Construction and Building Materials 39 (2013) 2632

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Construction and Building Materials

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

Study on the expansion of concrete under attack of sulfate and sulfatechloride ions
Minghua Zhang a, Jiankang Chen a,b,, Yunfeng Lv a, Dongjie Wang a, Jian Ye c
a

Department of Mechanics and Engineering Science, Ningbo University, Ningbo 315211, China
State Key Laboratory of Turbulence and Complex System, Beijing University, Beijing 100871, China
c
Department of Water Resources of Jiangsu Province, Nanjing 210029, China
b

h i g h l i g h t s
" The higher the concentration of sulfate, the greater the expansion in specimens.
" The higher the water-to-cement ratio used, the more severe the damage found.
" The chloride ions can substantially reduce the sulfate attack.
" The higher the concentration of chloride, the less the expansion in specimens.
" Expansion and damage can be described by a new model based on micromechanics.

a r t i c l e

i n f o

Article history:
Available online 26 May 2012
Keywords:
Concrete
Sulfate attack
Chloride
Expansion
Delayed ettringite
Damage evolution

a b s t r a c t
This paper describes an experimental study on the expansion and subsequent damage of concrete specimens immersed in pure water, sulfate solutions of different sulfate concentrations, and mixed solutions
of different sulfate and chloride concentrations. Based on experimentally obtained results, a theoretical
expansion model is proposed for predicting the stresses, strains and volume expansion developed during
the process of sulfate attack. The model proposed is based on the assumption that concrete may be treated as a porous visco-elastic material, and was developed by using a micromechanics approach method.
The internal expansion force produced by delayed ettringite and gypsum is considered as the main cause
of the expansion. The expansion model was validated using the experimental results obtained.
2012 Elsevier Ltd. All rights reserved.

1. Introduction
Durability of concrete materials is one of the most important
problems in the design of concrete structures. Durability deciency, which may result in premature failure and/or decrease of
serviceability, is a major concern in developing sustainable infrastructure systems [1]. Sulfate attack is one of the phenomena that
may cause gradual but severe damage to concrete structures.
Sulfate attack on concrete leads to the conversion of cement hydration products to ettringite, gypsum, and other possible phase
changes [2,3]. Accompanying the formation of gypsum and ettringite is a volume increase. The volume expansion within concrete
cannot only reduce the porosity of concrete but may also cause
damage and cracking of the concrete leading eventually to a

Corresponding author at: Department of Mechanics and Engineering Science,

Ningbo University, Ningbo 315211, China. Tel.: +86 574 87600075; fax: +86 574
87608358.
E-mail addresses: zhangminghua@nbu.edu.cn (M. Zhang), chenjiankang
1957@yahoo.com.cn (J. Chen), lvyunfeng2008@yahoo.com.cn (Y. Lv), wangdongjie
@nbu.edu.cn (D. Wang), yejian1960@163.com (J. Ye).
0950-0618/$ - see front matter 2012 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.conbuildmat.2012.05.003

strength loss [4].Theoretical and experimental studies on the

expansion and cracking resulting from sulfate attack have been
carried out by many researchers in last decade [511]. In recent
years, research interests have been concerned with the inuence
of chlorides on sulfate attack [1220]. This is because in practice
structures are often exposed to environments that involve chlorides and sulfates, both of which are able to penetrate the concrete
through its connective pores system.
It is well known that damage evolution will affect the durability
of the concrete material and subsequently the concrete structure.
Therefore it is necessary to investigate the expansion and damage
evolution for improving the durability of concrete structures. Since
blended cements are increasingly used worldwide in order to produce durable concrete, the performance of these cements in chloridesulfate environments also need to be investigated. In this
paper, the expansion and damage of concrete specimens immersed
in pure water, sulfate solutions of different sulfate concentrations,
and mixed solutions of different sulfate and chloride concentrations were investigated by using experimental methods. Based
on the experimentally obtained results, a theoretical expansion
model was proposed to predict the stresses, strains and volume

