Construction and Building Materials xxx (xxxx) xxx

Contents lists available at ScienceDirect

Construction and Building Materials

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

Marble waste characterization and reinforcement in low density

polyethylene composites via injection moulding: Towards improved
mechanical strength and thermal conductivity
Anam Khan a,b, Ravi Patidar a, Asokan Pappu a,b,⇑
a
CSIR - Advanced Materials and Processes Research Institute (AMPRI), Bhopal 462026, India
b
Academy of Scientific and Innovative Research (AcSIR), India

h i g h l i g h t s g r a p h i c a l a b s t r a c t

 Sustainable approach for marble

waste recycling in manufacturing
composite material.
 Composites have been prepared
under injection moulding system.
 Incorporation of 50% marble waste
enhanced the performance of
composite quality.
 Solution to reduce adverse effect of
marble waste mismanagement.

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

Article history: Enormous amount of accumulated waste is a matter of concern for environmental safety as it influences
Received 30 June 2020 other precarious issues such as air pollution, land degradation, in addition to contamination of water &
Received in revised form 23 September soil through leaching. A proficient recycling and management of generated solid waste is the key option
2020
to overcome such issues. Sustainable utilization of marble waste particulates as reinforcement in manu-
Accepted 4 October 2020
Available online xxxx
facturing LDPE-MW (low density polyethylene-marble waste) composites through injection moulding
technique has been investigated. The mineralogical study of marble waste particulates revealed existence
of dolomite (CaMg (CO3)2) and calcite (CaCO3) as major minerals with very small quantity of quartz
Keywords:
Marble waste
(SiO2). Parallel results were obtained by thermal and FTIR analyses of marble waste particulates. The
Sustainability average particle size of marble waste particulates was 15.98 ± 3.319 mm with the bulk density
Mechanical properties 1.49 ± 0.007 g/cc and porosity 35 ± 1.85%. The pH was adjusted at 7.86 ± 0.003 and electrical conductivity
Recycling was 3.78 ± 0.061 mS/cm. The FE-SEM analysis showed irregular morphology of marble waste particulates.
Injection moulding Mechanical properties such as tensile strength, tensile modulus, flexural strength, flexural modulus and
Thermal conductivity impact strength of LDPE-MW composites were determined. Thermal conductivity of LDPE-MW compos-
ites was also reported. The obtained results showed maximum enhancement in the strength and thermal
conductivity with incorporation of about 50% marble waste particulates. The findings of the present study
revealed that there is considerable potential for large scale recycling of marble waste in making LDPE
based hybrid materials, leads to create new application as architectural cladding wall panel, electrical
insulating floor tiles and damping pads.
Ó 2020 Published by Elsevier Ltd.

⇑ Corresponding author at: Chief Scientist, CSIR - Advanced Materials and

Processes Research Institute (AMPRI), Bhopal 462026, India.
E-mail addresses: pasokan@ampri.res.in, asokanp3@yahoo.co.in (A. Pappu).

https://doi.org/10.1016/j.conbuildmat.2020.121229
0950-0618/Ó 2020 Published by Elsevier Ltd.

