Science of the Total Environment 378 (2007) 42 – 48

www.elsevier.com/locate/scitotenv

Heavy metal contents in horticultural crops of a representative area

of the European Mediterranean region
Mónica Peris ⁎, Carolina Micó, Luis Recatalá, Raúl Sánchez, Juan Sánchez
Centro de Investigaciones sobre Desertificación (Universitat de València, CSIC, Generalitat Valenciana),
Camí de la marjal s/n. 46470-Albal, València, España

Available online 15 February 2007

Abstract

Heavy metal content (Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb and Zn) was analysed in the edible parts of two types of horticultural
crops (leaf and inflorescence crops) from 30 agricultural fields in Castellón (Spain), a representative area of the European
Mediterranean region. Selected soil properties relevant to control the mobility and bioavaibility of heavy metals were analysed for
the general characterisation of these agricultural soils. The levels of clay, high percentages of organic matter and the presence of
carbonate seem to suggest an important retention of heavy metals by these components in most of these soils. However, the high
salinity in some fields (N 4 dS/m) seems to facilitate the mobility of some heavy metals (e.g. Cu).
The mean values of total contents of heavy metals in soils were similar to values obtained in other works on Spanish agricultural
soils. However, there were some fields with a metal content (particularly Cu, Pb or Zn) higher than these works, reflecting an
important anthropogenic source. In seven fields, the crop contents of Cd and/or Pb were higher than the maximum levels
established by the Commission Regulation no. 466/2001 for horticultural crops. Heavy metal contents in leaf crops were higher
than in inflorescence crops, except for Zn. The differences for Cd, Cr, Cu, Fe and Mn contents between these two types of crops
were statistically significant. The analysis of crop heavy metal contents showed a higher absorption and/or accumulation of heavy
metals in leaf crops than in inflorescence crops. Differences in crop characteristics seem to be responsible for the differential
accumulation of heavy metals. Furthermore, agronomic practices and other sources of heavy metals (e.g. atmospheric deposition
for Cd and Pb) may also have some influence on crop accumulation. Given the relevance of horticultural crops in the
Mediterranean diet, it is highly necessary to extend the experience of this work to other areas of the European Mediterranean
region.
© 2007 Elsevier B.V. All rights reserved.

Keywords: Heavy metals; Agricultural soils; Leaf crops; Inflorescence crops; Castellón; Mediterranean region

