Early Age Cracking in Cementitious Systems 27

3.3 EVOLUTION OF SOLID BEHAVIOUR

Jan Bisschop
Microlab, Faculty of Civil Engineering and Geosciences, Delft University of Technology, The
Netherlands

3.3.1 Introduction

The main driving force for early-age shrinkage and cracking in cement-based materials with low
w/c ratio is the chemical reaction of cement with water. In hardening cement-based materials with
low w/c ratio, the on-going cement hydration can lead to self-desiccation shrinkage if the internal
humidity drops below 100%. Depending on the magnitude of self-desiccation shrinkage, the
development of the mechanical properties, and on the degree of internal or external restraint,
early-age cracking may occur in these concretes. Self-desiccation can only lead to significant
shrinkage stresses if the cement-based material behaves as a solid (i.e. has strength and stiffness).
This happens when, due to hydration, some rigid self-supporting skeleton has developed. The
process in which liquid cement-based material changes into a visco-elastic solid is called setting.
In this section the microstructural changes that take place in the cement paste during setting will
be described. It will be addressed what can be taken as time “zero” for autogenous shrinkage
measurements and modelling. Furthermore, this section deals with the development of mechanical
properties of cement-based materials at early ages after setting. Creep and relaxation may also
have an important effect on the mechanical behaviour at early ages (see sections 4.4, 6.4).

3.3.2 Setting of Cement Paste

Setting of cement paste is a transitional period between states of true fluidity and true rigidity [1].
Setting is a gradual change, controlled by the continuing hydration of the cement. Therefore it is
difficult to pinpoint the exact time of setting of a cement paste. There are a number of testing
methods for the determination of ‘setting’ time (see section 6.1). With the Vicat needle method
(EN 196-3) or the penetration resistance method (ASTM C 403) predefined initial set and final set
time can be measured. This method does not measure any specific change in mechanical property.
Methods which more directly measure changes in rigidity are acoustic - ultrasonic techniques [1-
5]. It is generally believed that the ultrasonic pulse velocity is directly related to the strength (and
modulus of elasticity) of the cement paste. Therefore, the setting process of cement paste and
development of strength can be monitored by recording the increase in (compressional) ultrasonic
pulse velocity. As ultrasonic shear waves are not transmitted in a fluid, the detection of these
waves can indicate the beginning of formation of solid material.
28 RILEM TC 181-EAS: Final Report - July 2002

On basis of results obtained with an ultrasonic method in combination with chemical and
autogenous shrinkage measurements (i.e. external volume changes) Barcelo et al. [4] described
setting, or more precisely the suspension-solid transition of cement paste. The following four
stages have been recognised (see Figure 3.3.1). During the suspension period (phases 1 and 2), the
solid grains are isolated in the liquid phase. The material cannot resist volume variations and
chemical shrinkage and autogenous shrinkage are identical. This period can be very short,
especially for low w/c-ratio pastes (e.g. 40 minutes for a paste with w/c-ratio of 0.28). During
phase 3 the rigidity of the material gradually increases as hydration proceeds. In this phase the
first ‘solid path’ appears in the cement paste. This so-called mineral percolation threshold can be
detected with the ultrasonic technique. According to Boumiz [6] this threshold corresponds to the
minimum of the compressional ultrasonic velocity. This threshold corresponds to the moment
when the curves of autogenous shrinkage and chemical shrinkage start to diverge (see Figure
3.3.2). Zones appear within the material where the volume variations imposed by the hydration
reaction are locally hindered by the solid contacts and therefore the rate of autogenous shrinkage
decreases and becomes lower than chemical shrinkage. According to Barcelo et al [4] this mineral
percolation may be seen as an unidirectional path for ultrasonic waves within the material.
Between phases 3 and 4 a transition occurs from a liquid to a solid type of behaviour. In phase 4
percolation of the solid network in three dimensions appears. From this phase onwards volume
variations caused by hydration are greater than bulk deformations of the mineral skeleton, and a
significant gaseous volume appears in the capillary pores (Figure 3.3.1). In low w/c-ratio pastes
(where the internal humidity drops below 100%), this phenomenon leads to self-desiccation and
results in autogenous shrinkage.

