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Results in Materials 11 (2021) 100195

Contents lists available at ScienceDirect

Results in Materials
journal homepage: www.sciencedirect.com/journal/results-in-materials

Physical and mechanical properties of porcelain tiles made from raw


materials in Uganda
William Ochen a, *, Florence Mutonyi D’ujanga b, Bosco Oruru b, Peter Wilberforce Olupot c
a
Physics Department, Kyambogo University, P.O Box 1, Kyambogo, Uganda
b
Physics Department, Makerere University, P.O Box 7062, Kampala, Uganda
c
Mechanical Engineering Department, Makerere University, P.O Box 7062, Kampala, Uganda

A R T I C L E I N F O A B S T R A C T

Keywords: This study was intended to determine the physicomechanical properties of porcelain tiles made from raw ma­
Porcelain tile terials in Uganda, hitherto not used for the same. The raw materials were mixed in proportions of 40–60% clays,
Flexural strength 30–40% feldspar and 10–30% sand, the goal was to identify a mixture with properties that meet the ISO 13006
Water absorption
standards after firing. Test tile samples were formulated at a pressure of 40 MPa and fired from 1050 to 1250 ◦ C
Mullite fibers
Linear shrinkage
in steps of 50 ◦ C. A firing rate of 40 ◦ C per minute and a dwell time of 2 h were applied. The microstructures and
Uganda phase analysis of the fired samples were studied using a scanning electron microscope (SEM) and X-ray
diffractometer (XRD), respectively. The XRD analysis revealed mullite and quartz as crystalline phases present in
the fired bodies. At 1150 ◦ C, the SEM micrograph depicted few, short and thick mullite fibers. At 1200 ◦ C, the
mullite population increased. The nature of the fibers (long, fine and more interlocking) resulted in an increase in
flexural strength. A further rise in temperature had no significant change on the nature of the fibers and flexural
strength of the samples. The best properties; flexural strength (33 MPa) and water absorption (0.08%) were
exhibited at 1200 ◦ C by samples with 30–40% kaolin, 30–40% feldspar, 20% ball clay and 10% sand. The results
indicate that these samples are comparable to the ISO 13006 standards for porcelain tiles which are ≥ 35±2 MPa
flexural strength and <0.5% water absorption. The other mix proportions did not meet these standards, spe­
cifically in terms of flexural strength (<25 MPa).

1. Introduction at a temperature of about 980 ◦ C. The liquid phase formed facilitates


vitrification through liquid state sintering mechanism [5]. Also, it helps
Porcelain tiles are vitreous ceramic products made of clay (kaolin to lower the kiln temperature during firing hence saving energy there­
and ball clay), feldspar and sand. The industrial production of these tiles fore, lowering the cost of the final product. Finally, sand (SiO2) is a filler
consists of milling and homogenization, uniaxial pressing at 40–50 MPa material, it reduces warping of the fired product [7]. Using X-ray fluo­
and fast firing at 1180–1220 ◦ C [1,2]. Porcelain tiles are known to have rescence method, it was possible to quantify these materials, the results
a high flexural strength of greater than 35± 2 MPa, and low water ab­ are recorded in Table 1.
sorption (<0.5%) which makes them suitable for both indoors and out The production of ceramic tiles has been increasing every year. In
door application either as floor or wall tiles [3,4]. The raw materials 2017, about 13.5 million square meters were produced globally giving a
used in these tiles have different roles. Ball clay helps in shaping by rise of 5% compared to 2012. In Africa, 0.7 million square meters were
providing plasticity. It also improves on dry mechanical strength [5]. produced giving an increase of 43% compared to 2013 [1]. In compar­
Kaolin clay (Al2O3Si2O5(OH)4) is the major source of kaolinite mineral ison to other types of ceramic tiles, porcelain tiles constitute one of the
that is expressed chemically as Al2O3 2 SiO2 2H2O. When fired at tem­ most complex ceramic materials. For this reason, it is studied widely in
peratures greater than 1100 ◦ C, it crystallizes into mullite fibers (3 Al2O3 relation to the firing conditions, material composition, phase and
2 SiO2). As a result, flexural strength is increased according to the microstructural evolution [8]. In the previous study [2], it was high­
mullite hypothesis [6]. Feldspar (KxNa1.x(AlSi3)O8) is a silicon alumi­ lighted that a better understanding of the properties of porcelains is
nate of alkali earth metals, it is a flux agent. When fired, it starts to melt needed most especially in relation to the mix proportions of the raw

* Corresponding author.
E-mail address: wocen@kyu.ac.ug (W. Ochen).

