activities

n
Corresponding author. Present address: SCK
CEN, Belgian Nuclear Research
Centre, Boeretang 200, B-2400 Mol, Belgium. Tel.: 32 14 33 32 38.
E-mail address: viktor.jobbagy@mail.com (V. Jobbgy).

0969-8043/$ - see front matter & 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.apradiso.2013.11.073

faces some specic problems that may refute the afore-mentioned

claims. There are many sources of interferences in gross alpha/beta
measurement that may corrupt the comparability of the measurement
results (Arndt and West, 2004; Rusconi et al., 2006; Semkow et al.,
2004; Montaa et al., 2012). First one is related to the radionuclide
composition of the sample. During gross alpha/beta activity measurement, a mixed radionuclide composition must be simultaneously
measured. Drinking water samples may contain different naturally
occurring alpha (238U, 234U, 232Th, 226Ra and 210Po) and beta (40K, 228Ra
and 210Pb) emitters, and articial radionuclides (241Am, 90Sr) in various
concentrations (UNSCEAR, 2000). Moreover, most of these are members of a complex decay chain, therefore the ingrowths of the daughter
products inuence the measurement result.
The second important source of interference is due to the nal
source thickness that causes self absorption of the emitted particles
already in the source itself. In this respect, it is crucial to use
standardized methods (Jobbgy et al., 2010). The WHO recommends
that, "Where possible, standardized methods should be used to
determine concentrations of gross alpha and beta activities" (WHO,
2011). For this reason, the most common standard methods based
on direct evaporation, co-precipitation and liquid scintillation counting are discussed in this paper with respect to the sample
preparation and counting techniques. Regarding the measurement
methods, the inuence of the following parameters must be considered: counting efciency, self absorption, moisture absorption,

430

V. Jobbgy et al. / Applied Radiation and Isotopes 87 (2014) 429434

chemical recovery and the interferences due to the isotopic composition of the water sample. Experimental comparisons of the
gross alpha/beta standard methods were done using real drinking
water samples with different salinity and radionuclide activity
concentration.
Besides the pitfalls of the gross measurements, the paper also
tries to give examples where gross measurements can be used as a
rapid alternative technique to the radionuclide-specic analysis.

2. Materials and methods

2.1. Reagents
All the chemicals (conc. H2SO4, FeCl3, BaCl2) were analytical
grade and all the stock solutions were prepared using de-ionized
water. Three water samples, with different salinity and radionuclide activity concentrations, were used for the described
experiments and in the interlaboratory comparison. Two water
samples (Water A and B) were commercially available natural
mineral waters. The third one (Water C) was prepared by spiking
de-ionized water with a known activity of 241Am and 90Sr/90Y
solutions standardized at IRMM by liquid scintillation counting
using the CIEMAT/NIST method. The total dissolved solid was set
to a nal total concentration of about 10 mg/L by adding the
following inactive inorganic salts: NaCl, CaCl2 and Sr(NO3)2. The
major sources of gross alpha activity for Water A are 234U and 238U
(  40 mBq/L each), for Water B this is 226Ra (  330 mBq/L) and for
Water C 241Am (  950 mBq/L).

2.2. Sample preparation

Sources were prepared in accordance with ISO 9696/9697
(thick source method) or ISO 10704 (thin source method).
The surface density of a source prepared under ISO 9696/9697
must exceed 10 mg/cm2. An aliquot of sample was evaporated to
dryness, and the dried residue converted to sulfate form by
sulfuric acid and ignited at 350 1C for an hour (ISO 9696, 2007;
ISO 9697, 2008). The surface density of the source in the thin
source method must be below 5 mg/cm2, and has been described
previously (ISO 10704, 2009; Montaa et al, 2012; Suarez-Navarro
et al., 2002). The pH of the ltered water sample was adjusted
with sulfuric acid and heated to purge radon and CO2. Then the
radium isotopes were co-precipitated as Ba(Ra)SO4, whereas
uranium, thorium and polonium isotopes are co-precipitated with
Fe(OH)3 after pH adjustment (pH E78) (ISO 10704, 2009;
Suarez-Navarro et al., 2002).

