Construction and Building Materials 198 (2019) 696–709

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Construction and Building Materials

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

Nondestructive experimental characterization and numerical simulation

on self-healing and chloride ion transport in cracked ultra-high
performance concrete
Jinyang Jiang a,⇑, Xuejiao Zheng a, Shengping Wu a, Zhiyong Liu a, Qi Zheng a
a
Jiangsu Key Laboratory for Construction Materials, Southeast University, Nanjing 211189, China

h i g h l i g h t s

The evolution of self-healing was simulated by the model CEMHYD3D.

Portlandite crystallizes in the middle of the crack.

C-S-H gel accumulates only on the crack surface.

Ions transport depths was simulated by finite difference method.

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

Article history: Ultra-high performance concrete (UHPC) contains a large number of unhydrated particles which are
Received 7 March 2018 prone for self-healing in the presence of water. In this work, three-dimensional X-ray microscope was
Received in revised form 30 September employed to investigate the self-healing degree. To aid in understanding the evolution of self-healing,
2018
a hydration model CEMHYD3D was utilized to simulate the distribution of solids and pores phase in a
Accepted 6 November 2018
cracked microstructure. Based on the random walk model, the influence of crack self-healing degree
on chloride ion transport process was analysed. The results show that the smaller crack width and the
longer healing time reflect a lager self-healing degree. According to the rehydration products, it was
Keywords:
Ultra-high performance concrete
found that portlandite crystallizes in the middle of the crack while C-S-H gel accumulates only on the
Crack crack surface. Moreover, the ions transport depths in cracked UHPC was simulated by finite difference
Self-sealing method. As time increases, chloride ions not only transport vertically along the crack, but also propagate
Transport properties in the horizontal direction of the crack. Mixture proportions have little influence on the diffusion coeffi-
Simulation cient of chloride ion.
Ó 2018 Elsevier Ltd. All rights reserved.

1. Introduction as harsh environmental exposure, excessive loading, poor con-

Ultra-high performance concrete (UHPC) usually refers to super
concrete with compressive strength more than 150 MPa, tensile
strength greater than 7 MPa. UHPC has super high strength [1],
high toughness [2], high impermeability [3], high corrosion
resistance [4], high explosion resistance [5] and high anti-
electromagnetic interference [6] and other excellent performance
[7]. With a high amount of cement and supplementary cementi-
tious materials, low water-to-binder (w/b) ratio, mixing with ultra-
fine powders and other reagents, UHPC usually exhibits large
early-age autogenous shrinkage, which can cause cracking [8,9].
In addition, cracks of UHPC often occur due to external factors such
⇑ Corresponding author.
E-mail address: jiangjinyang16@163.com (J. Jiang).
struction procedures, or design error. Accordingly, self-healing of
cracked concrete is a good way to extend the service life of the
structure and reduce the maintenance costs.
Self-healing of cracked cement-based materials can be classified
into three types: intrinsic healing, capsule based healing and vas-
cular healing [10]. Autogenous healing is an intrinsic characteristic
of concrete that can be mainly attributed to two mechanisms: fur-
ther hydration of the unhydrated cement particles [11] and subse-
quent carbonation of Ca(OH)2 [12–14]. In this paper, we mainly
study the intrinsic healing in self-healing caused by hydration.
The phenomenon of autogenous healing in cementitious materials
has been verified with experimental investigation and practical
experience. For mature UHPC, whether steam curing or conven-
tional curing unhydrated cementitious particles are above 50%
[16]. The alternative binder materials, such as silica fume and fly

https://doi.org/10.1016/j.conbuildmat.2018.11.054
0950-0618/Ó 2018 Elsevier Ltd. All rights reserved.
 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709 697

ash, react slower compared to cement and thus more unreacted 100 20
binder material remains available within the UHPC to cause crack
Cumulative curve (Silica fume)
healing by further hydration. So, there are more substances within
80 Cumulative curve (Cement) 16
UHPC that can produce self-healing. In wet or water environment,

Cumulative fraction (%)

Differential fraction (%)

external moisture enters the interior of the cracked UHPC causing Cumulative curve (Fly ash)