1. Introduction 1990). Atmospheric deposition, urban–industrial activ-

Heavy metal contents of agricultural soils can affect
human beings directly, through soil ingestion or through
the food web by ingestion of crops and/or animals, or
indirectly, damaging environmental health (Nriagu,
⁎ Corresponding author. Tel.: +34 961220540; fax: +34 961270967.
E-mail address: monica.peris@uv.es (M. Peris).
0048-9697/$ - see front matter © 2007 Elsevier B.V. All rights reserved.
doi:10.1016/j.scitotenv.2007.01.030
ities and agricultural practices (e.g. use of agrochemical
products and addition of organic amendments) are the
main anthropic sources of heavy metals in agricultural
soils (Nriagu, 1990; Alloway and Jackson, 1991). These
practices are occurring in the Castellón province (East
Spain), a representative area of the European Mediter-
ranean region. Castellón is characterised by a highly
technified agriculture that consumes huge amounts of
 M. Peris et al. / Science of the Total Environment 378 (2007) 42–48
agrochemicals, typical in this region. Moreover, over
recent decades its land-use pattern has seen an ex-
pansion of industrial–urban uses, which is consistent
with most of the European Mediterranean region
(Coccossis, 1991; Groom et al., 1995). As a conse-
quence, an increase in heavy metal contents in agri-
cultural soils and crops may be occurring and also
possible damage to human health through crop intake.
Several studies have focussed on heavy metal contents
in horticultural soils of the Mediterranean region (e.g.
Andreu and Gimeno, 1996; Pinamonti et al., 1997).
However, only a few studies have determined the heavy
metal contents in horticultural crops (e.g. Canet et al.,
1998) despite the impact these types of crops can have
on human health, particularly in this region giving their
relevance in the diet (Cuadrado et al., 1995). Taking
into account this issue, a systematic regional study of
heavy metals in soils under horticultural crops was
carried out within the framework of the research project
“Heavy metal contents and bioavailability in agricul-
tural soils and their influence in horticultural crops”,
funded by the Valencian Regional Government (Gen-
eralitat Valenciana).
In order to identify contaminated crops, the crop
contents were compared with the maximum limits es-
tablished for Cd and Pb in foodstuffs by the Commis-
sion Regulation no. 466/2001. Moreover, because
vegetable species and varieties differ in their ability to
uptake, accumulate and tolerate heavy metals (Turner,
1994; Angelova et al., 2004), a comparison has been
made between leaf (lettuces and Swiss chards) and
Fig. 1. Location map of study area.
43
inflorescence (artichokes) crops, the former as represen-
tative of accumulator crops and the latter as re-
presentative of non-accumulators (Ross and Kaye,
1994). An important number of studies have compared
heavy metal contents among species and/or varieties
under similar environmental conditions. These studies
show that there are differences in the crops’ ability to
absorb and/or accumulate heavy metals. Such differ-
ences can occur between different parts of the crops (e. g.
Jinadasa et al., 1997; Angelova et al., 2004). However,
the most relevant parts are the edible parts as heavy
metals can be easily transferred from them to other
ecosystem components (e.g. biota, human communi-
ties). For this reason, the comparisons made between
crops concerned their edible parts, since this reflects the
potential impact of each type of crop on human health. In
order to be realistic, the comparisons were made under
field conditions.
2. Materials and methods
The Castellón province is situated in the east of Spain,
within the European Mediterranean region. The province
covers 6632 km2 and approximately 61.9 km2 are
occupied by horticultural crops, including artichokes,
lettuces, tomatoes, cauliflowers and melons. The pro-
vince has been traditionally associated with agriculture,
although the agricultural area has been decreasing from
the last decades due to the expansion of industrial–urban
uses. This area has a Mediterranean climate, charac-
terised by an annual average temperature of 14–17 °C
44 M. Peris et al. / Science of the Total Environment 378 (2007) 42–48
Table 1
Descriptive statistics of soil properties
pHwater pHKCl EC (dS/m) Organic matter (%)
Mean 8.1 7.5 2.0 3.8
s.d. 0.2 0.1 1.8 1.3
Min. 7.6 7.1 0.7 2.0
Max. 8.4 7.9 8.8 7.2
s.d. standard deviation; Min. minimum value; Max. Maximum value.
