Construction and Building Materials 29 (2012) 158166

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Construction and Building Materials

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

Does the utilization of coal y ash in concrete construction present

a radiation hazard?
Konstantin Kovler
National Building Research Institute, Faculty of Civil and Environmental Engineering, Technion Israel Institute of Technology, Haifa, Israel

a r t i c l e i n f o a b s t r a c t

Article history: The advantages of utilization of coal y ash in concrete construction, as well as the technological and envi-
Received 4 June 2010 ronmental problems caused by an elevated content of chemical/radioactive contaminants, are discussed.
Received in revised form 13 September 2011 The paper deals with the question whether the utilization of coal y ash in concrete construction presents
Accepted 2 October 2011
a radiation hazard. The analysis of the experimental studies shows that although radon exhalation rate of
Available online 24 November 2011
concrete containing coal y ash can be sometimes slightly higher, than that of the reference concrete, radon
emanation coefcient is lower. In view of this, the standards regulating radioactivity of building materials,
Keywords:
but not addressing the decrease of radon emanation coefcient properly could be detrimental to the utili-
Radioactivity
Radon
zation of y ash in concrete construction. Drawing direct comparisons between results presented in differ-
Exhalation ent papers is challenging because of varying methodologies, sample sizes, material properties, such as age,
Emanation moisture and porosity, and experimental goals. The need in the systematic study considering different fac-
Concrete tors, which can inuence the radon release of a concrete, is emphasized.
Coal y ash 2011 Elsevier Ltd. All rights reserved.
Cement

1. Introduction The use of coal y ash in concrete is a well-recognized source of

Increased interest in measuring natural radionuclides and radon
emanation of building materials is due to the health hazards and
environmental pollution. Materials used by the building industry
that may be of radiological signicance include marl, blast furnace
slag, y ash, Portland cement clinker and clay.
The building industry uses large amounts of by-products from
other industries. In recent years there is a growing tendency in
European and other countries to use new recycled materials with
technologically enhanced levels of radioactivity. Coal y ash is
one of the most known examples [1,2].
Large quantities of coal y ash are expelled from coal-red ther-
mal power plants and these may contain enhanced levels of radio-
nuclides along with other toxic elements. More than 280 Mt of coal
ash (y ash and bottom ash combined) are produced annually.
About 40 Mt of these are used in the production of bricks and ce-
ment [3]. Since most of the process residues further processed into
building materials do not meet the required technical specica-
tions, they are typically mixed with pristine raw materials. The
net effect is a dilution of the NORM (Naturally Occurring Radioac-
tive Material) content relative to the process residues.
Decommissioning or rebuilding the structures made of y ash
and the ensuing dust generation or landlling of secondary wastes
may lead to exposure.
E-mail address: cvrkost@tx.technion.ac.il
gamma exposure due to the presence of activity concentrations of
226
Ra, 232Th and, to a lesser extent 40K, while the effect of coal y
ash via radon exhalation is controversial, in particular due to the
low emanation coefcient from the ash [2].
The interest to studying the inuence of coal y ash introduced
into concrete mix from the viewpoint of the gamma exposure and
indoor radon has been expressed recently in different countries
due to the last attempts of environmental authorities to implement
stricter regulations regarding the utilization of coal y ash in con-
crete construction. On May 4, 2010, the US Environmental Protec-
tion Agency (EPA) announced that it is proposing to regulate coal
combustion products, including y ash, under the Resource Con-
servation and Recovery Act (RCRA). The EPAs proposed regulations
would lead to stronger oversight of coal ash impoundments, be-
cause they would treat y ash as a hazardous waste when disposed
of. In some countries the environmental authorities go even fur-
ther, like it happened recently in Israel, where the Ministry of Envi-
ronmental Protection in 2008 announced coal y ash as simply
radioactive waste. In view of this, some in the concrete industry,
especially in such countries, where signicant part of electricity is
produced from coal, and where the problem of utilization of coal
combustion products is acute, believe that the new regulations
would be very detrimental to the use of y ash in concrete.
The goal of this paper is to make an objective and critical review
of the current state of the art in the eld of natural radioactivity
and radon emanation of concrete containing coal y ash, on one

0950-0618/$ - see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.conbuildmat.2011.10.023
 K. Kovler / Construction and Building Materials 29 (2012) 158166 159

hand, and to share with the readers the results of our own obser-
vations, on the other hand.
The legislation aspects of radiological protection of the building
occupants exposed to both direct gamma radiation and radon inha-
lation caused by building materials in general and concrete con-
taining coal y ash in particular are out of the scope of the
present paper, but have been addressed recently in a separate pa-
per by the author [4].
It has to be mentioned that radon generated in the material in-
cludes not only the radon in the air phase, but also the radon ad-
sorbed to pore walls and dissolved in the water phase. Radon
that is generated in water and adsorbed to pore walls is included
in the denition of the emanation coefcient.
2.2. Relation between radon emanation coefcient and radon
exhalation rate

