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Journal of Building Engineering 68 (2023) 106107

Contents lists available at ScienceDirect

Journal of Building Engineering


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

Study of fired clay bricks with coconut shell waste as a renewable


pore-forming agent: Technological, mechanical, and
thermal properties
Zineb Moujoud *, Achraf Harrati, Ahmed Manni, Amine Naim, Abdeslam El Bouari,
Omar Tanane
Laboratory of Physical Chemistry, Materials and Catalysis, Faculty of Sciences Ben M’Sick, Hassan II University of Casablanca, Morocco

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

Keywords: In the present work, coconut shell powder (CSP) is explored as a pore-forming agent in the
Fired clay bricks manufacturing of fired clay bricks. The bricks were produced by varying the amount of CSP (0,
Coconut shell waste 10, 20, and 30 wt%), and fired at different temperatures (900, 1000, and 1100 ◦ C). Mineralogical,
Pore-forming agent physical, mechanical, and thermal conductivity tests were performed to evaluate the properties of
Thermal conductivity the elaborated bricks. It is found that the addition of CSP does not influence the mineralogy of the
bricks. Besides, mechanical strength, bulk density, and firing shrinkage increase with sintering
temperature and decrease with increasing CSP content, while water absorption and porosity
decrease with temperature and increase with CSP addition. Otherwise, the combination of firing
at 1100 ◦ C with 30 wt% addition of CSP in clay brick provides lower thermal conductivity (0.37
W/(m.K)), while maintaining adequate tensile strength (9.88 MPa). This finding suggests the
reuse of CSP as a pore-forming agent to elaborate bricks with thermal insulating character.

1. Introduction
Energy conservation in the building sector has become one of the most important issues at the moment [1]. It was reported that
one-third of the world’s energy consumption is consumed in buildings [2], while 50% of this energy is lost; due to the low thermal
insulation of building materials [3]. Actually, building materials have been widely developed to improve thermal insulation and
optimize the energy performance of buildings [4]. Within the sustainability context, using ecological, lightweight, and low-cost
thermal insulation materials have recently emerged.
Fired clay brick is one of the most widely used building materials in the world [5], due to its remarkable physical and mechanical
properties, especially its durability, fire resistance and strength [6,7]. Indeed, fired clay brick relies on a simple manufacturing process
and the use of cheap and abundant raw materials: a mixture of clay, silica sand, feldspars, and water [8]. The approximate annual
production of bricks in the world is about 1391 billion units, which is expected to increase continuously due to the increased demand in
the construction sector [9]. In fact, fired bricks have a limited thermal conductivity value, usually about 1.0 ± 0.4 W/(m.K) depending
on the raw materials and the firing process, which means a significant heat loss through the house walls [10]. However, this unfa­
vorable property can be solved by introducing pores into the bricks. When pores are created, the thermal conductivity and density of
the bricks are reduced [10–12]. This can be achieved by introducing holes extending through the brick as in the case of a perforated

* Corresponding author.
E-mail address: [email protected] (Z. Moujoud).

https://doi.org/10.1016/j.jobe.2023.106107
Received 28 November 2022; Received in revised form 12 February 2023; Accepted 12 February 2023
Available online 13 February 2023
2352-7102/© 2023 Elsevier Ltd. All rights reserved.
Z. Moujoud et al. Journal of Building Engineering 68 (2023) 106107

