Environ. Sci. Technol.
2010, 44, 3181–3186
Sequestration of CO2 by Concrete
Carbonation
I S A B E L G A L A N , * ,† C A R M E N A N D R A D E , †
PEDRO MORA,‡ AND
MIGUEL A. SANJUAN§
Eduardo Torroja Institute IETcc-CSIC, Serrano Galvache 4,
28033 Madrid, Spain, Oficemen, Jose Abascal 53, Madrid
28003, Spain, and IECA, Jose Abascal 53. Madrid 28003, Spain
Received November 25, 2009. Revised manuscript received
March 3, 2010. Accepted March 3, 2010.
Carbonation of reinforced concrete is one of the causes of
corrosion, but it is also a way to sequester CO2. The characteristics
of the concrete cover should ensure alkaline protection for
the steel bars but should also be able to combine CO2 to a certain
depth. This work attempts to advance the knowledge of the
carbon footprint of cement. As it is one of the most commonly
used materials worldwide, it is very important to assess its
impact on the environment. In order to quantify the capacity
of cement based materials to combine CO2 by means of the
reaction with hydrated phases to produce calcium carbonate,
Thermogravimetry and the phenolphthalein indicator have been
used to characterize several cement pastes and concretes
exposed to different environments. The combined effect of the
main variables involved in this process is discussed. The
moisture content of the concrete seems to be the most influential
parameter.
Introduction
One of the main problems related to climate change is the
greenhouse effect produced by the partial absorption of
infrared radiation emitted by the Earth by the so-called
“greenhouse gases”, including CO2. The United Nations
Framework Convention on Climate Change defines “sink”
as “any process, activity or mechanism which removes a
greenhouse gas, an aerosol or a precursor of a greenhouse
gas from the atmosphere”. As part of the initiatives under-
taken by the cement industry to reduce the greenhouse effect,
this work studies the extent of the CO2 sink effect of concrete
carbonation.
Carbonation of concrete takes place when the CO2 from
the atmosphere reacts with the alkaline components of
concrete, mainly portlandite, and/or with the CsSsH
(hydrated calcium silicate) gel, resulting in the formation of
CaCO3. The reaction generally leads to a decrease in the pH
of the aqueous phase of the concrete pores, from very alkaline
values greater than 12 to values below 8. If the reaction reaches
the steel reinforcement, its passive layer may disappear,
exposing the steel surface to corrosion.
Most of the publications related to carbonation are mainly
focused on its relationship with rebar corrosion. Their main
objective is to measure and predict the progress of the
carbonation front and the evolution of corrosion due to the
* Corresponding author phone: +34913020440; fax: +34 913020700;
e-mail: isabelgalan@ietcc.csic.es.
†
Eduardo Torroja Institute IETcc-CSIC.
‡
Oficemen.
§
IECA.
10.1021/es903581d  2010 American Chemical Society
Published on Web 03/12/2010
steel depassivation. The phenolphthalein indicator technique
is used to measure the carbonation front, which is actually
a pH front that differentiates zones with pH below and above
8-9. Closest to the object of this publication, there are some
studies which focus on the amount of CaCO3 formed during
natural carbonation process. Leber and Blakey (1) used
chemical analysis to estimate the carbonation degree in
mortars and concretes, based on the assumption that all
absorbed CO2 reacts with the lime to form calcium carbonate.
Steinour (2) proposed a formula to calculate the amount of
CO2 incorporated by carbonation based on the clinker
composition. Thermogravimetry (TG) and differential ther-
mal analysis (DTA) have been used for both qualitative and
quantitative studies of the carbonation phenomenon by some
authors (3-6). Houst and Wittmann (7) used an induction
furnace and an IR analyzer to measure carbonation and
concluded that there is no simple corelation between depth
measurements and carbonates profiles. All these authors have
contributed to better delimit the depth of carbonation, and
also to provide information on the amounts of combined
CO2.
