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Construction and Building Materials 39 (2013) 28

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Application of electrochemical organic corrosion inhibitor injection

to a carbonated reinforced concrete railway viaduct
Junichiro Kubo a,, Yuji Tanaka b, Christopher L. Page c, Mary M. Page c

Central Japan Railway, 900 17th Street NW, Suite 520, Washington, DC 20006, USA
Nippon Sharyo, 1-1 Sambommatsu-Cho, Atsuta-Ku, Nagoya, Aichi 456-8691, Japan
University of Birmingham, Edgbaston, School of Civil Engineering, Birmingham B15 2TT, UK

a r t i c l e

i n f o

Article history:
Available online 14 June 2012
Electrochemical injection
Organic corrosion inhibitors
Railway viaduct

a b s t r a c t
As a possible means of alleviating carbonation-induced reinforcement corrosion in aging reinforced
structures, electrochemical injection of corrosion inhibitors has been proposed. This method involves
application of aqueous solutions of organic base corrosion inhibitors onto the concrete surface with controlled current densities passed between anodes placed within the inhibitor solutions and the embedded
steel bars acting as cathodes. This present contribution describes a site trial of electrochemical inhibitor
injection applied to a 40-year-old carbonated high-speed railway viaduct in Tokyo. The efciency of
inhibitor penetration to the embedded reinforcement and the electrochemical effects brought about by
the proposed method are discussed.
2012 Elsevier Ltd. All rights reserved.

1. Introduction
After long-term atmospheric exposure, many reinforced
concrete structures throughout the world have started to exhibit
signs of carbonation-induced reinforcement corrosion and therefore require maintenance to extend their service lives [1]. The corrosion of steel reinforcement and the bursting stress caused by
rust, which occupies a much larger volume than the parent metal,
can result in cracking or spalling of the cover concrete and reduction in structural strength. Several approaches have been used in
the remedial treatment of such structures; they include partial
replacement of concrete cover, electrochemical re-alkalisation,
cathodic protection, and surface application of corrosion inhibitors
[2,3]. The method of partial replacement is considered the conventional option, but it can be time-consuming, expensive and inconvenient, often associated with noise, dust and general disruption
during the repair process. As far as electrochemical re-alkalisation
is concerned, criteria for determining completion of a successful
treatment and its long-term durability have been somewhat
unclear [46] and, in the case of cathodic protection, the effectiveness of the technique as a means of repassivating steel in
carbonated concrete requires long-term monitoring and periodic
adjustment of the impressed current installation to be undertaken
Corresponding author. Tel.: +1 202 429 1900; fax: +1 202 429 1917.
E-mail addresses: (J. Kubo), YUJI-TANAKA@cm. (Y. Tanaka), (C.L. Page),
(M.M. Page).
0950-0618/$ - see front matter 2012 Elsevier Ltd. All rights reserved.

[7]. Regarding the use of surface-applied corrosion inhibitors of

different types, several aspects of their performance are poorly
understood and there is limited published information on the
conditions needed to achieve and sustain adequate inhibitor
concentrations at the depths of corroding reinforcement in real
structures [810].
In previous laboratory investigations aimed at developing more
effective methods of using corrosion inhibitors in remedial applications, we have studied transport mechanisms, kinetics and inhibitive properties of several amines and alkanolamines that could be
electrochemically injected into carbonated concrete and related
media under the inuence of an externally applied electric eld
[1114]. The results obtained were promising but it was recognized that short-term laboratory investigations of the types undertaken could not simulate the practical conditions that might be
encountered when attempting to apply these proposed electrochemical inhibitor injection (EII) techniques to actual structures
under site conditions and that the durability of such EII treatments
could not be established without data from carefully controlled
eld trials.
It was therefore decided to conduct a preliminary trial of a
proposed version of the EII technique using a real carbonated reinforced concrete railway viaduct, which has been used to carry bullet trains in Japan for 40 years. An initial assessment of the
effectiveness of this method was made by measuring the levels
of concentration of electrochemically injected inhibitors at the cessation of the treatment and of remaining inhibitors in the vicinity
of the steel 6 months after the treatment.