Please cite this article as: A. Khan, R. Patidar and A. Pappu, Marble waste characterization and reinforcement in low density polyethylene composites via injection moulding: Towards
improved mechanical strength and thermal conductivity, Construction and Building Materials, https://doi.org/10.1016/j.conbuildmat.2020.121229
A. Khan, R. Patidar and A. Pappu
1. Introduction
The ever-growing population gives rise to extensive need and
more utilization of natural resources. To fulfil the demand from
domestic, new technologies in agricultural and industrial area have
been developed, which generates solid and hazardous wastes as by-
products [1,2]. Industrial processes such as cutting, grinding and
mining operations produce large quantity of marble waste particu-
lates in the form of solid as well as liquid (Slurry). The improper dis-
posal of these wastes is responsible for several environmental
problems [3]. This includes land degradation, pollution in water
bodies due to leaching of toxic species which further affects the
habitat of flora, fauna and human health [4]. The state of Rajasthan
alone produces about 12 MT of marble waste annually [5].
Attempts have been made by various researchers to utilize mar-
ble waste particulates in making polymer composites (supplemen-
tary Table 1). The recycled artificial marble powder (60%) was used
as filler material for the production of AMP/HDPE wood composites
[6]. The resultant mechanical properties revealed that the compos-
ites possessed tensile strength of 28.00 MPa along with flexural
strength and flexural modulus of about 42.80 MPa and 2.70 GPa,
respectively. Borsellino et al. [7] studied the impact of marble
waste content and type of matrix (epoxy and polyester) on
mechanical properties of composites. The composites manufac-
tured using marble waste (60%) with polyester resin under rotation
moulding showed a flexural strength and flexural modulus of
30.70 MPa and 7.33 GPa with the water absorption of about
0.12% while with epoxy resin they showed flexural strength and
flexural modulus of 22.20 MPa and 4.86 GPa with water absorption
of about 0.07%. The needle- punched nonwoven jute fibre/epoxy
(NPNJE/E) composites were fabricated using marble waste content
of about 30% [8] and composites showed tensile strength and flex-
ural strength of 35.48 MPa and 71.87 GPa and the corresponding
density was found to be 1.29 g/cc. The study conducted by Cinar
& Kar [9] produced composites using marble dust (25%) and poly-
ethylene terephthalate. The reported tensile strength and flexural
strength were 16.00 MPa and 48.00 MPa, respectively. The work
done by Sales et al. [10] showed flexural strength of 14.90 MPa
with water absorption 0.30% and density of 1.40 g/cc. The influence
of compaction pressure and particle composition on properties of
crushed marble and unsaturated polyester resin slabs made by
Ribeiro & Rodriguez [11] showed flexural strength and flexural
modulus of 18.40 MPa and 9.70 GPa, respectively and the corre-
sponding density was 2.37 g/cc with water absorption of 0.42%.
The work done by Gokdai et al. [12] depicted that the polymer
matrix composites using pine cone, marble waste and ATH (alu-
mina trihydrate) exhibited a flexural strength of 57.48 MPa and
flexural modulus of 7.35 GPa with 1.73 g/cc of density, respec-
tively. It is evident from the results that polyester resin with pine
cone possessed higher mechanical strength due to the contribution
of fibres. The work carried out by Gomes Ribeiro et al. [13] on arti-
ficial marble showed flexural strength of 26.60 MPa and flexural
modulus of 21.50 GPa. The corresponding water absorption was
lower (0.16%) whereas density was higher (2.38 g/cc). The polymer
composites reinforced by chicken feathers with marble waste
(28%) have showed a density of 1.63 g/cc with flexural strength
and flexural modulus of 63.84 MPa and 6.55 GPa respectively while
the water absorption was 0.55% with the thickness 0.07% [14].
Ahmed et al. [15] used marble waste and natural rubber for making
hybrid composites and achieved a tensile strength of 6.50–
23.12 MPa using 60% of marble waste. The study carried out by
Icduygu et al. [16] on application of polyester with 77% marble
waste has resulted a flexural strength of 42.2 MPa. The use of
20% marble waste with epoxy resin has showed a tensile strength
and tensile modulus of 5.52 MPa and 17.66 GPa respectively [17].
2
Construction and Building Materials xxx (xxxx) xxx
Research done by Singh et al. [18], Saygili et al. [19] and Patel
et al. [20] have reported the utilization of marble powder to
improve soil properties while research done by Ghazy et al. [21],
Bhalothia et al. [22] and Godboley et al. [23] used marble powder
as an adsorbing material for lead, chromium and fluoride. The
study conducted by Khan et al. [24], Bilgin et al. [25] and Munir
et al. [26] utilized marble waste for manufacturing of bricks. The
other studies done by Sharma et al. [27], Asokan et al. [28], Vard-
han et al. [29] and Selim et al. [30] showed partial replacement
of sand, cement and immobilisation of hazardous wastes by incor-
poration of marble waste.
In the present study LDPE-MW composites were fabricated with
various concentrations of marble waste particulates (10–50%)
using injection moulding process at two different melt tempera-
tures (110 and 140 °C), since marble waste is inorganic in nature
therefore elevated temperature from the melting temperature of
LDPE has been used to ensure proper blending of marble waste
particulates with the matrix. The effect of marble waste particu-
lates on various properties of LDPE-MW composites has been
investigated. This study aims to recycle marble waste generated
in huge quantity as a reinforcing material for making LDPE-MW
composite under injection moulding for possible application as
architectural cladding wall panel, electrical insulating floor tiles
and damping pads as no work has been reported yet for use of mar-
ble waste recycling under injection moulding process.
2. Materials and methods
2.1. Processing and preparation of sample for characterization
The marble waste particulates (M 1) was collected from mar-
ble cutting and processing industries in Chittorgarh district,
Rajasthan, India. It was dried in an oven at 110 °C for 6 h. The dried
sample was crushed and passed through sieve (ASTM-35). The
sample was prepared to achieve 1.0% moisture content and used
for analysis. LDPE (16 MA400; density 0.918 g/cc) was purchased
from reliance polymers and used as received. For all the water
required experiments Millipore milliQ ultrapure water was used
with resistivity of 18.2 MO/cm.
2.2. Fabrication of LDPE-MW composite
The homogeneous mixture of marble waste and LDPE was pre-
pared manually. The as prepared mixture was transferred to the
injection moulding machine (Nova Servo 15, Milacron, India) at
different melt temperatures (110 and 140 °C). The weight fraction
of mixture of marble waste and LDPE is given in Table 1.
2.3. Characterization techniques
The pH and electrical conductivity were analysed using
Labman-LMPH 12 and Labman-LMCM 20, respectively. The analy-
sis was carried out in 1:2 solid: water ratio suspension. Physico-
chemical characteristics such as bulk density and porosity were
measured in accordance with ASTM: F1815-11 while specific grav-
ity was measured following ASTM: D854-00. In all cases replicate
samples have been tested and reported.
X-Ray Diffraction (XRD) analysis for marble waste particulates
was performed using X-ray diffractometer Rigaku Mini Flex II
(Japan) with Cu Ka radiation (k = 1.5401 Å) at room temperature
with scanning range of 10–75 (2 h).
Thermogravimetric analysis of marble waste was performed
using Mettler Toledo thermogravimetric analyzer TGA/DSC 1
(Germany) at inert atmosphere of nitrogen by continuous heating
from room temperature to 1200 °C with a heating rate of 10 °C/min.
A. Khan, R. Patidar and A. Pappu Construction and Building Materials xxx (xxxx) xxx

Table 1
Preparation and Formulation of LDPE-MW composite under injection moulding.

S. No. Sample ID Marble waste content (gm.) Polymer content (gm.) Pressure (bar) Temperature(oC)
1. LDPE-MW-0% 0 500 40 110 & 140
2. LDPE-MW-10% 50 500 40
3. LDPE-MW-15% 100 500 40
4. LDPE-MW-20% 150 500 40
5. LDPE-MW-25% 200 500 40
6. LDPE-MW-30% 250 500 40
7. LDPE-MW-50% 500 500 40

