Construction and Building Materials 180 (2018) 605–613

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Construction and Building Materials

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

Environmental aspects and pavement properties of red mud waste

as the replacement of mineral filler in asphalt mixture
Jizhe Zhang a, Shengjie Liu a, Zhanyong Yao a, Shaopeng Wu b, Hongguang Jiang a,⇑, Ming Liang a,⇑,
Yaning Qiao c
a
School of Qilu Transportation, Shandong University, Jinan, 250061, China
b
State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China
c
Department of Civil and Environmental Engineering, University of New Hampshire, W137 Kingsbury Hall, 33 Academic Way, Durham NH03824, US

h i g h l i g h t s

Natural mineral filler was replaced by red mud to prepare asphalt mastic.

Leaching toxicity and radioactivity of red mud waste were evaluated.

Improved stiffness and rutting parameter of asphalt mastic indicated improved rutting resistance.

The Sintering RM had the capability to improve the elastic recovery of asphalt mastic.

The red mud waste can be concerned as a secondary resource to replace the natural mineral filler for asphalt pavements.

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

Article history: The red mud waste generated from the alumina refining industry, which remains high alkalinity and
Received 22 February 2018 problematic pollutants, is occupying considerable land resource and causing significant environmental
Received in revised form 3 May 2018 problems worldwide. Instead of landfills, the utilization of the red mud waste as a substitution of mineral
Accepted 30 May 2018
filler in asphalt pavement mixtures has been investigated in this study. The physical and chemical prop-
erties of the red mud waste were first characterized. The experimental tests including softening point,
penetration, dynamic shear rheometer (DSR) and multiple stress creep recovery (MSCR) were then con-
Keywords:
ducted to evaluate the properties of asphalt mastic. Based on the results on leaching toxicity and radioac-
Asphalt mastic
Red mud
tivity, the red mud waste had no risk to be used as a building material. Moreover, the addition of red mud
Leaching toxicity waste can improve the stiffness and elasticity of asphalt mastic. The increased rutting parameter and the
High-temperature properties decreased accumulated creep strain were further found, especially the Sintering RM. In addition, the
Pavement Sintering RM had the capability to improve the elastic recovery of asphalt mastic, while the Bayer RM
had limited contribution to this behavior. Consequently, the red mud waste can be concerned as a sec-
ondary resource to replace the natural mineral filler for asphalt pavements.
Ó 2018 Elsevier Ltd. All rights reserved.

1. Introduction great demand with rapid development of road construction, espe-

Since 2016, the total expressway length in China has been over
130 thousand km and this is still increasing gradually with time. In
the field of road construction, asphalt mixture is the dominant
material for surface paving course. It is a composite material which
is produced in a predetermined ratio of aggregate, bitumen and fil-
ler at high temperatures and followed by compaction [1,2]. As an
integral part of asphalt mixture, the natural mineral filler is in a
⇑ Corresponding authors.
E-mail addresses: honguang_jiang@sdu.edu.cn (H. Jiang), ming.liang@sdu.edu.cn
(M. Liang).
cially in developing countries [3]. However, due to negative envi-
ronmental pollution during crushing and ball-milling processing,
many filler plants were closed in China and the filler price followed
an obvious increase. Consequently, it is of great importance to
search other alternative materials which can replace the natural
mineral filler in asphalt mixture.
Red mud (Bauxite residue) is a by-product generated in alumina
(Al2O3) refining process, which is based on the reaction of bauxite
with sodium hydroxide under high temperature and pressure [4].
Generally, the production of 1 ton of alumina results in 1.5–1.6
tons of red mud. Over 120 million tons of red mud is generated
annually throughout the world [5], in which China occupies nearly