There are also some recent publications regarding the
CO2 absorption capability of cement based materials from
U.S. (8, 9), Norway (10) and UK (11). One of the most
exhaustive studies was carried out by a consortium of research
institutes and cement industries from Denmark, Sweden,
Norway and Iceland (12-17). This work studies the CO2
absorption capacity of cement based products in these four
countries throughout their service life and after a process of
demolition and recycling, considering structures of 100 years
of total life, with 70 of service life and 30 of secondary life.
The percentages of CO2 absorption given by these authors
vary depending on the assumptions taken, the experimental
measurements on which the studies are based and the
calculations used to obtain the results. As it is very com-
plicated to extrapolate values and to generalize laboratory
results, the comparison of the results obtained in the different
studies is very difficult.
The main objective of this study was to estimate the
quantity of CO2 that is reabsorbed into cementitious materials
due to the carbonation phenomenon, taking into account
cements’ composition, environments, type of concrete, and
time. The study was based on Spanish cement, concrete uses
and applications, and the continental climate in Madrid.
Experimental Section
The cements used to fabricate the specimens are given in
Table 1. 10 × 10 × 60 mm prismatic paste specimens and
75 × 150 mm cylindrical concrete specimens were produced.
Two water/cement ratios (w/c) were used for the mixtures:
0.6 and 0.45. For the specimens with w/c 0.6, cements
numbered 1-12 were used. In addition to the 12 cements
selected for the 0.6 w/c specimens three more were added
for the 0.45 w/c specimens. This explains the ordering of the
cements in Table 1, grouped by type of additions. For the
specimens with w/c 0.45, all 15 cement types were used.
The concrete mix with 0.6 w/c and 300 kg/m3 is considered
representative of concrete used for building works, and the
one with 0.45 w/c and 400 kg/m3 for civil works. The curing
period was 48 h. The specimens were then dried inside for
26 days. After 28 days the specimens were placed in three
different environmental conditions: outside exposed to the
rain, outside sheltered from the rain, and inside, on the
Eduardo Torroja Institute campus in Madrid. As the speci-
mens were put on a grill, all surfaces were exposed to the
VOL. 44, NO. 8, 2010 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 3181
TABLE 1. Cements Selected for the Tests
ref cement clinker % additions CaO % producer origin
1 CEM I 42,5R 95-100 no additions 64 Lafarge-Asland Toledo
2 I 42,5R/ SR 95-100 no additions 63 Uniland Barcelona
14 CEM II/A-L 42,5R 80-94 limestone 62 Cosmos Huelva
3 CEM II/B-LL 32,5N 65-79 limestone 56 Cemex Alicante
4 CEM II/A-M (V-L) 42,5R 80-94 fly ash, limestone 57 Portland-Valderrivas Madrid
5 CEM II/B-M (S-V) 42,5N 65-79 GBFS, fly ash 54 Holcim Almerı́a
6 CEM II/A-P 42,5R 80-94 pozzolan 53 CEISA Las Palmas
7 CEM II/B-P 32,5N 65-79 pozzolan 49 Cemex Toledo
9 CEM II/A-V 42,5R 80-94 fly ash 56 Lemona Vizcaya
10 CEM II/B-V 32,5R 65-79 fly ash 49 Cosmos Córdoba
13 CEM IV/B (V) 32,5N 45-64 fly ash 41 Alfa Santander
8 CEM II/A-S 52,5N 80-94 GBFS 60 Tudela Veguı́n León
15 III/A 42,5N/SR 35-64 GBFS 56 Tudela Veguı́n Oviedo
11 III/B 32,5N/SR 20-34 GBFS 46 Alfa Santander
12 III/C 32,5N/SR/BC 5-19 GBFS 47 Cemex Tarragona

atmosphere. The specimens not sheltered from the rain
(Figure 1) were never submerged in water, as rain always
washed away.
In addition to these specimens made specifically for the
study, samples from old structures and specimens were taken
and analyzed in order to evaluate the effect of time. Three
types of concrete specimens made in 1991, 1999, and 2001
were selected. The specimens from 1991 were 7 × 7 × 28 cm
prisms fabricated with 395 kg/m3 and six different experi-
mental mixes: two without additions, two with fly ash, one
with silica fume, and one with fly ash and silica fume.
