Cement and Concrete Research 113 (2018) 86–98

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Cement and Concrete Research

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

Water penetration through cracks in self-healing cementitious materials T

with superabsorbent polymers studied by neutron radiography
⁎
D. Snoeck , P. Van den Heede, T. Van Mullem, N. De Belie
Magnel Laboratory for Concrete Research, Department of Structural Engineering, Faculty of Engineering and Architecture, Ghent University, Tech Lane Ghent Science Park,
Campus A, Technologiepark Zwijnaarde 904, B-9052 Gent, Belgium

A R T I C LE I N FO A B S T R A C T

Keywords: SuperAbsorbent Polymers (SAPs) are a promising admixture to obtain self-sealing and self-healing cementitious
Microcracking materials. They are able to physically block water penetration through cracks due to their swelling ability. This is
Absorption very useful in a cementitious material which is prone to cracking leading to a reduced durability. The effec-
Permeability tiveness of counteracting water penetration is of concern. Neutron radiography was performed in order to in-
Polymers
vestigate the influence of SAPs on the water permeability through healed cracks with respect to a reference
Fiber reinforcement
material without SAPs. The gravimetrically measured capillary absorption corresponded with the obtained re-
sults after image analysis and a quantitative analysis could be made. SAPs enhance the water impermeability and
are able to seal and heal a crack effectively up to 100 μm. The healing was a main factor to impede water
movement through cracks. This will lead to less water ingress in building infrastructures and a possible longer
service life.

1. Introduction cementitious material. In that way, less harmful substances will intrude
the material and the durability is less endangered. This self-sealing ef-
Cracking in concrete and especially the possible eventual gas or fect occurs instantaneously. It will depend on the swelling time of the
water ingress through these cracks is a major concern for buildings and SAP which is in the order of several seconds to tens of seconds. The
infrastructures. The water may contain harmful substances which can amount and size of the added SAPs needs to ensure proper sealing. An
start to deteriorate the cementitious material and may also lead to amount of 1 m% and an average size of 500 μm seems to be efficient
corrosion of the reinforcement. As effective manual crack repair may be [36, 37]. Furthermore, the absorbed water can be used to stimulate and
difficult due to inaccessibility, a self-healing material can be used. This promote autogenous healing. Autogenous healing, in the form of fur-
material is able to self-repair occurring cracks without the need for ther hydration of cement, pozzolanic activity of supplementary ce-
external repair and human intervention. Different approaches are pos- mentitious materials and calcium carbonate crystallization, can visually
sible, ranging from the use of encapsulated polymers [1–4], over cal- close cracks [22, 24]. Complete healing is possible up to 30–50 μm
cium carbonate precipitating bacteria [5–8] and microcapsules [9–11], crack widths in strain-hardening cementitious composites [18, 24]. This
crystalline admixtures [12–14] and vascular systems [15–17], to syn- healing leads thus to a physical pertinent closure of the cracks. In that
thetic microfibres [18–21] and SuperAbsorbent Polymers (SAPs) way, harmful gases may also no longer penetrate the structure and the
[22–24]. mechanical properties are regained [22, 24].
The SAPs are a new promising admixture for cementitious materials Depending on the efficiency of the (promoted) healing, the cracks
[25]. They are able to absorb up to thousand times their own weight in may show less or no water penetration over time. This can be studied by
liquid [26]. They can be used for internal curing [27–30], to increase means of capillary water absorption or water permeability tests, but the
the freeze-thaw resistance [31, 32], to change the rheology [33], as well water distribution can not to be studied in detail. It has not been studied
as to induce self-sealing [34–36] and self-healing [22–24] of cementi- whether the crack healing action provides full sealing or healing of the
tious materials. Their self-sealing and self-healing ability is interesting crack or whether there is still a part of the crack where water may
in terms of the permeability of a cementitious material. As the super- penetrate. Therefore, in this paper, the capillary water absorption re-
absorbent polymers swell, they will physically block a crack from in- sults are linked to neutron radiography analyses which can clearly vi-
truding fluids. This will lead to a regain in impermeability of the sualize water in a cementitious material as a function of time. In that

⁎
Corresponding author.
E-mail addresses: [email protected] (D. Snoeck), [email protected] (N. De Belie).

https://doi.org/10.1016/j.cemconres.2018.07.002
Received 8 November 2017; Received in revised form 4 May 2018; Accepted 12 July 2018
Available online 27 July 2018
0008-8846/ © 2018 Elsevier Ltd. All rights reserved.
D. Snoeck et al. Cement and Concrete Research 113 (2018) 86–98