and annual average rainfall of 400–600 mm. Coastal
areas present the hottest and driest climate of the
province, whereas inland areas present the lowest
temperature and the highest rainfall. Most of the fields
devoted to horticultural crops are irrigated using a flood
irrigation system. Only a few fields are irrigated using a
drip irrigation system or a sprinkler system.
A total of thirty fields were sampled in the Castellón
province (Fig. 1), following a simple random sampling
procedure. These fields were selected using a random
computer program and were located in the field by using
a GPS (Global Position System). Sixteen fields were
under inflorescence crops (Cynara scolymus L.) and
fourteen under leaf crops (Lactuca sativa L. and Beta
vulgaris L.). In each field, both a superficial composite
soil sample and a crop sample were taken. Composite
soil samples for each field consisted of 16 cores of soil
collected from the first 25 cm depth of topsoil. Cores
were mixed into one composite sample for each field
and analysed in triplicate. Furthermore, edible parts of
several crops (three or four) were also collected in each
field randomly. All the crops of each field were dried in
an oven (60 °C), mixed and sieved to 0.5 mm for
analysis of heavy metal contents.
Soil properties relevant to control the mobility and
bioavailability of heavy metals were analysed for the
characterisation of agricultural soils according to the
official laboratory methods of the Spanish Ministry of
Agriculture, Fisheries and Food (MAPA, 1994). Soil pH
was measured in a 1:2.5 soil:water suspension and
electrical conductivity was determined in the saturation
paste extract. Organic matter content was determined by
the Walkey–Black method, the total carbonate content
by the Bernard calcimeter and particle-size distribution
by the Robinson Pipette method. Cation exchange
capacity was determined by saturation with sodium
acetate solution (pH = 7.0), replacement of the absorbed
sodium with ammonium acetate (pH = 8.2) and deter-
mination of displaced sodium by flame (air–acetylene)
atomic absorption spectrometry (FAAS). On the other
hand, the total content of heavy metals in soils was
determined using the digestion USEPA 3051 A method
(USEPA, 1998). The extractable contents were deter-
Carbonates (%) CEC (cmolc(+)/Kg) Sand (%) Silt (%) Clay (%)
30.5 17.8 33 41 26
13.3 3.7 10 9 8
10.6 9.9 3 20 9
60.3 30.0 56 67 51
mined by extraction with EDTA (Boluda et al., 1993).
The contents in crops were determined using the USEPA
3052 method (USEPA, 1996). Heavy metals were
analysed by atomic absorption spectrometry (AAS),
using AAS-flame or AAS-graphite furnace depending
on the heavy metal contents at each extraction. These
methods were selected because they provided satisfac-
tory results in relation to recovery and precision data
(Peris, 2005).
The comparison of heavy metal contents between the
two crop types and soils, which were grouped by crop
types, was carried out using the T-test or Mann
Whitney-U depending on the population distribution.
Furthermore, correlation coefficients were obtained to
analyse relationships between heavy metal contents in
soils and in crops. These statistical analyses were
obtained using SPSS® (Statistic Program for Social
Sciences) for Windows.
3. Results and discussions
3.1. Soil properties and heavy metal contents in soils
and crops
Soil properties analysed in the study area (Table 1)
were similar to other agricultural soils characterised in
the Spanish Mediterranean region by some scientists
(e.g. Campos, 1997; Gil et al., 2004). The levels of clay,
high percentages of organic matter (N 2%) and the
presence of carbonate (11–60%) seem to suggest an
important retention of heavy metals by these compo-
nents in most of these soils. However, the high salinity
in some fields (N 4 dS/m) seems to facilitate the mobility
of some heavy metals (e.g. Cu). The crop having the
highest content of Cu (19.7 mg/kg) is located in the field
with the highest soil electrical conductivity (8.8 dS/m).
Total contents of heavy metals in soils (Table 2) were
similar to values obtained in other studies on Spanish
agricultural soils (e.g. Boluda, 1988; Andreu and
Gimeno, 1996; Pomares et al., 2000; Andrades et al.,
2000; Gil et al., 2004). However, mean contents of Cr,
Cu, Pb and Zn were higher than mean concentrations of
agricultural soils in the Castellón province obtained by
 M. Peris et al. / Science of the Total Environment 378 (2007) 42–48 45

