Employing Natural Bentonite Clay as Partial Replacement

of Mineral Filler in Asphalt Mixtures

Mousa Ibraheem Bani Baker 1; Raed Mohammad Abendeh 2; and Turki Al Suleiman Obaidat 3

Abstract: This study aimed to investigate the performance of asphalt mixtures after natural bentonite clay partial replacement of mineral filler
portion of aggregates. Different bentonite contents were used to replace the mineral filler by total weight of its portion of total aggregates,
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namely, 5, 10, 15, and 20%; additional bentonite contents were conducted for the stability test, namely, 25 and 30%. Marshall stability, flow,
bulk density, hydraulic conductivity, and indirect tensile strength (ITS) tests were performed. Results showed that replacing mineral filler by
natural bentonite clay in asphalt mixtures leads to the increase of density and stability, which increased to 11.57 kN for mixtures containing
15% bentonite (compared with 9.17 kN for the control specimen), with 23% loss when soaked with water for 24 h. Results indicate an increase
in both flow and ITS values and reduction in hydraulic conductivity of the modified mixtures compared with control specimens. DOI: 10.1061/
(ASCE)MT.1943-5533.0002375. © 2018 American Society of Civil Engineers.
Author keywords: Bentonite; Mineral filler aggregates; Marshal stability and flow; Asphalt mixtures; Hydraulic conductivity; Indirect
tensile strength; Bitumen–mineral interface.

Introduction by controlling draindown, as well as to provide improved adhesion

Asphalt (or bitumen) is used in road pavement as the binder of ag-
gregates worldwide. Therefore, asphalt pavements must sustain
heavy loads and environmental circumstances for a satisfactory time.
The most substantial restrictions of unmodified asphalts are high-
temperature rutting and low-temperature cracking (Kamiya et al.
2001). In order to enhance the base asphalt binder to improve high-
temperature performance, low-temperature cracking, and aging
resistance of asphalt mixtures, different types of materials have been
used as admixtures to extend the service life of pavements by
prevention of cracks in pavements (Sun et al. 2017; Ozen 2011).
Many researchers indicated that using fiber may improve cohesion
properties of asphalt mixes in medium temperature and reduces
fatigue-based damages for asphalt mixes during serving periods.
Similarly, other researchers studied the effect of two additives,
namely, waste plastic and traditional polymers, on fatigue function
of asphalt mixes (Shafabakhsh et al. 2015). Also, hydrated lime is
widely used throughout the world as an antistrip additive due to its
superior performance in decreasing the moisture sensitivity of warm-
mix asphalt (Button and Epps 1983). Furthermore, using polymer-
modified binders indicated that proper use of polymer and/or other
additives can allow the use of higher air voids (for drainage, and
hence prevent stripping in the underlying layer) and higher
asphalt binder content (for durability, and hence prevent raveling)
1
Assistant Professor, Dept. of Civil and Infrastructure Engineering,
Al-Zaytoonah Univ. of Jordan, P.O. Box 130, Amman 11733, Jordan
(corresponding author). Email: m.banibaker@zuj.edu.jo
2
Assistant Professor, Dept. of Civil and Infrastructure Engineering,
Al-Zaytoonah Univ. of Jordan, P.O. Box 130, Amman 11733, Jordan.
Email: r.abendeh@zuj.edu.jo
3
Professor, Dept. of Civil and Infrastructure Engineering, Al-Zaytoonah
Univ. of Jordan, P.O. Box 130, Amman 11733, Jordan. Email: president@
zuj.edu.jo
Note. This manuscript was submitted on July 10, 2017; approved on
February 9, 2018; published online on May 26, 2018. Discussion period
open until October 26, 2018; separate discussions must be submitted for
individual papers. This paper is part of the Journal of Materials in Civil
Engineering, © ASCE, ISSN 0899-1561.
and greater resistance to aging binder (Kandhal and Mallick 1998).
Nevertheless, most asphalt and modified asphalts cannot meet re-
quirements of both high-temperature stability and low-temperature
cracking resistance simultaneously (Zhang et al. 2016). Hence, other
types of additives were employed to enhance the performance of
asphalt mixtures such as nanoclay-modified mixtures, which were
found to have more rutting resistance than the conventional mixtures
(Iskender 2016). Nanoclay has a high surface area of 700–800 m2 =g
due to separation of clay discs from each other, which results in a
thorough interface between the nanoclay and the bitumen. Nanopar-
ticles, nanosilica, and nanotubes may also be added to the mixture to
increase the viscosity of asphalt binders and to improve rutting and
fatigue resistance of asphalt mixture materials (Yang and Tighe
2013). Additionally, in order to improve the rutting resistance
and low-temperature cracks of the modified asphalt, bentonite
clay and organically modified bentonite were utilized to enhance
and strengthen the asphalt binder (Zare-Shahabadi et al. 2010).
Moreover, bentonite clay may lead to a relative increase in indirect
tensile strength (ITS) and resilient modulus of asphalt mixtures
(Ziari et al. 2014).
Nowadays, mineral fillers are essentially characterized by their
ability to stiffen the bitumen. This clarifies that the main role for the
filler is to thicken the bitumen film. This effect was recognized
by Rigden (1947) of the British Road Research Laboratory in
1947 to be linked to the volume fraction of the filler and to be well
correlated with its overall porosity (Lesueur et al. 2017). Those
researchers presented results on the effect of increasing amounts
of filler in two different mixture formulas, a regular AC-16 and
an open-graded BBTM 11A. Two fillers were compared, limestone
filler (LF) with Rigden air voids of 30.2% and hydrated lime (HL)
with Rigden air voids of 61.9%. For both formulas and regardless of
the type of filler, the modulus versus filler content curves exhibited a
well-defined maximum. The filler content at which the maximum
was found was strongly filler dependent, with HL formulas peaking
at 4% by weight and LF formulas peaking at 10% by weight.
Natural clays like bentonite are not currently used as asphalt
additives. In fact, aggregate specifications eliminate aggregates
having too high of a clay content. The reason for this is that clay