https://doi.org/10.1016/j.rinma.2021.100195
Received in revised form 8 April 2021; Accepted 27 April 2021
Available online 25 May 2021
2590-048X/© 2021 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
W. Ochen et al. Results in Materials 11 (2021) 100195

Table 1 Table 2
Chemical composition of the raw materials. Mix proportions of formulated tile samples.
Oxide Raw Materials Raw materials Composition of the body (wt.%)

Kaolin (%) Feldspar (%) Sand (%) Ball clay (%) 1 2 3 4

SiO2 56.6 64.6 91.7 65.7 Ball clay 20 20 20 20


Al2O3 31.3 19.6 2.9 17.1 Kaolin 40 30 20 20
F e2O3 0.7 0.2 1.7 2.7 Feldspar 30 40 40 30
N a2O 0.3 1.0 0.5 0.3 Sand 10 10 20 30
K2O 1.8 10.1 0.5 0.8 Total 100 100 100 100
Ca2O 0.8 0.3 2.3 0.3
T i2O 0.1 0.6 0.3 1.9
M gO 0.3 0.4 0.7 0.3
LOI 10.4 2.3 1.7 8.0

materials and the process methods. This is necessary to improve their


mechanical strength.
In Uganda, ball clay is mainly used for making building bricks,
charcoal stoves and flower pots among others. Kaolin is used for making
paint, no commercial use is known for feldspar so far. Sand is used in
construction where it is mixed with cement, gravel and water to form
concrete. Lack of the required technology and equipment, high cost of
electricity, and lack of interest from government has hampered the local
production of porcelain tiles. Currently, these tiles are imported from
Europe, India, South East Asia and South Africa. Moreover, the country
is well endowed with the raw materials needed to make high quality
porcelain ware [9,10]. The objective of this study is to contribute to the
potential use of mineral resources from Uganda, hitherto not used
before. But also, to establish a mixture formulation and firing temper­
ature for successful application in porcelain tiles. The tiles will be
Fig. 1. Composition diagram of triaxial ceramic products including porcelain
evaluated based on ISO 13006 standard, and discussed in terms of
floor tiles [2,12].
microstructure and phase evolution.

2. Materials and methods triaxial ceramic products where porcelain tiles are included.

2.1. Location of the deposits 2.3. Sample formulation

The four raw materials: kaolin, feldspar, ball clay and sand were The mix proportions (Table 2) were homogenized for 1 h using a ball
sourced locally from selected deposits in Uganda. Kaolin was got from mill containing plastic balls a mixing media. A moisture content of 12 wt
Mutaka deposit in Bushenyi District, located in Western Uganda. Feld­ % was added, and the mixture was again homogenized for 30 min. Then,
spar was sourced from Lunya deposit in Buikwe District, located in 110 g was measured and poured in a rectangular steel mold, then a
Central Uganda. Ntawo deposit located in Mukono District and Lido pressure of 40 MPa was applied to form specimens measuring 110 × 50
beach in Wakiso District provided ball clay and sand, respectively, both × 10 mm. The green samples were left to dry in air for two days to avoid
deposits are located in Central Uganda. The chemical composition of cracking. They were later fired at peak temperatures of 1050–1250 ◦ C in
these raw materials was carried out using X-ray fluorescence (XRF) steps of 50 ◦ C, using a fast firing rate of 40 ◦ C per minute. During firing,
method, and the results can be seen in Table 1. the samples were soaked for 2 h at every peak temperature. Afterwards,
the furnace was switched off and the samples were left to cool naturally
2.2. Processing of raw materials in order to avoid macroscopic residual stresses [2]. The fired samples are
shown in Fig. 2.
From the deposits, about 50 kgs of each raw material was mined.
Sand was dried and then pulverized using a ball mill (Retsch PM 100) 2.4. Characterization of samples
that was running at a speed 350 rpm. The ball mill contained twenty two
steel balls of 14 mm in diameter as the grinding media. Afterwards, the 2.4.1. Microstructure and phase analysis
milled body was dry sieved using 45 μm mesh size. Ball clay was soaked Microstructural analysis of the fired specimens was carried out using
in water for about five days, to allow impurities to settle at the bottom of a FEG-SEM instrument, LEO 1530 with a GEMINI column. Sectioned and
the vessel. The suspension was poured on a plaster of paris in order to polished specimens of the fired tiles were used for the investigation. The
absorb water. Afterwards, it was dried under direct sunlight, and the dry specimens were polished, cleaned and dried. Thereafter, they were
sample was milled and sieved using a 45 μm mesh size. Kaolin was dipped in 40% concentrated hydrochloric acid for 25s, cleaned, dried
mined in form of a white powder. It was dry sieved using 300 μm mesh to and studied using FEG-SEM instrument. The cleaning procedures given
remove foreign bodies such as small stones, metallic objects and plastics. to all specimens before examination included washing in water and
It was then passed through a mesh size of 53 μm. Feldspar was sieved alcohol before drying.
using a mesh size of 80 μm to form fine powder. The sieve sizes used Phase analysis of the fired porcelain samples was determined by X-
were selected based on particle size that exhibited improvement on the ray diffraction using an X’pert PRO PANalytical X-ray diffractometer,
strength of porcelains [6,11]. The powder samples were then mixed PW 3050/60, with Ni-filtered K ~ Cu-radiation generated by a 40 kV
according to the designed proportions illustrated in Table 2. These acceleration voltage and a 40 mA anode current. Pulverized specimens
proportions were chosen based on a trial and error approach. But also, it were scanned from 10 to 75◦ operating the equipment at a 2θ scan speed
was guided using Fig. 1, which represents compositions of typical of 0.5 s/step and a 2θ step size of 0.02◦ . The X-ray peaks of the different