2.3. Gross counting system and activity calculation

For the gross alpha/beta measurement, a 10-detector, lowbackground gas-ow proportional counting system was used.
The high voltage was set to 1450 V and the counting gas (Ar/
CH4, 90/10) ow was kept stable with a ow rate of  25 mL/min.
The gross alpha/beta count of the ltered/dried precipitate was
measured in 5 h cycles repeating it several times (from three to
twelve cycles).
For the counting efciency and self absorption experiments,
241
Am and 90Sr standard solutions were used, since these are the
most frequently used radionuclides for this purpose. Gross alpha/
beta activity concentrations were calculated from count rates by
following the formulae of the corresponding ISO standard (ISO
9696, 2007; ISO 9697, 2008; ISO 10704, 2009; ISO 11704, 2010).

3. Results and discussion

3.1. Summary of the interlaboratory exercise
After radiochemical characterization of the three water samples at IRMM, they were sent to the European monitoring
laboratories for gross alpha/beta analysis. The gross alpha/beta
reference values were determined independently from the laboratory comparison from the results determined by the three laboratories involved in the reference value determination (Table 1).
Water C is, in principle, the easiest sample to measure since its
gross alpha/beta activity concentration is the highest among the
ILC samples. However, from a measurement point of view, the
gross alpha activity is not the only key factor, but the alpha/beta
emitting radionuclides and the total dissolved solid content have
to be considered as well. Taking into account all three factors one
can make an order of difculty in terms of measurement as
follows: Water C oWater A rWater B.
As is evident from the reported results (Fig. 1 and 2), the
outcome of the laboratory comparison exercise is far from satisfactory. The measurement results span a wide range, e.g. for Water
C the maximum reported gross beta activity was more than 3000
times higher than the minimum reported gross beta activity.
Furthermore, several laboratories (no. 49, 50 etc.) present for
one type of sample a measurement result several times higher
than the reference, whilst for another type of sample the same
laboratory has a result several times lower. The gross alpha activity
results for Water C (spiked sample, i.e. the best case scenario) are
sorted according to the applied counting techniques in Fig. 2.
For Water A and B (natural waters) we could observe a similar
data spread but with a higher degree of variation for each
technique. Possible reasons for the diversity of results are given
in the next sections, but a detailed evaluation of the laboratory
comparison itself will be published later in a separate report.
3.2. Method comparison
It is well-known that the sample form or geometry play a
signicant role in producing reliable results from thicker sources,
requiring a uniform thickness and a homogeneous layer of residue
material on a planchet (60 mm in diameter). The surface density,
inuencing the self absorption of alpha and beta particles, should
be controlled and determined very carefully (ISO 9696/9697; ISO
10704; Montaa et al., 2012; Suarez-Navarro et al., 2002; Semkow
et al., 2004; Parsa, 1998). A surface density higher than 10 mg/cm2
(ISO 9696/9697) achieves satisfying counting statistics and constant self absorption. The self absorption of the alpha and beta
particles limits their counting efciency to usually less than 50%.
It should be mentioned that no energy resolution is possible with
proportional counters.
Since the sample is evaporated and later heat-treated, ISO
9696/9697 does not allow determination of the volatile radionuclides (e.g. 3H, 210Po, 137Cs), which escape from the sample and
Table 1
The reference activity concentration values (Aref) in the ILC water samples with
their expanded uncertainties (Uref) with a coverage factor k 2. Reference values
determined by three laboratories external to the laboratory comparison.
Parameter

Reference value with expanded uncertainty

Aref 7 Uref (mBq/L)
Water A

Gross alpha activity

47.5 7 22.8
Gross beta activity
309.8 7 57.4
Total dissolved solids (mg/L)
955 7 44

Water B

Water C

434.7 7 56.6
190.4 7 32.6
3647 27

954.5 7 77.3
1037.3 7 83.0
10.2 7 0.1

V. Jobbgy et al. / Applied Radiation and Isotopes 87 (2014) 429434

431

Fig. 2. Laboratory results of gross alpha activity concentration sorted by techniques

for Water C. The solid line indicates the reference activity concentration (Aref) of
gross alpha activity. Its corresponding expanded uncertainty 7 Uref (k 2) is plotted
as dashed lines.

determination possible, no conclusion can be drawn on the

chemical recovery. It should be stressed that in the case of real
water samples it is difcult to quantify this without further
analysis as the original chemical composition is not always known
accurately. From the chemical composition of the sample, the
excess precipitate formed from the original inorganic cations could
be quantied.
Second, 40K cannot be included in the gross beta result because
it stays in the nal supernatant. For this reason, the gross beta
results obtained by co-precipitation methods are always lower
than the true gross beta values. The 40K content has to be
separately determined with either a radiometric method (low
background gamma-ray spectrometry) or with a non-radiometric
method (emission ame photometry).