J. Kubo et al. / Construction and Building Materials 39 (2013) 28

2. Electrochemical corrosion inhibitor injection

The EII technique, as described elsewhere [1114], involves passage of a constant current of fairly high density (A/m2) for a period
of several days between an embedded steel cathode and an anode
placed within an aqueous solution of organic base corrosion inhibitor in contact with the external surface of the carbonated material.
Ethanolamine (pKa = 9.5) was one of the organic base corrosion
inhibitors that were used in the above investigations, its speciation
as a function of pH being determined by the equilibrium represented in Eqs. (1) and (2) below. Its dominant form in solutions
of pH < 9.5 is therefore cationic HO  C2 H4  NH
3 while, in alkaline
solutions of pH > 9.5, it exists mainly as the neutral molecule
(HOC2H4NH2). Hence, under an applied electric eld, migration
of the cationic species occurs through a carbonated medium (pH
910) resulting in accumulation of largely molecular ethanolamine
in the vicinity of the embedded steel cathode, where a zone of
higher alkalinity is formed. The notional schematic view of the
EII technique system is as shown in Fig. 1.
It was previously demonstrated that the inhibitor could be
effectively injected into carbonated cement paste (w/c 0.6) at
depths corresponding to normal cover thicknesses for reinforcing
steel, under a high current density (5 A/m2) applied for up to a
week as shown in Fig. 2 [11]. The threshold concentrations at
which ethanolamine solutions of pH 79, which were neutralised
with CO2 and exposed to the air, are able to passivate bright steel
bars were investigated by immersion tests and found to be between 0.01 and 0.1 mol/l [13]. EII treatments using solutions of
1 M ethanolamine carbonate at 5 A/m2 applied for a week were
also shown to be effective in controlling the corrosion rates of
depassivated steel at a similar cover depth in carbonated concrete
specimens (w/c 0.86) during the exposure of treated specimens to
a cyclic wetting and drying regime for several months as shown in
Fig. 3 [13]. The other nding to note was that the restoration of
alkalinity near the cathode by EII with ethanolamine was more
moderate (pH < 12.0) than was the case when electrochemical

Fig. 1. Schematic view of EII system.

Concentration (mmole/1)















Distance from treated surface (mm)

Fig. 2. Concentration proles of ethanolamine in carbonated cement pastes.

Fig. 3. Steel corrosion rates in carbonated concrete after EII treatment cf. those of
untreated controls.

re-alkalisation was applied to carbonated concrete (pH > 13.0)

[4]. This was thought to be attributable to the consumption of signicant concentrations of cathodically generated hydroxyl ions by
deprotonation of the inhibitor ions injected at high concentrations,
as represented in Eq. (3) below

HO  C2 H4  NH3 () HO  C2 H4  NH2 H

Ka H HO  C2 H4  NH2 =HO  C2 H4  NH3 

HO  C2 H4  NH3 OH () HO  C2 H4  NH2 H2 O

3. Site trial
3.1. Target structure and preliminary survey
The target structure selected for trial application of electrochemical corrosion inhibitor injection was a viaduct that has been
in service carrying high-speed rail train cars for almost 40 years in
Tokyo. These reinforced concrete viaducts usually consist of three
elements as shown in Fig. 4(left). The designed concrete cover is
40 mm for a slab and a cantilever, 50 mm for the bottom of a beam,
and 60 mm for the side of a beam. The viaducts total surface of
56 m2 was used for the site trial as shown in Fig. 4(right). Based
on the survey record prior to the electrochemical treatment, the
reinforcing steel bars were found to be almost exactly where they
were expected to be located and the average carbonation depth
measured was 19 mm for cantilevers, 36 mm for slabs and
40 mm for bottom and side beams. The un-neutralised remainder (concrete cover minus carbonation depth), which is an indicator of the risk of initiation of carbonation-induced corrosion of
steel in concrete [15], was no greater than 10 mm in slabs and
beam bottoms. However, the corrosion potential (Ecorr, SCE scale)
and corrosion rate (Icorr) of the embedded steel, which were measured at 63 positions (for Ecorr) and 14 positions (for Icorr) in the
three sections, ranged between 67 mV and 148 mV, and
0.013 lA/cm2 and 0.123 lA/cm2 respectively. The corrosion rates
were obtained by means of EIS (electrochemical impedance spectroscopy) with an excitation signal of maximum amplitude of
20 mV applied for the interrogation of half of the steel surface
(length 40 mm) at each estimated area over a frequency swept
from 10 Hz to 0.1 mHz. The measurements were conducted by
means of portable equipment (CM-V, developed by Shikoku
Research Institute Inc.) utilising a double-electrode (DE) system
that polarises the embedded reinforcement with a round central
counter electrode (CCE, / 40 mm) and an additional ring-shaped
guard counter electrode (GCE, outer: / 106 mm, inner: / 45 mm)
surrounding the former one but captures the corrosion current
only owing through the CCE to interrogate the limited target area
[16]. These ndings implied a high probability that the steel still
remained in a largely passivated condition according to published

