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Effective dose in SMAW and FCAW welding processes using rutile consumables

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| Society for Radiological Protection Journal of Radiological Protection

J. Radiol. Prot. 34 (2014) 133–148 doi:10.1088/0952-4746/34/1/133

Effective dose in SMAW and FCAW


welding processes using rutile
consumables
M Herranz, S Rozas, R Idoeta and N Alegrı́a
Departamento de Ingenierı́a Nuclear y Mecánica de Fluidos, ETSI de Bilbao,
Universidad del Paı́s Vasco UPV/EHU, Alameda Urquijo s/n, E-48013 Bilbao, Spain

E-mail: m.herranz@ehu.es and saroa.rozas@ehu.es


Received 28 July 2013, in final form 25 September 2013, accepted for publication
1 October 2013
Published 13 December 2013

Abstract
The shielded metal arc welding (SMAW) and flux cored arc welding (FCAW)
processes use covered electrodes and flux cored wire as consumables. Among
these consumables, ones containing rutile are the most widely used, and since
they have a considerable natural radioactive content, they can be considered as
NORM (naturally occurring radioactive material).
To calculate the effective dose on workers during their use in a conservative
situation, samples of slag and aerosols and particles emitted or deposited during
welding were taken and measured by gamma, alpha and beta spectrometry. An
analytical method was also developed for estimating the activity concentration
of radionuclides in the inhaled air. 222 Rn activity concentration was also
assessed. With all these data, internal and external doses were calculated.
The results show that external doses are negligible in comparison with
internal ones, which do not exceed 1 mSv yr−1 , either in this conservative
situation or in any other more favourable one.
Radionuclides after Rn in the radioactive natural series are emitted at the
same activity concentration to the atmosphere, this being around 17 times higher
than that corresponding to radionuclides before Rn. Taking into account these
conclusions and the analytical method developed, it can be concluded that one
way to assess the activity concentration of natural radionuclides in inhaled
air and hence effective doses could be the early gamma-ray spectrometry of
aerosols and particles sampled during the welding process.

1. Introduction

Occupational exposure due to natural sources of radiation can occur as a result of certain work
activities. In Spain, these kinds of work activities were first incorporated into the national

0952-4746/14/010133+16$33.00 c 2014 IOP Publishing Ltd


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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

regulation in the Royal Decree 783/2001 [1], concerning health protection against ionising
radiation, which has been recently modified by the Royal Decree 1439/2010 [2].
This Royal Decree transposed the instructions of the Council Directive 96/29/EU-
RATOM [3], which considered the guidelines established in the International Basic Safety
Standards (BSS) issued in 1996 by the International Atomic Energy Agency (IAEA) [4].
Currently, there is a new Council Directive in the proposal stage [5] and an interim version
of BSS [6].
The Council Directive 96/29/EURATOM [3], in its title VII, lays down provisions on
natural radiation sources. Specifically, in article 40, it is considered necessary to conduct
surveys on the exposure of workers in activities such as the inhalation of thoron or radon
daughters in aboveground workplaces and the handling or storage of materials or residues not
usually considered as radioactive but which contain naturally occurring radionuclides.
The Spanish Nuclear Safety Council (CSN) has also produced standard recommendations
about the control of exposure to natural sources of radiation [7] and the methodology for
the assessment of the radiological impact of NORM (naturally occurring radioactive material)
industries [8].
Following all these recommendations, and since non-thoriated electrodes are very
commonly used welding consumables in Spain and covered electrodes are the only type of
electrode produced in this country, the CSN asked us to carry out this study. Our study
analysed the use of rutile consumables in the arc welding process, also taking into account
the production, storage and waste production of rutile-covered electrodes. The objective of this
study was to investigate the radiological impact of these consumables during their entire life.
Rutile (mainly titanium dioxide, TiO2 ) contains a variable amount of natural radionuclides,
and this amount is the largest among all the materials used to produce non-thoriated electrodes.
The radioactivity of this material depends mainly on its origin [9] and ranges between 0.1–1.0
and 0.07–0.45 Bq g−1 for the U and Th radioactive series, respectively [10]. Depending on the
producer, rutile is used at a variable rate; for instance, in the production of this specific type of
arc welding consumable rutile constitutes 50% of the covering. Sometimes, some of the other
raw materials used for this purpose may also contain natural radionuclides. All of these facts
contribute to the variability of the radioactive content of these types of consumables, which are,
in addition, the most widely used. In Spain, 70% of arc welding consumables are rutile based.
Therefore, they were chosen to be the subject of this study.
The first results of our previous study [9] revealed that workers exposed to rutile throughout
the manufacturing process of rutile-covered electrodes do not receive a dose exceeding the
established limit for members of the public, 1 mSv yr−1 , this dose being essentially external.
However, during welding processes the expected worker’s dose is mainly internal, and it is this
dose which is assessed in this paper.

1.1. Welding processes


Arc welding is the most frequently used welding process. In this process, an electric current
or electric arc is set up in an air or gas medium between two conductor pieces or electrodes,
the temperature provided by this arc (around 3600 ◦ C [11]) being enough to melt and weld the
electrodes, producing a bead in the welding point. In some cases, depending on the welding
process type, some slag appears over the bead.
According to the American Welding Society (AWS) there are eight different arc welding
processes [12], two of them being the most popular nowadays: shielded metal arc welding
(SMAW) and flux cored arc welding (FCAW).
In the SMAW process the electric arc is established between a base material and the rod
of an electrode, which is usually made of steel and fills the welding point. Around the core