https://doi.org/10.1016/j.conbuildmat.2018.05.268
0950-0618/Ó 2018 Elsevier Ltd. All rights reserved.
606 J. Zhang et al. / Construction and Building Materials 180 (2018) 605–613
60% of them. Due to its highly alkaline (pH 9–12.5), red mud is thus
classified as a corrosive hazardous material in some countries [6,7].
The NaOH and metallic oxide-bearing impurities are able to precip-
itate out from the red mud and contaminate the surface and under-
ground water resources [8]. Inadequate disposal of red mud pose a
potential to direct contact with fauna and flora, which eventually
threat to human health and environment [9]. Furthermore, evapo-
ration of alkali components could generate highly alkaline rainfalls
[10]. Consequently, enormous accumulation of red mud not only
occupies land resources, but also poses a serious environmental
problem [7].
In the literature, it has been reported that a target has been set
by Chinese government to utilize 20% of fresh red mud by the end
of 2015 [11]. Substantial research and field application have been
developed for the utilization of red mud in some field. Due to its
high metallic oxide content and presence of alkalis, many studies
have attempted to recover alumina, soda, ferric and titanium oxide
from red mud [12,13]. However, the material recovery strongly
depends on the metal present in the red mud and the high costs
and low yields prevent its large-operational application. Because
of its high specific surface area and hydroxides content, red mud
has been also considered as an absorbent for water treatment
[14]. By using red mud, pollutants such as dyes, toxic cations,
organic matter and heavy metals can be removed from aqueous
solutions [15,16]. In recent years, some researchers have been
focused no incorporating the red mud in construction materials
such as cement [17], clay-based ceramic [18], lightweight aggre-
gate [19] and bricks [20]. However, the use of red mud in Portland
cement has been terminated due to the limits of Na2O + K2O in new
standard [21]. Also, the bricks appeared with red mud appeared
efflorescence with the passage of time, which hurdle the utilization
of red mud [11]. Another factor which limits the utilization of red
mud is the transport distance between the refinery and the pro-
duction sites as the transporting cost is one of issues. Despite the
technology development in the red mud application, the commer-
cialization of applying red mud is still under consideration. Till
now, the accumulated red mud in the world is over 2.7 billion tons
and China occupies nearly 60% of them. So, the utilization of red
mud is an enormous challenge.
According to the reported studies, red mud has been considered
as a construction material, but there are a few reports on the uti-
lization of red mud in asphalt mixtures. Therefore, the objective
of this research is to investigate the possibility of utilizing red
mud to replace mineral filler in asphalt pavement mixture. Two
types of red mud materials produced from Sintering process and
Bayer process were selected. The red mud materials and mineral
filler at predetermined ratios were added to the hot bitumen to
prepare asphalt mastic. Experimental tests such as Softening Point,
Penetration, Dynamic Shear Rheometer (DSR) and Bending-Beam
Rheometer (BBR) were conducted to characterize the influence of
red mud on the mechanical performance of asphalt mastic at both
low and high temperatures. The optimum proportion of red mud
was evaluated and obtained based on the test results.
2. Materials and methods
2.1. Materials
2.1.1. Bitumen
70# base bitumen supplied by Huarui Asphalt Company in Shandong province,
PR China was used to prepare asphalt mastic. The bitumen was strictly evaluated
based on Chinese standards JTG E20-2011, and the results are presented in Table 1.
2.1.2. Red mud
Two types of red mud materials produced from sintering process and Bayer pro-
cess were obtained from Shandong Aluminium Industry co., ltd. In this company,
over 150 million tons of red mud is accumulated and occupies over 3 million m2
of arable land, as shown in Fig. 1. In light of using red mud to replace natural min-
Table 1
Physical properties of bitumen.
Bitumen test Result Technical Test
requirement standard
Softening point [°C] 46.2 =46 T0606
Penetration [25 °C, 68.2 60–80 T0604
0.1 mm]
Ductility [15 °C, cm] >100 =100 T0605
Viscosity at 60 °C [Pa s] 208 =180 T0625
Flash point [°C] 293 =260 T0611
Solubility in C2HCl3 99.73 =99.5 T0607
Relative density at 15 °C 1.004 – T0603
eral filler, these two red mud materials were first dried in an oven and then sieving
passing the size of 0.075 mm screen. The morphology of these two red mud pow-
ders was shown in Fig. 2. It can be seen that the Sintering RM was dull gray, while
the Bayer RM was dark red. One type of commonly used natural mineral powders
produced from a limestone quarry (Wenzu in Shandong Province) was used as a ref-
erence filler. The basic properties such as specific gravity and PH value were mea-
sured and shown in Table 2. It can be seen that these three filler samples had similar
specific gravity in the range of 2.55–2.85 g/m3. Higher PH value of red mud samples
demonstrating strong alkali component. As these two red mud materials were first
used to replace mineral filler in asphalt mixtures, their detailed physical and chem-
ical characterization were applied in the following section.
2.2. Asphalt mastic design and preparation
The asphalt mastics were prepared by using bitumen and fillers at a mass ratio
of 50:50%. With the view of evaluating the influence of red mud, the natural mineral
filler was replaced by the red mud materials at 0%, 25%, 50%, 75% and 100% by
weight of mineral filler. The asphalt mastics were prepared in a metal container
with the maximum capacity of 2 kg. The preparation process of asphalt mastics
was: the bitumen was first heated in an oven at 150 °C for 1 h until melt; the min-
eral filler and red mud in predetermined ratio were then added to the bitumen and
uniformly mixed at a temperature of 150 °C for 0.5 h at the speed of 1000 rpm; and,
the well blended asphalt mastics were stored at room temperature for further tests.
2.3. Experimental program
2.3.1. Particle size distribution
The particle size distribution of red mud and mineral filler was determined by
using a Laser Particle Size Analyzer (LS230). The theory of this method is based on
the interaction between monochromatic light and individual particles. During test-
ing, the scattered laser light by a set of monodispersed particles was analyzed by a
reverse optical scattering-based model to provide a sphere-equivalent size diame-
ter distribution [22].
2.3.2. Specific surface area and pore size distribution analysis
The specific surface area of powders were measured through a dynamic vapour
sorption system (Surface Measurement System, Middlesex, UK). By using this
approach, the particles mass increases due to the adsorption of probe vapour at
their surface and this increased mass is then measured by a sensitive balance.
The specific surface area of the particles was calculated by using the Brunauer-
Emmett-Teller (BET) approach as shown in Eq (1) [23]:
 