M. Zhang et al. / Construction and Building Materials 39 (2013) 2632

expansion developed during the process of sulfate attack. The

model proposed here is based on the assumption that concrete
may be treated as a porous visco-elastic material, and was developed using a micromechanics approach method. The internal
expansion force produced by delayed ettringite and gypsum was
considered the main cause of the expansion. The expansion model
was validated using the experimental results.
2. Materials and specimen preparation
A 425# normal Portland cement was used in the experiments, supplied by Sanshi Cement Co. Ltd., Zhejiang Province, China, and which contained 13.01% Al2O3,
2.63% SO3, and 2.91% Fe2O3, weight percentage. Sand and gravel used were obtained
from local suppliers. The size of the gravel was kept to less than 20 mm. A total of
50 cylinder specimens made with two different mixtures (see Table 1) were cast in
identical plastic molds, the length and diameter of which were 500 mm and 45 mm,
respectively. The fresh concrete mix was poured into the molds, and then vibrated
on a vibrating table to remove entrapped air. The molds were covered with plastic
sheets, kept under laboratory conditions for 24 h and then demolded. Specimens
were then cured in a laboratory room, in which the temperature and relative
humidity were kept at about 20 C and 95%, respectively for 28 days.
Five different solutions (see Table 2) were used in the experiments, and contained different concentrations of sodium sulfate (Na2SO4) and sodium chloride
(NaCl). The anhydrous sodium sulfate used was obtained from Fuchen Chemistry
Reagent Co. Ltd., Tianjin, China, and the sodium chloride was obtained from Heshun
Chemistry Reagent Co. Ltd., Hangzhou, China.
Ten specimens (ve of each mix) were immersed in each solution for 1 day and
then taken out from its solution tank for 30 min drying, before the specimen lengths
were measured using a Concrete Expansion Tester (see Fig. 1). After measurement
of elongation, the specimens were placed in an oven at a temperature of about 50 C
for 20 min and then underwent a natural cooling for about 10 h. After this drying
process the specimens were immersed in the solution again. This wetting and drying cycle was repeated for 54 days.

Table 1
Mix design of concrete specimens (wt.%).
Type

W/C

Cement

Water

Sand

Gravel

I
II

0.5
0.33

14
22

7
7

29
21

50
50

Table 2
Five different ionic solutions used in experiments (wt.%).
No

Na2SO4

NaCl

1
2
3
4
5

0
3
5
3
5

0
0
0
6
10

Fig. 1. Measurement of elongation of the specimen.

27

3. Experimental results
When the concrete specimens were immersed in a sulfate solution, sulfate ions penetrated into the specimens. The use of wetting
and drying cycles accelerated the penetration of ions from the
solution into the specimens. After sulfate ions entered the concrete
pores, they reacted with hydrated cement compounds and ions in
the pore solution or on the cement pore surface. The chemistry of
the reactions is rather complicated and involves numerous overlapping steps and mechanisms. The reactions lead to the formation
of tricalcium sulfoaluminate hydrate, known as ettringite, which is
expansive in nature. The formation of ettringite crystals and the
consequent volume increase in the hardened material are considered to be responsible for expansive forces and micro-cracking
[2].The following is one of the examples of these reactions [3],