brick or by incorporating particles as pore-forming agents in the clay mixture [13,14]. The latter method is widely used by the bricks
industry [14]. When a pore-forming agent is used, the organic matter burns during the firing process and leaves behind pores, thus
improving the thermal insulation properties of the brick [10,11,15,16]. However, the choice of the pore-forming agent depends on its
physico-chemical characteristics, its availability, and its ability to combust completely [14]. Therefore, with ecological awareness,
researchers are increasingly interested in using various wastes (agricultural, industrial, and urban) as pore-forming agents in fired
brick making [14]. The use of wastes in brick industry could have environmental and energetic advantages, on the one hand, by
valorizing wastes that are not widely used or usually end up in landfills and, on the other hand, by reducing the energy needed to
produce bricks due to their high calorific value [17–19].
Upon a review of the literature, it was found that using wastes with large amounts of organic matter can promote more pore
formation in the clay body during the firing process due to the chemical degradation and the corresponding gas release [14,20,21].
Among organic wastes, many agricultural and industrial co-products have been used as pore-forming agents due to their wide
availability and low costs, such as waste tea [11], rice husks [22,23], corn cob [16,24], cigarette butts [15,25], olive mill waste [26,
27], paper pulp [20], and sawdust [28]. Furthermore, the content and the particle size of the pore-forming agent influence the thermal
conductivity of bricks. Aouba et al. [29] investigated the use of olive stone flour (OSF) with a particle size of 50 μm and wheat straw
(WS) with a particle size of less than 500 μm as pore-forming agents. The results showed that the lowest thermal conductivity value was
obtained for 7 wt% WS (~0.30 W/(m.K)) compared to OSF (~0.39 W/(m.K)) when 8 wt% is incorporated. Similarly, Ahmad et al. [30]
revealed a decrease in the thermal conductivity of bricks by 27%–68% and by 48%–92% with an increase in coal and wheat husk
content from 5 to 50 wt%, respectively. This indicates the influence of the content and the particle size of the pore-forming agent on the
total porosity and thermal conductivity. Nevertheless, increasing the content and particle size of the pore-forming agent is undesirable
due to their negative effect on the strength and physical properties of bricks [30]. Therefore, the content and particle size of the
pore-forming agent must be controlled.
In this study, organic coconut shell waste is investigated as a pore-forming agent in fired bricks. The coconut tree, a member of the
palm tree family (Arecaceae), is grown in more than 100 countries. The global production of coconut is about 250–300 million tons for
the year 2018 [31]. The coconut shell, which represents 15–20% of the coconut, is a hard lignocellulosic waste that takes a long time to
decompose [32]. Coconut shell is commonly discharged by farmers and processors as abundant agro-industrial waste or open burned,
creating serious problems in the local environment [33]. Therefore, different approaches to recycle coconut shell waste have been
proposed, such as charcoal briquettes production [34,35], and activated carbon production [36,37]. In addition, the use of coconut
shell waste in the building sector has been investigated. Gunasekaran et al. [38] recommended using coconut shell as alternative coarse
aggregates in the production of hollow blocks, which can reduce the self-weight and material transportation and handling costs.
Another study confirmed the use of coconut shell as lightweight aggregates for concrete production in practice without any hesitation
given their durability properties [39]. However, the amount of coconut shell waste reused is less compared to its availability.
Therefore, recycling coconut shell powder (CSP) as a pore-forming agent in bricks production is a viable way to manage this waste and
minimize the volume sent to landfill. CSP contains a high volatile matter content (~80 wt%) with low compositions of ash (~2 wt%),
and carbon and oxygen are the major elements [40–42]. When burnt, CSP leads to the emission of CO2 which can create pores in the
brick body. On the other hand, local availability, renewable nature, and low cost are the main reasons for using CSP as a pore-forming
agent in this work.
To the authors’ knowledge, there is no study on using CSP as a pore-forming agent. This can be valuable to explore its performance
as a pore-forming agent compared to other currently used pore-forming agents. In this study, the effects of CSP incorporation and the
firing temperatures on the technological properties (i.e., linear shrinkage, porosity, water absorption, and bulk density), mechanical
strength (i.e., diametral compression strength), microstructure, and thermal conductivity of the developed bricks were investigated.
The results obtained in this study are intended to help future research to pay attention to this waste and to promote its economic and
environmental use.

2. Materials and methods


2.1. Raw materials
The red clay sample used in this study to prepare the fired bricks was collected from the Safi region (Safi, Morocco). Locally, this
clay is used for making pottery. The selected clay was crushed and stored in the laboratory under controlled conditions (T = 25 ◦ C,
Humidity = 50%). Similarly, coconut shell waste was taken from local vendors in Casablanca-Morocco. The coconut shell was oven
dried, ground in a ball mill, and sieved to obtain fine powder (CSP) before being used as a pore-forming agent in the fired specimens.

2.2. Methods
The methodological approach adopted in this study can be resumed as follow: the first step consists of preparation and charac­
terization of the raw material (i.e., XRF, CHNS–O, XRD, IR and DTA/TG). The second step of the process consists in preparing the brick
samples incorporating varying percentages of CSP at 0%, 10%, 20%, and 30% by weight. Three specimens were prepared for each level
of CSP addition. Finally, many tests were done on the elaborated bricks (i.e., XRD, SEM, linear shrinkage, porosity, water absorption,
bulk density, thermal conductivity and diametral compression strength) to investigate and evaluate their properties. For each test, the
obtained results present the average of three values.

2.2.1. Characterization of raw materials


The chemical composition of the raw materials was determined by X-ray fluorescence (XRF) using the Epsilon 4 instrument. The

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Z. Moujoud et al. Journal of Building Engineering 68 (2023) 106107

content of H, O, S, and C in coconut shell powder was measured by a PerkinElmer EA2400 series II CHNS–O Elemental Analyzer. N
detection limit was 1.20%. The particle size distribution of the raw materials was carried out using the Malvern Mastersizer 2000. X-
ray diffraction (XRD) of the raw and elaborated materials was carried out using a BRUKER D8 ADVANCE diffractometer. XRD ex­
periments were achieved in step-scan mode from 10◦ up to 65◦ (2θ). Fourier Transform infrared spectroscopy (FTIR) using a Bruker
Tensor 27 FTIR spectrometer operating in the range 4000–400 cm− 1. Thermal analyses (DTA-TG) were carried out using a LABSYSEVO
multichannel instrument apparatus. The scanning was carried out at different ranges of temperatures depending on the phenomena
appearing in the studied material (from 23 ◦ C to 1000 ◦ C for the clay sample, and to 600 ◦ C in the CSP) with a heating rate of 5 ◦ C/min
under air atmosphere.