relatively high content of unhydrated cementitious particles to
continue to hydrate and promote crack healing. The current
research on the degree of crack healing focuses on the recovery
of permeability [15] and mechanical properties (compressive or
flexural strengths) [14,16–18]. And micro-focus X-ray computed
tomography(X-CT) [19–21] was used to characterize the amount
of crack healing products. However, these studies mostly analyze
the effect of the cracks on the self-healing properties from the
macro perspective, and lack the analysis of self-healing properties
from a mesoscopic point of view. Hydration model CEMHYD3D
[19] was used to simulate the self-healing degree of the meso-
scale cracks from the meso perspective and analyze the distribu-
tion of the healing products in the cracks.
Cracks after autogenous healing will improve the possibility of
regaining mechanical performance and durability of concrete.
Self-healing of cracks can significantly reduce the ingress of harm-
ful agents through cracks into cement-based materials and thus
prolong the service life of concrete structures, even if the cracks
are not completely filled with new reaction products [22]. Ingress
of water in cement-based materials has been simulated by the
Fick’s law and water interaction with the unhydrated cement par-
ticles led to later hydration based on a hydration model [23]. Fur-
thermore, self-healing can also affect the evolution of geometry
and transport properties of existing cracks [24,25]. Crack autoge-
nous healing seems to have a beneficial influence on water or chlo-
ride penetration and Maes [26] studied the transmission rate of
chloride ions in cracks after cracks healed to some extent, the
quantitative relationships between these variables are not clear.
Despite being constrained by many factors related to the exter-
nal environmental conditions and the material characteristics,
cracked UHPC materials have the ability to self-healing. In this
work, the influence of self-healing in cracked UHPC is investigated
by digital image based model. In detail, chloride ion diffusion coef-
ficient was obtained by random walk model according to the
microstructure of crack. In addition, the effect of self-healing
degree on chloride ion transport process is considered in the pro-
posed finite difference method.
2. Experimental program
2.1. Materials and mix design
Three main cementitious materials, cement, fly ash and silica fume were used in
this experiment. Portland cement type I was supplied by Onoda Cement Plant,
Jiangsu province, P.R. China, which has a density of 3.15 g/cm3 and a specific surface
area of 362.2 m2/kg. Fly ash with class I was provided by Nanjing Hotspring Plant,
with a density of 2.24 g/cm3 and a specific surface area of 454 m2/kg. Silica fume is
Ekeen grade 95 with a density of 2.25 g/cm3 and a specific surface area of
29,900 m2/kg. The specific chemical composition of the three cementitious materi-
als is given in Table 1. Particle size distribution of cementitious materials was char-
acterized by using particle size analyzer that presented in Fig. 1. High efficiency
polycarboxylate superplasticizer was provided by Jiangsu Subote company, with
the solid content of 40%.
60 Differential curve (Silica fume) 12
Differential curve (Cement)
Differential curve (Fly ash)
40 8
20 4
0 0
0.01 0.1 1 10 100 1000 10000 100000
Size (um)
Fig. 1. Particle size distribution of cementitious materials.
The ultra-high performance concrete (UHPC) mixture proportions are listed in
Table 2. All mixtures were prepared using a 19JJ-5 planetary mortar mixer at room
temperature (20 °C). The mixing procedure was composed of two steps: (1) dry
cementitious materials were homogenized at 60 rpm for 3 min; (2) the liquid solu-
tion composing of superplasticizer and water was added and then mixed at
120 rpm for 5 min. For each UHPC mixture, samples were cast with vibration table
shaking 60 times. Immediately after casting, the samples were covered with plastic
sheets and demolded after 1 d. The samples were then cured at 20 °C and RH of 95%
until the testing age. The molded specimens were prismatic specimens of
40  40  160 mm, and cylindrical specimens with a bottom diameter of 100 mm
and a height of 200 mm. In addition, the samples subjected to the X-CT test were
samples cut from a prism sample.
2.2. Experimental method
2.2.1. Three-dimensional X-ray microscope
X-ray three-dimensional microscope is a combination of traditional X-ray com-
puted tomography technology and optical microscopy. X-ray three-dimensional
microscope mainly relies on optical microscope to obtain high-resolution, different
magnification and field of view by changing the optical lens of different magnifica-
tion, without changing the working distance of the detector. Samples can be ran-
domly observed at various magnifications. Not only low-resolution observation of
the overall structure of the sample, but also to achieve high-resolution observation
of the sample local area.
Since the grayscale value obtained by the X-ray three-dimensional microscope
method is related to the X-ray absorption rate of the material since different mate-
rials have different grayscale values. Hence it can be used to characterize different
materials in cement-based materials considering the various grayscale value levels.
Namely, the unhydrated cement particles have a higher X-ray absorptivity than
cement hydration products, which means this type of products have greater bright-
ness. The cracks and pores do not have the ability to absorb X-rays, showing the
lowest gray value. According to the change of the gray value, cracks, pores, hydra-
tion products and unhydrated cement particles in the cement-based material can
be effectively distinguished. In this paper, Zeiss Xradia 510 Versa three-
dimensional X-ray microscopy was used to analyze the microstructure of
cement-based composites. Small cylindrical samples with a height of 5 mm and a
diameter of 3 mm were drilled from the casted specimens along their height
because this method requires smaller samples when the casted specimens were
cured for 28 days. In order to prevent collapse during the manufacture of cracks,
the sample was wrapped around. And samples were split in two halves using a dia-
metrical compression test (Brazilian test). For cracks on the same section, select the
mid position of the section and measure the crack width by measuring 20 locations
equally (interval distance 100 lm).

Table 1
Chemical composition of cementitious materials (Mass Proportions).

Raw materials Chemical composition (%)

SiO2 Al2O3 Fe2O3 CaO MgO SO3 Na2O K2O LOI
Cement 21.4 4.7 3.3 62.5 3.1 2.3 0.5 0.2 1.5
Silica fume 91.2 2.2 0.88 1.2 1.25 0.6 2.1
Fly ash 54.1 26.5 6.4 4.7 1.0 1.3 2.2 0.9 2.9
698 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709

Table 2
Sample number and mixture proportions.

No. Cement (%) Silica fume (%) Fly ash (%) Water (%) Superplasticizer (%)
Wc18 100 18 2
Wb18SF10 90 10 18 2
Wb18SF15 85 15 18 2
Wb18SF20 80 20 18 2
Wb18SF15Fa25 60 15 25 18 2
Wb18SF15Fa35 50 15 35 18 2