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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

rod there is a covering, made with different raw materials depending on the specific industrial
formula of each manufacturer. In some cases this raw material is, or contains, rutile. This
covering is used to produce CO2 (which protects against oxidation and contamination of the
welding point), to ionise the air and to facilitate the melting of electrodes. The covering mainly
becomes slag or goes into the air in the form of gases, aerosols and particles.
On the other hand, the consumable used in the FCAW process is a metal wire, which is
provided continuously by a gun handled by the welder. While the wire and the base metal are
melting, a suitable gas protects the welding from the atmosphere and prevents oxidation of
the base metal. Because of this, the FCAW process produces less smoke than the SMAW one.
The wire is flux cored, the flux being a mixture of different raw materials that, in some cases,
contains rutile.
In Spain, large amounts of these two types of consumables are consumed annually. This
consumption can be estimated to be several millions of covered electrodes and kilometres of
flux cored wire, 70% of them being rutile based.
The main objective of this study is the evaluation of the radiological impact derived from
the use of rutile-covered electrodes and cored wires. The dose received by the welder during the
use of these rutile consumables is mainly internal, due to the gases, aerosols and particles that
appear during the welding process and that can be inhaled or ingested by the welder throughout
the process or once they have been diffused in the working place. That is why samples of the
material emitted during welding were collected by means of a particle and aerosol sampling
system placed in a position equivalent to those of the nose and mouth of the welder. Also, some
adhesive tape was placed on the hands of the welder and samples of the slag produced were
also taken to evaluate their radioactive content.
Samples were immediately analysed by gamma spectrometry and then by alpha
spectrometry and beta counting to find the activity concentration of their radionuclides. After
that, and because of the very short half-life of some of these radionuclides, an analytical method
that allows the determination of the activity concentration of those radionuclides present in the
inhaled air from the experimental results obtained from the samples taken was developed. It
should be pointed out that it is interesting to know all the radionuclides present in the inhaled air
because, although the internal dose coefficients for short half-life radionuclides are lower than
those for long-lived radionuclides, their emitted activity concentration might be the opposite.
In addition, and in order to quantify radon concentration in the air of the workplace during
welding and to verify whether it exceeded the reference level of 1000 Bq m−3 [4], an active
sampling system was used.
With all these values, it was feasible to determine internal and external effective doses by
means of DCAL (dose and risk calculation software) [13].
An analysis of the mass and activity distribution between slag and particles was also carried
out, in order to find out whether both mass and activity had the same distribution pattern.
Below, the materials and methods used in this study are described.

2. Materials and methods

2.1. Materials
2.1.1. Rutile consumables. The consumables used in the SMAW and FCAW processes are
the subject of this study, and the main characteristics of the ones selected for this study are
described below.
The covered electrodes used in SMAW consist of two parts: a metal rod and the covering
that surrounds it. In the most commonly used electrodes, this covering is approximately 30%
of the weight of the electrode.

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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

The rod must be compatible with the metal to be welded and, therefore, its composition
should be very similar to the base metal. Its length normally ranges between 200 and 450 mm,
while its diameter is between 1.5 and 6 mm.
The covering is classified according to the ISO 2560:2009 standard [14], depending on
its composition, in the following way: acid (A, iron and manganese oxides), basic (B, calcium
carbonate and other basic carbonates), cellulosic (C, organic substances), rutile (R, titanium
dioxide), rutile–acid (RA), rutile–basic (RB), rutile–cellulose (RC) and coarse rutile (RR).
The covered electrodes chosen for this work were rutile type, as it is the most commonly
used type and the one which has the highest radioactivity content [9]. Among the different
existing brands of this electrode, the one most commonly used in Spain was chosen. Its rod is
350 mm long and 4 mm in diameter. It weighs about 42 g, 12 g being the covering weight, and
50% of this covering is rutile.
The cored wire used in the FCAW process consists of a metal tube with a diameter ranging
from 0.6 to 3.25 mm and filled with a mixture of deoxidise and/or alloy elements, which is
called flux. The flux composition determines the type of cored wire, which can be rutile, basic
or metallic, among others.
The cored wire used in this study was also made of rutile, due to the widespread use of this
raw material, and it had a diameter of 1.2 mm.
It must be taken into account that the rutile used to produce these consumables is not
always the same; there are different types based on the mineral type and its origin. However, in
the composition of the rutile mineral there are always traces of radioactive substances, mainly
238 U and 232 Th natural radioactive series [9], and as a result industries that use this material are

or may be classified as NORM industries.

2.1.2. Sampling equipment. To assess the internal dose due to inhalation during welding, it is
necessary to collect representative samples of aerosols and particles emitted during the welding
process and inhaled by the welder. For this purpose, an active air-sampling device consisting of
an air pump and a fibreglass filter placed in a head collector was used. The emitted gases were
not sampled because they are too hot to be retained by active carbon cartridges.
The pump (Radeco DKB, trademark Kobold) was adjusted to a constant air flow of
0.001 m3 s−1 ; in this way, we maximised dust loading and enabled the measurement of
unsupported short-lived radionuclides, like 214 Pb and 214 Bi. The head collector stood at the
height of the nose and mouth of the welder. Inside it there was a Whatman glass microfibre
filter 47 mm in diameter and 1.2 µm in pore size, with 90% activity retention efficiency and
about 99% mass retention efficiency for this type of sample and in these sampling conditions.
As a part of a study on ambient radon levels in different workplaces commissioned by
the CSN, to verify whether Rn content in the workplace is below the reference level of
1000 Bq m−3 [4], an active sampling system was placed 2 m away from the welder so that it
could avoid the high temperature gases but still represent the atmosphere in the working place.
The device consisted of an air pump, a radon collection step and a previous air drying step. The
pump (Radeco DKB, trademark Kobold) was adjusted to an air flow of 0.0003 m3 s−1 . In the
radon collection step 583 g of specific activated charcoal (Nusorb G30 and G35) was placed in
a cylindrical collector. In the air drying step 900 g of silica-gel from Panreac with a grain size
larger than 2 mm was placed in another cylindrical collector, just above the radon collection
step. The radon retention efficiency of this system was greater than 85% [15].
Also, and in order to assess the internal dose due to ingestion and the external dose due
to the deposition of particles, 45 cm2 adhesive tapes were placed on the hands of the welder.
Besides this, the slag produced in the welding was collected to analyse the mass and activity
distribution between particles and slag. It should be noted that in the FCAW process, with flux
cored wire, unlike in the SMAW process, no slag is produced.