way, the (im)permeability can be studied in great detail and conclu- research of Li et al. [18, 48] and Snoeck et al. [22, 24]. The fly ash-to-
sions can be drawn on the effectiveness of the sealing and healing of cement ratio was 1, the sand-to-binder ratio was 0.35, the super-
cracks in cementitious materials with and without SAPs. plasticizer-to-binder ratio amounted to 0.005 and the water-to-binder
Neutron radiography is a powerful technique to non-destructively ratio was 0.3 for both mixtures. An amount of 2 v% of PVA fibres was
study fluids containing hydrogen in a system. It has been applied on added to ensure strain-hardening. The SAP-to-cement ratio was 0.01
cementitious materials to study the water movement through cracks as (1 m% of cement weight). Additional water was added to the SAP
the technique can be used to visualize and quantitatively evaluate the mixture to ensure no loss in workability. This amount is the ideal
kinetics of water ingress into porous solids [38–40]. A study on con- amount which is absorbed and was verified using optical microscopy
crete strengthened by strain-hardening cementitious materials showed [49, 50] and X-ray computed microtomography [23]. The effective
that neutron radiography is able to prove the effectiveness of a repair water-to-binder ratio is the same for the REF and the SAP mixture.
product [41]. Also water repellents which hydrophobize cracks pre- The SAP was stored in dry and sealed conditions prior to testing or
venting water movement were studied [42, 43]. Furthermore, the water mixing in the cement paste mixture. First, the cement, fly ash and
release of the SAPs can be studied by neutron radiography measure- possibly SAPs (depending on the mixture composition) were equally
ments during hydration of the cementitious material [44]. The SAP distributed with a mortar mixer. Then, the total amount of water and
particle shrinks as it releases its stored mixing water and an empty superplasticizer were added and mixed for 30 s at 140 rpm. The fine
macro pore remains [45], possibly partly filled with hydration products silica sand was added during the next 30 s at 140 rpm. To ensure a
[46]. Autogenous healing by SAPs was not studied up till now with homogeneous dispersion of all components, the speed was increased for
neutron imaging. The water penetration through cracks autonomously the following 30 s to 285 rpm. The edges of the bowl were scraped
healed by encapsulated polyurethane-based agents, was studied and it during 30 s and the mixture was then allowed to rest for a period of
was found that the ingress of water into the crack can be prevented 60 s. Subsequently, while mixing at a speed of 140 rpm, microfibres
depending on the type of agent [40]. However, in presence of two or were slowly added during 30 s. The final step was mixing for 60 s at
more cracks, only one can be properly healed by this approach [47]. 285 rpm.
The current study continues on the previously mentioned research since Moulds (160 × 20 × 40 mm3) which had a rebar (sandpapered
neutron radiography results regarding the water permeability through messing surface with 2 mm diameter) at a height of one third of the
autogenously healed cementitious materials with and without SAPs are total height were filled and the samples were compacted by jolting 60
lacking in literature. times. The moulds were then covered using plastic foil and put at a
temperature of 20 ± 2 °C. The samples were demoulded after 48 h and
2. Materials and methods were stored wrapped in plastic foil at a temperature of 20 ± 2 °C until
the age of 28 days. Series used within this study consisted of minimum
In this section, the two different studied mixtures and samples are three 160 × 20 × 40 mm3 samples per healing condition and per test
described (Section 2.1). Next, the cracking method (four-point-bending) method in order to obtain statistical sound results.
and the microscopic analysis are discussed (Section 2.2). The capillary
absorption measurements are explained next (Section 2.3). In the end, 2.2. Cracking and healing conditions with microscopic analysis
the neutron radiography principle and apparatus together with the
performed image analysis to investigate the water movement through After being stored for 28 days, the specimens were cracked using a
the cracked material is explained (Section 2.4). four-point-bending test. The bottom side of the specimens is equal to
160 × 20 mm2. A servo hydraulic testing system (Walter+Bai DB 250/
2.1. Studied mixture compositions 15) ensured a displacement-controlled test (0.005 mm/s to imitate a
quasi-static load). The lower and upper supports were 140 mm and
Two mortar mixes (REF and SAP) were studied in detail and con- 50 mm apart from each other, respectively. The strain at the bottom
sisted out of cement (CEM I 52.5 N, Holcim, Belgium), fly ash (Class F, side of the specimen was limited to 2.5%, theoretically calculated from
OBBC, Belgium), fine silica sand (M34, D50 = 170 μm, Sibelco, the curvature and the vertical displacement during loading. This strain
Belgium), a polycarboxylate-type superplasticizer (Glenium 51 conc. is lower than, but close to, the maximum possible strain at ultimate
35%, BASF, Belgium), PVA microfibres (oil-coated, 15 dtex, 8 mm strength (3–4% [37]) of such a strain-hardening specimen, so the actual
cutting length, 12 cN/dtex, Kuraray, Japan), water and, depending on service cracks could be studied.
the mixture, superabsorbent polymers. The chemical composition of the After four-point-bending, the cracks were measured using an optical
cement and fly ash can be found in [22, 30]. microscope (Leica S8 APO mounted with a DFC 295 camera). Then, the
The SAP used is called SAP B, a cross-linked potassium salt poly- specimens were stored in three different conditions for 28 days to allow
acrylate (particle size 476.6 ± 52.9 μm (n = 100)). The nomenclature crack healing:
of the SAP is the same as in previous research of the authors [22–24,
36]. The SAP is bulk-polymerized and consists of irregular crushed 1) At 20 ± 2 °C with application of wet/dry cycles (alternatively
particles. It is able to absorb 283.2 ± 2.4 g/g SAP in demineralized stored in demineralized water for 1 h, and exposed to a relative
water and 58.4 ± 1.7 g/g SAP in cement filtrate solution. The swelling humidity (RH) of 60 ± 5% for 23 h);
time in a fluid to full absorption was 60 ± 5 s in standard laboratory 2) In a room with a RH = 95 ± 5% (> 90%);
conditions (a temperature of 20 ± 2 °C and a RH of 60 ± 5%). The 3) In a room with a RH = 60 ± 5%.
absorption capacity was determined using the filtration method and the
swelling time using the vortex method [26]. REF samples were exposed to the first two healing conditions and
The mortar composition can be found in Table 1 and is based on the SAP samples to all three healing conditions. Storing REF samples in a

Table 1
Mortar composition of the studied mixtures.
Sample code Cement [kg/m3] Fly ash [kg/m3] Sand [kg/m3] Water [kg/m3] Superplasticizer [kg/m3] PVA Fibres [kg/m3] SAP [kg/m3]