Particle size analysis of the marble waste was carried out using
Horiba Partica Laser Scattering Particle Size Distribution Analyzer
LA-950 V2 (Japan). Ethanol was used as a dispersion medium.
The refractive indices used for ethanol and marble waste were
1.360 and 1.560, respectively.
Elemental analysis (CHNS) of marble waste particulates was
carried out using Vario EL III elemental analyser (Germany). Sul-
phanilic acid (E. Merck, 64,271 Darmstadt, Germany) was used as
a standard. Tungsten (VI) oxide (Elementar, Art No. 11.02-0017)
was used as a catalyst along with the sample.
FTIR analysis of marble waste particulates and LDPE-MW com-
posites have been done at room temperature using Thermo Scien-
tific Nicolet iS50 FT-IR spectrometer (USA) equipped with diamond
crystal ATR accessory. The total number of scans were 64.
Microstructural analysis of marble waste particulates and LDPE-
MW composites was done using Nova NanoSEM 430 (USA, IE syn-
ergy 250) at 3 kV operating voltage. The marble waste particulates
were gold-coated before image attainment. EDX analysis was car-
ried out using JEOL JCM-6000 plus (Japan) instrument.
Mechanical properties such as tensile strength and tensile mod-
ulus were calculated according to ASTM D638 while flexural
strength and flexural modulus were calculated following ASTM
D790. The testing was done using universal testing machine
(UTM), 5 kN capacity (LRX Plus, Lloyd, UK). For tensile testing
LDPE-MW composites, 50 N load cell was used with cross head
speed of 20 mm min 1 at 50 mm gauge length. The cross head
speed of 10 mm min 1 was used for flexural testing. Impact
strength was measured following ASTM D256 using Tinius Olsen
model 104 (UK). For each parameter at least five samples have
been tested.
Thermal conductivity was measured using QTM-710 (Japan) at
30 °C with the heater value of 0.3 A.
3. Results and discussion
3.1. Marble waste
3.1.1. Physico-chemical characterization
The physico-chemical properties of marble waste particulates
collected from Chittorgarh have been reported in Table 2. The bulk
density of marble waste particulates (M 1) was found to be 1.49
± 0.007 g/cc which showed variations in the size and arrange-
ments of particles in the given volume as bulk density depends
on the size of powder particles, the spatial arrangement of particles
in the powder bed and presence of ions in the sample. Research
done by Patel et al. [31] showed bulk density in the range of 1.3–
1.5 g/cc while Bdour et al. [32] showed bulk density in the range
of 1.25–1.65 g/cc.
The specific gravity of marble waste particulates (M 1) was
observed to be 2.32 ± 0.016 which suggests degree of saturation
and void ratio in the sample. The reported value was observed to
be less as compared to the work carried out by Aruntas et al.
[33] and Ercikdi et al. [34], where it is Turkish based marble and
there is a possibility of increase in specific gravity due to geograph-
ical formation of different region. The Marble waste particulates
(M 1) showed porosity of 35.24 ± 1.85% which refers to pore
spaces in the sample. The research work carried out by Kelestemur
et al. [35] and Sutcu et al. [36] showed almost similar porosity val-
ues (24.64, 22.3–42.8) as compared to present work.
The pH of marble waste particulates (M 1) was found to be
7.86 ± 0.003 and electrical conductivity was 3.78 ± 0.061 mS/cm.
This work has been supported by the work carried out by Kabas
et al. [37], Moreno et al. [38], Melgar et al. [39] and Perez et al. [40].
3.1.2. Elemental analysis
Elemental analysis was carried out to ascertain the amount of
Carbon, Hydrogen, Nitrogen, and Sulphur elements present in the
marble waste particulates (M 1). Elemental analysis of the marble
waste particulates is reported in Table 2. The obtained results
showed that marble waste particulates (M 1) possess noticeable
amount of carbon while very less amount of hydrogen, nitrogen
and sulphur due to less availability of organic matter. The consid-
erable amount of carbon content (9.55 ± 0.018%) in marble waste
sample was probably due to the decomposition of dolomite (CaMg
(CO3)2) into carbon-based by-products since the reported carbon is
inorganic in nature. The negligible amount of hydrogen
(0.11 ± 0.008%) in marble waste particulates is observed which
might be due to presence of moisture in sample. The nitrogen is
absent in the sample which is possibly due to absence of nitrogen
oxides in marble waste sample. The presence of very less amount
of sulphur (0.21 ± 0.032%) indicates the presence of traces of sul-
phates and sulphites respectively. The research work carried out
by Eliche-Quesada et al. [3] showed the amount of carbon, hydro-
gen, nitrogen and sulphur to be 11.89%, 0.01%, 0.00%, and 0.00%.

Table 2
Physico-chemical, Elemental and Particle Size analysis of Marble Waste particulates.

Sample Replication Bulk Specific Porosity pH Electrical Carbon Hydrogen Nitrogen Sulphur Mean D10 D60 D90
Density Gravity (%) Conductivity (Wt.%) (Wt.%) (Wt.%) (Wt.%) (mm) (mm) (mm) (mm)
(g/cc) (mS/cm)
M 1 1 1.49 2.31 35.23 7.86 3.70 9.53 0.10 0 0.18 12.82 1.18 3.90 39.25
2 1.50 2.34 33.40 7.86 3.79 9.56 0.12 0 0.25 15.69 1.12 3.40 42.73
3 1.48 2.31 37.09 7.86 3.85 9.55 0.12 0 0.21 19.44 1.13 3.40 57.87
Mean 1.49 2.32 35.24 7.86 3.78 9.55 0.11 0 0.21 15.98 1.14 3.56 46.61
SD 0.007 0.016 1.85 0.003 0.061 0.018 0.008 0 0.032 3.319 0.032 0.288 9.899