Table 2
Concentration of heavy metals (mg/kg in dry weight) in the edible parts of two horticultural crops (Leaf crops: Swiss chard (n = 10) and lettuces
(n = 4); Inflorescence crops: artichoke (n = 16)); total and extractable contents of heavy metals (mg/kg dry weight) in soils, which are grouped by their
crop types
Crop types Crop content (mean ± s.d.) Total soil content (mean ± s.d.) Extractable soil content (mean ± s.d.) % Ext/total CF
Cd Leaf 1.47 ± 2.16a 0.358 ± 0.221a 0.100 ± 0.032a 34.14 6.17
Inflorescence 0.24 ± 0.12b 0.352 ± 0.154a 0.112 ± 0.042a 34.90 0.87
Co Leaf 0.57 ± 0.54⁎ 7.9 ± 2.0a 0.226 ± 0.136a 3.06 0.01
Inflorescence n.d.⁎ 7.3 ± 1.3a 0.223 ± 0.093a 3.12 0
Cr Leaf 3.35 ± 5.54a 32.2 ± 9.3a 0.059 ± 0.014a 0.20 0.12
Inflorescence 0.68 ± 0.72b 32.2 ± 5.2a 0.072 ± 0.018b 0.23 0.02
Cu Leaf 13.2 ± 4.1a 35.4 ± 8.1a 5.09 ± 3.23a 13.6 0.39
Inflorescence 8.7 ± 2.2b 36.0 ± 10.8a 6.50 ± 2.86a 17.7 0.26
Fe Leaf 431 ± 692a 17 487 ± 5 270a 27.6 ± 19.3a 0.17 0.03
Inflorescence 65 ± 43b 17 373 ± 3 515a 21.0 ± 10.3a 0.12 0
Mn Leaf 63 ± 37a 408 ± 119a 37.6 ± 13.8a 9.87 0.18
Inflorescence 21 ± 4b 379 ± 82a 38.5 ± 16.4a 10.11 0.06
Ni Leaf 3.84 ± 7.24a 19.9 ± 5.2a 0.485 ± 0.165a 2.49 0.25
Inflorescence 1.32 ± 0.92a 19.4 ± 3.1a 0.537 ± 0.164a 2.79 0.07
Pb Leaf 1.99 ± 1.74⁎ 56.1 ± 84.3a 11.4 ± 19.0a 18.53 0.06
Inflorescence 0.28 ± 0.17⁎ 85.5 ± 251.8b 20.0 ± 62.1a 18.73 0.01
Zn Leaf 41.7 ± 16.6a 76.8 ± 20.9a 11.1 ± 5.8a 14.81 0.55
Inflorescence 44.3 ± 12.3a 94.5 ± 53.6a 18.3 ± 9.9b 19.54 0.56
Percentage of extractable fraction relative to total concentration (% Ext/total). Concentration factor (CF). n.d. non-determined. If the letters are equal
(a, a) there are no statistical differences between the two crop types, whereas if the letters are different (a, b) there are statistical differences between
the two crop types. ⁎ No statistical tests applied.