2. Terminology Usually the radon emanation coefcient of the material is deter-

It makes sense to dene the terms, which will be consistently
used herein.
Radiation exposure due to building materials can be divided
into external and internal exposure. The external exposure is
caused by direct gamma radiation. The internal exposure is caused
mainly by the inhalation of radon (222Rn) and its short lived decay
products. Radon is part of the radioactive decay series of uranium
(238U), which is present in building materials. This decay series is
often called decay chain of radium (226Ra), which is radon parent.
Therefore, the rate of generation of radon is proportional to the
amount of radium. As radium concentrations are generally consid-
erably higher in the solid matrix than in the pore space, it is rea-
sonable to assume that all radon is produced in the solid phase.
The knowledge of the characteristics of radon release from
building materials is important for accurately assessing radiation
exposure of the population in buildings. Two main terms are used
in the professional literature: emanation and exhalation. Let us de-
ne them.
2.1. Radon emanation
mined from the measured radon exhalation rate. If we assume all
emanated radon is exhaled during the radon-release measurement,
i.e. radon in the sample due to adsorption and low diffusion rates
are negligible, the emanation coefcient e can be calculated either
from the measured mass radon exhalation rate and the 226Ra activ-
ity concentration of the material:
Em
e 1
kRn ARa
or from the measured surface exhalation rate, Es (assuming that ra-
don exhales freely from the innite wall with a constant thickness
symmetrically towards both outdoors and indoors):
2Es
e 2
dqkRn ARa
where e is the radon emanation coefcient; Em the free mass radon
exhalation rate (Bq kg1 s1); Es the free surface radon exhalation
rate (Bq m2 s1); ARa the 226Ra activity concentration (Bq kg1);
kRn the radon decay constant (s1); d the wall thickness (m); q is
the material density (kg m3).

Because radon is an inert gas, it can move rather freely through
porous media such as building materials, although usually only a
fraction of that produced in the material reaches the surface and
enters the indoor air. The radon emanation coefcient, e, is dened
as the fraction of the total amount of radon produced by radium
decay that escapes from the solid phase and gets into the pores
of the material. However, sometimes it is dened in the literature
as the ratio between radon escaped from the material and the total
amount of radon produced in the material. This denition is not
sufciently accurate, because not all radon getting into the pores
enters the indoor air.
The radon emanation coefcient is also called the emanating
power, emanating fraction, release ratio, and escape-to-production
ratio. The radon emanation coefcient is a dimensionless parame-
ter and is represented as either a fraction or a percentage. The ema-
nation coefcient ranges from 0 (no radon escapes) to 1 (all radon
escapes). The rest of the produced radon (fraction 1  e) remains
trapped in the material.
3. Natural radionuclides in concrete and its raw materials
Concrete is considered as the main building material in most of
the countries, because it is made from locally available raw mate-
rials, is cheap and versatile material. Concrete, whether in the form
of a ready mixed product, factory produced (precast) or masonry
block, nds its way into a multitude of applications: buildings,
bridges, roads, dams, industrial facilities, urban infrastructure
and numerous other applications. From the construction sustain-
ability point of view, concrete industries contribute in several
areas:
 Supplementary cementitious materials, such as coal y ash, can
be used to improve the performance of concrete products.
 Demolished concrete products can be recycled and reused in
new construction.
 Industrial by-products containing organic matter are burned as
a fuel in cement manufacturing process.

Table 1
Typical and maximum activity concentrations in common building materials and industrial by-products used for building materials in Europe (RP-112, 1999 [6]).

Material Typical activity concentration (Bq kg1) Maximum activity concentration (Bq kg1)
226 232 40 226 232 40
Ra Th K Ra Th K
Most common building materials (may include by-products)
Concrete 40 30 400 240 190 1600
Aerated and light-weight concrete 60 40 430 2600 190 1600
Clay (red) bricks 50 50 670 200 200 2000
Sand-lime bricks 10 10 330 25 30 700
Natural building stones 60 60 640 500 310 4000
Natural gypsum 10 10 80 70 100 200
Most common industrial by-products used in building materials
Phosphogypsum 390 20 60 1100 160 300
Blast furnace slag 270 70 240 2100 340 1000
Coal y ash 180 100 650 1100 300 1500
160 K. Kovler / Construction and Building Materials 29 (2012) 158166