2.2.2. Manufacturing of bricks


The raw materials (red clay and coconut shell waste), separately, are oven dried at 105 ◦ C for 24 h, ground in a ball mill, and sieved
to a particle size <63 μm. The bricks were manufactured through the dry-pressing technique. The coconut shell powder (CSP) was
added to the red clay at 0, 10, 20, and 30% by weight, and re-crushed for 15 min to obtain homogeneous powders. The powders were
moistened with a sprayer to the limit of 4–6% water. Next, the moistened powders were pressed using a hydraulic press of 40 MPa in a
cylindrical steel mold to prepare specimens of 50 mm in diameter and 25 mm in thickness. The samples were oven-dried at 105 ◦ C for
24 h to remove excess moisture that might cause cracking during the firing process. Finally, the samples were fired at 900, 1000, and
1100 ◦ C in the furnace with a heating rate of 5 ◦ C/min and then naturally cooled in the furnace.

2.2.3. Characterization of elaborated bricks


The loss on ignition (LOI) of the brick samples was determined by measuring the mass loss of the sample between the drying and
sintering stages. The following equation was used [43]:
Md − Mf
LOI(%) = × 100 (1)
Md

where Mf is the sample mass after firing, and Md is the sample mass after oven drying.
For the diametrical shrinkage, the diameter of the specimens was measured before and after the sintering step using a caliper
(accuracy ±0.01 mm). The resulting values are used to calculate the diametrical shrinkage according to ASTM C326-09 [44]:
Dd − Df
Diametrical shrinkage (%) = × 100 (2)
Dd

where Df is the sample diameter after firing, and Dd is the sample diameter after oven drying.
A procedure based on ASTM C373-88 standard [45] was used to measure the water absorption, bulk density, and apparent porosity
of the bricks by the following formulas:
Mwet − Mdry
Water absorption (%) = × 100 (3)
Mdry

( / ) Mdry ( / )
Bulk density g cm3 = × water density g cm3 (4)
Mwet − Msuspended

Mwet − Mdry
Apparent porosity (%) = × 100 (5)
Mwet − Msuspended

where Mdry is the constant mass of the specimen after drying at 105–115 ◦ C, Mwet is the mass of the specimen after water saturation and
Msuspended is the mass of the water-saturated sample.
The mechanical properties of the fired samples were assessed using an indirect tensile test. The Brazilian Test (diametral
compression) was used to measure the tensile strength of the specimens (ASTM C496 [46]). This test consists of applying a load
vertically on the diameter of a rather thin disk (typically 50 mm in diameter and 10 mm in thickness). The tensile strength σ r (MPa) is
given by the following equation [47]:
2×P
σr (MPa) = (6)
π×D×t

where P is the maximum applied load (N), D is the diameter (mm), and t is the thickness of the sample (mm).
Thermal conductivity of brick samples was performed according to the standard ASTM C177 [48] using a Thermal Conductivity
Analyzer type λ-Meter EP500e. This technique consists in applying variable heat flux in a block comprising a sample taken between
two plates. The measurement is carried out at three temperatures 10, 25, and 40 ◦ C, and under a pressure of 2500 Pa for each
temperature.
The surface morphology of the elaborated bricks specimens was observed using Hirox SH-4000 M scanning electron microscope at
an accelerating voltage of 10 kV and using a secondary electron detector (SE).

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3. Results and discussion


3.1. Characterization of raw materials
3.1.1. Chemical composition (XRF, CHNS–O)
The chemical composition of the red clay is shown in Table 1. The results reveal important contents of silica and alumina 51.69%
and 20.04% respectively, with a silica/alumina ratio ≈2.58 which explains the high content of quartz in the clay sample. A relatively
high content of Fe2O3 (5.35%) makes it appropriate for dark red coloring products (%wt of Fe2O3 > 3%) [49], and responsible for the
reddish color of the brick body after high-temperature treatment. The content of alkaline earth oxides CaO and MgO are low; 3.20%
and 2.86% respectively, which explains the relatively low carbonate content. The high percentage of K2O (4.44%) explains the richness
of the red clay in illitic clay minerals and also the presence of potassium feldspars responsible for the decrease of the melting tem­
perature of the material at high temperatures. The loss on ignition content (12.00%) is related to the elimination of adsorbed and
structural water as well as the decomposition of organic matter and carbonates. The rest of the oxides (Na2O, P2O5, TiO2) are present in
insignificant contents (≈0.43%).
Table 2 displays the chemical composition of the coconut shell powder (CSP) in its raw state by CHNS–O analysis. The CSP is
composed totally of organic matter 48.4% C, 44.59% O, 6.8% H, with low traces of N, S, and Cl. Moreover, the ash content after the
combustion of the raw CSP is about 1.8% of the total mass. XRF analysis of dry ash of CSP (Table 1) demonstrates the predominant of
SiO2 (48.45%) along with MgO (16.21%), Al2O3 (15.61%), and Fe2O3 (13.60%), with some negligible traces of other oxides. The
obtained results are following those found in the literature [40,50].

3.1.2. Particle-size distributions


In bricks manufacturing, it is commonly known that the particle size of the raw materials used influences the porosity after the
sintering process. For this reason, Fig. 1 shows the particle size distribution for the red clay and coconut shell powders. The analyzed
powders show a bimodal and unimodal shape in the range of 0.1–59 μm and 0.1–76 μm for the clay and CSP samples, respectively. The
curve shows that the CSP was ground to a fineness that is close to that of the red clay powder. According to the results, the particle size
corresponding to cumulative volume percentages below 10, 50 and 90% are 1.99, 10.7 and 32.9 μm, and 3.2, 10.5 and 30.5 μm for red
clay and CSP, respectively. On closer observation, it can be deduced that the majority of the particles are smaller than 33 μm for both
clay and CSP samples. These results confirm that the powders used are very rich in fine fractions which help to minimize the pore size
without the appearance of macropores or/and cracks.

