Journal of Environmental Management 92 (2011) 994e1002

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Journal of Environmental Management

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

Technological behaviour and recycling potential of spent foundry sands

in clay bricks
R. Alonso-Santurde a, A. Andrés a, J.R. Viguri a, M. Raimondo b, G. Guarini b, C. Zanelli b, M. Dondi b, *
a
Department of Chemical Engineering and Inorganic Chemistry, University of Cantabria, Avda. Los Castros s/n, 39005 Santander, Spain
b
CNR-ISTEC, Via Granarolo 64, 48018 Faenza, Italy

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

Article history: The feasibility of recycling spent foundry sand in clay bricks was assessed in laboratory, pilot line and
Received 3 May 2010 industrial trials, using naturally occurring sand as a reference. Raw materials were analyzed by X-ray
Received in revised form fluorescence, X-ray diffraction, particle size distribution, and leaching and combined to produce bodies
14 October 2010
containing up to 35% wt. sand. The extrusion, drying and firing behaviour (plasticity, drying sensitivity,
Accepted 1 November 2010
Available online 3 December 2010
mechanical strength, bulk density, water absorption, and shrinkage) were determined. The micro-
structure, phase composition, durability and leaching (EN 12457, granular materials, end-life step,
European Waste Landfill Directive; NEN 7345, monolithic materials, use-life step, Dutch Building
Keywords:
Clay brick
Material Decree) were evaluated for bricks manufactured at optimal firing temperature. These results
Foundry sand demonstrate that spent foundry sand can be recycled in clay bricks. There are no relevant technological
Leaching drawbacks, but the feasibility strongly depends on the properties of the raw materials. Spent foundry
Waste recycling sand may be introduced into bricks up to 30% wt. Most of the hazardous elements from the spent
foundry sand are inertized during firing and the concentrations of hazardous components in the
leachates are below the standard threshold for inert waste category landfill excepting for chromium and
lead; however, their environmental risk during their use-life step can be considered negligible.
Ó 2010 Elsevier Ltd. All rights reserved.

1. Introduction
Foundries produce metal castings by pouring metal into pre-
formed moulds made of bentonite-bonded sand. The moulds can be
reused many times, but when they wear out, they are removed from
the production process and disposed in landfills. In the foundry
industry, millions of tons of spent materials are wasted worldwide,
and over 70% of the spent materials consist of sands (Ji et al., 2001).
Consequently, waste sand moulds are considered the foremost
problem in foundries (European Commission, 2005; Magnani
Andrade et al., 2005).
Moulds are mainly composed of quartz, bentonite, carbonaceous
additives and water; however, they sometimes contain significant
quantities of heavy metals, such as chromium, lead, copper, nickel
and zinc, and organics like phenols (EPA, 1981; Dungan et al., 2006).
To reduce or eliminate the risks associated with these hazardous
substances, spent moulds are commonly solidified and stabilized
* Corresponding author. Tel.: þ39 0546699728.
E-mail addresses: alonsor@unican.es (R. Alonso-Santurde), andresa@unican.es
(A. Andrés), vigurij@unican.es (J.R. Viguri), mariarosa.raimondo@istec.cnr.it (M.
Raimondo), guia.guarini@istec.cnr.it (G. Guarini), chiara.zanelli@istec.cnr.it (C.
Zanelli), michele.dondi@istec.cnr.it (M. Dondi).
with calcium hydroxide (Coz, 2001; Coz et al., 2004) and then
deposited in landfills. Growing ecological concerns and rising
disposal costs have made these current practices unsustainable.
Therefore, there is newfound interest in incorporating these wastes
into alternative production cycles in modern industry.
Spent sands can be recycled within foundry manufacturing
(Zanetti and Fiore, 2002) or in several other industrial sectors
(Siddique and Noumowe, 2008). For instance, spent sands can be
used in the flowable fill (Tikalsky et al., 2000; Guney et al., 2006;
Deng and Tikalsky, 2008), concrete (Kraus et al., 2009; Siddique
et al., 2009), highway embankment construction (Partridge et al.,
1998; Azizian et al., 2003), and soil reinforcement (Lindsay and
Logan, 2005) sectors.
Numerous types of wastes have been evaluated as alternative
raw materials for brick manufacturing, including paper-making
pulp (Maschio et al., 2009; Sutcu and Akkurt, 2009), steel slag
(Cunico et al., 2003; Shih et al., 2004; El-Mahllawy, 2008), fly ash
(Lin et al., 2006; Sarkar et al., 2007; Cultrone and Sebastián, 2009),
water treatment sludge (Monteiro et al., 2008; Chiang et al., 2009),
thin film transistor liquid crystal display optical glass (Lin, 2007;
Dondi et al., 2009), processed tea (Demir, 2006), sawdust (Demir,
2008), and granite sludge (Acchar et al., 2006; Torres et al., 2009).
The results of these studies indicated that the incorporation of