Table 2 We can conclude that typical activity concentrations in cements

Typical activity concentrations in Portland cement.
Reference Typical activity concentration (Bq kg1)
226
Ra 232
Th
Kovler et al. [8] 40 20
Shousha [9] 70 20
Turhan [10] 40 30
Damlaa et al. [11] 50 40
At the same time, concrete is made with raw materials of min-
eral origin that may contain natural radionuclides 226Ra, 232Th and
40
K, and their content should be limited from the radiological point
of view.
As can be seen from Table 1 adopted from RP-112 [5], typical
radioactivity concentrations in concrete shown in the rst raw of
the table are rather close to the median values of the activity con-
centrations of 226Ra, 232Th and 40K in the earths crust, which are
35, 30 and 400 Bq kg1, respectively [6].
The concentrations found in coal y ash and in some other
industrial by-products can be signicantly higher in comparison
with most common building materials, including concrete. For
example, the typical activity concentrations of 226Ra, 232Th and
40
K in y ash (FA) are 180, 100 and 650 Bq kg1, respectively (the
last row of Table 1). The arithmetic averages of the activity concen-
trations of 226Ra, 232Th and 40K in y ash reported by the UNSCEAR
[7] are also high: 240, 70 and 265 Bq kg1, respectively.
Portland cement is the viable part of concrete mix, although ce-
ment content is usually not so high (915% by mass). Typical con-
centrations of 226Ra, 232Th and 40K in cement reported in the last
publications are shown in Table 2.
These data are consistent with those available in the literature
for cement and coal FA. For example, the following typical activity
concentrations have been reported by UNSCEAR [6]:
Portland cement clinker: 80 Bq kg1 in 226Ra-series and 50 Bq kg1
in 232Th-series (the content of radionuclides in Portland cement
clinker is usually very close to that in Portland cement, because
Portland cement is made by milling clinker with a simultaneous
addition of about 5% gypsum only, therefore clinker chemical
composition dictates the content of radionuclides in cement);
226 232
Coal FA: 200 Bq kg1 in both Ra- and Th-series.
Man et al. [12] found that the mean radium equivalent of FA cal-
culated as
ARa-sq ARa 1:43ATh 0:077Ak
where ARa, ATh and AK are activity concentrations of 226Ra, 232Th and
40
K, respectively, was about four times that of ordinary cement,
which corresponds well with the data shown in Tables 1 and 2.
are usually several times lower than those measured in coal y ash.
In the last years, in view of the world policy to reduce carbon
40
K dioxide emission, more low-clinker cements (including those
blended with coal y ash and blast furnace slag) have been intro-
140
130
duced in the market by cement manufacturers in different coun-
270 tries. As a result, a gradual increase of the activity concentrations
320 in cements is observed in the last years. Still, the low content of
the modern cement in concrete, which usually does not exceed
15% by mass, even taking into account its slightly higher NORM
activity concentrations, will hardly inuence the nal specic radio-
activity of concrete mixes.
Most of the volume in concrete mix (up to 80%) is occupied by
aggregates, which are produced, mainly, from natural rocks. Thus,
specic radioactivity of aggregates is the dominating factor in the
overall radiation dose caused by exposure from concrete.
Certain types of rocks can have higher contents of uranium and
thorium than others. Examples of such rocks are certain types of
basalt, granite, acidic gneiss, pegmatite, carbonatites and black
shales such as alum shale, a uranium-rich Cambrian black shale,
which occurs in Sweden, Norway and the Danish island Bornholm.
Uranium-rich granites are found often in different countries. In
general, it is expected, that specic radioactivity of concrete con-
taining aggregates made of these rocks should be higher. For exam-
ple, in Sweden, where about 300,000 dwellings with walls are
made of lightweight concrete based on alum shale, both gamma
radiation and the radon emanating from building materials is a
major problem [13].
Examples of rocks with low contents of uranium and thorium
are many sedimentary rocks, such as gypsum, limestone, dolomite,
sandstone, quartz and shale, and sometimes volcanic rocks (with a
basic composition).
Table 3 illustrates typical activity concentrations of 226Ra, 232Th
and 40K in rocks used for producing concrete aggregates in the Nor-
dic countries, as an example.
Today coal y ash is widely used in concrete mixes as a partial
replacement of cement or the nest part of sand. When y ash is
used as a partial cement replacement in concrete, the y ash content
of the nal concrete product is usually 23% (by mass), assuming a
1525% cement replacement rate and an 8 to 1 ratio of aggregate
and water to cementitious material [14]. This EPA document [14]
concludes that since the average 226Ra content of y ash exceeds that
of cement by a few pCi g1, the use of y ash as a cement replacement
in habitable structures will, on the average, result in only a slight in-
crease in the gamma radiation exposure to people.
As a partial replacement of sand, y ash can be introduced in
3 normal-weight concrete mixes by much larger amount. At the
same time, the level of 120 kg m3 is usually not exceeded in con-
crete mixes applied in construction of habitable structures.
Although high-volume y ash (HVFA) concrete mixes containing

Table 3
Typical activity concentrations in common rocks in Nordic countries, by kerblom [13].