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 Table 1. Gradation of aggregates
Aggregates type and
Sieve size Specification Percent Cumulative Percent passing their percentage
(opening mm) limits (% passing) retained percent retained at midpoint of total aggregates
3=4 in. (19.5 mm) 100 0 0 100 Coarse aggregates (70%)
1=2 in. (12.5 mm) 80–100 10 10 90
3=8 in. (9.5 mm) 56–80 22 32 68
No. 4 (4.75 mm) 35–56 23 55 45
No. 8 (2.36 mm) 23–38 15 70 30
No. 20 (0.85 mm) 13–27 10 80 20 Fine aggregates (25%)
No. 40 (0.425 mm) 8–12 10 90 10
No. 200 (0.075 mm) 2–8 5 95 5
Pan — — 100 0 Mineral filler (5%)
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creates a mineral coating on the aggregate and the hot asphalt then Asphalt
binds to the clay instead of the aggregates below. The resulting mix
One penetration grade of asphalt 85=100 obtained from the Jordan
is very prone to moisture damage because the water would then
Petroleum Refinery Company in Zarqa, Jordan, was used in this
easily displace the clay particles, and hence the binder, from the
research because it is commonly used in flexible pavement con-
aggregate surface. In this research, the performance of modified
struction in Jordan. Table 4 presents the physical properties of this
asphalt mixtures by partial replacement of the mineral filler portion
asphalt. Following the test processes outlined in ASTM D5 (ASTM
of aggregates with natural bentonite clay is investigated.
2013), ASTM D70 (ASTM 2009), ASTM D113-99 (ASTM 1999),
ASTM D36 (ASTM 2014), and ASTM D92 (ASTM 2016).
Materials
Bentonite
Aggregates
Natural bentonite clay from the Al-Azraq area of Jordan that passes
A local limestone aggregate brought from the Al-Hizam quarries of Sieve No. 200 (sieve size 0.075 mm) with bulk specific gravity of
Amman, Jordan (known for its light weight compared with other 2.62 g=cm3 , 8% moisture content, 420 m2 =g average specific sur-
limestone aggregates) was used in this research. The Jordanian face area, and 190% water absorption by weight was used in this
Ministry of Public Works and Housing gradation specifications research. The chemical composition of the used bentonite clay is
(MPWH 2010) were employed. Table 1 illustrates the gradation given in Table 5. The collected samples were subjected to an X-ray
of aggregates, while Table 2 shows the tested compositions of coarse diffraction (XRD) test for mineral characterization. Separation of
aggregates, fine aggregates, mineral filler, and bentonite, and Table 3 the clay size fraction was accomplished by using Atterberg’s
summarizes the aggregate properties used in the research, the tests method (Khoury 2002; Khoury and Al-Zoubi 2014; Poppe et al.
procedures are outlined in ASTM C127 (ASTM 2015b) and ASTM 2001). H2 O2 and HCOOH (acetic acid) were added to 10 g of the
C128 (ASTM 2015a). crushed sample and left for 1 night to liberate the organic matter.
After washing the sample with distilled water, NH4 OH was added
Table 2. Tested compositions of coarse aggregates, fine aggregates, and left for 1 night to remove any siliceous cement. After washing,
mineral filler, and bentonite
Bentonite partial Mineral Coarse Fine Total
Table 4. Properties of the Jordanian petroleum refinery asphalt
replacement of Bentonite filler aggregates aggregates mass
miner filler (%) (g) (g) (g) (g) (g) Properties Test method Test result
0 0 55 770 275 1,100 Penetration at 25°C (1=10 mm) ASTM D5 85=100
5 2.75 52.25 770 275 1,100 Ductility at 25°C (cm) ASTM D113 100
10 5.5 49.5 770 275 1,100 Specific gravity at 25°C ASTM D70 1.01
15 8.25 46.75 770 275 1,100 Softening point (°C) ASTM D36 49
20 11 44 770 275 1,100 Flash point (°C) ASTM D92 235
25 13.75 41.25 770 275 1,100 Fire point (°C) ASTM D92 249
30 16.5 38.5 770 275 1,100 Solubility in trichloroethylene (%) — 99