0301-4797/$ e see front matter Ó 2010 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jenvman.2010.11.004
 R. Alonso-Santurde et al. / Journal of Environmental Management 92 (2011) 994e1002 995

Table 1 2002; Hamer and Karius, 2002; Baruzzo et al., 2006; Laursen et al.,
Raw material formulation and hygroscopicity of the brick bodies (% wt.). 2006; Samara et al., 2009). These studies indicated that the incor-
Sample Clay Reference Foundry Paper Hygroscopicity poration of spent sands into clay bricks reduced the problems
sand sand pulp related to landfill disposal and minimized the costs of both brick
B1 92 e e 8 1.11 manufacturing and waste sand treatment. Furthermore, the high
B2A 82 10 e 8 0.85 temperature process required to produce the bricks is hypothesized
B2B 72 20 e 8 0.89
to stabilize pollutants and decrease leaching.
B2C 67 25 e 8 0.91
B2D 62 30 e 8 0.85 The purpose of our research was to evaluate the use of waste
B2E 57 35 e 8 0.8 foundry sands in ceramic bricks. We performed a technological and
M1A 82 e 10 8 1.05 environmental evaluation of clay bodies containing waste foundry
M1B 72 e 20 8 0.96 sands using clay/quarry sand bodies as a reference material. The
M1C 67 e 25 8 0.89
M1D 62 e 30 8 0.81
rationale implies: (1) a laboratory simulation of the industrial
M1E 57 e 35 8 0.76 brickmaking process, to assess technological feasibility and best
firing schedule; (2) firing in industrial furnace to assess the best
waste amount; (3) industrial trial to validate prior results.