Type of rock Typical activity concentration (Bq kg1)

226 232 40
Ra Th K
Granite, normal 20130 2080 6202400
Granite, uranium- and thorium-rich 100500 40350 12001900
Carbonatites 10650 4010,000 1001000
Diorite, gabbro and basic volcanic rocks 130 240 501000
Sandstone and quartz 560 540 601500
Limestone and dolomite 230 0.510 <30150
Shale 10150 1060 6001900
Alum shale 1004300 1040 11001900
 K. Kovler / Construction and Building Materials 29 (2012) 158166
125225 kg m3 of y ash are known [15], such mixes are usually
cast in pavements, foundations and road construction applications,
where they have technological and economic success. However,
these applications are not of concern from a radiological point of
view. Lightweight concrete (including aerated concrete) used for
manufacture of masonry blocks is substantially different from nor-
mal-weight concrete by density, porous structure, product geome-
try (the masonry blocks can be hollow), sensitivity to climatic
conditions (higher temperature and moisture gradient, sensitivity
to indoors-outdoors air pressure difference), and therefore is out
of the scope of the present paper.
4. Radon emanation of cement, coal y ash, aggregates and
cement paste
The raw materials for concrete have different emanation coef-
cients, and this variety is expected to be an important input factor
inuencing emanation of concrete as a composite material. Some-
times this difference achieves several orders of magnitude. The dif-
ference in microstructure, morphology of the solid particles and
specic surface area of concrete constituents seem to be the most
inuencing factors explaining a different potential of radon atoms
to escape the solid matter.
Fig. 1 shows typical values of the emanation coefcient for Port-
land cement and y ash (both reported in [2]). Portland cement
(EN 197.1 CEM I 52.5N) had an emanation coefcient of 7.65%,
and y ash 0.52% only. If coal y ash is added to the clinker,
the emanation coefcient of the cement will be different, depend-
ing on the emanation properties of the y ash, its dosage and spe-
cic surface of the clinker particles, which is dened by grinding. It
can be seen from this gure that the trend in radon emanation is
exactly opposite to the trend observed in activity concentrations.
Still, it can say nothing about the expected radon emanation of ce-
ment paste.
Stoulos et al. [16] found that radon emanation coefcient for or-
dinary Portland cement (containing less than 3% of FA),
PozzolanPortland cement (containing less than 20% of FA) and
y ash was 8 2%, 2 1% and <1%, respectively. This demonstrates
clearly that the addition of FA reduces the emanation potential of
cement, which is expected, because radon emanation from the
dense glassy structure of FA particles is extremely low.
Emanation coefcients of concrete aggregates are usually simi-
lar or higher, then those of Portland cement. For example, quartz
Fig. 1. Effective activity concentrations of natural radionuclides and emanation coefcients of Portland cement and y ash [2].
161
sand has emanation coefcient of about 6% [17], granite about
15% [18].
In general, the higher is surface to volume ratio of a granular
material, the higher is its emanation power [6]. Therefore, the ema-
nation coefcients of concrete aggregates should not signicantly
inuence the emanation ability of concrete, which depends mainly
on the emanation properties of cement paste.
It is well-known that calcium silicate hydrates formed by ce-
ment hydration, have an extremely ne structure. They develop
as a mass of extremely small irregular particles of indenite mor-
phology. For example, measurements using physical adsorption of
water vapor on D-dried calcium silicate pastes indicate that CSH
has surface area of 250450 m2 g1, which is three orders of mag-
nitude higher than specic surface area of the unhydrated cement
[19].
At the same time, there is no direct proportionality between the
exhalation rate and specic surface area of cement paste, because
many additional factors inuence radon release, such as moisture
content, water and water vapor ows to the surface of the harden-
ing cement paste, heat of hydration, and porosity (not only total
porosity, but also pore size distribution and types of the pores
interconnected or closed).
A very important would be to realize that formulas (1) and (2) are
valid for the free exhalation under steady state conditions only. Free
exhalation means that radon activity at the surfaces of the building
product is zero. It is known, for example, that the extremely high
surface area of the newly formed calcium silicate hydrates (together
with other factor listed in the previous paragraph) signicantly pro-
motes radon emanation in the beginning of hydration, while poros-
ity is still high [20]. In particular, it was shown that when cement
sets, mass exhalation rate measured in hardening cement paste
can easily achieve an extremely high value about 1 mBq kg1 s1,
which would correspond to abnormally high value of the emanation
coefcient about 800% (!), if it is formally calculated by formula
(1). Obviously, in steady state the emanation coefcient, which is
a fraction of the total amount of radon produced in the solid phase
that escapes cannot exceed 100% by denition.
Radon emanation of concrete as a multiphase composite mate-
rial, containing unhydrated cement, y ash particles in their initial
form, cement gel (produced as a result of cement hydration, as well
as a result of pozzolanic reaction between y ash, calcium hydrox-
ide and water), and aggregates, will be discussed later on, where
the picture is more complicated, than that presented in the current
section.
162 K. Kovler / Construction and Building Materials 29 (2012) 158166
5. Effect of coal y ash on radon emanation of concrete
Ordinary concrete is not of radiological concern because of the
relatively low activity concentrations of natural radionuclides
(see Table 1). However, among different building materials con-
crete is generally accounts for the highest contribution to indoor
radon [21,22], and the highest radon exhalation rate normalized
to the 226Ra content [23]. This is mainly because of the unique