Al2 SO4 3 6CaOH2 18H2 O ! 3CaO  Al2 O3  3CaSO4  32H2 O

The solid ettringite shown in the above reaction equation,
formed by the sulfate ions not only can ll the pores but may also
cause concrete swelling, which can damage the pore structure and
thus reduce the strength of the concrete [4]. That is the so-called
sulfate attack. The typical damage of the sulfate attack is the
expansion and cracking of the concrete [511] caused by the
ettringite.
Fig. 2 shows images of the concrete specimens after they were
immersed in the ve different solutions for 54 days. As is to be expected, no macro-cracking was observed in the specimens immersed in the pure water solution (see Fig. 2a). Macro-cracking
was observed in the type-I specimens immersed in both the 3%
and 6% sodium sulfate solutions (see Fig. 2b and c). While for the
type-II specimens macro-cracking was only observed in the specimens immersed in the 6% sodium sulfate solution (see Fig. 2c). The
former is due to the high water-to-cement ratio of the type-I specimens. Since the higher the water-to-cement ratio, the larger the
porosity the concrete will have, and therefore more sulfate ions
can penetrate into the concrete. The latter is due to the high concentration of sodium sulfate solution in which the type-II specimens were immersed. As the higher the sulfate concentration in
the solution, the more sulfate ions can penetrate into the concrete.
This can be further demonstrated by comparison of the images of
type-I specimens shown in Fig. 2b with those shown in Fig. 2c.
One can clearly see that the cracking damage is much severer in
the specimens immersed in the 6% sodium sulfate solution than
in those immersed in the 3% sodium sulfate solution.
Interestingly, when the solution included chloride ions no
macro-cracking was observed in the type-II specimens (see
Fig. 2d and e). In the type-I specimens there were some macrocracks observed, but these were only in the specimens immersed
in the mixed solution of lower chloride concentration (see
Fig. 2d). Also, the macro-cracking found was smaller in the type-I
specimens shown in Fig. 2d compared to that shown in Fig. 2b,
although in both cases the solutions have the same sulfate concentration. This implies that the involvement of chloride ions in the
solution can actually reduce the sulfate attack in concrete. Chemically, this is probably due to chloride ions reacting preferentially
with the critical components and ions in the concrete. As a consequence of this, less solid ettringite will be formed. As the concentration of chloride ions increases in the pore solution, more
sulfate ions will be replaced by chloride ions and therefore less sulfate-related solid ettringite products will be formed. This is why
even in the type-I specimens immersed in a mixed solution of relatively high sulfate concentration there was still no micro-cracking
observed (see Fig. 2e). This indicates that not only water-to-cement ratio but also the concentrations of chloride and sulfate ions
can affect the sulfate attack in concrete.

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M. Zhang et al. / Construction and Building Materials 39 (2013) 2632

Type I

Type II

Type I

Type II

(a)

(b)
Type I

Type I

Type II
Type II

(d)

(c)
Type I

Type II

(e)
Fig. 2. Images of specimens (after 50 days) immersed in ve different solutions. (a) Pure water, (b) 3% sodium sulfate solution, (c) 5% sodium sulfate solution, (d) 3% sodium
sulfate and 6% sodium chloride mixed solution, and (e) 5% sodium sulfate and 10% sodium chloride mixed solution.

3.0

water
3% Na2SO4

2.5

Expansion,%

5% Na2SO4

3% Na2SO4+6% NaCl

2.0

5% Na2SO4+10% NaCl

1.5
1.0
0.5
0.0
0

10

20

30

40

50

60

Exposure time,Days
Fig. 3. Axial expansion of type-I specimens immersed in ve different solutions.

Fig. 3 shows the evolution of the average axial strains of the

type-I specimens immersed in the ve different solutions, in which
each average strain was calculated based on the measured elongations from the ve tested specimens immersed in the same solution using the Concrete Expansion Tester. It can be seen from the
gure that, the largest expansion was in the specimens immersed

in the 5% sodium sulfate solution, whereas the expansion was almost negligible in the specimens immersed in the pure water solution and in the two mixed solutions. The expansion of the
specimens immersed in the 3% sodium sulfate solution was found
to be about a half of that of the specimens immersed in the 5% sodium sulfate solution during the rst 35 days and became about
one-third of it after 35 days. It can be seen from the gure that
the expansion undergoes a slow-quick-slow-quick process. It is believed that the rst slow expansion is attributed to the hydration of
cement paste, since 28 days hydration may not be sufcient so that
the concrete will continue to hydrate when it is immersed in
water, resulting in a slight expansion of the specimen. The second
quick expansion is due to local expansion caused by sulfate attack
in the region where pores are small. The third slow expansion is
the overall volume increase generated while the sulfate products
are lling the pores. The last quick expansion is mainly due to
the macro-cracking.
Fig. 4 shows the evolutions of the average axial strains of the
type-II specimens immersed in the ve different solutions. Compared to the type-I specimens, the type-II specimens have only
small expansions. For example, the maximum average axial strains
of the type-II specimens immersed in 3% and 5% sodium sulfate
solutions are only 0.315% and 0.259%, respectively, whereas the
maximum average axial strains of the type-I specimens immersed
in 3% and 5% sodium sulfate solutions are 0.922% and 2.67%,
respectively. This indicates that the water-to-cement ratio has a
large inuence on the sulfate attack. It should be pointed out that,
the marginally larger average axial strain found in the specimens