2
W. Ochen et al. Results in Materials 11 (2021) 100195

Fig. 2. Visual aspect of the tile samples fired at 1050–-1250 ◦ C.

phases were identified with the software of the equipment.


Dg − Df
L.S = x 100% (1)
Dg
2.4.2. Physical properties
The physical properties of fired samples were based on texture, color,
where Dg is the dimension of the green body and Df is that of fired sample
linear shrinkage and water absorption. Texture was studied by feeling
in millimeters. The water absorption, W.A, was determined according to
using bare hands, while color was analyzed by observation using un­
ASTMC 373-88 standard for materials testing. Here, the mass of the fired
aided eyes. In linear shrinkage, L.S, the dimensions of the green and fired
samples, M1, was measured. The samples were then boiled in distilled
samples were measured using a caliper. The linear shrinkage was eval­
water for 2 h, and soaked for 24 h at room temperature. After impreg­
uated using Equation (1) [12,13].
nation, the mass of the saturated samples, M2, was measured. The water

3
W. Ochen et al. Results in Materials 11 (2021) 100195

absorption expresses a relationship between the mass of water absorbed


to that of the dry sample, it was calculated using Equation (2) [13,14].
M2 − M1
WA = x100% (2)
M1

2.4.3. Mechanical property


This was based on the flexural strength of fired samples. A three
point flexure tests method was applied. A loading force, P, at a rate of 2
mm per minute was directed to the center of the test sample. It’s value
was recorded at a point of failure of the test sample. Flexural strength
was calculated as the modulus of rupture (MOR) using a span length of
70 mm. The MOR was evaluated using Equation (3) [12,15].
3PL
MOR = (3)
2bt2

where L is the span length, b is the breadth and t is the thickness of the
test sample in millimeters.