microstructure of cement matrix, which is made of the hydration
products with an extremely large surface area providing easy ema-
nation of radon into the pores and its further transport to the sur-
face of concrete elements. Therefore, concrete in buildings can
contribute to indoor radon levels more than other building materi-
als with the same 226Ra content.
Different researchers were interested to study how the intro-
duction of coal y ash inuences radon exhalation rate and radon
emanation of concrete. There are no general conclusions for results
from y ash substituted concrete. Previous studies have sometimes
shown that there is an enhancement, sometimes a reduction, and
sometimes no effects at all upon radon exhalation rates.
However, before making a more detailed analysis of these data,
it has to be noted that the accurate measurement of radon exhala-
tion rate and correct interpretation of the measurement results,
including the determination of radon emanation coefcient, is a
complicated task. As was mentioned before, the tests for radon
emanation of building products are not standardized yet in na-
tional and international norms, due to the differences in simulating
ideal conditions of free radon exhalation and in avoiding the inu-
ences of specimen geometry and sealing conditions, age of the
material and its moisture during the test. The exception are two
national standards, in the Netherlands, NEN 5699 [24] and Israel
(SI 5098, 2009) [25]. The methods standardized in these countries
are slightly different: according to NEN 5699, the free radon exha-
lation rate is determined by ushing the radon activity using nitro-
gen from the free volume during a dened period and by collecting
it on an adsorber (so called purge and trap method), but accord-
ing to SI 5098, the radon exhalation rate is determined in a hermet-
ically closed chamber, where the tested sample is placed (so called
closed can method). It is not obvious that the results obtained by
these two standard methods will be the same, without making a
round-robin test.
The absence of the standard method of testing radon exhalation
is not only a problem. The real problem in the research works deal-
ing with the introduction of FA into concrete is to isolate the effect
of the FA from other factors inuencing radon emanation, such as
age and moisture of the material, and its porosity (or strength, or
water to cementitious materials ratio). For example, de Jong et al.
[26] showed that when water to cement ratio of concrete increased
from 0.40 to 0.65, radon emanation coefcient increased from 10%
Table 4
Effect of introduction of y ash into concrete mixes upon radon exhalation rate.
Reference Effect of introduction of FA into concrete upon radon exhalation rate
Enhancement
Stranden [28]
Siotis and Wrixon [29] +
Ulbak et al. [30]
van der Lugt and Scholten [31]
Ackers et al. [32]
van Dijk and de Jong [33]
Roelofs and Scholten [34]
Yu [35]
de Jong et al. [26]
Man and Yeung [36]
Yu et al. [37]
Kovler and Perevalov [38]
Kovler et al. [27]
to 24%, while radon exhalation rate increased even more from 2.3
to 5.5 Bq m2 h1. Kovler et al. [27] demonstrated that each extra
percent of porosity in hardened cement pastes containing FA (from
0% to 60%), resulted in the increase of radon exhalation rate by
0.85 Bq m2 h1. It was in spite of the fact that the cementFA
compositions were designed to keep constant effective water to
cementitious materials ratio in order to provide a constant
strength and porosity. The same remark is relevant also for the ef-
fect of concrete age and moisture, which can signicantly inuence
the results of radon measurements.
Table 4 assembles the main conclusions obtained from the mea-
surements of radon exhalation rate of concrete specimens con-
ducted in different laboratories under controlled conditions. It
has to be mentioned that these results are obtained on normal-
weight concrete mixes only, while the light-weight concrete prod-
ucts (which are used mainly for building masonry blocks, which
have a completely different micro- and macro-structure and can
contain almost 100% of y ash by mass) are out of the scope of
the present paper.
Let us review in more details some of these results. It makes no
sense to repeat the literature review, which has been published re-
cently by the author [2]. Therefore, the focus here will be on those
studies, where different contents of FA were introduced in the
material, as a substitution of cement or ne aggregate, and where
radon emanation was evaluated experimentally. After nishing the
joint project, which is conducted nowadays by the group of
researchers from the National Building Research Institute, Tech-
nion, Israel Institute of Technology (K. Kovler and R. Becker), and
the Soreq Nuclear Research Center (G. Haquin and J. Koch), which
is focused on the measurements of radon exhalation rates in both
laboratory and in the rooms located at high oors and built of con-
crete (with and without y ash) at different air ventilation condi-
tions, a more reliable estimation of the inuence of coal y ash
on radon emanation will be available.
As can be seen from Table 4, the exhalation rate and emanation
coefcient of concrete containing coal FA has been studied experi-
mentally in several works, however only Siotis and Wrixon [29]
found the enhancement of radon exhalation rate of concrete con-
taining y ash. These authors measured radon exhalation rate of
concrete made of cement containing various proportions of y ash
of extremely high 226Ra activity concentration, 330 and 880 (!)
Bq kg1, signicantly higher than the mean activity concentrations
for y ash. This circumstance is often forgotten in the later publica-
tions, which refer the work of Siotis and Wrixon [29]. Indeed, these
authors found that concrete specimens containing y ash had high-
er exhalation rate. They also estimated that the additional radon
concentrations in a model dwelling would be 1.5 Bq m3. However,
this extra radon concentration indoors is so small, that it could be
hardly measured. Moreover, it can be practically neglected in radio-
Reduction No effect
+
+
+
+
+
+
+
+
+
+
+
+
 K. Kovler / Construction and Building Materials 29 (2012) 158166 163