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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

2.1.3. Measuring equipment. Analyses were conducted according to conventional methods


used by the Laboratory of Low Activity Measurements of the UPV/EHU and that were within
the scope of accreditation of the laboratory, ENAC 350/LE560, according to the ISO 17025
standard [16]. The measuring equipment used included the following.
The equipment used for gamma spectrometry included two EG & G ORTEC gamma
spectrometers equipped with high-purity germanium detectors (HPGe), with 40% and 110%
total relative efficiencies and resolutions of 1.88 and 2.10 keV (FWHM) for the 1.33 MeV peak,
respectively. The obtained spectra were processed using EG & G ORTEC Gamma Vision 6.01
commercial software [17]. Calibrations were made using calibration sources prepared with a
multi-gamma ray emitters standard and with the same geometry and composition as the samples
to be measured.
Alpha spectrometry was performed using Canberra spectrometers equipped with passivated
implanted silicon detectors (PIPS detectors), showing 0.05 counts h cm−2 nominal background.
The acquired spectra were analysed with internal software.
For beta counting a gas flow proportional counter, with detectors of 7 cm in diameter
equipped with 1.5 µm thick mylar windows, was used. These detectors were calibrated with
standard sources of 210 Pb, with 35% efficiency for their beta emissions and their background
always less than 1 cpm. Results were analysed with internal software.

2.1.4. DCAL. DCAL (dose and risk calculation), version 8.4, which uses the effective dose
definition from ICRP 60 [18], is Oak Ridge National Laboratory software that enables the
calculation of effective dose coefficients [13].
In this study, this software was used to obtain committed effective dose coefficients e(50)
(Sv Bq−1 ) for inhalation and ingestion, with the following selection of parameters: biokinetic
model from ICRP 68 [19]; radionuclides of 232 Th, 235 U and 238 U decay series; adults; slow lung
absorption and 5 µm AMAD (activity median aerodynamic diameter) only for inhalation [8];
and progeny with same kinetics as parent (ICRP 30 [20]) except in 232 Th, 228 Th, 212 Pb, 235 U,
234 U, 230 Th, 226 Ra, 214 Pb and 210 Pb cases, whose kinetics is independent.

In addition, DCAL was used to obtain the effective dose coefficients for external exposure
to photons and electrons from submersion in a contaminated cloud and also from an emitter
surface, as defined in the Federal Guidance Report (FGR) 12 document [21]. DCAL offers
effective dose coefficient values (Sv s−1 ) per activity concentration in air (Bq m−3 ) or surface
(Bq m−2 ) for each radionuclide.
The cloud that the document refers to is an infinite hemisphere that contains
uniformly-distributed monoenergetic gamma emitters, with a constant activity concentration
in air, and that surrounds a human phantom standing on the soil, which is considered as the
surface.
Thus, by multiplying internal or external dose coefficients, the activity concentration
of each isotope (Bq m−3 or Bq m−2 ), the breathing rate (m3 h−1 , only for internal dose
calculation) and the time of exposure (h), the internal committed effective dose and the external
effective dose received by the welder can be calculated.

2.2. Methods
2.2.1. Sampling. At the beginning of this study two different welding processes, SMAW and
FCAW, were carried out and representative samples of emitted radon, aerosols and particles and
produced slag were taken with the equipment described in section 2.1.2. Sampling was carried
out according to a worst-case scenario: in a closed place with no air extraction and no welder
respiratory protection.
During 46 min of the SMAW process, 25 rutile-covered electrodes were used. Each
electrode weighs 42 g, approximately 12 g being rutile covering and 30 g rod.

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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

However, during the FCAW process 1.5 kg of rutile flux cored wire was consumed in
30 min, i.e. about 375 g of rutile flux.
The filters used were weighed before and after the sampling process in order to calculate
the sampled masses.

2.2.2. Activity determinations. After sampling, the samples collected by the glass microfibre
filters were immediately analysed by gamma spectrometry in a sequential way, recording the
accumulated counts every 20 min, in order to follow the time evolution of the short-lived
radionuclides. Then, they were dissolved and in the resulting solution U, Th, Ra, Po and Pb
were isolated following a radiochemical process. After that, the activities of 232 Th, 228 Th, 235 U,
238 U, 234 U, 230 Th and 210 Po were determined by alpha spectrometry; 226 Ra activity by gamma

spectrometry; and 210 Pb activity by beta counting.


The adhesive tapes and slag were only analysed by gamma spectrometry, following the
corresponding general procedure and 2 h after sampling. Then, the slag was milled and placed
in a Petri dish, in order to carry out gamma measurements again and improve previous results.
Density corrections were not needed as the standards and samples had approximately the same
density.
The activity, relative uncertainty and detection limits of the measured radionuclides
were calculated by gamma spectrometry using Gamma Vision 6.01 software. For the other
measurements, the following expressions were used.
For alpha spectrometry:
AT C i
Ai = (1)
CT
where Ai is the activity of radionuclide i, in Bq; AT is the activity of the added tracer, in Bq; Ci
is the net peak area of radionuclide i, in counts; CT is the net peak area of the added tracer, in
counts.
For beta counting:
[CB − χa→b CA ]
A= (2)
Rtε
where A is the 210 Pb activity, in Bq; CB are the net counts obtained in the beta channel; χa→b is
the crosstalk or spillover of the alpha channel into the beta one; CA are the net counts obtained
in the alpha channel; R is the radiochemical yield obtained by a gravimetric method; t is the
counting time of sample and background, in s; ε is the beta detector efficiency for 210 Pb.
To obtain C values, the contribution of the background was subtracted. This background
was obtained by measuring a blank that was prepared in a similar way to the samples for the
same time as the samples.
The relative standard uncertainty of the activity is determined according to the
methodology proposed in the ISO/IEC 98 standard [22]:
sX
uAi = u2j (3)
j

