Carpth. J. of Earth and Environmental Scie nces, 2008, Vol. 3, No. 2, p. 65 – 82 [600319]

Carpth. J. of Earth and Environmental Scie nces, 2008, Vol. 3, No. 2, p. 65 – 82

HEAVY METALS CONCENTR ATION OF THE SOILS
AROUND ZLATNA AND COP ȘA MICĂ SMELTERS
ROMANIA

Floarea DAMIAN1, Gheorghe DAMIAN1, Radu LĂCĂTUȘU2,3 &
Gheorghe IEPURE1
1North University of Baia Mare, 62A Dr. Victor Babe ș Street, 430083 Baia Mare, Romania,
e-mail: [anonimizat]
2 National Research & Development Institute for Soil Science, Agrochemistry and Environment
Protection Bucharest, Blvd. Marasti, 61, 011464, sector 1, Bucharest, Romania;e-mail:
[anonimizat]
3 “Al. I. Cuza” University, Iassy

Abstract. The concentration and distribution of Pb, Cu, Zn and Cd in the soils from
Zlatna and Cop șa Mică (Romania) highly polluted by metallurgical activity, have been studied
in the soil profile for different types of soils related with the physical an d chemical properties of
the soils. In Zlatna area, there have been studied the Aluviosol, Dystricambosol and Alosol
types and in Copș a Mică area the Aluviosol and Phaeozem types. Content of humus, pH, cation
exchange capacity, base saturation, organic carbon , C/N ratio, nutrient elements, texture and the
heavy metals concentration in total and mobile form were determined for each pedogenetic
horizon. The heavy metals concentration varies within the soil profiles related with different
properties of the soils and with the metal species. The highest concentrations of lead, of 245
ppm to763 ppm, are in relation with the organic horizons, in conditions of acid pH (3.12 – 3.85)
of Dystricambosols and of Alosols from Zlatna zone, and of 561 ppm to 2768 ppm in
Aluviosols and Phaeozems from Cop șa Mică area, in conditions of alkaline pH. Lead contents
decrease suddenly, under the maxi mum allowable limit in C horizons within the soil profiles.
The affinity of Pb for surface horizons is em phasized by the excessive contents of global
samples of 995 ppm in Z-T, 980 ppm in Z-2 and of 5000 ppm in CM-T. The copper contents of
the soil profiles, close to the maxi mum allowable limit are specific for the surface horizon of
Dystricambosols (73.8 ppm), for the global sample Z-T, (99.7ppm) and for the Aluviosols in
Copșa Mică area (71.1 to 96.9 ppm). Copper concentrations of 1165 ppm from Zlatna area
increase towards the site of smelter in the global sample Z-2. The copper concentration of
Copșa Mică global sample, representative for Aluvi osols type exceed maximum allowable
limit, being of 199 ppm. In conditions of acid pH , Zn presents concentrations of 775 ppm and of
820 ppm at C and B horizons, rich in clay and with a higher content of Fe and Mn in Aluviosol and Dystricambosol types in Zlatna area. In conditions of neutral to alkaline pH (5.03, 7.10,
7.26) in the soils from Copșa Mică , Zn immobilization in quantities of 7500 ppm, 4900 ppm in
Aluviosols, 684 ppm in the Phaeozem type and 8591ppm in global sample at the surface
horizons it is associated with values of the humus content between 0.48-4.56 percent. The Cd
contents of 5.05 ppm exceed the maximum allowable limit in the global sample Z-2. In Bv
65

horizon of Dystricambosols, the content of Cd is of 2.87 ppm in comparison with the contents
under 1 ppm from the surface horizons. The increase of Cd content with the depth is related with the increase of the clay content and with acid pH conditions (3.72-4.59). In soils from
Copșa Mică , Cd represents a concentration in the surface horizons of the soil’s profiles,
between 100-400 ppm in Aluviosols and 17.99 ppm in Phaeozem type. The high concentrations
of Cd (175ppm) and of As (1500ppm) are related with the organic horizon of the soils from the
global sample in Cop șa Mică area. In comparison with lead and copper, cadmium has mobility
on the soil’s profile because it maintains the contents over maximum allowable limit values and
the intervention limit in the intermediate horizons of the soil’s profiles.

