Ceramics International 43 (2017) 8912–8921

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Ceramics International
journal homepage: www.elsevier.com/locate/ceramint

Usage of marble wastes in traditional artistic stoneware clay body MARK

a,⁎ b c
Selvin Yeşilay , Münevver Çakı , Hakan Ergun
a
Anadolu University, Faculty of Fine Arts, Glass Department, Eskisehir, Turkey
b
Anadolu University, Faculty of Fine Arts, Ceramic Department, Eskisehir, Turkey
c
Afyon Kocatepe University, Faculty of Fine Arts, Ceramic Department, Afyonkarahisar, Turkey

A R T I C L E I N F O A BS T RAC T

Keywords: Recycling of industrial wastes aids environmentally friendly production and has the advantage of lowering costs.
Marble waste Marble production generates large amounts of waste. Recycling of such wastes by incorporating them into
Waste management ceramic industry is a practical solution for pollution problem. The aim of this work is to assess the possibility of
Ceramic the recycling of marble wastes in the production of stoneware clay bodies as a raw material for ceramic artwork
Clay body
production. Five different clay body mixes containing marble waste up to 27% were prepared and evaluated for
Environment
firing color, water emission, morphology, microstructure, thermal expansion coefficient and thermal behavior.
Recycling
The results of the tests show that the utilization of marble waste in stoneware body is feasible for ceramic
artwork production.

1. Introduction
Industrial waste management constitutes one of the major global
problems of our times. Recycling of non-biodegradable waste is
particularly difficult. Ceramic waste has been classified in this group
[1,2].
Ceramic waste are hard, durable and extremely resistant to
chemical, physical and biological degradations and highly thermally.
It has been estimated that about 30% of the daily production in the
ceramic industry goes to waste. Nowadays, the ceramic industry creates
a significant amount of waste for disposal. These solid waste lead to
severe environmental pollution and significant land occupation. Huge
amount of ceramic waste (in the form of pellets and powder) is
produced in different stages such as grinding, cutting, dressing and
polishing inside the industrial plant. Wastes can be used to produce
new products or can be used as admixtures so that natural sources are
used more efficiently and the environment is protected from waste
deposits Recycling and reuse of waste materials suggest energy saving,
cost reduction, possibly superior products and less or no hazards to the
surrounding environment [3–6].
Marble is a metamorphic rock, such as limestone, that contains
largely calcium carbonate (CaCO3). Furthermore, in marble, small
amounts of silica, feldspar, iron oxide, mica, fluorine and organic
matters may be found [7]. It is one of the most extensively used
aesthetic stones [8]. Marble waste dust is an inert material which is
obtained as an industrial by product [9]. A 90% of dried marble slurry
having very fine dust is smaller than 200 µm in size [10].
Turkey has large deposits of high quality marble and is one of the
leading producers. Large quantities of wastes are produced in different
stages of marble quarrying and processing operation [11].
There are many studies on the use of natural stone (marble and
dolomite) wastes as reinforcement material or raw material in various
areas and applications [12–19]. Natural raw materials used in the
fabrication of clay-based ceramic products show a wide range of
compositional variations and the resulting products are very hetero-
geneous. Therefore, such products can tolerate further compositional
fluctuations and raw material changes, allowing different types of
wastes to be incorporated into the internal structure of ceramic tiles
and bricks as part of their own matrix. Some wastes are very analogous
in composition to the raw materials used, moreover they often contain
materials that can also be helpful in improving the fabrication of
ceramic products. Many attempts were made to incorporate solid
wastes into raw materials mixtures in order to produce different
ceramic products. Recent studies demonstrated the possibility of
incorporating marble and granite sludge slime as additives into clay-
based ceramic products [20–22].
A key issue for the recycling of solid waste material as an alternative
raw material in the ceramic field is the knowledge of its chemical,
mineralogical, and physical characteristics [23]. In this work we mainly
focused on the recycling of waste generated by marble industries. The
aim of this work is to study the possibility of the use of marble powder
waste generated in the Afyonkarahisar-Merdivenci Mermer Inc. of
Turkey, in ceramic mixtures, for manufacturing of stoneware clay
bodies. The effects due to the use of waste marble powder were

⁎
Corresponding author.
E-mail address: selvin.yesilay@gmail.com (S. Yeşilay).