Admittedly, we could not monitor the crack width during the test. We artifi-
cially created the cracks by controlled compression tests. Once the cracks are cre-
ated, X-CT tests are followed to determine the crack width. In fact, we have
conducted nearly 20 samples with different crack widths and we choose the sample
presented in this work because the width seems to be the most appropriate.
Fig. 2 shows the cracked cement-based materials images after phase separation
by gray value. Green is the cracks and pores, blue is the unhydrated cement parti-
cles, and red is the hydration products.
2.2.2. Chloride ion diffusion coefficient in matrix
Three cylinder specimens of each mix proportion with 100 mm in diameter and
50 mm in height which were cut form 100 mm in diameter and 200 mm in height
were saturated for 48 h by using vacuum water saturation instrument, and then the
specimens were placed between two upstream and downstream cells. Two mesh
electrodes were placed on both sides of the sample, one of which was used as a
cathode which was filled with 3.0% NaCl solution, and the other was an anode
which was filled with 0.3 mol/L NaOH solution. The cells were forced to a 30 V
DC constant Voltage. During the test, the chloride ion concentration was deter-
mined from the solution in the anode cell by using titration method with 0.01 N
AgNO3 standard solution. It illustrated the chloride flux reached steady state when
the chloride ion concentrations versus time curves become linear. According to
Nernst-Planck equation [28], the chloride diffusion coefficient can be expressed
by Eq. (1) and Eq. (2):
RT
DCl ¼ J ð1Þ
CFE Cl
DCCl Vcomp
JCl ¼
A s  Dt
where, JCl is the constant flux of chloride in the anode cell (mol=m2 =s), T the absolute
temperature (K), C the chloride concentration in the cathode cell, E the electrical
field (V/m), R the universal gas constant (8.30 J/mol/K) and F the Faraday constant
(F = 96487 C/mol), Dt the interval time observed (s), As surface of the body of test
exposed to the chlorinated solution (m2), Vcomp the solution volume of anode cell
(m3), DCCl the change of chloride ion concentration in anode cell and As the actual
diffuse area of chloride ion transported in specimens (m2).
According to the above test method, the chloride ion diffusion coefficient of dif-
ferent mix proportion samples is shown in Table 3.
3. Numerical methods
3.1. Hydration microstructure of cementitious materials
CEMHYD3D model is a computer program developed by NIST
[27,29] in the early 1990s to simulate the cement hydration pro-
cess and paste microstructure via cycles of dissolution, diffusion,
and reaction. It was used to simulate the healing of crack. The par-
ticle size distribution and substance content were obtained by a
combination of laser diffraction and X-ray analysis of the cement
and mineral admixtures, respectively.
3.2. Self-healing of cracked microstructure
As mentioned above, the CEMHYD3D model can effectively sim-
ulate the reaction process and the internal microstructure of
cement-based system such as pure cement system, cement-silica
fume-fly ash system. Besides, it can be used to simulate the self-
healing of cracked cement-based composites in order to get the
reaction process of internal materials, the self-healing degree of
cracks and the microstructure of the cracked cement-based
composites.
When it comes to the particle size distribution, the inputs are
strictly controlled, consistent with the experimental details. Gen-
ð2Þ
erally, the PSD is totally the same as the results shown in Fig. 1.
First, we determine the PSD of the specific particles, cement, fly
ash and silica fume. Then, we randomly distribute the particles into
a box, according to the PSD curves. Finally, the hydration regime is
initiate through CEMHYD3D.
After simulation the hydration and microstructure of cement-
based composites for 28 days, a crack was prefabricated inside it
and assumed that the straight crack was in the middle of the
microstructure. It is known that the model was a cube of

Fig. 2. Segregation of cracked cement-based materials. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this
article.)
 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709 699

Table 3
Diffusion coefficient of chloride ion with different mixture (Mass proportion).

Wc18 Wc18sf15 Wc18sf15fa25 Wc18sf15fa35

2
Diffusion Coefficient (m /s) 2.22e12 4.85e14 6.57e14 6.02e14

100  100  100 lm. When the crack width is 10 lm, all voxels in
the model in the z-direction 45–55 are represented as water-filled
pores. When the crack width is 30 lm, all voxels in the z = 35–65
range are represented as pores filled with water. And so on, cracks
of different widths can be prefabricated in the CEMHYD3D model.
It is undeniable that the production of cracks in the cement matrix
will have a certain impact on the content of the original substances
in the microstructure. However, since the delivery of particles in
the initial microstructure is a random process, the content of each
substance in an area is basically the same as the content of each
substance in the whole area. Taking the structure of wb18sf10 as
an example, the distribution of different substances with different
crack widths is shown in Table 4. Since the amount of material dis-
tribution does not differ much before and after the production of
the crack, the change in the content of the material due to the pro-
duction of the crack is ignored in this paper.
Since the water transport rate is much faster than the rehydra-
tion rate of the cementitious matrix, both the cracks and their sur-
rounding cement-based composites are fully saturated with Fig. 3. The simulated crack microstructure after self-healing behavior.
sufficient water to provide the material reaction conditions
required. The crack model was then continued to hydration, the
cracked microstructural changes of cement-based composites with fusion coefficient of chloride ions in cement matrix and in water.
different rehydration can be obtained. The simulated microstruc- When the crack width is small, the diffusion coefficient of chloride
ture of wb18sf15fa25 with crack width of 10 lm rehydration for ion in the crack with different crack width will be different due to
200 h is shown in Fig. 3. the edge blocking effect and the self-healing of the crack. The crack
The degree of self-healing of the cracked cement-based material wall will hinder most of the chloride ion transport, and the self-
can be acquired and the content and distribution of each phases healing crack will also fill a part of the crack to reduce the internal
inside the crack can be determined. C-S-H gel and other substances chloride diffusion coefficient. When the crack is large, the two
will be generated around the original C-S-H gel and unhydrated effects have little effect on the chloride diffusion coefficient in
cement particles and the healing products will first be produced the crack. At this time, the diffusion coefficient of chloride in the
on the crack surface, then gradually extend to in the middle of crack is equal to the diffusion coefficient of chloride in water.
crack. It could be found that the degree healing around crack was
significantly higher than that in the middle of the crack. Notably, 3.3.1. Random walking method
the healing degree of the crack is characterized by the evolution In order to study the diffusion coefficient of chloride ion in the
of the internal porosity of the crack in this study. crack and analyze the effect of the crack wall effect and the degree
The healing degree of crack (H) can be expressed as Eq. (3): of self-healing on the chloride diffusion coefficient, the microstruc-
ture of the crack under different healing time was obtained by
V crack CEMHYD3D model. Assuming diffusion is a statistical result of ions
H¼1 ð3Þ
V0crack random movement, random walking method is used for the
numerical modeling of ions diffusion process [31,32]. Put an ‘‘ant”
V0crack is the volume of the initial crack. V crack is the volume of the into any position of the three-dimensional structure which was
crack after a period of self-healing. When the initial crack width is obtained by the hydration of the CEMHYD3D model. And then it
10 lm, V0crack is 100,000 voxels in volume. When the crack width begins to walk. The ant has the same probability of walking one
is 20 lm, V0crack becomes 200,000 voxels. step in each direction (X, Y, Z direction). Each step is independent
of the previous step and the size of step is constant length. In this
3.3. Chloride diffusion coefficient in crack paper, the random walking model was used in cement-based
materials. The ants will walk in the water-filled capillary pores
The chloride diffusion coefficient of ions in the crack is closely and C-S-H gels of cement paste. The step size of each ant equals
related to the crack width [28–30], and its size is between the dif- to the size of voxels of the microstructure.