Table 5 The similar conclusions have been obtained by van der Lugt and
Activity concentrations, radon exhalation rates and radon emanation coefcients of Scholten [31], which postulated that the ash changes the basic
concrete with and without FA [32].
structure of the material such that radon emanation is reduced.
Concrete Activity Radon Emanation Yu [35] compared the radon exhalation rates from concrete
concentrations exhalation coefcient made from ordinary Portland cement and concrete with 15% ce-
(Bq kg1) rate (%)
(Bq m2 h1)
ment substitution by FA. The radon exhalation rates from concrete
226 232 40
Ra Th K with FA were slightly higher, but not signicantly. Therefore, for
With Portland cement 11.3 10.4 111 2.5 25 the batch of FA investigated, its use as a partial cement replace-
With PortlandFA 14.5 14.8 140 1.6 13 ment in concrete was considered radiologically safe.
cement
Kovler and Perevalov [38] tested concrete mixes containing
With both PortlandFA 55.0 38.0 328 2.7 7
cement and sintered 0300 kg m3 of coal y ash, as a partial replacement of Portland
FA coarse aggregate cement and quartz sand (Table 6). It was shown that although
the activity concentrations of natural radionuclides increased line-
arly with the introduction of FA, the radon emanation coefcient
logical calculations, especially when compared with the radon ac- determined for concrete cubes, which were tested in oven-dried
tion level accepted in Europe and some other countries (200 conditions at the age of 50 days, substantially decreased more
Bq m3). Using the conversion factor of 0.017 mSv year1 per or less in the same proportion (Fig. 2). In order to neutralize the
1 Bq m3, we can estimate easily the additional inhalation dose effect of moisture on radon emanation, before the exhalation tests,
caused by introduction of this specic y ash in concrete products: which were conducted at the same age of 28 days, the specimens
0.03 mSv year1. At the same time, Siotis and Wrixon [29] also (150-mm cubes open from all sides) were oven-dried until con-
found that the emanation coefcient in concrete containing y stant mass.
ash was 5%, which is relatively low value. UNSCEAR [7] assumes that the use of y ash in building mate-
Stranden [28] presented a range of 25% for the emanation rials does not result in any additional dose due to inhalation of ra-
coefcient for concrete, with a value of 25% for concrete that con- don. This assumption is based on a number of studies, which have
tains FA. He found that the radon exhalation rate was signicantly indicated that radon exhalation rates from concrete are reduced or
lower in concrete containing FA than that in ordinary concrete. He unchanged as a result of incorporation of FA. It is assumed in these
also calculated the doses and suggested that FA will contribute to a studies that FA alters the structure of cementitious materials,
reduction in effective dose equivalent due to the reduced radon which affects radon exhalation rate.
exhalation rate. Man and Yeung [36] found that y ash substitute for cement (in
The radon exhalation of concrete, in which a part of the cement the range between 0% and 25%) changed the radon exhalation
has been substituted by coal y ash, has been studied by Ulbak properties of the concrete in such a way that it compensated for
et al. [30]. They found that while only 25% by volume of the cement the increased radium concentrations.
was replaced by FA, the 226Ra concentration in concrete was ele- Yu et al. [37] studied radon exhalation from concrete made with
vated by a factor of 1.5. At the same time, the radon exhalation rate FA substituted 25% of Portland cement similarly to the replace-
of concrete made with Portland cement and FA increased only ment ratio used in the work [30]. Concrete specimens were moni-
slightly or even decreased, despite the higher 226Ra content. The re- tored during 1 year in the lab maintained at 23 C and 60% relative
sults also indicated that measurements of radon exhalation from humidity. The authors found that exhalation rate slightly de-
samples of concrete have to be standardized on a certain humidity creased in concrete with FA. The measurements made on speci-
and age of the sample. mens at the age of 28 days1 year did not reveal any signicant
Roelofs and Scholten [34] concluded that under certain condi- effect of the age, while the measurements conducted during the
tions, the addition of FA to the concrete could even reduce the ra- rst month of curing showed that radon exhalation rate increased
don exhalation rate. a little.
Ackers et al. [32] studied radon emanation from different Concrete made with two types of cement produced in the Neth-
concrete mixes: concrete made with Portland cement, concrete erlands (Portland cement and blast furnace slag cement containing
made with PortlandFA cement and concrete made with both 30% of clinker), while 15%, 25% and 35% of the cement was substi-
PortlandFA cement and sintered FA grains as a replacement of tuted with y ash of three different types, was tested for radon
gravel. The results are self-explanatory (Table 5): it can be seen exhalation in the work by van der Lugt and Scholten [31]. The results
that the results for radon emanation coefcient are substantially showed that substituting part of the cement by y ash has almost no
lower for concrete containing y-ash products than for ordinary effect on the exhalation rate. In other words, the emanation coef-
concrete, although the radon exhalation rates for concrete made cient was lower in concrete made with FA. For concrete with Port-
with Portland cement and concrete made with both PortlandFA land cement the exhalation rate decreased using y ash with
cement and FA coarse aggregate are practically the same. average radium content. It was also found that the exhalation of