J. Kubo et al. / Construction and Building Materials 39 (2013) 28

Fig. 4. Target RC viaduct (left) and electrochemically treated area (right, indicated as grey box).

criteria [17] and this was conrmed by visual inspection of the

embedded reinforcement after chipping the concrete cover, which
revealed only partial thin brown rust on the exposed metal surface.
Nevertheless, judging from the un-neutralised remainder data,
it was considered likely that an increasing proportion of the steel
would become depassivated in the near future. The objective of this
site trial was therefore to examine the effectiveness of the proposed
EII treatment in accelerating the transport of ethanolamine into a
substantially carbonated concrete structure as a preventive measure against embedded steel corrosion. Other ndings obtained
through the preliminary survey were that the concentration of chloride was observed to be not signicant in terms of steel corrosion
even within the outermost 10 mm of the concrete (0.50.8 kg/m3)
and that the chloride concentration prole decayed to a negligible
level at a depth of 20 mm. This suggests that most of the chlorides
measured were not initially included in the concrete at the time
of construction but were subsequently carried to the structure by
wind from Tokyo bay. By means of mercury porosimetry, the average porosity of concrete (volume to volume) was found to be 13.0%
in carbonated areas and 13.3% in non-carbonated areas.
3.2. Preparation for electrochemical treatment
Before the current application, the concrete surface was inspected visually and by sounding with hammers to conrm that
there were no signicantly large cracks or regions of cover de-lamination. Small cracks with widths of <0.2 mm found during the
inspection of the concrete surface were sealed with silicone sealant
to avoid short circuits. To establish electric circuits, the cover concrete was rst chipped to expose the steel bars. One end of a wire
was then connected to the embedded steel (/ 13 mm) that would
act as the cathode and a cementitious mortar patch was applied to
reinstate the concrete that had been removed. The other end of the
wire was connected to a stainless steel anode mesh (/ 13 mm and
100 mm grid), xed at a 20 mm distance from the concrete surface,

via a DC power supply (galvanostats and convertors) that was able

to provide a constant current to the circuit (max capacity: 150 V
and 100 A). Independent electrical circuits were carefully prepared
for three sections surrounding each different part respectively
(cantilever, beam, and slab). The schematic view and the site picture of the circuits are shown in Fig. 5.
A solution of 1 M ethanolamine is moderately alkaline with a
pH close to 12. In order to generate a high proportion of
HO2H4NH3+ ions initially in the external inhibitor solution to be
applied onto the concrete surface, it was desired that the solution
be neutralised. However, the use of a solution with an initial excessively lowered pH as an external anolyte would be expected to
cause erosion of the concrete surface during the electrochemical
treatment because the pH of the applied solution would drop still
further during electrolysis owing to the generation of protons by
the anodic process. In a previous laboratory investigation, it was
found that the use of carbonated ethanolamine solution with its
pH adjusted to around 9.0 as an external electrolyte resulted in
efcient injection of inhibitors without damaging the concrete surface [13]. This was due to the fact that the solution contained a reasonably high proportion of inhibitor cations to be injected into
concrete and also had good buffering capacity, based on the following two chemical equilibria, which enabled it to prevent a sharp
drop in the solution pH from occurring around the anode [18]:

() HCO3 pK2 : 10:33
3 H


() CO2 H2 O pK1 : 6:35

For this site trial, the solution in a large container (1 m cube)

was therefore carbonated by bubbling carbon dioxide gas from a
cylinder (CO2 99%) at 44 l/min as shown in Fig. 6 (left). The pH
was carefully measured by means of a digital pH meter with a
glass-bodied combination electrode until it was lowered to 9.0.
Cellulose ber that was soaked with the carbonated ethanolamine
solution was sprayed onto the concrete surface to a thickness of

Fig. 5. Schematic view (left) and site picture (right) of electric circuits.