where uj is the standard relative uncertainty associated to parameter j, j being each parameter
present in (1) or in (2), respectively.
Critical limits (CL) and detection limits (DL), developed [23] from the method proposed
by Currie [24] and ISO 11929 standards [25], are given by the following.
For alpha spectrometry:
AT √
CL = k 2F (4)
CT
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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

k2 CATT + 2CL
DL = (5)
1 − k2 (u2AT + u2CT )
where k is the quantile of the standard normal distribution that has a value of 1.65 according to
a 95% confidence level and F is the background for the peak of radionuclide i.
For beta counting:
k q
CL = 2FB + χa→b CA + CA 2 u2 + χ 2 (u2 + u2 )
χ a→b CA FA (6)
Rεt
k2
Rtε + 2CL
DL = (7)
1 − k2 [u2ε + u2R ]
where FA and FB are the backgrounds in the alpha and beta channels, respectively, in counts.

2.2.3. Activity concentration determinations in the inhaled air. For internal dose calculations,
it is necessary to obtain the activity concentration in the air inhaled by the welder, which
is represented by the air that goes through the filter in the sampling process. Build-up of
radionuclides in the work place due to long welding periods has not been considered because,
as 3600 ◦ C is the temperature at the welding point, the thermal expansion wave moves aerosols
and particles away from the welding point.
Although the radionuclides found in the covering of rutile type electrodes and in flux cored
wire are in equilibrium [9], they are not emitted in the same way into the air during welding.
Depending on their chemical properties, some go mainly to the slag, like Ra, and others to the
air, like Po. Among the latter, some are quickly oxidised and retained in the filter and others go
through it, like Rn. That is why the activity concentration of each radionuclide in the radioactive
series was assessed, despite the large differences in dose coefficient values.
The activity concentration of some radionuclides can be assessed directly from
measurements. However, for the assessment of the activities of radionuclides with short
half-lives, which may be significantly higher those that of their parents, some detailed analysis
must be made. For some of them, the value can be assessed considering that, although the
temperature at the welding point may affect elements differently, the radionuclides from each
element are emitted at the same rate into the air. That is why the activity concentrations of
230 Th, 210 Pb and 210 Po in the air could be assessed by measuring the activity concentrations of
234 Th, 214 Pb and 218 Po in the filter. However, for radionuclides like 214 Bi, and also 214 Pb and
208 Tl, which can be measured in the filter, it is necessary to develop an analytical method to

model their time evolution in the filter and to know their activity concentration in the inhaled
air.
This analytical method is able to assess 214 Bi, and also 214 Pb and 208 Tl, in the inhaled
air from its sequential gamma measurements in filters and from the measurement of other
radionuclides in the natural decay series. Finally, following the procedure established in the
previous paragraph, the activity concentration of 210 Bi could also be assessed. The same
procedure could be applied to the evaluation of 212 Bi, 216 Po and 212 Pb activities, which belong
to the 232 Th decay series.
To develop this analytical method, it is assumed that the activity concentration of each
radionuclide in the inhaled air is constant during the welding time, since the sampling system
is located very near to the welding point so that it only takes air from this point.
Taking this into account, the evolution of the activity of the 238 U and 232 Th radioactive
decay series in the filter during sampling, measurement and during the waiting time between
these two processes was analysed, using the general Bateman solution [26].

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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

Thus, the activity evolution of the 238 U and 232 Th series in the filter during sampling
follows equation equation (8), in which a term corresponding to the collection [27] was added:
dNi
= Qi q + λi−1 Ni−1 − λi Ni (8)
dt
where dN i −1
dt is the variation of radionuclide i in the filter with time, in nuclei s ; Qi is the
−3
concentration of radionuclide i in the sampled air, in nuclei m ; q is the constant air flow, in
m3 s−1 ; λi is the decay constant of radionuclide i, in s−1 ; Ni is the number of radionuclide i in
the filter.
According to the set hypothesis, Qi is constant and the air flow, q, is 0.001 m3 s−1 . As
a result, multiplying Qi by q, the rate of radionuclides that go directly towards the filter is
obtained.
Integrating the previous equation (8), the amount of radionuclides of each isotope at the
end of the sampling can be obtained. These Ni values evolve during the waiting time from the
end of the sampling until the beginning of the measuring process, according to the Bateman
solution for nonzero initial conditions [26] in the corresponding equation (9):
dNi
= λi−1 Ni−1 − λi Ni . (9)
dt
Integrating equation (9), the amount of each isotope Ni in the filter at any time t after sampling
is determined and so are their theoretical activities Ai .
These theoretical values are matched with the experimental ones obtained from alpha and
gamma spectrometry and beta counting. To do this, all values have been referred to the same
time point at the beginning of the measurements.
This match allows us to obtain Qi values for those radionuclides that are experimentally
measured and best estimations for 214 Bi, 214 Pb and 208 Tl, reproducing in this way the sequential
activity values obtained by gamma spectrometry.