3.1.3. Mineralogical composition (XRD)


X-ray diffraction (XRD) patterns of red clay and coconut shell powder are shown in Fig. 2. In Fig. 2-a, it was observed that quartz (Q)
is the main mineralogical phase in clay. However, other mineralogical phases revealed in clay such as dolomite (D), calcite (C),
feldspar (F), illite (I), kaolinite (K), and chlorite (Ch) offering favorable properties for ceramic use.
As shown in Fig. 2-b, the most important diffractions in coconut shell waste are observed by three crystalline peaks at the following
angles: 2θ = 14.84◦ , 22.67◦ , and 34.23◦ represent the plane (120), (002), and (123) respectively, which corresponds to the planar
crystallographic family of cellulose [51].

3.1.4. FTIR characterization


The FTIR spectrum of the raw materials was recorded in the range of 4000–400 cm− 1 as shown in Fig. 3. The assignments of the
bands were based on literature data. From the FTIR spectrum of red clay in Fig. 3-a, the presence of absorption bands at 3620 cm− 1 can
be attributed to the asymmetric stretching of structural hydroxyl groups OH. The broad band located at 3416 cm− 1 is assigned to the
stretching vibration of adsorbed water. The band around 1632 cm− 1 is assigned to OH bending vibration of adsorbed water in the
structure of silicate [49]. The band observed at 1042 cm− 1 is attributed to Si–O stretching [52]. The bands in 694 cm− 1 and 472 cm− 1
are attributed to Si–O stretching and Si–O bending modes, respectively [52]. Absorption at 535 cm− 1 is related to Si–O–Al, where the
Al is in octahedral coordination [53].
From the FTIR spectrum of coconut shell powder shown in Fig. 3-b, the peak at about 3404 cm− 1 is due to hydrogen-bonded O–H
stretching. The peak at 2927 cm− 1 is due to the C–H stretching that causes vibrations of CH, CH2, and CH3 groups [42]. The peak at
1728 cm− 1 is due to the carbonyl group C–– O stretching [54]. The peak at 1636 cm− 1 is reflected to N–H bending in the primary amine
group presents in the sample. The peak at 1512 cm− 1 is due to the stretching vibrations in aromatic structure C– – C [42]. The peak at
1245 cm− 1 represents Si–CH2 stretching in alkane or C–C plus C–O plus C– – O stretching and deformation bands in cellulose and lignin
[42,55]. The absorbance peak at 1052 cm− 1 is assigned to C–O deformation in secondary alcohol and aliphatic ether [55]. A peak at
898 cm− 1 is attributed to the C–H in plan deformation plus C–O deformation in primary alcohol [55]. The peak at 1461 cm− 1 cor­
responds to the C–H bending of CH3 groups. The peak at 1376 cm− 1 is reflected to the symmetric and asymmetric bending of CH3
groups. The peak at 1103 cm− 1 is due to the C–N stretching [56]. The peaks at 597 cm− 1 and 830 cm− 1 contributed to the C–H

Table 1
XRF analysis of red clay and CSP after combustion (Ash state).

Oxide content (wt%) SiO2 Al2O3 Fe2O3 CaO MgO K2O Na2O P2O5 TiO2 LOIa

Safi clay 51.69 20.04 5.35 3.20 2.86 4.44 0.12 0.18 0.13 12.00
CSP (Ash state) 48.45 15.61 13.60 0.56 16.21 0.87 0.44 0.29 0.01 –
a
Loss on ignition obtained after calcination at 1000 ◦ C for 1 h

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Table 2
CHNS–O analysis of the coconut shell powder (CSP) in the raw state.

Elements Composition (wt%)

C 48.4
H 6.8
N 0.13
O 44.59
Cl 0.07
S <0.01

Fig. 1. Particle size distribution of (a) Red clay, (b) Coconut shell powder.

stretching vibrations [54].

3.1.5. Thermal analysis (DTA-TG)


The DTA-TG curves of the raw materials are shown in Fig. 4. Fig. 4-a shows four peaks for the red clay. The first endothermic peak
below 100 ◦ C represents the evaporation of absorbed water molecules. The second endothermic peak 514 ◦ C is due to the desorption of
structural water (i.e., dehydroxylation of kaolinite and illite) [49]. The third endothermic peak at 694 ◦ C is due to the reversible α/β
quartz transition. Finally, the small peak at 943 ◦ C which does not correspond to a loss of mass is reflects the formation of spinel
structure and/or primary mullite.
During the heating process of the clay sample, two significant stages in weight loss percentage were detected: at 25–200 ◦ C with
3.34% and 400–700 ◦ C with 8.75%, respectively. At 25–200 ◦ C, the weight loss is mainly attributed to the rapid desorption of adsorbed
water and interlayer water in the clay surface and interlayer space. At the temperature range of 400–700 ◦ C, the weight loss is mainly
due to the combustion of organic matter and the dissipation of structural water (structural OH groups). When the temperature reaches
700–1000 ◦ C, the clay mass remains unchanged.
Fig. 4-b presents the DTA-TG curves of coconut shell powder (CSP). The first peak at 64 ◦ C is related to the elimination of water and
other primary volatile substances [40]; where the sample loses only about 9.41% of its original mass. Furthermore, the CSP presents

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Fig. 2. XRD diffractograms of raw materials: (a) Red clay and (b) Coconut shell powder.

two degradation steps, the first observed at 324 ◦ C is explained by the simultaneous decomposition of cellulose, hemicellulose, and
pectin, and the second at 435 ◦ C is related to the decomposition of lignin [40]. The material loses about 88.82% of its original weight,
that’s mean is almost totally carbonized.