Keywords: soil type, heavy metals, pollution, mobility, soil profile

1. INTRODUCTION

The pollution with heavy metals has been researched in adjacent soils of
metallurgical factories from Zlatna and Cop șa Mică , in Romania. Generally, soils
nearby smelters, present high risk of pollutio n with heavy metals on long term (Kabala
& Singh, 2001). High concentrations of Cu, Pb, Cd and Zn, have been reported in
Poland (Pichtel et al. 1997), in Příbram region (Czech Republic) (Vaněk et al. 2005),
Kola Peninsula, (Koptsik et al. 2005), in Finland, (Peltola & Åström, 2003), in
Romania (L ăcătușu et al. 1998, 1999, Damian et al. 2007). Pollution with heavy metals
from the atmospheric emissions affects the ecological functions of soils (Koptsik et al. 2005). The urban soils from several cities in Europe are subject to heavy anthropogenic disturbance, (L ăcătușu et al 2007, Biasioli et al. 2007).
Soils nearby those two cities cannot be used for agriculture, (Fig. 1a) forest
field, (Fig. 1b) because of excessive polluti on with heavy metals, being an affectation
source for the population’s health.

a

b
Figure 1: a. Copșa Mică ; b. Zlatna. Effects of pollution with heavy metals on soils

Unfortunately, the industrial ac tivities that have place in Cop șa Mică , (Fig. 2),
are not correlated with research and devel opment activities for environment protection,
(Fekete 2006).
66

The negative effects of the
atmospheric emissions on soils,
vegetation, water and animals, from
Zlatna and Cop șa Mică areas, have
been studied by L ăcătușu et al. (1998,
1999), Har et al. (2004), Rusu et al.
(2004) and Williamson et al. (2003).
The study of the behaviour of
heavy metals in soils, from the two
areas affected by the metallurgical
industry, has had in view the following: investigation of the distribution of those four heavy
metals, Pb, Cu, Zn and Cd in the soil’s
profiles, contamination rate and heavy
metals mobility in relation with the physical-chemical properties of soils.

Figure 2. Image in 2008 from Cop șa Mică Pb-Zn
smelter
Generally, the soil, through its component s and properties, controls solubility,
mobilization and deposition of toxic metals, resulted from anthropogenic sources,
(Narwal et al. 1999, Siegel 2002). The influence of the soil’s properties over the
relative distribution of the heavy metals, (L ăcătușu 1998), is better observed in the soil
profiles (Kabala & Singh 2001).

2. MATERIALS AND METHODS

2.1. Location of the studied areas
The two areas (Fig. 3) have been selected for this study because the soil’s
contamination with heavy metals has b een caused by the mining and non-ferrous
metallurgical activity.
Zlatna town is located
in the Zlatna depression area
from Apuseni Mountains, on the
upper course of the Ampoi River, at an altitude of 450-500 m, at 38 km west of Alba Iulia town. The depression area is dominated by terraces, motion
cones and alluvial formations in
the meadow area. The annual atmospheric emissions have been of 150-450t of sulphur dioxide and of 3498t of dust
loaded with heavy metal
particles. Cop șa Mică town is located in the central part of Transylvania, in the
depression zone of the Târnava Mare River, surrounded by hills, at 43 km of Sibiu
town, being dominated by hill formations and floodplains.

Figure 3. Location of the studied area
67

2.2. Soil Types Description

The identification of soil types from the adjacent areas of the two industrial
plants has been achieved on the basis of soil profiles excavated up to 1.20 m depth. The description of the soils has been achieved, according to the Soil systematic, by the
"Romanian System of Soil Taxonomy" (RSST-2000) (Florea & Munteanu, 2003).
The most representative soils of the i nvestigated area from Zlatna are:
Aluviosols, Alosols, Dystricambosols. The Aluviosol type (AS) develops in the river Ampoi’s meadow, on alluvial
parental material, represented by gravel with coarse sand levels, and on the tributaries
terraces. Gravels are formed, predominantly , of sedimentary, igneous and metamorphic
rocks. The Ao horizons (Fig. 4) are found in the top 15-20 cm of the soil profiles.
These horizons are composed of mineral materials with the brown colour and variable
texture from sandy with little quantities of silt and clay, to loam. The humus content is
low, of 1.02-1.56% and the pH is neutral to alkaline. The great quantity of potassium, of 251 ppm in profile Z-1 certifies the presence of clays of illite type. Under Ao
horizon there is a C horizon. In the C horizon the sandy fraction prevails, and the silt
and clay decrease, (Table 1). The C horizon c onsists of partially decomposed parental
material represented by sand and gravel.