REF 611 611 428 367 6 26 0

SAP 575 575 402 396 6 26 5.75

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RH condition of 60% would result in approximately the same healing as suction in the cement-based material could be followed as a function of
at a RH of > 90%, i.e. almost none [23]. To use the measuring time as time. The relation between the intensity values and composition of the
efficiently as possible, these specimens were thus not studied as no sample is described by the law of exponential attenuation, also known
additional information would be obtained. as the Beer-Lambert law (Eq. 1). The wet and dry radiographs were
After 28 days healing, the cracks were once more studied micro- compared to each other and the water content could be calculated
scopically. The visual closure of the crack width served as a qualitative quantitatively (Eq. 2–6) by logarithmically dividing the wet and the dry
measure for the autogenous healing capacity. The percentage is calcu- state and multiplying this value by the density of water and dividing it
lated as the difference between the subsequent measurements and the by the attenuation coefficient of water and the thickness of the sample.
initial crack width immediately after cracking and unloading of the
I = I0 ∙e−Σ ∙ d (1)
specimens.
Additionally, the compressive strength was measured (NBN EN 196- Idry = I0 ∙e−Σdry ∙ d (2)
1) on 160 × 40 × 40 mm3 mortar beams with a testing machine Walter
+Bai DB 250/15. The mechanical properties were studied at 28 days Iw = I0 ∙e−Σdry ∙ d − Σw ∙ dw (3)
after casting. The samples were stored at a relative humidity of > 95%
and a temperature of 20 ± 2 °C until the age of testing. ρw ∙Vw ρ ∙d w
W= = w
V d (4)
2.3. Capillary water absorption tests
−Σw ∙ W ∙ d
Iwet = Idry ∙e ρw
(5)
3
Three 160 × 20 × 40 mm specimens per test series and healing
condition were subjected to capillary water absorption tests in analogy ρw I
with the standard EN 13057. At the age of 56 days, all samples were W=− ∙ln ⎛⎜ w ⎞⎟
Σ w ∙d I
⎝ dry ⎠ (6)
first dried in an oven at 50 ± 1 °C for 7 days to exclude all moisture,
−2 −1 −1
prior to testing. All surfaces, except the bottom and top faces of the where I is the flux through a sample [cm ·s ·μA ], I0 the flux pe-
specimens, were covered with self-adhesive aluminium foil to induce netrating into the sample [cm−2·s−1·μA−1], Σ the attenuation coeffi-
unidirectional water flow during the test. The lower surface contained cient [cm−1], d the thickness of the sample [cm], Idry the flux trans-
the multiple (un)healed crack mouths through which the water may mitting through dry material [cm−2·s−1·μA−1], Iw the flux through wet
penetrate. The samples were put on supports and immersed for 3 mm in material [cm−2·s−1·μA−1], Σdry the attenuation coefficient of dry ma-
water. The method uses the increase in weight (0.01 g accuracy) due to terial [cm−1], Σw the attenuation of water [3.64 cm−1], dw the thick-
capillary absorption of water over a period of time. The results are ness of the observed water layer [cm], W the water content [kg·m−3],
expressed as the water uptake per unit area. Thus, the mass was divided ρw the density of water [kg·m−3], Vw the volume of water [m3] and V
by the length and width of the bottom contact surface to obtain the total the volume of the sample [m3].
water uptake per square meter. The gradient, as determined by EN Before the start of the capillary absorption tests, the specimens were
13057 is defined as the sorption coefficient S [kg·m−2·h–0.5]. The weighed with a Sartorius BP 3100 S balance (0.01 g accuracy). After the
weight of absorbed water is in such a way expressed as a coefficient 2 hour test, the wet mass was determined using the same mass scale.
indicating the tendency of the specimen to allow water penetration by The total amount of absorbed moisture was quantified and compared to
capillary action. The samples were weighed before and after 5 min, the value obtained by post-processing the neutron radiographs.
15 min, 30 min, 1 h, 2 h, 4 h, 8 h and 24 h of water contact. First, each radiograph obtained with neutron radiography needed to
be filtered with the image correction tool “Quantitative Neutron
2.4. Neutron radiography Imaging” (QNI) [52] for qualitative and quantitative information.
Several deviations on the attenuation were taken into account. The
Cracked specimens used for the neutron radiography measurements, images were corrected using the dark current, the open beam (flat field)
consisted of another three 160 × 20 × 40 mm3 samples per test series and the black body radiographs. These separate radiographs were made
(sample composition and healing condition). The samples were condi- before every new test series. The dark current is a radiograph where all
tioned after healing in the same way as mentioned in Section 2.3. The shutters of the beam were closed. The open beam shows a radiograph
samples were transported to the neutron measuring station in sealed with the spatial distribution and inhomogeneity of the neutron beam
conditions (plastic foil) during 24 h. intensity as a measure for the background noise. The black body
The beam used for measuring the water penetration was the neutron radiograph was made when boronated polyethylene blocks were placed
beam line at the measuring station NEUTRA, the thermal neutron in front of the samples. These blocks are able to absorb the neutrons and
radiographic facility at the Swiss spallation source SINQ of the Paul gave an estimate of the background scattering correction. All correc-
Scherrer Institute (PSI) [51]. The proton current was approximately tions were based on an average of five radiographs per correction
970–980 μA with a peak energy of 25 meV throughout all tests. The factor, to further optimize the obtained results.
neutron beam travelled through the studied object and hit the 100 μm All further image operations were performed using the image pro-
LiF/ZnS scintillator screen as neutron-to-light converter. Then it hit a cessing software ImageJ. After post-processing of the radiographs, the
mirror in the dark room and was recorded by a CCD camera, a cooled measured wet states images were divided by the dry state images as a
slow-scan Andor SCMOS camera with a 50 mm AF-S NIKKOR lens. The qualitative measurement of the moisture distribution and content. The
recording resulted in a radiograph consisting out of an array of grey dry states were calculated by averaging five subsequent dry images. The
level intensity values. The pixel size obtained with an exposure time of total water content in the not-immersed part of the sample was calcu-
20 s was 138.89 μm/pixel. lated. The part which was immersed was assumed to have a water
Per test run, a maximum of ten samples were placed on line supports content equal to the immediately adjacent part just above the water
into five water basins mounted on a support frame (Fig. 1). First, dry level obtained after 2 h of capillary water absorption through the ce-
reference images were taken before the containers were filled with mentitious matrix. This amount was added to the already obtained
water. Subsequently, water was added manually 3 min before the actual value of the total water content of the not-immersed part of the sample.
start of neutron radiography. The samples were approximately 4 mm As water was present in front of and behind the specimen, using the
immersed in the liquid. Post-processing revealed an immersion of initial darker value for the immersed part would result in higher and
4.12 ± 1.00 mm. Subsequent radiographs were made for a total mea- false quantitative measurements.
suring time of 2 h. In this way, the water penetration due to capillary Furthermore, two distinct water content profiles along the