3.1.6. Microstructural observation (SEM)


SEM observations of raw materials (Fig. 5) demonstrate the microstructural aspect of the studied powders. Fig. 5-a and Fig. 5-b
confirm the morphology and fundamental size of the illite clay, the images show a lath-like shape of the illite grains with a size of less
than 5 μm. Agglomerations are also observed due to the ability of the raw clay to absorb moisture water, which attaches the fine clay
particles together forming agglomerated particles of larger size.
Fig. 5-c and Fig. 5-d show the morphology of the CSP used in this work. As shown, the CSP appears to be very fine, however, on
higher magnifications, it can be seen that the powder consists of particles with a size of about 60 μm and below. It can be noticed that
the CSP appeared to be small pebble shaped and had a surface containing closed pores due to the presence of volatiles and other
contaminants on the surface [42,57]. In order to be a pore-forming agent, the material must be in the form of very fine particles, and
the results obtained show that CSP is a good candidate to be used in the mixture with clay as a pore-forming agent.

3.2. Characterization of elaborated bricks


3.2.1. Macroscopic aspect of bricks
The appearance of the brick samples in terms of surface color and crack development is shown in Fig. 6. The color of the brick is
essential to classify bricks [58]. The red color is thought to be caused by iron oxide content after firing at appropriate temperatures
[49]. No significant impact of coconut shell powder incorporation on color is observed [59]. Moreover, no surface defects were
observed in any specimens.

3.2.2. Phase composition of bricks


The X-ray diffraction patterns of the prepared brick mixtures (0, 10, 20, and 30 wt% CSP) fired at 900, 1000, and 1100 ◦ C for 1 h are

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Fig. 3. FTIR spectrum of raw materials: (a) Red clay and (b) Coconut shell powder.

given in Fig. 7. It can be observed that the primary minerals composing the studied clay sample (e.g., dolomite, calcite, feldspar, illite,
kaolinite, and chlorite) disappeared after the heat treatment with the appearance of newly formed phases. At 900 ◦ C, kaolinite
(Al2Si2O5(OH)4) is no more observed and transformed into metakaolinite through the removal of the hydroxyl groups of the silicate
lattice above 450 ◦ C [60]. Anorthite (CaAl2Si2O8) is the first new mineral that appeared at 900 ◦ C and its maximum abundance is
observed at 1100 ◦ C. Anorthite was probably formed by the multistage solid-state reactions between the clay matrix and carbonate [49,
60]. Gehlenite (Ca2Al2SiO7) and spinel (MgAl2O4) were firstly identified at 900 ◦ C, and their abundances were noticed at 1100 ◦ C.
Gehlenite is formed by a reaction between calcium oxide CaO from calcite and metakaolinite [49]. Spinel is formed by a reaction
between magnesia (MgO) and alumina (Al2O3). The MgO was derived from the dehydroxylation of chlorite and dolomite minerals and
alumina (Al2O3) resulting from the destruction of clay minerals and K-feldspar [49]. The peaks of orthoclase appeared at 900 ◦ C and
completely disappeared at 1000 ◦ C. This is due to their contribution to the formation of the mullite phase [61]. Quartz (SiO2) was the
only primary mineral to be able to resist higher temperatures (up to 1100 ◦ C). The peaks of quartz are present during all firing
temperatures and decreased at higher temperatures due to its dissolution and/or its conversion into minor amounts of cristobalite [60].
Mullite appeared at all tested temperatures (900–1100 ◦ C) in small amounts, which could be related to the presence of sufficient illite
content. After the destruction of illite by hydroxylation, they reacted with quartz and modified it into mullite [49]. Diopside
(CaMgSi2O6) is probably formed from the reaction of CaO, MgO, and SiO2 at high temperatures; CaO was probably supplied from
calcite and dolomite, however, MgO seems to be originated from chlorite and dolomite; its formation was marked mainly by a sharp
decrease in quartz content [60]. Furthermore, based on the XRD patterns (Fig. 7), the addition of CSP does not modify the mineral­
ogical composition compared to bricks without additives, which is confirmed by the appearance of the same formed phases at all
mixtures and sintering temperatures [62].

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Fig. 4. DTA/TG diagrams of raw materials (a) Red clay and (b) Coconut shell powder.

Fig. 5. The morphological aspect of raw materials: (a) and (b) Red clay powder; (c) and (d) Coconut shell powder.

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Fig. 6. Macroscopic aspect of fired clay bricks at 900–1100 ◦ C.