López and Grau (2004). In this context, high values of
Cu obtained in horticultural soils may be due to an
excess use of agrochemicals, such as fungicides with Cu
often applied by farmers in the agricultural soils of the
Spanish Mediterranean region, especially in irrigated
land (e.g. Rico et al., 2003), which is the main
management system applied to horticultural soils. On
the other hand, the highest values of Pb and Zn seem to
be due to contamination processes occurring in three
fields, located near ceramic industries. In these indus-
tries, ceramic pigments and ceramic enamels were found
to contain Pb and Zn, respectively (Roig et al., 1997).
Mean contents of EDTA-extractable fraction of
heavy metals (Table 2) were also similar to values
obtained by Andreu and Gimeno (1996) in agricultural
soils in the Valencian province (located in the South of
the Castellón province), except for extractable Pb. In
fact, the Pb extractable content was higher in the
Castellón province than in the Valencia province. This
could be due to the huge total content of Pb found in one
field, which also had high contents of other heavy
metals (e.g. 44 mg/kg of Cu and 115 mg/kg of Zn).
The high percentages of extractable contents with
respect to the total concentration (%Ext/tot) of Cd, Cu,
Pb and Zn (N 10%) seem to indicate that these elements
can be more mobile than Co, Cr, Fe, Ni and Mn in the
horticultural soils analysed. These percentages can also
indicate a higher bioavailability for the former group of
elements than for the latter group.
Mean concentrations, in fresh weight, of Cd (0.21 ±
0.31 mg/kg for leaf crops; 0.04 ± 0.02 mg/kg for
inflorescence crops) and Pb (0.29 ± 0.27 mg/kg for leaf
crops; 0.05 ± 0.03 mg/kg for inflorescence crops) in
crops did not exceed maximum levels established by the
Commission Regulation no. 466/2001 (DOCE, 2001)
for these elements. Seven samples had a content of Cd
and/or Pb that exceeded maximum levels. Specifically,
three samples of inflorescence crops exceeded the
maximum levels for Cd (0.05 mg/kg), whereas three
samples of leaf crops exceeded the maximum levels for
Cd (0.2 mg/kg) and four for Pb (0.3 mg/kg). These fields
are in an area influenced by industry and/or roads.
Therefore, according to the aforementioned regulation,
several contaminated crops were identified in the study
area.
The concentration factor refers to the ratio between
the heavy metal concentration in crops (mg/kg dry
weight) and in soils. This has been used in several
studies (e.g. Hooda et al., 1997; Alam et al., 2003) to
determine the relationship between heavy metal con-
tents in crops and soil contents. In the study area, the
concentration factors of Cd and Zn were higher than the
concentration factors of the other elements (Table 2), as
several scientists have also found elsewhere (e.g. Hooda
46 M. Peris et al. / Science of the Total Environment 378 (2007) 42–48
et al., 1997; Wang et al., 2004). In fact, only the Cd and
Zn concentration factors were above 0.5, whereas the
other concentration factors were lower than 0.5. There
were major differences in the concentration factors
between fields for each element. In most of the samples,
the concentration factor values decrease as the metal
concentrations in the soils increase.
3.2. Comparisons between fields, grouped by crop types
The comparison of soil properties, having grouped
the soils by crop type (inflorescence crops and leaf
crops), reflected significant differences between organic
matter content and CEC. Both properties showed higher
values in soils devoted to leaf crops (4.4% of organic
matter and 19.4 cmolc(+)/kg of CEC) than in soils
devoted to inflorescence crops (3.3% of organic matter
and 16.5 cmolc(+)/kg of CEC). According to these
results the bioavailability of heavy metals would be
expected to be low in the soils devoted to leaf crops.
However, the heavy metal contents in these crops were
higher than in inflorescence crops, illustrating the
metabolic differences between these crops for absorbing
or accumulating heavy metals from soil. Also a different
source (e.g. atmospheric deposition) could be responsi-
ble for the different content of some heavy metals (e.g.
Pb).
The concentrations of Cd, Cr, Cu, Fe and Mn showed
significant differences between inflorescence and leaf
crops (Table 2), being lower in the former crop type than
in the latter. There were no significant differences for
Co, Ni, Pb and Zn contents between the two crop types.
The Ni concentration was twice as high in leaf crops
than in the inflorescence crops and the Zn content was
higher in inflorescence crops than in leaf crops.
However, these differences are not statistically signif-
icant. The Co content could not be determined in
samples of inflorescence crops and Pb content could not
be determined in several samples of inflorescence crops,
Table 3
Correlation coefficients of heavy metal contents in crops with their contents in soils, total content (Total) and EDTA-extractable content (EDTA)
Cd Co Cr
Leaf crops
Total − 0.441 − 0.754 −0.064
EDTA 0.183 − 0.029 −0.228
Inflorescence crops
Total − 0.670 b – 0.140
EDTA − 0.113 – 0.288
a
Correlation is significant at 0.05 level.
b
Correlation is significant at 0.01 level.
and for this reason we did not apply statistical tests to
these data. However, leaf crops showed higher contents
of these metals.
Cd, Co, Cu, Fe, Mn and Ni contents in soils, grouped
by the two crop types, did not show significant
differences between fields with inflorescence or leaf
crops (Table 2). It follows, therefore, that the metabolic
differences between species should be the main reason
for the high contents of Cd, Co, Cu, Fe and Mn found in
leaf crops (Ge et al., 2000). These results were similar to
those achieved by other studies carried out within and
outside the European Mediterranean region, in which
Cd and Pb contents of several crops (artichoke, sweet
beet and lettuce) were compared (e.g. Zurera et al.,
1987; Bosque et al., 1990).
On the other hand, there were some significant