3. Results and discussion


Fig. 4. XRD patterns for all compositions fired at 1200 ◦ C.
3.1. Microstructure and XRD analysis
The figure shows that only mullite and quartz appear as crystalline
The microstructures of selected samples fired at 1150–1250 ◦ C are
phases. The patterns practically demonstrate identical peaks for all the
shown in Fig. 3. From the figure, the microstructures consist of mullite
compositions fired at 1200 ◦ C. Thus, the crystalline phases formed have
fibers (denoted as M), quartz crystals (denoted as Q) and pores seen as
equal quantities in the fired samples. At 2θ = 20–30◦ , there is a bump for
dark spots. As expected, the morphology of the pores changed with
all the compositions corresponding to the glass phase. As a result, one is
firing temperature. At 1150 ◦ C, due to a low amount of molten sub­
expected to find the same amounts of glass in all the samples.
stance, large and interconnected pores are formed (Fig. 3a and b). As a
result, the samples exhibited high water absorption (3.6%) and low
strength (20 MPa). Fig. 3c–e shows a denser and pore free microstruc­ 3.2. Physical properties
ture for samples fired at 1200 ◦ C. It is associated with liquid state sin­
tering where a large quantity of liquid substance glues the pores and the The texture of fired samples was smooth. Their color changed from
particle that did not dissolve during firing. This results in a vitreous body white to brown and then to gray as illustrated in Fig. 2. This observation
with water absorption of 0.08%. is due to thermal reaction of the impurities such as iron II oxide and
The nature of the mullite fibers formed was also affected by a rise in titanium dioxide present in ball clay (Table 1) [3]. The gresification
the firing temperature [16,17]. At 1150 ◦ C, the fibers appear short, thick diagram (Fig. 5a–b) is used to describe the densification of fired tile
and less interlocking as illustrated in Fig. 3b. According to Iqba and Lee samples. It illustrates the variation of linear shrinkage and water ab­
[5], this crystalline phase is called primary mullite fibers. Porcelains that sorption with firing temperature. As can be seen, linear shrinkage in­
experience this type of crystalline phase are known to have low strength creases with temperature however, it decreases sharply for compositions
compared to those with secondary mullite fibers. This explains why 3 and 4 (20–30% sand) at 1250 ◦ C. This as anticipated is expected to
samples fired at 1150 ◦ C and below had low strength and therefore did reduce shrinkage at high temperatures when the fluxing effect of feld­
not satisfy the ISO 13006 standards. At 1200 ◦ C, the population of the spar and clay cease to be dominant. For compositions 1 and 2, when
fibers increased, they are longer, finer and more interlocking (Fig. 3c–e). sintered at 1200 ◦ C, they exhibited linear shrinkage in a range of
A further rise in temperature however, had no significant effect on the 8.1–8.7% which is in accordance with the limits reported for floor tiles
nature of the fibers (Fig. 3f). Carty and Senapati [8] classify this type of [19]. In addition, the tile samples were highly vitreous with water ab­
fibers as secondary mullites. Their high interlocking ability is a reason sorption of about 0.08% in a temperature range of 1200–1250 ◦ C. This is
for the high mechanical strength of the materials (>30 MPa) [18]. due to the formation of an abundant liquid phase that infiltrates the
The XRD patterns of the samples fired at 1200 ◦ C are shown in Fig. 4. open pores of the structure and causes densification via liquid state
sintering. This value of water absorption is less than the value of 0.5%
required by ISO 13006 for porcelain floor tiles [4].

3.3. Mechanical property

Fig. 5c illustrates a variation in flexural strength with firing tem­


perature for different compositions. The results can be grouped into two,
thus compositions 1 and 2 (group A) contains 10% sand, kaolin and
feldspar in a range of 30–40%, and 20% ball clay. Compositions 3 and 4
constitute group B that contains sand in a range of 20–30%, kaolin and
feldspar in a range of 20–40% and 20% ball clay (Table 2). Flexural
strength increased for group A however, it declined for group B when
Fig. 3. (a) low mag. (500x) of composition 2 at 1150 ◦ C showing large and
interconnected pores, (b) high mag. (10kx) of composition 2 at 1150 ◦ C temperature was raised beyond 1150 ◦ C. At 1200 ◦ C, group A samples
showing primary mullite fibers (M) and pores, (c) composition 1 at 1200 ◦ C exhibited a value of about 33 MPa while group B exhibited 24 MPa.
showing secondary mullite fibers (M) and quartz crystals (Q), (d) composition These results indicate that for group A, flexural strength is comparable
3 at 1200 ◦ C mullite fibers (M) and quartz (Q), (e) composition 4 at 1200 ◦ C and to ISO 13006 standard (35±2 MPa) for porcelain floor tiles [3]. But also,
(f) composition 2 at 1250 ◦ C. group B can be used as wall tiles because their strength is greater than

4
W. Ochen et al. Results in Materials 11 (2021) 100195

12 MPa, and water absorption is less than 10% [4].


The increase in flexural strength with temperature is attributed to
both vitrification and mullitization of the samples. The vitrification of
samples at 1150 ◦ C and below was not well facilitated. Large and
interconnected pores can be seen (Fig. 3a and b) which indicates that
due to a low vitreous phase during sintering, agglomeration of particles
and pores is not well fostered. As a result, the strength of the fired
samples is low (<23 MPa). At 1200 ◦ C and above, liquid state sintering
dominates, and the pores are blocked (Fig. 3c–f) consequently
strengthening the material. Another process to explain the increase in
flexural strength is the morphology of the mullite fibers [3,6,11]. The
formation of a desired amount and structure of mullite fibers are
important in acquiring the required strength of a porcelain material.
Previous studies have shown that these fibers are formed in a temper­
ature range of 1100–1250 ◦ C [20]. During the firing process of porce­
lains, kaolinite mineral found in kaolin clay undergoes dehydroxylation
at about 600 ◦ C to form metakaoline (Al2O3 ⋅ 2 SiO2). At 950–1000 ◦ C, it
transforms into alumina spinel and amorphous silica [5]. A viscous
liquid is formed when feldspar reacts with amorphous silica. It flows and
occupies the pores hence increasing vitrification of the material. The
alumina spinel reacts with the liquid phase to form primary mullite
(Fig. 3b). At 1200 ◦ C, secondary mullites are formed (Fig. 3c–e) from the
reaction of primary mullite with the liquid phase. As seen, their popu­
lation and interlocking network is high, this is responsible for the in­
crease in flexural strength as suggested by the mullite hypothesis [6,21],
and equations (4) and (5) shows the thermal reaction of kaolinite. The
tile samples sintered at 1200 ◦ C (group A) exhibited properties (linear
shrinkage, water absorption and flexural strength) that are acceptable
for porcelain tiles according to published data.
Al2 O3 2 SiO2 2 H2 O→Al2 O3 2 SiO2 2 H2 O (4)