Table 6
Composition of four concrete mixes with different content of FA [38].

Raw material Composition of concrete mixes (kg m3)

Mix no. 1 2 3 4
Coal y ash (FA) 0 100 200 300
Coarse aggregate (dolomite), dmax = 19 mm 750 750 750 750
Coarse aggregate (dolomite), dmax = 14 mm 250 250 250 250
Multifractional aggregate (dolomite), dmax = 9.5 mm 400 400 400 400
Fine aggregate (quartz sand), dmax = 1.2 mm 602 510 415 323
Portland cement CEM I 52.5 220 190 160 130
Water 120 120 120 120
164 K. Kovler / Construction and Building Materials 29 (2012) 158166

Fig. 2. Effective specic radioactivity and radon emanation coefcient of concrete made with coal y ash as a replacement of cement and sand [38].

concrete was greater than the sum of the exhalation values of the
constituting components.
Van Dijk and de Jong [33] and de Jong et al. [26] studied radon
emanation of concrete with ordinary Portland and Portlandy ash
cements and found that radon emanation coefcient of concrete
made with Portlandy ash cement was lower by 20%. The latter
publication reported also that radon exhalation rate was directly
proportional to water to cement ratio, but did not nd an effect
of the concrete age, which varied from 3 months to 8 months,
while after initial sealed curing all the specimens before the test
were air-conditioned at 20 C and 50% relative humidity.
The dependence of the radon exhalation rate on the FA content
changed in a wide range in cement pastes cured in water has been
studied in the works by Kovler and Perevalov [38] and by Kovler
et al. [27]. Before testing radon exhalation, the specimens were
oven-dried at 105 C. The inuence of introducing FA into the
cement-based materials on their radon exhalation rate normalized
to their radium content is shown in Fig. 3 for the specimens tested
at different ages: 7, 28 and 90 days.
The results shown in Fig. 3 support the nding of Stranden [28]
that radon exhalation rate decreases, when FA replaces a part of
cement.
It could be also seen that the radon exhalation rate at age of
28 days in the pastes containing FA was higher than that at 7
and 90 days [27,38]. In other words, the age of 28 days was favor-
high surface area should promote the radon exhalation in time, as
can be seen from the measurements on pure cement paste.
There are two competing tendencies, which can explain obtain-
ing the maximum radon exhalation rate of cement FA materials
namely in 28 days age:
 densication of the macro-structure due to both cement hydra-
tion and pozzolanic reaction; and
 formation of the new CSH gel with extraordinarily high sur-
face area; in addition, FA particles having a dense glassy struc-
ture before the pozzolanic reaction, and as a result of that very
low radon emanation power (see the results of testing radon
emanation from cement and FA described in the paper [2]),
slowly take a part in the pozzolanic reaction, and therefore
the number of radium atoms available for emanation into the
ne microscopical pores of newly formed CSH gel, increases.
These two effects are competing, which may result in achieving
the highest radon exhalation rate in a certain age, which was
28 days (see Fig. 3). It is known that the cement hydration is much
faster than the pozzolanic reaction. Therefore, in the early age the
increase of radon exhalation rate should be dominating; but the
Radon exhalation rate to Ra content ratio,

0.12
able for releasing radon from the hardened cement FA material.
To explain this result, we would like to remind that in the course 7 days
of: (a) cement hydration and (b) pozzolanic reaction between FA 0.1 28 days
mBq m-2 s-1 per Bq kg -1

and calcium hydroxide releasing in cement hydration (both occur- 90 days

ring in time, although with different time rate), one might expect 0.08 7 days
28 days
226