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D. Snoeck et al. Cement and Concrete Research 113 (2018) 86–98

Field of view

Shelf
Frame

Basin

Sample

Water

40 mm

Fig. 1. Experimental setup showing the 20 × 40 × 160 mm3 cracked samples immersed in approximately 4 mm of water for capillary absorption during neutron
radiography. Ten samples were placed on 5 shelfs mounted on a frame. The dashed lines show the field of view during neutron radiography measurements.

horizontal axis were calculated using a rectangle grey-level profile plot: limited to 50 μm to 60 μm due to the proper mixture design. If the
material would be loaded further the weakest crack would open,
1) Adjacent to the water level but not immersed; leading to a complete failure of the composite. This is called strain-
2) At approximately two thirds of the total height of the specimen. softening. The fibres are no longer able to cope with the additional
forces and are completely pulled out or experience failure.
In this way the water movement in time could be studied and vi- In the curves in Fig. 2, the stresses increase and several drops
sualized in detail. The profiles were made at 5 min, 10 min, 15 min, (multiple crack formations) are seen. The first-cracking-strength
45 min and 2 h in measuring time. amounts to 6.3 ± 0.6 MPa for REF samples and 5.9 ± 0.4 MPa for
SAP samples. These are typical values for such kind of strain-hardening
3. Results and discussion materials [19] and the difference between SAP and REF samples is not
statistically significant. All samples were pre-loaded till 2.5% strain and
In this section, the observed characteristics of the REF and SAP upon unloading, this value decreased to approximately 1.8%. The ul-
samples are discussed (Section 3.1). These include the stress-strain timate strain is 3–4% [37], so the serviceability limit state crack widths
diagrams and the observed visual closure of the multiple cracks by are studied. The SAP samples would even show a more pronounced
means of microscopic analysis. Next, the capillary absorption as cal- strain-hardening effect, compared to the REF specimens, as the SAP
culated by means of image analysis on the neutron radiographs are particles act as stress initiators [53], helping in the formation of mul-
compared to the results obtained with gravimetric capillary water ab- tiple cracks. These specimens show a higher possible strain compared to
sorption tests (Section 3.2). In the end, the different obtained water REF samples. The observed crack widths are comparable between the
profiles are discussed in detail. The water penetration through cracks REF and the SAP samples.
towards the cementitious matrix is discussed (Section 3.3). When studying the compressive strength of the materials, REF
samples show a compressive strength of 77.4 ± 1.2 MPa and SAP
specimens (with 1 m% of cement weight SAP) 67.0 ± 1.4 MPa. This
3.1. Material characteristics: Mechanical properties and visual closure means a reduction of 15.6% in compressive strength. However, this
strength suffices for most applications. The strength reduction is due to
The typical obtained stress/strain curves are shown in Fig. 2. In a dual effect. First of all, there is a positive effect of internal curing [29],
these curves, upon loading, the stress increases till the point of first but this is combined with a negative effect of macro pore formation [49,
cracking. This can be seen as a small drop in stress at about 0.5% to 54] reducing the cross-sectional area and thus the overall strength. For
0.7% strain (as depicted with arrows on the top curve). After this first the first-cracking-strength both effects balance each other while for the
crack, the synthetic microfibres are pulled out and are able to take over compressive strength the influence of the macro pore formation seems
the additional stresses in the material as they are bridging the cracks. to be more pronounced. The amount of 1 m% was based on previous
The progression in crack width increase is thus stopped and the ce- research to get optimal sealing [36] and healing [22, 24, 37]. A further
mentitious material is forced to crack somewhere else upon stress in- increase in SAP content would lead to a detrimental effect of the macro
crease. Therefore, another crack is formed, but again, fibres are able to pores on the mechanical properties and thus huge strength losses.
deal with the increased load and the material will be able to take up When studying the formed healing products, it was clear that when
higher forces. In this way, not a single large crack, but multiple small being exposed to wet/dry cycling, the cracks were able to close to full
cracks are formed due to this strain-hardening effect. These cracks are extent (Fig. 3), both in REF and in SAP samples. The healing products
beneficial in terms of autogenous healing as the crack widths are

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D. Snoeck et al. Cement and Concrete Research 113 (2018) 86–98

Stress σ [MPa]
15

10

― REF
― SAP
σfc
5

Strain ε [%]
0

Fig. 2. Typical stress strain curves of the 20 × 40 × 160 mm3 samples loaded till 2.5% strain using four-point-bending. Both series show a first-cracking strength σfc
around 6 MPa. A clear strain-hardening effect with multiple crack formation (as depicted by arrows on clear stress drops) is observed.