Plasticizers and superplasticizers were used for all mixes.
The specimens were kept outside sheltered from the rain.
The specimens from 1999 were 7.5 × 15 cm cylinders
fabricated with 400 kg/m3 and microsilica and fly ash
additions as well as superplasticizer. These specimens were
kept inside. The specimens from 2001 were taken from
concrete used to build a house. A standard mix for building
works was assumed for making the calculations, cement
without additions, 300 kg/m3 and 0.5 w/c. For the first four
years these specimens were kept outside exposed to the rain
and the rest of the time sheltered from the rain.
Two reinforced concrete structures designed by Eduardo
Torroja were chosen for taking old samples: the roof of the
Zarzuela Hippodrome, built in 1935, and a column from the
pergola built in 1951 in the gardens of the Eduardo Torroja
Institute. From the documentation available about concrete
in Spain before the seventies and from suggestions from
experts in the field, it was assumed that, in both cases, cement
FIGURE 1. Specimens Outside Not Sheltered from the Rain.
without additions, 0.5 w/c and 300 kg/m3 were used. The
thickness of the Hippodrome roof varies from 65 cm in the
area of the columns to 6 cm at the edges. Samples,
approximately 50 mm thick, were taken from both the upper
and the lower part of the roof. The upper part is covered by
an asphalt layer added after the construction of the structure.
In the pergola, the thickness of the columns also varies from
approximately 30 to 10 cm. The sample taken from the upper
part of one of the columns was about 20 mm thick. All
columns were painted some years after the construction and
in 1993 some of them were repaired using different methods.
The column chosen for the study was repaired with traditional
mortar.
After one year of exposure, the carbonation depth, that
is, the depth at which the pH drops below 8-9, was measured
in the new specimens by means of phenolphthalein col-
oration. From the uncoloured carbonated part a representa-
tive sample was taken to perform thermogravimetry (TG)
and differential thermal analysis (DTA). These techniques
allow the determination of the carbon dioxide present in the
sample from the mass lost in the dissociation of calcium
carbonate.
The quantities of calcium carbonate formed in this
“carbonated” front may change with depth; the surface may
absorb more CO2 than the inner part. For this study the whole
“carbonated” part was taken, that is, the average value of
CO2 absorption in the zone with pH lower than 8-9 was
considered. Also, the “noncarbonated” part may absorb CO2
even though the pH does not drop below 8, but this
absorption is not taken into account. In this sense the “real”
CO2 absorption might be underestimated.
As the samples’ masses change with time and carbonation
due to the uptake and release of water and the uptake of
CO2, some calculations were done to obtain all values in
percentages of CO2 per gram of cement instead of per gram
of sample. For this, samples were also characterized at the
age of 28 days, and the amount of cement in the sample
(mass that remains after TG calcinations) and the initial
CaCO3 content were taken as reference values. In order to
express the results in CO2 absorbed per mol of CaO available
for carbonation, the CaO content in the different cements
was measured by chemical analysis (Table 1).
For performing TG in the concrete samples, the “mortar”
part was taken, that is, the coarse aggregates were removed
from the samples and the fine aggregate/cement mix
proportions were assumed to perform the corresponding
calculations.
The old specimens were also characterized by the same
two techniques at their corresponding age. It was possible
to determine the carbonation depth in the old specimens

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FIGURE 2. Carbonation rates of concrete specimens 0.6 w/c.
FIGURE 3. Carbonation rates of concrete specimens 0.45 w/c.
but not in the case of the old structures because the samples
taken were not thick enough to perform the coloration test
accurately. The characteristic parameters of environmental
conditions were regularly measured both inside and outside.
Results
Environmental Conditions. The relative humidity (RH)
measured inside varied between 24 and 68% with an average
value of 38%. Outside it varied between 27 and 97% being
the average value 57%. The inside temperature was in the
range of 13-25 °C, with an average value of 22 °C, and outside
0-31 °C, with an average value of 16 °C. The CO2 concentra-
tion measured inside varied between 500 and 850 ppm.