29

M. Zhang et al. / Construction and Building Materials 39 (2013) 2632

0.35

4. Expansion model of concrete in chloridesulfate

environments

water
3% Na2SO4

0.30

The expansion of concrete under the attack of sulfate and chloride ions can be represented by the model shown in Fig. 5, in which
the pressure in the voids, P, and the micro-cracks in the matrix are
induced by delayed ettringite. Therefore, the concrete can be treated as a composite material consisting of micro-voids and viscoelastic matrix with micro-cracks. In the present model the microcracks are denoted by a dimensionless factor, D, which is a function
of time t and can be determined by experimental methods.
The following linear, visco-elastic constitutive relation can be
assumed for concrete materials with damage [21]:

5% Na2SO4

3% Na2SO4+6% NaCl

Expansion,%

0.25

5% Na2SO4+10% NaCl

0.20
0.15
0.10
0.05

rm 1  D

Lt  s : e_ m sds

0.00
0

10

20

30

40

50

60

Exposure time,Days
Fig. 4. Axial expansion of type-II specimens immersed in ve different solutions.

immersed in the 3% sodium sulfate solution than in those immersed in the 5% sodium sulfate solution was probably due to
the non-uniform expansion in the specimens and experimental
errors.
It may be observed from Fig. 4 that the specimens immersed in
pure water and those immersed in the mixed solution of 5% Na2SO4
and 10% NaCl have very close expansion evolutions, whereas those
immersed in the 3% and 5% sodium sulfate solutions have similar
expansion evolutions. The former indicates that the presence of
chlorides can indeed mitigate the sulfate attack. In the early stages
continuing hydration will lead to a slight expansion of the specimens. Because the diffusion rate of chloride ions is faster than that
of sulfate ions, when expansion and cracks resulting from sulfate
attack develop in the specimens, the chloride ions will penetrate
deep into the specimen through both concrete pores and the micro-cracks. In the presence of calcium hydroxide, chloride ions will
react with hydrated calcium aluminate to form single- and tricalcium chloroaluminates which will block the formation of ettringite. This is why a high chloride concentration in the solution can
result in the reduction of expansion of the specimens. The decrease
of chloride concentration in the solution will reduce the blocking
effect on the formation of ettringite and thus increase the expansion of the specimen, as is demonstrated by the expansion curve
of the specimens immersed in the mixed solution of 3% Na2SO4
and 6% NaCl.

em

1
1D

Jt  s : r_ m sds

where rm and r_ m are the stress and stress rate tensors, em and e_ m
are the strain and strain rate tensors, L(t) is the fourth order relaxation modulus, and J(t) is the fourth order creep compliance. Note
that L(t) can be expressed as follows,

Lt ltL0

L0 3km0 Im 2lm0 Is



where lt exp  stm if the Maxwell model is used, sm = 0.3375
day is the relaxation time of the concrete material, and L(0) is the
initial fourth order relaxation modulus, which can be expressed,

in which

1
i0  i0 ; Is I  Im ;
3
Em0

21 mm0

Im

km0

Em0
;
31  2mm0

lm0

where i0 and I are the unit tensors of the second- and fourth-order,
respectively, Em0 = 2.7 GPa is the initial modulus and vm0 = 0.2 is the
Poissons ratio. The incremental form of the constitutive Eq. (1) can
be expressed as:

Drm 1  Dt Dt

tDt

: e_ m sds  1  Dt

Lt Dt  s
Z

Lt  s : e_ m sds

By use of Taylor series expansion and omitting the terms of higher

order indenite small, L(t + Dt  s) and D(t + Dt) can be written as
follows:

Lt Dt  s Lt  s
Dt Dt Dt
Microcrack

@Lt  s
Dt
@t

@D
Dt
@t

Substituting Eqs. (6) and (7) into (5), and using the mid-value theorem of integration, we obtain,


Z t
@Lt  s
Dt
@t
0
Z t
dD
: e_ m sds 
Dt
Lt  s : e_ m sds 1  DtL0
dt
0
: e_ m sDt

Drm 1  Dt

Using the following variable separation,

Fig. 5. Sketch map of a concrete under internal expansion forces.