nm N o
SSA ¼ a ð1Þ
M
where SSA is the specific surface area (m2/g), nm is the monolayer specific amount of
vapour adsorbed on the surface of aggregate (mg), No is Avogadro’s number (6.022 
1023 mol1), M is the molecular weight of the vapour (g/mol) and a is the projected
or cross-sectional area of the vapour single molecule (m2).
The Barret-Joyner-Halender (BJH) method was employed to determine the pore
size distribution of powders. This method uses the N2 desorption branch of the iso-
therm and relates the amount of adsorbate desorbed to the average size of pores,
which is affected by this desorption with the detailed introduction of this test
can be seen in [24].
2.3.3. Chemical and mineral compositions
Chemical compositions of red mud and mineral filler were measured by X-ray
fluorescence spectroscopy (XRF) (PHILIPS MAGIX) [25]. The X-ray was generated
from rhodium target at an accelerated voltage of 20 kV. The spectra were then col-
lected using a collimator with the smallest aperture. Finally, the spectra were then
analyzed for elemental composition according to the calibrated procedure [9].
 J. Zhang et al. / Construction and Building Materials 180 (2018) 605–613
Fig. 1. Red mud storage yard in Shandong Aluminium Industry co., ltd.
Sintering RM Bayer RM
Fig. 2. Morphology of two types of red mud produced from Sintering process and
Bayer process.
Table 2
Basic properties of red mud and mineral filler.
Property Mineral filler Sintering red mud Bayer red mud
Specific gravity [g/m3] 2.701 2.553 2.852
PH value 8.2 9.9 10.0
2.3.4. Leaching toxicity and radioactivity evaluation
As the red mud is industrial solid waste which contains different heavy metal
elements, it is important to confirm the safety of red mud to be applied as a con-
struction material. Herein, the heavy metal elements of red mud were leached by
TCLP (Toxic Characteristic Leachability Procedure) with the concentrations deter-
mined by Inductively Coupled Plasma- Atomic Emission Spectrometer (ICP-AES,
IRIS Advantage). The concentrations of different heavy metal elements were com-
pared with the threshold requirements complying with GB 5085.3-2007 in order
to evaluate the safety of each waste material [26].
To assess the radiation safety of red mud, radioactivity test was performed by
using the FYFS-2002 c-spectrometry instrument. The internal exposure index and
external exposure index of red mud were then calculated based on the specific
activity of radionuclide. The calculated parameters were then compared with the
requirement in accordance with Chinese Standard GB6566-2010 [27].
2.3.5. Microscopic morphology
Microstructure and surface morphology of the red mud and mineral filler were
characterized by using scanning electron microscopy (SEM). Samples were pre-
pared by attaching a certain amount of powder on an aluminium stub using adhe-
sive patch. Then, the aluminium stub was coated with platinum to minimize surface
charging. During testing, a JSM-6610LV SEM equipped with a field emission gun at
an accelerating voltage of 20 kV was operated and the images were taken in the sec-
ondary electron (SE) imaging mode [28].
2.3.6. Conventional bitumen tests
The ring and ball test was performed based on the JTG E20-2011 standard for
evaluating the softening point of bitumen before and after modification. According
to JTG E20-2011, the penetration test was carried out at 25 °C with the view of mea-
suring the influence of modification on bitumen hardening.
The obtained softening point and penetration results had been applied to calcu-
late the penetration index (PI) of asphalt mastic based on the proposed equation of
the Shell Bitumen Handbook [29]:
607
1952  500log ðPen25 Þ  20SP
PI ¼ ð2Þ
50log ðPen25 Þ  SP  120
where Pen25 is the penetration at 25 °C (0.1 mm) and SP is the softening point (°C).
2.3.7. Temperature sweep tests
A Dynamic Shear Rheometer (AR2000ex) was used to evaluate the dynamic
mechanical properties of asphalt mastic by applying a sinusoidal load within the
linear visco-elastic range (JTG E20-2011). The temperature sweep ranged from
46 °C to 82 °C with a 6 °C increment at a set frequency of 10 rad/s with the sweep
strain of 1%. Parallel plates with the diameter of 25 mm were used to prepare mas-
tic specimen with the thickness of 1 mm. During testing, parameters such as com-
plex modulus (G*) and phase angle (d) were measured and recorded with the
temperature increase. The G* is the ratio of maximum shear stress to maximum
shear strain which represents the resistance of asphalt mastic to deformation
[30]. The d is the time delay between the applied stress and the measured strain
which represents the viscoelastic balance of the measured mastic [31].
2.3.8. Multiple stress creep recovery (MSCR) test
In order to evaluate the resistance of asphalt mastic to permanent deformation
at high-service temperature, MSCR test was performed in accordance AASHTO TP
70 2009. This test was developed based on the fixed-stress repeated creep-
recovery method to enable assessing the delayed elastic response and plastic defor-
mation of bitumen [31]. The test procedure including 10 creep-recovery cycles of
low stress (0.1 kPa) and followed by 10 creep-recovery cycles of extreme stress
(3.2 kPa), with one creep-recovery cycle composed of one second of shear loading
and nine seconds of recovery phase. Fig. 3 presents a single cycle of creep and recov-
ery curve and calculated equations for related parameters at a stress level of r0. In
this paper, the MSCR test was performed at 60 °C by using 25 mm diameter parallel
plates with the thickness controlled at 1 mm. Two parameters including Percent
Recovery (R) and Non-Recoverable Creep Compliance (Jnr) were obtained to evalu-
ate the related properties. Percent Recovery (R) reflects the how much the sample
returns to its previous shape after repeated stretch-relax cycle and higher result
indicates better fatigue resistance [32,33]. Non-Recoverable Creep Compliance
(Jnr) is the amount of residual strain left in the specimen after the repeated creep
and recovery which reflects the resistance of bitumen to permanent deformation
[34].
0.1
J nr ur 0 R r r ur 100
0.08
0.06
Strain [%]
εr
0.04
0.02
εur
0
0 2 4 6 8 10 12
Time [Second]
Fig. 3. One cycle of creep and recovery representation.
608 J. Zhang et al. / Construction and Building Materials 180 (2018) 605–613