http://dx.doi.org/10.1016/j.ceramint.2017.04.028
Received 1 November 2016; Received in revised form 5 April 2017; Accepted 5 April 2017
Available online 08 April 2017
0272-8842/ © 2017 Elsevier Ltd and Techna Group S.r.l. All rights reserved.
S. Yeşilay et al. Ceramics International 43 (2017) 8912–8921

Table 1 measured in both condition of air and water for dry weight (Dw) and
Recipes of the standard (STD1) and marble waste added bodies. wet weight (Ww). Then the water absorption has been calculated (2)
after the excessive water had been wiped off [25].
Raw Material STD R1 R2 R3
W (%) = [(Ww − Dw )/Dw] × 100 (2)
Sodium-feldspar 15 15 15 15
Potassium-feldspar 8 8 8 8 After firing, color changes and surface texture of bodies were
Quartz 7 7 7 – visually investigated. Then some experimental tests have been carried
Kaolin 20 10 – –
out with the ceramic clay bodies. Optical parameters of the samples
Marble Waste – 10 20 27
Fire Clay 10 10 10 10 were investigated by Minolta 3600-d spectrophotometer. Crystal
Clay 40 40 40 40 phases developed during firing were determined with X-ray diffraction
(XRD- Rigaku Rint 2000 Series) and scanning electron microscopy
(SEM- Zeiss EVO 50) techniques. In order to determine thermal
expansion coefficient values samples were heated in a dilatometer
investigated in laboratory experiments and discussed in terms of firing (Netzsch DIL 402 PC) at a rate of 10 °C/min up to 600 °C.
behavior and main physical–microstructural properties. After characterization tests, artistic applications were done by using
these standard and waste added stoneware clay compositions. In the
first application, tiles pressed in 15×15 cm dimensions. After drying,
2. Materials and methods alkali-boron-zinc glaze containing 3% CuCO 3 was applied on to
tiles which were conducted to biscuit firing at 1000 °C oven. Then
The typical stoneware clay body recipe (STD) that used by ceramic they fired at 1160 °C. In the second application, standard clay and
artists in their works was prepared with dry marble waste. In this study marble waste added clay compositions were mixed with electrolyte
very fine marble powder was used. It was obtained as a by-product of additive to obtain casting slurry. Andesite plates were selected for
marble sawing and shaping. Marble wastes were supplied from the the application. Andesite is a silica-containing (53–63%), fine-
facility in the form of sludge and then milled and sieved through 100 grained volcanic rock, with a color between grey and black [26].
mesh. After drying, they became ready to use as raw material. Andesite plates were gathered from the mine and cut in the factory
Firstly, XRF analyses of marble waste and the other raw materials to desired dimensions (1,5×15×30 cm). After cleaning their sur-
in the recipe were conducted in order to determine the chemical faces, andesite plates were surrounded by the tapes which have
compositions. Also XRD (X-ray powder diffraction), particle size and different thicknesses on all sides in order to obtain a reservoir for
hot stage microscope analyses of marble wastes were performed. casting. A prepared slurries poured into the reservoir in andesite
Throughout the whole study 3 different groups of clay body recipes plates and set aside until the slurry becomes as hard as skin.
in terms of waste content from 10, 20 and 27 wt% of marble waste was Benefiting from the porosity of andesite stone, some cracks were
selected and prepared. Standard and waste added stoneware body allowed during the drying process. The cracks were partly oriented
recipes were coded as STD, R1, R2 and R3 and their composition are by changing the direction of the drier. In order to obtain small
given in Table 1. cracks, thin slips and faster drying are used; thick slips are used for
In order to prepare stoneware clay bodies suitable amounts of Na- larger cracks. After the cracking and drying processes were com-
feldspar, K-feldspar, quartz, kaolin and marble waste with water were pleted, some of the cracked pieces were removed from the andesite
ground in a ball mill for 1 h and sieved through 100 mesh. This mixes tablet surface as a part of the designing project. Glaze was not
were dewatered by leaving them on plaster boards, then kneaded and applied between andesite muds and andesite plates. Andesite melts
plastic mud was obtained. Afterwards, the samples with the dimensions in 1160 °C when it is in powder form and andesite created semi-
of 200×20×15 mm were formed in a plaster mold for the shrinkage and vitreous surface when it is in the form of plates. Because of these
water absorption tests. After having been dried at 75 °C for 1 day, the properties, an interface was formed between stone and applied
samples were fired at 1160 °C for 7 h in a laboratory type electrical slurry [27,28].
furnace (soak time 10 min). Linear shrinkage and water absorption
values are directly related with open porosity, are properties easy to 3. Results and discussion
measure. The linear shrinkage, LS (%), of fired samples has been
determined by means of the following equation [24]: Chemical analysis of the raw materials and marble wastes used in
L − Lc the study are presented in Table 2. As it seen from the Table 2, the
LS= s × 100 waste is high in calcium oxide content, followed by magnesium oxide.
Ls (1)
Basically, the source of each waste material is recognized from the
All samples of each composition have passed through the water waste composition with regard to the rate of contamination in
absorption test after firing. The weight of the test samples has been processing and production methods [29].