Table 4
The distribution of different substances with different crack widths.

Cement SF CH CSH C3AH6 ASG CAS2

Wb18sf10 0 0.2510 0.0224 0.0250 0.5300 0.0299
10 0.2513 0.0222 0.0251 0.5177 0.0299
30 0.2524 0.0218 0.0255 0.5203 0.0298
Wb18sf15fa35 0 0.1718 0.2034 0.0014 0.2914 0.0410 0.0869 0.0581
10 0.1693 0.2061 0.0014 0.2916 0.0415 0.0819 0.0556
30 0.1725 0.2107 0.0013 0.2874 0.0412 0.0786 0.0546
700 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709

3.3.2. Random walking model used in healing cracks
The ants are assumed as virtual ionic species. When chloride
ions are transmitted in a certain degree of healing cracks, the ants
were only allowed to step into the pore and C-S-H gel. When ’ant’
encounter pores, the transfer time is 1/Dpore (diffusion coefficient
in pore); when ‘ant’ encounters CSH gel, the transmission time
through CSH gel is 1/DC-S-H (diffusion coefficient in C-S-H gel);
a low-density C-S-H gel [34], the diffusion coefficient is chosen
to be 7  10–11 m2/s. Fig. 4 is a ’ant’ in the two-dimensional struc-
ture of the walking process, in which the shadow of the cracks in
the newly formed product, the blue for C-S-H gel, the red for the
other products. As can be seen from the figure, within a limited
range of activities, ‘ant’ walk 26 steps, the chloride ion diffusion
p ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
coefficient in the crack is 152 þ 32 /(19/Dpore + 7/DCSH), which
2

chloride does not transfer within some solid phase (Such as CH is about 1.63  10–10 m2/s.
crystals which do not contain the pores that the chloride ions
can pass through), it will return to its original position. The time 3.4. Finite difference method
which takes for this step is related to the material composition of
the previous step. If the materials of last step is C-S-H gel or pore, For saturated cement-based composites, the main mode of
the walking time is 1/DC-S-H or 1/Dpore, respectively. transport of chloride ions is diffusion. The diffusion process satis-
‘Ant’ walking process shown in Fig. 4. Each successful step of fies the law of conservation of mass. Therefore, the chloride ion
the ant will make its walking distance plus 1. The time taken to transport equation can be expressed as Eq. (6):
transport 100,000 steps is used to represent the transmission Z Z
behavior in the cement paste. The longer the time used, the more dC
dV þ n  JdS  Q Cl ¼ 0 ð6Þ
difficult the transmission and the smaller the diffusion coefficient. V ct S
At the same time to prevent the initial position caused by the dif- where, V is the volume, S the surface area, n the outward direction
fusion coefficient error, selecting the 1000 ‘‘ants” to calculate the perpendicular to S, J the concentration flow of the diffusion phase,
chloride diffusion coefficient. Therefore, the chloride ion diffusion and is the concentration flux. In this study, the binding effect of
coefficient in the crack can be expressed as: cement-based materials on chloride ions was ignored and the Q Cl
Pn di was zero. J can be expressed as Eq. (7):
1 t
Dcr ¼ ð4Þ @/
n J ¼ DCl  ð7Þ
@X
Xk
t¼ 1=Di ð5Þ Among them, DCl is the chloride diffusion coefficient, / is the chlo-
1
ride ions flux and X is the distance from surface.
where di is the displacement of ant walk 10,000 steps, n is the num- Therefore, the formula for the transport of chloride ions in sat-
ber of ants, Di is the diffusion coefficient of the substance at the urated cement-based materials is:
position i, t is the time taken for the ant to walk k steps. @C
The diffusion coefficient of chloride ion in pores is 2  10–9 m2/s ¼ r  ðDCl  rCÞ ð8Þ
@t
[32,33]. The diffusion coefficient of chloride ion in low density
C-S-H gel and high density C-S-H gel is 7  10–11 m2/s and
40 Experimental results 7d 40
8.3  10–13 m2/s, respectively [33]. Since the C-S-H in the crack is
Experimental results 14d
35 35

Self-healing degree (%)

Experimental results 28d
Self-healing degree (%)

Numerical results 7d
30 30
Numerical results 14d
25 Numerical results 28d 25
20 20
15 15
10 10
5 5

10 20 30 40 50 60
Crack width ( m)
Fig. 4. The ‘ant’ walking diagram of the diffusion coefficient of crack.
Fig. 6. Self-healing degree of crack with different time.

A B C

100

Fig. 5. Three-dimensional X-ray microscope images of wc18 samples during different self-healing periods, a) 0d, b) 7d, c) 28d.
 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709 701

 
The general equations for chloride ion transport are solved by Diþ1;j C niþ1;j  Diþ1;j þ Di1;j C ni;j þ Di1;j C n
C nþ1
i;j  C ni;j i1;j
C nþ1
2 2
¼
2 2
means of the finite difference method. And an iterative way of clas- i;j
Dt Dx2
sical explicit format was adopted. The cracked cementitious mate-  
rial is treated as a two components system which includes crack Di;jþ1 C i;jþ1  Di;jþ1 þ Di;j1 C ni;j þ Di;j1 C n
n
2 2 2 2 i;j1
and mortar which have different diffusion coefficient. So the rela- þ ð9Þ
Dy 2
tionship between the concentration field from time t to time Dt
in the system can be established from the classical explicit format.