J. Kubo et al. / Construction and Building Materials 39 (2013) 28

Fig. 6. Ethanolamine carbonation setup (left) and inhibitor solution spray (right).

40 mm, so that it could sandwich a stainless steel anode mesh in

the middle (see Fig. 6 (right)). Three concrete cores (/ 50 mm
and 50 mm long) were extracted from the structure as control
specimens. The bottom surfaces of the cores were immersed in carbonated ethanolamine solutions without applied current for
7 days. The other sides of the cores were coated with an epoxy resin to minimize interaction with the air.
3.3. Electrochemical inhibitor injection
After the electric connection was conrmed to be appropriate,
electrochemical treatment was started at a constant current density of 5.0 A/m2 of the embedded steel surface. The period of treatment was 4 days (equivalent to a total charge of 480 A h/m2) for
half of the area of each of the circuits and 7 days (840 A h/m2) for
the other half. The changes in the current and voltage over time applied to each circuit were monitored. Soon after commencing the
current application, the beam circuit showed a gradual increase
in voltage, whilst the voltages recorded for the other two circuits
remained unchanged. Five hours later the voltage of the beam circuit had reached almost double the initial voltage value. It was
found that the beam concrete surface was signicantly heated. This
was probably attributable to current density application from two
directions (bottom and side) to the relatively small beam crosssection, as well as a higher resistance of the beam owing to the fact
that its concrete cover was greater than those of the cantilever and
slab. From the viewpoint of safety, it was decided that a reduced
current density of 3.0 A/m2 was to be applied for the beam circuit
during the rest of the treatment, whilst maintaining the total
charge densities of 480 A h/m2 and 840 A h/m2. This required a
longer period than initially planned. The heat generated from the
anode mesh and the concrete surface during the treatment partially dried the inhibitor-soaked cellulose ber. Therefore a small
amount of extra carbonated ethanolamine solution was sprayed
onto the ber that was attached to the concrete surface three times
each day to keep it damp. The change in pH of the external solution
in the ber was also monitored with a pH meter every 6 h. As soon
as the treatment was nished, the anode mesh and ber used for
the treatment were removed, and the concrete surface was visually
examined for any defects. The corrosion potential and corrosion
rate of the steel embedded in the electrochemically treated and

neighbouring areas were measured 2 weeks (1 week for the beam)

and 6 months after the end of the treatment to assess whether the
steel passivation was maintained or not.
3.4. Inhibitor penetration proles in concrete
At the end of the treatments at 480 A h/m2 and 840 A h/m2
respectively, cores were extracted from each area of concrete exactly beneath the embedded steel bars. Some of the cores were
used for measuring carbonation depth with phenolphthalein and
pH values in the cathodic region with pH paper (range: pH 11.0
13.6, scale unit: 0.20.4). Others were sliced into discs of
10 mm thickness with a diamond saw in order to obtain inhibitor
penetration proles with respect to the depth in the concrete by
means of ion chromatography (see Table 1). Further details of the
procedure are given elsewhere [11,12]. The nal form of inhibitor
concentration (presented in mol/l) was estimated by assuming that
the volume of concrete pore solution is calculable from the measured bulk density and porosity of the concrete and that binding
of the inhibitor by solid phases may be neglected. The concrete
cores that had been exposed to an immersion test without an applied current for 7 days were also analysed in a similar manner
to that used for the control specimens. Approximately 6 months
after the treatment was nished, cores were extracted at two positions on the slab (No. 40 and 80 in Table 1) just next to where cores
had been obtained immediately after the treatment for the inhibitor concentration analysis. The concentration proles of the inhibitor remaining in the concrete were analysed and compared with
those obtained immediately after the treatment.
4. Results and discussion
4.1. Appearance of concrete after treatment
After the treatment, no generation of new cracks or defects was
observed on the concrete surface even for beams that were temporarily exposed to higher voltage than other parts. The pH of the
external inhibitor solutions in the ber remained 9.0 throughout
the electrochemical treatment. As mentioned in Section 3.2, this
would be mainly attributable to the buffer function of the carbonated ethanolamine solutions with signicant concentrations of

Table 1
Extracted cores for inhibitor penetration analysis.


