Journal of Cleaner Production 319 (2021) 128678
Contents lists available at ScienceDirect
Journal of Cleaner Production
journal homepage: www.elsevier.com/locate/jclepro
Assessment of the recycling potential of stone processing plant wastes based
on physicochemical features and market opportunities
Lisandro Simão a, d, *, Marcelo Tramontin Souza b, Manuel J. Ribeiro c, Oscar Rubem Klegues
Montedo d, Dachamir Hotza a, e, Rui M. Novais f, Fabiano Raupp-Pereira a, d
a
Graduate Program in Materials Science and Engineering (PGMAT), Department of Mechanical Engineering (EMC), Federal University of Santa Catarina (UFSC), PO
Box 476, 88040-900, Florianópolis, SC, Brazil
Graduate Program in Science, Innovation, and Modelling in Materials (PROCIMM), State University of Santa Cruz (UESC), 45662-900, Ilhéus, BA, Brazil
c
Materials Research and Development Center (UIDM), Polytechnic Institute of Viana Do Castelo (IPVC), Rua Escola Industrial e Comercial de Nun’Álvares, 4900-347,
Viana Do Castelo, Portugal
d
Graduate Program in Materials Science and Engineering (PPGCEM), Research Group on Residues Valorisation (VALORA), Universidade Do Extremo Sul Catarinense
(UNESC), 88806-000, Criciúma, SC, Brazil
e
Graduate Program in Chemical Engineering (POSENQ), Department of Chemical Engineering (EQA), Federal University of Santa Catarina (UFSC), 88040-900,
Florianópolis, SC, Brazil
f
Department of Materials and Ceramic Engineering, CICECO-Aveiro Institute of Materials, University of Aveiro (UA), 3810-193, Aveiro, Portugal
b
A R T I C L E I N F O
A B S T R A C T
Handling editor: Prof. Jiri Jaromir Klemeš
The extraction of raw materials in many productive sectors has become problematic for the environment because
of the negative impacts of the process and the inappropriate destination of the generated waste. Stone waste (SW)
from the dimension stone industry has physical and chemical characteristics with great potential for use as an
alternative raw material in several industrial activities. Its main constituents include silica, alumina, alkaline,
and alkaline earth oxides, usually combined as calcite and dolomite in the crystalline phases. In this work, a case
study was conducted with SW from a processing plant of dimension stones (also known as ornamental rocks)
located in Viana do Castelo, Portugal. In this new methodology, the SW powder samples were characterised by Xray fluorescence spectrometry, X-ray diffraction, differential thermal analysis, and thermogravimetry. Physical
features, such as moisture content, specific surface area, particle size distribution, and true density were also
determined. The pH and electrical conductivity of the SW as a suspension were also evaluated. The specific SW
was analysed against the literature considering aspects related to environmental legislation and standards (waste
classification), physical and chemical characteristics (potential), production data (quantity), recycling avail­
ability (viability), and market opportunities (applicability). This novel way in terms of the form and content of a
paper is an intermediate approach between an original article and a state-of-art review. SW is normally
considered inert but, owing to its high fineness (<200 μm), some potentially hazardous compounds can been
leached. The state-of-the-art of SW applications suggests that this waste is promising raw materials for ceramics
and cement, which eventually encapsulate contaminants in their structure. A critical discussion of the literature
was conducted to reduce the knowledge gap about the most promising valorisation strategies for SW. New
recycling proposals are also suggested.
Keywords:
Dimension stones
Ornamental rocks
Stone sawing waste
Marble waste
Recycling
1. Introduction
Considering the population increase over the last decades (from 3 to
7.8 billion people between 1960 and 2020), followed by growing ur­
banisation (from 34 to 56% in the same period) (Worldometer, 2020)
and the industrial processes of modernisation, the global waste gener­
ation per capita is growing exponentially. In the USA alone, each citizen
produces an average of 808 kg of waste per year (Sensoneo, 2020). It is
estimated that 90% of the raw materials used for manufacturing durable
products become waste even before the product leaves the factory
* Corresponding author. Graduate Program in Materials Science and Engineering (PGMAT), Department of Mechanical Engineering (EMC), Federal University of
Santa Catarina (UFSC), PO Box 476, 88040-900, Florianópolis, SC, Brazil.
E-mail address: lisandrosimao@gmail.com (L. Simão).
https://doi.org/10.1016/j.jclepro.2021.128678
Received 5 December 2020; Received in revised form 26 July 2021; Accepted 14 August 2021
Available online 16 August 2021
0959-6526/© 2021 Elsevier Ltd. All rights reserved.
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
(industrial waste), and approximately 80% of the finished product is
discarded within the first six months of its use (municipal waste gen­
eration) (Arts, 2013). A report by the World Bank (The World Bank,
2018) estimated that global waste production is predicted to increase by
70% by 2050 unless urgent action is taken. Indeed, waste recycling is
one of the most discussed issues in the 21st century and is the subject of
thousands of academic papers.
There are essentially three ways of dealing with inorganic waste,
namely, reuse, recycling, or disposal in landfills. Reuse and recycling are
the preferred waste management methods that consider environmental
sustainability and the opportunity to generate important economic
returns. Reuse means to use by-products with the same purpose for
which they were conceived, while recycling is related to material val­
orisation in other processes, by converting waste into new materials.
However, consolidating a sustainable waste management process re­
quires investments and long-term efforts, which is the main reason why
disposal to landfills is the most widely used approach, especially in
economically fragile countries. Even when local governments manage
waste through regulations, laws are not always followed, and poorly
managed waste continues to contaminate the environment and
adversely affect animals and humans.
The proposal and consolidation of a recycling process begin with a
case-by-case examination by considering the physical and chemical
characteristics of the waste. Many wastes have chemical and mineral­
ogical compositions remarkably like those of traditional raw materials,
allowing industries to earn environmentally friendly seals by using these
wastes as feedstock in their manufacturing processes, thus reducing the
costs of the final products.
This work presents and discusses the potential and the challenges of
recycling stone waste (SW) generated from a processing industry of
dimension stones (also known as ornamental rocks), using a new waste
valorisation systematic (detailed in section 3). The SW characteristics
depend on the composition of the original stones. Marble and granite are
the most used, and its main constituents include silica, alumina, alkaline
and alkaline earth oxides (Segadães et al., 2005), usually in the crys­
talline forms of calcite and dolomite in the case of marble, as well as
quartz, feldspar, and mica, corresponding to granite (Acchar et al., 2006;
Uygunoğlu et al., 2014). Despite the promising physicochemical SW
features with great potential for use as raw materials in other industrial
sectors (Tugrul Tunc, 2019), landfills are still its main SW destination.
The countries that extract and process dimension stones, and
consequently generate larger SW quantities, are in the following order:
China, India, Turkey, Iran, Brazil, and Italy (ABIROCHAS, 2018a;
Montani, 2019). In most Middle Eastern and Mediterranean countries,
dimension stone processing is the main source of economic revenue. In
Palestine, this industry represents approximately 34% of the national
income (Abu Hanieh et al., 2014). Major importers, including the USA,
South Korea, Germany, and Canada, also generate large SW quantities
(ABIROCHAS, 2018a; Demirel and Alyamaç, 2018).
Although many published studies highlighted the SW characteristics
and recycling potential as alternative raw materials in other industrial
processes (as will be reported in Section 7), SW remains unknown in
most industries. As a large part of the waste generated comes from small
companies scattered in urban centres, there is not always an inspection
for the correct handling, especially in emerging cities. In this sense, nonhazardous SW are impacting the air, soil, and water (Davini, 2000;
Demirel and Alyamaç, 2018; Ercikdi et al., 2015). The main reasons
behind these current management practices (landfilling) are discussed in
this study.
The present work provides the most detailed characterisation of SW,
as a case study, including chemical, physical, thermal, and microstruc­
tural analyses, and discusses the main applications, including cementi­
tious materials and ceramic formulations, as well as less conventional
recycling proposals, such as alternative binders, environmental appli­
cations, filler in industrial products including paints, paper, rubber, and
reinforcement for polymeric matrices (Careddu et al., 2014). This
methodology is an intermediate approach between an original article
and a state-of-art review, which consists in a novel way in terms of the
form and content of a paper.
It is worth mentioning that there are some published reviews on SW
recycling covering different technical aspects of this waste, especially
focusing on building materials, such as mortar and concrete (Rana et al.,
2016; Rodrigues et al., 2015; Şahan Arel, 2016; Singh Chouhan et al.,
2019; Singh et al., 2017a; Thakur et al., 2018; Tugrul Tunc, 2019).
Nevertheless, few studies suggest alternative applications (Careddu
et al., 2018; Mehta et al., 2016; Tozsin et al., 2015). However, even with
literature showing varied recycling solutions for SW, landfills are still its
main destination. In this sense, this work gathers the knowledge of the
most relevant publications to address and discuss the accurate SW
recycling potential, which includes the characterization of the waste
followed by a critical analysis of the feasibility of the proposed appli­
cations. Novel recycling proposals for future work are also suggested.
2. Dimension stones processing and generated waste
There is a wide variety of dimension stones with different shapes and
shades originating from a variety of igneous, metamorphic, and sedi­
mentary rocks. These rocks are commonly known as marble, granite,
limestone, travertine, quartz-based stone (sandstone, quartzite), and
slate. Alyamaç and Aydin (2015) and Sarkar et al. (2006) proposed
classifying them into two general categories, namely, i) polished stones,
including, marble (metamorphic rock) and granite (igneous rock), the
most popular, as well as travertine and onyx; and ii) unpolished stones,
such as basalt (although some polishable basalts run away from this
classification, as noted in Careddu and Grillo (2019)), schist, and tuff.
Differently, Careddu et al. (2016), proposed classifying them into three
main groups, i) marbles (carbonate stones as real marbles, mostly calcite
and dolomite-based); ii) granites (silicate stones as real granites, mostly
quartz and alkali feldspar-based); and iii) other stones such as basalts
(igneous), trachyte (igneous) and sandstones (sedimentary).
This work is focused on marble and granite stones, which are by far
the most produced dimension stones currently. The production process
of these stones normally comprises main stages, such as prospecting,
quarrying, transportation, cutting/sawing, and finishing (polishing,
flaming, bush-hammering) (Careddu and Dino, 2016). Stones are
extracted in the form of blocks and sent to sawing and polishing plants.
After sawing to a previously defined size and thickness, the stones are
polished, cleaned, and shined. A large amount of water is used in all
processing steps (see Fig. 1) to prevent overheating of the cutting and
polishing discs and to reduce the incidence of dust (Alyamaç and Aydin,
2015; Demirel and Alyamaç, 2018; Ulubeyli and Artir, 2015), resulting
in large amounts of effluents in the form of sludge (Demirel and Alya­
maç, 2018), which will be referred to hereinafter as stone waste (SW).
Settling tanks and filter presses can be used to remove water and reduce
the volume of sludge generated (Torres et al., 2009). In some industrial
plants, it is also common to store the generated sludge in open or closed
settling dams for weeks. In this case, the suspended particles settle
down, and water slowly evaporates, increasing the solid concentration
in the sludge.
3. Materials and methods
The CPQvA (Classification, Potentiality, Quantity/Viability and Ap­
plications) valorisation system (Oliveira, 2017; Raupp-Pereira et al.,
2006, 2007) was adopted in this work (Fig. 2) in the context of recycling
potential of stone processing plant wastes. It is divided into SW col­
lecting and characterizing; classification according to hazardousness
and potentiality, besides addressing aspects related to their quantity and
possible applications, seeking the best SW destination.
This waste recovery analysis methodology suggests carrying out a
complete analysis of the waste characteristics prior to the design of the
recycling solution. Therefore, this work initially brings a detailed
2
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
Fig. 1. Flowchart of polishing and sawing of dimension stones (ornamental rocks) including processing steps and effluent generation.