1.0 1.0
CSH CSH
Total solids POZZCSH
0.8 0.8 Total CSH
Total solids

Volume fraction
Crack width= 32 m
Volume fraction

0.6 0.6 Crack width= 32 m

0.4 0.4

0.2 0.2

0.0 0.0
0 10 20 30 40 0 10 20 30 40
Position ( m) Position ( m)
(a) (b)
1.0
CSH 1.0
CSH
POZZCSH
0.8 POZZCSH
Total CSH 0.8 Total CSH
Total solids
Volume fraction

Total solids
Volume fraction

Crack width= 32 m Crack width= 32 m

0.6
0.6

0.4 0.4

0.2 0.2

0.0 0.0
0 10 20 30 40 0 10 20 30 40
Position ( m) Position ( m)
(c) (d)
Fig. 7. The distribution of healing products within the crack width of 32 lm (a) wc18 (b) wb18sf15 (c) wb18sf15fa25 (d) wb18sf15fa35.

0.8 0.4
wc18 wc18
wb18sf15 wb18sf15fa25
wb18sf15fa35 wb18sf15fa35
0.6 0.3
wb18sf15fa25
Volume fraction
Volume fraction

Crack width= 32 m

0.4 Crack width= 32 m 0.2

0.2 0.1

0.0 0.0
0 10 20 30 40 0 10 20 30 40
Position ( m) Position ( m)
(a) (b)
Fig. 8. The distribution of (a) C-S-H (b) CH for different mixtures within the crack width of 32 lm.
702 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709

2Diþ1;j Di;j 2Di;j1 Di;j

Diþ1;j ¼ Di;j1 ¼ ð10Þ
2 Diþ1;j þ Di;j 2 Di;j1 þ Di;j

2Di1;j Di;j ehere C ni;j is chloride ion concentration at (i,j) node at time n.
Di1;j ¼ This article focuses on the transmission of chloride ions in two-
2 Di1;j þ Di;j
dimensional structures. Its boundary conditions and initial condi-
2Di;jþ1 Di;j tions can be expressed as Eq. (11)
Di;jþ1 ¼
2 Di;jþ1 þ Di;j C ni;0 ¼ 0:5

C ni;y ¼ 0
30
C 0i;j ¼ 0 ð11Þ
25
Self-healing degree (%)

20 4. Results and discussion

wc18
wb18sf15
4.1. Crack self-healing degree of UHPC
15 wb18sf20
wb18sf15fa25 Fig. 5 shows the two-dimensional X-ray microscope slices of
wb18sf15fa35 wc18 with cracks after 28 days of rehydration. The crack is obvious
10
observed at 0 d and there is a clear dividing line between the crack
and the matrix. The grayscale of the crack and pores is obviously
5
lower than that of the matrix. When the cracked sample is cured
in water for 7 d, the boundary between the matrix and the crack
0 is not obvious, and the grayscale of the crack is brighter. This
0 500 1000 1500 2000 2500 3000 3500 shows that the unhydrated cement particles and water occur
Time (h) hydration reaction, resulting in new hydration products clogging
cracks. When the cracked sample is cured in water for 28 d, the
Fig. 9. Healing degree of 50 lm crack.
phenomenon of clogging cracks become more obvious, and the

100 100
90 10μm 90 10μm
30μm 30μm
Self-healing degree (%)
Self-healing degree (%)

80 80
50μm 50μm
70 70
60 60
50 50
40 40
30 30
20 20
10 10
0 0
0 500 1000 1500 2000 2500 3000 3500 4000 0 500 1000 1500 2000 2500 3000 3500 4000
Time (h) Time (h)
(a) (b)

100 100
10μm
90 90 10μm
30μm
Self-healing degree (%)

30μm
Self-healing degree (%)

80 50μm 80
50μm
70 70
60 60
50 50
40 40
30 30
20 20
10 10
0 0
0 500 1000 1500 2000 2500 3000 3500 4000 0 500 1000 1500 2000 2500 3000 3500 4000
Time (h) Time (h)
(c) (d)
Fig. 10. The healing degree evolution with different widths of cracks. a) wc18 b) wb18sf15 c) wb18sf15fa25 d) wb18sf15fa35.
 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709 703

Table 5
Fitting parameters for the relationship between crack width and crack healing degree.

NO. Width a1 t1 y0 R
Wc18 10 lm 0.64 845.30 0.77 0.986
30 lm 0.34 737.91 0.40 0.992
50 lm 0.23 610.91 0.25 0.986
Wb18sf15 10 lm 0.63 600.08 0.76 0.984
30 lm 0.36 650.88 0.41 0.990
50 lm 0.22 544.36 0.24 0.991
Wb18sf15fa25 10 lm 0.56 575.21 0.66 0.986
30 lm 0.32 835.87 0.36 0.990
50 lm 0.23 1133.17 0.26 0.991
Wb18sf15fa35 10 lm 0.56 731.73 0.65 0.990
30 lm 0.40 1199.05 0.44 0.995
50 lm 0.25 1334.43 0.27 0.994
Wb18sf20 50 lm 0.22 517.45 0.24 0.991

gap between the crack and the matrix is less obvious. In addition, 55.4 lm respectively is selected to compare the change of crack
water enters the surrounding pores through cracks and hydrates width at different rehydration time determined as the average
with unhydrated particles, resulting in a decrease or even disap- width of the crack in a two-dimensional slice. The degree of self-
pearance of the pores. healing of cracks obtained by X-ray microscope method and CEM-
The change of gray value is used to distinguish the cracks from HYD3D model is shown in Fig. 6. It is found that the crack width
the cement matrix in this subsection. The same grayscale threshold obtained by CEMHYD3D results has similar trends as the experi-
was applied in different rehydration times. In this paper, the gray mental results. The CEMHYD3D model is effective and accurate
values of X-ray microscope images were used to distinguish in simulating the self-healing behavior of cracked cement matrix
between cracks and cement matrix. Notably, the grey value thresh- However, the experimental values are generally lower than the
old is 95/256, in 8-bit images. When the gray value of the X-ray numerical values. The reason is due to the fact that the minimum
microscope image is greater than 95, the position is a cement resolution of the model is only 1 lm and the simulated cracks are
matrix; when the gray value is less than 95, the position is a crack smaller than the real ones, resulting in a lower predicted self-
or a capillary pore. The crack width of 15.4 lm, 32.1 lm and healing degree.
Chloride diffusion coefficient(10-12m2/s)
hloride diffusion coefficient(10-12m2/s)