Outside it was almost constant 500 ppm. This high value
compared to the average atmospheric concentration is
probably due to the highway which is close to the site where
the specimens were placed. The daily precipitation varied
between 0 and 40 mm.
Carbonation Depths and Rates. A similar behavior in the
carbonation depth with regard to the environment was found
in the paste specimens made for the study. In general,
specimens outside sheltered from the rain presented maxi-
mum depth after 1 year, appearing colorless throughout the
tested area. Specimens kept inside also appeared fully
carbonated throughout the cross section, but in this case
with very soft pink color, indicating that the pH did not drop
below 8. Finally, about half of the specimens kept outside
exposed to the rain presented maximum depth colorless,
and the other half partial depth with a pink core.
In Figures 2 and 3, the rates of carbonation for the concrete
specimens with 0.6 and 0.45 w/c in the three exposures are
represented. The rate was calculated with the formula x )
k · t1/2. The specimens are grouped according to type of
additions, with the reference numbers shown in Table 1.
The results clearly show a higher rate of carbonation in
the concretes made with the mixes considered representative
of building works (lower cement content) than in the ones
made with the mixes representative of civil works. This
difference is in some cases as much as double.
In general, the specimens that were kept outside sheltered
from the rain are the ones with the highest carbonation rates,
while the ones that were kept inside present the lowest rate.
In this regard, the 0.45 w/c specimens present a more
homogeneous behavior than those with 0.6 w/c. It is worth
highlighting the increase in carbonation depth with the
percentage of addition within some of the groups of cement
types; this effect is indicated by arrows in Figures 2 and 3.
Concrete specimens 1 and 2 show very similar behavior
in the carbonation rate of the front advance in each of the
environments, with both w/c ratios. The fact that cement
has low C3A and cement 1 has normal C3A content does not
appear to have an effect on the carbonation rate.
Regarding the old specimens, most of them presented
rates lower than 3 mm/year1/2, with four of the 1991
specimens not reaching 1 mm/year1/2. The 1999 specimen
is the one which presents the highest rate, close to 5 mm/
year1/2.
The carbonation rates are not easily comparable to the
data published by some of the authors that have studied the
natural carbonation phenomenon from the point of view of
calcium carbonate formation (4, 6, 7), as the environmental
conditions and type of specimens are very different. However
it should be noted that none of the rates published by theses
authors exceeds 6.5 mm/year1/2.
Quantities of Combined CO2. Figures 3 and 4 represent
the molar percentages of CO2 absorbed per mol of CaO in
the “carbonated zone” (indicated by the colorless phenol-
phthalein) after 1 year in the pastes made with 0.6 and 0.45
VOL. 44, NO. 8, 2010 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 3183
FIGURE 4. CO2 quantities absorbed in paste specimens 0.6 w/c.
FIGURE 5. CO2 quantities absorbed in paste specimens 0.45 w/c.
w/c, respectively. These values were measured with TG
analysis, taking the values at 28 days as references.
The behavior of the 0.6 w/c specimens (Figure 4) was
very homogeneous with regard to the influence of the
environment on their CO2 sequestration capacity. The
specimens that absorbed less CO2 were those kept inside,
not reaching values higher than 13%. On the contrary, the
ones that absorbed more CO2 were those that were outside
exposed to the rain reaching values of absorption of 33 mol
of CO2 per 100 mols of CaO in the carbonated zone. The
specimens that were kept outside sheltered from the rain
absorbed between 12 and 23% of CO2 per mol of CaO. These
results demonstrate the great importance of the sample
moisture content in the combination of CO2.