Table 2
Chemical analysis of the raw materials and marble waste used in the bodies (wt%).

a
Raw Material SiO2 Al2O3 Fe2O3 CaO MgO Na2O K2O TiO2 L.O.I

Sodium feldspar 69,37 18,90 0,20 0,54 0,45 9,16 0,24 0,30 0,84
Potassium feldspar 70,08 15,37 0,20 0,55 0,05 2,51 10,65 – 0,59
Quartz 99,50 – – – – – – 0,07 0,43
Kaolin 57,58 26,75 1,38 0,37 0,52 0,82 0,33 0,67 11,58
Fire Clay 47,44 32,45 2,76 0,54 0,82 0,46 1,00 0,85 13,68
Clay 53,02 28,28 1,92 0,39 0,88 0,2 1,71 0,84 12,76
Marble Waste 0,52 – 0,10 53,51 1,66 0,09 – – 44,12

a
Loss on ignition.

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Fig. 1. XRD pattern of marble waste.

Fig. 2. The particle size distribution curve of marble waste.

Fig. 3. The hot stage microscope curve of marble waste.

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Table 3 Table 5
Water absorption and shrinkage values (%) of the fired stoneware bodies. Thermal expansion coefficient values (α) of the bodies at 400 °C.

RECIPE NO 1160 0C Sample Code α (10−6 1/K)

Total Shrinkage (%) Water Absorption (%) STD 53 ±

R1 58 ±
STD 9,6 6,6 R2 64 ±
R1 5,0 13,9 R3 63 ±
R2 4,6 14,5
R3 4,8 11,21

In XRD analyses of marble waste the calcite and dolomite was

observed (Fig. 1). According to the XRD results, the major crystal
phase is seen to be Calcite (CaCO3) for marble waste.
The particle size distribution curve of marble waste is given in
Table 4 Fig. 2. According to the results the average particle size of waste is
Optical parameters of the stoneware bodies fired at 1160 °C. 20,943 µm, d (0,1) value is 1,925 and d (0,9) value 76,925 µm.
From Fig. 3 the hot stage microscope analysis of marble waste
Recipe No L* a* b*
indicates the sintering and softening temperatures of waste being
STD 83,01 2,86 12,27 1073 °C and 1368 °C respectively.
R1 86,6 1,99 14,06 Water absorption and shrinkage values of all prepared stoneware
R2 86,66 1,77 19,97
bodies are given in Table 3. Water absorption rate has been used as
R3 85,36 1,21 13,39
an indication for porosity of the ceramic body [30]. The water
absorption capacity of the clay bodies increased with the increase of

Fig. 4. Firing colors of the standard and waste added stoneware clay bodies fired at 1160 °C.

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Fig. 5. Comparative dilatometer curves of standard and waste added stoneware bodies.
Fig. 6. XRD patterns of standard and waste added stoneware clay bodies.
waste addition up to % 20 ratio. Stoneware clay body with 27%
substitution of marble waste had lower water absorption than the
one containing 20% marble waste. It has been known that calcium
carbonates cause increase in porosity and water absorption and
decrease in density in clay [31]. From Table 3, it can be observed
that the total linear shrinkage was reduced with increasing marble
waste content. A presence of calcite waste decreases a sample
contraction during sintering [32,33].
Table 4 illustrates the optical parameters of fired bodies. It is clearly
seen that whiteness (L*) increased and redness (a*) decreased with the
increase of the waste input into bodies. Normally the firing color of
stoneware clays ranges from a very light grey or buff to a darker grey or
brown [34]. During the firing of clay of different chemical composition
different compounds are formed and this is the reason for a different
color of the ceramic body [35].
The photos of STD, R1, R2 and R3 coded unglazed forms fired at
1160 °C are depicted in Fig. 4.
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Thermal expansion coefficient values (α) of the bodies at 400 °C
changing between 52 and 63×10-6 1/K are listed in Table 5 and the
comparative curves are presented in Fig. 5. By increasing waste content
thermal expansion coefficient of the samples were increased. It was
considered that this increase was caused by the Calcium Oxide (CaO)
that was incorporated with marble waste to the composition, since it
causes an increase in expansion linked to humidity in the ceramic
bodies [36].
XRD patterns of the bodies are represented in Fig. 6. According to
the results quartz, mullite and small amount of anorthite phases are
present in the standard body fired at 1160 °C. When the waste was
added, XRD peak intensities of both quartz and mullite decreased
unlike anorthite ones increasing (noteworthy when 27% waste was
utilized). In the case of quartz this is normal since the level of silica in
the recipes decreased with waste incorporations. Higher amount of
CaO with such a compositional modification especially in the R3 recipe
was thought to be the reason for a possible interaction with some of
S. Yeşilay et al. Ceramics International 43 (2017) 8912–8921