absorb moisture even without being into direct contact with liquid
water [50], they are able to stimulate autogenous healing as well at
sufficiently high relative humidity [24]. Especially in the interior of the
sample, these formed healing products play an important role. As near
the crack tip the crack width is much smaller compared to the one at the
crack mouth, limited healing products may already bridge a crack lo-
cally. This leads to physical blocking of the crack and possibly also in a
regain of mechanical properties [22, 24]. In wet/dry cycles, the healing
mostly occurs near the crack mouth (to 700–1000 μm below the crack
mouth [23]). Most of this healing occurs in the first three to seven wet/
dry cycles. As the crack is sealed quite quickly, the healing in the in-
terior of the sample is partially inhibited. This may have a consequence
for the water penetration in a crack. Therefore, in this paper, we aimed
at investigating the water profiles in these materials by means of neu-
tron radiography (see later on).
The crack closure in percentage as measured by comparing the
crack widths before and after 28 days of healing is shown in Fig. 4. In all
samples, the crack widths were limited to approximately 60 μm. By
studying this figure, it is clear that no healing was observed in REF
samples stored at a relative humidity condition higher than 90%. This
absence of healing would be the same when storing the samples at a RH
of 60%. When SAP samples were stored at 60% RH conditions, limited
healing was observed. At > 90% RH, partial visual closure was ob-
served in the form of further hydration. Especially in the interior of the
sample [23], this healing could lead to the observed regain in me-
Fig. 3. Visual closure on the bottom of samples after being healed for 28 days in chanical properties [24]. The main cause for this healing is the ability of
wet dry cycling. Clear further hydration and calcium carbonate crystallization SAPs to absorb moisture from the environment. They are able to absorb
can be seen. The scale bar on the bottom part of the figure amounts to 500 μm. up to 3 to 4 times their weight in moisture [50]. This already seems to
be sufficient for stimulating and promoting autogenous healing in the
vicinity of the SAP particles.
are formed due to a combination of further hydration, pozzolanic ac-
When subjected to wet/dry cycles, the healing of REF samples was
tivity of the fly ash, and the formation of whitish calcium carbonate
more pronounced compared to the samples stored at high RH condi-
crystals. Fig. 3 shows the performance of a strain-hardening material in
tions. Cracks up to 30 μm are able to close completely. Larger crack
terms of autogenous healing. Small multiple cracks show complete
widths are able to partially close. It was clear that in SAP specimens,
healing (30–50 μm) [18, 24]. As the crack widths are limited, the
this healing was even more pronounced compared to the REF samples.
amount of building blocks and healing products is sufficient. A larger
As SAPs are able to retain water in their structure, water is also avail-
crack would not be healed as effectively (partial healing up to 150 μm)
able during the dry periods and optimal conditions for autogenous
[18, 24]. So, when comparing these multiple, small, but healable cracks
healing are present. In this way, they stimulate and promote auto-
with a single, large and unhealable crack, the former condition has the
genous healing. Larger crack widths are able to close and an improved
preference.
healing is observed. The results are in correspondence to results ob-
In an environment with a relative humidity of > 90%, only the
tained with X-ray microtomography [23]. In the latter research, only
samples with SAPs show partial healing, mainly due to further hydra-
the outer 700–1000 μm are completely sealed by healing products. This
tion in a kind of stitching pattern. As the SAP particles are also able to
optimal healing leads to the regain in mechanical properties [24] and to

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D. Snoeck et al. Cement and Concrete Research 113 (2018) 86–98

Crack closure [%]

100

75

SAP-wd
50 REF-wd
SAP-90
SAP-60
25 REF-90

0
0 20 40 60 80
inial crack width [μm]

Fig. 4. Percentage of visual closing found in the observed cracks for every test series. The crack widths were limited to approximately 60 μm. More healing is
observed in healing conditions with liquid water present.

a possible regain in water tightness. But, the extent of this healing, compared to REF-90), REF samples in wet/dry cycles (−52% compared
especially in the interior of the cementitious material, is still object of to REF-90) and SAP samples in wet/dry cycles (−75% compared to
discussion and was therefore studied further on in the next section. REF-90). The latter shows almost no absorption compared to the other
The autogenous healing leads to a regain in mechanical properties test series. Furthermore, there seems to be a good correlation with
[22, 24]. The healed specimens are able to regain some of their me- Fig. 4 which shows the percentage of visual closure of the initial cracks.
chanical properties (up to 75%). Even second reloading of those healed If the healing is better, the absorbed water content is lower. This means
samples leads to partial additional regain in mechanical properties (up that the (promoted) healing of the cracks is important in terms of the
to 66%) [22]. capillary water absorption. It has to be mentioned that the SAP particles
are storing their absorbed water when measuring the mass of the
samples. Taking this into account, the value in the matrix itself is even
3.2. Capillary absorption using gravimetric analysis and neutron
lower.
radiography
It would be interesting to study the absorption of water as a function
of time. When all radiographs are studied and analysed, Fig. 6a is ob-
The masses as obtained with image analysis of the neutron radio-
tained. Here, the mean water absorption in grams is shown together
graphs and as obtained with mass-scale measurements (after 2 h of
with the standard deviation on the single results (n = 3). The averages
capillary absorption) are shown in Fig. 5 as an average of the neutron
undergo small deviations with respect to the general trend for the dif-
radiography measurements on three different samples. A good statis-
ferent test series. This is due to fluctuations of the neutron beam itself.
tical correlation exists between both measurement techniques, showing
The current needs to be constant as a function of time to get uniform
the positive aspect of neutron radiography as a quantitative measure-
images, but sometimes the proton current decreases due to sudden
ment technique. The small difference may be due to the assumption
failure of the beam. These images thus showed a slight decrease in
that the water content in the immersed part of the samples is the same
overall dose. The average proton current was 970–980 μA, but the
as the water content just above the water level (see Section 2.4).
threshold value was 900 μA. Generally, these observed fluctuations are
From Fig. 5, it is clear that more water is absorbed by less healed
minor compared to the deviation on the water penetration itself, so the
specimens and less water is absorbed by healed specimens. In order of
different test series could be compared.
decreasing amount of absorbed water; SAP specimens at a RH of 60%,
As a function of the square root of time, the overall absorbed mass
REF samples at a RH > 90%, SAP samples at an RH > 90% (−45%
increases. The conclusions drawn earlier, based on the water absorption
Absorpon
after 2 h (Fig. 5), are confirmed. The highest amount of water is ab-
Gravimetry with mass balance
mass [g] sorbed by REF samples stored at a relative humidity condition
Image analysis of neutron radiography
9 of > 90%, closely followed by the SAP specimens stored at a RH con-
dition of 60%. There seems to be an increase in water uptake rate for
the SAP samples compared to the REF specimens. Then, there is a sig-
nificantly lower amount of absorption by the SAP specimens at > 90%
6
RH and the REF specimens stored in wet/dry cycling. The SAP speci-
mens stored in wet/dry cycles show the best results in terms of im-
permeability. Here, the water absorption rate is very low and only a
3 minor increase in mass absorption is observed in time. Even though the
scatter is noteworthy due to the cracked nature of the samples and the
healing, differences in absorption could be noticed.
0
The results obtained with neutron radiograph analysis seem to
correspond perfectly compared to the results obtained by capillary
water absorption measurements (Fig. 6b). In time, the absorption rate
Fig. 5. Comparison between the masses obtained by gravimetric mass balance
measurements and by image analysis of the obtained and corrected neutron seems to be comparable. The same conclusions can be drawn. However,
radiographs, both at 2 h of capillary absorption. Both masses are comparable. when looking at the results obtained from neutron image analysis, the