Table 3. Properties of aggregates

Aggregate type Apparent
(limestone) Al-Hizam Test Bulk specific gravity specific gravity Absorption
quarries, Jordan designation [Gsb ¼ A=ðB − CÞ] [Gsa ¼ A=ðA − CÞ] [% ¼ ðB − AÞ100=A]
Coarse ASTM C127 2.50 2.52 4.5
Fine ASTM C128 2.47 2.485 7.0
Mineral filler ASTM C128 2.515 2.534
Note: A = mass of oven-dried aggregates in air (g); B = mass of saturated surface-dry (SSD) aggregates in air (g); and C = mass of submerged aggregates in
water (g).

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 Table 5. Chemical analysis by X-ray fluorescence of Al-Azraq, Jordan, counts (intensity) as shown in Fig. 1, which also indicates that the
natural bentonite clay natural clay bentonite used in this research was impure clay con-
Oxide Percent sisting of smectite montmorillonite with amounts of illite, kaolinite,
quartz, dolomite, and calcite.
SiO2 53.11
Al2 O3 16.84
Fe2 O3 9.15
MgO 4.4
Test Methods
CaO 0.45
Na2 O 0.91 Marshall Stability and Flow of Asphalt Mixtures
K2 O 2.32
TiO2 1.7 Marshal stability, flow of asphalt mixtures [ASTM D1559 (ASTM
MnO 0.05 1989)], air void contents, and bulk density of saturated surface-dry
Loss on ignition 10.23 asphalt mix samples [ASTM D2726-11 (ASTM 2011)] were per-
formed by mixing limestone aggregate with bitumen used in this
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research to obtain the optimum binder content (OBC) that satisfies