Fig. 2. CPQvA methodology adopted in this work. CPQvA stands for Classification, Potentiality, Quantity/viability and Applications.
characterization of a SW and the production data (items Classification,
Potentiality, Quantity, and Viability). The experimental findings are
compared with literature data, such as an original article, while in the
subsequent sections the recycling proposals viability was validated by
using available literature studies, such as a state-of-art review (item
Applications).
days. The stones processed by the company are composed of marble
(~80 wt%) and volcanic stones (~20 wt%). The samples were dried at
110 ◦ C for 24 h and sieved #200 (74 μm) for deagglomeration.
The SW powder samples were characterised by X-ray fluorescence
spectrometry (XRF, Philips X’Pert PRO MPD spectrometer) with the loss
on ignition (LOI) determined at 1000 ◦ C. X-ray diffraction (XRD, Bruker
D8 Advance DaVinci equipment with Cu Kα radiation) was applied in
the range of 5–80◦ , with steps of 0.02◦ and 0.5 s/step and the diffraction
patterns were analysed using the ICDD database (International Centre of
Diffraction Data, PDF 4) in the EVA software (Bruker). Differential
thermal analysis (DTA) and thermogravimetry (TG) were performed
◦
using a simultaneous thermal analyser (402 EP, Netzsch) at 10 C/min
3.1. Materials and characterisation
Three SW batches (SW1, SW2, and SW3) were collected from different
bags from the deposit of dimension stones (ornamental rocks) sawing
and polishing plant located in Viana do Castelo, Portugal, on random
3
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
4. Classification and environmental impacts
up to 1000 ◦ C under an air atmosphere.
Physical features, such as moisture content, specific surface area by
N2 adsorption (Brunauer–Emmett–Teller; Gemini 2380, Micromeritics),
particle size distribution (laser diffraction, Coulter LS230 analyser), and
true density (Helium pycnometer, Multipycnometer, Quantachrome),
were also determined.
Finally, the pH (Hanna HI8424) and electrical conductivity (HACH
44600) of the SW suspensions were evaluated by adding 5 g of powder to
50 mL of deionised water, followed by manual stirring for 5 min. The
analyses were conducted after 10 min and according to the procedure
adopted by Davidovits (2008).
Waste is managed according to the regulations of the country in
which they are generated. In the USA, hazardous and non-hazardous
solid waste must follow the Environmental Protection Agency (EPA)
recommendations. According to the EPA, “hazardous waste is hazardous
or potentially harmful to our health or the environment” (EPA-USA,
2020). The EPA monitors eight heavy metals that are extremely toxic,
even at low concentrations (Table 1), and has set limit concentrations for
As (5 mg/L), Ba (100 mg/L), Cd (1 mg/L), Cr (5 mg/L), Pb (5 mg/L), Hg
(0.2 mg/L), Se (1 mg/L), and Ag (5 mg/L) (EPA-USA, 2012). These el­
ements, when present in lakes, rivers, or soil, may be harmful to the
environment, affecting fauna and flora.
Table 1 lists the quantifications of the main metals present in the
three SW samples studied in this work, and for comparison, some typical
compositions of granite and limestone rocks, according to Alloway et al.
(2010). As shown, among the EPA-monitored elements, the referred
amounts of Ba, Cr, and Pb commonly found in SW samples could be
higher than the legal limit. In this sense, the species’ leachability will
ultimately dictate the real environmental impact of SW. Despite this, the
naturally occurring heavy metals are expected to show poor
leachability.
The European waste catalogue (EPA-EU, 2002) classifies waste from
mining and sawing dimension stones as code 01 or “wastes resulting
from exploration, mining, quarrying, and physical and chemical treat­
ment of minerals”; and sub code 01 04 or “wastes from physical and
chemical processing of non-metalliferous minerals.” These codifications
include cut waste, gravel, crushed rocks, dust, and other unspecified
forms (Careddu and Siotto, 2011; Dino et al., 2015; EPA-EU, 2002; Rana
et al., 2016). As natural stones are considered inert materials
(non-hazardous) for most applications, despite the significant presence
of some hazardous elements, SW has also been considered inert, as it
contains metals in similar proportions to the original stone (Al-Zboon
et al., 2010; Rana et al., 2016). It has been overlooked that these ele­
ments can be incorporated during the extractive and processing opera­
tions (Karaca et al., 2012; Rana et al., 2016). Indeed, because of the false
idea that these materials are non-hazardous, incidents of soil and
ground/surface water contamination have been documented (Tabelin
3.2. Databases and search methodology
Extensive research was conducted using Scopus, Web of Science,
SciFinder, Scielo, Springer, and Wiley databases, and papers filtered
using the following keywords: “stone cutting waste”, “stone sawing
waste”, “marble waste”, “marble powder sludge”, “marble sludge
waste”, “marble dust”, and “stone and marble sector”. The most cited
and recent articles were thoroughly evaluated according to the defined
analysis criteria CPQvA. This systematic method is guided by five
decision-making criteria, namely, classification, potential, quantity,
viability, and applicability, considering aspects related to environmental
regulation and standards (classification), physicochemical characteris­
tics and purity (potential), production data (quantity), recycling chal­
lenges (viability), and market opportunities (applicability). This
systematic guide is a simple and useful tool for investigating the recy­
cling potential of industrial wastes, as adopted by authors in previous
studies (Oliveira, 2017; Raupp-Pereira et al., 2006, 2007, 2007; Simão
et al., 2018; Souza et al., 2019). Other references, including environ­
mental laws and regulations (ABNT, 2004a, 2004b; EPA-USA, 2012;
European Union, 2008), books (Alloway, 2010; Davidovits, 2008), and
websites (ABIROCHAS, 2018b, 2018a; Worldometer, 2020) have also
been used to include economic and environmental aspects. The envi­
ronmental law was used to compare the legal limits of metals in SW and
classify them concerning their real hazardousness.
Table 1
Chemical composition (trace elements in ppm) of the SW samples.
Elements
Ba
Cr
Pb
Ce
Co
Cs
Cu
Ga
La
Mo
Nb
Nd
Ni
Rb
Sc
Sn
Sr
Th
U
V
Y
Zn
Zr
a
b
This work
Alloway (2010)
SW1
SW2
a
190.0
12.8
11.7
42.8
5.4
9.4
19.1
3.0
25.6
2.1
9.5
22.5
3.2
13.5
17.4
5.2
340.0
4.3
2.4
9.4
7.0
30.7
39.9
180.0
55.8
5.0
53.5
8.9
51.4
3.5
26.7
1.7
12.6
29.6
39.1
17.0
9.2
8.5
320.0
4.7
2.7
14.9
9.5
26.0
56.1
SW3
66.4
5.6
23.6
6.2
8.4
16.8
1.2
0.9
13.0
48.5
6.0
7.3
130.0
1.6
6.9
5.2
15.2
4.0
Granite
a
b
USA Standard EPA limits (2012) (mg/L)
b
Brazilian Standard NBR 10005 (2004b) limits (mg/L)
Limestone
600.0
10.0
20.0
90.0
5.0
5.0
4.0
0.1
12.0
6.0
1.5
0.3
5.0
5.0
3.6
0.3
4.0
70.0
1.0
15.0
50.0
40.0
100.0
5.0
5.0
70.0
5.0
1.0
Natural stones.
After leaching tests in water.
4
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
et al., 2018).
In Europe, leaching tests are performed to guide the classification of
wastes as inert, hazardous, or non-hazardous, according to the Landfill
Directive and Council Decision 2003/33/EC (European Union, 2008).
The leaching simulation tests may be conducted in different ways, that
is, through a double-stage leaching process, where the first step is per­
formed at a liquid to solid ratio (L/S) equal to 2 and then at L/S = 8 (this
procedure mimics the natural conditions of leaching by rainwater for
materials with a high solid content). The second step follows an up-flow
percolation test at low L/S ratios (simulating behaviour in disposal
scenarios). Alternatively, a single-stage leaching process can be applied
with L/S = 10. The latter procedure is the most common. The European
leaching limits are more rigorous than those from the EPA-USA, with
more elements being monitored.
In other countries, such as Brazil, which follows specific standards
(ABNT NBR 10004/2004), industrial wastes are classified into three
classes, namely, hazardous (Class I) when corrosive, pathogenic, flam­
mable, or toxic characteristics are present; non-hazardous but non-inert
(Class II-A), when biodegradability, combustibility, or water solubility is
demonstrated; and non-hazardous and inert (Class II-B) when none of
the previously cited characteristics are demonstrated (ABNT, 2004a).
The Brazilian standard establishes limit concentrations for several
compounds (Table 1) determined by leaching tests according to ABNT
NBR 10005/2004 (ABNT, 2004b). These include Cr, Ba, and Pb, which
are common in SW. If the limits of these elements exceed 5, 70, and 1
ppm (or mg/L), respectively, the waste is considered hazardous (Class I)
(ABNT, 2004b).
This study did not perform leaching tests on the samples in compli­
ance with the American, European, or Brazilian regulations. However,
the literature shows that the data are sufficient for the proposed objec­
tives. Hameed and Sekar (2009) characterized a sludge predominantly
composed of granite-based stones from Indian factories and noticed the
presence of barium (12 mg/L), chromium (1.2 mg/L), lead (0.9 mg/L),
minor contents of arsenic (0.5 mg/L), and cadmium (0.3 mg/L), all
within acceptable limits. Dino et al. (2015) reported that when the
cutting and polishing steps were conducted using a gang saw, Cr (166
ppm), Cu (188 ppm), and Zn (76 ppm) were the main leached species,
probably because of cutting disc abrasion and wear and the cleaner
water jet. When diamond saws are used, the elements commonly
detected are Zn (99 ppm), Co (89 ppm), and Cu (24 ppm) (Dino et al.,
2015; Rana et al., 2016).
Tabelin et al. (2018) discussed the presence of heavy metals in debris
excavated from tunnels and other large infrastructure projects in
megacities. According to these authors, substantial portions of the
excavated debris are often naturally contaminated with hazardous ele­
ments, which are readily released in substantial amounts once exposed
to the environment. This contaminated excavation debris is loosely
referred to as “naturally contaminated rocks”. They can contain several
hazardous and toxic inorganic elements, such as As, Se, B, and heavy
metals such as Pb, Cd, Cu, and Zn. If not properly treated, these naturally
contaminated rocks can cause severe problems to the surrounding
ecosystems.
Simsek et al. (2005) studied the effects of marble waste disposal on
the water and sediment quality in the district of Torbali, Izmir, Turkey.
According to the authors, approximately 35000 tons of marble waste
was disposed of on the riverbed in a single year (2005). They reported an
increase in the number of ions present in the water (mainly Ca and Mg)
and sediments, resulting in highly turbid water. The authors also noticed
traces of Fe, Al, As, and Pb in sufficient amounts to compromise the
quality of the drinking water (Simsek et al., 2005). Çelik and Sabah
(2008) also reported a high concentration of solubilised Ca, Mg, and Cl
in wastewater from marble processing.
From an environmental perspective, the increased turbidity of wa­
tercourses can reduce light penetration, consequently, decreasing
photosynthesis and the reproduction of organisms, reducing nutrients,
modifying the food chain, and threatening aquatic biodiversity
(Khyaliya et al., 2017; Torres et al., 2009). Consistent with these ob­
servations, some studies have highlighted the mutagenic effects of or­
ganisms exposed to SW effluents. Aguiar et al. (2016) evaluated the
mutagenic effect of SW on onion root cells and fish erythrocytes. The
authors concluded that the analysed waste had mutagenic potential
under the studied conditions (Aguiar et al., 2016). Venturoti et al.
(2019) evaluated the toxic effects of SW effluents on Geophagus brasi­
liensis and highlighted the toxic effects of the waste on these organisms.
The problems associated with the extraction, processing, and
improper disposal of SW can affect water, soil, and air (Abu Hanieh
et al., 2014; Careddu and Siotto, 2011; Yavuz Çelik and Sabah, 2008). In
quarries, extraction pollutes the air with the generated dust, in addition
to the excavations, which have a strong impact on the soil and land­
scape. In the stone sawing industry, dust is partially mitigated by adding
water to the process, but it generates another problematic waste,
namely, the sludge in the settling dams (Abu Hanieh et al., 2014).