Z-1

Figure 5. Associated surfaces
of the Dystricambosol and the
soil profile Z-3

Z-2
Figure 4. Profiles of the Aluviosols

The Dystricambosol type (DC) occupies the biggest surface around Zlatna
town. These soils are specific to hill and mountain areas. They were formed in
delluvium deposits, from the fine sandstone in the slope areas of the right versant of
Ampoi Valley. The soil’s surface is eroded, (Fig. 5). Within the soil profile, the
following horizons are distinguished: Ao–Bv- C. The Ao horizon has brown colour and
has the high percentage of humus. The pH va riation in the soil profile correlated with
the depth is from 3.72 to 4.59. The textural differentiation is weak within the soil
profile and skeletally moderated. In Bv horizon, the clay fraction that has been
produced by weathering increases slightly, (Buol et al. 2003). The C horizon contains a
high rate of parental material fragments , intensely weathered up to 56.65%. Base
saturation is low and increases with the depth.
68

The Alosol type (AL) develops in the south-western part of the Zlatna area.
These soils have formed in areas with slopes of 25-40°, on delluvial and colluvial
sediments, represented by pyroclastic rocks, sandstone, clay, conglomerates resulted
from Badenian formations, colour being predominantly red. The typical vegetation is that of deciduous forests (durmast, beech). The soil profile is well differentiated,
including the horizons: Ao-El-E/B-Bt-C. The texture varies within profile from sand loamy to clay loamy with the depth. The content of humus is low of 1.38% in Ao horizon. The pH variation is low and maintains itself in the high acid domain. The base saturation is very low, of 8.24-3.66%. Th e Bt horizon is found from 62-112 cm, has a
high quantities of clay, and contain the angular fragments in different degrees of
weathering. The colour is yellow-brown, du e to accumulations of iron oxyhydroxides.
The colour of C horizon is yellowish. It is composed of disintegrated and weathered
fragments of parental material and a high quantity of clay. The clay minerals are
represented by smectite, kaolinite, illite.
Soils from Cop șa Mică have been formed in vari ed conditions of relief with
morphologic characteristics, which succeed on vertical, from mountains, hills, and depressions. In the bottom land area of Târn ava Mare River are developing Aluviosols,
and in the terrace and hill areas preva il Eutricambosol and Phaeozem types.
The Aluviosol type (AS) develops on the fluvial parental material, being
represented by sands and gravel in alternation with centimetre levels of clay. The
underground water level can be found at 2 m of soil profile and can influence its
formation. Within the soil profile, the water drainage is very good.

Figure 7. Aluviosol CM-2

Figure 8. Phaeozem CM-3

Figure 6. Aluviosol CM-1
Aluviosols has a well-developed profile , (Fig. 6, Fig. 7) formed of the
following horizons: Ao-C and Ao-C-bAo-bC. The Ao horizon with a thickness of 18
cm, has a black-grey colour due to pollution with carbon black. The content of humus
is 2.2%, the pH is neutral and presents a high content of potassium. The texture is
69

loamy. The C horizon is in progress of form ation, unstructured, with low content of
humus. The mineral material of this horizon is represented by quartz, illite, feldspars,
kaolinite and smectites.
The Phaeozem type has a considerable de velopment, especially in the inferior
part of the hill and terrace areas, at north and south of Cop șa Mică area. The relief is
weakly inclined, 20-30°. The original vege tation is represented by durmast forest. The
parental material is represented by marl s, clays and Pannonian siltstone. The soil
profile, CM-3, is typical for this type of soil, Am-Bv-C (Fig. 8). The Am horizon has a thickness of 24 cm, black colour, and with a high content of humus. The structure of this horizon is very well formed, prevaili ng granular soil aggregates related to the
amount of organic matter, (Layton et al. 1993). The texture is clay-loam, with a high
content of potassium and mobile phosphorus. Th e content of soluble salts is low. The
mineral material of the soil is represented by illite and smectite, and fine quartz. The
Bv horizon is predominantly clayey with a lo w content of carbonate. It is developed on
a thickness of 70 cm with brown-yellowi sh colour due to accumulation of Fe
oxyhydroxides. It is a very little structured horizon and has a low content of humus and
low quantities of potassium and mobile phosphorus.
2.3. Sampling
There have been accomplished four soil profiles for copper smelter in Zlatna
area and three profiles for Pb-Zn smelter in Cop șa Mică area, on different types of soils
and different distances from the smelters. The location of soil prof iles had in view the
ascertainment of soil’s contamination with heavy metals for different uses, the forest
field, and the arable field. The soil samples have been yielded from different depths, which correspond with the pedoge netic horizons in each soil profile up to 1.20 m deep.
The contamination rate of soils on a surface limited by soil profiles from the
two areas has been checked by yielding some global samples from the depth of 0-20
cm, of 100 kg each. For Zlatna there have been yielded 2 global samples that correspond with the development area of Dystricambosols (Z-T) and with the development area of Aluviosols from the location area of metallurgical factory (Z-2T).
For Copșa Mică , the global sample (CM-T) is representative for the Aluviosols nearby
the factory.