Absolute volume variations : chemical shrinkage

Water

Hydrates

Cement

hydration Mineral skeleton percolation

t=O

1 2 3 4
Gas
Apparent volume variations

Figure 3.3.1: Self-desiccation as a consequence of chemical shrinkage [7,8]

 Early Age Cracking in Cementitious Systems 29

The transition from a 1-D to a 3-D solid percolation (i.e. suspension-solid transition) can also be
monitored with the ultrasonic technique. According to Morin [9] three dimensional percolation is
reached when the so-called Transversal Wave Reflection (TWR) factor becomes independent to
the used frequency. The transition occurs roughly when the rate of autogenous shrinkage
decreases drastically (see Figure 3.3.2). It has been determined that initial and final set values
determined with the Vicat needle method constitute the lower and upper bound of the suspension-
solid transition [10]. In the cement paste of Figure 3.3.2 this transition (at the knee-point of the
curve) took place 3.2 hours after mixing (4% in terms of degree of hydration).

Cement paste - Fine OPC - W/C=0.35

8 1.2

7
1
Autogenous shrinkage (mm3/g.

Slope = 1
6
0.8
5
cement)

Slope
4 Autogenous shrinkage 0.6

3
0.4

2
Slope 0.2
1

0 0
0 1 2 3 4 5 6 7 8
Chemical shrinkage (mm3/g. cement)
Figure 3.3.2: Autogenous versus chemical shrinkage – the suspension-solid transition occurs at the
knee-point of the autogenous shrinkage curve [4].

It was found by Boivin [10] that the suspension-solid transition occurred earlier for low w/c-ratio
pastes and finer cements, which could be explained by earlier and more uniformly distributed
solid-solid contacts compared to higher w/c-ratio pastes and coarser cements. Jiang and Roy [1]
and Justnes et al. [3] found the same trends using ultrasonic methods. Justnes et al. [3] determined
that the degree of hydration required to bring about initial setting (determined by Vicat needle)
was in the order 3-8% (2-7 hours after mixing) and this seemed to be lower for low w/c and
cement of increased fineness and/or C3A content.

Justnes et al. [3] studied the correlation between the knee-point of the external shrinkage
(autogenous shrinkage in [4]) curve (i.e. the deviation point between external and chemical
shrinkage) with setting times determined with ultrasonic technique and the Vicat needle technique.
The speed of ultrasound through paste had been calibrated against compressive strength of the
paste. Setting was considered to take place when strength of 0.35 MPa was achieved. They found
that the setting time estimated in this way fell in between the initial and final setting times
30 RILEM TC 181-EAS: Final Report - July 2002

determined by the Vicat needle. The knee-point of the external chemical shrinkage (autogenous
shrinkage) curve did not follow the setting time by Vicat for different w/c. The final setting time
corresponded well with this point for w/c = 0.40, but occurred earlier at w/c = 0.30 and later at w/c
= 0.50. According to the authors this was due to higher contracting forces in lower w/c-ratio paste,
which had a larger effect on the autogenous shrinkage (i.e. the timing of the knee-point) than on
the penetration resistance of the Vicat needle.

3.3.3 Time ‘zero’

What should be taken as time ‘zero’ for autogenous shrinkage measurements and modelling?
Since autogenous shrinkage is generally used for prediction of cracking, the strain generated in a
period when the cement-based material is fresh (i.e. before setting) is excluded, and of interest is
the moment when autogenous shrinkage leads to stresses. The review above highlighted the
difficulty in pinpointing exactly the moment when cement paste (and concrete) sets is difficult to
pinpoint exactly. Therefore it is difficult to determine time ‘zero’ from ultrasonic measurements.
Moreover, after setting, cement-based materials with low w/c-ratio often show a short period of
swelling in longitudinal autogenous shrinkage measurements [11,12]. The reason of this swelling
has been attributed to the reabsorption of bleeding water [11], or to the ‘crystallization pressure’
of growing hydration products [4,13,14]. Due to this swelling the start of shrinkage and tensile
stresses can be delayed, while the material already turned into a solid.