wastes into the ceramic process is feasible at percentages ranging 2. Materials and methods
between 2 and 50%. These studies demonstrated that the use of
waste materials can save energy and enhance brick quality. A few Spent foundry sand was supplied from an automotive factory
studies have analyzed clay/waste bricks from an environmental located in the Basque Country (Spain), and brick clay was supplied
point of view using leaching tests (Dondi et al., 2002; Basegio et al., by brick works located in La Rioja (Spain). The raw materials were
physically, chemically and thermally characterized. The particle
size distribution was measured by sieving. The chemical composi-
Table 2 tions were measured using X-ray fluorescence (XRF) spectrometry
Chemical and mineralogical composition and particle size distribution of raw using an ARL Advant XP XRF analyser with UNIQUANT 5.0 software.
materials.
The mineralogical compositions of the raw materials were
Sample label Clay Foundry sand Reference sand Paper pulp measured using X-ray diffraction (XRD) analysis with a Bruker D8
Particle size distribution (%) Advance XRD instrument (CuKa radiation). The thermal behaviour
0e0.063 mm 2.2 1.1 3.2 0.3 was characterized using differential thermal analysis (DTA) and
0.063e0.1 6.3 1.7 3.6 1.2 thermogravimetric analysis (TGA) with a Setaram Setsys Evolution
0.1e0.2 14.1 3.5 4 1.5
0.2e0.4 31.1 35.6 4.8 1.8
Thermogravimetric analyser.
0.4e0.75 60 83.7 42.9 4.1 Additionally, the raw materials were environmentally charac-
0.75e0.8 84.9 84.3 62.1 6.6 terized using standard leaching tests (UNE-EN 12457-1, 2003;
0.8e2 94.9 98.4 99.1 10.1 UNE-EN 12457-2, 2003). The amounts of elements released from
>2 100 100 100 100
the specimens during contact with aqueous solutions with liquid-
solid (L/S) ratios of 2 and 10 were determined according to the
Chemical composition
Major oxides (% wt.) European Directive 2003/33/CE (OJEC, 2003). Chromium, zinc,
SiO2 49.89 83.88 90.38 10.73 cadmium, nickel, barium, molybdenum, copper, lead, arsenic,
TiO2 0.66 0.1 0.37 0.21 antimonium, selenium and mercury were measured with an
Al2O3 14.81 7.31 4.25 6.71 inductively coupled plasma-mass spectrometry (Agilent 7500ce).
Fe2O3 5.02 1.6 0.55 0.44
MgO 1.92 0.46 0.07 1.6
The measured concentrations were compared to the acceptable
CaO 9.31 0.71 0.11 25.87 regulatory limits in the European Directive 2003/33/CE (OJEC,
Na2O 0.7 0.78 0.17 0.16 2003) for inert waste in landfills.
K2O 3.03 3.82 2.85 0.16 In the laboratory simulation of the ceramic manufacturing
SO3 0.94 0.28 e 0.25
process, the body included spent foundry sand, in proportions
L.O.I 13.34 2.67 0.42 52.37
varying from 10 to 35%, clay and paper pulp. Reference bodies were
Trace elements (mg/kg) prepared to compare the behaviour of the waste sand with that of
Cr 86 3070 207 65 the sand conventionally used in brickmaking (Table 1). The
Ba 451 529 280 148 mixtures were homogenized and extruded (Verdes Mod. 050-C) to
Zn 101 105 18 134
obtain bars of 10  7  2 cm. The bars were dried at an ambient
Ni 38 110 108 30
Cu 35 20 4 237 temperature in a non-controlled atmosphere for seven days and
Pb 23 80 21 64 then in an electric oven at 100  C for 24 h. The dried specimens
As 18 2 18 2 were then fired in an electric chamber kiln (Nabertherm) at three
Sb 2 1 2 1 maximum temperatures (800, 850 and 900  C, thermal rate of
1.6  C/min, 4 h soaking).
Phases composition (%wt)
Quartz 16 64 78 e
Each stage of the brick manufacturing process was evaluated.
Calcite 15 e e 46 The extrusion stage was evaluated using Atterberg limits (CNR-UNI
K-Feldspar 3 18 16 e 10014), in which the plastic limit represents the minimum water
Plagioclase 5 7 Traces content at which the sample can be rolled by hand (Bain, 1970), and
Hematite 4 e e e
the plasticity index represents the range in which the material is in
Illite-Mica 34 6 Traces e
Kaolinite 8 e e 16 the plastic state. The drying stage was evaluated by measuring
Montmorillonite 5 Traces e e Bigot’s curves with an Adamel barellatograph (Dondi et al., 1998).
Vermiculite 5 e e e The storage stage was evaluated through hygroscopicity measure-
Accessories 4 3 5 3 ments (Keeling, 1958). The firing stage was evaluated by measuring
Organic matter Traces 2 e 35
the firing shrinkage, flexural strength (ASTM C674, 1994), water
996 R. Alonso-Santurde et al. / Journal of Environmental Management 92 (2011) 994e1002

Fig. 1. Thermal behaviour of the raw materials (TGA bold line, DTA thin line).