3.2.3. Technological and mechanical properties of bricks


The weight loss of fired bricks with respect to CSP content is presented in Fig. 8-a. It is well shown that the firing temperature has
less effect on brick weight loss compared with the CSP content. By increasing the CSP content in the clay mixtures, the weight loss
apparently increased. A similar finding was observed in other studies [12,63–65]. This increase trend of brick weight loss is related to
the departure of water, the combustion of organic matter, and the decomposition of carbonate minerals present in both clay and CSP
[63]. During the firing process below 950 ◦ C, all the organic matter is volatilized [64]. Typically, brick weight loss results are
compatible with thermal results (DTA-TG) of raw materials (Fig. 4).
Fig. 8-b symbolizes the diametric shrinkage of the CSP incorporated fired bricks between 900 ◦ C and 1100 ◦ C. The diametric
shrinkage increased with the increase in sintering temperature as reported in previous works [12,24,65–67]. This increasing trend of
shrinkage may be the consequence of the formation of liquid-phase and inter-particle cohesion in the bricks during the firing process
[63]. Moreover, it was observed that shrinkage decreased as the amount of incorporation of CSP increased. This may be related to the
distribution and burning of CSP which cause the existence of residual porosity resulting during the firing process [24]. According to the
literature, firing shrinkage is a significant parameter that affects the brick quality [24,68]. If the shrinkage is more than 8%, it could
increase the risk of cracks and dimensional defects in bricks [69]. However, it was observed that for CSP incorporated fired bricks, the
diametric shrinkage was below the value of 8%.
Apparent porosity is a significant factor affecting the physico-mechanical and thermal properties of fired bricks [12]. The increase
in the porosity decreases the strength and the thermal conductivity properties [70]. Fig. 8-c shows that the apparent porosity increases
with increasing CSP content. This may be attributed to the increase in pore number in the brick structure due to the addition of CSP that
burned during the firing process. The combustion of the organic matter contained in the additive leads to the emission of CO2 which
gradually releases from the material and creates pores in the brick [62]. However, the apparent porosity decreases with increasing
sintering from 900 to 1100 ◦ C. This reduction is associated with the densification and vitrification of the clay bodies at higher firing
temperatures [24,49]. Similar results have been observed in other studies. Making bricks with the addition of agricultural waste such
as 7 wt% wheat straw [29], 8 wt% olive stone flour [29], 15 wt% corn cob [24], and 50 wt% wheat husk waste [30], increase the
porosity by 43.5%, 40.6%, 48%, and 65%, respectively. In the present study, the maximum apparent porosity value was 52.85% for 30
wt% CSP content. Considering the literature data, the present experimental results suggest using CSP as a pore-forming agent in brick
manufacturing, thus increasing the porosity and thermal insulation performance.
Bulk density is strongly influenced by the pores and voids formed in the clay brick structure during the firing process [30]. As shown
in Fig. 8-d, the bulk density value of samples without any addition was the maximum, while it decreased with increasing CSP content in
brick bodies. Similar findings have been reported in previous studies [12,67,68]. The bulk density correlates inversely with porosity.
The lower bulk density is more noticeable from 30 wt% CSP content. Pores and voids are formed in the brick samples due to the almost
complete carbonization of CSP, which eventually results in porous structures and lower bulk densities [62]. Lightweight samples with
high porosity could be interesting for thermal or acoustic insulation or for partitions, as recommended by Njeumen Nkayem et al. [24].
On the other hand, with a constant CSP content, the bulk density increases with the firing temperature. This is attributed to the
formation of vitreous phases helping to fill the open porosity [24,64].
Water absorption is essential to determine the durability of building materials. The more brick absorbs water, the less durable it
becomes [66]. The results in Fig. 8-e show that the addition of CSP increases the water absorption of bricks regardless of the firing
temperature. This improvement is expected since the CSP contained in clay bodies is almost completely carbonized during the firing
process, leading to an increase in the open porosity of the brick samples [24,66,71]. Moreover, the increase in firing temperature leads
to a decrease in the water absorption rate of brick samples. The values obtained at 1100 ◦ C are lower than the others owing to the
intense brick densification related to the formation of vitreous phases, which leads to a coalescence phenomenon of the closing pores
[24]. For 10 wt% addition, the water absorption of bricks fired between 900 ◦ C and 1100 ◦ C still lies below the maximum value of 22%

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Fig. 7. XRD diagrams of different bricks fired at (a) 900 ◦ C, (b) 1000 ◦ C, and (c) 1100 ◦ C.

required by the ASTM C62 standard [72]. Therefore, according to ASTM C62 [72] standard, the bricks containing 20 wt% and 30 wt%
CSP can be used for negligible weathering conditions. These bricks may be evaluated in insulation applications where there is no
contact with water. Similar findings have been reported by many researchers [12,73,74].
Fig. 8-f reveals that the tensile strength values are significantly degraded when the additive in the brick increases from 0 wt% to 30
wt%. This decrease can be explained by the increase in pores due to the combustion of CSP, which results in a considerable decrease in
tensile strength [67,75]. Similarly, Monedero et al. [65] revealed that adding agro-industrial waste ashes (exhausted olive cake and
almond shell) decreases the tensile strength of bricks. However, the tensile strength shows an increasing trend with the firing tem­
perature. The maximum tensile strengths (19.46 MPa and 15.71 MPa) were achieved in bricks with 0 wt% and 10 wt% CSP at 1100 ◦ C,