Another environmental impact related to this activity is the trans­
portation of these materials, which generates emissions from fossil fuel
combustion, in addition to dust (Abu Hanieh et al., 2014). Because of its
high fineness, the presence of SW (Alyamaç and Ince, 2009) can result in
excessive soil compaction, occupying voids, preventing water percola­
tion, and reducing fertility (Khyaliya et al., 2017). Therefore, the safe
disposal of heavy metal-containing solid wastes, such as SW, is a chal­
lenging task.
The numerous environmental concerns associated with the dimen­
sion stone sector can be remedied in several ways (Abu Hanieh et al.,
2014; Careddu and Siotto, 2011), such as separation and treatment of
the waste before deposition (Table 2) or reusing it in new applications. If
the waste has leachable elements, it is important to use it in materials
able to encapsulating them. Thus, the waste can provide social and
economic benefits. The immobilisation of metal elements in cementi­
tious materials and through thermal treatments are examples of
encapsulating techniques in a certain structure through physical and
chemical processes (Guo et al., 2017). The potential applications are
broadly discussed in section 7.
5. Potentialities: chemical and physical features
As previously reported, the physical and chemical characteristics of
the SW are mainly dependent on the original stones, with marble and
granite being the most common. Accordingly, it is advisable to start by
investigating the chemistry of these stones.
Marble is a crystalline metamorphic limestone resulting from the
recrystallisation of limestone (CaCO3) and dolomite (CaMg(CO3)2) at
high temperatures and pressures (Demirel and Alyamaç, 2018; Segadães
et al., 2005). It contains large amounts of calcium carbonate (CaCO3)
and minor impurities, such as silica, feldspar, iron oxides, mica, fluorine,
and organic matter (Acchar et al., 2006; Uygunoğlu et al., 2014). Granite
is an igneous stone mainly composed of minerals such as feldspar,
quartz, and mica (Segadães et al., 2005; Vieira et al., 2004), and its main
constituents are silica, alumina, calcium oxide, and alkaline oxides
(Segadães et al., 2005). Because of the chemical composition differences
Table 2
Main impacts and remediation practices of the stone cutting and polishing
industry.
Environmental
impacts
Particle size
(mm)
Remediation practices
Coarse waste
>5.0
Fine waste
0.1–5.0
Dust
Liquid mud
<0.1
–
Screening for use as a concrete
aggregate
Use in concrete mixes or paper
production
Use of particle filters
Production of artificial stones
Source: Adapted from Abu Hanieh, Abdelall and Hasan (Abu Hanieh et al.,
2014).
5
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
between the stones, the sludge composition will vary in the processing
plants, depending on the amount of marble or granite-based stones
processed, according to stone availability and customer demand.
Fig. 3a shows the X-ray diffractograms of the SW samples used in this
study. In the SW1 and SW2 patterns, calcite (JCPDS card 01-085-1108)
predominates, whereas, in SW3, calcite has a leading role with dolo­
mite (JCPDS card 00-036-0426). This is because the SW samples in this
study were mainly derived from marble stones (~80 wt% of stones
processed) with variations in the carbonate content.
The XRD patterns are aligned with the chemical composition of the
samples, as shown in Table 3. In SW1 and SW2, large amounts of CaO
(50.59 and 46.48 wt% respectively) and a high LOI (~36 wt%) were
identified. In SW3, in addition to the CaO (~42 wt%), a significant
concentration of MgO (~10 wt%), from the dolomite phase (CaMg
(CO3)2), was detected.
The effect of temperature on SW (only for SW1) was investigated
using DTA/TG analysis (see Fig. 3b). The decomposition of carbonates
(endothermic event E3) was initiated at approximately 700 ◦ C and was
observed up to approximately 970 ◦ C. The thermal decomposition of
pure CaCO3 usually does not exceed 800 ◦ C (Karunadasa et al., 2019;
Souza et al., 2017), but the presence of a very low percentage of alkali
salts can modify the decomposition range. For example, for CaCO3 with
1% NaCl, thermal decomposition ranges from 700 to 975 ◦ C (Chattaraj
et al., 1973). Chlorides were not detected in the samples considered here
(by XRF) but were detected by Yavuz Çelik and Sabah (2008) in marble
sludge water.
Other thermal events identified in SW are those resulting from the
evaporation of the adsorbed and combined water between 20 and 250 ◦ C
(endothermic event, E1) and the combustion of polymeric resin and
other organic waste materials from the cutting and polishing processes,
between 300 and 500 ◦ C (exothermic event E2). The presence of poly­
meric resin in the sludge depends on the SW generation process of each
industry. In this case, honeycomb-like Al sheets were bonded with
epoxy-based glue on the stone surfaces before sawing (see Fig. 4).
The main purpose is to obtain thinner stone slabs than traditional
ones (~6 mm), reduce the weight of the stone, and maintain mechanical
properties. The particularity of this company to introduce other mate­
rials (Al sheet and glue epoxy) to the process may be responsible for the
small compositional differences in the waste generated. This becomes
important for certain applications, as it can change the properties of the
material obtained, even at low concentrations.
To date, few studies evaluated the variations in the chemical
composition of the SW, the exception being the works of (Careddu et al.,
2014; Careddu and Marras, 2015). The majority of studies consider that
the chemical heterogeneity can be mitigated by storing them in big lots.
Table 3 lists the chemical compositions of the SW samples. As seen, the
chemical characteristics of the sludge depend on the original stones
processed. The chemical compositions of the SWs collected from various
literature studies are provided for comparison.
The results show that the main oxides presented are referred to as
marble and granite stone wastes (Table 3). When waste is mostly derived
from marble stones, the main minerals present are calcite and occa­
sionally dolomite, and the chemical compositions are remarkably
similar. Magnesium oxides and silica are the main secondary com­
pounds. The Mg mass content depends on the limestone deposit, which
can be classified into three types, namely, calcitic limestone when the
MgO content is less than 5%, dolomitic limestone if the MgO content is
between 5 and 12%, and magnesian limestone when the MgO content
exceeds 12% (LaborSolo, 2020). This limestone type classification is
important for waste applications in the soil to supply the Ca or Mg
deficiency.
When waste is not derived from marble stones, the minerals present
are heterogeneous, with several crystalline phases such as quartz, mica,
kaolinite, feldspar, anorthite, and marble waste (calcite and dolomite).
The chemical composition reveals the presence of SiO2 and Al2O3 as the
main oxides, with other minorities dependent on the composition of the
cutting stone (Table 3).
Table 4 lists the main physical features of SW1 as compared to the
literature. The moisture content of the three SW batches varied between
22 and 27 wt%, and the true densities between 2.4 and 2.9 g/cm3, near
to the theoretical densities of the main minerals present in the samples,
calcite (2.71 g/cm3) and dolomite (2.84 g/cm3).
The SW particle size distribution ranged from 3.4 to 200 μm
(Fernández-Caliani and Barba-Brioso, 2010; Kabas et al., 2012; Sarkar
et al., 2006; Tozsin et al., 2014a) and the specific surface area ranged
from 0.2 to 2.5 m2/g (Demirel and Alyamaç, 2018; Rana et al., 2016).
The high fineness is especially related to the polishing and sawing
processes (Demirel and Alyamaç, 2018). Likewise, Fig. 5 shows the SW1
particle size distribution, revealing that 100% of the particles were
below 40 μm.
The medium alkalinity shown in Table 4 is associated with the
presence of carbonates, ranging from pH 8.1 to 9.6. Incidentally, this
alkalinity might favour recycling in some applications, such as in geo­
polymers, which are an eco-friendly alternative to Portland cementderived binders. Previous studies have shown that under alkaline con­
ditions, calcite is thermodynamically unstable, and thus highly reactive
(Locat et al., 1991; Palmero et al., 2017).
Indeed, pH is an important parameter that triggers the alkaliactivation process in these materials, driving the hardening process for
pH ranges between 8 and 11 or even flash-setting when the pH exceeds
Fig. 3. Characterization of SW samples: a) XRD patterns (C = calcite; D = dolomite), and b) thermogravimetry and differential thermal analysis (TGA/DTA) of the
SW1 sample up to 1000 ◦ C.
6
0.7
0.8
4.9
Studies carried out by the author considering 30 works.
Cal – Calcite; Dol – Dolomite; Mi – Mica; Q – Quartz; Al – Albite; Bi – Biotite; An – Anorthite; Or – Orthoclase; M – Microcline; Kao – Kaolinite; Pla – Plagioclase; Fel – Feldspar; I – Illite.
From granite stone
b
0.1
<0.1
0.7
3.6
2.6
0.1–3.4
2.9
3.3
2.3
37.9
64.1
59.6–88.9
67.1
62.1
47.9
2.7
0.2
Traces-15.2
Trace
0.2
0.8
13.6
13.2
6.6–13.8
14.9
12.8
12.6
0.1
<0.1
<0.1
From marble stone
a
0.3
0.3
0.6
1.0
<0.1–0.6
0.6
<0.1
<0.1–0.3
<0.1
4.3
4.4
0.1–3.6
5.2
4.3
2.3
0.2
0.3
0.1
0.1
<0.1
0.3
0.1
0.1
<0.1
0.1
<0.1
<0.1
<0.1
0.4
0.6
0.2
0.4
<0.1
0.1
<0.1
This work
SW1
SW2
SW3
SW/average
Careddu et al. (2014)
Ercikdi et al. (2015)
Ercikdi et al. (2015)
Aruntas et al. (2010)
Raupp-Pereira et al., (2008)
Yavuz çelik et al. (2008)
Yavuz çelik et al. (2008)
Yeşilay et al. (2017)
Omar et al. (2012)
Vardhan et al. (2019)
a
.Demirel et al. (2018)
Khyaliya et al. (2017)
Kabeer et al. (2018)
Tozsin et al. (2014a)
Acchar et al. (2006)
Monteiro et al. (2004)
Menezes et al. (2005)
Vieira et al. (2004)
Torres et al. (2009)
Segadães et al. (2005)
50.6
46.5
41.9
46.3
53.2–54.9
55.1
56.4
54.4
54.5
54.0
55.1
53.5
42.1
28.7
30.4–83.2
33.1
32.2
50.8
19.9
3.6
4.5–6.0
1.9
4.0
12.6
1.0
2.4
10.3
4.5
0.4–0.5
0.2
0.1
0.6
0.3
0.4
0.2
1.7
2.8
22.3
0.1–21.6
17.9
19.8
9.8
3.5
1.6
7.0
9.0
2.2
6.1
<0.6
1.2
0.1
0.7
0.6
0.8
0.0
0.5
14.1
4.7
0.1–44.1
3.8
1.6
2.4
3.2
0.6
2.1
<0.3
0.5
0.0
0.1
0.1
0.5
0.2
<0.1
<0.1
<0.1
<0.1
0.6
0.8
0.1
0.5
<0.1
<0.1
<0.1
0.1
<0.1
0.0
0.0
0.1
0.9
0.1
<0.1–1.1
1.2
1.7
0.4
1.1
<0.1
0.1
0.1
0.1
0.2
0.1
0.0
0.1
1.9
0.5
<0.1–9.7
0.1
1.2
0.5
3.6
8.2
6.0–6.3
4.4
10.6
3.0
0.1
<0.1
0.1
0.1
0.7
0.2
0.4
37.2
12.4
1.6
2.6–4.4
0.5
0.7
13.1
43.7
2.5–46.2
45.1
<0.1
36.2
35.2
44.2
38.6
45.1–43.8
42.7
43.3
43.4
43.0
43.4
43.8
44.1
0.2
0.3
<0.1
0.2
<0.1
<0.1
<0.1
Cal
Cal
Cal; Dol
Cal; Dol
Cal
Cal
Cal
Cal
Cal
Cal
Cal
Cal
Cal
Cal; Dol
Cal; Dol
Cal; Dol
Dol
Dol
Q; Bi; Al; An; Or; Cal; Dol
Mi; Q; M; Pla
Mi; Q; Cal; Kao; Fel
Fel; Mi; Pla; Q
Q; Kao; Mi; Al; I; Cal
Mi; Q; Al; Cal; Dol
LOI
P2O5
SO3
K2O
Fe2O3
Na2O
MnO
Al2O3
SiO2
MgO
CaO
References
Table 3
Chemical and mineralogical compositions (mass percent) of SW and different references.