30

M. Zhang et al. / Construction and Building Materials 39 (2013) 2632

rm f trm0

em gtem0

10

hDrm11 i hDrm22 i hDrm33 i

0 if

nv
DP
1  nv

and hDrmij i

ij

18

and substituting Eqs.(9) and (10) into (3) and (4), it yields,

gt

1
1  Dt

jt  sf_ sds

hDem11 i hDem22 i hDem33 i

nv
1

H1 H1
1122 H1133 DP
1  nv 1111

11

By using Eqs. (11) and (18) can be expressed as follows,

0 if

Drm HDem

12

and hDemij i

ij

19

Substituting Eqs. (15) and (19) into (17) yields,

in which

hDe11 i hDe22 i hDe33 i nv q1 q2 DP

H GtL0

hDeij i 0 if


Z t
1
@lt  s
_ sds
g
Gt 1  Dt
Dt
_
@t
gt
0
Z t
dD 1
_ sds 1  DtDt

Dt
lt  sg
_
dt gt
0

q1
q2

1
H1
kl22 Hkl33

21

To simplify the analysis, only the linear and quadratic terms are
considered in the above pressure expression. Therefore,

where De1 is the incremental remote strain, which can be taken as

zero because no external loads are applied to the material, S is
1
Eshelbys tensor of the fourth-order, Dev is the incremental eigen-strain of a void caused by matrix materials and is equal to
2
Dev [22], and Dev is the incremental eigen-strain induced by the
incremental pressure of the void, which can be expressed as follows
[22],

DP

dP
Dt  C 1 2C 2 tDt
dt

22

where C1 and C2 are the parameters to be determined by experimental results.

5. Numerical results and discussion

14

In this case Eq. (13) may be simplied as follows,

Dev DPI  S1 : H1 : i0

20

P C 1 t C 2 t2 . . .

13

1
De2
v DPH : i0

1
H1
1122 H 1133
1
1
I11kl  S11kl Hkl11

Eq. (20) is the incremental expansion model of concrete materials

under internal expansion pressure. From Eq. (22) one can see that
the incremental expansion strain of concrete is directly proportional to the incremental pressure. Note that the pressure P can
be written into a power series of time, t, that is,

Eq. (12) indicates that the relationship between the incremental

stress and incremental strain is approximately linear elastic. Therefore, the incremental strain of a void, Dev , can be calculated by using
the Eshelby equivalent inclusion method as follows [22],



2
Dev  De1 S : De1
v Dev

ij

H1
1111

The micro-cracks in concrete can generally be described by

using a dimensionless factor, D, which may be approximately assumed as the function of time as follows,

15

The incremental average stress and incremental average strain of

the concrete material may be expressed by their components as
follows,




t
Dt a0 1  exp aD
t0

hDrij i 1  nv hDrmij i  nv DPdij

16

hDeij i 1  nv hDemij i nv Dev ij

17

where a0 and aD are the material constants to be determined by

experimental data, t is the time, and t0 is a referenced time. By using
mercury intrusion porosimetry and ultrasonic experiments, the values of a0 and nv can be determined (see Table 3). The material constant aD is determined based on the experimental data and is given
in Table 4 for specimens immersed in different solutions.
The stresses and strains induced by the pressure increment can
be calculated using the present expansion model. Fig. 6 shows a
comparison of the axial strains of the specimens immersed in different solutions calculated from the model and those obtained
from the experiments. The parametric values used in the expansion model are given in Table 5. It can be seen from the gure that
there is a reasonably good agreement between the model prediction and experimental data. Note that the linear and quadratic
terms in the pressure expression reect the amount of expansion
and corresponding expansion rate, whereas the different values
employed for C2 in the mixed solutions are due to the inuence
of chloride ions on the sulfate attack.

where nv is the porosity of the concrete material and dij is the component of the unit tensor of second-order, i0. Note that
hDr11 i hDr22 i hDr33 i 0 because there is no external force applied to the material. Hence, Eq. (16) can be further simplied as
follows,

Table 3
Parametric values of a0 and nv.
Type

nv

a0

I
II

0.1717
0.1547

0.8283
0.8453

23

Table 4
Parametric values of aD (to = 730 days).
Solution

0% Na2SO4 + 0% NaCl

3% Na2SO4 + 0% NaCl

5% Na2SO4 + 0% NaCl

3% Na2SO4 + 6% NaCl

5% Na2SO4 + 10% NaCl

W/C = 0.5
W/C = 0.33

0.5
1.0

3.7
2.6

6.2
3.5

0.6
1.3

0.5
1.0

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M. Zhang et al. / Construction and Building Materials 39 (2013) 2632