3.2.1. Liquid scintillation counting (ISO 11704)

Ultra low-level /-discrimination LSC, due to its high detection efciency (up to 100%) and low background count rate, is a
useful tool for the determination of alpha- and beta emitting
radionuclides (Schnhofer, 1995). The basic steps of the sample
preparation for liquid scintillation counting are very simple. It
consists of a thermal pre-concentration, pH adjustment and
sample mixing with scintillation cocktail (ISO 11704, 2010).
Advantages are:
Fig. 1. Laboratory results for gross alpha/beta activity concentration for different
water samples. The solid lines indicate the reference activity concentrations (Aref) of
gross alpha and gross beta activity, respectively. Their corresponding expanded
uncertainties 7 Uref (k 2) are plotted in dashed lines.

the residue during heat treatment. Therefore, the gross alpha and
beta activity concentration might be underestimated. For instance,
210
Po losses, varying with the chemical form of the element, have
been reported beginning above 100 1C (Momoshima et al., 2002;
Matthews et al., 2007). However, ISO 9696 claims that losses of
polonium are not expected for samples which have been acidied
with nitric acid and subjected to sulfation and treated at 350 1C
(nitrate salts have been converted to the sulfate form).
Some of these drawbacks of the thick source approach can be
avoided by using co-precipitation of the water sample (SuarezNavarro et al., 2002; ISO 10704). On one hand, this method needs
more chemical treatment than the evaporation methods. On the
other, more uniform and homogeneous residues can be obtained,
especially for higher salt concentrations (e.g. in mineral waters).
However, it suffers from two very severe drawbacks. Firstly,
since neither is a radiotracer applied nor is gravimetric yield

no self absorption occurs in the sample,

LSC methods can be adapted to monitor low-energy beta

emitters such as 3H and 14C (Schnhofer, 1995; Gruber et al.,

2009), and
radon in water can be determined separately using liquid
scintillation methods (Salonen, 2010).

One of the disadvantages is quenching (chemical, color and

physical) which reduces the counting efciency; therefore, a
quench correction must be made. Furthermore, the separation of
beta energies from all alpha energies can be difcult, because it
depends on many factors in LSC counting (Rusconi et al., 2006;
Schnhofer, 2012). For this reason, the optimal setting of the
different parameters (type of the vial, cocktail, / pulse discrimination, counting efciency) is essential for gross alpha/beta
measurements by LSC. Many other factors like the physical or
chemical behaviour of the radionuclides, dissolved ions and the
energies of the emitted particles may inuence the detection, too.
As stated by Rusconi et al. (2006) the same settings should be used
during measurement and calibration.

V. Jobbgy et al. / Applied Radiation and Isotopes 87 (2014) 429434

3.3. Sources of interferences

3.3.1. Self absorption
Most gross alpha/beta standard methods apply proportional
counter or solid state scintillation counters as detector (ISO 9696,
2007; ISO 9697, 2008; ISO 10704, 2009). The counting efciency of
these methods is strongly affected by the total dissolved solids and
the surface density of the sample. The direct evaporation approach
of ISO 10704 allows the use of a binding agent that contains a
polymer to produce evenly spread counting sources (ISO 10704,
2009). This polymer stays on the planchet, increasing the surface
density which cannot exceed 5 mg/cm2. To get equivalent alpha/
beta self-absorption for the sample and the calibration source in a
multi-component microchemical environment is not easy to
accomplish. The sample and the calibration source must be as
similar as possible in terms of surface density, homogeneity, and
distribution of radioactivity in the precipitate. The sequence of
precipitation during evaporation, which is related to the solubility
of the dissolved compounds, also inuences self-absorption
(Zikovsky, 2000). During our experiments, the typical surface
density for the ISO 10704 method varied in the range of 0.8
1.3 mg/cm2. The self absorption factor for gross alpha counting
was 0.927 0.03 at 0.5 mg/cm2 and 0.57 70.02 at 1.5 mg/cm2.