Journal of Cleaner Production 319 (2021) 128678
TiO2
b
Minerals
L. Simão et al.
7
11 (Davidovits, 2008). As the SW1 sample reached pH > 8 (after 10 min
of contact with water), it might be a potential candidate to accelerate the
geopolymerization reactions. Nevertheless, the chemical composition of
SW must also be considered to enable it to be used as a reactive precursor
in the synthesis of geopolymers (or alkali-activated materials). The
required presence of reactive silica and alumina is dependent on the
stone origin, that is, marble-derived stones typically contain fairly low
amounts of SiO2 and Al2O3, while granite contains significant amounts
of these oxides. Therefore, the chemical composition of granite-based
stones is more suitable for the envisioned applications.
Additionally, calcite dissolution might promote the acidity neutral­
isation of effluents, water, and soils, as demonstrated by Equation (1),
which has been reported for many applications (Ercikdi et al., 2015;
Fernández-Caliani and Barba-Brioso, 2010).
CaCO3 + H2 O ↔ Ca2+ + HCO−3 + OH −
(1)
These ions drive the electrical conductivity values (Table 4) for the
SW1 sample and SW, as reported by Kabas et al. (2012).
Therefore, the SW recycling potential depends on its chemical and
physical characteristics. As previously mentioned, the SW chemical
composition depends on the heterogeneity of the stones processed dur­
ing different periods and their mineralogy. When the chemical compo­
sition is heterogeneous, applications are restricted to the physical
potential of the SW by exploring their fineness, especially as a filler in
the mortar and concrete formulations. When the chemical composition
is homogeneous, SW can be exploited as a source of CaCO3 and/or
magnesium carbonate. Section 7 discusses the main applications pro­
posed in the literature.
6. Quantity and viability: generation data and disposal costs
The global production of dimension and coverings stones increased
from 1.8 Mt/year in the 1920s to 153 Mt/year in 2018. The production
values between 2014 and 2018 (see Table 5) show an increase of
approximately 12% within this period (from 136.5 to 153.0 Mt). In
2019, it was estimated that these numbers also exceeded 100 Mt
(Careddu, 2019).
China, India, Turkey, Iran, and Brazil (ABIROCHAS, 2018a; Montani,
2019) are the largest producers globally. China contributed 31.4% of
global production in 2018, reaching absolute values of ~48 Mt of
dimension stones.
In 2017, this sector negotiated at US$ 20.6 billion globally, of which
US$ 5.0 billion corresponded to Brazil (ABIROCHAS, 2018a, 2018c).
Brazil was the fourth-largest producer in 2014, 2015, and 2016, being
overtaken by Iran in 2017 and 2018 due to the gradual, but steady,
increase in stone production in this country over the recent years
(Table 5). The production of dimension stones in Portugal, where the SW
samples were collected, reached ~3 Mt in 2018, occupying a ninth place
among the largest global producers and having a ~2% share of global
production.
The 14 largest stone producers represent 85.2% of the global pro­
duction and, consequently, are the locations that face major problems
due to the inappropriate waste management of these materials (ABIR­
OCHAS, 2018a; Montani, 2019).
The amount of waste generated during the processing of dimension
stones has been estimated to be between 20% and 50% of the mined
blocks. The volume depends on various parameters, such as the pro­
cessing type, size, type of cutting and polishing discs, and the type and
size of the stones (Alyamaç and Aydin, 2015; Demirel and Alyamaç,
2018; Gencel et al., 2012; Karaşahin and Terzi, 2007; Rana et al., 2016;
Saboya et al., 2007; Sarkar et al., 2006; Ulubeyli and Artir, 2015). If
tailings from mining are considered, the total waste volume can reach
around 70–80% (Hebhoub et al., 2011; Tozsin et al., 2014b). Dhana­
pandian and Gnanavel (2009) stated that 20–25 wt% of raw-stone
blocks become waste at production. According to Torres et al. (2009),
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
Fig. 4. Flowchart of the stone-cutting process with honeycomb aluminium panels, adapted from Mineral System company (Mineral System, 2020).
each ton of processed stone generates approximately 0.1 m3 of SW, with
0.08 m3/ton from the sawing operations and 0.02 m3/ton from the
cutting and polishing operations. By considering that this waste usually
contain 20-25 wt% humidity and present a density of 2700 (±100)
kg/m3, it is estimated around 23 wt% dry SW generated from processing
stones, with ~18 wt% from sawing and ~5 wt% from cutting and pol­
ishing steps.
However, according to a report by Montani (2019), which exposes
detailed information about the world production, consumption, tech­
nology, and profiles of leading countries of stones in the world, the
processing waste generated represents 41% of raw-stone production.
Table 6 lists data on the SW volume generated between 2003 and 2018
from the production of raw-stone and processing waste operations
worldwide, obtained from Montani’s report. As listed, the volume of
both raw stone and waste from both operations doubled in the same
period.
According to Dino et al. (2015), the costs related to sludge landfilling
represent approximately 3% of the operating stone-working plant costs,
and this suggests economic advantages, besides the obvious environ­
mental benefits, which can be obtained from proper waste recycling
avenues.
Table 4
Physical properties of SW1 compared with literature data.
Parameters
Density
(g/cm3)
Surface
area
(m2/g)
Mean
particle
size
(μm)
pH
Electric
conductivity
(μS/cm)
SW1
2.6
6.3
8.8
136.4
Ercikdi et al.
(2015)
Careddu et al.
(2014)
Omar et al. (2012)
Fernández-Caliani
et al. (2010)
Tozsin et al.
(2014a)
Kabas et al. (2012)
Rana et al. (2016)
Vardhan et al.
(2019)
Sarkar et al.
(2006)
2.7
2.5 ±
0.2
0.3
2.7–2.8
1.8–2.4
3.4–5.0
9.5–9.6
2.5
11.4
8.2
8.8–9.2
a
8.1
a
b
2.4–2.9
2.9
0.2–0.7
35.0
5.0–10.0
8.0
2200.0
b
200.0
d80.
d90.
7. Potential applications
This Section presents the main proposed applications for SW recy­
cling from the most relevant literature studies. Additionally, by
considering the previously collected SW data this study introduced
innovative recycling proposals not yet evidenced in the literature.
Although there are many possible applications for stone sawing
waste, they can be summarised into three main general applications,
namely, fillers for binders, ceramic formulations, and environmental
applications. Table 7 summarizes these applications. There are also
some specific applications related to the production of paper, paints,
rubber, and other polymers which are exposed at the end of this Section.
7.1. Mortars and concretes
Several studies have investigated SW incorporation into mortars and
concrete formulations as a full or partial replacement for cement or fine
aggregates. Some also used marble pieces as coarse aggregates. As the
annual global concrete consumption reached approximately 25 billion
tons (Tiwari et al., 2016) and aggregates account for 60–75% of the
volume of traditional concretes, this could theoretically enable the reuse
Fig. 5. Particle size distribution of SW1 as received.
8
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
Table 5
Latest available production data (in millions of tons) of the main world producers of dimension stones (2014–2018).
# Countries
1
2
3
4
5
6
7
8
9
10
11
12
13
14
2014
China
India
Turkey
Iran
Brazil
Italy
Egypt
Spain
Portugal
USA
Greece
France
Saudi Arabia
Pakistan
Subtotal
Others
Total
2015
2016
2017
2018
Mt
%
Mt
%
Mt
%
Mt
%
Mt
%
42.5
20.0
11.5
7.0
8.8
6.8
4.2
4.8
2.8
2.6
1.3
1.2
1.3
1.0
115.8
20.7
136.5
31.1
14.7
8.4
5.1
6.4
4.9
3.1
3.6
2.0
1.9
1.0
0.9
1.0
0.7
84.8
15.2
100.0
45.0
21.0
10.5
7.5
8.2
6.5
5.0
4.8
2.7
2.7
1.2
1.2
1.2
1.0
118.6
21.4
140.0
32.1
15.0
7.5
5.4
5.9
4.6
3.5
3.4
1.9
1.9
0.9
0.9
0.9
0.7
84.3
15.7
100.0
46.0
23.5
10.8
8.0
8.5
6.2
5.2
5.0
2.6
2.8
1.2
1.3
1.2
1.1
123.5
21.5
145.0
31.7
16.2
7.4
5.5
5.9
4.3
3.6
3.4
1.8
1.9
0.8
0.9
0.9
0.7
85.0
15.0
100.0
49.0
24.5
12.3
8.7
8.3
6.3
5.3
4.9
2.8
2.8
1.5
1.4
1.3
1.2
130.3
21.7
152.0
32.2
16.1
8.1
5.7
5.4
4.1
3.5
3.2
1.8
1.8
1.0
0.9
0.8
0.8
85.4
14.3
100.0
48.0
26.0
12.0
9.0
8.2
6.0
5.0
4.9
3.0
2.9
1.4
1.3
1.3
1.2
130.3
22.6
153.0
31.4
17.0
7.8
5.9
5.4
3.9
3.3
3.2
2.0
1.9
1.0
0.9
0.8
0.7
85.2
14.8
100.0
Source: (ABIROCHAS, 2018a; Montani, 2019)
15% SW does not significantly alter the mechanical properties of the
mortar/concrete (Ergün, 2011; Mashaly et al., 2016; Rana et al., 2015;
Singh et al., 2017b).
Omar et al. (2012) reported improvements of 30% in the compres­
sive strength of concrete cured for 3 days, and approximately 20% after
7 and 28 days using 5 to 15 wt% marble powder as an additive in the
concrete. The authors did not provide the particle size of marble powder,
but the measured specific surface area (11400 cm2/g) reveals its very
high fineness, even higher than typical OPC’s, which usually range from
3000 to 6000 cm2/g. In this sense, the filler effect is probably associated
with.
Some authors reported improvements with higher contents of SW.
Khyaliya et al. (2017) studied the workability of mortars by partially
replacing sand with SW. The authors bring data of the particle size and
water absorption of the marble powder with the river sand, allowing a
more reliable comparison. The river sand and marble powder presented
water absorption and fineness modulus of, respectively, 9.9% and
8.23%, and 2.13 and 1.45. They found that by incorporating marble
waste from 25 to 50%, it was achieved improvements in mechanical
performance due to the less water requirement. At 50% substitution, the
water required to attain the required workability fell by 6% and
compressive strength increased from 2.84 to 7.04 MPa. In this case, the
main contribution of marble dust comes from the improvement of the
workability instead of the filler effect, allowing for reducing the w/c
ratio. However, this improvement in workability goes in the opposite
direction to what most works reported.
Şahan Arel et al. (2016) noticed a reduction in workability as the
marble powder amount, in place of the fine aggregate, was increased.
However, the loss of workability and, consequently, the higher water
requirement due to the marble waste addition seems to be overcome
with the usage of superplasticizers, also noted by Ergün et al. (2011).
Gesoğlu et al. (2012) studied the effect of up to 20% of marble powder in
place of the concrete binder. The water/cement ratio was kept at 0.35.
The authors noticed that the higher content of marble powder, the
higher contents of superplasticizer were required to keep the same
slump flow. Tests carried out by Binici and Yilmaz (2007) and Hebhoub
et al. (2011) also reported slump losses by replacing fine aggregates with
marble powder. According to Rodrigues et al. (2015), superplasticizers
are highly recommended. Without them, they noticed negative effects
on the mechanical performance of concrete with up to 10% of marble
waste in place of cement. The authors also found an increase in the
compressive strength for concretes containing up to 5 wt% of waste as a
partial replacement for cement. Other studies have also adopted this
strategy (that is, superplasticizers) to preserve the workability of
Table 6
Raw-stone production and waste generated in the world (2003–2018).