3. Results
3.1. Particle size distribution
The results on particle size distributions of red mud and mineral
filler are shown in Fig. 4. It can be seen that the characteristic par-
ticle diameter X10, X50 and X90 of the natural mineral filler was
10.69 mm, 37.48 mm and 113.4 mm, respectively. However, these
three parameters were 13.91 mm, 74.67 mm, 160.1 mm and 2.79
mm, 93.95 mm, 203.8 mm for sintering RM and Bayer RM, respec-
tively. Even though these two red mud materials were passed
the 0.075 mm griddle, their particle were coarser than that of min-
eral filler. It was demonstrated that the red mud particle tends to
aggregate together once exposed to air. In addition, the particle
size distribution of Bayer RM was significantly wider than other
two powder. The Bayer RM contains more than 20% (by weight)
of fine particles with the grain size smaller than 10 lm.
3.2. Specific surface area and pore size evaluation
The BET method was used to measure the specific surface area,
while the BJH method was applied to obtain the pore diameter
information of different powders. The diameter derivative of the
pore volume curves of the three powders were shown in Fig. 5. It
can be seen that most of the pores in the mineral filler were dis-
tributed with the diameter between 2 and 7 nm. Compared with
the Sintering RM and Bayer RM, their pore size distributed in a
much wider range with the diameter from 2 to over 50 nm. It
was noticed that most of the pores in Sintering RM and Bayer
RM with the diameter smaller than 10 nm. Table 3 shows the
BJH pore volume and average pore diameter as well as BET specific
100
Mineral filler
80 Sintering process
Bayer process
Passing [%]
Table 3
Pore volume, average pore diameter and Specific surface area of mineral filler and red
mud.
Surface properties Mineral filler Sintering Bayer red
red mud mud
Pore volume [cc/g] 0.017 0.097 0.099
Average pore diameter [nm] 3.933 3.911 3.702
Specific surface area [m2/g] 9.988 35.419 30.996
surface area for three samples. It can be found that the pore vol-
ume of the mineral filler was 0.017 cc/g, which was significantly
lower than these two red mud powders (0.097 and 0.099 for Sin-
tering and Bayer, respectively). These three specimens showed
similar pore diameters with the values of Mineral filler, Sintering
RM and Bayer RM were 3.933 nm, 3.911 nm and 3.702 nm, respec-
tively. With respect to the SSA calculated by the BET equation, the
mineral filler got the lowest result of 9.988 m2/g, which was obvi-
ously lower than those of red mud samples with the values being
35.419 m2/g for Sintering RM and 30.996 m2/g for Bayer RM. The
difference in terms of pore volume and specific surface area may
influence the preferred adsorption of red mud to bitumen compo-
nents, which in turn affect the mechanical properties of asphalt
mastic.
3.3. Chemical composition
Table 4 shows the chemical properties of mineral filler and red
mud powders. It can be seen that CaO was the predominant phase
for mineral filler with the contents nearly 90%. There were other
two main components MgO and SiO2 detected in natural mineral
filler with a percentage of over 3% by mass. The main components
of the Sintering RM were CaO, SiO2 and Fe2O3, which accounted for
80% of total mass. In terms of the Bayer RM, Fe2O3, Al2O3 and SiO2
were the dominant components with the summations reached
nearly 80% of the total weight. The Na2O that contributes strong
alkali was detected in these two red mud samples with the con-
tents of 3.21% and 12.27% for the Sintering RM and the Bayer

