Rheologica Acta (2020) 59:47–61

https://doi.org/10.1007/s00397-019-01171-x

ORIGINAL CONTRIBUTION

Rheological properties for fresh cement paste from colloidal

suspension to the three-element Kelvin–Voigt model
Jena Jeong1 · Edgar Chuta1 · Hamidréza Ramézani2 · Samuel Guillot3

Received: 19 May 2019 / Revised: 23 August 2019 / Accepted: 28 August 2019 / Published online: 7 December 2019
© Springer-Verlag GmbH Germany, part of Springer Nature 2019

Abstract
In the present work, rheological behaviors of fresh cement paste are studied based on multi-disciplinary approaches, i.e.,
colloidal suspension using attractive van der Waals force, rheology using the Bingham model and Bingham–Papanastasiou
model, which are able to describe the behavior of cement pastes before and after yield stress, and finally the continuum
mechanics based on Maxwell and Kelvin–Voigt models. To achieve this, the fresh cement paste with different water-to-
cement ratios of 0.3 up to 0.6 is prepared. The attractive van der Waals forces are estimated based on the distances between
solid cement particles, which vary at every single water-to-cement ratio. The rheology experiments of all water-to-cement
ratios are performed using a rheometer. According to our experimental outcomes, the Bingham and Bingham–Papanastasiou
models are applied in the modeling of the experimental curves and determination of yield stress and viscosity. Maxwell and
the Kelvin–Voigt models are utilized in describing solid-like behavior before yield stress and fluid-like behavior beyond yield
stress. It is observed that the increase of water generates a decrease in the viscosity, yield stress, and packing concentration of
solids. It also increases the distances between two cement particles in the cement pastes. According to the modeling results,
the Bingham–Papanastasiou model is well adapted for the cement paste flow due to its additional modeling parameter, which
is known as m. The role of m is understood and described by linking the van der Waals interaction, rheology, and three-
element Kelvin–Voigt model as a whole in function of water-to-cement ratio. m is understood as a key parameter in which
the distance between particles affects the rheological behavior of fresh cement pastes. Lastly, the two-phase flow simulations
have been successfully achieved and compared with the experiments. The conclusion and outlooks are summarized and
discussed at the end of the paper.

Keywords Bingham–Papanastasiou’s model · Colloidal suspension · Fresh cement paste · Distance of particles ·
Three-element Kelvin–Voigt model · Viscoelastic material