the sample was poured into the Atterberg cylinder, which was
then filled with distilled water to 20 cm height. A dispersant agent
(three to five drops of 10% sodium hexametaphosphate) was added.
According to Stokes’s law, the clay size (less than 2 μm) was
removed after 14 h from the bottom opening of the Atterberg cyl-
inder. Random slides were prepared by packing and pressing the
powdered sample in the window of the aluminum holder. Oriented
slides were prepared by dropping the suspended clay on the glass
slides using a pipette (four different air-dried samples were pre-
pared, the first one was normal without heating, the second was
heated at 350°C, the third was heated at 550°C, the fourth was gly-
colated overnight at 80°C and heated to 550°C for 2 h). The samples
were X-rayed using Cu-Kα radiation with a scan range of 2–60°2θ.
A compact X-ray diffractometer system (Philips XRD system,
Netherlands, whose basic components are a PW 1830 HT gener-
ator, a PW 1050 goniometer, PW 3710 control electronics, and
X-Pert system software) was used. For clay patterns, data were col-
lected and results were presented as peak positions at 2θ and X-ray
the design criteria requirements for medium traffic conditions (most
of roads in Jordan are city roads, therefore designed according to this
criteria) in terms of stability > 5.338 kN (544.1 kg), flow = 8
to 16 quarter millimeter, 0.25 mm (0.01 in.), density>2.1 g=cm3 ,
air voids ¼ 3–5%, the voids in the mineral aggregate ðVMAÞ > 14%,
and the voids filled with asphalt ðVFAÞ ¼ 65–78%. Fifty blows were
applied on each end of the specimen. OBC was found to be 5.5% by
weight of total mixture, and therefore it was employed in specimen
preparation (101.6-mm diameter) and the stability correction factor
for thickness was used to obtain the standard stability thickness
of 63.5 mm. Natural bentonite clay was used in this research to par-
tially replace the mineral filler part of aggregates by weight in the
asphalt mixture with different contents starting from 0% (control
sample), 5, 10, 15, and 20%; additional bentonite contents were
conducted for stability test, namely, 25 and 30%. The values are
the average of three tested specimens for each bentonite content.
The mixing process involved preparation of aggregates accord-
ing to the gradation as given in Table 1 after drying at 105°C; the

Fig. 1. Representative XRD patterns of oriented samples for Al-Azraq, Jordan, natural bentonite clay.

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Fig. 2. Permeability testing setup.

natural bentonite clay was also dried at 105°C. Then mineral filler
was replaced by bentonite clay by weight, after which all parts were
mixed together manually (each sample was prepared separately to
assure accuracy of results). The aggregates–bentonite mix was
introduced to the bowl first, then asphalt (heated at 160°C) was
added to the bowl and mixed manually with aggregates–bentonite
mixture at mixing temperature of 165°C for 5 min.

Hydraulic Conductivity
To measure the vertical permeability of the core samples, a simple
design was prepared at the laboratory using the constant head
method according to ASTM D2434-68 (ASTM 2006). The setup
consisted of an air compressor equipped with a pressure gauge, per-
meability cell, containment cylinder (pressure cell), rubber mem-
brane, water release valve, outlet reservoir, and graduated cylinder
as illustrated in Fig. 2. The sample was fixed between two plates
connected to an aluminum pipe that allows water to flow thorough
the sample. Porous stones were placed between the plates and the
sample on the top and bottom of the specimen. The specimen was
wrapped carefully and tightly with rubber membrane to direct the
flow vertically through the tested specimens. An air compressor
was used to compress water in the pressure cell, which was con-
nected to the permeability cell in both axial (through the sample)
and horizontal directions to create confining pressure around the
tested sample. Values were the average of three tested specimens
for each bentonite content.

Indirect Tensile Strength

An indirect tensile strength test of cylindrical asphalt mixture sam-
ples using a splitting device following ASTM D6931 (ASTM 2007)
was conducted as shown in Fig. 3. This method consists of applying
a diametric compressive force at a constant rate of 50 mm=min at
25°C along the length of a cylindrical specimen until failure occurs.
The following formula was applied to calculate indirect tensile
strength: ITS ¼ 2,000Pmax =πDt, where ITS is the indirect tensile
strength (kPa), Pmax is the applied load at failure (N), D is the diam-
eter of specimen (mm), and t is the specimen thickness (mm).
Results and Discussions
Marshall Stability and Flow
Fig. 4 shows the density with bentonite variation for asphalt mix-
tures. The density increased with increasing the amount of bentonite
Fig. 3. Indirect tensile strength testing equipment.
and reached its maximum when bentonite content was 15%, which
coincides with 2.188 g=cm3 . The density increase was due to the
increase of bentonite in the mixture, which has a higher specific
gravity than mineral filler. Based on the properties of aggregates
listed in Table 3, the aggregates tend to be on the lighter weight
side; this justifies the low specific gravity of the mixtures. Density
decreased when bentonite content increased content over 15% be-
cause the higher content of bentonite clay in the mixture separates
the aggregates in the specimen.
Air voids and VMA reached their minimum values when
bentonite content was 15% with 3.5 and 15.67%, respectively, as
seen in Figs. 5 and 6. Moreover, for modified mixtures with 15%
bentonite clay the VFA reached its maximum as shown in Fig. 7.