700 700

10μm 10μm
600 600
30μm
30μm
500 50μm 500
50μm
400 400

300 300

200 200

100 100

0 0
0 500 1000 1500 2000 2500 3000 3500 4000 0 500 1000 1500 2000 2500 3000 3500 4000

Healing time (h) Healing time (h)

(a) (b)
Chloride diffusion coefficient(10-12m2/s)
Chloride diffusion coefficient(10-12m2/s)

700 700

600
10μm 10μm
600
30μm 30μm
500 500
50μm 50μm
400 400

300 300

200 200

100 100

0 0
0 500 1000 1500 2000 2500 3000 3500 4000 0 500 1000 1500 2000 2500 3000 3500 4000
Healing time (h) Healing time (h)
(c) (d)
Fig. 11. Chloride diffusion coefficient of crack. a) wc18, b) wb18sf15, c) wb18sf15fa25, d) wb18sf15fa35.
704 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709

by CEMHYD3D model, Self-healing on the moisture transfer and

Chloride diffusion coefficient(10-12m2/s)

700
wc18 chloride ion transport is of great significance.
600 The cracks morphology and the number and distribution of heal-
wb18sf15fa35
ing products can be observed and characterized in our model. The
500 wb18sf15fa25 distribution of healing products within the crack width of 32 lm
wb18sf15 is shown in Fig. 7. The distribution of various substances in the
400
crack was consistent with the results in Hilloulin’s research [33].
wb18sf20 Fig. 8(a) shows the distribution of C-S-H gels in different mix-
300
tures. The content of C-S-H gel in the cracks of UHPC with wb18s-
200 f15, wb18sf15fa25 and wb18sf15fa25 is higher than that of wc18.
Since the cement-based material with mineral admixtures occurs a
100
pozzolanic reaction, a large amount of C-S-H gel generate with
0
development of hydration. The C-S-H gel content is getting higher
0 500 1000 1500 2000 2500 3000 3500 4000 and higher in the cracks. Fig. 8(b) shows the distribution of CH in
Healing time(h) different mixtures. Due to the large amount of CH consumed with
the pozzolanic reaction, the content of CH in the cement matrix is
Fig. 12. Chloride diffusion coefficient of 50 lm crack with different mix proportion. higher than that of the UHPC with mineral admixture. The total
content of CH in the mixture with wc18 in the crack is also signif-
icantly higher than that of the cement-based materials with min-
Compared with the self-healing of cracks obtained by experi- eral admixtures. In addition, a large amount of unhydrated
mental method, the degree of reaction of each substance within cement particles of the crack surface can hydrate with sufficient
the fracture and the position of each substance can be obtained water, so that the content of CH at the crack surface is increased,

10 m 30 m 50 m

(a)

10 m 30 m 50 m

(b)

10 m 30 m 50 m

(c)
Fig. 13. Chloride ion concentration distribution in saturated UHPC after 5 months (a) wb18sf15 (b) wb18sf15fa25 (c) wb18sf15fa35.
 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709 705

which is obviously higher than that in the matrix. It is noted that than that of the silica fume-fly ash-cement ternary system when
there is almost no restriction on the formation position of CH. the crack started to heal. With the increase of healing time, the
Therefore, there is also a large amount of CH in the middle of the healing rates of the three system fractures all decreased. The heal-
crack, which is different from the phenomenon that C-S-H gel ing rate of silica fume -fly ash -cement ternary composite cement-
accumulates only on the crack surface. based system gradually caught up with the healing rates of the
The degree of self-healing of the crack is closely related to the other two systems. With the increase of healing time, the cracks
width of the crack, the mixtures of the cement-based material healing rates of three types of UHPC decrease, but the healing rate
and the healing time. For the convenience of calculation, this paper of the silica fume - fly ash - cement ternary system gradually catch
mainly simulated and analyzed the self-healing and chloride ion up with the healing rate of the other two systems. This is mainly
transmission of cracks with crack widths of 10, 30, and 50 lm.
Fig. 9 shows the time-dependent changes of the self-healing degree
with different proportions when the crack width is 50 lm. From
0.5 not considering healing
Fig. 9, with the increase of healing time, the unhydrated cement

Chloride ion concentration wt.(%)

particles, fly ash and silica fume on the crack surface gradually 50μm
react with each other and fill in the cracks, resulting in the crack 0.4 30μm
width gradually decreases and the crack healing degree increases. 10μm
In the early stage of reaction, the healing rate of the crack is larger, 0.3
and the later stage will gradually slow down with the increase of
the healing time, and the healing degree of the crack will no longer
be produced. It can be seen from the figure that the healing degree 0.2
of UHPC cracks with the same water-cement ratio is basically the
same after healing 3000 h. For different mixtures for healing 0.1
3000 h, about 25% of the crack space is filled by the reaction prod-
ucts. The pure cement system had a lower degree of total reaction 0.0
degree than the binary and ternary cement-based systems at
28 days, and had relatively higher unreacted particles around the
-2 -1 0 1 2 3
crack. Therefore, the crack healing of the pure cement system
Distance of perpendicular to the crack (mm)
was slightly higher than that of other cement-based materials with
mineral admixtures. However, the crack healing rates of pure Fig. 15. The chloride ion concentration distribution at 5 mm from the contact
cement system and silica fume-cement binary system was faster surface of saturated wb18sf15fa25 matrix and chloride salt solution after 5 months.