3
A. Khan, R. Patidar and A. Pappu
The study done by Ji et al. [41] showed the amount of carbon to be
8.82%. In a research work done on marble sludge in Spain, C, H, N, S
were found to be 11.61%, 0.14%, 0.14% and 0.99% respectively [42].
In other research works done by Kabas et al. [37] and Zornoza et al.
[43] the value of Carbon and Nitrogen were found to be NIL in mar-
ble waste.
3.1.3. Particle size analysis
The particle size distribution graph is shown in Fig. 1c. From the
particle size data (table 2) of marble waste particulates (M 1), it
can be observed that the average particle size in marble waste
sample was found to be 15.98 (mm). About 10% of the total popu-
lation was under the size of 1.14 (mm), 60% of the total population
was under the size of 3.56 (mm) while 90% of the total population
was under the size of 46.61 (mm). The literature studies on particle
size of marble waste showed average particle size below 20 (mm)
[44] and [45]. It was observed from the table that maximum parti-
cle size of marble waste sample was under the size of 46.61 (mm)
which might be due to the agglomeration of many small particles
in the collected sample.
3.1.4. Mineralogical characterization
XRD studies have been done to identify the mineralogical com-
position of marble waste particulates. The sharp peaks observed in
the XRD graph suggests the crystalline nature of the sample. It was
observed from the Fig. 1a that marble waste particulates (M 1)
showed three major mineral phases of calcite (CaCO3) (JCPDS:05–
586), dolomite (CaMg (CO3)2) (JCPDS:36–0426) and quartz (SiO2)
(JCPDS:46–1045) and a peak corresponds to actinolite (Ca2 (Mg,
Fe)5Si8O22(OH) 2 was also detected. Both Calcite and Dolomite have
been reported as major constituents of Marble waste powder in
other research works. The work carried out by Yesilay et al. [46],
Kavas et al. [47] and Firat et al. [48] showed calcite and dolomite
as a major mineral while research done by Mlayah et al. [49]
Fig. 1. XRD diffractogram (a), TGA thermogram (b), Particle size distribution (c) and FTIR graph (d) of marble waste particulates.
4
Construction and Building Materials xxx (xxxx) xxx
showed cerussite and hydrocerussite along with the calcite and
dolomite minerals.
3.1.5. Thermal characterization
It can be observed from Fig. 1b that marble waste particulates
(M 1) exhibited a decomposition onset temperature beyond
700 °C while an endset temperature in vicinity of 850 °C. marble
waste particulates (M 1) showed a single well-defined decompo-
sition in their respective temperature range. In one of the research
works, Marble waste has been used for cement manufacturing
[44]. The authors didn’t report any specific values of onset and end-
set temperatures except the inflection point which was approxi-
mately 849 °C with only a single clear differential peak with no
splitting. A cursory look at the reported TGA thermogram gives a
temperature range of approximately 700–870 °C for onset and
endsettemperature. In another study, an in-depth thermal analysis
was conducted to analyze various Marble samples in order to dif-
ferentiate them geographically [50]. According to the authors, the
main decomposition of Marble occurs between 700 and 850 °C,
mainly attributed to Calcite. Decompositions that occur between
380 and 650 °C have been linked with significant presence of Dolo-
mite [51] which means the presence of Magnesium Carbonate in
addition to that of Calcium. The Calcite and Dolomite both decom-
pose in a continuous manner between 650 and 850 °C, when the
atmosphere changes from air to CO2, the decomposition of Magne-
sium Carbonate undergoes first [52].
3.1.6. FTIR analysis
The FTIR spectra of marble waste particulates (M 1) is shown
in Fig. 1d. The peaks observed at 1424 cm 1 and 1812 cm 1corre-
sponds to stretching vibration of carbonate radical which is due to
the presence of dolomite and calcite mineral in the marble waste
sample [4], [53] and [54]. The sharp peaks observed at 875 cm 1
and 728 cm 1attributed to Mg-O bonds which confirms the pres-
A. Khan, R. Patidar and A. Pappu
ence of magnesium based dolomite as a major mineral in the sam-
ple [53]. The parallel results have been observed by XRD analysis of
the samples. The small peaks at 463 cm 1 and 517 cm 1 indicates
the presence of Si-O bonds which is possibly due to the presence of
small amount of quartz mineral in the sample as indicated by min-
eralogical studies of the marble waste [55]. The broad peak at
998 cm 1corresponds to C = C bending. The peak at 1081 cm 1 cor-
responds to C-O stretching while small peak observed at
3613.54 cm 1 was due to stretching vibration of O–H group [53]
and [54].
3.1.7. FE-SEM and EDX analysis
The microstructure of marble waste particulates (M 1) is
shown in Fig. 2 (a, b). It can be observed from the figure that mar-
ble waste particulates are irregular in shape, variable in size and
are randomly arranged. However, at high magnification distorted
rectangular shape of marble waste particulates is observed. These
variations in shape and size would affect the properties of compos-
ites. Moreover, it can be observed from the images that there was
enough surface area present for the dispersion of particulates
within the matrix. The EDX analysis was performed to get the ele-
mental composition of marble waste particulates. From the Fig. 2
(c) it was observed that marble waste particulates contain calcium
(18.31%) and magnesium (7.83%) as major elements with the
traces of silicon (6.44%), aluminium (0.80%), sodium (0.08%), potas-
sium (0.58%), manganese (0.06%) and iron (0.59).
Fig. 2. FE-SEM images (a,b) and EDS (c) of Marble waste particulates.
5
Construction and Building Materials xxx (xxxx) xxx
3.2. LDPE-MW composites
3.2.1. Mechanical properties
The mechanical properties obtained for LDPE-MW composites
are shown in table 3. The obtained results showed that the flexural
strength and flexural modulus of LDPE-MW composites increased
with increase in percentage of marble waste particulates at both
the temperatures. However, more increment in the flexural
strenghth of LDPE-MW composites at 140 °C was observed as com-
pared to 110 °C with the addition of marble waste particulates. The
diffrence in the flexural strength revealed proper melting and mix-
ing of LDPE with the mable waste particulates at 140 °C . The flex-
ural strength of LDPE-MW composites at 110 °C was found in the
range of 11.08–14.85 MPa while at 140 °C the flexural strength
of LDPE-MW composite was found in the range of 10.50–
17.18 MPa. The increased flexural strength with reinforcing mate-
rial content was observed due to the resistance provided by the
particulates towards the applied bending force and transfer of
effective stress from matrix to particulates. Similar results was
observed by Adeosun et al. [56] and Abdel Salam et al. [57].
On contrary, tensile strength and tensile modulus of LDPE-MW
composites was found to be decreased with addition of marble
waste particlutes. The decrease in tensile strength and tensile
modulus was possibley due to increase in the void content and
weakened interfacial bonding between the particulates and resin.
Morover, the larger particle size of marble waste particulates also
contributes for the initiation of crack [58]. Similar trend was
A. Khan, R. Patidar and A. Pappu Construction and Building Materials xxx (xxxx) xxx

Table 3
Mechanical properties of LDPE-MW Composites.