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 Fig. 4. Percentage of bentonite versus density (g=cm3 ).
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Fig. 5. Percentage of bentonite versus air void (%).
Fig. 6. Percentage of bentonite versus VMA (%).
The average value of three specimens were used for each mixture
for stability analysis. Fig. 8 shows the results of original stability;
then, to test specimens in severe environmental conditions, retained
stability was tested after soaking the samples in water for 24 h, the
results of which are shown in Fig. 9. The soaking process included
soaking the samples in a water bath at 25°C for 24 h to simulate
severe conditions, then the samples were soaked in a water bath
at 60°C for 30–40 min. It can be noticed that stability increased
by increasing bentonite content and reached a maximum value of
11.57 kN when the modified mixture contained 15% bentonite
compared with 9.17 kN for the control specimen, a 26% improve-
ment. Stability of modified mixtures decreased with increasing ben-
tonite clay content over 15%, which is also consistent with the trend
of density values for a modified mixture with bentonite clay, which
might be a result of reduction in adhesion of bitumen to aggregates
and separation of the aggregates in the specimen. Moreover, a
© ASCE 04018167-5
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Fig. 7. Percentage of bentonite versus VFA (%).
Fig. 8. Percentage of bentonite versus original stability.
Fig. 9. Percentage of bentonite versus retained stability.
higher content of bentonite clay appears to reduce dispersion of ben-
tonite clay particles, which results in reducing physical properties of
asphalt mixtures. The loss in retained stability (Fig. 10) varied from
10.8% for the control sample to 23% for samples containing 15%
bentonite. However, all specimens containing bentonite clay for
both original and retained stability as seen in Fig. 11 meet the re-
quirements for stability of an asphalt mixture as per ASTM D1559.
Fig. 12 shows that flow values of asphalt mixtures increased by
increasing the content of bentonite in the modified mixture; they
reache 4.4 mm for 10% and 3.85 mm for 15% bentonite content.
Soaking specimens in water for 24 h increased the flow values
(Fig. 13). However, for higher bentonite content above 20%, the
flow decreased.
J. Mater. Civ. Eng.
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Fig. 10. Percentage of bentonite versus loss of stability (%). Fig. 12. Percentage of bentonite versus flow (unit: millimeters).

Fig. 13. Percentage of bentonite versus flow (unit: millimeters) after

soaking specimens in water for 24 h.
Fig. 11. Percentage of bentonite versus original and retained stability.

The replacement of mineral filler by bentonite clay affected the

stiffness factor of asphalt mixtures since this factor is a function of
both stability and flow (stiffness factor = stability/flow); because
flow values increased with the increasing bentonite content and
reached a maximum value when bentonite content was 10%, flow
started to decrease for modified mixtures with bentonite content
over 10%. Hence, the results of partial replacement of mineral filler
with bentonite clay (up to 10% bentonite) yielded a lower stiffness
factor than the base asphalt; in fact the stiffness factor was reduced
gradually and reached its minimum when bentonite clay content
was 10% (Fig. 14). The stiffness factor increase can be seen when
bentonite clay content was over 10%, which indicates higher sta-
Fig. 14. Percentage of bentonite versus stiffness factor.
bility and lower flow.