a reduction in radon exhalation rate at later ages. Indeed, the ce-

90 days
ment paste structure is densifying, which should result in decreas- 0.06
ing the radon ux. At the same time, we remember, that calcium
silicate hydrates (CSH) forming by these reactions, have very ne
0.04
structure. CSH is not a well-crystallized material. In fact, it is very
nearly amorphous. As a result, it develops as a mass of extremely
small irregular particles of indenite morphology. As a consequence 0.02
of this hydrated cement pastes has very high surface areas. For
example, measurements using physical adsorption of water vapor 0
0 200 400 600 800 1000 1200
on D-dried calcium silicate pastes indicate that CSH has surface
-
area of 250450 m2 g1, which is about three orders of magnitude FA content, kg m 3
higher than unhydrated cement [19]. Measurements by N2 adsorp-
Fig. 3. Normalized radon exhalation rate (per 1 Bq kg1 of 226Ra) of hardened
tion can give even higher specic surface areas. This extraordinarily
Portland cementy ash pastes tested at 7, 28 and 90 days vs. FA content [27,38].
 K. Kovler / Construction and Building Materials 29 (2012) 158166
longer is the age of the material, the stronger is the densication of
the macro-structure, which should result in the opposite effect
decrease of radon ux from the material.
It has to be noted that under too high FA contents, which exceed
the stoichiometric ratios required for pozzolanic reaction, a signi-
cant part of the FA particles remain inert all the time. It may explain
the observation that the radon exhalation rate almost does not
change in the range of very high FA dosages of 6001100 kg m3.
It can be seen that the normalized radon exhalation rate for the
cement FA pastes slightly varies around the mean value, which is
shown separately for each age. For example, the mean value of nor-
malized radon exhalation rate was obtained 0.027, 0.035 and
0.026 mBq m2 s1 per 1 Bq kg1 of radium concentration for 7,
28 and 90 days age, respectively. In other words, the potential of
radon exhalation remains roughly the same for all the blended ce-
ment FA materials, depending mainly on the age of the material,
i.e. on the kinetics of the structure forming. However, the differ-
ence between pure cement and cement FA pastes is clearly ob-
served in any case. The normalized radon exhalation rate in pure
cement paste is 34 times higher than that in the blended materi-
als and can exceed 0.1 mBq m2 s1 per 1 Bq kg1 of radium.
Finally, the different dependences of normalized radon exhala-
tion rate in pure cement and cement FA pastes can be observed.
In contrary to its increase in time (within the ages tested) for the
pure cement paste, in cement FA pastes this characteristic
achieves the maximum value at 28 days and then decreases. The
possible reasons of such behavior have been discussed before. The
data obtained in the 2nd series of tests, in general, show that the
dosage of FA in cement paste has a limited inuence on normalized
radon exhalation rate. It is kept around 0.03 mBq m2 s1 per
1 Bq kg1 for the cement FA pastes made with different FA con-
tent. In any case, the normalized radon exhalation rate in cement
FA pastes is signicantly less than that in pure cement paste.
Literature review provided in the work by Siegel et al. [39] sug-
gests no statistical correlation between y ash content and radon
emanation, but a signicant correlation when the specic activity
of the y ash has been found. At the same time, it is shown that
when a simulation of a typical residential building is considered,
concrete containing y ash is unlikely to represent a serious risk
as it would barely elevate 222Rn concentrations in typical homes.
6. Conclusions
The use of coal y ash in concrete is a well-recognized source of
gamma exposure that is due to the presence of activity concentra-
tions of natural radionuclides 226Ra, 232Th and 40K, while the effect
of coal y ash upon radon release properties is different. Radon
exhalation rate in concrete containing coal y ash can be
sometimes slightly higher, and sometimes lower than that of the
reference mix. However, even in cases when radon exhalation rate
of concrete with y ash is slightly higher than in the reference con-
crete, radon emanation coefcient (or radon exhalation rate nor-
malized to the content of 226Ra) is lower. In view of this, the
standards regulating radioactivity of building materials, but not
addressing the decrease of radon emanation coefcient properly
could be detrimental to the utilization of y ash in concrete
construction.
It has to be emphasized that when interpreting the results, the
effect of introduction of FA into the concrete mixes on their radon
release properties should be isolated from the numerous accompa-
nying effects, which are related to the age and moisture of the mate-
rial, its porosity (or strength, or water to cementitious materials
ratio). The tests for radon emanation of building products are not
yet standardized in the international level, due to the differences
in simulating ideal conditions of free radon exhalation and in avoid-
ing the inuences of specimen geometry, sealing conditions, age of
165
the material and its moisture during the test. This is certainly a topic
for the future studies, which should precede any further standardi-
zation activities. The standards regulating radioactivity and radon
emanation of concrete containing coal y ash and other building
materials of mineral origin are out of the scope of the present paper,
but will be addressed in the separate paper of the author.
In general, drawing direct comparisons between results pre-
sented in different papers seems to be really challenging task be-
cause of varying methodologies, sample sizes, physical parameters
of the material studied and experimental goals. There is a need of
a systematic study considering different factors, which can inu-
ence the radon release from concrete, with and without coal y
ash. Such studies should include two types of the tests:
 laboratory tests of concrete specimens of the same geometry
and boundary conditions under well-controlled ventilation,
thermal and hygral conditions and
 in situ tests of radon exhalation, which should be conducted
under stable (as much as possible) climatic conditions in living
rooms built from the known building materials and products
with well-determined properties, such as density, geometry
and radium activity concentrations.
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