 Jena Jeong
jena.jeong@gmail.com; jjeong@estp-paris.eu
 Hamidréza Ramézani
hamidreza.ramezani@univ-orleans.fr
1 Université Paris-Est, Institut de Recherche en Constructibilité,
ESTP, 28 Avenue Président Wilson, Cachan, 94234, France
2 École Polytechnique de l’Université d’Orléans, Université
d’Orléans, ICMN, UMR CNRS 7374, Interfaces,
Confinement, Matériaux et Nanostructures, 8 rue Léonard
de Vinci, Orléans, 45072, France
3 Université d’Orléans, ICMN, UMR CNRS 7374, Interfaces,
Confinement, Matériaux et Nanostructures, 1b rue de la
Férollerie, CS 40059, Orléans Cedex 45071, France
Introduction
Generally, the study of rheology can be handled via a multi-
disciplinary approach, i.e., non-Newtonian fluid, continuum
solid mechanics like viscoelastic solids using Maxwell and
Kelvin–Voigt models, physical chemistry analysis using
interparticle interaction energies based on van der Waals
forces, wherein granulometry and size of particles and che-
mical composition of particles play a key role in colloidal
suspensions. The fresh cement paste transforms from a
liquid phase as a colloidal suspension into a solid phase
during the hydration period. Nowadays, fewer studies have
been done for such complex colloidal suspension in
cement and concrete society due to a highly complicated
physical chemistry-based feature of fresh cement paste.
48
Consequently, the present paper aims to study fresh cement
paste behavior using three approaches, i.e., classical
rheology (Bingham and Bingham–Papanastaiou), the inter-
molecular force interactions in colloidal suspension, and
continuum mechanics (Maxwell and Kelvin–Voigt models).
Let us get started with observation at the micrometer
scale. The fresh cement paste can be considered a col-
loidal suspension, wherein anhydrous grains are floating in
the water. Basically, the particle size of ordinary Portland
cement (OPC) is less than 60 μm and the range of BET
specific surface area would be typically between 0.7 and
2.5 m2 /g. According to the literature, 50% of the ordinary
Portland cement has a diameter of less than 10 μm in
some cases and 12 μm in other cases (Ferraris and Hack-
ley 2004; Treviranus 2008). Due to the large size of cement
particles, cement suspension is more sensitive to shear
force than any other force like Brownian movement.1 In
fact, since anhydrous grains are in contact with water,
the agglomeration and flocculation due to the hydration of
anhydrous grains provoke rapid electrolyte concentration.
This produces the interaction energy due to the repul-
sive and attractive forces between particles. The hydrate
nucleation at the grain surface leads to an increase in the
interparticle forces (Conte 2017). Such a very complex
system is often considered as colloidal particle suspen-
sion for superplasticizer admixture application for self-
compacting concrete. We can determine the yield stress
when the interaction links among particles are weak enough
to provide fluid flow. However, the yield stress point is
not always easy to be determined and its value depends
strongly on the concrete formulation, i.e., water-to-cement
ratio, admixtures, and so on.
On the other hand, fresh cement paste is often considered
as Bingham (Bingham 1922), Herschel-Bulkley (Herschel
and Bulkley 1926; de Larrard et al. 1998; Zhu et al. 2005;
Vajravelu et al. 2011) and sometimes Casson fluid (Cas-
son 1959) in rheology science. The abovementioned models
can be used for non-Newtonian fluids including various vis-
cosities beyond the yield stress. However, the disadvantage
of these models is that they are available if only the system
arrives at yield stress. That is inconvenient for numerical
modeling of the behavior of cement paste before and after
yield stress. To overcome the problems coming from this
issue, Papanastasiou (1987) added an additional parame-
ter called m to handle this behavior around the transition
area from solid-like to liquid-like systems. His suggestion
offers smooth and continuous rheological curves before and
after yield stress. Although m contains very interesting fea-
tures, there are only a few studies in dealing with linking
1 Forthis reason, the maximum interparticle force which is known as
colloidal force is the most relevant parameter in rheology rather than
Brownian movement.
Rheol Acta (2020) 59:47–61
interparticle force/distance between anhydrous grains in
water and m parameter implying shear stress and transition
from solid-like systems to liquid-like systems.
This paper aims to understand transition zone around
yield stress, which is known as offset yield point in
continuum mechanics, and interact energy linking to m
parameter of Papanastasiou’s benchmark paper. The main
goal of the present contribution is to enlighten offset yield
point by taking into account behavior of shear stress versus
strain rate, and the distance between particles relating to m
parameter around yield stress point.
The paper is organized as follows:
First, we give an overview of the fluid flow of fresh cement
paste using rheology science (Bingham and Bingham–
Papanastasiou) and continuum mechanics (Maxwell–Kelvin–
Voigt) model. Afterward, the van der Waals interaction energy
and repulsive/attractive force in terms of Hamaker’s con-
stant in cement colloidal suspension will be presented and
discussed in the section “Theoretical background.” More-
over, a simple analytical method is presented in determining
the distance between solid particles in cement paste accord-
ing to the size of particles. In the section “Materials and
experiments,” the experiments of the rheological behavior
of cement paste are presented. To study the impact of water
in cement paste, a series of cement paste samples have been
prepared at various water-to-cement ratios. These water-to-
cement ratios manipulate the interparticle distance and they
also change the necessary energy to cut the attractive forces.
The rheological behavior of every single sample is analyzed
using the Bingham and Bingham–Papanastasiou model. The
yield stress and various viscosities are determined via the
aforementioned models. In the section “Results and dis-
cussion,” the transition area from solid-like to liquid-like
systems is studied in various water-to-cement ratios using
the m parameter of Papanastasiou compared with viscoelas-
tic solid and liquid system behaviors. The Kelvin–Voigt
model in the classical continuum mechanics is applied
to investigate the rheology of cement paste in terms of
the m parameter and distance of particles in function of
water-to-cement ratio. Some conclusions and outlooks are
summarized and discussed at the end of the paper.
Theoretical background
Rheological flow of non-Newtonian fluid
In a general manner, the cement-based materials, fresh
cement paste, and fresh concrete are used to be considered
as a non-Newtonian fluid. Basically, the rheology of these
liquids depends on the formulation of concrete (nature
and granulometry of aggregates, water to cement ratio,
and effect of admixtures) and hydration process (Papadakis
Rheol Acta (2020) 59:47–61 49

et al. 1989; 1991; Nelson 1990; Ulm and Coussy 1998; a 10

Rixom and Mailvaganam 2002; Ramézani et al. 2014;
9
Jeong et al. 2013; Jeong et al. 2014; 2016; Jeong et al.
2019). To describe the rheological behavior, several semi- 8
m=100
empirical models have been developed to find a relation 7
m=50
m=10
between shear stress and shear strain rate after yield stress. m=5

Shear stress [Pa]

6 m=1
In non-Newtonian fluids, the most frequently used model m=0.5
in dealing with the behavior of concrete is the Bingham 5
model (Bingham 1922; Dufour and Pijaudier-Cabot 2005; 4
Ramézani et al. 2015) and it can be written as:
3
τ0
τ = τ0 + μγ̇ and η= γ̇ +μ where τ  τ0 (1) 2

Where, τ0 , γ̇ , μ, and η are the yield stress, the shear 1

strain rate, plastic viscosity, and apparent viscosity, respec- 0

0 2 4 6 8 10
tively. The Bingham model presents a perfect linear relation
Shear strain rate [1/s]
between the shear stress and shear strain rate. However,
b 10
for most of the non-Newtonian fluid flows, the unyielded m=100
and yielded zones cannot be easily distinguished and the 9 m=50
m=10
numerical modeling becomes possible if only the shear 8 m=5
m=1
stress is greater and equal to yield stress point (Chuta m=0.5
Apparent viscosity [Pa.s] 7
2018). To handle these difficulties, it is necessary to develop
numerical techniques to identify and describe the behav- 6

ior of the transition zone from yielded to unyielded zones. 5

This can be carried out by introducing a so-called continu-
4
ity parameter in Bingham’s model. In fact, Papanastasiou
(1987) was inspired by 3D von Mises criterion whose 3

application enables us to control and track randomly dis- 2

tributed yield material surfaces. Consequently, Papanasta-
1
siou proposed a simple and efficient modification in the
plastic Bingham model. The incorporation of this continu- 0
0 2 4 6 8 10
ous parameter in Eq. 2, which has an exponential function Shear strain rate [1/s]
around yield stress τ0 , is applied in Bingham’s model as the
Fig. 1 Papanastasiou–Bingham’s model with different m values (τ0 =
following: 5 Pa and μ = 0.5 Pa s) a Shear stress versus shear strain rate. b
Apparent viscosity versus shear strain rate
τ=
Bingham’s yield stress Papanastasiou’s

function multiplier
 
  
τ0 (1 − exp (−mγ̇ )) for viscous strain ˙ , which is a typical response of fluids.
  