Total charge (A h/m2)

Concrete cover (mm)



Total charge (A h/m2)

Concrete cover (mm)


Beam (side)
Beam (bottom)
Slab (6 months)




Beam (side)
Beam (bottom)
Slab (6 months)



J. Kubo et al. / Construction and Building Materials 39 (2013) 28

Fig. 7. Concentration proles of injected ethanolamine in concrete just after the electrochemical treatment ((a) cantilever, (b) slab, (c) beam, and (d) control. Solid vertical
line: rebar position, broken vertical line: carbonation front).

carbonate and bi-carbonate ions shown as chemical equilibria (4)

and (5), which prevent the solution pH from dropping sharply
due to the acidity generated at the anode by electrolysis. This resulted in avoidance of any acid erosion of the concrete surface.
4.2. Carbonation depth
It was found that after the treatment the cover concrete was
seemingly re-alkalised throughout and its apparent carbonation
depth, as measured by a phenolphthalein test, was 0 mm. When
electrochemical re-alkalisation is carried out with sodium carbonate solution as the external electrolyte, it is believed that the realkalised concrete will be resistant to pH reduction during further
exposure to CO2 ingress, maintaining its alkalinity owing to the buffer function of injected carbonates in the vicinity of the concrete
surface, associated with the carbonate/bicarbonate equilibrium [4]:

Na2 CO3 CO2 H2 O () 2NaHCO3

It is suggested that a similar buffering equilibrium will also apply in the case of electrochemical injection of carbonated ethanolamine. Although the task of bubbling CO2 to produce a carbonated
ethanolamine solution of pH 9.0 during preparation of the external
electrolyte to be used for the EII treatment required time and effort, the procedure was thought to be benecial in terms of longterm durability and harmlessness to the original structure.
4.3. Efciency of electrochemical injection
Overall penetration proles of ethanolamine that was electrochemically injected into concrete are shown for the various parts

Fig. 8. Concentration proles of injected ethanolamine just after and 6 months after
the electrochemical treatment (in the slab). Solid vertical line: rebar position,
broken vertical line: carbonation front).

of the structure in Fig. 7. These results conrm that injection of

the inhibitor within the concrete was accelerated by the applied
electric eld, which caused signicant amounts of ethanolamine
to accumulate around the embedded steel. In all cases, the estimated concentrations of ethanolamine near the steel cathode exceeded the inhibitive concentration threshold (0.1 mol/l) observed
for bright steel bars immersed in neutralised ethanolamine solutions (pH 79) that were exposed to the air [13]. The difference in
injected ethanolamine concentrations recorded for the side and
the bottom of the concrete beam may be attributable to differences
in cover concrete resistances associated with their differing cover
thicknesses, which signicantly affected the magnitude of the
current density passed between the concrete surface and the

J. Kubo et al. / Construction and Building Materials 39 (2013) 28

Table 2
Evolutions of steel corrosion potential (left: mV) and corrosion rate (right: lA/cm2).


Before treatment

After treatment











Non-treated (distance)