2.4. Laboratory Analyses

Soil samples have been homogenized and dried in the air and sieved through 2 mm sieve. From each sample, there have been effectuated analyses for the
concentrations in the total and mobile form of heavy metals as Pb, Cu, Zn, Cd, and for
the physical-chemical properties of soils: pH, humus content, cation exchange
capacity, C
org, base saturation, content of nutritive elements, C/N ratio, texture type.
The analyses have been effectuated at the Research Institute for Soil Science
Agrochemistry and Environment Protection, Bucharest. Determination of pH has been
accomplished in watery suspension in report with the soil: water of 1:2.5. The sum of basic cations of exchange has been achieve d by the extraction with HCI 0.05 n, after
70

71Kappen method (me/100 g soil). The hydroly tic acidity has been determined at
equilibrium in solution of acetate of sodium 1 n, the soil report: solution of 1:2.5; by
titration with NaOH, in presence of phenolphthalein of extracted acidity (me/100 g
soil). The total cation exchange capacity h as been determined through calculation:
CEC= SB + Ah (me/100 g soil). Mobile content of heavy metals have been extracted in
ammonium acetate 1 n and EDTA 0.01 m, the soil report: solution of 1:5 and dosing
with the spectrophotometer with atomic absorption. Total contents of heavy metals have been obtained by wet mineralization with HC1O
4 and HNO 3 and dosing with the
spectrophotometer with atomic absorption. The humus volumetrically has been determined used through the wet oxidation method (after Walkley-Black). The amount
of total nitrogen has been obtained by Kjeldahl method. Phosphorous and potassium
soluble has been determined in solution of ammonium acetate lactate of at pH = 3.7
(after Egner-Riehm-Domingo).
Particle size distribution has been determined by sieving and sedimentation.
Determination of the content of clay and silt has been effectuated by sedimentation
with the Kubien pipette method.
The X-ray diffraction analyses have been performed at the North University of
Baia Mare using a Philips-Muller Diffract ometer with PW 1050/25 goniometer and
copper tube PW 1043/01 and the speed of registration of 1 degree per minute.

3. RESULTS AND DISCUSSION

3.1. Soil properties

Texture differentiation on soil profiles is low in both areas, and reflects the
specific conditions of formation of soil types. In Zlatna, the Aluviosols with transition
horizon, under the Ao horizon, the clay c ontent decreases with the depth, and the sand
content increases. In Dystricambosols and Alos ols, the content of clay increases in Bv
horizons towards Ao horizons, making a transition from sandy loam to loam. In Cop șa
Mică, within the soil profile the Aluviosols over the entire depth are sandy, poor in
clay (6.6-13.7%), with the exception of Ao horizon from profile CM-1, where the content of clay is of 27.9% . In the Phaeozem type, the granulometric fractions are
distributed in equal quantities betw een Am and Bv horizons (Tab. 1).
The cation exchange capacity is mode rated in all A horizons (12.58-21.96
meq/100g soil) in Zlatna area and 16.65 meq/100g for Phaeozem type in Cop șa Mică
area. The increase of clay content from hor izons B influences an increase of cation
exchange capacity towards A horizons. The content of humus varies from low to moderate (1.02-3.12%) in surface horizons in the soils from Zlatna, and from very low
to moderate (0.48-2.76%) in the soils from Cop șa Mică. Generally, the content of
humus decreases with the depth on soil profil es. In global samples, the content of
humus varies from low (1.44%) in Z-2T (Zlatna) to high (4.38%) in Z-T Zlatna, and
(4.56%) CM-T (Cop șa Mică ). After the values of pH, Aluviosols from both areas
correspond to the class of neutral reaction to alkaline (6.39 – 8.16). The lower values of
the pH are associated with the organic horiz ons, and the increase of pH with the depth
is less than 1% in this type of soils.