Non-Newtonian fluid flow part (2) 1 1
+ μ γ̇ = σ and ˙ = σ (3)
   E η̄
Newtonian fluid flow part
and η = μ + τγ̇0 (1 − exp (−mγ̇ )) Where, , ˙ , σ , E, and η̄ are strain, strain rate, stress,
Young’s modulus, and viscosity, respectively. The spring
where, m is the regularization or continuous parameter of part for elastic solid and dashpot part for fluid in serial
unyielded and yielded zones. For Bingham–Papanastasiou’s configuration emphasize the Maxwell model for which
model: if m → 0, we arrive at the Newtonian fluids, strain rate is summation of spring part and viscous part. The
whereas for m  1, the flow would become the ideal illustration of Maxwell model is shown in Fig. 2a and the
Bingham fluids in Fig. 1. Therefore, the yield stress point constitutive model is expressed as following:
becomes more and more visibly clear.
η̄
Additionally, the continuum mechanics can also provide η˙ = σ + σ̇ (4)
the constitutive model in describing viscoelastic materials E
behavior (Mase and Mase 1999). Basically, there are Considering creep and relaxation tests, Maxwell model
Maxwell and Kelvin–Voigt models using spring for provides a time-dependent behavior related to viscous
instantaneous strain  related to solid behavior and dashpot element in terms of the creep–compliance function J (t) and
50
Fig. 2 Fundamental rheological behavior using spring and dashpot
elements: a Maxwell model and b Voigt–Kelvin model
relaxation time tR as following:
(t) = σ0 J (t) where J (t) = η̄1 + E1
σ (t) = 0 E(t) where E(t) = E exp(−t/tR ) (5)
and tR = Eη̄
This fundamental equation can be applied either to shear
stress or to uniform tension as shown in Fig. 2a and b.
Considering two elements, spring for elastic solid and
dashpot for viscous fluid in parallel, the Kelvin–Voigt model
is that the applied shear stress (or stress) is the summation
of the stress of the spring part and the other viscous part
(Fig. 2b). Consequently, the model is expressed as follows:
σ = E  + η̄ ˙ (6)
Considering creep and relaxation tests, the Kelvin–Voigt
model provides a creep–compliance function J (t) and
retardation time tR as follows:
(t) = σ0 J (t) where
η̄ (7a)
J (t) = E1 (1 − exp (−t/tR )) and tR = E the harmonic average radius between particles of radii a1
σ = 0 E (7b)
Setting the strain 0 as constant, the stress remains
constant. Interestingly, one can find a dimensionless term,
which is t/tR in both Maxwell and Kelvin–Voigt models.
This parameter is nothing else than effective time related
to dashpot element reaction time compared with the spring
reaction. This represents one interesting feature of non-
Newtonian fluid flow which could be triggered before or
after the yield stress. Intuitively, this dimensionless term
(t/tR ) is similar to that of Papanastaisou’s mγ̇ . Generally,
Papanastasiou’s dimensionless term can be applied to
describe various viscous behaviors of fluid around the yield
stress point. This means that when the system is about
to exceed yield stress, this activates the viscous part and
it gives rise to irreversible strain. This can present the
way of how the system would react when shear stress
remains constant like the creep test. One can observe that
when Papanastasious’s dimensionless term mγ̇ is small, the
Rheol Acta (2020) 59:47–61
system would react instantaneously, like a quasi-Newtonian
fluid. But, for large dimensionless term values, the viscous
features of the system are getting more important, and it
results in the quasi-viscoelastic solids.
Cement paste flow as a colloidal suspension
From a physical point of view, the fresh cement paste
can be considered as a suspension of cement particles of
different sizes in a fluid (water). The factors, which con-
tribute most to the overall nature of a colloidal system
like cement, are the particle size, particle shape and flexi-
bility, surface properties, particle–particle interactions, and
particle-solvent interactions. The particles have then an
effect on the rheological aspects such as yield stress and vis-
cosity (Roussel 2016). Due to dipole–dipole interaction in
cement colloidal suspension, van der Waals interaction force
F between particles is presented by the derivative of interpar-
ticle separation distance λ with respect to the interparticle
potential φ in Eq. 8a and 8b wherein the Hamaker constant
AH is a constant value according to microscopical points
of view. However, the Hamaker constant value depends on
the interparticle distance according to the continuum the-
ory. The last represents the effective Hamaker constant or
so-called retarded Hamaker constant.
AH a
ϕ=− (8a)
12λ
dϕ AH a
F =− = (8b)
dλ 12λ2
where, F is the attractive force, λ is the distance between
particles, AH (λ) is called retarded Hamaker’s constant. a is
and a2 .
According to the literature (Yang 2012), a colloid
suspension can be defined as a suspension of particles
smaller than 10 μm with three basic types of forces
that determine the rheological behavior, i.e., Brownian
force, colloidal force (van der Waals attractive force and
electrostatic repulsive force), and hydrodynamic forces
occurring during the settling or mixing. The Brownian
motion is usually used in colloidal science and engineering.
However, it does not appear as a valid criterion for the
cement suspensions due to the large size of the particles.
On the other hand, the large particles, due to their inertia,
produce more viscous forces. This means that the Brownian
forces are negligible compared with the viscous forces in
cementitious systems (Flatt 1999). In Houst et al. (2002),
the colloidal forces in the cement pastes are defined as a set
of forces called dispersion forces, electrostatic forces, and
steric forces. Among these three forces, only van der Waals
forces are the most important force “prevalent” (dispersion
Rheol Acta (2020) 59:47–61 51