A combination of two testing set-ups -free and restrained shrinkage tests- is desirable to determine
when autogenous shrinkage leads to stresses, and when these stresses become tensile stresses
(Figures 3.3.3 and 3.3.4). As found by Bjøntegaard [11] and Lura et al. [12] the initial swelling
may lead to low compressive stresses (see Figure 3.3.4). One may argue from a practical point of
view, that the time when tensile stresses start (after swelling, when detected) should be taken as
‘time zero’, because from this point onwards autogenous shrinkage causes tension. A second
possibility is to take the end of expansion as time ‘zero’ [11]. Although this is the time when
autogenous shrinkage starts (in case when initial swelling occurs), it is not the moment when
tensile stresses start to develop. However, the weight of the literature supports the view that time
‘zero’ should be taken when stresses start (including the compressive stresses caused by swelling),
since it represents the time when the material is turning into a visco-elastic solid.

It should be mentioned that deformations measured at the very early ages after setting under sealed
conditions are not necessarily due to autogenous deformation only. Also the contribution of
thermal dilation should be considered. In fact the initial swelling after setting, between 6 to 12
hours has also been related to thermal effects [15]. The separation of thermal and autogenous
deformations has been dealt with by [11,16,17].
 Early Age Cracking in Cementitious Systems 31

Figure 3.3.3: Total deformation of three high-strength concretes A', B', and C' measured in free
shrinkage test [20]. Shrinkage is plotted negative. Notice the initial swelling for B' and C'.

50

Total deformation (μstrain)

0

-50
B'
-100
A'

-150
C'
-200

-250
0 24 48 72 96 120 144
Time (hours)

Figure 3.3.4: Self-induced stress inthe high-strength concretes in Figure 3.3.3 measured in a
restrained shrinkage test [20]. The crosses indicate failure of the specimens. The initial swelling is
accompanied by compression only in C'.

3.00
X
2.50
Self-induced stress (MPa)

A'
X
2.00
B'
1.50
1.00
0.50
0.00
C'
-0.50
0 24 48 72 96 120 144
Time (hours)

3.3.4 Strength in relation to microstructure development

The resistance to early-age shrinkage and cracking depends on the development of the mechanical
properties of the cement-based material. In cement paste, hydration leads to development of
material structure on the nano- and microscales. These changes in the material structure are
accompanied by changes in the mechanical properties (e.g. strength and elasticity) of the cement
paste.

On the nanoscale the relation between strength and structure is governed by physico-chemical
processes binding hydrated cement particles (i.e. primary and secondary bonding), but also by the
increasing number of contact points/surfaces of particles – a so-called stereological (i.e.
geometrical) aspect [18]. For example the effect of w/cratio on strength development can be
explained from a geometrical point of view, as are temperature effects and chemical composition
of the cement, because a decrease in porosity basically means an increase in particle contacts [18].
32 RILEM TC 181-EAS: Final Report - July 2002

That strength development has a geometrical aspect can be indicated by referring to the strength
development of low porosity pastes (i.e. low w/c-ratio pastes). The fact that in these pastes high-
strength values are reached at relatively low degrees of hydration can be attributed to a large
extent to the initial dense packing of the cement particles which results in only small amount of
gel being required for “gluing” the hydrating particles together [18]. It should be mentioned,
though, that in low w/c-ratio pastes more cement reacts than in a high w/c ratio paste (of same
volume) for a given degree of hydration.

On the microscale, the distribution and proportions of clinker minerals (i.e. cement type, particle
size distribution), and the air-void content and flaws (i.e. stress-concentration) can be expected to
influence the cement paste strength.

The development of strength with can be expressed as a function of hydration time. But a
development of strength in time can not directly be linked to the evolution of microstructure, as
the rate of hydration is influenced by temperature, humidity, cement type, additives, w/c-ratio and
other factors. The relation between microstructure and strength can be described indirectly by
means of a linear relationship between degree of hydration and strength [19]. The degree of
hydration can be expressed as the amount of cement that has hydrated compared to the initial
amount of cement. This definition of degree of hydration cannot be measured by simple means.
Other effects due to hydration of cement are more practical to measure and can be used to identify
the degree of hydration. The parameters that are most often used are the heat liberated and non-
evaporable water content [19].