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Fig. 8. Evolution of physical and mechanical properties of brick specimens at 900, 1000 and 1100 ◦ C: (a) LOI (%), (b) Diametric shrinkage (%), (c) Apparent porosity
(%), (d) Bulk density (g/cm3), (e) Water absorption (%), and (f) Tensile strength (MPa).

respectively. This enhancement is mainly related to the densification of the clay bodies. This is due to the gradual formation of
anorthite and mullite, which are strong phases contributing to the formation of vitreous phases helping to fill the open porosity and
improve the strength of bricks [67,76]. This is confirmed by the X-ray pattern (Fig. 7).

3.2.4. Thermal conductivity of clay bricks fired at 1100 ◦ C


Lower thermal conductivity is beneficial because it reduces the energy consumed for cooling and heating [15,16]. Based on the
mechanical results, the thermal performance of bricks fired at 1100 ◦ C is presented in Fig. 9. It is shown that the thermal conductivity
was reduced with increasing CSP content, which represents a promising diminution of 51% for the incorporation of 30 wt% CSP. This
reduction is influenced by the increase in porosity. From the results presented in Fig. 8-c, it has been shown that the addition of CSP,
which burns during the firing process, leads to an increase in the porosity of bricks and thus a decrease in thermal conductivity.
However, this reduction in thermal conductivity is a promising avenue for specific applications, such as thermal insulation, which
allows for greater energy savings in residential applications [29,30,49].

3.2.5. Microstructural observation (SEM) of clay brick samples


SEM micrographs of the different brick mixtures fired between 900 and 1100 ◦ C are shown in Fig. 10. It is well displayed that the
addition of CSP affects the microstructure of the bricks. The images show an increase in the porosity of the samples as well as the pore
size with increasing CSP addition. Bricks with 30 wt% CSP incorporation have a large porous texture compared to bricks with 0 wt%
CSP incorporation. This is related to the combustion of the organic matter present in the CSP, which releases CO2 and creates a set of
pores in the brick bodies. Furthermore, it is also well shown that increasing the firing temperature improves the densification of the
bricks. At 900 and 1000 ◦ C, SEM images illustrate typical heterogeneous microstructures with a wide distribution of pores in the
samples. However, the porosity decreases significantly after firing at 1100 ◦ C. The bodies exhibit a more densified microstructure,
which is due to the progressive formation of anorthite and mullite, which are strong phases contributing to the formation of glassy
phases, as confirmed by X-ray diffraction analysis (Fig. 7). An increase in pore size from a spherical shape of 2–5 μm in diameter to an
irregular shape up to 25 μm in diameter, according to the SEM scale, is obtained between 0 and 30 wt% CSP, which explains the
improvement of the mechanical properties with the decrease of the open porosity compared to bricks fired at 900 and 1000 ◦ C as
reported by Ref. [67]. However, the effect of CSP content and firing temperature on brick properties can be better understood after
SEM observation. These results confirm the results of the technological, mechanical and thermal conductivity tests (Figs. 8 and 9).

3.2.6. Comparison with previous works


Table 3 provides a summary of the technological and thermal characteristics of fired clay bricks mixed with various types of waste
as pore-forming agents and the processing temperature ranges used in some recent studies. In order to better understand the features of
using wastes as pore-forming agents, researchers have varied the firing temperature and waste amount, as indicated in Table 3. Each
work’s sintering temperature typically ranges between 900 and 1150 ◦ C. Importantly, the principal crystalline phases (i.e., gehlenite,
anorthite, diopside, and wollastonite) occur at temperatures of approximately 1000 ◦ C, which is consistent with the findings of the

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Fig. 9. Thermal conductivity of brick specimens (0, 10, 20, and 30 wt% of CSP) sintered at 1100 ◦ C.

Fig. 10. SEM micrographs of different brick specimens sintered at 900, 1000, and 1100 ◦ C.

current study. Although, lower sintering temperatures reduce energy consumption in the brick industry, all studies have found that
mechanical strength values are moderate to higher and more significant after sintering at 1000 ◦ C and above [8]. In addition, the waste
content affects the overall serviceability characteristics of fired bricks. The content varied differently in each work, but the common
goal was to develop porous bricks with optimal physico-mechanical and thermal properties. In all research, shrinkage values range
from medium to high; in our study, the shrinkage value is reported as a medium (0.3–3.8%) and falls within the normal range [69].

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Z. Moujoud et al.
Table 3
Comparative table of our fired bricks with previous works.