force) (Bergström 1997; Roussel et al. 2007; Conte 2017).2 i.e., φm .3 φm is assumed to be equal to 0.6 in the present
In the literature (Flatt 1999), the effective Hamaker constant study. Additionally, the solid volume concentration of
for three basic mineral elements in cement suspension, i.e., cement paste φ and the specific surface area of particles in
calcite, oxide magnesium, and silicate, are estimated and cement paste can be defined as:
presented. All these values become nearly zero when the ρp − ρw
separation distance is greater than 1000 nm and therefore φ= (12)
ρc − ρw
van der Waals forces must be negligible. It is of much
where, ρp is the wet density of cement paste, ρc is the
importance to point out that the cement suspension initially
density of cement, and ρw is the density water, respectively.
contains the CSH weak links which are studied and they
In a general manner, the viscosity of a cement paste
are very weak links compared with the colloidal force
increases as its solid particles’ concentration increases (Guo
(Roussel et al. 2012). Afterward, there are several types of
et al. 2017). This phenomenon shows one interesting feature
non-contact interactions. For short distances, there are van
of colloidal suspension. There are several mathematical
der Waals force and electrostatic force resulting from the
expressions in dealing with the rheological issues in
adsorbed ions at the surface of particles. The magnitude
the literature. In Table 5, some outstanding models are
of the mentioned interaction forces mainly depends on
summarized (see Appendix for more details). To evaluate
the separation distance, and not exclusively on the size
the rheological properties, we can use the initial packing of
of particles. In the fresh cement suspensions, this can be
particles in fresh cement paste. Many authors have found
manipulated via the water-to-cement ratio with the same
out that there is a relation between the yield stress of cement
particles’ granulometry curve, i.e., particle concentration.
paste and solid volume concentration, i.e., particle size and
Let us have a look at the available analytical method of
distance between particles (Guo et al. 2017).
estimation of distance between grains in cement suspension.
In our study, the abovementioned analytical estimation
As a critical parameter of the behavior of suspensions
of separation distance (Eqs. 9, 10, and 12) will be
is the volume fraction of the suspended particles, when
applied including the assumption that all cement particle
the volume fraction of particle is sufficiently small, the
diameters are assumed to be identical and this determines
distance between particles is far from each other. In the
the separation distance. As pointed out before, we have
literature (Guo et al. 2017), the distance between particles
achieved the experiments on the cement paste with various
λ is calculated by two times of water coating thickness Tw
water-to-cement ratios to evaluate its rheological properties
between two particles:
using Bingham and Bingham–Papanastasiou’s models. By
We taking advantage of rheological properties of cement paste,
λ = 2 Tw where Tw = (9)
As we find the parameter m, which can be related to the
interparticle interaction force between two grains of cement
Where As and We are surface areas of particles in unit
and interparticle distance. Finally, the combined rheological
volume of cement colloidal suspension and volume of
model based on Maxwell and Kelvin–Voigt called a three-
excess water, respectively. The volume of excess water can
element model will be suggested to present fresh cement
be defined as below:
paste flow in function of water-to-cement ratio.
1 − φm
W e = W w − Vm where Vm = (10)
φm
where, Ww is the volume ratio of water-to-cement and Vm
Materials and experiments
is the minimum volume ratio. The latter parameter can be
In this section, the experiments of determination of
estimated based on maximum solid volume concentration,
rheological features of cement paste are presented. For
determining the impact of water in cement colloidal
2 The electrostatic forces (FES ) between cement particles can be either suspension, the ratio of water-to-cement is varied from 0.3
repulsive between particles of identical charge or attractive between up to 0.6, which are called P030, P035, P040, P050, P055,
particles of opposite charge. The evaluation of the magnitude of these
forces, whether attractive or repulsive, is complicated by the fact that 3 According to the literature, this value should be independent of
the medium is a highly concentrated electrolyte in which ion activities
particle size but it depends on ratio of water-to-cement. Basically, the
cannot be approximated (Hackley et al. 2001). The improved fluidity
value of φ depends on the size distribution and flow conditions (Dames
of concrete by adding the organic admixture is considered to be caused
et al. 2001) as well. [η]1 stands for the linear part factor of Taylor
mainly via the dispersion of solid particles. This comes from the
series expansion of relative viscosity as below (Wagner and Woutersen
electrostatic repulsive force due to the increase of the surface potential
1994):
caused by the admixture adsorbed to the surface of solid particles.
μ
Additionally, it also comes from the steric repulsive force (FSte ) ξ= = 1 + [η]1 φ + [η]2 φ 2 + ... + [η]m φ m + ... (11)
based on the interaction between the adsorption layers of admixture μ0
(Uchikawa et al. 1997). ξ is the maximum solid volume concentration of cement paste.
52 Rheol Acta (2020) 59:47–61