Year
Raw-stone production (Mt)
Processing waste (Mt)
2003
2004
2005
2006
2007
2008
2009
2010
2011
2012
2013
2014
2015
2016
2017
2018
75.0
81.2
85.2
92.8
103.5
105.0
104.5
111.5
116.0
123.5
130.0
136.5
140.0
145.0
152.0
153.0
30.8
33.3
34.9
38.0
42.5
43.0
42.8
45.7
47.6
50.6
53.3
56.0
57.4
59.4
62.3
62.8
Source: (Montani, 2019).
of all the generated SW (~63 Mt in 2018) in concrete formulations, by
replacing aggregate or cement.
Concrete aggregates are divided into two distinct categories, namely,
fine (predominantly smaller than 5 mm) and coarse (9.5–37.5 mm)
(Kosmatka et al., 2002). Fine aggregates represent a quarter of the total
concrete matrix volume (Tiwari et al., 2016), and natural river sand is
considered the most suitable fine aggregate for concrete, but its
exploitation might lead to serious environmental impacts, compelling
authorities to implement restrictions (Bravard et al., 2013) and, conse­
quently, stimulating the usage of alternative materials. The same
concern exists to find alternative materials to cement due to
well-documented related environmental problems. Taking into account
its high fineness, we focused on the usage of dimension stone waste in
place of cement and fine aggregates.
There is a consensus on the recycling viability of SW into cementbased matrices, however, many controversies regarding the optimal
content, the influence on the workability of mortars and concretes, and
the possible chemical interactions between the cement paste and the
waste have arisen. The literature survey shows that the ideal SW content
can vary to an extent, depending mainly on the characteristics of the
waste, especially the particle size distribution, specific surface area, and
chemical composition, and on the application designed for the concrete/
mortar.
Many authors have shown that replacing Portland cement with up to
9
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
the cement content in the mix was reduced by 33%, reducing shrinkage
and improving water and carbonation resistance. Rana et al. (2015)
replaced the 10 wt% Portland cement with SW without compromising
the mechanical properties of the concrete. The authors also reported that
the higher the SW surface area, the lower the concrete workability.
Mashaly et al. (2016) replaced up to 20 wt% of cement with marble
sludge and observed an improvement in the mechanical properties of the
obtained concrete without changing the hydration products. Vardhan
et al. (2015) indicated that the replacement of up to 10% cement with
marble powder did not compromise the characteristics of the mixture,
and as opposed to the studies previously mentioned, the workability was
increased. The authors did not explain the reasons for this increase in
workability, but the SW used in the study by Vardhan (2015) had a
specific surface area ~50% smaller than that used by Rana et al. (2015).
The larger particle size of the waste might explain the improvement in
workability.
Singh et al. (2017b) demonstrated that 10–15% of cement can be
effectively replaced by marble sludge. The authors noticed an increase in
chloride permeability resistance with up to 15% replacement, but the
resistance to carbonation decreased with an increasing waste addition.
They attributed the improvement of chloride permeability resistance to
pore refinement, and the reduced carbonation resistance to the lower
bicarbonate alkalinity of the waste (89 mg/L) as compared to that of
cement (113 mg/L). The mechanical properties were maintained for
waste incorporation of less than 15%.
Some authors have specifically studied the stability of the hydration
products, especially in the long term and in adverse conditions (high
temperature, marine environment, and under the effect of bad weather).
Sudarshan and Vyas (2019) employed marble mining waste as a coarse
aggregate in concretes exposed to high temperatures (between 200 and
800 ◦ C). The properties were like those of the control mixtures up to
400 ◦ C, whereas above this temperature, the concrete undergoes dete­
rioration. The results obtained are not out of common sense since it is
known that marble-based or calcareous aggregates undergo decarbon­
ization in the 400 to 800 ◦ C range, resulting in higher porosities.
However, the authors stopped the heating process right after achieving
the maximum temperature. Without a holding time at 800 ◦ C, it is not
guaranteed that all CO2 was released. Kelestemur et al. (2014) investi­
gated the compressive strength of mortars with up to 50 wt% of marble
dust in place of sand at high temperatures. They held samples for 1 h at
the maximum temperature. From the authors’ data, it is possible to
notice a significant increase in porosity, but the authors claim that
marble dust improved the compressive strength. This improvement is
not well evidenced since glass fibres were randomly used together.
Khodabakhshian et al. (2018) evaluated the properties and dura­
bility of sixteen concrete mixtures containing powdered marble waste as
a partial replacement for mortars, replacing cement and fine aggregates.
It was found that substitutions of up to 5 wt% improved the mechanical
properties of the concrete obtained and with 10 wt% of marble powder,
the properties were like control. Due to the high fineness of marble
waste, higher than the fineness of fine aggregates used, the filler effect is
probably present. The authors also raise that the CaCO3 from marble
sludge can react with the cement paste to form calcium carboalumi­
nates. They support that calcium carboaluminates hydrates in the
interfacial transition zone and changes the surface of the aggregate,
turning it rougher and improving the bonding strength of
paste-aggregate. Lastly, it is mentioned that the rate of hydration of alite
is accelerated in the presence of CaCO3, resulting in a shorten induction
period. However, they did not investigate the microstructure of mortars
to provide evidence to support these statements.
Gencel et al. (2012) partially replaced the aggregates of
cement-paving blocks with marble waste. The authors noted that, in
proportion to the increase in the waste content, the mechanical strength
decreased, while the durability by freeze-thaw and resistance to abrasive
wear increased. In addition to technical properties, feasibility studies
have shown that the cost of concrete dropped from 34 to 30 US$/m3
Table 7
Main potential applications for SW.
Main group
Building
materials
Hydraulic and
alkaliactivated
binders
Specific
applications
References
Filler
Fine sand
replacement
Fine aggregate
Aliabdo et al. (2014)
Khyaliya et al. (2017)
Fine aggregate for
self-compacting
concrete
As starting material
for clinkers
Geopolymers
Asphalt mixtures
Portland cement
replacement
Ceramic
formulations
Tiles and
bricks
Porcelain
stoneware tiles
Bricks
Floors and tiles.
Industrial bricks
Light bricks
Environmental
applications
Other
applications
Adsorbents
and soil
rehabilitation
Functional
filler
Removal of toxic
elements in
aqueous media
Removal of toxic
elements in
gaseous media
Correction of acidic
soils
Cemented landfills
of sulfide tailings
Landfill
waterproofing
material and
artificial soil
For paper, rubber,
paints and
pharmaceuticals
products
(Gencel et al., 2012;
Kore Sudarshan and
Vyas, 2019)
Vardhan et al. (2019)
(Alyamaç and Ince,
2009; Tennich et al.,
2015; Uygunoğlu
et al., 2014)
Sadek et al. (2016)
(El-Alfi and Gado,
2016; Raupp-Pereira
et al., 2008)
(Clausi et al., 2018;
Palmero et al., 2017;
Simão et al., 2020b;
Tekin, 2016; Thakur
et al., 2019)
(Akbulut and Gürer,
2007; Karaşahin and
Terzi, 2007)
(Khodabakhshian
et al., 2018; Mashaly
et al., 2016; Rana
et al., 2015)
Yeşilay et al. (2017)
(Menezes et al., 2005;
Saboya et al., 2007)
(Acchar et al., 2006;
Segadães et al., 2005)
Bilgin et al. (2012)
Eliche-Quesada et al.
(2012)
(Ghazy et al., 2005;
Mehta et al., 2016)
Davini (2000)
(Tozsin et al, 2014b,
2015, 2014b)
Ercikdi et al. (2015)
Careddu and Dino
(2016)
Careddu et al. (2014)
mixtures at suitable values (Corinaldesi et al., 2010; Gesoğlu et al., 2012;
Hebhoub et al., 2011; Kaplan and Yilmaz, 2007; Topçu et al., 2009).
The feasibility of using this waste while still meeting the re­
quirements implemented by specific legislations has already been
considered. Alyamaç et al. (2015) found an ideal proportion of 40 vol%
of waste while still meeting the TS EN 197-1 standard (TSE, 2002). This
standard specifies compliance criteria, including physical and chemical
requirements for commercial cement. Aruntas et al. (2010) showed that
samples containing up to 10 wt% of waste in cement mixtures resulted in
compressive strengths exceeding 30 MPa at 7 days, also in agreement
with the TS EN 197-1 standard (TSE, 2002).
Li et al. (2018) replaced an equal volume of cement with waste (as a
filler) without changing the proportions of the mixture. In contrast to the
common route (that is, replacement of cement or aggregates by waste),
the authors replaced the cementitious paste with SW. With this method,
10
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
(~10%), when using 40% of marble waste as an aggregate, that is, 0.1
US$/m3 for each % waste added.
Other studies used marble waste to improve the properties of the
fresh and hardened state of self-compacting concretes (SCC) (Alyamaç
and Ince, 2009; Tennich et al., 2015; Uygunoğlu et al., 2014). The use of
SCC in construction is widespread because it combines high perfor­
mance and launching ease without the need for vibration and other
additional processes. The preparation of this type of concrete requires
the use of very fine aggregates and additives, which influence the con­
crete fresh state performance and are usually expensive. Accordingly,
SW is potentially useful because of its high fineness and particles smaller
than 200 μm (see Table 4). These characteristics are effective for the
cohesion of mortar and concrete, without loss of energy during work­
ability, as is usual in other ultrafine mineral additions (such as silica
fume) (Corinaldesi et al., 2010).
Sadek et al. (2016) used three SW types (single or mixed marble and
granite powder) in SCC. The results indicated that up to 50 wt% of the
material could be used as a mineral additive. Corinaldesi et al. (2010)
showed that a 10% replacement of commercial sand with marble pow­
der provided the maximum mechanical strength (~52 MPa) with the
same workability in the fresh state. In the early stages, the authors also
identified a positive filling effect on the samples.
Durability studies for SCC have also been reported in the literature.
Tennich et al. (2017) evaluated the incorporation of marbles, marble
tiles, and gravel into different self-compacting concretes exposed to
attack by sulphates, with the samples being immersed in seawater and a
solution of sodium sulphate. The results showed that the SW incorpo­
ration had a positive effect on the durability of these concretes, as it
increased the compaction and decreased the sulphate ion permeation
that may be present in the air, water, and aggressive soils.
Vardhan et al. (2019) evaluated the strength, permeation, and
microstructure of concretes with marble waste partially replacing river
sand as a fine aggregate. According to the authors, the maximum
improvement was achieved at a 40% replacement level. The authors
attributed the improvement in strength to the filler effect. The higher SW
density as compared to the sand used probably also contributed to the
improved mechanical properties. The higher fineness and the
angular-shaped particles led to a concrete workability loss.
Another point is whether the contribution of dimension stone pow­
der comes from the exclusive filler effect, or if there are also chemical
interactions involved. Şahan Arel et al. (2016) reported an improvement
in the mechanical properties and associated this phenomenon with the
presence of CaCO3 and SiO2 but did not provide evidence. Omar et al.
(2012) state the possible contribution from the filler effect and chemical
interactions on mechanical performance. The authors state that active
SiO2 from marble powder can react with Ca(OH)2 from cement to form
secondary calcium silicate hydrate, making the structure more stable
and denser. However, no evidence has been provided it. Since the au­
thors used low contents of waste with a relatively low content of SiO2
(14 wt%), this phenomenon seems improbable.
The existence of a pozzolanic effect would be more plausible in
granite-based stones due to the higher SiO2 contents in which can be
directly noticed by quantifying the calcium hydroxide consumption by
the Chapelle test. Indeed, Musil et al. (2021) did it and noticed that
although granites contain large quantities of silicon (higher than 50 wt
%), they are not very reactive, with a calcium hydroxide consumption
under 400 mg Ca(OH)2 by a gram of sample.