As the hydration process produces heat, the reaction becomes self-accelerating, because the rate of
hydration increases with increasing temperature. The strength development of cement-based
materials is closely linked to the progress of cement hydration which is at the base of the concept
that the strength development can be expressed as a function of a time-temperature combination,
the maturity concept. In the maturity concept, the strength developments at any arbitrary
temperature history are transformed to an equivalent hydration time at 20°C. A limitation of the
maturity concept is that it assumes that the final property is not influenced by temperature. This is,
however, not the case for most practical situations, as higher temperatures produce a different
microstructure and weaker bonds between particles and thus limit the strength potential [11].

3.3.5 Mechanical Properties at Early Ages: Paste Versus Concrete

The development of mechanical properties in cement paste can be linked to changes in the
microstructure by means of the degree of hydration or the maturity concept. These concepts are
more difficult to apply in concretes and especially in concrete with a low w/c ratio. This is because
the development of mechanical properties at early ages is dependent also on processes on length
scales beyond that of the plain cement paste. The relation between strength and microstructure
described in the previous paragraph is valid for the cement paste matrix in concretes. However,
in concretes, especially low w/c-ratio concretes, processes on the scale of the aggregate content
(the meso-scale) also contribute to the development of mechanical properties; these processes
cannot be easily linked to development of paste microstructure.

First, autogenous shrinkage in the paste matrix is internally restrained by the aggregates [20]. The
internal stresses caused by the aggregate restraint can be expected to influence the mechanical
properties of the concrete. Secondly, the presence of aggregates changes the rate of hydration and
 Early Age Cracking in Cementitious Systems 33

the microstructure of the cement paste. In the interfacial zone between the cement paste matrix and
the aggregate the w/c-ratio of the cement paste can be locally higher compared to the bulk paste.
Therefore, the hydration rate and porosity in the interfacial zone are higher [23].

The relation between the mechanical properties and autogenous shrinkage of cement paste and the
mechanical properties and autogenous shrinkage of concrete can be studied by means of
modelling [21-24].

3.3.6 Development of Mechanical Properties at Early Ages

Autogenous and thermal deformations are the driving forces for the development of early-age
stresses and cracking in concretes with low water-cement ratio. However, the magnitude of the
stresses and the risk of cracking will depend on the degree of restraint as well as the development
of the mechanical properties at this stage. Significant mechanical properties start to develop after
setting. For example, it was demonstrated that for a 0.40 w/b ratio concrete, significant mechanical
properties started to develop at about 10 hours [25]. For a 0.50 w/b ratio concrete this time
corresponded to a degree of hydration of about 25% [26]. Laube [27] reported that concrete of
0.58 w/c ratio started to achieve mechanical properties (typically around 8-10 hours) at a degree
of hydration of about 20%.

The mechanical properties (compressive strength, tensile strength and modulus of elasticity) all
increase as a function of hydration time, equivalent time or degree of hydration. An important
issue is the relative development of the mechanical properties at early ages, since it controls the
likelihood of early-age cracking. From test results and theoretical models for tensile strength it
was shown that the tensile strength at early ages tends to grow faster than the compressive strength
[25,28,29]. On the other hand, experimental work done by Weigler and Karl [30] showed that in
the first two days the tensile strength develops in a similar way as the compressive strength. In this
work it was also found that the E-modulus increased to 60% of its 28 days value after 1 day and to
90% after 3 days. This study and others demonstrate that the relative rate of development of
modulus of elasticity is much higher than the relative rate of development of compressive and
tensile strength, Byfors [31], Laube [27] and De Schutter and Taerwe [26] (Figure 3.3.5). This
difference in rate is a manifestation of early age cracking sensitivity, since the stress generated
will be dependent on the modulus of elasticity whereas the resistance to cracking will be
dependent on the tensile strength.
34 RILEM TC 181-EAS: Final Report - July 2002

100
90
Relative Value of Property, %

80
70 Modulus of Elasticity

60
50
40
30 Tensile Strength
20
10
0
0 20 40 60 80 100
Degree of Hydration, %

Figure 3.3.5. Schematic description of the relative development (%) of E-modulus and tensile
strength in high-strength concrete, adopted from data of De Schutter and Taerwe [26].