Table 1 Cement colloidal suspension with different water-to-cement

ratios

Materials P030 P035 P040 P045 P050 P055 P060

Cement (g) 450 450 450 450 450 450 450

Water (g) 135 157.5 180 202.5 225 247.5 270

and P060, respectively (Table 1). The fresh cement sample

preparation has been done without adding admixtures for all
experiments reported in the present paper. Firstly, all fresh
cement paste samples are analyzed via density variation,
packing fraction, and distance between particles in function
of water-to-cement ratio for every single specimen.
The experiments have been achieved using our available
rheometer in laboratory-based upon a predefined protocol
to determine the yield stress and the plastic viscosity.
Afterward, the extracted experimental outcomes have been
processed and analyzed by non-linear regression technique
using the Gauss–Newton algorithm. To describe the flow of
cement pastes, we use the rheological model of Bingham
and Bingham–Papanastasiou. By using the experimental
findings, we study the impact of water on the cement
colloidal suspension in terms of interparticle distance and
the related rheological features.
Cement colloidal suspension sample preparation
The samples are prepared in an airconditioned laboratory
with an average temperature of 25◦ C and relative humidity
of 50% using a mixer with a bowl volume of 5 l.
The samples are prepared from ordinary Portland cement
(CEM I) (Table 2).
The cement and water are poured into the mixer into the
bowl and mixed immediately at low speed for 1 min. Then,
the mixer is stopped for 90 s. During this time, the sidewall
of the bowl is scraped with a squeegee to remove any cement
adhering to the walls and it is placed in the middle of the
bowl. Then, the mixing is continued for 30 s at high speed
prior to set rheometer.
Table 2 Chemical composition of the ordinary Portland cement in
weight percent
CaO SiO2 Na2 O SO3 Al2 O3 Fe2 O3 MgO K2 O Others
60.84 13.26 10.05 3.59 3.42 3.14 2.35 1.17
Fig. 3 Presentation of granulometry analysis of applied cement for the
experiments in the present study: cumulative passing versus particle
diameter
Analysis of cement colloidal suspension
First of all, the density of each sample is determined using
the experiment. It is observed that the cement paste density
is roughly proportional to the inverse of the water-to-cement
ratio. To determine the distance between two particles, first,
packing fraction (solid volume concentration, φ) is calcu-
lated by the previously obtained densities of the cement
paste samples. The ordinary Portland cement density is
equal to 3.09 g/cm3 and its average particle size around
10.35–10.8 μm with 13,788 cm2 /cm3 for its specific surface
area. The granulometry analysis of the applied cement in
this study is presented in Fig. 3.
As pointed out earlier, all cement particles are assumed
to have the same size and their size is equal to the average
value of 10 μm highlighted in Fig. 3. Consequently, the
packing concentration (φ) can be calculated for every single
specimen. The results are plotted in Fig. 4a and b. According
to the experiments, maximum solid packing concentration
can be up to 55% for sample P030 and solid packing
concentration decreases with increasing water-to-cement
ratio (Fig. 4a). However, some authors confirm that this
value can reach 64% using vibration for uniform spheres as
solid particles (Roussel 2016).
Based on the relation in Eq. 9, the distances between
particles are calculated and presented in Fig. 4b. The solid
volume concentration has been obtained from experiments
on every single sample in Fig. 4a. By applying the average
value of solid volume concentration, the distance between
particles is assessed (Fig. 4b). It is observed that the
distance between particles quasi-linearly increases when
the water-to-cement ratio increases but decreases with the
2.18
concentration of solids. Also, the interparticle distance in
average would change from less than 0.5 μm for P030 up
Rheol Acta (2020) 59:47–61 53

a available measurements by means of 4-blade vane geometry

0.6
in the literature (Saak et al. 2001). In the present study, the
Cement paste
vane geometry is applied with a diameter of 16 mm height
Solid volume concentration

0.55 P030
of 25 mm for all experiments as shown in Fig. 5c. To mea-
0.5 P035 sure the rheological behavior, we prepare the mixture first
in the same way that the sample used for the colloidal sus-
P040
0.45 pension feature in the previous section. Once the mixture
is ready, it is introduced into the rheometer measuring cell.
P045
0.4 P050 The rheometer has a moving geometry that is attached to a
P055
motor, which rotates it. The rheological measurements are
0.35 P060 made during less than 10 min and 20 min for all required
preparations including sample preparation before experi-
0.3 ments. This is a period when the cement hydration is at the
0.25 0.3 0.35 0.4 0.45 0.5 0.55 0.6 starting point. As a result, one can assume that there is no
W/C significant change in the rheological aspects of the cement
b 2 paste at this stage.
The protocol of experiment consists of subjecting the
Distance between particles ( m)

Cement paste
cement paste at a shear rate of 500 1/s for 30 s called pre-
1.5 shear to avoid any memory effects, i.e., thixotropic effect
and also homogenization of microstructure in terms of any
agglomeration and/or segregation.4 The cement pastes are
1 left standing for 30 s (minimum time that is necessary to
wait for the first measurement) before being subjected to
increasing stress for 60 s. The measurement point is per-
0.5 formed every 0.1 s and experiments are carried out at every
single specimen. It is well worth noting that the decreasing
shear rate ramp is more adequate for cementitious samples
0 and, also, steady shear stress values cannot be recorded if
0.25 0.3 0.35 0.4 0.45 0.5 0.55 0.6
W/C
measurements are taken just after 0.1 s from the application
of the shear rate. This last is relevant because models like
Fig. 4 Presentation of cement colloidal suspension features. a Solid Bingham are valid for steady measurements.
volume concentration of fresh cement pastes versus water-to-cement
ratio. b Average distance between particles versus water-to-cement
ratio Results of cement paste flow behavior