Fig. 7. SEM images of (a) STD (b) R1, (c) R2 and (d) R3 coded stoneware clay bodies.

Fig. 8. EDX pattern taken from (a) STD (b) R1 (c) R2 (d) R3 stoneware bodies.

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Fig. 9. CaO-Al2O3-SiO2 phase diagram [38].
free quartz leading to more anorthite crystal formation. Additionally,
due to the higher fluxing oxide contents in the bodies the dissolution of
some mullite crystals may be occurring [37].
Fig. 7 shows scanning electron microscopy (SEM) micrographs of
the ceramic samples fired at 1160 °C, coded as STD, R1, R2 and R3.
These micrographs indicate that there is interconnected porosity,
which showed no preferential orientation or shape, and which in-
creased with increasing marble waste content in the ceramic samples of
these batches. The formation of needle-like mullite crystals supplying
mechanical strength to wares [37] worsens with waste additions.
EDX patterns taken from produced ceramics were presented in
Fig. 8.
After evaluating SEM, EDX and XRD results together, it was
concluded that adding waste to the recipe resulted increase in the
anorthite phase amount and decrease in the mullite and quartz amount.
STD, R1 and R2 glaze compositions are in the SiO2 −3Al 2O 3 .2SiO 2-
CaO.Al 2O 3 .2SiO 2 triangle in the CaO-Al2 O 3-SiO 2 phase diagram
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while R4 glaze composition is in the SiO 2-CaO.SiO 2 (wollastonite)
-CaO.Al2 O 3.2SiO 2 (anorthite) triangle (Fig. 9). When the positions
in the phase diagram of the compositions are evaluated according
to the firing temperatures, it is expected that the anorthite +
mullite + liquid phase will be formed for STD, R1 and R2
compositions depending on the amount of increased marble
waste. Depending on the increasing amount of marble waste, the
amount of anorthite increases while position in the phase diagram
shifts to the anorthite theoretical composition, while the amount of
mullite decreases. The quartz detected in the compositions shows
that the quartz added at the beginning cannot enter the reaction
because the firing temperature is relatively low [38].
At the end of the study, ceramic artworks produced by using
standard clay and waste added clay recipes presented in Fig. 10.
It has been seen that all clay bodies which contains marble waste in
different ratios can be shaped by both pressing and slip casting
techniques.
S. Yeşilay et al. Ceramics International 43 (2017) 8912–8921

Fig. 10. Artistic ceramics produced by (a) pressing and (b) slip casting.

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Fig. 10. (continued)
4. Conclusion
The present study proved the feasibility of the use of significant
amounts of marble waste as an additive in stoneware ceramic
manufacturing for artistic purposes.
Firing color of clays seems to be influenced by clay micro-structure.
Firing colors change to darker tones with waste addition. Ratio of the
waste used, properties and amount of the other components in the
recipe have an effect on the color. Clay properties in terms of the
plasticity and shaping capability are very important. It was concluded
that these wastes could be evaluated in the stoneware clay body up to
27% without causing any deterioration in the dimensional stability of
the products. The incorporation of marble wastes in stoneware clay
body production gives environmentally friendly recycling products. It is
also suggested that the waste can be utilized in the production of other
traditional ceramics and forms.
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Acknowledgments
The authors would like to thank Anadolu University, Scientific
Research Projects Administration Unit for supporting the project
numbered 1505E358.
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