An important issue in this discussion is the effect of early-age creep, and especially the rate of
stress relaxation with respect to the rate of stress built-up [12]. Kovler et al. [32] found that early-
age creep of silica fume concrete is greater than that of a plain concrete with a similar w/b-ratio.
This enhanced early tensile creep may be an important mechanism mitigating the tensile stress
induced in silica fume concrete when its autogenous shrinkage is restrained.

Wiegrink et al. [33] found that even though their studied high-strength concrete studied in their
work had higher tensile strength than normal concrete at all ages, their early age shrinkage
cracking performance was substantially poorer. They contributed this to the higher free shrinkage
(if demolded after 6 hours), lower specific creep, higher modulus of elasticity, and lower
aggregate interlock along crack faces for the high-strength concretes.

3.3.7 References
1. Jiang, W. & Roy, D.M., ‘Microstructure and flow behaviour of fresh cement paste’, in Mat. Res. Soc.
Symp. Proc. Volume 289 (1993) 161-166.
2. De Haas, G.D. et al., ‘The shrinkage of hardening cement paste and mortar’, Cement and Concrete
Research, 5 (1975) 295-320.
3. Justnes, H., Clemmens, F., Depuydt, P., Van Gemert, D. and Sellevold, E.J., ‘Correlating the deviation
point between external and total chemical shrinkage with setting time and other characteristics of hydrating
cement paste’, in Proceedings of the Int. RILEM workshop on shrinkage of concrete – Shrinkage 2000, Paris,
October, (RILEM 2000) 57-74.
4. Barcelo, L, et al., ‘Early-age shrinkage of concrete: back to the physical mechanisms, UEF conference’ in
‘Advances in Concrete and Cement’, Mt-Tremblant, Canada, August, 2000.
5. Reinhardt, H.W., Große, C.U., Herb, A.T., ‘Ultrasonic monitoring of setting and hardening of cement
mortar – A new device’, Materials and Structures, 33 (2000) 580-583.
6. Boumiz, A., ‘Etude comparée des évolutions mecaniques et chimiques de pâte de ciment et mortiers a tres
jeune age’. PhD-thesis of Université Paris 7 (1995).
 Early Age Cracking in Cementitious Systems 35