The rheological behaviors of all samples (P030, P035,

to more than 2 μm for P060. In the next sub-subsection, we
focus on the rheology of cement pastes.
Rheology of cement pastes
Measurement protocol
To study the rheology of cement pastes, we use a “Rhe-
olabQC” rotational rheometer available at the IRC-ESTP
laboratory (Fig. 5a and b). This rheometer provides the
rheological behavior. The dimension of the cup (height of
72 mm and diameter of 27 mm) is suitable in order to ensure
the simple shear condition is accomplished, specifically for
non-Newtonian samples (Banfill 2003; 2006). There are
several configurations of mobile geometry adapted to mea-
sure the rheological behavior of different materials. Among
these geometries, the 4-blade vane geometry is highly rec-
ommended for cement-based materials and there are some
P040, P045, P050, P055, and P060) are determined using
the rheometer. At least four experiments are performed
per specimen type. The number of achieved experiments
4 In the colloid science, the property of thixotropy is the most famous
rheological feature, which is found in many complex materials,
especially colloidal systems (Wallevik 2005). It is associated with
changes in rheological properties with time, even when the applied
stress or strain rate is kept constant. The decrease of viscosity with
time by application of shear and the recovery of viscosity when the
material is at rest. Besides, viscosity changing is reversible. Based on
the microstructural point, the thixotropy for cement paste comes from
the break of flocculation or connected particles. The thixotropy of
cementitious materials can be considered the coagulation of particles
when shearing is not applied to the cement particles. Once the external
shearing is applied to the cement paste, the particles will be separated.
It is noted that the reversible behaviors of coagulation, separation,
and coagulation of cement particles contribute to thixotropic behavior
of cement paste. The decrease of viscosity of cement paste during
the mixing with time is contributed by the change of microstructure
(Wallevik 2003).
54 Rheol Acta (2020) 59:47–61

Fig. 5 Presentation of
rheometer for measurement of
rheological feature of cement
paste: a rheometer global view,
b rheometer cup, and b vane
geometry used for our cement
suspension samples

usually depends on the water-to-cement ratio. In Fig. 6, the According to the experimental results, as expected, zone
experimental outcomes of rheological behavior of P050 are II becomes less important when the water-to-cement ratio
shown. As shown in Fig. 6, we can see that the flow curve of is increasing. Therefore, the plastic viscosity of the sample
the fresh cement paste at the beginning is divided into three is decreased as shown in Fig. 7. For the sample P035, the
flow zones before the yield stress.
Three zones are explained as follows:
– Zone I: This is the first zone where the rheological
experiment starts, some disturbances can be observed.
This is nothing else than the initial positioning in the
fresh cement paste inside the rheometer cell.
– Zone II: This is the second zone, a non-flow zone or
unyielded zone, where the fluid remains immobile. The
non-flow zone corresponds to the solid-like system like
the spring element in the Maxwell/Voigt–Kelvin model
and the dashpot element has not activated yet.
– Zone III: This is the third zone where the system is
nearly close to the yield stress point or it may exceed
this zone. According to rheological model, this zone can
be described using the dashpot element only.
a

Fig. 6 Presentation of shear stress versus shear strain rate of sample Fig. 7 Rheological behavior of fresh cement paste with different
P050 highlighting three distinct zones around the yield stress point water-to-cement ratios extracted from the classic Bingham model
Rheol Acta (2020) 59:47–61 55

sample behaves as a solid-like system, which can be Table 3 Rheological parameters of cement pastes using Bingham’s
compared with brittle materials until the yield stress point model
and fluid-like after that point. For the sample P060, Name Bingham’s model parameters
rheological behavior is very different from P035. It means
that the system is nearly liquid-like and then it starts flowing Sample Yield stress, Viscosity, Correlation
without a clear-cut yield stress point. It is easy to understand τ0 in Pa μ in Pa s coefficient, in R 2
that more water is introduced in the system and less solid
P030 1857 0.94 0.96
part can be found.
P035 558 0.61 0.98
The rheology experiments have been carried out and
modeled using firstly classic Bingham’s - in Fig. 7 and P040 218 0.58 0.94
secondly Bingham-Papanastasou’s model in Fig. 8. The P045 113 0.41 0.92
rheological features, i.e., yield stress and plastic viscosity, P050 95 0.35 0.92
are determined using the classic Bingham model in Table 3
and Bingham–Papanastasiou model in Table 4 in zone III. P055 61 0.24 0.93
In Table 3, we can observe the curve modeling by means P060 42 0.19 0.93
of Bingham’s model and least square fitting technique
alongside the experimental outcomes. As seen in Fig. 7, the
model is quite well adapted when the cement pastes are viscous but they are less suitable when the cement pastes are
very fluid.
In Fig. 8, the Bingham–Papanastasiou model outputs
are plotted. Clearly, we see that Bingham–Papanastasiou’s
model is fairly adapted compared with Bingham’s model.
As presented in Tables 3 and 4, the correlation coefficients
give rise to the better values for the Bingham–Papanastasiou
model rather than the Bingham model for nearly all water-
to-cement ratios. However, the correlation coefficient for
P030 using Bingham’s model is better than Bingham–
Papanastasiu’s model (Tables 3 and 4). This comes from
the fact that the water-to-cement ratio is less than that of
the other case studies and the fluid turns to be more solid
rather than fluid. In this condition, the Bingham model fits
better rheological behavior. The correlation coefficient for
P035 is nearly identical between the two abovementioned
models. We can also see in Tables 3 and 4 that the decrease
a of the yield stress with water-to-cement ratio increase is an
expected value obtained with both models.