Regarding the 0.45 w/c specimens (Figure 5) the ones
kept inside were also those that absorbed less CO2, with the
exception of specimen 2 without additions and specimen 4
with fly ash and limestone. However, the specimens that
absorbed more CO2 were in half of the cases those sheltered
from the rain, and in the other half the ones that were exposed
to the rain. The behavior of the two groups of concrete
specimens, w/c 0.6 and 0.45, is similar to the paste specimens
with 0.6 w/c with regard to the environment. In general, with
few exceptions, the specimens of concrete made with w/c
0.45 absorb less CO2 than the specimens made with w/c 0.6,
being the percentages of CO2 uptake quite similar to those
found in the paste specimens.
In the old specimens and structures, the quantities
absorbed varied from zero to 36%. From the group of
specimens produced in 1991 three of them did not practically
absorb CO2 during the exposure time. The other three 17
years old specimens did absorb CO2 but did not reach 14%
of absorption, being the specimens made with fly ash the
ones that absorbed more CO2. The specimen made in 1999
absorbed less than 10% of CO2 per mol of CaO in nine years.
The specimens made in 2001 with a building type of concrete
absorbed between 27 and 36% CO2 in seven years. In the
tested sample of the Pergola, a quantity of 33% of CO2
absorbed over about 57 years was measured. The two samples
from the Hippodrome absorbed very different amounts of
CO2: about 30% in the upper part and 3% in the lower part.
The difference might be explained as a consequence of the
3184 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 44, NO. 8, 2010
difference in humidity between the upper and lower parts
of the roof. The humidity in the upper part might have been
higher due to its likely exposure to the rain at some points
in time. However, this is only a hypothesis. In general, it is
very difficult to give an explanation as we do not know exactly
about the repairs, alterations and paintings the old structures
have undergone throughout their life.
Figure 6 represents all the data of CO2 absorbed as a
function of time collected in this study, both for specimens
made for the study and for the old ones, as well as for the
data collected from the literature. In some cases, as the data
are expressed in different units, some calculations and
estimations have been made to express the results in the
same units as the rest of the results in the study.
The two horizontal gray and black lines represent the
maximum possible absorption according to the proposals of
Steinour (2) and Pade and Guimarares (17), respectively.
Since these are different samples and different conditions
the values can not be directly compared, however, it can be
said that in most of the cases absorptions above 50% per mol
of CaO in the carbonated part are not reached.
Discussion
Indicator Parameters and Characterization Techniques.
The depth of carbonation x measured by means of the
phenolphthalein indicator and the carbonation rate k are
parameters of interest when studying the corrosion of steel
reinforced concrete because they help to identify the pH
change front and its evolution with time. However, they do
not provide information on the amount of calcium carbonate
formed since no general relationship between the depths of
carbonation and the quantities of calcium carbonate formed
was found. Trends in the relationship could only be seen
within groups of samples.
The amount of CO2 absorbed is also a key parameter not
only to calculate the ability of cement based materials to
reabsorb CO2, but also to model the progress of carbonation.
Using Thermogravimetrical techniques the carbon dioxide
absorbed and combined as calcium carbonate can be
determined. Other techniques should be used to measure
other possible minor contributions to CO2 absorption arising
from other phases, and more research should be performed
FIGURE 6. Quantities of CO2 absorbed as a function of time 0-80 years.
in the future in order to complement these data and to avoid
the underestimation of the CO2 absorption.
Influence of the Exposure Environments. Humidity is
one of the most influential factors in the advancement of the
carbonation front and in the amount of CO2 combined. In
general terms, specimens made for the study that were kept
outside sheltered from the rain presented higher carbonation
depth after one year than those that were outside not
sheltered. In contrast, the amounts of CO2 absorbed in this
“carbonated” zone were greater in the specimens that were
outside exposed to the rain than in the ones kept outside
sheltered. These differences are attributed to the degree of
water saturation of the pores resulting from the moisture
changes that occur inside the concrete as a consequence of
the rain-drying cycles.
The amount of CO2 combined in the specimens and the
carbonation depth reached during the first year of exposure
were considerably lower in the internal environment than in
the external environment. This result indicates that a higher
concentration of CO2 in the interior does not imply a greater
sequestration of CO2 in the range of CO2 concentrations
considered. The other parameters involved, mainly the
relative humidity, appear to have a greater influence.