7. Buil, M., ‘Comportement physico-chimique du système ciment – fumées de silici’, in Annales de L’LTBTP
(1990) 19-29.
8. Hua, C., ‘Analyses et modélisation du restrait d’autodessiccation de la pâte de ciment et mortiers a tres
jeune age’, Ph.D Thesis of Ecole Nationale des Ponts Chaussées: Paris (1995) 159.
9. Morin, V., ‘Etude de la transition de solidification de matériaux par méthodes ultrasonores’, Ph.D thesis of
Université Paris 7: Paris (1999).
10. Boivin S., ‘Retrait au jeune âge du béton: Développement d'une méthode expérimentale et contribution à
l'analyse physique du retrait endogène’, PhD-thesis of Ecole Nationale des Ponts et Chaussées (1999)
11. Bjøntegaard, Ø., ‘Thermal dilatation and autogenous deformation as driving forces to self-induced
stresses in high performance concrete’, Ph.D Thesis, Division of structural Engineering, The Norwegian
University of Science and Technology, Norway, (1999).
12. Lura, P, Van Breugel, K., Maruyama, I., ‘Effect of curing temperature and type of cement on early-age
shrinkage of high performance concrete’, Submitted to Cem. Con. Res. Special issue, Proc. of symposium
‘Materials Science of High Performance Concrete’ MRS 2000 Fall Meeting, Boston.
13. Bažant, Z.P., Wittmann, F.H., Creep and shrinkage in concrete structures, John (Wiley & sons, New
York, 1982).
14. Tezuka Y., et al., ‘Hydration characteristics and properties of mixtures of cement and high content of
calcium’, Proc. Symp. on Chemistry of Cement, Rio de janeiro, Vol II (1986) 323-329.
15. Lepage, S., Ballbaki, M., Dallaire, E., Aitcin, P-C., ‘Early shrinkage development in a high performance
concrete’, Cement Concrete and Aggregates, 21 (2) (1999) 31-35.
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Autoshrink’98, Proc. Int. Workshop on Autogenous Shrinkage of Concrete’ AUTOSHRINK 98, Japan
Concrete Institute, Japan (1998) 233-244.
17. Hedlund, H., Jonasson, J-E., ‘Effect on stress development of restrained thermal and moisture
deformation’, in Proceedings of the Int. RILEM workshop on shrinkage of concrete – Shrinkage 2000, Paris,
October, (RILEM 2000) 355-380.
18. Van Breugel, K. ‘Simulation of hydration and formation of structure in hardening cement-based
materials’, Ph.D Thesis, Delft Technical University of Technology, second edition (Delft University Press)
1997.
19. Van Beek, A. ‘Dielectric properties of young concrete’, Ph.D Thesis, Delft Technical University of
Technology, (Delft University Press) 2000.
20. Bisschop, J., Lura, P., Van Mier, J.G.M, ‘Shrinkage microcracking in cement-based materials with low-
water-cement ratio’, in Proc. RILEM Int. Conf. on Early Age Cracking in Cementitious Systems, K.Kovler and
A.Bentur, editors, (Haifa 2001) 79-88.
21. Goltermann, P., ‘Mechanical predictions of concrete deterioration - Part 2: classification of crack patterns’,
ACI Materials Journal 92 (1) (1995) 58-63.
22. Sadouki, H. and Wittmann, F.H., ‘Shrinkage and internal damage induced by drying and endogenous
drying’, in Proceedings of the Int. RILEM workshop on shrinkage of concrete – Shrinkage 2000, Paris, October,
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23. Koenders, E.A.B. ‘Simulation of volume changes in hardening cement-based materials’, PhD-thesis, Delft
University of Technology, (1997).
24. Ishikawa, M., Imamoto, K., Watanabe, H. and Ito, M., ‘An evaluation of autogenous shrinkage of concrete
based on mechanical properties of the matrix cement paste’, in proceedings of the Int. workshop on ‘Control of
Cracking in Early-Age Concrete’. Sendai, Japan, August, (2000) 215-222.
25. Bjøntegaard, Ø., Kanstad, T. Sellevold E., Hammer, T.A., Stress-inducing deformation and mechanical
properties of concrete at very early ages, in ‘Utilization of High-Strength/High Performance Concrete
Technology’, Proc 5th Int. Symp., Sandefjord, Norway, (1999) 1027-1040.
26. De Schutter, G., Taerwe, L., ‘Degree of hydration-based description of mechanical properties of early
age concrete’, Materials and Structures, 29 (1996) 335-344.
27. Laube, M., ‘Werkstoffmodell zur berechnung von temperaturspannungen in massigen betonauteilen
imm jungen alter’, Docotral Thesis TU Braunschweig (1990).
28. Kasai, Y., Yokoyama, K., matsui, I., and Tobinai, K., ‘Tensile properties of early age concrete’,
Mechanical Behaviour of Materials, The Society of Materials Science, Japan, 2 (1974) 433-441.
36 RILEM TC 181-EAS: Final Report - July 2002

29. Khan, A. A., Cok, W.D., and Mittchell, D., ‘Tensile strength of low medium and high-strength concretes
at early ages’, ACI Materials Journal 93 (5) (1996) 487-493.
30. Weigler, H., Karl, S., ‘Junger Beton’, Betonwerk + Fertigkeit – Technik, 6 (1974) 392-401; 7 (1974)
481-484.
31. Byfors, ‘Plain concrete at early ages’, Swedish Cement and Concrete Institute, Fo 3:80, Stockholm
(1980).
32. Kovler, K. Igarashi, S., Bentur, A., ‘Tensile creep behaviour of high-strength concretes at early ages,’
Materials and Structures, 32 (1999) 383-387.
33. Wiegrink, K., Marikunte, S., Shah, S.P., ‘Shrinkage cracking of high-strength concrete’, ACI Materials
Journal, 93 (5) (1996) 409-415.