Vuk et al. (2001) evaluated the effect of 5% limestone addition on
the compressive strength, setting time, and heat of hydration of clinkers.
The authors observed a reduction in initial and final setting time with
limestone addition. The compressive strength improved at 2 and 7 days
but reduced with 28 days of hydration. The heat of hydration is not
significantly altered within the first 3 days but decreases after 14 days.
Some authors reported the formation of carboaluminate (Cochet and
Sorrentino., 1993; Ramachandran, 1988; Sawicz and Heng, 1996; Tsi­
vilis et al., 1999) and carbosilicate hydrates (Chloup-Bondant; and
Edvard., 1998; Péra et al., 1999) from the interactions of CaCO3 and
C3A, and CaCO3 and silicate phases, respectively. It has been reported
that the CaCO3 might accelerate the hydration of cement, especially C3S
in the early stages, providing new nucleation sites for calcium silicate
hydrates. CaCO3 can also react with C3A to form carboaluminates
(Kakali et al., 2000; Ramachandra and Chun-Mei, 1986; Trezza and
Lavat, 2001). According to Feldman et al. (1965), this reaction is driven
by a solid-state mechanism, where the addition of CaCO3 modifies the
initial reaction of C3A with water because of the barrier formation of
hydrated calcium carboaluminates (C3A.CaCO3.xH2O) on the surface of
C3A. Ramachandran and Zhang (1986) reported that the higher the
amount and fineness of CaCO3, the higher the hydration rate of C3S.
Husson et al. (1992) demonstrated the formation of calcium silicocar­
bonate hydrates for large quantities of CaCO3.
Many works reported that the increase in resistance is related to the
densification of cementitious matrices by the combined action of the
filler effect and the possible formation of carboaluminates inside the
pores, contributing to the reduction of residual porosity. Vardhan et al.
(2019) stated that in addition to the filler effect, the densification of the
mix was achieved by the improvement in the binding ability due to the
presence of the calcium carboaluminate phase. However, this phase did
not appear in their XRD analyses. Ramachandran (1988) showed the
effect of CaCO3 on the C3S and C3A + gypsum systems. The authors
evidenced that CaCO3 produces an acceleration effect and influences the
early setting and early strength development. The formation of com­
plexes would be expected to influence the durability of cement. The rate
of ettringite formation and its conversion to the monosulphoalumimate
is accelerated by CaCO3.
Even in the literature reporting that CaCO3 can react with calcium
aluminate and calcium silicate phases to form hydrated products, there
is no clear evidence that carboaluminate and carbosilicate hydrates are
formed with marble waste incorporation. The particle size of waste and
the crystallinity of those phase formed has to be considered. When the
waste is used to replace fine aggregates, the average particle size must be
compatible with the sand, which is large enough to be considered inert.
In these cases, the physical filler effect is possibly the main reason
behind the increase in resistance. When the waste fineness is comparable
to those of cement, its replacement as a limestone filler is enabled, and
secondary hydrated products, such as carboaluminates and carbosili­
cates, can (or not) be formed. This hypothesis still needs further inves­
tigation from a microstructural point of view. If, on the one hand, the
formation of this compound was attributed to the increase in mechanical
strength, the durability of concrete tends to be reduced, especially in the
presence of chloride. Carboaluminate is unstable in a chloride envi­
ronment. The Cl ions from the environment react to form chlor­
oaluminates (Feldman et al., 1992) but Singh et al. (2017b) observed
improvements in chloride resistance.
Lastly, carboaluminates are also unstable in sulphated environments.
Khyaliya et al. (2017) tested mortars containing 25 wt% SW replacing
the river sand exposed to sodium sulphate and sulphuric acid solutions.
The mixes were compared with a reference mortar, and it was concluded
that SW can be safely used in both aggressive and non-aggressive
environments.
Most of the literature reveals that the positive effects of marble
powder were more pronounced when used in place of natural sand than
as a cement replacement. The main influencing factor is the grain size of
the aggregates, with the filler effect explaining the gains in strength due
to the high fineness of marble powder. On the other hand, the same
effect led to a loss of workability, requiring the usage of plasticizers. The
greater the surface area and lower particle size, the higher the loss of
workability and water demanding (or superplasticizer). But even on
keeping similar grading curves for marble waste and natural sand, the
workability of concrete mixtures also decreased with increasing per­
centages of marble. This can be related to the chemical interactions of
marble waste with cement or the uneven morphology of marble dust,
with angular structure against the smooth and round natural sand
11
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
particles. SEM surface images of marble powder and river sand particles
can be observed in (Awad and Abdellatif, 2019) and (Khyaliya et al.,
2017), respectively.
Concerning the chemical interactions between SW and hydrated
cement, to the best of our knowledge, there is not enough evidence to
support the chemical interaction of marble powder and hydrated
cement. The probable phenomenon is the filler effect due to the high
fineness of the waste. That is why many authors observed an improve­
ment in mechanical strength when used in place to natural sand with a
higher average particle size, mostly up to 10–15%. When spaces are
filled and the filler effect no longer exists, maximum improvement was
achieved. So, the content of marble powder and the positive effects
obtained will depend on the mix design of the control mixture. The
better the mix proportioning of the original mixture, the less the
contribution of the waste. Table 8 summarizes the approach and im­
provements from the literature analysed.
Some authors have evaluated the use of SW materials as a component
of eco-clinkers and the subsequent functionalisation of mortars.
Raupp-Pereira et al. (2008) formulated new cementitious materials
(clinkers) from industrial wastes, such as Al anodising mud, water
treatment plant mud, marble sawing mud, and foundry sand.
Belitic calcium sulphoaluminate cement was successfully obtained
by El-Alfi et al. (2016) using 55 wt% marble sludge, 20 wt% gypsum,
and 25 wt% kaolin at temperatures ranging from 1200 to 1250 ◦ C. These
types of cement, usually used in precast and cold environments, are an
alternative to conventional Portland cement, being more friable and can
be obtained at lower temperatures.
The use of marble waste as a filler in asphalt mixtures has also been
evaluated (Akbulut and Gürer, 2007; Karaşahin and Terzi, 2007). In
addition to the technical properties, the transport cost assessed in the
study by Karaşahin and Terzi (2007) proved to be viable when compared
to the cost involved with other commercial fillers. This is because
samples using SW and limestone had similar plastic deformations, and
the costs of transporting this waste were lower than the costs from
commercial samples.
Recently, Davidovits argued that the use of fly ash for the production
of geopolymers would not be as sustainable as previously thought
(Davidovits, 2020). According to this author, the generation of ash from
the burning of coal generates large amounts of CO2, for example, 10 t of
coal produces 1 t of fly ash and emits 33 t of CO2. Alternatively, the
researcher encourages new studies on geological raw materials, that are
available worldwide. Accordingly, some authors have used SW materials
in geopolymerisation processes (Clausi et al., 2018; Tekin, 2016; Thakur
et al., 2019). Palmero et al. (2017) used SW in geopolymers, composed
of quartz, feldspar, biotite, and dolomite, with thermal curing at
80 ◦ C/48 h. Choi et al. (2010) studied the replacement of up to 30 wt%
of the raw materials with SW in geopolymer formulations. The use of
these materials tends to improve their mechanical strength.
Simão et al. (2020b) studied different concentrations of stone sawing
powder to replace metakaolin (0–90 wt%), generating products with
different properties and possible applications. At 50 wt% SW, the
compressive strength was satisfactory for application as a building ma­
terial (>25 MPa), while at 75 wt% the compressive strength was
compatible with coating mortar (>6 MPa) achieving ~15 MPa. For
comparison, previous studies achieved compressive strengths between
10 and 15 MPa using 75 wt% of biomass ash (De Rossi et al, 2019, 2020,
2019; Simão et al., 2020a). These results demonstrate that SW can be
used as an alternative material to fly ash in geopolymer materials and
provide great opportunities for advances in the reaction mechanisms.
7.2. Ceramic formulations
Many studies have examined and characterised sludge derived from
the sawing of granite, quartzite, and marble stones, envisioning their use
in traditional ceramic formulations (Torres et al, 2004, 2007). Yesilay
et al. (2017) obtained positive results when evaluating the possibility of
using these materials (up to 27 wt%) in the production of artistic
stoneware clay bodies sintered at 1160 ◦ C. Plasticity and shaping
capability are particularly important for these products. According to
the authors, and the addition of up to 27% of SW did not cause any
deterioration in the dimensional stability of the product. However, the
authors report a huge increase in water absorption (between 11 and
14%) in comparison to the standard sample (~7%). Although the au­
thors did not evaluate porosity, the increase in water absorption sug­
gested that this occurred very probably due to the release of CO2 from
marble waste.
Table 8
Compiled data from published works that used SW in mortars and concretes.
Reference
SW as a replacement of
Content (wt.%)
Improvements on
Ergün et al. (2011)
Aruntas et al. (2010)
Rana et al. (2015)
Mashaly et al. (2016)
Vardhan et al. (2015)
Singh et al. (2017b)
Cement
Cement
Cement
Cement
Cement
Cement
up to 5.0
up to 10.0
10.0
20.0
up to 10.0
10.0–15.0
Compressive strength
Compressive strength
Durability
Mechanical properties
Workability
Chloride permeability resistance
Omar et al. (2012)
Khodabakhshian et al.
(2018)
Rodrigues et al. (2015)
Şahan Arel et al. (2016)
Cement
Cement
up to 15.0
up to 10.0
Compressive strength
Compressive strength
Cement
Cement and Fine aggregates
Compressive strength
Compressive strength
Workability
Workability
Gesoğlu et al. (2012)
Hebhoub et al. (2011)
Binici and Yilmaz (2007)
Gencel et al. (2012)
Fine aggregates
Fine aggregates
Fine aggregates
Fine aggregates
Up to 5.0
5.0–10.0 (in place of cement); 50.0–70.0 (in
place of aggregates)
5.0–10.0
25.0
15.0
40.0
Workability
Workability
Workability
Corinaldesi et al. (2010)
Tennich et al. (2017)
10.0
Vardhan et al. (2019)
Khyaliya et al. (2017)
Fine aggregates
Limestone filler in selfcompacting concretes
Fine aggregates
Fine aggregates
Compressive strength
Compressive strength
Compressive strength
Durability by freeze-thaw and the resistance
to abrasive wear
Mechanical strength
Durability
Uysal (2011)
Uysal and Yilmaz (2011)
Aliabdo et al. (2014)
Fine aggregates
Cement
Fine aggregates
10.0
10.0
10.0
40.0
25.0–50.0
Mechanical properties
Mechanical performance, workability, and
durability
Compressive strength
Compressive strength
Mechanical properties
12
Deterioration on
Carbonation
resistance
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
In addition to the use in white ceramic formulations, some authors
have studied the use of these materials in red ceramic formulations
(Menezes et al., 2005; Monteiro et al., 2004). Menezes et al. (2005)
evaluated the possibility of using granite cut waste as an alternative raw
material to produce bricks and tiles. The authors reported a gradual loss
of plasticity with increasing additions of SW, but not enough to exceed
the required values defined for extrusion. The results also showed that
the waste has a chemical composition similar to commercial raw ma­
terials, which include clays, quartz, and feldspar. Samples with up to
50% of waste presented water absorption values below the maximum
recommended values of 25% for bricks and 20% for tiles as well as a
minimum module of rupture values of 5.5 MPa for bricks and 6.5 MPa
for tiles. Even so, it can be evidenced a tendency of the higher the
content of SW, the higher the porosity, especially in the case of bricks. In
this case, this happens as SW is more refractory than the clay used.
Segadães et al. (2005) used waste from sawing marble and granite in
a mixture based on red clay to produce floors and tiles. The results show
that the addition of ~30 wt% did not promote negative effects on the
mechanical properties of the final product and has the additional benefit
of enabling the use of lower temperatures during firing. The porosity
induced by decarbonization of calcium carbonated was counteracted by
the melted liquid formed especially due to the presence of alkaline and
iron oxides, which act as fluxing agents.