3.3.2. Time delay and radon ingrowth

Radon ingrowth can result in variations of count rate and
measurement result. Many natural waters contain 226Ra at up to
several Bq/L concentration. From a measurement point of view,
progenies of 226Ra play a signicant role in gross alpha/beta
measurements since they are produced from 226Ra continuously
after the source preparation and contribute to the gross count
rates which can vary as a function of time. A measurement started
immediately after source preparation, as required in ISO standards,
renders lower gross alpha activity than a delayed measurement as
shown in Fig. 3. Careful control of timing, such as the elapsed time
between source preparation and start of measurement and measurement duration, are absolutely required.
One approach is to wait for secular equilibrium between
226
Ra/222Rn and its progenies (  30 days) before measurement.
To reach equilibrium with certainty is, however, difcult to assess,
since 222Rn can escape from the source itself. To quantify the
escaped/emanated radon fraction (i.e. the level of equilibrium) is
difcult because the microstructure and density of the dry residue
inuence the emanation rate.
Parsa (1998) pointed out that short-lived 224Ra (T1/2 3.64 d)
can remain undetected because of the time delays between
sampling and routine gross alpha analysis. In order to assess the
224
Ra contribution, the gross alpha activity should be performed as

soon as possible after the time of sampling. In addition, the

duration of the drying step may vary, leading to an unknown
increase in gross count rates.
3.3.3. Calibration
Since determination of self-absorption is a crucial step, calibration standards must be appropriate for the measurement samples
(e.g. electrodeposited standard sources cannot be used for calibration of dry precipitate samples). The counting efciency of certain
counters shows energy dependence (ISO 9696; Semkow et al.,
2004; Montaa et al., 2012). Therefore radionuclides used for
efciency calibration have to be carefully selected. Finally, spatial
variation of the counting efciency may also occur for proportional
counters as shown in Fig. 4, which means that a calibration source
with the same diameter as the sample should be used and both
sources must be positioned relative to the counter in the
same way.
3.3.4. Moisture
Moisture has to be controlled and kept constant during the
measurement to maintain stable measurement conditions. Some
of the participants did not take this into account. Applying the
direct evaporation approach, the adsorption of moisture from
ambient air can be comparable (up to 40%) to the net mass of
dry residue. If nitrates are still present, most dry residues are
hygroscopic. Mass change of the sample can continue during
measurement affecting signicantly the self absorption.
3.3.5. Sources of bias and uncertainties
Details on sources of uncertainties for gross alpha/beta measurements are given in Table 2.
40
35
30

Alpha count rate (cpm)

432

25
20
15
10
5
-3

-2

-1

0
1
Distance from the detector centre (cm)

Fig. 4. Spatial variation of the alpha count rate for a proportional counter (error
bars represent the uncertainty from the counting statistics, with k 2).

Alpha count rate (cpm)

6.0
5.5

Table 2
Uncertainty budget for ISO 10704 gross alpha/beta activity concentration measurements in water samples (Water A-B-C), giving the standard uncertainties (1 s) for a
single measurement of a single sample (5 h counting time) measured at IRMM.

5.0
4.5

y = 0.036x + 2.317

4.0

R2 = 0.967

Uncertainty component

Gross alpha
(%)

Gross beta
(%)

Counting statistics (minmax)

Counting efciency/Self absorption
Volume of the test sample
Calibration source
Weighing
Chemical yield
Partialn combined standard uncertainty (uc)
(minmax)

2.512.4
4.5
0.5
1
0.2
Not known
5.313.2

1.86.5
3.1
0.5
1
0.2
Not known
3.87.3

3.5
3.0
2.5
2.0

20

40

60

80

100

Elapsed time (hours)

Fig. 3. Variation of alpha count rate due to the ingrowth of 226Ra progenies in the
co-precipitated source (error bars represent the uncertainty from the counting
statistics, with k 2).

Excluding chemical yield.