2.2.4. Estimation of internal dose. The internal dose depends on the ingestion and inhalation
of gases, aerosols and particles. Internal dose due to ingestion is quite unlikely in this type of
process, but some of the deposited material, e.g. on gloves, could be accidentally ingested. In
order to assess what the maximum internal dose derived from this would be, different deposited
aerosol and particle samples were taken using 45 cm2 adhesive tapes placed on the hands of the
welder, and measured by gamma spectrometry.
For internal dose due to inhalation, each corresponding DCAL e(50) coefficient, obtained
as described in section 2.1.4, is multiplied by the activity concentration of the corresponding
radionuclide in the inhaled air (Bq m−3 ), obtained from the analytical method described in
section 2.2.3, and also by the breathing rate of the welder (1.7 m3 h−1 [28]) and the estimation
of the real welding hours per year, 850 h yr−1 , in a 1700 h mean working year [29]. In this way,
the committed effective dose E(50) per year of exposure and radionuclide is obtained. Thus, the
total committed effective dose is calculated, adding the E(50) values of all given radionuclides.
For internal dose due to ingestion of deposited aerosols and particles, each corresponding
DCAL e(50) value is multiplied by the consumed activity in the welding that goes to the air and
is deposited on the hands of the welder, and by the estimated ingestion rate (1% of deposition
on the hands).
For radon and thoron there is no committed effective dose coefficient for internal radiation;
therefore, in order to estimate their internal effective dose and that of their short-lived decay
products, the equilibrium equivalent radon concentration (EERC), the equilibrium equivalent
thoron concentration (EETC) [30] and dose conversion factors for radon (9 nSv m3 h−1 Bq−1 )
and thoron (40 nSv m3 h−1 Bq−1 ) [31] are used.

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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

The uncertainties reported correspond only to combined uncertainties coming from the
radioactivity measurements.

2.2.5. Estimation of external dose. It is considered that the external dose received by the
welder has a triple potential source: particles emitted into the atmosphere and deposited on
environmental surfaces, the dust cloud in which the welder is submersed and the rutile-covered
electrodes or rutile flux cored wire that are near the welder.
Thus, for the first two cases, the external effective dose received by the welder is obtained
by multiplying the corresponding dose conversion factors given by DCAL by the exposure time
(850 h yr−1 ) and by the activity concentration of each radionuclide in air (Bq m−3 ) obtained
from the analytical method described in 2.2.3, or by the activity concentration in the adhesive
tape, depending on the source.
Since the measured values were below the detection limit, the activity concentration in the
adhesive tape could be obtained by dividing the consumed activity that goes to the air and is
deposited on the adhesive tapes by their area. In any case, as is shown in section 3.4, this value
is negligible.
The simulation method described in our previous study [9], which uses the MCNP code,
enables the assessment of the external effective dose due to covered electrodes or flux cored
wire that are near the welder.
The uncertainties reported correspond only to combined uncertainties coming from the
radioactivity measurements.

3. Results and discussion

3.1. Activity concentration in the inhaled air

From the measurements of the filters—where 238 U, 234 U, 232 Th, 230 Th, 228 Th and 210 Po have
been by alpha spectrometry, 210 Pb by beta counting, and 214 Pb, 212 Pb, 214 Bi, 212 Bi and 208 Tl by
gamma spectrometry—and from the developed analytical method presented in section 2.2.3, the
results obtained for the activity concentration of radionuclides of the 238 U and 232 Th natural
series, at the moment they were inhaled during the welding of rutile-covered electrodes and
rutile flux cored wire, are shown in tables 1 and 2.
In these tables, three groups of data are presented: the first group (M) corresponds
to the measured values of long-lived radionuclides, obtained directly by gamma and alpha
spectrometry and beta counting. The second group (C) corresponds to the short-lived
radionuclides, whose activities were assessed using the method proposed in 2.2.3. The
third group (‘Eq’.) corresponds to those radionuclides whose activities have been assessed
considering that all the isotopes from the same element are emitted with equal relative
probability. As all the radionuclides from a radioactive series are in equilibrium in the
electrode [9], it can be concluded that the obtained activity concentration values can be different
between elements but they should be equal between radionuclides of the same element and
same decay series.
Therefore, in the 238 U radioactive decay series the activity concentrations of 238 U, 234 U,
230 Th, 210 Pb and 210 Po were experimentally determined. From these measurements, the activity

concentrations of 234 Th, 218 Po and 214 Pb could be assessed. Finally, the expected activity con-
centrations of 214 Bi and 214 Pb were obtained by the proposed theoretical method and 210 Bi was
assessed taking into account the activity concentration equilibrium between radionuclides of the
same element. In this series, 226 Ra and 234 Pa were always found to be below detection limits.
In the 232 Th radioactive decay series, the activity concentrations of 232 Th and 228 Th have
been experimentally measured; the other radionuclides have been found to be below their

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Table 1. Activity concentrations (Bq m−3 ) for each radionuclide in the inhaled air, due to arc
welding using rutile-covered electrodes, with their uncertainties. (Note: uncertainty: coverage
factor = 1; γ M: gamma measurement; αM: alpha measurement; βM: beta measurement; Eq.:
equilibrium; C: calculated from the analytical method.)
Rutile-covered electrode
Sp. activity Uncertainty Sp. activity Uncertainty
238 U series (Bq m−3 ) (Bq m−3 ) 232 Th series (Bq m−3 ) (Bq m−3 )

αM 238 U 1.36 × 10−3 9.39 × 10−5 αM 232 Th 4.89 × 10−4 5.18 × 10−5
Eq. 234 Th 1.35 × 10−3 8.80 × 10−5 Eq. 228 Ra — —
— 234 Pa — — γM 228 Ac — —
αM 234 U 1.74 × 10−3 1.09 × 10−4 αM 228 Th 5.29 × 10−4 5.46 × 10−5
αM 230 Th 1.35 × 10−3 8.80 × 10−5 γM 224 Ra — —
γM 226 Ra — — — 220 Rn — —
γM 222 Rn — — Eq. 216 Po 1.19 × 10−2 5.38 × 10−4
Eq. 218 Po 3.03 × 10−2 1.37 × 10−3 Eq. 212 Pb 1.03 × 10−2 9.65 × 10−4
C, Eq. 214 Pb 2.64 × 10−2 2.48 × 10−3 Eq. 212 Bi 1.04 × 10−2 —
C 214 Bi 2.66 × 10−2 — C 208 Tl 1.12 × 10−2 —
βM 210 Pb 2.64 × 10−2 2.48 × 10−3
C, Eq. 210 Bi 2.66 × 10−2 —
αM 210 Po 3.03 × 10−2 1.37 × 10−3