Type of Cement. There are significant differences in the
resistance to carbonation (amount combined and carbonated
depth) of the different specimens depending on the type of
cement used, linked both to the type of additions and to the
amount of clinker per m3 of concrete. In general, with
increasing amount of clinker, the amount of CaO increases,
that is, material subject to carbonate. When introducing
additions to the cement, it is important to take into account
that the water/clinker ratio will increase, but it is also very
important to know the contribution of the additions to the
CaO content.
By increasing the amount of CaO, the amount of CO2
absorbed increases generally and the depth of carbonation
decreases, being the relationship with depth much more clear
than the relationship with the combined CO2. Both relation-
ships become more evident when considering the groups of
additions separately, and also when dividing them by
environments. In any case, it is important to note the presence
of exceptions.
It can be stated that there is a combined dependence of
the type of cement and the environmental conditions on the
carbonation.
Life Time. There are several models to predict the progress
of the carbonation front, mostly based on the solution of
Fick’s law. The effectiveness of these models has been
experimentally tested on numerous occasions. However, it
is important to be cautious when using them as the constants
of proportionality depend on many factors.
Regarding CO2 combined there are very few models or
proposals. The evolution of CO2 combination with time is
not evident. Young samples may have greater uptake than
older ones. In general, the ones studied here do not exceed
50% of CO2 absorption (per CaO mol) in the carbonated
zone.
Composition of Concrete. By increasing the amount of
cement in the concrete, both the carbonation depth and the
amount of CO2 absorbed decrease, being the main cause for
that the decrease in porosity. The fact that the amount of
CO2 decreases as the cement content increases indicates that
a decrease in porosity has a higher influence than an increase
of the amount of carbonatable material.
Calculation of CO2 Absorbed. Based on the carbonation
depth data, the CO2 absorbed in the carbonated zone, the
exposed surface of the concrete, and the mix proportions,
the amount of CO2 absorbed per m3 of concrete in a structure
can be calculated.
The corresponding CO2 absorbed in the carbonated
concrete is determined by multiplying the CO2 absorbed
per kg of cement in the carbonated zone by the amount
of cement in the concrete. On the other hand, by
multiplying the carbonation depth by the relationship
between exposed surface and concrete volume, the
relationship between carbonated concrete volume and
total concrete volume is determined. Finally multiplying
these two terms, the CO2 absorbed per total concrete
volume is calculated.
The results can also be expressed per ton of cement
produced taking into account the relationship between
cement produced and concrete consumed. To express the
results per ton of CO2 emitted, the relationship between the
amount of cement produced and the amount of CO2 emitted
in their production should be considered.
As there are not enough available data of surfaces exposed
to carbonation and as the cement and concrete market is
continuously changing, the calculations of the CO2 seques-
tration should be done very carefully. Considering the
carbonated zone as the region where the pH is lower than
8-9 may underestimate the real CO2 absorption in the whole
volume, because, as stated before, there might be absorption
as well in the region with higher pH. To obtain more accurate
calculations absorption profiles at all depths in the samples
should be measured in the future, both in front and behind
the pH front.
From the data obtained in this study, it can be concluded
that the carbonation depth is not a correct indicator of the
amount of sequestered CO2. Regarding the parameters
influencing the CO2 sequestration, higher water/cement ratio
implies normally higher porosity which, in turn, leads to
higher CO2 absorption. Within groups with the same type of
VOL. 44, NO. 8, 2010 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 3185
additions, the amount of CO2 bound increases with the CaO
content. The big differences between exposure sheltered and
not sheltered from the rain demonstrate that the moisture
content of the concrete is a key parameter in the sequestration
of CO2 by natural carbonation. In general, while the influence
of the type of cement and the proportion of cement can help
to predict the degree of carbonation, these are comparatively
less important than the effect of humidity in the process of
carbonation.
Acknowledgments
This work was supported by the Spanish Ministry of Science
and Technology, Oficemen, and CSIC to whom the authors
are grateful.
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