1.0

Experimental result for Type I

Experimental result for Type II
Theoretical model for Type I
Theoretical model for Type II

0.08

0.06

Expansion,%

Expansion,%

0.8

0.04
Experimental result for Type I
Experimental result for Type II
Theoretical model for Type I
Theoretical model for Type II

0.02

0.00

0.6
0.4
0.2
0.0

10

20

30

40

50

60

10

20

Exposure time,Days

(a)
0.18
Experimental result for Type I
Experimental result for Type II
Theoretical model for Type I
Theoretical model for Type II

50

60

Experimental result for Type I

Experimental result for Type II
Theoretical model for Type I
Theoretical model for Type II

0.16
0.14

Expansion,%

Expansion,%

2.5

40

(b)

3.5
3.0

30

Exposure time,Days

2.0
1.5
1.0

0.12
0.10
0.08
0.06
0.04

0.5

0.02

0.0

0.00
0

10

20

30

40

50

60

Exposure time,Days

10

20

(c)

40

50

60

(d)

0.09

Experimental result for Type I

Experimental result for Type II
Theoretical model for Type I
Theoretical model for Type II

0.08
0.07

Expansion,%

30

Exposure time,Days

0.06
0.05
0.04
0.03
0.02
0.01
0.00
0

10

20

30

40

50

60

Exposure time,Days

(e)
Fig. 6. Axial strains of specimens immersed in ve different solutions. (a) Pure water, (b) 3% sodium sulfate solution, (c) 5% sodium sulfate solution, (d) 3% sodium sulfate and
6% sodium chloride mixed solution, and (e) 5% sodium sulfate and 10% sodium chloride mixed solution.

Table 5
Parametric values used for the expansion force.
Solution

0% Na2SO4 + 0% NaCl

3% Na2SO4 + 0% NaCl

5% Na2SO4 + 0% NaCl

3% Na2SO4 + 6% NaCl

5% Na2SO4 + 10% NaCl

W/C = 0.5
W/C = 0.33

C1 = 1, C2 = 0.1
C1 = 1, C2 = 0.1

C1 = 1, C2 = 1
C1 = 1, C2 = 0.8

C1 = 1, C2 = 2
C1 = 1, C2 = 1.2

C1 = 1, C2 = 0.2
C1 = 1, C2 = 0.3

C1 = 1, C2 = 0.1
C1 = 1, C2 = 0.2

32

M. Zhang et al. / Construction and Building Materials 39 (2013) 2632

6. Conclusions
This paper has presented an experimental study on the expansion and damage of concrete specimens with two different waterto-cement ratios, immersed in pure water, sulfate solutions of different sulfate concentrations, and mixed solutions of different sulfate and chloride concentrations. From the present study the
following conclusions can be drawn.
 The concentration of sulfate ions in the solution has important
effect on the expansion and damage developed in concrete
specimens immersed in the solution. The higher the concentration of sulfate ions in the solution, the greater the expansion
and the more severe the damage found in the concrete
specimens.
 Water-to-cement ratio has signicant inuence on the sulfate
attack in concrete. The higher the water-to-cement ratio used,
the greater the expansion and the more severe the damage
found in the concrete specimens.
 The presence of chloride ions in the concrete pore solution can
substantially reduce sulfate attack. The higher the concentration of chloride ions in the solution, the lower the expansion
and the less the damage found in the concrete specimens.
 The expansion and damage in concrete induced by the sulfate
attack can be described by the theoretical expansion model
based on the concept of micromechanics. The model can be
used to predict the stresses, strains and volume expansion
developed during the process of sulfate attack.

Acknowledgments
The authors would like to acknowledge the nancial support received from the China National Natural Science Foundation (Grants
#10932001 and #51079069), the National Basic Research Program
of China (973 Program, 2009CB623203), the Key Research Program
of Ministry of Education of China (No. 20103305110001), the Impact and Safety of Coastal Engineering Initiative, a COE Program
of Zhejiang Provincial Government at Ningbo University (Grant
No. zj1003), and K.C. Wong Magna Fund in Ningbo University.
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