V. Jobbgy et al. / Applied Radiation and Isotopes 87 (2014) 429434

Not unexpectedly, the major contributions are counting statistics and self absorption. The uncertainty due to sample preparation (sample volume, weighing) contributes only 1.1% to the
combined standard uncertainty. There can be a signicant bias
due to the variation of counting efciency as a function of alpha
particle energies and from the tting of the self-absorption curve.
The bias from the counting efciency can be up to 75% (ISO 9696),
making the appropriate calibration and determination of selfabsorption absolutely crucial. We obtained approximately 20%
bias using different electrodeposited and drop deposited calibration sources (for alpha energies of 4 MeV to 7 MeV). However,
positioning of these sources was more important as shown in
Fig. 4. The uncertainty from chemical yield cannot be quantied,
since the determination of the chemical yield itself is difcult in
the case of the co-precipitation approach of ISO 10704. Due to
chemical manipulations, the yield can never be assumed to be
100%. Loss of precipitate occurs during the ltration step and some
precipitate can adsorb to the walls of the glassware as was
observed in these experiments.

433

are analyzed. It should be noted, however, that there is one

parameter that cannot be xed as analysts simply cannot control
it: the original radiochemical composition of the samples.
Replacing gross methods of drinking water analysis with
radionuclide-specic methods would not take a lot of effort or
expense. Radionuclide measurements can be done using the same
instrumentation (gas-ow proportional counter, liquidand solid
scintillation counter) that are used for gross alpha/beta analysis.
Only more expertise/prociency and validated methods are
needed, but in a routine radiochemistry laboratory they should
already exist. Routine laboratory measurement protocols must be
up-dated to the new food safety-, health- and environmentrelated challenges where rapid, specic and accurate responses
are needed. There are simultaneous methods that allow performing multi-radionuclide analysis focusing on the main naturally
occurring radionuclides of interest (226Ra, 228Ra, 210Po, 210Pb, and
the uranium isotopes) with a comparable speed to gross alpha/
beta methods such as described by Chalupnik and Lebecka, 1992;
Vajda et al., 1997; Schnhofer and Wallner, 2001; Eikenberg et al.,
2004; Benedik et al. 2009; Jia et al., 2009.

4. Conclusions
Acknowledgments
4.1. Recommendations for the gross alpha/beta method applied
to drinking water analysis
It was shown that gross methods are not as simple as usually
stated (Montaa et al., 2012; Semkow et al., 2004), and they are far
from accurate. In some cases they fail to determine certain radionuclides, therefore they give only an activity index rather than
an approximate activity concentration, as shown by Schnhofer
(2012) and conrmed by the data spread from this laboratory
comparison. The difference between laboratory results in this ILC
is sometimes two or three orders of magnitude, which is far
beyond the measurement uncertainties. These ndings lead us to
conclude that gross alpha/beta methods are not t to be used as an
independent method to assess activity concentration. Gross measurement should be used for monitoring only after the radionuclide composition is known from radionuclide specic analysis
of representative samples. It can be used as a complementary or
substitute method for radionuclide-specic measurement only
with important restrictions: (1) no temporary change is expected
in the radiochemical composition (no signicant ingrowth of
progenies during the measurement); (2) no complex decay chains
are present; (3) a true standardized method is used; and (4) the
measurement parameters are xed. Radionuclide specic analysis
should be repeated on a regular basis in accordance with the
drinking water directive concerning check and audit monitoring
(EC, 1998). Any suspected change in parameters requires more
frequent nuclide specic analysis.
4.2. True standardization of methods
The main reason for unreliability of gross methods and
the noncomparability of gross alpha/beta measurement results is
the lack of knowledge of the real radionuclide composition of the
water. Since there are many variables playing a key role in gross
measurement (Arndt and West, 2004; Semkow et al., 2004;
Jobbgy et al, 2010; Montaa et al., 2012), it is important to x
as many parameters as possible. The radionuclides used in the
calibration, the geometry of the source, quenching parameters, the
chemical form and any time delay must be clearly dened.
Acceptable time delays for each step (e.g. between sampling and
sample preparation, source preparation and start of measurement)
must be set in the written measurement standards, which is
particularly important when 226Ra- and 224Ra-containing waters

The authors wish to thank Pieter Kwakman (RIVM, The Netherlands), Edmond Dupuis (SCK
CEN, Belgium), Timotheos Altzitzoglou, Mikael Hult and Andrej Rozkov (EC-JRC-IRMM, Belgium) for
their contributions to the reference value determination.
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