Table 4 Rheological parameters of cement pastes using Bingham–

Papanastasiou’s model

Name Bingham–Papanastasiou’s model parameters

Sample Yield stress, Viscosity, m Correlation

τ0 in Pa μ in Pa s in s coefficient, R 2

P030 1799 1.02 38.95 0.89

P035 558 0.69 8.79 0.97
P040 252 0.53 1.37 0.98
P045 158 0.35 0.15 0.98
P050 134 0.29 0.11 0.97
b
P055 87 0.19 0.08 0.98
Fig. 8 Rheological behavior of cement paste with different water-to- P060 65 0.15 0.04 0.99
cement ratio determined from the Bingham–Papanastasiou model
56 Rheol Acta (2020) 59:47–61

Results and discussion
As discussed in the previous section, even if the variations
of the yield stress and the plastic viscosity are almost
similar among the two mathematical models, it can be found
out that the best modeling in describing the rheological
behavior of cement pastes can be found out for Bingham–
Papanastasiou’s model. This can not only well describe the
behavior of cement pastes whatever water-to-cement ratio
is, but also it is very well suitable in describing the variation
of the yield stress at various strain rates. Indeed, in Fig. 9a,
the yield stress changes are now shown in function of water-
to-cement, in where the yield stress decreases for higher
water-to-cement ratios.
Besides, these two models can also be used as a function
of the distance between particles. The distance between
particles in function of water-to-cement ratio is already
presented in Fig. 9b. The latter graph is combined with the
yield stress obtained by Bingham–Papanastasiou’s model in
Fig. 9a to provide the relation between the yield stress and
interparticle distances. According to the results in Fig. 9b,
we can observe that the increase in the distance between
particles in the cement paste decreases the yield stress
and plastic viscosity. Now, let us look at other parameters,
which play a key role in the sample behavior, i.e., m and
interparticle distance. In Fig. 10a and b, the parameter m
in Bingham–Papanastasiou’s model is plotted versus water-
to-cement ratio and distance between particles in the fresh
cement paste, respectively. Here, it is noticed that the
distance of interparticle has been obtained using the average
particle diameter as explained in the previous sections. Once
again, we can notice the same trend in Fig. 9.
According to the experimental findings for the fresh
cement paste, we can conclude that the increase of water-
to-cement ratio leads to the decrease of the concentration of
solids and increases the distance between the particles. On
the other hand, the observed parameter m that we have found
out from the Bingham–Papanastasiou model also decreases
with the increase of water and the distance between

a 102
a 2000

Bingham-P Bingham−Papanastasiou
1
10
1500
Yield stress [Pa]

Parameter m

0
10
1000

−1
10
500

−2
10
0 0.25 0.3 0.35 0.4 0.45 0.5 0.55 0.6
0.25 0.3 0.35 0.4 0.45 0.5 0.55 0.6
W/C
W/C
b 102
b 2000
Bingham−Papanastasiou
Bingham-P
1
10
1500
Parameter m
Yield stress [Pa]

0
10
1000

−1
10
500

−2
10
0 0 0.5 1 1.5 2
0 0.5 1 1.5 2 Distance between particles (μm)
Distance between particles ( m)
Fig. 10 a Parameter m of cement pastes versus water-to-cement ratio
Fig. 9 a Yield stress versus water-to-cement ratio. b Yield stress (W
C ). b Parameter m of cement pastes versus distance between two
versus distance between particles grains in the cement paste mixture
Rheol Acta (2020) 59:47–61
a b c
Fig. 11 Illustration of three-element rheological models for cement
colloidal suspension from the Kelvin–Voigt model for the solid-like
system to quasi-Newtonian fluids according to the m parameter (D
stands for distance between particles): a Zener model known as
standard linear solid model, b Jeffreys model, and c single dashpot
model
particles. This parameter that varies with the distance
between particles could describe physical or chemical
phenomena inside the fresh cement pastes as a colloidal
suspension.
The experimental outcomes show an exponential trend as
a function of distance and it is very similar to the dispersion
force observed in the literature. This colloidal force depends
on retarded Hamaker’s constant, which is very important
when the cement particles are very close to each other (less
than 1 μm), whereas it decreases rapidly and becomes nearly
zero when the particles move away (more than 1 μm). From
this observation, we can evaluate the retarded Hamaker
constant/colloidal attractive force, which is linked between
the shear stress and the distance between particles. It can be
described as a multi-disciplinary problem as illustrated in
Fig. 11a, b, and c:
– Colloidal suspension (water-to-cement ratio  0.35):
According to Fig. 11a, it can be found that cement paste
can be described like a viscoelastic solid-like system
when m is more than 10. It means that the distance
between particle is less than 1 um where attractive
van der Waals forces could be too big and strong and
then the system behaves like a solid. The system can
be explained using a three-element solid Kelvin–Voigt
model (Zener model)
– Non-Newtonian fluid (0.35  water-to-cement ratio
< 0.45): When adding more water in the sample, the
distance between particles starts to increase and the
attractive and repulsive forces begin to decrease. That
phenomenon may be illustrated by replacing the spring
57
by dashpot in Fig. 11b. Basically, it is not always clear
how such a system will behave around the yield stress
point and the way the yield stress happening due to
the dashpot element effective time. The system can
be explained using a three-element fluid Kelvin–Voigt
model (Jeffreys model),
– Quasi-Newtonian fluid (water-to-cement ratio 
0.45): The abovementioned system appears when the m
parameter is less than 1. In this case, the interparticle
distance becomes too big and then any colloidal force
cannot be found out. The system is Newtonian fluid as
depicted in Fig. 11c.
In the present study, the samples P040 as non-Newtonian
fluid and P050 as quasi-Newtonian fluid are chosen for
comparison of numerical simulations with experiments. To
achieve that, the Plexiglass box of the total length of 16 cm
and height of 17 cm is made for cement paste flow
experiments. This makes it possible to observe cement paste
flow very carefully. Based on the Bingham–Papanastasiou’s
parameters obtained previously for P040 and P050, their
rheological behaviors before and beyond yield stress have
been successfully implemented in the finite element code
for simulation of two-phase non-Newtonian flow, i.e.,
cement paste and air. The fluid flows extracted from the
simulation are compared with the experimental fluid flows
for P040 and P050 as shown in Fig. 12a, b, c, and d. The
numerical simulation is performed using the two-phase flow
framework for which the red color presents the air and the
blue color presents the cement paste sample. The white
zones in Fig. 12b and d deal with the boundaries wherein
there is no fluid flow. The contact angle between the fluid
and wall of the box is 90◦ , allowing cement paste to flow
without friction. Additionally, the mesh size is less than
0.25 cm] and the runtime is less than 10 h for P040 and 5 h
for P050 using direct parallel solver on a cloud server of 16
CPUs including 128 Gb.
For comparison, let us focus on the sample flows at 1 s
for P040 in Fig. 12a and b and P050 in Fig. 12c and d: it can
be easily observed that the simulation of cement paste flow
for P040 and P050 matches quite well with the experiments
(Fig. 12a and c).
Conclusion and perspectives
In the present paper, the rheological behaviors of fresh
cement paste with various water-to-cement ratios are stud-
ied using a multi-disciplinary approach, i.e., (1) colloidal
suspension based on the distance between particles, (2) rhe-
ology using Bingham’s and Bingham–Papanastasiou’s mod-
els highlighting role of the m parameter, and (3) continuum
mechanics by Maxwell and Kelvin/Voigt models.
58 Rheol Acta (2020) 59:47–61