absorption, open porosity and bulk density (ASTM C373, 1994) of the
fired bodies. The real density was determined using a helium
picnometer (Micromeritics FlowSorb II 2300); total porosity was
calculated as 1-(bulk density/real density); closed porosity is the
difference total porosity e open porosity. Microstructure was
observed using scanning electron microscopy (SEM, Leica, Cam-
bridge Stereoscan 438 VP).
Industrial firing was carried out in a brickwork kiln at a
maximum temperature of 850  C to introduce the optimum
percentage of spent sand into the ceramic matrix. To measure the
extent to which this was accomplished, the firing shrinkage, flexural
strength, bulk density, water absorption, loss on ignition, real
density and both open and closed porosity of the fired bodies were
measured. Moreover, the soluble salts (UNE-EN-772-5, 2001) and
efflorescence (ASTM C67, 1994) tests were carried out.
Quantitative phase analysis (QPA) of the fired bodies was per-
formed by X-ray diffraction (Bruker D8 ADVANCE diffractometer,
filtered Cu Ka radiation, 5e80 2q range, scan step 0.02 2q, 1 s per
step using a LynxEye detector) following a combined RIR (Reference
Intensity Ratio) and Rietveld refinement (GSAS-EXPGUI softwares)
technique, by adding 10% wt. corundum as reference material in
order to quantify the amorphous phase (Gualtieri, 2000).
Durability was indirectly estimated using mercury intrusion
porosimetry and by calculating Maage’s durability factor (Maage,
1984). The specimens were then submitted to the leaching tests
proposed in the 2003/33/CE Directive to see if they complied with
the regulatory waste limits.
Once the optimum percentage of sand was selected, an industrial
trial was undertaken with large clay blocks (67  52  7 cm). The
large clay blocks contained 30% spent sand and were manufactured
in the brickwork (fired at 850  C). The finished products were
evaluated and the bulk density, flexural strength, water absorption
and specific surface were measured. Leaching tests were performed
on both the granular materials according to UNE-EN 12457-1, 2003;
UNE-EN 12457-2, 2003 and the ceramic blocks according to NEN
7345, 1995. The concentrations of elements released in the Fig. 2. Environmental behaviour of the raw materials assessed using leaching tests
compliance leaching test UNE 12457 were compared to the limits in described in UNE-EN 12457-1, 2003; UNE-EN 12457-2, 2003. (a,b) clay, (c,d) foundry
the European Directive 2003/33/CE (OJEC, 2003), while immission sand, (e,f) reference sand. Left column: L/S ¼ 2, right column: L/S ¼ 10.
 R. Alonso-Santurde et al. / Journal of Environmental Management 92 (2011) 994e1002
Fig. 3. Plasticity of brick bodies.
values (e64) obtained from the amounts of elements released from
the monoliths were compared with the limits in the Dutch Building
Materials Decree (VROM, 1999).
3. Results and discussion
3.1. Characterisation of raw materials
The physical and chemical characterisation of the raw materials is
presented in Table 2. Clay is mainly composed of quartz, calcite,
hematite and a mixture of clay minerals including kaolinite, smectite
and illite plus vermiculite in smaller amounts. The clay chemical
composition is approximately 50% silica,15% alumina and 9% calcium
oxide, with smaller amounts of iron and potassium oxides. There is
a relatively high quantity of fluxing agents, such as K2O, in the
foundry sands, which contain bentonite as their most important
binding agent, and in the reference sands, which are composed of
quartz and feldspars. There is a rather high quantity of chromium in
the foundry sand, which came from the casting process. In terms of
particle size, the clean sand has a coarser distribution than the
foundry sand.
Foundry sand and paper pulp undergo exothermic reactions
(Fig. 1) due to the combustion of organic components (European
Fig. 4. Drying behaviour of bodies containing reference sand (left) or foundry sand (right).
997
Commission, 2005) and cellulose (Sutcu and Akkurt, 2009),
respectively. This observation is confirmed by the loss on ignition
(LOI) values, which are 2.7% for the foundry sand and 52% for the
paper pulp.
As shown in Fig. 2, the Cd, Mo, Pb, Se, As, Sb and Hg leachate
concentrations are all within the regulatory limits for inert waste in
landfills. The Cr concentration is above the acceptable limit
(0.057 mg/l) in both foundry and reference sand leachates. Mean-
while, the Cu concentration is below the acceptable limit (0.049 mg/l)
in reference sand leachates. Due to the agglomerated state of the
paper pulp sample, only the leaching test with an L/S ratio of ten
could be performed. The following concentrations were measured:
0.14 mg/l Zn, 0.10 mg/l Ni, 0.04 mg/l Ba, 0.03 mg/l Cu, 0.52 mg/l F,
40.07 mg/l Cl and 24.11 mg/l SO24 . It is notable that the higher the L/
S ratio, the lower the amounts of Ni, Cu, fluoride, chloride and
sulphate concentrations. Despite the high quantity of Cr in foundry
sand (3070 mg/kg), it is not detectable in the leaching tests. This is
may be because Cr is present as Crþ3 and precipitates as Cr2O3 due to
the mild-alkaline pH (8.2 and 8.5) of the test (Beverskog and
Puigdomenech, 1997).
3.2. Laboratory simulation
Figs. 3 and 4 display the Atterberg’s limits and Bigot’s curves,
which characterize the ceramic mixtures. The addition of sand
reduces the plasticity of both foundry-sand-bearing and reference-
sand-based bodies, which makes a decrease of molding water
possible (Fig. 3). The drying sensitivity, shown in Bigot’s curves, is
reduced in presence of sand (Fig. 4). The reduced drying sensitivity
is due not only to drying shrinkage, but also to the improved drying
ratio (water loss without shrinkage/water loss with shrinkage).
As shown in Table 1, hygroscopicity, i.e. the equilibrium mois-
ture adsorbed from the air by the body after drying, is rather low in
all the samples. As expected, the M1 series (incorporating molding
sand) values (Table 1) are inversely related with the amount of
sand; however, the B2 (incorporating reference sand) series values
are quite stable at approximately 0.85%.
The influence of firing temperature on the technological prop-
erties of the bodies was evaluated at the three firing temperatures
(Fig. S1). The introduction of sand produced a small decrease
in both firing shrinkage (from 2.5 to 3.5%) and water absorption (in
the 15e18% range). These results may be related to the decrease
998 R. Alonso-Santurde et al. / Journal of Environmental Management 92 (2011) 994e1002