Mechanical properties of LDPE-MW Composites at 110 °C

Sample ID Flexural Strength (MPa) Flexural Modulus (MPa) Tensile Strength (MPa) Tensile Modulus (MPa) Impact Strength (KJ/m2)
LDPE-MW-0% 10.50 ± 0.14 223.36 ± 14.39 9.15 ± 0.09 54.86 ± 1.18 28.98 ± 0.35
LDPE-MW-10% 12.20 ± 0.47 289.63 ± 14.82 8.88 ± 0.07 72.97 ± 1.79 21.21 ± 0.19
LDPE-MW-15% 12.61 ± 0.23 323.27 ± 73.64 8.79 ± 0.04 71.83 ± 1.34 19.15 ± 0.17
LDPE-MW-20% 12.64 ± 0.23 321.85 ± 7.94 8.75 ± 0.12 76.33 ± 2.25 18.08 ± 0.33
LDPE-MW-25% 13.01 ± 0.21 350.49 ± 32.94 8.68 ± 0.14 78.53 ± 3.27 16.42 ± 0.11
LDPE-MW-30% 14.07 ± 0.37 430.04 ± 30.57 8.68 ± 0.13 90.49 ± 2.03 15.07 ± 0.18
LDPE-MW-50% 14.85 ± 0.40 508.74 ± 61.90 8.80 ± 0.44 90.22 ± 2.90 12.57 ± 0.14
Mechanical properties of LDPE-MW Composites at 140 °C
LDPE-MW-0% 11.08 ± 0.43 244.39 ± 9.54 7.85 ± 0.19 56.19 ± 2.77 24.98 ± 0.27
LDPE-MW-10% 12.37 ± 0.09 296.42 ± 15.56 7.83 ± 0.15 71.45 ± 0.96 15.40 ± 0.13
LDPE-MW-15% 12.61 ± 0.40 343.48 ± 59.49 7.70 ± 0.25 84.99 ± 5.40 12.51 ± 0.20
LDPE-MW-20% 13.65 ± 0.47 374.53 ± 36.05 7.71 ± 0.25 88.93 ± 9.37 10.86 ± 0.26
LDPE-MW-25% 14.59 ± 0.46 487.15 ± 70.58 7.85 ± 0.14 99.11 ± 2.94 9.39 ± 0.11
LDPE-MW-30% 15.90 ± 1.03 610.91 ± 90.49 8.20 ± 0.39 122.11 ± 5.30 8.13 ± 0.28
LDPE-MW-50% 17.18 ± 0.22 704.29 ± 89.54 8.76 ± 0.14 123.40 ± 4.92 6.60 ± 0.41

observed for impact strength of LDPE-MW composites where
impact strength decreases with the addition of marble waste par-
ticulates. The reduction in impact strength with reinforcing mate-
rial content may attributed to the brittle nature of marble waste
particulates. The variations in size of the particulates also reduces
ability to absorb and dissipate energy uniformly hence, responsible
for fracture [57].
3.2.2. FE-SEM analysis
The insight of all the injection moulded LDPE-MW composites
at two different melt temperatures (110 °C and 140 °C) are shown
in Fig. 3 (a, b). The fractured surfaces obtained after tensile test was
used for microstructure analysis. In the morphological images of
pure LDPE (Fig. 3b, 0%) smooth surface was visible which indicates
proper melting of LDPE at 140 °C. However at 110 °C (Fig. 3a, 0%)

Fig. 3. FE-SEM images of LDPE-MW composites: (a) 110 °C (b) 140 °C.

6
A. Khan, R. Patidar and A. Pappu Construction and Building Materials xxx (xxxx) xxx

slight rough surface was visible due to improper melting of LDPE.
The well adhesion between reinforcing material and polymer
was observed in Fig. 3 (b, 20%) . The good adhesion between rein-
forcing material and polymer was achieved due to well dispersion
of reinforcing material with the polymer without any agglomera-
tion which in turn responsible for the improvement in the mechan-
ical strength. Moreover the difference in the amount of reinforcing
material can be observed in Fig. 3 (a, b).
3.2.3. FTIR analysis
The FTIR spectra of LDPE-MW composites at two different melt
temperatutres (110 °C and 140 °C) have been shown in Fig. 4 (a, b).
The peaks observed at 2915 cm 1, 2848 cm 1, 1463 cm 1 and
1377 cm 1 were attributed to CH2 asymmetric, CH2 symmetric,
bending deformation and CH3 symmetric deformation vibrations,
respectively. The bands obtained at 729 cm 1 and 719 cm 1 were
ascribed to the deformation vibrations [59] and [60]. At both the
temperatures, LDPE-MW-20% and LDPE-MW-50% showed some
additional peaks as compared to neat LDPE due to presence of mar-
ble waste particulates in the composites. These peaks corresponds
to magnesium oxide and carbonates. Moreover, the band obtained
at 1463 cm 1 in composites was broader as compared to neat LDPE
sample. The difference in the intensity of these additional peaks
varries with the reinforcing material.
3.2.4. Thermal conductivity
The thermal conductivity recorded for LDPE-MW composites at
two different melt temperatures have been shown in table 4. Ther-
mal conductivity analysis was carried out to measure the heat
resistance of composites. It is clear from the results of thermal con-
ductivity of LDPE-MW composites that with the addition of marble
waste particulates thermal conductivity increases, which indicates
that marble waste particulates are well dispersed in the matrix
system which provide crystalline and better medium for heat to
transfer [61]. The obtained results showed slight variations in the
thermal conductivity values and indicates that values are almost
constant. However at higher temperature (140 °C) the thermal
conductivity was found to be more as compared to lower temper-
ature (110 °C) which was due to proper melting and mixing of
polymer with the reinforcing material. At temperature 110 °C,
the highest thermal conductivity (0.38 ± 0.004) was obtained for
LDPE-MW-50% while at 140 °C the highest thermal conductivity
was found to be 0.45 ± 0.008 for LDPE-MW-50%.