30 cm
120 cm









1 Week

reinforcing bars. Application of this treatment to concrete structures with substantially varied cover thickness using a single electric circuit would therefore be liable to result in non-uniform
inhibitor injection. This suggests that, for the treatment to be generally effective, every circuit needs to be arranged to cover a zone of
fairly similar concrete cover thickness throughout. Reasonably detailed information on concrete cover distribution in the structure
concerned would therefore be useful in the planning stage of an
EII project.
The other notable feature of the results shown in Fig. 7 is that
treatments carried out at total charge densities of 480 A h/m2
and 840 A h/m2 did not result in major differences in the concentrations of inhibitors injected into the concrete, which implies that
a charge density greater than 480 A h/m2 may be excessive. It may
be relevant to note here that, in the case of electrochemical realkalisation, one of the issues over which it has proved difcult
to achieve a broad consensus of agreement in the literature has
concerned criteria to determine the completion of a successful
treatment [46]. Similarly for EII, the completion criteria of this
treatment must obviously be rened, taking into consideration
the long-term durability of this method in maintaining steel
4.4. Pore solution pH near cathode
The pH values recorded near the steel cathode in the core extracted from concrete at the end of the treatment at 840 A h/m2
were in the range of 12.613.2. Taking into account that this region
had not been fully carbonated before the treatment and thus the
initial pH would have been expected to exceed 13, the alkalinity
generated at the steel cathode during the electrochemical treatment did not seem to have raised the pH signicantly. The values
recorded are lower than those reported previously when electrochemical re-alkalisation was applied in the conventional manner
to columns of a different partially carbonated reinforced concrete
railway viaduct of a similar design with an un-neutralised remainder of approximately 2030 mm (pH: 13.013.6) despite the fact
that a smaller total charge density of 360 A h/m2 was used than
those involved in the present investigations [19]. As mentioned in
Section 2, the difference is readily explicable because of the consumption of cathodically generated hydroxyl ions by deprotonation
of ethanolamine cations migrating towards the cathode in the concrete. This restraint on the increase in pH near the cathode during
the treatment might be considered advantageous if electrochemical
injection of inhibitors were to be applied to concrete containing
aggregates that are susceptible to the alkali-silica reaction [20,21].
4.5. Evolution of inhibitor concentration proles after treatment
The penetration proles of the electrochemically injected
inhibitor, obtained immediately after and 6 months after the completion of the treatment of the slab are presented in Fig. 8. As was
found in previous research [13,14], when the penetration proles
of the inhibitors are compared at the two different occasions, the

2 Weeks

6 Months

paired proles resemble one another quite closely. This demonstrates that substantial concentrations of the inhibitor still remained
in the vicinity of the steel after 6 months of normal exposure
4.6. Electrochemical monitoring
The average corrosion potential (vs SCE) and corrosion rate proles of the steel bars embedded in the electrochemically treated
concrete are shown in Table 2, together with those measured at
positions in the non-treated region at a distance of 30 cm and
120 cm from the boundary. Just after the electrochemical treatment, the steel potential would have been around 1000 mV owing to electrolysis, as was observed previously [13]. The steel
potential showed recovery to more noble values with time. The relatively high corrosion rates of above 1.0 lA/cm2 observed 1 week
or 2 weeks after the treatment also recovered to 0.10.2 lA/cm2.
The average steel potential in the beam 1 week after the treatment
showed a wide range between 210 mV and 514 mV. The lower
potentials (<400 mV) were recorded at the steel bar embedded in
the region positioned at the central part of the beam. It was found
that the steel embedded in the non-treated region at 30 or 120 cm
distance from the boundary showed a similar trend in negative
shift of steel potential after the treatment, as well as its recovery
in 6 months. However, it would be worthwhile to continue electrochemically monitoring the steel embedded in the boundary area
between treated and non-treated regions to investigate the effect
of partially applied electrochemical treatment on the steel passivation in surrounding regions of the structure.
5. Conclusions and suggestions for further work
From the site trial described above, the electrochemical injection of the organic base corrosion inhibitor, ethanolamine, into
an existing aged carbonated concrete railway viaduct was found
to allow penetration of an adequate concentration of the inhibitor
in the vicinity of the steel for passivation of the steel under the
conditions studied. The moderate pH change near the steel cathode
during the electrochemical treatment, which is presumably attributable to the buffering action of signicant concentrations of ethanolamine injected to this region, would be likely to mitigate the
risk of alkali-silica reaction in concrete with certain types of potentially reactive siliceous aggregate. It was also found that variability
in concrete cover, as is usually the case in real concrete structures,
signicantly affects the current density distribution in the medium, resulting in an uneven injection treatment if the individual
anode zones are made too extensive. Detailed information on the
distribution of concrete cover within the structure is therefore
needed in order to establish a reasonable treatment plan for successful inhibitor injection. In addition, it was found in this trial that
there seems to be little advantage in increasing the total charge
density beyond a certain magnitude as this does not contribute
to further signicant enhancement of inhibitor injection. Further
work needs to be done to establish acceptance criteria to deter-

J. Kubo et al. / Construction and Building Materials 39 (2013) 28

mine the completion of a successful treatment in which efcient

inhibitor injection is achieved at a reasonable cost. This also should
include further investigation on the durability of this treatment by
continued monitoring of the condition of steel embedded not only
in the electrochemically treated area but also in its adjacent
We are grateful to the Central Japan Railway Company for
providing funds to support this site trial work.
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