Fig. 5. Real density, closed porosity and total porosity of the sand/clay bodies fired at 850  C.

in density and increase in flexural strength, which is confirmed by
the decrease in total porosity (Fig. 5), even if unexpected trends are
found in the mechanical strength values. The differences in density
and porosity properties observed in bodies fired at different
temperatures may be due to microstructural transformations at
some stage in firing, during which new high-density phases with
small pores may form. The decrease in flexural strength may be
a consequence of the b-quartz to a-quartz transition, which may
create defects on the specimen that result in a lower mechanical
resistance. Since these observations indicate that firing tempera-
ture has little influence on the parameters analyzed, we selected
the intermediate temperature of 850  C, which is the closest to that
of the industrial furnace, for further testing.
3.3. Industrial firing
Firing tests were performed in an industrial kiln to determine
the optimal percentage of waste sand (Fig. S2). In discussing these
results, it is necessary to account for the differences existing in the
unfired bricks. The dry density increases with the addition of sand,
implying that there is better body packing. This fact, together with
the decreasing LOI, generates a lower porosity and a higher bulk
density in the sand-bearing bricks. Consequently, water absorption
decreases even if the firing shrinkage tends to diminish. Mechanical
strength presents an unexpected decreasing trend with growing
sand incorporation. The sand-bearing specimens are denser with
a lower mechanical resistance.
The phase composition of the bricks is consistent with that of
the raw materials (Table 3). Both series containing foundry and
reference sands contain residual phases that are already present in
the clay and sands, such as quartz, feldspars, hematite and mica-
illite. They also contain new phases that formed during firing,
including Ca-rich plagioclase, which comes from calcite decom-
position and reaction with the silicate matrix. Quartz in the M
samples appear to be more reactive during firing, as expected by
the particle size distribution.
The durability of bricks may be reduced due to deterioration
processes, such as freeze/thaw cycles or crystallization pressure
due to precipitation of soluble salts (Benavente et al., 2007). The
incidence of these deterioration processes mainly depends on the
porosity of the system. Frost resistance can be predicted based on
pore size distribution and pore volume according to the approach

Table 3
Phase composition of bricks fired at 850  C.

Quartz K- Feldspar Plagioclase Hematite Illite-Mica Amorphous

Phase
B1 26.7  0.2 6.2  0.1 9.0  0.3 2.9  0.1 25.3  0.1 29.9  0.8
B2A 29.0  0.3 9.6  0.2 4.7  0.1 2.2  0.1 26.1  0.3 28.5  1.0
B2B 39.1  0.3 5.7  0.2 4.2  0.1 1.6  0.1 17.4  0.2 32.1  0.9
B2C 41.3  0.4 6.0  0.1 6.3  0.1 1.7  0.1 17.5  0.2 27.3  0.9
B2D 44.5  03 6.4  0.1 4.0  0.2 2.3  0.1 19.5  0.2 23.0  0.9
B2E 44.0  0.2 6.2  0.1 3.5  0.1 2.4  0.1 19.3  0.2 24.6  0.7
M1A 29.3  0.2 4.7  0.1 4.4  0.1 2.3  0.1 17.7  0.1 41.7  0.6
M1B 30.2  0.3 9.1  0.1 5.5  0.1 3.3  0.1 24.9  0.2 27.0  0.8
M1C 35.6  0.3 7.4  0.2 10.1  0.2 1.2  0.1 21.0  0.2 24.6  1.0
M1D 29.8  0.3 6.2  0.2 4.2  0.1 1.1  0.1 14.4  0.1 44.3  0.8
M1E 33.6  0.1 8.0  0.2 13.2  0.1 3.5  0.1 19.2  0.3 22.5  0.8
 R. Alonso-Santurde et al. / Journal of Environmental Management 92 (2011) 994e1002 999