3(Al2 O3 2 SiO2 )→3 Al2 O3 2 SiO2 4 SiO2 (5)


The decline in flexural strength for group B at temperatures greater
than 1150 ◦ C was unexpected (Fig. 5c). This however, can be attributed
to the high content of sand/quartz used in the samples (Table 2). Quartz
has a deleterious effect on the strength of porcelain tiles most especially
when its amount is greater than 10% [22]. It has low sinterability
compared to clay and feldspar which increases the amount of pores in
the microstructure of fired bodies. Due to the pores, the strength of these
materials decreases. In addition, quartz is known to have a high thermal
expansion (23 × 10− 6 K-1) as compared to its surrounding (3 × 10− 6
K− 1) [23,24]. During cooling, cracks can be formed due to residual
stresses hence reducing the strength of porcelains.

4. Conclusion

The results achieved in this study were encouraging. It demonstrated


that high quality porcelain floor tiles can be made using locally sourced
materials. The tile samples were evaluated at different temperatures and
composition of mixtures. The water absorption of the samples was not
affected by the composition of the raw materials, but rather the firing
temperature. At 1200 ◦ C, water absorption values were below 0.5% for
all compositions studied. It satisfied the ISO 13006 standards for por­
celain floor tiles. At the same temperature, the mullite fibers exhibited
good properties (long, fine and interlocking). As a result, the strength of
the samples increased. In fact, samples with feldspar in a range of
30–40%, kaolin in a range of 30–40%, 10% sand and 20% ball clay
exhibited flexural strength comparable to 35±2 MPa. Therefore, they
were classified as porcelain floor tiles (ISO 13006). At 1250 ◦ C, there
Fig. 5. Characterization of temperature with (a) linear shrinkage, (b) water
was no significant change in the nature of the fibers and the strength of
absorption and (c) flexural strength of tile samples.
the fired samples.

Funding

This research received no funding.

5
W. Ochen et al. Results in Materials 11 (2021) 100195

Authors contributions [6] G. Stathis, A. Ekonomakou, C. Stournaras, C. Ftikos, Effect of firing conditions,
filler grain size and quartz content on bending strength and physical properties of
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W. Ochen formulated the samples and drafted the manuscript. P.W [7] L. Boussouf, F. Zehani, Y. Khenioui, N. Boutaoui, Effect of amount and size of
Olupot carried out SEM and XRD analysis, and reviewed the final quartz on mechanical and dielectric properties of electrical porcelain, Trans. Indian
manuscript. F.M D’ujanga and B.Oruru also reviewed the final Ceram. Soc. 77 (3) (2018) 132–137.
[8] W.M. Carty, U. Senapati, Porcelain raw materials, processing, phase evolution, and
manuscript. mechanical behavior, J. Am. Ceram. Soc. 81 (1) (1998) 3–20.
[9] G.W. Nyakairu, C. Koeberl, Mineralogical and chemical composition and
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Declaration of competing interest [10] J.B. Kirabira, S. Jonsson, J.K. Byaruhanga, Powder characterization of high
temperature ceramic raw materials in the lake victoria region, Silic. Ind. 70 (10-
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[11] O.I. Ece, Z.-e. Nakagawa, Bending strength of porcelains, Ceram. Int. 28 (2) (2002)
interests or personal relationships that could have appeared to influence 13–140.
the work reported in this paper. [12] Y. Sawadogo, L. Zerbo, M. Sawadogo, M. Seynou, M. Gomina, P. Blanchart,
Characterization and use of raw materials from Burkina Faso in porcelain
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[14] A. Bernasconi, N. Marinoni, A. Pavese, F. Francescon, K. Young, Feldspar and firing
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equipment used to formulate test samples. They are also grateful to the [15] K. Fan, Relationship between Residual Stresses and Mechanical Behavior in
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