4. Conclusions

The following conclusions have been drawn from this study:

1. The fabricated composites showed improved mechanical

strength as compared to neat LDPE and reduced the amount
of polymer (plastic) by incorporating marble waste, resulting
in high strength composites.
2. Flexural strength and thermal conductivity of LDPE-MW com-
posites increased with the addition of marble waste
particulates.
3. About 55% enhanced flexural strength and 45% enhanced ther-
mal conductivity was observed with the addition of 50% marble
waste particulates.
4. The microstructure analysis showed very good bonding
between particulates and matrix. The characteristics band of
LDPE with additional bands of marble waste were observed
through FTIR.
5. Obtained flexible composites have potential to use for multi-
functional applications in which more than 50% marble waste
can be used as a filler and reinforcing materials.
6. Large quantity of marble waste generated during marble pro-
cessing can be utilised for fabrication of LDPE-MW composites.
This alternative solution can minimize precarious effect of mar-
ble waste disposal and its environmental pollution.
Fig. 4. FTIR graph of LDPE-MW composites (a) 110 °C (b) 140 °C.

Table 4
Thermal conductivity of LDPE-MW Composites (110 °C & 140 °C).

Thermal conductivity (W/mK)

Replication 110–0% 110–15% 110–50% 140–0% 140–15% 140–50%
1 0.33 0.36 0.38 0.30 0.42 0.44
2 0.33 0.37 0.38 0.30 0.41 0.44
3 0.33 0.37 0.38 0.32 0.40 0.46
Mean 0.33 0.37 0.38 0.31 0.41 0.45
SD 0.001 0.004 0.004 0.009 0.007 0.008