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D. Snoeck et al. Cement and Concrete Research 113 (2018) 86–98

Absorpon [g]

SAP-60
8
REF-90 SAP-60
REF-90
7 SAP-90
REF-wd
6 SAP-wd

SAP-90
4

REF-wd
3

2 SAP-wd

Time [√(h)]
0
0 0.5 1 1.5

(a)

12 Absorpon [g] SAP-60 SAP-60

REF-90 REF-90
SAP-90 SAP-90
REF-wd REF-wd
10 SAP-wd SAP-wd

Time [√(h)]
0
0 0.5 1 1.5 2 2.5 3 3.5 4 4.5 5

Fig. 6. Capillary water absorption [g] as a function of the square root of time [√(h)] showing the increase in mass in the cracked healed specimens using image
analysis on the neutron radiographs (a). The lower the curve, the better the sealing and/or healing capacity. Comparison between the obtained results by image
analysis of neutron radiographs (solid lines) and the capillary water absorption mass method following the Standard EN 13057 (dashed lines) (b).

initial absorption seems to be higher. This is due to the assumption that wet/dry cycles and SAP wet/dry cycles, respectively. The specimens
the immersed part of the specimen would have a water content equal to showing limited crack healing started to become more and more satu-
the water content just above the water level after 2 h of water ab- rated.
sorption test. This may not be true. As the mixture is a self-compacting When one would divide the mass by the exposed contact surface (which
and quite dense mixture, the water penetration could be more delayed is 160 × 20 mm2), the absorption per square meter can be obtained. Using
in time. However, when penetration in cracks accounts for the largest the standard EN 13057, the sorption coefficient could be calculated. This
part of the absorbed mass of water, this assumption is of less im- coefficient represents the ability to absorb water due to capillary suction.
portance. If the assumption would not be made and only the upper part The sorption coefficients for the test series were 0.68 ± 0.03 kg·m−2·h–0.5,
of the sample would be studied, an underestimation would be made. 0.40 ± 0.03 kg·m−2·h–0.5, 0.20 ± 0.04 kg·m−2·h–0.5, 0.62 ± 0.06 kg·m−2
When looking at the results from 1 h onwards, the trends obtained from ·h–0.5 and 0.31 ± 0.02 kg·m−2·h–0.5 for SAP = 60% RH, SAP > 90% RH,
neutron radiography are the same as when using capillary absorption SAP wet/dry, REF > 90% RH and REF wet/dry, respectively. Even though
tests. After 24 h of capillary absorption testing, the mass gain amounts cracked samples are tested, the results show that the SAPs are able to
to 10.7 ± 0.5 g, 9.8 ± 0.9 g, 6.3 ± 0.4 g, 4.8 ± 0.2 g and prevent water penetration in cracked cementitious materials. The results are
3.2 ± 0.6 g for SAP 60% RH, REF > 90% RH, SAP > 90% RH, REF closely linked to the visual crack closure observed by microscopic analysis.

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D. Snoeck et al. Cement and Concrete Research 113 (2018) 86–98

0.5 Fig. 7. The water content [g/cm3] above the level of

Water content submersion and at two thirds of the total height in REF
[g/cm³] 5 min 10 min 15 min 45 min 120 min
specimens healed at a RH of > 90% showing three distinct
cracks and a clear and high water uptake through the
0.4 cracks. The top water profiles are shifted upwards with a
constant 0.25. The water profiles show the water content
after 5 min, 10 min, 15 min, 45 min and 120 min of water
contact, respectively. As a reference, the locations of the
0.3
studied rectangles (dashed lines) and the observed visual
cracks by means of microscopy are shown beneath the
water profile curves. The measured initial crack widths
0.2 are shown underneath the respective cracks.