Saboya et al. (2007) used marble-derived waste into ceramic bricks
fired in the 750 to 950 ◦ C range. The authors reported a loss of plasticity
with the incorporation of waste, requiring higher contents of water for
extrusion. They also noticed some improvements in the water absorption
and strength with up to 20% waste. Acchar et al. (2006) used waste
percentages composed of marble and granite between 10 and 50 wt%
into fired the ceramic products sintered at temperatures ranging from
950 to 1150 ◦ C. The authors claim that granite and marble sludge can be
added to the clay-based material with no detrimental effect on the
properties of the sintered red-clay products. However, it can be noticed
from their results a significant increase in water absorption and reduc­
tion in apparent density and flexural strength, except to the composition
with the highest content of waste (50 wt%) at the highest temperature
(1150 ◦ C), where the flexural strength is improved even with higher
porosities. The authors attributed this phenomenon to the waste acting
as a fluxing agent, strengthening the matrix.
Vieira et al. (2004) studied the incorporation of granite waste (up to
40 wt%) in red ceramic formulations. The authors also found a reduction
in plasticity with the increasing addition of SW. However, as the partner
factory where the study was performed preferred to use excessively
plastic formulations to soften the wear of equipment, the loss of plas­
ticity was not an issue for extrusion. Different from the previously cited
works, the authors evidenced an increase in thermal shrinkage and bulk
density with a gradual reduction in water absorption with up to 40 wt%
of waste. Even so, the flexural strength was little altered by considering
the standard deviation.
Torres et al. (2004) studied a lot of formulations with granite-derived
waste in place of feldspar in porcelain tiles, due to the similarity between
waste and feldspar chemical compositions. According to them,
depending on the dosage of waste and sintering temperature it is
possible to obtain superior properties comparing to the commercial
porcelains, with regards to water absorption, flexural strength.
Torres et al. (2007) used granite and quartzite-based waste in
red-clay-based stoneware tiles with high levels (60–70 wt%) of incor­
poration sintered between 1100 and 1200 ◦ C. The authors noticed
values flexural strengths more than triplicate and water absorption
decreased by more than one order of magnitude with the incorporation
of granite sludge.
Bilgin et al. (2012) added marble waste (up to 80 wt%) in the pro­
duction of industrial bricks sintered in the range of 900–1000 ◦ C. Ac­
cording to the authors, the addition of up to 10 wt% did not produce
significant changes in the technical properties of the final product.
However, their results show a clear tendency to increase water
absorption and decrease flexural strength for most of the samples tested.
Eliche-Quesada et al. (2012) produced bricks with marble waste
(5–20 wt%) sintered at 950 and 1050 ◦ C. They claim to be possible to
add up to 15 wt% of waste with no significant deterioration on me­
chanical properties when samples are fired at 1050 ◦ C. Lower temper­
atures increased the open porosity and, consequently, decreased the
mechanical properties.
Table 9 summarizes the analysed literature that used SW in ceramic
products. Most of the raw materials used to produce the aforementioned
ceramics, such as feldspars, kaolin, clays, and quartz are predominantly
composed of silica and alumina, whose combination at high tempera­
tures generates mullite. Mullite is an aluminosilicate, which is stable at
ambient conditions and exists over a composition interval ranging from
3:2 to 2:1 of the ratio Al2O3 to SiO2. Although the production of mullite
from starting materials with particle sizes in micrometer-scale requires
temperatures higher than ~1300 ◦ C (or from ~1100 ◦ C with nano-scale
starting materials), metastable mullite can be formed at lower temper­
atures in multi-phase systems such as ceramic formulations due to the
presence of other components.
Granite and quartzite-based wastes are also predominantly
composed of silica and alumina, allowing for to be added even at high
concentrations without significantly changes the overall chemical and
mineralogical composition of the targeted product. Most authors re­
ported improvements in the mechanical performance of ceramic prod­
ucts with this waste, with higher flexural and compressive strength and
lower water absorption. The explanation for these achievements is the
presence of fluxing agents on the chemical composition of waste, very
especially the sum of iron, sodium, and potassium oxides, mostly in the
Table 9
Compiled data from published works that used SW in ceramic products.
Reference
Product
Content
(wt.%) and
type of
dimension
stone
Sintering
temperature
(◦ C)
Main results
Yesilay
et al.
(2017)
Artistic
stoneware
clay bodies
10.0–27.0
(marble)
1160.0
Menezes
et al.
(2005)
Bricks and
floor tiles
20.0–60.0
(granite)
1150.0–1200.0
Segadães
et al.
(2005)
Floor tiles
10.0–30.0
(mix of
marble and
granite)
1100.0–1150.0
Saboya
et al.
(2007)
Vieira
et al.
(2004)
Bricks
5.0–20.0
(marble)
750.0–950.0
Increase in water
absorption and
decrease in thermal
shrinkage
Little increase in the
water absorption
and improvement on
mechanical
performance with up
to 35% of SW
No significant
detrimental changes
on
physicomechanical
properties
Increase in porosity
and flexural strength
Bricks
10.0–40.0
(granite)
970.0
Torres
et al.
(2004)
Porcelain
tile
20.0–50.0
(granite)
1140.0–1200.0
Torres
et al.
(2007)
Red-claybased
stoneware
tiles
Bricks
60.0–70.0
(granite
and
quartzite)
10.0–80.0
(marble)
1100.0–1200.0
Bilgin
et al.
(2012)
13
900.0–1100.0
Decrease on the
water absorption
and increase on
thermal shrinkage;
no changes in
flexural strength
Reduction on water
absorption and
improved flexural
strength
A great increase in
flexural strength and
reduced water
absorption
Increase in water
absorption and
decrease in flexural
strength
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
range of 7–18%. Therefore, the usage of granite-derived waste in place
of starting materials with fewer contents of fluxing agents is the key to
obtain ceramic products with improved properties. Torres et al. (2007)
which obtained the best results with exceptional improvements con­
cerning strength and water absorption had the waste with the highest
content of fluxing agents (~18% of iron, sodium, and potassium oxides
summed).
In summary, the presence of fluxing agents promotes the formation
of phases with lower melting points. The melted liquid fills the pores and
improves the bonding strength of the ceramic matrix, reducing the
overall porosity and improving the mechanical performance. There are a
lot of possible phases from the combinations of sodium, potassium, and
iron oxides with silicoaluminate-based materials, as can be noticed
through phase diagrams (Lecomte et al., 2004; Moosavi-Khoonsari and
Jung, 2017; Roth, 1970; Yeşilay et al., 2017). However, different from
the highly-controlled environment in which phase diagrams are built, in
industrial processes, the chemical interaction between those oxides at
high temperatures commonly results in a glassy phase, making their
identification a challenging task.
When marble-derived waste is added, especially at concentrations
above 10 wt%, mullite is partially converted into anorthite (CaO.
Al2O3.2SiO2). While mullite melts at around 1890 ◦ C, the melting point
of anorthite is 1553 ◦ C (see Fig. 6). Therefore, even being calcium oxide
highly thermally stable, its thermal interaction with silicoaluminatebased materials leads to the formation of anorthite, reducing the
melting and sintering temperatures of ceramics. The formation of
anorthite is helpful concerning the mechanical performance of ceramics.
On the other hand, the formation of this phase does not seem to
compensate for the open porosity generated from the decarbonization of
marble waste. Still, anorthite just appeared in the mineralogy of prod­
ucts sintered at above 1000 ◦ C.
Typical starting materials used in the production of clay-based
ceramic commonly show variations in their chemical and mineralog­
ical compositions but still are broadly used. In this sense, even granitebased waste also presenting some fluctuations in their chemical com­
positions, their recycling can be viable by storing big lots of materials as
done for other raw materials. In the case of marble-based waste, its
incorporation in ceramic material aiming to increase the mechanical
strength and reduce the specimens’ porosity might not be the best
strategy. An interesting alternative can be its use as foaming agent to
replace the commonly used calcium carbonate in the production of
porous ceramics.Simão et al, 2013, 2015
Simão et al. (Simão et al, 2013, 2015) used CaCO3 (a commercial raw
material) as a pore-forming agent in porous ceramics for filtration ap­
plications. The generation of pores was due to the decarbonization of
CaCO3 at ~800 ◦ C, releasing CO2 and producing porosity.
Some authors used commercial calcium carbonate (Zhu et al., 2016)
or calcium carbonate-based waste (Souza et al., 2017; Teixeira et al.,
2017) to produce glass foams for thermal insulation applications. Glass
foams are materials with high porosity, generally above 60% by volume.
They are widely used as structural materials due to their low density,
low thermal conductivity, high sound absorption, high stiffness, and
good chemical inertia. The ecological glass foams obtainment, using SW
as a pore-forming agent, which presents interesting thermo-acoustic
properties, seems to be a suitable destination for this waste containing
high calcium carbonate contents.
Porous anorthite-based insulating firebricks are another promising
option. According to ASTM classification, which considers the bulk
density and maximum service temperature, anorthite (CaO.Al2O3.2­
SiO2) is suitable for maximum temperature limits of around
1100–1200 ◦ C. Insulating firebricks must have a highly porous structure
(usually between 45% and 90% porosity) and exhibit low thermal
Fig. 6. Ternary phase diagram of the CaO–Al2O3–SiO2 system (Adapted from Yeşilay et al., 2017) with the highlight in the region of anorthite (CaO.Al2O3.2SiO2).
14
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
conductivity values. Some authors (Sutcu et al., 2012; Sutcu and Akkurt,
2009, 2010) successfully obtained anorthite-based refractories by using
paper industry waste as a source of calcium carbonate. Analogously,
these materials might be produced with SW instead. Finally, it is
important to mention that, unlike recycling in cementitious materials,
the use of SW in ceramic materials result in the release of CO2 during
sintering process. Therefore, these applications do not fit perfectly into
the concept of sustainability and circular economy, which aims not only
to minimize the use of resource inputs and waste generation, but also
carbon emissions (Geissdoerfer et al., 2017). This said, a life cycle
analysis should be carried out in order to fully perceive the environ­
mental impacts of the proposed route compared to conventional foam­
ing agents.
capacity of 1.20 mg/g in a neutral medium after 3 h of contact and was
considered an effective adsorbent for fluoridated water (Mehta et al.,
2016).
Davini (2000) tested white marble SW from northern Tuscany “in
nature” and calcined at 900 ◦ C as an SO2 sorbent material for atmo­
spheric emissions. After calcination, the desulphurisation properties of
the waste were better than those obtained from commercial limestone.
This improved performance is the result of combining a larger surface
area with adequate distribution of the CaO pore size after heat
treatment.
When these environmental applications are suggested, one must
consider the other ions that the waste may be solubilising at the time of
application, as discussed in Section 4. These questions should be part of
the study so that, in the end, there is no removal of an element toxic and
the leaching of another. For these reasons, environmental applications
are less explored, as compared to the numerous studies on traditional
ceramics and cementitious materials.
7.3. Environmental applications
The use of marble waste in environmental remediation applications,
such as the removal of toxic elements from aqueous media (Ghazy et al.,
2005; Mehta et al., 2016) and gaseous media (Davini, 2000), to the
correction of acidic soils (Tozsin et al, 2014b, 2015, 2014b), has also
been considered.
Ercikdi et al. (2015) studied the use of marble granules as an additive
to Portland cement applied to the cemented landfills of sulphide tailings.