differences between heavy metal contents in soil,
specifically Cr and Zn extractable contents and total
Pb contents (Table 2). Nevertheless, these differences
did not influence the crop contents of Cr, Pb and Zn. The
total and extractable soil content of Pb and extractable
soil content of Cr were higher in fields under
inflorescence than in fields under leaf crops, whereas
Cr and Pb contents were lower in inflorescence crops
than in leaf crops. Zn contents were higher in soils under
inflorescence crops than in soils under leaf crops,
although only EDTA fractions showed significant
differences. Differences in Zn concentrations between
fields, which were grouped by crop type, were higher in
soils than in crops. Consequently, differences in
physiology between crop types are the main factors
influencing the crop contents of Cr, Pb and Zn.
Furthermore, atmospheric deposition can also be an
important process for the entrance of some heavy metals
(e.g. Pb) into the crops.
In addition, there were large differences in the
concentration factors between crop types in the study
area. Concentration factors were higher for leaf crops
than for inflorescence crops, except for Zn. In fact,
Cu Fe Mn Ni Pb Zn
0.156 − 0.240 −0.644 a − 0.253 0.051 0.429
0.196 − 0.101 0.386 − 0.415 0.073 0.363
0.514 a 0.214 0.159 − 0.349 0.487 0.285
0.393 0.324 0.098 0.272 0.354 0.009
 M. Peris et al. / Science of the Total Environment 378 (2007) 42–48
concentration factors were more than twice as high in
leaf crops as in inflorescence crops, except for Cu and
Zn, as shown in the Table 2. These results show again
the importance of how metabolic differences between
crop types influence the absorption and transportation of
heavy metals in plants. For instance, field MPC-06,
which is cropped with Swiss chards, showed the highest
concentration factor of Co, Cr, Cu, Fe, Ni, Pb and Zn,
although heavy metal contents in the soil of this field
were not the highest of the study area. This must be due
to the fact that this is an accumulator crop.
3.3. Relationships between heavy metal contents in
soils and crops
There were no significant correlations between
EDTA-extractable heavy metals in soils and heavy
metal contents in the edible parts of inflorescence or leaf
crops (Table 3). However, several scientists consider
that EDTA-extractable contents could indicate the
bioavailability of heavy metals for several crops (e.g.
Haq et al., 1980; Rauret, 1998). The results obtained in
this study reflect that EDTA-extractable contents cannot
be used to predict the heavy metal contents in the edible
parts of lettuce, Swiss card and artichoke crops in the
study area.
On the other hand, the few significant correlations
between total heavy metal contents in soils and in crops
were negative for Cd in inflorescence crops and for Mn in
leaf crops, whereas they were positive for Cu in in-
florescence crops. Negative correlations of Cd and Pb
contents were also obtained between soil and crop
contents by Alegría et al. (1991) in similar soils. These
scientists explained these results by the importance of
atmospheric deposition. These results seem to indicate
that heavy metal contents in crops cannot be predicted
using total contents, because crop contents depend on
more factors (e.g. atmospheric deposition, soil proper-
ties). It follows, therefore, that a reduced use of agro-
chemicals would not be sufficient to guarantee the non-
contamination of crops by heavy metals. In addition to
these agricultural practices it would be recommendable to
carefully plan the location of industries so that crops were
not affected by air emissions with contaminants such as
heavy metals. This would be particularly relevant for leaf
crops. Given that the land-use pattern in the study area
over the last few decades has been similar to that in other
parts of the European Mediterranean region (Coccossis,
1991; Groom et al., 1995), the results achieved here can be
extended to the whole region, where the planning
recommendations outlined here should be considered in
order to improve crop quality.
47
4. Conclusions
Soil properties and heavy metal contents in soils and
crops were analysed in thirty fields devoted to
horticulture in the province of Castellón, a representa-
tive area of the Mediterranean region. Soil properties
analysed in the study area were similar to other
agricultural soils characterised in the Spanish Mediter-
ranean region. Soils were basic, carbonated, having high
organic matter contents, and loam textures. These
properties suggest a low bioavailability of heavy metals
in these soils. Only in a few fields having high electrical
conductivity (N 4 dS/m), the mobility of some heavy
metals (e.g. Cu) seems to be facilitated.
A total of seven crops had Cd or/and Pb contents that
exceeded the maximum levels established by Commis-
sion Regulation no. 466/2001 (DOCE, 2001). These
results indicate that it is necessary to carry out further
research, to determine heavy metals in crops, in order to
guarantee crop quality in the European Mediterranean
region, where these types of crops are relevant for the
diet and can have a negative impact on human health.
Differences in metal absorption and/or accumulation of
metal contents by two crop types (inflorescence and leaf
crops) were analysed in their edible parts. Heavy metal
contents (Cd, Co, Cr, Cu, Fe, Mn, Ni and Pb) were higher
in leaf crops than in inflorescence crops, except for Zn.
The high contents of heavy metals in leaf crops seem to be
due to metabolic processes as these crops are accumula-
tors. Furthermore, these crops absorb more easily heavy
metals that are deposited on their leaves by atmospheric
deposition (e.g. industrial sources or agrochemical appli-
cations). From these results we can conclude that it is not
only highly necessary to reduce the consumption of agro-
chemicals within the region but also to carefully plan the
location of industries in order to guarantee crop quality
and avoid serious damages to human health.
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