0.5 0.5
Chloride ion concentration wt.(%)
Chloride ion concentration wt.(%)

no crack no crack
10 m 10 m
0.4 0.4 30 m
30 m
50 m 50 m
0.3 0.3

0.2 0.2

0.1 0.1

0.0 0.0
0 5 10 15 20 25 0 5 10 15
Depth (mm) Depth (mm)
(a) (b)
0.5 0.5
Chloride ion concentration wt.(%)

Chloride ion concentration wt.(%)

no crack no crack
10 m 10 mm
0.4 30 m 0.4 30 mm
50 m 10 m
50
0.3 0.3

0.2 0.2

0.1 0.1

0.0 0.0
0 5 10 15 0 5 10 15
Depth (mm) Depth (mm)
(c) (d)
Fig. 14. The chloride ion concentration distribution through with crack of saturated UHPC after 5 months (a) wc18 (b) wb18sf15 (c) wb18sf15fa25 (d) wb18sf15fa35.
706 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709
due to the lower activity of fly ash compared to silica fume, the
lower reaction of fly ash in the early hydration, resulting in a lower
degree of healing of cracks in the early rehydration reaction. How-
ever, with the progress of the reaction, the degree of fly ash reac-
tion increased and the reaction product fills the cracks, so that
the total healing degree of the cracks is similar to that of the other
several mixtures.
Fig. 10 shows the healing degree evolution curve of cement-
based material with different widths of cracks. According to
Fig. 10, for different mixtures of UHPC, as the crack width
increases, the degree of self-healing decreases. According to the
numerical results, the amount of total healing products produced
by the cracked UHPC with different crack widths at the same heal-
ing time is basically the same. However, the wider cracks indicate
0.5
Chloride ion concentration wt.(%)
wb18sf15
wb18sf15fa35
0.4
wb18sf15fa25
0.3
0.2
0.1
0.0
0 5 10
Depth (mm)
Fig. 16. Concentration distribution of chloride along the crack (10 lm) direction
after 5 months in different mixture proportions of saturated UHPC.
Fig. 17. Concentration distribution of chloride ion in UHPC of wb18sf15fa25 with crack length of 2 mm, 5 mm, 10 mm (a) crack width of 10 lm (b) crack width of 50 lm.
that the larger the volume of cracking, leading to smaller degree of
healing.
As crack healing degree increases, most newly formed hydra-
tion products continuously fill the crack surface, causing the width
of crack reduce. In order to quantify the variation of crack width,
the crack width change is characterized by the crack healing evo-
lution. Therefore, the relationship between the crack width and
crack healing degree can be expressed as Eq. (12). The fitting
results of related parameters are shown in Table 5.
t
xðtÞ ¼ x0 ð1  ða1  et1 þ y0 Þ ð12Þ
x (t) represents the crack width (lm) at different self-healing time,
x0 is the initial crack width (lm), t represents self-healing time (h),
a1, t1 and y0 are other correlation coefficients, respectively.
4.2. Effect of crack self-healing on chloride ions transport
For cracked UHPC, there is a large amount of unhydrated parti-
cles around the cracks taking a certain amount of healing over
time. Crack width becomes smaller and tortuous degree becomes
larger and this will reduce the rate of chloride ion transport with
development of self-healing. Therefore, in order to study the trans-
port of chloride ions in cracked UHPC, the impact of self-healing of
cracks on water or chloride ion transport process need to be fully
considered.
As the cracks are easily filled with water, it is assumed that the
cracked concrete is saturated in this work and the main transport
of chloride ion is diffusion for saturated UHPC. According to the
obtained diffusion coefficient and the chloride ion transport equa-
tion of chloride ion in cement matrix and crack and the random
walking method, the chloride ion transport depth can be obtained
using the finite difference method. The chloride ion diffusion coef-
15
ficient in cracks is affected by the crack width, crack length, mix-
ture proportion of matrix, and transport time, which is fully
considered from the four variables to obtain the chloride transport
depth of cracked UHPC.
 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709
4.2.1. Effect of self – healing on chloride ion diffusion coefficient in
crack
The hydration microstructure of crack calculated by the digital
based method and the random walk method can determine the dif-
fusion coefficient of chloride ions in a crack with different healing
extent. Fig. 11 is chloride ion diffusion coefficient changes over time
with different crack width and different proportions. According to
the calculation results, the diffusion coefficient decreases rapidly
with the initial crack of 10 lm in width, and the diffusion coeffi-
cient of chloride ion in crack decreases to 10–12 m2/s, which has
the same order of magnitude as pure cement matrix. As the crack
width increases, the effect of self-healing on the rate of chloride
ion transport in the crack decreases. When the crack width is
50 lm, the diffusion coefficient of chloride ion in the crack is
reduced to the order of 1010 m2/s. Even for the pure cement
system, the chloride ion diffusion coefficient in the crack is signifi-
cantly higher than that in the cement matrix. For the cement-based
cementitious system with silica fume, the chloride ion diffusion
coefficient in the crack is 3 to 4 orders of magnitude larger than
the chloride ion diffusion coefficient in matrix. According to
Fig. 12, under the same water-cement ratio, the diffusion coefficient
0.5
Chloride ion concentration wt.(%)
0.4
0.3
0.2
0.1
0.0
0 5
Depth (mm)
Fig. 18. Chloride ions Concentration distribution in UHPC (transport time is 5 m, 1 y, 5 y, 10 y, 50 y) at a crack with 5 mm length and 10 lm width and chloride ion
concentration curve along the crack direction.
707
of chloride ion in the cement-based system with three phases of sil-
ica fume-fly ash-cement mixed decreased slowly at the early stage,
and gradually catched up with pure cement system and silica fume-
cement system. When self-healing for about 3000 h, the diffusion
coefficient of chloride ions in the cracks of the three-phase mixed
cement-based composite system is slightly lower than the binary
system and the pure cement system. This phenomenon is closely
related to the degree of self-healing of the crack.
4.2.2. The effect of crack width on chloride transport depth
Fig. 13 shows the concentration profile of chloride ion transport
in saturated UHPC with different crack widths. The crack lengths
are all 20 mm in these concentration profiles in cement-based
materials. In addition, the crack width is 10 mm and crack width