Although this material has not demonstrated a pozzolanic effect (reac­
tivity with calcium hydroxide), its use has improved the mechanical
performance of the landfill in the short and long term, in addition to
favouring the acid buffering capacity of the tailings (Ercikdi et al.,
2015). The acid buffering capacity is the result of the alkaline character
of the CaCO3 present in the waste, which can also be used for the
remediation of acidic and calcium-deficient soils (Tozsin et al, 2014b,
2015, 2014b). Tozsin et al. (2014a) determined the effectiveness of
using these materials to neutralise soil acidity. The results showed that
the pH of the soil increased from 4.7 to 6.4 after using this material. In a
similar study, the same authors (Tozsin et al., 2014b) employed stone
and marble powder in hazelnut-producing fields, increasing the soil pH
from 4.71 to 5.88, thus improving the production yield from 1120.3
kg/ha to 1605.5 kg/ha. The results suggest that marble waste can be
successfully used to buffer acidic soils, thus reducing the negative
environmental impacts (Tozsin et al., 2014a).
Kabas et al. (2012) studied the possibility of recovering native
vegetation in a deactivated tailing pond in south-eastern Spain using
marble waste and pig farming mud. The results showed that these ma­
terials were effective in increasing the growth of vegetation, increasing
plant cover and biodiversity, and reducing the mobility of heavy metals,
such as Pb, Zn, and Cd (Kabas et al., 2012).
Rapid industrialisation has led to an increase in the disposal of waste
containing metals that are toxic to the environment. This, in turn, has
created the need for alternative treatments to adapt the concentrations
of these elements to the limits stipulated by environmental agencies
(Ghazy et al., 2005). Accordingly, some studies applied SW to adsorb
heavy metals (Ghazy et al., 2005; Mehta et al., 2016).
Laboratory experiments were conducted in aqueous solutions to
remove Al ions (Al3+) using marble powder as a sorbent material. The
procedure was successful, and SW was not leached by acids because of
the solubility of the sorbent. The control of this element is important
because it is present in several compounds used worldwide for several
applications, such as Al salts used as coagulants in water treatment
plants (Ghazy et al., 2005).
Similar to Al, other elements are controlled in drinking water
worldwide. Fluoride is a chemical compound that can cause adverse
effects when in high concentrations in the drinking water consumed by
the population, leading to dental fluorosis and, in more severe cases,
skeletal fluorosis. Accordingly, alternative techniques have been studied
to solve problems with fluoridated water. Mehta et al. (2016) used
marble powder after calcination at 650 ◦ C as an adsorbent for fluoride
ions in aqueous solutions. The obtained powder showed an adsorption
7.4. Other applications
By following the industrial applications of calcium carbonate, it is
possible to identify other specific applications for marble-derived SW.
For instance, calcium carbonate is widely used as an extender or filler in
paints. The main purpose of an extender is cost reduction and also to
increase spreadability and strength. They generally have weak colouring
power. As marble-derived SW usually contains traces of chromophoric
agents such as chromium and lead, its use can change the shade of the
paints.
Very recently, Tressmann et al. (2020) published the first research
into the use of untreated marble waste (up to 80 wt%) as mineral filler in
soil pigment-based paints and as an active pigment in waterborne paints.
The authors observed through hiding power, abrasion resistance,
microbiological attack, and resistance to weathering analyses that paints
manufactured with marble waste meet the normative specifications for
economical latex paint. The performance of the paints produced with
soil pigments was improved by incorporating marble waste powder as
mineral filler, especially for higher contents than 40%. The indicated
formula with the highest total desirability was the paint with 30%
polyvinyl acetate resin and 70% marble waste.
Since marble-derived waste is an inert material for paints, other SW
can be analogously tested. Lopes et al. (2019) studied the influence of
the granite waste, actuating as mineral filler, on the performance of
polyvinyl acetate latex paints produced with soil pigments. They found
satisfactory results with a paint presenting 29% of PVA resin and 71% of
granite waste. Although some studies report favourable results with the
addition of SW in paints, the content and the influence of the SW
chromophoric elements in the colour variations of the paints were not
investigated. Indeed, the content of chromophoric elements in paints
can broadly vary for different colours and manufacturers. Among the
elements present in the SW, lead and chromium are widely detected in
all colours, including white. Exemplifying, Megertu and Bayissa (2020)
investigated commercially available oil-based house paints for residen­
tial use and found chromium contents ranging from 43 ppm (white) to
5450 (orange). Also, they found lead in all samples with different col­
ours from different manufacturers, with contents between 41 ppm and
51200 ppm.
In this case, by considering that SW contains those elements at lower
concentrations than found on commercial paints, the SW recycling as
filler seems viable. The content of chromophoric agents can be later
adjusted in the formulations. On the other hand, the presence of heavy
metals, with or without SW, turns on the alert for another discussion, the
health problems associated with human exposure to those paints (Sor­
oldoni et al., 2018; Turner et al., 2016; Wang et al., 2020).
Differently, some authors carried out studies to obtain pure calcium
carbonate from marble waste for use as a filler, enabling its use also in
the paper industry, which is much more rigorous concerning the purity
15
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
of fillers (El-Sherbiny et al., 2015; Erdogan and Eken, 2017; Lu et al.,
2018).
Calcium carbonate, as well as carbon black, silica, clays, and others,
are used as fillers of natural rubber compounds aiming for improving
physical and mechanical properties. Ahmed et al. (2013) evaluated the
potential of marble sludge as a filler in natural rubber. In this case, the
efficiency of reinforcement into filled rubber compounds depends on a
complex interaction of filler-related parameters and bonding quality
between fillers and rubber matrix. The authors tested the rheological,
mechanical, and swelling behaviour of composites. From their results, it
can be noticed no improvements with marble waste incorporation in
place to silica. Even so, they recommended its usage based on the cost
reduction.
Still concerning the usage SW into polymeric matrices, Awad and
Abdellatif (2019) used dimension stone waste as reinforcement (10–50
wt%) in low-density polyethylene matrix and achieved improvements in
mechanical and thermal properties. Abenojar et al. (2021) sought a
composite material based on marble waste into a polyester matrix for
being used as a floor or wall in buildings with improved fire resistance.
According to the authors, marble improves the mechanical properties
and fire resistance of polyester. The endothermic decomposition reac­
tion of CaCO3 releasing CO2 at around 700–800 ◦ C is responsible for the
high fire resistance and the flame extinction. Similar findings with
polyester-based composites with marble waste were reported by Nayak
et al. (Nayak et al., 2020; Nayak and Satapathy, 2020). Lastly,
pre-calcined dolomite and calcite are commonly used as solid base
catalysts for steam reforming to H2 production (Constantinou et al.,
2010), inspiring researchers to use SW instead (Kannapu et al., 2021).
2013). Analogously, recycling centres could be created near urban areas
where SW could be managed and stored in large batches, aiming to
homogenize their chemical composition. These recycling centres would
reduce the disposal costs for companies, new jobs would be created, and
would be easier inspected and regulated. Therefore, this strategy would
bring environmental, economic, and social benefits to the region.
Exemplifying the potential economic and environmental gains with
SW recycling, Şahan Arel et al. (2016) estimated (from 2014 data on
Turkey) a reduction of costs from US$40/m3 for concrete production to
US$36/m3 when 50% of the fine aggregates is replaced by marble dust,
representing 0.08 US$ for each % of waste added. Nevertheless, these
values should be considered with caution as the potential cost-benefit
will be hugely dependent on context, the mix design, and the type of
concrete being produced. Uysal and Sumer (2011) reported a cost
reduction of around US$ 4/m3 for each 10% of marble dust added into a
self-consolidating concrete while preserving a mechanical performance
similar to the control mix.
9. Final remarks
This work conducted a systematic review on the cutting and pol­
ishing waste of dimension stones, including features such as classifica­
tion, potentiality, quantity, viability, and possible applications.
Generally, SW is normally considered a inert meterial, as it contains
elements that are already naturally found in natural stones. However,
owing to the high fineness of SW (<200 μm) resulting from the cutting
and polishing process, the possibility of some potentially hazardous
compounds leaching must be considered. In this sense, the species’
leachability will ultimately dictate the real SW environmental impact. In
addition, the leaching limits are different in some normative. As an
example, the European leaching limits are more rigorous than those
from the EPA-USA (Environmental Protection Agency of United States of
America), with more elements being monitored.
Concerning the possible applications for SW recycling covered in
Section 7, its usage as starting materials in cement-based materials and
ceramic formulations - as they are materials that traditionally encap­
sulate possible contaminants in their structure - seems the most prom­
ising destination up to now.
In addition to the low particle size, it can be noticed a reasonable
compositional and mineralogical regularity for different samples of
marble-derived waste, but higher variability appears for other stones,
such as granite-based waste. Even so, good predictability of the final
composition can be expected, as the typology of the processed stones is
well characterised. Also, the creation of recycling centres is another
alternative to overcome this issue, ensuring the sustainability of the
process.
For beyond recycling possibilities reported in the literature for SW
recycling, this work also brought new insights about possible applica­
tions and ways of dealing with SW aiming to inspire companies and local
governments to put into practice such solutions, as well as future re­
searchers to try the new proposed applications described at this work or
find other management ways and feasible recycling applications.
8. Challenges for SW recycling and economical and
environmental aspects
As with any mineral extraction activity, there will always be mate­
rials with little or no commercial interest and waste from processing.
The best solution will always be the recovery and reuse of this waste
material. To reduce waste generation through the circular economy in
the dimension stone industry, some criteria can be adopted, including
the carrying of better geological and geotechnical studies in the region;
the adoption of improved quarrying technologies; and improve infra­
structure, water, and power lines (Careddu, 2019).
The works cited in this study reveal that there are countless possi­
bilities for recycling SW waste, but those applications must be developed
considering the chemical and mineralogical compositions of each waste
and the local needs of the regions where the waste is generated.
Applications based on sintered ceramics and cementitious materials
appear to be the most promising recycling possibilities. In addition to
the properties achieved, these applications emphasise the inertisation of
possible contaminants that may be present in the waste, as discussed in
Section 4. These applications are feasible almost everywhere and are a
market opportunity because they are commonly consumed materials.
Environmental applications, despite the alkaline character of SW and
the consequent positive results for the remediation of effluents and
acidic soils, have become more challenging. This challenge is mainly
explained by the possible contaminants, which, unlike the application in
ceramic materials, can be leached and contaminate the environment
where the waste is applied.
Another important factor is to perform greater management of these
materials seeking a specific application, quantifying the local genera­
tion, characterising the compositional and mineralogical variability, the
costs of transportation, and the adequacy of this alternative raw mate­
rial. Few studies encompass all variables, and few studies have examined
different batches or compositional seasonality. Therefore, the applica­
tion of the material becomes more challenging.
The creation of recycling centres can also be an interesting alterna­
tive for recycling these materials. Indeed, this approach was put into
practice in Orosei Marble district in Sardinia, Italy (Careddu et al.,
CRediT authorship contribution statement
Lisandro Simão: Conceptualization, Methodology, Investigation,
Writing – original draft. Marcelo Tramontin Souza: Conceptualization,
Methodology, Writing – original draft. Manuel J. Ribeiro: Conceptu­
alization, Resources, Writing – review & editing, Supervision, Project
administration, Funding acquisition. Oscar Rubem Klegues Montedo:
Conceptualization, Resources, Writing – review & editing, Supervision,
Funding acquisition. Dachamir Hotza: Resources, Writing – review &
editing, Project administration, Funding acquisition. Rui M. Novais:
Resources, Writing – review & editing. Fabiano Raupp-Pereira:
Conceptualization, Resources, Writing – review & editing, Supervision,
Funding acquisition.
16
L. Simão et al.
Journal of Cleaner Production 319 (2021) 128678
Declaration of competing interest
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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.
Acknowledgments
The authors are grateful for the financial support provided by the
following Brazilian institutions: National Council for Scientific and
Technological Development (CNPq, process n. 310328/2020–9) and
Coordination for the Improvement of Higher Education Personnel
(CAPES). L. Simão thanks the Human Resources Program of the National
Agency for Petroleum, Natural Gas and Biofuels (PRH-ANP) and the
Agency for Financing Studies and Projects (FINEP) for supporting this
work. R. Novais acknowledges the support of FCT (CEECIND/00335/
2017 and 2020.01135.CEECIND).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jclepro.2021.128678.
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