60
RM, respectively. The higher Na2O content indicates why these
two red mud powders have higher PH values in comparison with
40 the natural mineral filler.

20 3.4. Leaching toxicity and radioactivity

The concentrations of heavy metals (Cd, Pb, Cr, As, Cu, Zn, Ni) in
0
1 10 100 1,000
the leachates were measured with the results shown in Table 5. As
Particle size [microns] presented in this table, all heavy metal concentrations of these two
red mud samples were under the limits according to GB5085.3–
Fig. 4. Particle size distribution of mineral filler and red mud powders. 2007. The Cd concentration was even lower than that of the

2.E-02

Mineral Filler Sintering RM Bayer RM

d[Pore Volume]/d[Pore

1.E-02
Diameter]

8.E-03

4.E-03

0.E+00
0 10 20 30 40 50 60 70 80
Pore Diameter [nm]

Fig. 5. The derivative pore size distribution curves of mineral filler and red mud.
 J. Zhang et al. / Construction and Building Materials 180 (2018) 605–613 609

Table 4 agglomerated particle, the pores with different sizes and shapes
Chemical composition (wt%) of the three samples: mineral filler, sintering RM and can be observed. The presence of these pores would result in the
Bayer RM.
high specific surface area and absorb more bitumen from the
Chemical type Composition [wt%] asphalt mastic. The Bayer RM particles were platy in shape for
Mineral filler Sintering red mud Bayer red mud coarse aggregate in a range of 50–100 lm. In addition, more fine
Al2O3 1.84 8.03 25.11
particles with irregular shapes were observed in the Bayer RM.
As2O3 – – 0.18 For the mineral filler, its particles had angular shapes with the sizes
CaO 88.65 44.64 1.54 presented a homogeneous distribution in the range of 10–100 lm.
CeO2 – 0.08 – Therefore, these two red mud powders had similar grain size, but
Cl 0.04 0.09 0.11
significantly different particle shapes in comparison with the min-
Cr2O3 – 0.07 0.07
CuO 0.02 0.01 – eral filler. The difference in terms of particle shape may finally
Fe2O3 1.13 17.54 36.43 influence the physical and rheological properties of asphalt mastic.
K2O 0.51 0.40 0.13
MgO 3.15 1.34 0.14
MnO 0.04 0.05 0.03
3.6. Conventional physical properties of asphalt mastic
Na2O 0.08 3.21 12.27
Nb2O5 – 0.01 0.01 Conventional physical properties (including softening point and
P2O5 0.09 0.26 0.20 penetration) of asphalt mastic were measured with the results
PbO – 0.03 0.01
shown in Fig. 7(a) and (b), respectively. As the mineral filler was
SO3 0.06 0.90 0.57
SiO2 4.11 18.19 16.93 replaced by different dosage of red mud powders, there was an
SrO 0.09 0.11 0.01 obvious change in the softening point and penetration values. In
ThO2 – 0.02 0.01 Fig. 7(a), the softening point increased from 53 °C to its highest
TiO2 0.19 4.81 6.02 value (77.5 °C) when mineral filler was entirely replaced by the
Y2O3 – 0.01 0.01
Sintering red mud. The Bayer red mud showed a lower softening
ZnO 0.01 0.01 0.01
ZrO2 – 0.18 0.20 point increase with the peak value been 59.5 °C. The penetration
results showed an opposite trend with the values decreased by
14.7 and 5 for Sintering red mud and Bayer red mud, respectively,
detection limit. It can be demonstrated that the utilization of red as shown in Fig. 7(b). It is indicated that the addition of red mud
mud for pavement construction would be safe. may contribute to the high-temperature performance of asphalt
Specific activity parameters (226Ra, 232Th and 40K) of red mud mixture. In terms of the same red mud dosage, the mastics with
were measured and used to evaluate the radiation safety in civil the addition of Sintering RM showed significantly higher softening
engineering works, as shown in Table 6. Based on the standard point and lower penetration values in comparison with the Bayer
GB 6566-2010, the safety thresholds of internal exposure index RM.
(IRa) and external exposure index (Ir) must be less than 1.0 and The Penetration Index (PI) were calculated with reference to Eq.
1.3, respectively. Table 6 shows that the IRa and Ir values of these (2) in order to evaluate the temperature susceptibility of asphalt
two red mud were all under the limits, which indicates the utiliza- mastic, with the results presented in Fig. 8. Based on previous
tion of these two red mud as building material meets the require- researchers, higher PI value indicating less temperature suscepti-
ment in GB 6566-2010. It should be noticed that much higher 232Th bility and more elastic behavior [2,35]. From this figure, the PI
and 40K activity of Bayer RM in comparison with Sintering RM increased with the replacement of mineral filler by red mud. The
demonstrating higher radioactivity of the Bayer RM. PI results demonstrated that the red mud can be able to improve
the elasticity of asphalt mastic, which would in turn contribute
3.5. Microstructural characterization to the rutting resistance of asphalt mixture. However, it should
be noticed that the Sintering RM showed significantly higher PI
The SEM microstructural images of the three samples are pre- value in comparison with the Bayer RM.
sented in Fig. 6. Based on the captured images, these three materi-
als yielded different surface textures and grain morphologies. The 3.7. Rheological property evaluation
near-spherical particles with different sizes (10–100 lm) can be
observed in the Sintering RM. The big aggregate was made of much The complex modulus (G*) and phase angle (d) parameters of all
smaller particles due to the agglomeration. On the surface of the asphalt mastic specimens were characterized by using the