of 10 lm, 30 lm and 50 lm, respectively. For UHPC with different
water-cement ratios and the same mineral admixture, the depth of
chloride ion transport in the saturated cracked cement-based
materials increases with the increase of the crack width, and the
increase effect is obvious. Fig. 14 shows the concentration profile
of chloride ion along the crack direction. The chloride ion concen-
tration in the crack increases as the crack width increases. Fig. 15
5months
1year
5years
10years
50years
10 15
708 J. Jiang et al. / Construction and Building Materials 198 (2019) 696–709
shows a chloride ion concentration profile at 5 mm from the inter-
face of the chloride salt solution and the cement-based material.
Due to the self-healing effect, the chloride ion diffusion coefficient
in the crack decreases. The depth of chloride ion transport perpen-
dicular to the crack direction decrease compared to the case with-
out considering self-healing. This degree of change increases with
decreasing width of the crack. After reaching the end of the crack,
the chloride ion concentration drops rapidly because the chloride
ion transport rate in matrix is much lower than that in crack. As
a result, chloride ions penetrate only a small depth in matrix. In
addition, as the crack width increases, the transport depth of chlo-
ride ion along the crack direction also increases to a certain extent.
4.2.3. The effect of mixture proportion chloride transport depth
Fig. 15 shows the distribution profile of chloride ion with differ-
ent mixture proportion along the crack direction when the crack
width is 10 lm and the length is 10 mm. According to Fig. 16, it
can be seen that for the binary and ternary cement-based compos-
ite systems with silica fume added, change of mixture proportion
has little influence on the transport depth of chloride ion along
the crack direction. According to the change of chloride ion diffu-
sion coefficient with time for different mixture proportions, it
could be found that, when cracks have the same width, the differ-
ent mixture proportions have no obvious effect on the diffusion
coefficient of chloride ion, and have little influence on the transport
depth of chloride ion in cracked cement-based material either. In
addition, the chloride ion diffusion coefficients of binary and tern-
ary cement-based materials with different mixture proportions
have some differences. Due to chloride diffusion coefficient of
UHPC matrix is very small, the difference of chloride ion transport
depth in the UHPC is small.
4.2.4. The effect of crack length chloride transport depth
From the above study, it is found that the mixture proportion of
UHPC has no obvious effect on the chloride ion transport depth in
the cracked matrix with the same water-binder ratio. Therefore,
one of various proportions is used to study the influence of crack
length. Fig. 17 shows the concentration distribution of chloride
ion in UHPC matrix of wb18sf15fa25 for 5 months when the crack
length is 2 mm, 5 mm and 10 mm, respectively. Due to the better
impermeability of UHPC matrix, the chloride ion transport rate is
lower, and the transport rate of chloride ion in crack is obviously
higher than that in the matrix, even if the crack width is very small.
Therefore, the crack length will significantly affect transport depth
of the chloride ion. The greater the crack depth, the greater the
transport depth of chloride ion. Comparing the concentration dis-
tributions of cracks with different depths, the peak of the concen-
tration curve becomes sharper when the crack depth is larger.
When the crack depth is smaller, the concentration around the
crack is larger and the concentration difference is smaller.
4.2.5. The effect of transport time chloride transport depth
Fig. 18 shows the concentration distribution of chloride ion
with different transport time for UHPC of wb18sf15 with crack
length 5 mm and width 10 lm. With the increase of transport
time, the chloride ion transport depth in the matrix gradually
increases, and the influence of the crack on the transport depth will
gradually decrease. Due to the fast transport rate of chloride ion in
the crack, chloride ion also transport to the direction of vertical
crack except transport along the crack direction. As the transport
time increases, the chloride ion depth increases along the vertical
crack direction. Therefore, as the transport time increases, the peak
of concentration curve will become flat and the influence of the
cracks on the transport depth decreases.
5. Conclusions
Based on the previous experimental and numerical results, the
following conclusions can be drawn:
1) Three-dimensional X-ray microscope and digital-based com-
puter model CEMHYD3D can be used to investigate the self-
sealing degree evolution of cracked UHPC. The self-healing
degree of the crack is closely related to the width of the
crack, the types of UHPC and the healing time.
2) In the self-healing progress, portlandite crystallizes in the
middle of the crack, while C-S-H gel accumulates only on
the crack surface.
3) The influence of crack self-healing degree on chloride ion
transport process is considered in the proposed finite differ-
ence model. Mixture proportions have little influence on the
diffusion coefficient of chloride ion. However, there is an
effect on the concentration of chloride ions inside the crack.
The cracked binary composite cement-based material has
lower chloride ion concentration in the cracks compared
with ternary composite cement-based material.
4) As time increases, chloride ions not only transport vertically
along the crack, but also propagate in the horizontal direc-
tion of the crack.
5) With the increase of crack width, the diffusion coefficient of
chloride ions in cracks increases. The concentration of chlo-
ride ions in the crack increases, and the concentration of
chloride ions in the direction perpendicular to the crack
cross section increases.
Conflict of interest
None declared.
Acknowledgements
The authors greatly acknowledged the support from National
Natural Science Foundation of China (No. 51438003, No.
51508091 No. 51578143). This work was also supported by the
National Basic Research Program of China ‘‘973 Project” (No.
2015CB655105). We were grateful to the High Performance Center
(HPCC) of Nanjing University for doing the numerical calculations
in this paper on its IBM Blade cluster system.
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