Fig. 12 Comparison of
numerical simulations using
Bingham–Papanastasiou’s
model with experiments after 1 s
of cement paste flow: a and b
Non-Newtonian fluid flow for
sample P040; c and d
Quasi-Newtonian fluid flow for
sample P050

a b

c d

First of all, the distance between anhydrous particles
is estimated and then the attractive van der Waals forces
are estimated in function of water-to-cement ratio. The
experiments of the rheology of cement paste samples are
performed and the yield stress and viscosity as well as the
m parameter are obtained at every single water-to-cement
ratio. Different water-to-cement ratios present a different
type of flow. Consequently, we can classify the fresh cement
paste as a colloidal suspension, the non-Newtonian fluid
flow as a three-element Kelvin-Voigt model, and the quasi-
Newtonian fluid flow in function of water-to-cement ratio.
Lastly, the numerical feature of m and the transition zone
around yield stress are understood and enlightened across
various types of fresh cement pastes.
Appendix: Different models in describing
the viscosity of suspensions
Different models in describing the viscosity of suspensions
are summarized in Table 5 (Chuta 2018). In Table 5, φm is
the maximum packing fraction (0  φ < φm < 1).
For the larger solid fractions where the elements
significantly interact (>2%), we can use the Mooney,
Krieger–Dougherty, and Quemada’s mathematical models
which are addressed in Table 5.
Nomenclature
Constants

Acknowledgments The authors gratefully acknowledge the anony- [η]1 constant of linear part of Taylor series expansion
mous reviewers whose comments and suggestions improved the of relative viscosity
content of the present paper. η¯1 first viscosity in Fig. 11 (Pa s)
η¯2 second viscosity in Fig. 11 (Pa s)
Funding information The authors received financial support from η̄ viscosity in Fig. 2 and related equations (Pa s)
École Française du Béton (https://www.efbeton.com/). τ0 non-Newtonian fluid yield stress (Pa)
Rheol Acta (2020) 59:47–61 59

Table 5 Different models in describing the viscosity of suspensions

Model name Expression Year Reference

   2
φ
Eilers μe = μ0 1 + 12 [η]1 1941 Eilers (1941)
1− φφm
  
φ
Robinson μr = μ0 1 + [η]1 φ 1949 Robinson (1949)
1− φm
  
[η]1 φ
Mooney μm = μ0 exp 1951 Mooney (1951)
1− φφm

−[η]1 φm
Krieger-Dougherty μk = μ0 1 − φφm 1959 Krieger and Dougherty (1959)

−2
Quemada μq = μ0 1 − φφm 1978 Quemada (1978, 1998)

ξ = μμ0 relative viscosity ( Pa.s

Pa.s ) Vm minimum void ratio]
A(λ, a) retarded Hamaker’s constant (N m) We volume of excess water (m3 )
E Young’s modulus or modulus of elasticity (Pa)
R2 correlation coefficient Ww volume ratio of water-to-cement
tR relaxation time (s) ˙ strain rate for continuum mechanics application
η apparent viscosity (Pa s) ( 1s )
μ plastic viscosity (Pa s) σ̇ stress rate for continuum mechanics application
( Psa )
 strain for continuum mechanics application
Scalar quantities
σ stress for continuum mechanics application (Pa)
γ̇ shear strain rate ( 1s )
W
C water-to-cement ratio
λ distance between particles (m) Vector quantities
μ0 pure fluid phase with viscosity (Pa s)
μe Eilers’ viscosity definition (Pa s) F (λ, a) colloidal force (N)
μk Krieger–Dougherty’s viscosity definition (Pa s)
μq Quemada’s viscosity definition (Pa s)
μm Mooney’s viscosity definition (Pa s) References
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