Table 5
Concentrations of toxic metal elements in the leachates of red mud and the standard threshold.

Toxic metal elements Cd Pb Cr As Cu Zn Ni

Sintering RM [mg/L] N 0.046 0.457 0.682 0.643 1.203 1.546
Bayer RM [mg/L] N 0.813 8.624 0.180 2.776 3.303 1.062
Toxicity thresholds [mg/L] 1 5 15 5 100 100 5

Table 6
Specific activity of radionuclide and related indexes in red mud.

Sample Specific activity of radionuclide [Bq/kg] Main material for building

226 232 40
Ra Th K IRa Ir
Sintering RM 103.2 143.3 36 0.516 0.839
Bayer RM 97.9 218.6 69 0.490 1.121
Safety thresholds – – – 1.0 1.3
610 J. Zhang et al. / Construction and Building Materials 180 (2018) 605–613

Sintering RM Bayer RM

agglomeration

pore
coarse
fine

Mineral filler

Fig. 6. Scanning electron micrograph of three samples: Sintering RM, Bayer RM and mineral filler.

a 80 b 40

75 Sintering RM
35
Bayer RM
70
Penetration [0.1 mm]
]
Softening point [

65 30

60
25 Sintering RM
55
Bayer RM

50 20
0 25 50 75 100 0 25 50 75 100
Red mud percentage [%] Red mud percentage [%]

Fig. 7. Softening point (a) and penetration results of asphalt mastic with the red mud replacing mineral filler.

temperature sweep tests at a frequency of 10 rad/s, and the results
for Sintering RM and Bayer RM are shown in Fig. 9(a) and (b),
respectively. It can be seen that the complex modulus of all sam-
ples declined gradually with the temperature increasing. In terms
of the same temperature, the asphalt mastic prepared with the nat-
ural mineral filler showed the lowest complex modulus. When
replacing it by the red mud, the complex modulus had an increase
tendency with the highest value at the replacement percentage of
100% red mud. This implies that the addition of red mud results in
a harder asphalt mastic which in turn improves the resistance to
permanent deformation at high temperatures. In terms of the
phase angle curves, the asphalt mastic prepared with the 100%
mineral filler showed the highest value. With the addition of red
mud, the phase angle of asphalt mastic took on a slight decrease.
This phenomenon indicates that the red mud leads to the increase
of the elastic component of the modified asphalt mastic, which
may contribute to the elasticity of asphalt pavement. The increase
of complex modulus and the reduced phase angle can be explained
by the pore volume and SSA of related powders. Jeon and Curtis
[36] stated that surfaces of aggregates with high porosity can act
as molecular sieves, separating high and low molecular bitumen
fractions. As the pore volume and SSA of red mud are significantly
higher than that of the mineral filler, there would be more light
components absorbed by the red mud and the bitumen remaining
on the outside becomes hard and brittle.
When comparing the difference between Sintering RM and
Bayer RM, the complex modulus and phase angle values of all spec-
imens at 60 °C and 70 °C were selected and presented in Table 7.
Under the same temperature, the addition of Sintering RM
obtained higher complex modulus and lower phase angle in com-
parison with the Bayer RM, which correlated well with the soften-
ing point as well as the penetration tests. The complex modulus of
 J. Zhang et al. / Construction and Building Materials 180 (2018) 605–613 611