Table 2. Activity concentrations (Bq m−3 ) for each radionuclide in the inhaled air, due to arc
welding using rutile flux cored wire, with their uncertainties. (Note: uncertainty: coverage factor =
1; γ M: gamma measurement; αM: alpha measurement; βM: beta measurement; Eq.: equilibrium;
C: calculated from the analytical method.)
Rutile flux cored wire
Sp. activity Uncertainty Sp. activity Uncertainty
238 U series (Bq m−3 ) (Bq m−3 ) 232 Th series (Bq m−3 ) (Bq m−3 )

αM 238 U 9.42 × 10−4 8.86 × 10−5 Eq. 232 Th 3.08 × 10−4 2.90 × 10−5
Eq. 234 Th 9.75 × 10−4 2.44 × 10−4 Eq. 228 Ra — —
— 234 Pa — — γM 228 Ac — —
αM 234 U 9.33 × 10−4 8.08 × 10−5 Eq. 228 Th 3.08 × 10−4 2.90 × 10−5
αM 230 Th 9.75 × 10−4 2.44 × 10−4 γM 224 Ra — —
γM 226 Ra — — — 220 Rn — —
γM 222 Rn — — Eq. 216 Po 4.04 × 10−3 2.85 × 10−4
Eq. 218 Po 1.28 × 10−2 8.30 × 10−4 Eq. 212 Pb 4.92 × 10−3 7.51 × 10−4
C, Eq. 214 Pb 1.56 × 10−2 2.38 × 10−3 Eq. 212 Bi 4.96 × 10−3 —
C 214 Bi 1.57 × 10−2 — C 208 Tl 4.64 × 10−3 —
βM 210 Pb 1.56 × 10−2 2.38 × 10−3
C, Eq. 210 Bi 1.57 × 10−2 —
αM 210 Po 1.28 × 10−2 8.30 × 10−4

detection limits. Thereby, the nuclei ratios Th–Po, Pb and Bi obtained in the 238 U series are used
to estimate the activity concentrations of 216 Po, 212 Pb and 212 Bi. The activity concentration of
208 Tl was obtained following the proposed theoretical method. Also, in this series, 228 Ra, 224 Ra

and 228 Ac were always below their detection limits.


As is shown in both tables 1 and 2, when two radionuclides from the same element have
been measured (e.g. 238 U and 234 U or 232 Th and 228 Th), the values obtained for the activity
concentration are compatible with the hypothesis of radionuclides from the same element being

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emitted at the same rate into the air. This allows the use of this hypothesis for other cases, for
example, 214 Pb–210 Pb and 218 Po –210 Po.
214 Pb was obtained by two approaches: the experimental measurement of 210 Pb and the

developed analytical method, both results being equal.


Data presented for both radioactive series and both types of consumables show that all the
progeny of Rn is emitted into the air at almost the same activity concentration. All long-lived
radionuclides before Rn are also emitted into the air at the same activity concentration, but with
values 17 times lower because those radionuclides probably remain in the slag. In light of this
relation, and only from a dosimetric point of view, it can be considered that values for the 234 Pa,
228 Ac and Ra isotopes in the inhaled air can be assigned the same activity concentration as the

other radionuclides before Rn in their respective radionuclide series.


It is also observed that the ratio between 238 U and 232 Th activity concentrations in air
is the same as the one observed in the welding consumables (see table 7). That is, both in
the electrodes and in the atmosphere created after welding, the relation between activities of
radionuclides from the 238 U and 232 Th radioactive series is the same.
From the results obtained it can be concluded that the activity concentration of each
radionuclide from the 238 U and 232 Th series in the inhaled air can be estimated with only the
developed analytical method and the early gamma-ray measurement of 214 Pb and 214 Bi. From
the early gamma measurements of 214 Pb and 214 Bi their activity concentration values can be
assessed at the moment they are inhaled, and so can those for 210 Pb, 210 Bi, 218 Po and 210 Po,
by equilibrium. 238 U, 234 Th, 234 U and 230 Th can be estimated using the established ratio of 17
between radionuclides before and after Rn, and the radionuclides from the 232 Th series can be
assessed by considering the ratio between the activities of both series in the electrodes and in
the air. In this way, alpha spectrometry and beta counting are no longer necessary and results
are obtained sooner and more cheaply.
Apart from this, and since Rn was not retained in the filter, an active sampling system
was used to detect it. It was placed 2 m away from the welder, vertically, thus capturing
Rn distributed into the work atmosphere. The measured activity concentration of 222 Rn was
9.18 ± 0.38 Bq m−3 , which is consistent with the usual ambient radon level, and, therefore,
clearly below the reference level of 1000 Bq m−3 .

3.2. Activity concentration deposited in slag and hand adhesive tapes

In addition to the aforementioned measurements in filters, gamma activity concentration was


measured in the slag produced during the welding of 25 electrodes through the SMAW process,
and the obtained results are shown in table 3.
The adhesive tapes placed on the hands of the welder during both welding processes were
also measured by gamma spectrometry, with the activity concentration results being below
detection limits, as shown in table 4.
It should be pointed out that 40 K, which appears in the covering and in the flux cored
wire (see table 7) of the analysed consumables, does not come from rutile [9] and its presence
depends on the other raw materials used to produce these consumables. In table 4 it can be
seen that it goes almost completely to the slag, the results being below the detection limit in its
measurement in filters and adhesive tapes.

3.3. Internal dose

The dose coefficients e(50) obtained by DCAL for inhalation and ingestion were very similar to
the coefficients that appear in the regulations [2, 3], except in those isotopes with independent
kinetics, because in the regulations all the progeny have the same kinetics as the parent.