0.1

0
0 2 4 6 8 10 12 14 16

Posion [cm]
-0.1

3.3. Obtained water profiles for the different test series ingress of water through these cracks. Even after 5 min of contact time,
the ingress is already substantial. The water penetration through the
Figs. 7–11 show typical results for the obtained water profiles using cracks towards the cementitious matrix further increases as a function
neutron radiography after 5, 10, 15, 45 and 120 min of water contact. of time. On the left hand side a double crack is found as two clear peaks
The water profiles of all samples of the different test series are provided are seen in the lower water content profile. In the upper part, the effect
as Supplementary material. Generally, when looking at the cementi- of both cracks is combined. It is clear that this double crack leads to
tious matrix itself, it is clear that the water front only gradually pro- more water ingress compared to the single crack observed on the right
gresses due to capillary action. In a crack, this water front quickly in- hand side. As there is no healing of the crack (see Section 3.1), water is
trudes the matrix leading to an increase of the observed grey values and not inhibited to move in the cementitious matrix through the cracks.
thus absorption in time (see results in Section 3.2). Two different lo- This is not beneficial in terms of durability and therefore unwanted. The
cations were studied, being right above the water level and at a height sample quickly becomes saturated. The water movement from a crack
of approximately two thirds of the total height. These locations are also towards the cementitious matrix propagates inwards over approxi-
shown on the radiograph after 2 h of capillary absorption testing by mately 3 mm, 4 mm, 5 mm, 7 mm and 10 mm after 5 min, 10 min,
means of a dashed rectangle. To be complete, the visually observed 15 min, 45 min and 2 h in the lower rectangle. In the upper rectangle,
crack pattern by means of microscopic analysis is depicted as well (red this is approximately 1 mm, 2 mm, 3 mm, 4 mm and 6 mm, respectively.
lines). The clear peaks in the water profiles correspond to the locations For the REF specimens stored in wet/dry cycles (Fig. 8), the water
of the cracks themselves. The combinatory approach of studying the movement is only partially prevented by the healed cracks. The cracks
cracks visually and together with water profiles leads to solid conclu- are still clearly seen as peaks in water content. The peaks in the upper
sions in terms of the observed healing of the cracks and water pene- part of the sample are masked as less water is penetrating through the
tration through them. In that way better conclusions can be drawn cracks. The rate of water penetration in the cementitious matrix is also
about the water penetration in the interior of the specimen, after being lower compared to the unhealed REF samples. The distances of pene-
healed. tration in the lower part are approximately 2 mm, 3 mm, 4 mm, 5 mm
When looking at the results for the REF samples stored in a relative and 6 mm after 5 min, 10 min, 15 min, 45 min and 2 h of testing. This is
humidity condition of > 90% (Fig. 7), it is clear that there is a vast already lower compared to unhealed specimens, but still noteworthy.

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D. Snoeck et al. Cement and Concrete Research 113 (2018) 86–98

0.5
Water content
5 min 10 min 15 min 45 min 120 min
[g/cm³]

0.4

0.3

0.2

0.1

0
0 2 4 6 8 10 12 14 16

Posion [cm]
-0.1

Fig. 8. The water content [g/cm3] above the level of submersion and at two thirds of the total height in REF specimens healed in wet/dry cycling showing five distinct
cracks and a partial water uptake in healed cracks. The top water profiles are shifted upwards with a constant 0.25.

Samples with SAPs may show better results. Not only is the healing in the SAPs into the crack is also somewhat hindered due to the smaller
REF samples of inferior quality compared to the healing in SAP samples, crack. Capillary action is still prominent even though SAPs are able to
the SAP are able to swell and physically block a crack for intruding swell as water may be absorbed in between single SAP particles. When
fluids. In the upper region of the REF samples, the absorption is delayed studying the water permeability in cracks of larger magnitude, the SAPs
with half an hour approximately. The grey levels are lower compared to are able to seal a crack for further intrusion of water flow [36] as they
the case where the specimens' cracks would not have healed properly. are partially deformed in a crack, i.e. they are able to change form to
This vaguer color shows that only part of the crack is prone to water small extent.
penetration and thus that the healing action was not entirely sufficient. The water penetration from the cracks into the cementitious matrix
For the SAP specimens stored at a RH of 60% it is clear that a quick occurs at the same rate as for unhealed REF samples. The healing in SAP
ingress of water is observed (Fig. 9). Capillary action is also observed in samples was still too low to seal cracks physically by healing products.
the higher regions. In the left crack, the capillary action is only visible The rate of water intrusion in the cementitious matrix for REF and SAP
after 10 min of testing. Partial blockage by the SAPs may be the reason samples is the same as the cementitious matrix shows the same effective
for the delay. As the SAP particles are able to swell, they will physically water-to-cement ratio and microstructure [49, 50]. Even though the
hinder the water moving further in the crack. From the crack, a clear SAPs are able to swell within their formed macro pores, the water
horizontal movement can be seen as well. On the right hand side, a movement through the same overall microstructure in between the
double crack is found, as was the case for the REF samples at > 90% macro pores is the same.
RH. Even though the ingress is still substantial, the swelling action of For SAP samples stored at a RH of > 90% (Fig. 10), the ingress of
the SAPs partially prevents water movement through the cracks, as water is further delayed and the total absorbed water mass is less
compared to REF samples. In this study, the width is substantially lower compared to the SAP specimens at 60% RH. The rate of water pene-
compared to the 200 μm wide cracks studied in previous research [36]. tration in the cementitious matrix is again comparable. The healing of
There thus was a very fast capillary action and the SAP particles seemed only narrow cracks may have an influence, as the larger cracks were not
not able to perfectly seal a crack upon water intrusion. The swelling of healed effectively (see Section 3.1). The smaller middle crack only

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D. Snoeck et al. Cement and Concrete Research 113 (2018) 86–98

0.5
Water content
5 min 10 min 15 min 45 min 120 min
[g/cm³]

0.4

0.3

0.2

0.1

0
0 2 4 6 8 10 12 14 16

Posion [cm]
-0.1

Fig. 9. The water content [g/cm3] above the level of submersion and at two thirds of the total height in SAP specimens healed at a RH of 60% showing three distinct
cracks and high water penetration through the cracks. The top water profiles are shifted upwards with a constant 0.25.