3 a positive impact on the high-temperature properties of asphalt

2.25 mixture.
2 The rutting parameter G*/sin d had been calculated using the
results obtained from the temperature sweep tests, as shown in
Penetration Index

0.77
1 Fig. 10. The rutting parameter was considered as an important
0.35
0.03 parameter in characterizing the rutting resistance, where the
0 -0.32 -0.28
-0.52 -0.6 related material with higher value is correlated to better rutting
-1.04 resistance at high temperature [37,38]. As observed in Fig. 10,
-1 the rutting parameters for all specimens decreased with the
increase of temperature, indicating the reduction in the rutting
-2
resistance. The addition of red mud caused an increase in the
G*/sin d, which would be expected to be more resistant to the

5
25

50

00
r

0
75

5
le

r-5

r-7
10

r-2

r-1
g-

g-

g-
fil

g-

ye

ye
ye
in

in

in

ye
al

in

Ba

Ba
er

er

Ba
er

permanent deformation.
er

Ba
er
nt

nt

nt
in

nt
Si

Si

Si
M

Si

Fig. 8. Penetration Index values of all asphalt mastic specimens.

1.E+07
Mineral Filler
Sintering-50
1.E+06
Sintering-100
Bayer-50
1.E+05

G*/Sinδ [Pa]
Bayer-100

1.E+04

1.E+03

1.E+02
45 50 55 60 65 70 75 80 85
Temperature [ ]

Fig. 10. Effect of temperature on rutting parameter for asphalt mastic at a

frequency of 10 rad/s.

1
a
Mineral Filler
0.8 Sintering-50
Accumulated Strain [%]

Sintering-100
0.6 Bayer-50
Bayer-100

0.4

0.2
Fig. 9. Complex modulus and phase angle of asphalt mastic specimens at a
frequency of 10 rad/s: mineral filler replaced by red mud (a) Sintering RM and (b)
Bayer RM. 0
0 20 40 60 80 100
Time [Second]
Table 7 40
Complex modulus and phase angle of specimens at 60 °C and 70 °C. b
Specimen 60 °C 70 °C Mineral Filler
32
Accumulated Strain [%]

G* [Pa] d [°] G* [Pa] d [°] Sintering-50

Sintering-100
Mineral filler 8445 15.041 2482 30.566
24 Bayer-50
Sintering-25 10,502 15.078 3096 29.622
Sintering-50 13,665 15.439 4067 29.457 Bayer-100
Sintering-75 14,974 14.700 4484 26.146 16
Sintering-100 19,845 13.946 6022 24.228
Bayer-25 8818 15.812 2615 30.824
Bayer-50 10,889 15.484 3248 29.554 8
Bayer-75 12,258 15.228 3659 26.329
Bayer-100 13,502 14.822 4072 24.482
0
100 120 140 160 180 200
Time [Second]
specimens with 100% red mud is about twice the values of conven-
tional mastic. Consequently, the utilization of red mud can be able Fig. 11. Creep compliance results of asphalt mastic obtained from MSCR tests at 60
to improve the stiffness and elasticity of asphalt mastic, which has °C under different stress levels: (0–100 s) 0.1 kPa (a) and (100–200 s) 3.2 kPa (b).
612 J. Zhang et al. / Construction and Building Materials 180 (2018) 605–613