7
A. Khan, R. Patidar and A. Pappu
CRediT authorship contribution statement
Anam Khan: Experimentation, testing, Data curation, Writing -
original draft finalysing and submission of the manuscript, Soft-
ware. Ravi Patidar: Exprimentation, Data curation, Software. Aso-
kan Pappu: Supervision, Conceptualization, Methodology,
Visualization, Writing - review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgement
Authors are thankfull to Dr. A.K. Shrivastava, Director CSIR-
AMPRI and Dr. Krishnakanth Pulicherla DST New Delhi for the
moral and financial support. First author is thankful to Dr. SAR
Hashmi, coordinator, AcSIR, India. The assistance provided by Dr.
MK Gupta, Dr. Edward Peters and others are thankfully
acknowledged.
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.conbuildmat.2020.121229.
References
[1] P. Asokan, M. Saxena, S.R. Asolekar, Hazardous jarosite use in developing non-
hazardous product for engineering application, J. Hazard. Mater. 137 (2006)
1589–1599.
[2] D. Gosh, U. Bhattacharyya, Solid Waste Hazards and Strategies for Better
Management in India, Int. J. Inf. Res. Rev. 2 (2015) 420–425.
[3] D. Eliche-Quesada, F.A. Corpas-Iglesias, L. Pérez-Villarejo, F.J. Iglesias-Godino,
Recycling of sawdust, spent earth from oil filtration, compost and marble
residues for brick manufacturing, Constr. Build. Mater. 34 (2012) 275–284.
[4] E.A. El-Alfi, R.A. Gado, Preparation of calcium sulfoaluminate-belite cement
from marble sludge waste, Constr. Build. Mater. 113 (2016) 764–772.
[5] A.K. Thakur, A. Pappu, V.K. Thakur, Resource efficiency impact on marble waste
recycling towards sustainable green construction materials, Curr. Opin. Green
Sustain. Chem. 13 (2018) 91–101.
[6] H. Chen, H. He, S. Tian, S. Chen, Recycling of waste artificial marble powder in
HDPE-wood composites, Polym. Compos. 39 (2016) 2347–2355.
[7] C. Borsellino, L. Calabrese, G. Di Bella, Effects of powder concentration and type
of resin on the performance of marble composite structures, Constr. Build.
Mater. 23 (2009) 1915–1921.
[8] A. Sharma, A. Patnaik, Experimental Investigation on Mechanical and Thermal
Properties of Marble Dust Particulate-Filled Needle-Punched Nonwoven Jute
Fiber/Epoxy Composite, Jom. 70 (2018) 1284–1288.
[9] M.E. Çınar, F. Kar, Characterization of composite produced from waste PET and
marble dust, Constr. Build. Mater. 163 (2018) 734–741.
[10] J.L. Sales, C.R.S. Morais, L.M.R. Lima, J.L. Araújo, J.C.B. Cibalde, Characterization
of ceramic composite waste of granite, marble and caulim for production of
coating plates, Mater. Sci. Forum. 798–799 (2014) 300–305.
[11] C.E.G. Ribeiro, R.J.S. Rodriguez, Influence of compaction pressure and particle
content on thermal and mechanical behavior of artificial marbles with marble
waste and unsaturated polyester, Mater. Res. 18 (2015) 283–290.
[12] D. Gokdai, A.A. Borazan, G. Acikbas, Effect of Marble: Pine Cone Waste Ratios
on Mechanical Properties of Polyester Matrix Composites, Waste and Biomass
Valorization. 8 (2017) 1855–1862.
[13] C.E. Gomes Ribeiro, R.J. Sanchez Rodriguez, E.A. D. Carvalho, Microstructure
and mechanical properties of artificial marble, Constr. Build. Mater. 149 (2017)
149–155.
[14] A.A. Borazan, D. Gokdai, Polymer composites reinforced with waste marble
dust and fibers from chicken feathers as an alternative material, Fresenius
Environ. Bull. 26 (2017) 2095–2103.
[15] K. Ahmed, S.S. Nizami, N.Z. Raza, F. Habib, The effect of silica on the properties
of marble sludge filled hybrid natural rubber composites, J. King Saud Univ. -
Sci. 25 (2013) 331–339.
[16] M.G. Icduygu, L. Aktas, M.C. Altan, Characterization of composite tiles
fabricated from poly (ethylene terephthalate) and micro marble particles
reinforced by glass fiber mats, Polym. Compos. 33 (2012) 1921–1932.
8
Construction and Building Materials xxx (xxxx) xxx
[17] G. Ahmetli, M. Dag, H. Deveci, R. Kurbanli, Recycling studies of marble
processing waste: composites based on commercial epoxy resin, J. Appl Polym
Sci. 125 (2011) 24–30.
[18] P.S. Singh, R.K. Yadav, Effect of marble dust on index properties of black cotton
soil, Int. J. Engg. Res. & Sci. & Tech. 3 (2014) 158–163.
[19] A. Saygili, Use of waste marble dust for stabilization of clayey soil,
Medziagotyra. 21 (2015) 601–606.
[20] Patel Bindiyaben Bharatbhai, H.B. Prof, Dr Thakar, H.R. Varia, C.B. Prof, Mishra,,
Use of Waste Marble Powder to improve the Characteristics of Black Cotton
Soil, Int. J. Eng. Res. V 6 (2017) 817–821.
[21] S.E. Ghazy, A.H.M. Gad, Lead separation by sorption onto powdered marble
waste, Arab. J. Chem. 7 (2014) 277–286.
[22] M. Bhalothia, N. Suman, P.K. Baroliya, R. Dashora, A.K. Goswami, Marble slurry
waste as a scavenger material for Cr(III) ions from aqueous medium, Desalin.
Water Treat. 57 (2016) 17377–17383.
[23] B. Godboley, P. Nagarnaik, Marble powder: An adsorbent for removal of
fluoride from aqueous solution, Int. J. Civ. Eng. Technol. 7 (2016) 41–50.
[24] Z. Khan, M. Umar, K. Shahzada, A. Ali, Utilization of marble dust in fired clay
bricks, J. Environ. Monit. XVI I (2017) 4–10.
[25] N. Bilgin, H.A. Yeprem, S. Arslan, A. Bilgin, E. Günay, M. Maroglu, Use of waste
marble powder in brick industry, Constr. Build. Mater. 29 (2012) 449–457.
[26] M.J. Munir, S.M.S. Kazmi, Y.F. Wu, A. Hanif, M.U.A. Khan, Thermally efficient
fired clay bricks incorporating waste marble sludge: An industrial-scale study,
J. Clean. Prod. 174 (2018) 1122–1135.
[27] Nitisha Sharma, Ravi Kumar, Use of Waste Marble Powder as Partial
Replacement in Cement Sand Mix, Int. J. Eng. Res. V 4 (2015) 501–504.
[28] Asokan Pappu, Vijay K Thakur, Ravi Paditar, Asolekar R Shyam, Mohini Saxena,
Recycling marble wastes and Jarosite wastes into sustainable hybrid
composite materials and validation through Response Surface Methodology,
J.Clean Prod. 240 (2019) 118248, https://doi.org/10.1016/j.
jclepro.2019.118249.
[29] K. Vardhan, S. Goyal, R. Siddique, M. Singh, Mechanical properties and
microstructural analysis of cement mortar incorporating marble powder as
partial replacement of cement, Constr. Build. Mater. 96 (2015) 615–621.
[30] F.A. Selim, F.S. Hashem, M.S. Amin, Mechanical, microstructural and acid
resistance aspects of improved hardened Portland cement pastes