Sample Pore-agent material Firing Firing Porosity Pore size Bulk density Water Mechanical strength Thermal conductivity Ref
temperature (◦ C) shrinkage (%) (%) (μm) (g/cm3) Absorption (%) (MPa) (W/(m.K))

Fired clay bricks Eggshell waste, (0–15 800–1000 ◦ C – ≈14.9-22 – 2.1–1.5 11.1–15.6 4.8–1.2(compressive – [8]
wt%) strength)
Fired clay bricks Tea Waste, (2.5-10 wt 1050 ◦ C – – – 1.58–1.37 15.1–21 8.3–3.1(compressive 0.61–0.32 [16]
%) strength)
Corrn cob, (2.5-10 wt 1.69–1.18 12.6–19.4 5.4–1.1 (compressive 0.61–0.38
%) strength)
Rice Husk, (2.5-10 wt 1.63–1.39 16.5–19.7 10.8–3.2 (compressive 0.58–0.36
%) strength)
Lightweight clay Corn cob waste, (0–15 900–1100 ◦ C ≈1.7–5.1 ≈33.8-48 – ≈1.9–1.2 ≈17-38 6-1 (flexural strength) – [24]
bricks wt%)
13

Fired clay bricks WheatStraw, (1-7 wt%) 920 ◦ C 3.8–5.2 27.9–43.5 – 1.85–1.57 15.3–28.6 36.2–18.1 0.49–0.34 [29]
(compressive
strength)
Olive Stone Flour, (2-8 5.5–5.8 29.6–40.6 1.79–1.58 15.2–26.3 34–24.8 (compressive 0.49–0.39
wt%) strength)
Fired clay bricks Coal waste, (5–50 wt%) 1000 ◦ C 0.5–1.7 24–63 70–100 – 14–35 25–4 (compressive 0.49–0.25 [30]
strength)
Wheat husk waste, 0.6–1.8 26–65 – 16–37 24.9–3 (compressive 0.35–0.08
(5–50 wt%) strength)
Lightweight Coffee waste, (0–30 wt 1150 C

– 17.4–42.8 100–1000 1.66–1.46 13.5–29.25 20.76–10.75 (flexural 0.73–0.39 [49]
ceramics %) strength)
Fired clay bricks Solid paper residue, 900 ◦ C 4.3–7.6 ≈27-33 – 1.76–1.39 16–24 11-3 (compressive 0.53–0.41 [63]

Journal of Building Engineering 68 (2023) 106107


(2.5–17.5 wt%) strength)
Fired clay bricks Coconut shell powder, 900–1100 ◦ C 0.3–3.8 11.9–52.8 5–50 2–1.15 11.21–46.80 19.46–4.51 (tensile 0.56–0.37 This
(0–30 wt%) strength) work
Z. Moujoud et al. Journal of Building Engineering 68 (2023) 106107

Moreover, the values of bulk density in all studies are noticed between 1.18 and 2.1 g/cm3 and this is almost similar to our results
(2–1.15 g/cm3). In our study, bricks fired at 900 ◦ C with 30 wt% of CSP addition showed higher porosity and water absorption of
around 52.8% and 46.8%, respectively. While Muñoz et al. [63] found the highest porosity of 33% with the addition of 17.5 wt% solid
paper residue after firing at 900 ◦ C. Besides, Ahmad et al. [30] pointed out similar average values regardless of the different firing
temperature (i.e. 1000 ◦ C) with a porosity of 63% for 50 wt% addition of charcoal waste. However, the increase in porosity improves
the thermal insulation of the bricks. In our work, incorporating 30 wt% of CSP reduces the thermal conductivity to 0.37 W/(m.K),
while Muñoz et al. [63] found 0.41 W/(m.K) with 17.5 wt% addition of solid paper residue and Aouba et al. [29] reached 0.34 W/(m.
K) with 7 wt% addition of wheat straw. Concluding that the technological and thermal properties of fired bricks are significantly
influenced by the type, content and size of the pore-forming agent, as well as by the sintering temperature.

4. Conclusion
This study evaluated the feasibility of using coconut shells waste powder (CSP) as a renewable pore-forming agent in fired clay
brick making. The effect of coconut shell powder addition and the variation in firing temperature were investigated. Based on the
obtained results, the addition of CSP did not change the mineralogy and color of the bricks. On the other hand, it appears that the bulk
density decreased with increasing CSP addition, which ultimately leads to lighter bricks. This is due to pores forming in the brick
samples due to the almost complete combustion of CSP. However, the incorporation of CSP is limited due to the increase in water
absorption and the decrease in mechanical properties. In particular, the combination of firing at 1100 ◦ C with 30 wt% addition of CSP
results in clay brick with lower thermal conductivity (0.37 W/(m.K)), while maintaining adequate tensile strength (9.88 MPa).
Therefore, the use of CSP as pore-forming agent is a valuable way to develop lightweight bricks with promoting thermal insulating
character.

CRediT authorship contribution statement


Zineb Moujoud: Investigation, Methodology, Validation, Writing – original draft, review & editing. Achraf Harrati: Investigation,
Validation, Formal analysis, Writing – original draft, review& editing. Ahmed Manni: Formal analysis, Writing – review& editing.
Amine Naim: Formal analysis, Writing – review& editing. Abdeslam El Bouari: Supervision, Validation. Omar Tanane: Writing –
review & editing, Supervision, Validation.

Declaration of competing interest


The authors declare that they have no known competing financial interests or personal relationships that could have appeared to
influence the work reported in this paper.

Data availability

Data will be made available on request.

Acknowledgements
This work was financially supported by the National Center for Scientific and Technical Research (CNRST), Rabat, Morocco). We
thank also the Hassan II University, Morocco, through the platform of analysis for characterization techniques support.

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