3.8. Creep and recovery evaluation
The MSCR tests were performed at 60 °C under two stress levels
of 0.1 kPa and 3.2 kPa in order to evaluate the creep compliance
and elastic response of related asphalt mastic. Fig. 11 shows the
accumulated strain of selected specimens at two different stress
levels. By comparing Fig. 11(a) and (b), it can be seen that a higher
creep stress level correlated with a higher accumulated creep
strain. At the same stress level, the addition of red mud decreased
the accumulated strain, and the mastic containing 100% of Sinter-
ing RM had the lowest value. It is demonstrated that the Sintering
RM significantly improves the resistance of asphalt mastic for per-
manent deformation. In terms of the Bayer RM, a higher accumu-
lated strain value in comparison with the Sintering RM indicates
its less contribution to rutting resistance. This phenomenon corre-
lates well with the rutting parameter in temperature sweep test.
Fig. 12 shows non-recoverable compliance (Jnr) to evaluate the
strain response of the asphalt mastic to stress. This parameter
has widely been used as a means of reflecting resistance against
deformation under repeated loading at high temperature [39,40].
From this figure, the Jnr decreased from over 0.8 to less than 0.4
for as the dosage of Sintering red mud increased from 25% to
100%. However, the Bayer red mud has limited influence on the
Jnr result, with the values only decreased by around 10%. It implies
that the replacement of mineral filler by Sintering red mud reduced
the non-recoverable deformation of the asphalt mastic, which may
contribute to the rutting resistance of related asphalt mixtues.
1
0.8
0.6
Jnr [1/kPa]
The influences of red mud type and dosage on elastic recovery
(R) at two stress levels are presented in Fig. 13. It can be observed
that specimens prepared with the Bayer RM had much lower
recoveries than those prepared with the Sintering RM. For the
same specimen, the lower stress level correlates with a higher elas-
tic recovery, where the sample prepared with the Sintering RM
obtained the highest recovery at the 0.1 kPa stress. When increas-
ing the Sintering RM content, the recovery value increased from
around 8% to nearly 40%. However, the vibration of the Bayer RM
dosage had little effect on recovery values. This indicates that Sin-
tering RM has the capability to improve the elastic recovery of
asphalt mastic, but the Bayer RM has slight contribution to this
parameter.
4. Conclusion
Environmental aspects and potential utilization of the red mud
waste, as a replacement of virgin mineral filler for preparing
asphalt mixture in pavements, were investigated in this study.
The physical, chemical as well as environmental aspects of red
mud powders were first characterized and compared with a natu-
ral mineral filler. The properties of asphalt mastic prepared with
different replacement percentages of red mud powders was evalu-
ated by using conventional physical tests and rheological measure-
ments. The following conclusions can be given:
1) According to the particle size distribution, the two types of
red mud materials used had coarser particles, which could
be attributed to the agglomeration of the fine red mud par-
ticles. The pore volume of red mud is over 5 times of the nat-
ural mineral filler. In addition, the specific surface area of red
mud is over 30 m2/g while the value of natural mineral filler
is less than 10 m2/g. The difference in terms of pore volume
and specific surface area would influence the preferred
adsorption of red mud to bitumen components, which in

turn would affect the mechanical properties of asphalt

Sintering-0.1kPa
0.4 mastic.
Bayer-0.1kPa 2) On basis of the XRF tests, the higher Na2O content indicated
Sintering-3.2kPa that these two red mud powders had higher alkalinity in
0.2
comparison with the natural mineral filler. Leaching toxicity
Bayer-3.2kPa
and radioactivity results demonstrated that the utilization of
0 these two types of red mud materials as a building material
0% 20% 40% 60% 80% 100% 120% had less environmental risks.
Red mud dosage [%] 3) According to the microscopic analysis, the Sintering red mud
contains more aggregated particles with the size of 50–100
Fig. 12. Non-recoverable creep compliance (Jnr) of mastic specimens at different
stress levels.
lm, which shows significantly different particle shape in
comparison with the Bayer red mud even tough they have
similar particle size.
40 4) The addition of red mud increased the softening point while
decreased the penetration values of asphalt mastics, and the
Sintering-0.1kPa Sintering red mud showed more obvious influence. A signif-
32
Bayer-0.1kPa icant higher PI value for the samples prepared with the Sin-
Sintering-3.2kPa tering RM indicated its apparent improvement of high-
24
Bayer-3.2kPa
temperature performance.
5) With the addition of the red mud waste, the complex mod-
R [%]

ulus increased while the phase angle increased, which indi-

16
cated the increase of elastic behavior. The complex modulus
of specimens with 100% red mud is about twice the conven-
8 tional mastic at high temperatures. The increased rutting
parameter further showed the improvement of high-
temperature performance after replacing the mineral filler
0
0% 20% 40% 60% 80% 100% 120%
by the red mud, especially the Sintering RM.
Red mud dosage [%] 6) The addition of red mud significantly decreased the accumu-
lated creep strain and this modification would be able to
Fig. 13. Elastic recovery (R) of mastic specimens at different stress levels. improve its rutting resistance. Moreover, the Sintering RM
 J. Zhang et al. / Construction and Building Materials 180 (2018) 605–613
significantly decreased the Jnr (from 0.8 to 0.4) while
increased the R values (from 8% to 38%). It is indicated that
the Sintering RM can improve the elastic recovery of asphalt
mastic, while the Bayer RM had slight contribution to this
behavior.
7) Both DSR and MSCR results showed the performance
enhancement of the asphalt mastic specimens prepared
with the Sintering RM. All these results would encourage
industry to envisage the utilization of the red mud in asphalt
pavements.
Conflict of interest
The authors declared that they have no conflicts of interest to
this work. We declare that we do not have any commercial or asso-
ciative interest that represents a conflict of interest in connection
with the work submitted.
Acknowledgements
The authors acknowledge the financial support of the China
Postdoctoral Science Foundation (Project No. 2017 M622207) and
Special Funding for Postdoctoral Innovation Project in Shandong
Province (Project No. 201702011). Special thanks are to the State
Key Laboratory of Silicate Materials for Architectures (Wuhan
University of Technology) (Project No. SYSJJ2018-07).
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