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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

Table 3. Activity concentration (Bq kg−1 ) of detected radionuclides in the slag produced during
arc welding using rutile-covered electrodes, measured by gamma-ray spectrometry, with their
uncertainties (coverage factor = 1).
Rutile-covered electrode
Isotope Sp. activity (Bq kg−1 ) Uncertainty (Bq kg−1 )
228 Ra (via 228 Ac) 6.37 × 101 6.97 × 100
228 Th (via 224 Ra) 6.52 × 101 1.68 × 101
238 U (via 234 Th) 1.10 × 102 1.30 × 101
226 Ra 9.16 × 101 2.22 × 101
210 Pb 1.23 × 101 6.44 × 100
235 U 9.75 × 100 2.73 × 100
40 K 1.04 × 103 7.22 × 101

Table 4. Detection limits (Bq) for radionuclides in adhesive tapes, measured by gamma-ray
spectrometry.
Isotope LID (Bq)
228 Ra (via 228 Ac) 6.54 × 10−1
228 Th (via 224 Ra) 1.74 × 100
238 U (via 234 Th) 1.63 × 100
226 Ra (via 214 Pb) 2.32 × 10−1
210 Pb 8.87 × 100
235 U 4.22 × 10−1
40 K 3.06 × 100

Table 5. Committed effective dose rate (µSv h−1 ) of each radioactive series due to inhalation
by the welder using rutile-covered electrodes or rutile flux cored wire and their uncertainties
(coverage factor = 1).
Rutile-covered electrode Rutile flux cored wire
E(50) Uncertainty E(50) Uncertainty
Series (µSv h−1 ) (µSv h−1 ) (µSv h−1 ) (µSv h−1 )
238 U 0.469 0.023 0.254 0.022
232 Th 0.036 0.003 0.038 0.002
222 Rn 0.033 0.001 0.033 0.001
Total 0.538 0.023 0.325 0.022

Considering the independent kinetics in those isotopes, which is close to reality as shown in
this study, dose coefficients are about 5% lower.
The committed effective dose (E(50)) received per year of exposure is obtained by
taking into account DCAL coefficients for inhalation and the activity concentration (Bq m−3 )
determined in the air inhaled by the welder during a welding process, 458 ± 20 µSv yr−1 in the
SMAW process and 277 ± 19 µSv yr−1 in the FCAW process. Results are presented in table 5,
per hour of exposure.
For the calculation of the internal dose due to ingestion of deposited aerosols and particles
in the welding processes an estimation was performed, because the activity concentration values
in adhesive tapes were below the detection limit. This estimation was based on the hypothesis
that the area of each adhesive tape corresponds to 0.3% of the total deposition area. Therefore,

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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

Table 6. External effective dose rates (µSv h−1 ) for each radioactive series received by a welder
using rutile-covered electrodes or rutile flux cored wire, with their uncertainties (coverage factor
= 1).
Rutile-covered electrode Rutile flux cored wire
ED Uncertainty ED Uncertainty
Series (µSv h−1 ) (µSv h−1 ) (µSv h−1 ) (µSv h−1 )
238 U 2.52 × 10−4 1.97 × 10−5 3.81 × 10−4 1.22 × 10−5
232 Th 1.68 × 10−4 1.87 × 10−5 2.10 × 10−4 1.78 × 10−5
Total 4.10 × 10−4 2.72 × 10−5 5.91 × 10−4 2.16 × 10−5

Table 7. Activity concentration (Bq kg−1 ) in rutile covering and rutile flux cored wire, with its
standard uncertainty (coverage factor = 1).
Rutile-covered electrode Rutile flux cored wire
Sp. activity Uncertainty Sp. activity Uncertainty
Series (Bq kg−1 ) (Bq kg−1 ) (Bq kg−1 ) (Bq kg−1 )
232 Th 5.35 × 101 5.56 × 100 7.65 × 100 2.40 × 100
238 U 1.26 × 102 1.09 × 101 2.42 × 101 3.81 × 100
235 U 1.02 × 101 2.68 × 100 — —
40 K 8.92 × 102 5.65 × 101 2.10 × 101 1.19 × 101

in the SMAW and FCAW processes, the internal committed effective dose was 2.32 ± 0.15
and 1.43 ± 0.17 µSv yr−1 , respectively, which means that ingestion is negligible compared
to inhalation in terms of dose. In this way, it can be concluded that only inhalation has to be
considered in the internal dose calculations in this type of process.
Considering that the data shown in table 5 were obtained for the welder working in the
worst-case working conditions (a closed place without artificial air extraction and a worker
welding all the working year without any respiratory protection), it can be concluded that both
types of rutile consumables produce doses that in no case would exceed the established limit
of 1 mSv yr−1 . Anyway, these results, which are close to the established limit, support the use
of individual protective equipment as part of the optimisation process required by radiation
protection principles.

3.4. External dose


Using the method described in section 2.2.5, the values of external doses due to radioactivity
concentration in a cloud were calculated, and the results obtained were 0.014 ± 0.001 µSv yr−1
in the SMAW and 0.008 ± 0.001 µSv yr−1 in the FCAW processes.
Using the approach mentioned before to estimate the activities in the adhesive tapes, the
estimated values were 0.25 ± 0.02 and 0.13 ± 0.02 µSv yr−1 in the SMAW and FCAW
processes, respectively. Any real dose will always be lower than these values and, as such,
negligible.
The effective dose values per year of exposure due to the third potential source, calculated
by MCNP and according to the methodology described in our previous paper [9], were 0.093
± 0.003 µSv yr−1 for rutile-covered electrodes and 0.370 ± 0.001 µSv yr−1 for the rutile flux
cored wire.
Table 6 shows the total external effective dose values per hour of exposure for such rutile
consumables and each decay series.
The doses from 40 K and 235 U are even lower. As can be seen in table 6, the external
dose results are negligible compared with the internal ones, and no matter what type of rutile

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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

consumable is used in the welding process. As a result, it can be considered that the external
dose does not contribute to the total dose, which can be calculated as only internal dose.