published by Maage (1984) (Fig. 6). The M1 samples have a higher

Fig. 6. Durability predicted by Maage’s parameters: M1 (full triangles), B2 (squares).
percentage of pores smaller than 3 mm in diameter (P3); however,
the B2 samples have a lower porosity. Accounting for the stronger
influence of P3 on frost resistance, the M1 samples are likely to be
more resistant than the B2 samples.
We considered firing shrinkage, water absorption and mechan-
ical strength to be the most relevant properties when selecting the
optimal amount of sand to be added to the matrix. The M1D batch
was the optimal choice in terms of the above criteria. Consequently,
the M1D sample microstructure was compared to the B1 and B2D
sample microstructures using SEM (Fig. 7). Quartz grains are visible
in the matrices of the B1 and B2D samples. However, the M1D
sample analysis was inconclusive because the rough surface did not
permit appropriate graphitization before SEM analysis.

Fig. 7. SEM microstructure of the bodies. B1: compact structure, B2D: quartz grains with irregular shapes and sharp edges, M1D: rounded grains of quartz, apparently gently
bonded, limited sintering of coarse grains with the brick matrix may be the cause of the deteriorated mechanical performance.
1000 R. Alonso-Santurde et al. / Journal of Environmental Management 92 (2011) 994e1002

Table 4
Compliance leaching tests results on the granular industrial bodies. Threshold limits
were collected from the Council Decision of 19 December 2002 establishing criteria
and procedures for the acceptance of waste at landfills (OJEC, 2003). pH L/S ¼ 2:
10.86; pH L/S ¼ 10: 10.88.

Concentration (mg/l) Threshold (mg/l)

L/S L/S

2 10 2 10
As < 0.00005 0.004  0.001 0.05 0.05
Ba 0.140  0.006 0.100  0.002 3.5 2
Cd < 0.000005 <0.00005 0.015 0.004
Cr 0.780  0.015 0.293  0.010 0.1 0.05
Cu <0.00005 <0.00005 0.45 0.2
Hg <0.000001 <0.000001 0.001 0.001
Fig. 8. Industrial body. Mo <0.00005 <0.00005 0.15 0.05
Ni <0.00001 <0.00001 0.1 0.04
3.4. Industrial trial Pb 0.270  0.051 0.340  0.050 0.1 0.05
Sb < 0.00001 <0.00001 0.01 0.006
Se <0.00001 <0.00001 0.03 0.01
Industrial hollow blocks (67  52  7 cm) composed of 30%
Zn 0.050  0.005 0.050  0.008 1 0.4
foundry sand were manufactured, fired at 850  C (Fig. 8) and F 2.030  0.060 1.420  0.100 2 1
characterized. The industrial bricks have a bulk density of Cl 20.25  1.20 4.700  0.150 225 80
2.67  0.04 g/cm3, a water absorption value of 12.7  0.2%, a flex- SO¼4 1800  0.005 970  26.8 280 100
ural strength of 83.7  0.3 kg/cm2 and a specific surface of
5.44  0.05 m2/g. The specimens fulfil the requirements prescribed
by the Spanish Association for Normalization and Standardization and sulphates were measured and compared to the regulatory
(AENOR), according to the European Standard EN-771-1 (UNE-EN limits (2003/33/CE) to determine if the sand/clay bricks met the
12457-1, 2003). acceptable requirements for disposal in inert waste landfills. Fig. S4
presents the concentrations of the chemical species measured.
3.5. Environmental aspects Barium, fluoride and chloride demonstrate a trend in which the
higher the L/S ratio, the lower the amount of component leached;
3.5.1. Soluble salts and efflorescence however, this trend is not observed for chromium and sulphate.
Fig. S3 presents the results of the soluble salts tests (UNE-EN- Thus, the leaching behaviours of barium, fluoride and chloride are
772-5, 2001) on the sand/clay bodies. The amounts of sodium, not significantly affected by the amount of sand incorporation in
potassium, fluoride and chloride leaching remain relatively the matrix. However, the leaching test results for chromium and
constant upon the sand addition, while sulphate leaching decreases, sulphate indicate a decreasing trend in sand incorporation. These
especially in monoliths containing foundry sand. In comparison to results indicate that only the chromium and sulphate levels met the
the standards (UNE-EN-771-1, 2003), the waste-based ceramics proposed limits for ceramics that incorporate foundry sand.
should be placed in the best category (S2, i.e. Naþ þ Kþ content < Therefore, foundry sand/clay ceramics fail to meet the proposed
0.06%, Mg2þ< 0.03%). In all of the samples, there is a ‘medium’ to disposal standards, and they cannot be accepted in inert waste
‘strong’ degree of efflorescence, indicating that the foundry sand has landfills. The industrial specimens have been analyzed by means of
no detrimental effect compared to the reference sand. the compliance leaching test UNE 12457 and the diffusion test NEN
The efflorescence composition can be predicted based on the 7345. Table 4 displays the results of the leaching tests developed in
levels of soluble salts (Dondi et al., 1997). In the B2 samples, the the granular materials. The Cr, Pb, fluoride and sulphate concen-
efflorescence composition is primarily calcium sulphate; however, trations are above the inert waste landfill limits, and the specimens
in the M1 series, the composition included calcium carbonate and must to be transported to a non-dangerous category site. However,
sulphate (Fig. 9). the leaching tests carried out on the monolithic materials (Table 5)
shows that foundry sand/clay ceramic bricks are environmentally
3.5.2. Leaching safe during their life-stage and can be used as building material
The sand/clay bricks fired at 850  C were environmentally without environmental impact.
evaluated using leaching tests with L/S ratios of 2 and 10 according
to UNE 12457. As with the raw material analyses, the concentra-
tions of As, Ba, Cd, Cr, Cu, Hg, Mo, Ni, Pb, Sb, Se, Zn, fluoride, chloride Table 5
Diffusion test results on the monolithic industrial bodies. Threshold limits were
collected from the Dutch Building Materials Decree (VROM, 1999).