Hydraulic Conductivity Indirect Tensile Strength

The hydraulic conductivities were reduced with increasing benton-
ite contents (Fig. 15) due to the swelling capacity of bentonite clay
when contacting water (the only change while applying the same
testing procedure on control and modified samples was the benton-
ite content, and due to the high swelling capacity of bentonite
clay it might have resulted in expanding and filling the voids in
the specimens, which led to the reduction in permeability) and also
because of the reduction of air voids with increasing bentonite clay
content as shown in Fig. 5. For hydrostatic head of 500 cm, the
average hydraulic conductivity for nonmodified specimens was
9 × 10−4 cm=s, while for modified specimens with 15% bentonite
clay content there was a onefold reduction. By increasing the
hydrostatic head, the permeability reduced for all specimens in
the same trend.
Fig. 16 shows the average ITS values of three tests for each asphalt
mixture; for the control specimens the average strength was 292 kPa.
Replacement of mineral filler in asphalt mixtures by bentonite clay
resulted in significant increase in the indirect tensile strength, which
reached 378 kPa for samples containing 10% bentonite and 340 kPa
for both 15 and 20% bentonite.
Modifying asphalt mixtures by replacing mineral filler with ben-
tonite clay up to 10% resulted in an increase in indirect tensile
strength and fracture energy of the mixtures; however, modifying
the asphalt mixture with more than 10% bentonite reduced the
share of elastic energy, so did not show an important increase in
fracture energy in the mixture.
The natural bentonite clay had a bigger specific surface area than
limestone mineral filler and limestone aggregates, that is to say,

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Fig. 15. Hydraulic conductivity (k) of specimens versus percentage of bentonite with different hydrostatic heads (unit: centimeters).
Fig. 16. Percentage of bentonite versus average indirect tensile
strength (kPa).
limestone filler and limestone aggregates had less contact area with
asphalt (Tan and Guo 2013), which is the reason for lower interfacial
reaction between limestone filler–aggregates and asphalt than ben-
tonite clay with asphalt.
Furthermore, asphaltene and other polar fractions in the binder
content in the residual binder after subjecting it to adsorption with
mineral fillers were preferentially adsorbed on to the surface of fillers
(Guo et al. 2017). Since the bentonite clay possessed net negative
charge, the polar fractions in the bitumen were adsorbed to the ben-
tonite clay surface and formed a double layer, which resulted in
lower contact between the binder and aggregates and reducing the
interlocking of coarse aggregates; hence, the friction will be reduced
between coarse and fine aggregates in the asphalt mixture when in-
creasing natural bentonite clay content as a partial replacement of
mineral filler (more than 10%). Increasing the natural bentonite clay
content in the asphalt mixture resulted in decreasing the adhesion
between the film thickness and coarse aggregates. Likewise, the film
thickness of mastic will be increased, resulting in the reduction of
absorption of the binder, subsequently reducing the indirect tensile
strength values of the modified mixtures with more than 10%
bentonite clay.
Conclusions
Based on experimental test results, the following conclusions
are drawn when partially replacing the mineral filler portion of
aggregates in the asphalt mixture by natural bentonite clay:
• The Marshall stability and indirect tensile strength values
compared with the control sample’s (0% bentonite) values
© ASCE
J. Mater. Civ. Eng., 2018, 30(8): 04018167
are increased when natural bentonite clay content is less
than 20%;
• The indirect tensile strength reached its maximum value when
natural bentonite clay content is 10%, then it decreased when
increasing the bentonite clay content above 10%;
• Using natural bentonite clay as a partial replacement of mineral
filler exhibited a well-defined maximum for density, VFA, and
stability versus bentonite clay content at 15%;
• Partial replacement of mineral filler by natural bentonite clay
also exhibited a minimum for air voids and VMA versus ben-
tonite clay content at 15%;
• Both original and retained Marshall stability values for modified
mixtures meet the requirement for medium traffic conditions;
• Partial replacement of mineral filler by natural bentonite clay
with 15% satisfies the design criteria for medium traffic condi-
tions; and
• The hydraulic conductivity decreased for modified mixtures
with natural bentonite clay.
Acknowledgments
The authors would like to acknowledge the deanship of research
and graduate studies at Al-Zaytoonah University of Jordan for their
financial support (Award No. 25/15/2015) and the technical support
of the civil engineering labs and geology labs at the University of
Jordan (Amman, Jordan), and the mechanical engineering labs at
the University of Toronto.
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