3.5. Mass/activity distribution


In the glass microfibre filter from the SMAW process, which was about 35 cm away from
the welding point to maximise the dust loading, 0.03 g of aerosols was collected after having
sampled 2.76 m3 of air. Considering that the area of the filter represents around 0.25% of
the area of a hemisphere and an isotropic emission, about 4% of the total covering consumed
(300 g) was emitted into the atmosphere.
Thus, after welding 25 electrodes with 300 g of covering, roughly 95% of this covering
went to the slag and the rest went to the air. However, this welding produced approximately
310 g of slag. Therefore, 90% of the slag came from the covering and the other 10% from the
rod.
In the FCAW process 0.045 g of aerosols was collected in the glass microfibre filter after
having sampled 1.8 m3 of air. Therefore, with the same calculation procedure, 18 g of the flux
was emitted into the atmosphere, which is about 5% of the total flux consumed. Since no slag
was produced during the welding, around 95% of the rutile flux went to the bead.
In the same way, considering the activity obtained in the filters (see tables 1 and 2) and
the activity contained in the electrodes and in the flux cored wire (see table 7), which were
observed to have their decay series in radioactive equilibrium [9], the mass distribution of the
covering and the flux can be compared with the activity distribution.
If 25 electrodes are consumed, the activity obtained in the filter for 238 U and long-lived
radionuclides before Rn in the radioactive series is consistent with the 5% of the activity emitted
into the atmosphere and matches quite well the results obtained for mass. These results are also
consistent with the values obtained for these radionuclides in the slag (see table 3), where, and
despite the high uncertainty values obtained, more than 90% of the activity remains. In this
way, the distribution of radionuclides before Rn in the radioactive series matches the results
obtained for mass distribution, and this implies that these radionuclides behave like the mass
during the welding process.
However, for the progeny of Rn, and from the results shown in table 1, it can be concluded
that 90% of the consumed radionuclides go to the atmosphere, and so only 10% remain in
the slag. This conclusion implies that radionuclides after Rn in the radioactive series do not
follow the mass distribution tendency in the welding process nor the distribution tendency of
the long-lived radionuclides before Rn. Unfortunately, from the progeny of Rn only 210 Pb has
been detected in the slag. Although the high uncertainty of 210 Pb prevents us from obtaining
a clear conclusion, its results are compatible with 90% emission into atmosphere and 10%
retention in the slag.
In the FCAW process, radionuclides before Rn were emitted into the air at a rate of
approximately 5%, whereas radionuclides after Rn were emitted at a rate of 30%. Therefore,
as in this process there is no slag, radionuclides that were not emitted into the air (95 and 70%
respectively), went to the bead.

4. Conclusions

Rutile-covered electrodes and flux cored wire have an appreciable natural radioactive content
in both the covering of the electrodes and the flux of the cored wire. When these consumables
are welded, radionuclides of the 238 U and 232 Th series are distributed in aerosols, particles and
slag, or bead, when slag is not produced.
From the measurements, a set of hypotheses and an analytical method, the activity
concentrations of radionuclides of the 238 U and 232 Th series in the inhaled air have been

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J. Radiol. Prot. 34 (2014) 133 M Herranz et al

assessed. These results, for both types of rutile consumables analysed, show that radionuclides
before Rn in the series have been emitted with the same activity concentration, this being about
17 times lower than the activity emitted from radionuclides after Rn, which also has the same
value for all of them. It should also be mentioned that build-up of radionuclides in the work
place due to long welding periods has not been considered because of the thermal expansion
wave produced by the high temperatures used in welding, which moves aerosols and particles
away from the vicinity of the welding.
Taking this into account, together with the ratio between activities of both series in the
consumables and the early gamma measurements of 214 Pb and 214 Bi, the developed analytical
method becomes a useful tool to estimate the activity concentration of each radionuclide from
the 238 U and 232 Th series in the air in similar conditions. In this way, alpha spectrometry and
beta counting are no longer necessary and results are obtained sooner and more cheaply.
The radioactivity concentration in the slag and the adhesive tapes placed on the hands of
the welder has also been measured with the following results. More than 90% of long-lived
radionuclides before Rn in the series are mainly present in the slag for the SMAW process,
or in the bead when the process is FCAW, whereas about 5% is in aerosol and particle form.
Thus, these radionuclides follow the same distribution as the covering or flux mass. In contrast,
only 10% of short-lived radionuclides after Rn are mainly in the slag in the SMAW process,
and 70% in the bead in the FCAW process, since 90 and 30% are, respectively, in aerosols and
particles. On the contrary, 40 K ends up in the slag.
The internal committed effective dose in both the SMAW and FCAW processes due
to the radioactive content of rutile consumables is mainly due to inhalation and is below
1 mSv yr−1 in the worst working conditions. In real conditions it would be lower and always
below the limit. Anyway, the fact that these results are close to the established limit supports
the use of individual protective equipment, which is mandatory for welders, as part of the
optimisation process required by radiation protection principles. In any case, the measured
activity concentration of 222 Rn is clearly below the reference level of 1000 Bq m−3 .
The external dose due to all possible sources of external exposure is totally negligible
compared to the internal dose, sometimes because the activity is insignificant (e.g. adhesive
tapes), sometimes due to its small amount of mass (e.g. slag). Due to this, the total effective dose
the welder receives is essentially internal, unlike in the manufacturing process of rutile-covered
electrodes, in which the dose is mostly external.

Acknowledgments

We would like to thank the Nuevas Técnicas Profesionales (NTP) welding workshop and the
welding laboratory of the E U de Ingenierı́a Técnica de Bilbao UPV/EHU, which enabled the
achievement of data during the arc welding processes performed in this work.

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