incorporating marble dust and fine kaolinite sand, Constr. Build. Mater. 251
(2020) 118992.
[31] N. Patel, A. Raval, J. Pitroda, Marble waste: Opportunities for development of
low cost concrete, Glob. J. Res. Anal. 2 (2013) 2277–8160.
[32] A.N. Bdour, M.S. Al-Juhani, Utilisation of waste marble powder in cement
industry, Int. J. Environ. Waste Manag. 11 (2013) 399–409.
[33] H.Y. Aruntasß, M. Gürü, M. Dayi, I. Tekin, Utilization of waste marble dust as an
additive in cement production, Mater. Des. 31 (2010) 4039–4042.
[34] B. Ercikdi, G. Külekci, T. Yilmaz, Utilization of granulated marble wastes and
waste bricks as mineral admixture in cemented paste backfill of sulphide-rich
tailings, Constr. Build. Mater. 93 (2015) 573–583.
[35] O. Kelesßtemur, E. Arici, S. Yildiz, B. Gökçer, Performance evaluation of cement
mortars containing marble dust and glass fiber exposed to high temperature
by using Taguchi method, Constr. Build. Mater. 60 (2014) 17–24.
[36] M. Sutcu, H. Alptekin, E. Erdogmus, Y. Er, O. Gencel, Characteristics of fired clay
bricks with waste marble powder addition as building materials, Constr. Build.
Mater. 82 (2015) 1–8.
[37] S. Kabas, A. Faz, J.A. Acosta, R. Zornoza, S. Martínez-Martínez, D.M. Carmona, J.
Bech, Effect of marble waste and pig slurry on the growth of native vegetation
and heavy metal mobility in a mine tailing pond, J. Geochemical Explor. 123
(2012) 69–76.
[38] F. Moreno-Barriga, V. Díaz, J.A. Acosta, M.Á. Muñoz, Á. Faz, R. Zornoza, Organic
matter dynamics, soil aggregation and microbial biomass and activity in
Technosols created with metalliferous mine residues, biochar and marble
waste, Geoderma. 301 (2017) 19–29.
[39] R. Melgar-Ramírez, V. González, J.A. Sánchez, I. García, Effects of application of
organic and inorganic wastes for restoration of sulphur-mine soil, Water. Air.
Soil Pollut. 223 (2012) 6123–6131.
[40] C. Pérez-Sirvent, M.L. García-Lorenzo, M.J. Martínez-Sánchez, M.C. Navarro, J.
Marimón, J. Bech, Metal-contaminated soil remediation by using sludges of the
marble industry: Toxicological evaluation, Environ. Int. 33 (2007) 502–504.
[41] Y. Ji, X. Rong, H. Zhong, Y. Wang, S. Wang, L. Lu, Making Marble Powder Waste
Profitable by Using Nano-TiO2 Surface Modification for Air Quality
Improvement Applications, J. Nanomater. 2017 (2017) 1–6.
[42] C.J. Cobo-Ceacero, M.T. Cotes-Palomino, C. Martínez-García, J.M. Moreno-
Maroto, M. Uceda-Rodríguez, Use of marble sludge waste in the manufacture
of eco-friendly materials: applying the principles of the Circular Economy,
Environ Sci Pollut Res. 26 (2019) 35399–35410.
[43] R. Zornoza, A. Faz, D.M. Carmona, S. Martínez-martínez, J.A. Acosta, Plant Cover
and Soil Biochemical Properties in a Mine Tailing Pond Five Years After
Application of Marble Wastes and Organic Amendments, Pedosphere. 22
(2012) 22–32.
[44] H.A. El-Sayed, A.B. Farag, A.M. Kandeel, A.A. Younes, M.M. Yousef,
Characteristics of the marble processing powder waste at Shaq El-Thoaban
industrial area, Egypt, and its suitability for cement manufacture, HBRC J. 14
(2018) 171–179.
[45] G. Marras, A. Bortolussi, R. Peretti, N. Careddu, Characterization methodology
for re-using marble slurry in industrial applications, Energy Procedia. 125
(2017) 656–665.
A. Khan, R. Patidar and A. Pappu
[46] S. Yesßilay, M. Çakı, H. Ergun, Usage of marble wastes in traditional artistic
stoneware clay body, Ceram. Int. 43 (2017) 8912–8921.
[47] T. Kavas, A. Olgun, Properties of cement and mortar incorporating marble dust
and crushed brick, Ceram. - Silikaty. 52 (2008) 24–28.
[48] S. Firat, J.M. Khatib, G. Yilmaz, A.T. Comert, Effect of curing time on selected
properties of soil stabilized with fly ash, marble dust and waste sand for road
sub-base materials, Waste Manag. Res. 35 (2017) 747–756.
[49] A. Mlayah, S. Jellali, Study of continuous lead removal from aqueous solutions
by marble wastes: efficiencies and mechanisms, Int. J. Environ. Sci. Technol. 12
(2015) 2965–2978.
[50] T. Gatta, E. Gregori, F. Marini, M. Tomassetti, G. Visco, L. Campanella, New
approach to the differentiation of marble samples using thermal analysis and
chemometrics in order to identify provenance, Chem. Cent. J. 8 (2014) 1–9.
[51] L. Campanella, C. Costanza, M. Tomassetti, S. Vecchio, Kinetic processing of
thermoanalytical curves of cellulose samples and finds assessment of possible
archaeometric applications, Curr. Anal. Chem. 6 (2010) 260–268.
[52] P.G. Caceres, E.K. Attiogbe, Thermal decomposition of dolomite and the
extraction of its constituents, Miner. Eng. 10 (1997) 1165–1176.
[53] D. Mehta, P. Mondal, S. George, Utilization of marble waste powder as a novel
adsorbent for removal of fluoride ions from aqueous solution, J. Environ. Chem.
Eng. 4 (2016) 932–942.
[54] J. Lu, X. Cong, Y. Li, Y. Hao, C. Wang, High strength artificial stoneware from
marble waste via surface modification and low temperature sintering, J. Clean.
Prod. 180 (2018) 728–734.
Construction and Building Materials xxx (xxxx) xxx
[55] B.K. Shahraki, B. Mehrabi, R. Dabiri, Thermal behavior of Zefreh dolomite mine
(Centeral Iran), J. Min. Metall. Sect. B Metall. 45 (2009) 35–44.
[56] S.O. Adeosun, M.A. Usman, E.I. Akpan, W.I. Dibie, Characterization of LDPE
Reinforced with Calcium Carbonate—Fly Ash Hybrid Filler, J. Miner. Mater.
Charact. Eng. 02 (2014) 334–345.
[57] I. Abdel-Salam Sabah, M.S. Metwally, A.A. Abdel- Hakim, S. El Begawy, E.S.
Elshafie, Effect of Mineral Fillers on Rice Straw Fiber/High Density
Polyethylene Composites, Nat Sci. 9 (2011) 116–124.
[58] C.Y. Chee, N.L. Song, L.C. Abdullah, T.S.Y. Choong, A. Ibrahim, T.R. Chantara,
Characterization of mechanical properties: Low-density polyethylene
nanocomposite using nanoalumina particle as filler, J. Nanomater. 2012
(2012) 1–6.
_ Kaya, Conducting polymer composites based on
[59] F. Doğan, K. Sßirin, F. Kolcu, I.
LDPE doped with poly(aminonaphthol sulfonic acid), J. Electrostat. 94 (2018)
85–93.
[60] A. Popelka, I. Krupa, I. Novák, M.A.S.A. Al-Maadeed, M. Ouederni, Improvement
of aluminum/polyethylene adhesion through corona discharge, J. Phys. D.
Appl. Phys. 50 (2017).
[61] I. Krupa, I. Novák, I. Chodák, Electrically and thermally conductive
polyethylene/graphite composites and their mechanical properties, Synth.
Met. 145 (2004) 245–252.