shows water penetration after 10 min of testing. It does not show the Here, the healing together with the blocking effect of the SAPs in the
presence of water in the upper regions. This crack seems to be healed interior prevent further movement of water in the crack, thus leading to
partially and the water movement is prevented along the height. The a regain in impermeability. In the two left cracks, perfect healing was
stimulated healing action by the SAPs leads to this feature. The delay in observed. The healing at the crack mouth seemed to be efficient in
water penetration may be due to slower capillary action through a counteracting the water ingress.
partially healed crack. The crack does not progress as high as the other In REF specimens exposed to > 90% RH the penetration and
observed cracks and this may lead to the absence of water in the upper amount of water is highest compared to all test series. As there is no
rectangle. The smallest crack at the right hand side, however, does not hindrance for water penetration, when coming into contact with water,
show any kind of water penetration whatsoever. Only a small increase the crack immediately fills with water. In order to prevent corrosion of
at the 12 cm position is noticed. This crack (6 μm) was small enough to the reinforcement (especially when the fluid contains dissolved chlor-
be healed completely. ides), it is important that the water penetration does not reach the re-
When studying the results of the SAPs samples exposed to wet/dry inforcement. Unhealed specimens show a high capillary rise of water in
cycling, it is obvious that the healing of the cracks prevented further the cracks which should be avoided. In the healed specimens, some
ingress of water in the cracked matrix (Fig. 11). Even though several cracks are efficiently sealed with healing products, preventing the in-
cracks were formed, only two distinct cracks are seen in the lower gress of water. SAPs further aid in hindering the water movement as
profiles, while only one single crack is seen after 120 min of testing in they are able to swell and block a crack if water comes into contact with
the upper curves. The water profile of the upper part progresses through the polymer. The time at which corrosion may start is thus delayed.
the crack. In the right crack, the water movement is also very slow and These aids in the possible increase in durability and the possible longer
the water front moves vertically in time, comparable to the horizontal service life of structures built with a strain-hardening materials and
movement of the water as in all other test series. The rate is the same. incorporated superabsorbent polymers.

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D. Snoeck et al. Cement and Concrete Research 113 (2018) 86–98

0.5
Water content
[g/cm³] 5 min 10 min 15 min 45 min 120 min

0.4

0.3

0.2

0.1

0
0 2 4 6 8 10 12 14 16

Posion [cm]
-0.1

Fig. 10. The water content [g/cm3] above the level of submersion and at two thirds of the total height in SAP specimens healed at a RH of > 90% showing three
distinct cracks and a partial blockage of water uptake. The top water profiles are shifted upwards with a constant 0.25.

4. Conclusions – Neutron radiography is a powerful tool to visualize and quantify the

moisture profiles in cracked cementitious materials. The results are
Based on the findings of the research on the permeability of ce- comparable to the gravimetrical analysis of the capillary absorption
mentitious materials with and without SAPs as studied by means of in time.
neutron radiography following conclusions can be drawn: – Compared to REF stored in a relative humidity of > 90%, REF ex-
posed to wet/dry cycles shows a decrease of −52% in absorbed
– The best healing was obtained for SAP samples exposed to wet/dry mass, SAP at a RH > 90% a decrease of −45% and SAP in wet/dry
cycles, followed by REF exposed to wet/dry cycles, SAP at a relative cycles a decrease of −75% in absorbed water mass.
humidity of > 90%, SAP at a relative humidity of 60% and REF at a – When studying the reference material without SAPs in a relative
relative humidity of > 90%. humidity condition, the water penetration is high and this is un-
– In high relative humidity condition the REF specimens do not show wanted in terms of durability aspects. The water penetration should
healing in any kind of form as there is no presence of liquid water. be prevented or counteracted.
When being exposed to wet/dry cycles, these REF samples show – SAPs are able to cause a regain in impermeability and the water
clear visual closure of cracks up to 30 μm. movement is partially counteracted. The ingress is delayed in time
– The SAPs are able to stimulate and promote autogenous healing, due to the swelling action of the SAPs.
even at high relative humidity conditions of > 90%. – As the healing is more pronounced in SAP specimens, the cracks are
– Healing of specimens with SAPs in a relative humidity condition also sealed in a better way compared to REF samples. This leads to a
of > 90% is comparable to the healing of REF specimens exposed to lower ingress of water through these cracks as the path is physically
wet/dry cycles. When subjected to wet/dry cycles, the SAP speci- and pertinently blocked. The swelling action of the SAPs further aids
mens show a pronounced healing and cracks larger than 50 μm also in this mechanism as possible intruding water is inhibited from in-
show some extent of healing. trusion in the cementitious matrix.

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D. Snoeck et al. Cement and Concrete Research 113 (2018) 86–98

0.5
Water content
5 min 10 min 15 min 45 min 120 min
[g/cm³]

0.4

0.3

0.2

0.1

0
0 2 4 6 8 10 12 14 16

Posion [cm]
-0.1

Fig. 11. The water content [g/cm3] above the level of submersion and at two thirds of the total height in SAP specimens healed in wet/dry cycling showing five distinct
cracks and a low water uptake in healed cracks. Some cracks do not show any kind of water penetration. The top water profiles are shifted upwards with a constant
0.25.

– SAPs are a promising admixture to be used in a cementitious ma- Data availability statement
terial for self-sealing and promoted autogenous healing. The dur-
ability may be enhanced as less fluids can penetrate the structure. The datasets generated during and/or analysed during the current
This may lead to an increase in service life. study are available from the corresponding author on reasonable re-
quest. Supplementary material (water profiles for all samples) are
Acknowledgements available and submitted next to this manuscript.

As a Postdoctoral Research Fellow of the Research Foundation- Appendix A. Supplementary data

Flanders (FWO-Vlaanderen), D. Snoeck would like to thank the foun-
dation for the financial support (12J3617N). The authors would like to Supplementary data to this article can be found online at https://
thank the Paul Scherrer Institute (PSI) for granting neutron beam time doi.org/10.1016/j.cemconres.2018.07.002.
at the NEUTRA SINQ facility to execute the research proposal (ID No.
20170327). The staff of the Paul Scherrer Institute (PSI), and especially References
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