Immission value e64100 years (mg/m2) Threshold (mg/m2)

As N.d. 435
Ba N.d. 6300
Cd N.d. 12
Cr 31.1  0.5 1500
Cu N.d. 525
Mo N.d. 150
Ni N.d. 525
Pb N.d. 1275
Zn N.d. 2100
F 2.15  0.02 140
Cl 21.5  0.1 30000*
SO¼4 798.1  5.0 45000*
Fig. 9. Relationship between soluble salts and phase composition of efflorescence.
*
(Dondi et al., 1997). Values per year. N.d.: not detected.
 R. Alonso-Santurde et al. / Journal of Environmental Management 92 (2011) 994e1002
4. Conclusions
Spent foundry sand can be successfully recycled in brickmaking
as a substitute for plasticity-reducing raw materials, such as
naturally occurring sands. We assessed the feasibility of this
proposal in laboratory experiments, pilot line and scaled industrial
trials, which resulted in a product quality that matched the stan-
dard requirements.
The technological behaviour of clay bodies containing foundry
waste is fully comparable to that of reference sand-bearing bodies.
Changes in technological parameters were expected because of the
sand addition, including the reductions in plasticity, hygroscopicity,
drying sensitivity, and mechanical strength, as well as drying and
firing shrinkage. No rheological or drying problems were observed
due to the presence of bentonite in the foundry moulds, indicating
that bentonite is fully inert in the spent sand.
Spent foundry sand can be introduced in clay bodies in variable
amounts, depending on the clay rheological behaviour. The higher
the plasticity of the spent foundry sand, the larger the recyclable
amount. In this case study, the recyclable amount was 30% wt.
Extending these conclusions to other foundry sand sources and/or
industrial plants should be cautioned. The percentage of recyclable
sand is strongly influenced by the characteristics of the raw mate-
rials (both clay and sand) and the brickmaking process (e.g. shaping
technique, drying and firing schedule). Performing the appropriate
technological and environmental testing is highly recommended
prior to re-using unknown foundry sands in ceramic bodies.
In our study, most hazardous elements are rendered inert
during firing, or their concentrations in the leachates are below the
proposed disposal limits. The only heavy elements exceeding these
limits are chromium and lead, which are in relatively low concen-
trations compared to the raw materials content. In spite of the
environmental risk at the end-life step as consequence of the
chromium and lead leaching, the environmental impact derived of
their use can be considered negligible. However, the landfilling of
the foundry sand/clay bricks in an inert waste category landfill
requires a prior treatment of the foundry sands.
Acknowledgements
This work was conducted within the framework of the Spanish
Ministry of Education and Science Projects (CTM2009-11303).
R. Alonso-Santurde was funded by the Spanish Ministry of Educa-
tion and Science on an F.P.I. fellowship.
Appendix. Supplementary data
Supplementary data related to this article can be found online at
doi:10.1016/j.jenvman.2010.11.004.
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