Table 1. The physical and chemical proper ties of the soils from Zlatna and Cop șa Mică areas
Humus C org Nt P K Sand Silt Clay Soil
Type/Horizon Depth
(cm) pH
% C/N
ppm % Texture
class CEC
(meq/
100gsol) Base
saturation,
(%)
Aluviosol,
Z-1 Ao
A/C 0-20
20-70 7.36
7.78 1.02 0.30 0.59 0.17 0.056 0.016 12.3 12.7 7.2 6.2 251
65 71.8 80.7 9.9 5.5 18.3 13.8 SG SG – – – –
Z-2
Ao
A/C 0-20
20-73 6.39 6.70 1.56 1.08 0.90 0.62 0.128 0.100 8.2 7.3 1.1 2.8 72 60 56.1
51 19.1 23.8 24.8 25.2 LL
SL 21.96 22.33 20.51 21.34
Dystricambosol
Z-3 Ao
Bv
C 0-20
20-47 47-97 3.72 3.90 4.59 3.12 0.78 0.42 1.81 0.45 0.24 0.124 0.060 0.108 17.0
8.8 2.6 5.0
– – 39 40 93 64.2 59.9 62.6 18.7 21.0 10.5 17.1 19.1 26.9 SL SL
LL 15.63 11.02 18.53 4.50 2.83
12.82
Alosol
Z-4 Ao
E
Bt 0-20
20-45 45-90 3.85 3.98 4.13 1.38 0.66 0.48 0.80 0.38 0.27 0.070 0.038 0.036 13.3 11.7
9.0 0.8 3.8
– 49 61 81 53
46.5 45.7 27.1 26.4 22.1 19.9 27.1 32.2 SL
LL LL 12.58 12.92 21.80 3.66 3.66 8.24
Z-T Global 0-20 3.49 4.38 2.54 0.180 16.5 34.1 39 65.61 16.4 18.05 SL 21.61 3.49
Z-2T Global 0-20 7.64 1.44 0.83 0.050 19.5 17.4 115 70.4 11.5 18.1 SM
Aluviosol
CM-1 Ao
A/C
C 0-18
18-47 47-73 7.26 7.96 8.16 2.22 0.54 0.30 1.28 0.31 0.17 0.16
0.014 0.016 9.3
26.1 12.7 6.3
10.3
7.2 232
53 39 54
88.3 84.7 18.1
2.3 5.9 27.9
9.4 9.4 LL
UM UM – – – – – –
CM-2 Ao
C 0-25
25-32 7.10
8.02 0.48 0.42 0.27 0.24 0.028 0.022 11.6 12.9 13.4
8.7 84 81 84.9 90.7 5.2 2.7 9.9 6.6 UM
UG – – – –
bAo
bC 32-49
49-61 7.55 7.89 1.56 0.54 0.90 0.31 0.062 0.048 17.0
7.6 79..3
13.9 149 115 84.4 74.2 6.0
12.1 8.6
13.7 UG SM – –
Phaeozem
CM- Am
Bv 0-24
24-74 5.03 5.94 2.76 0.96 1.60 0.55 0.11
0.076 15.8
8.5 38.3
8.5 237
74 63
62.8 13.3 13.8 23.7 23.4 LN LN 16.65 17.65 11.15 15.52
CM-T Global 0-20 6.94 4.56 2.64 0.140 22.0 20.4 170 65.1 12.7 22.2 LN – –
Z-1-4 soil profile Zlatna, CM-1-3, soil profile Cop șa Mică ; Texture class: SG-sandy loam, LL- loam; SL-sandy clay loam; UM-loamy sand; UG-sand; SM-sandy loam; LN-clay loam
72

The Dystricambosol and Alosol types from Zlatna have the pH on soil profiles
between 3.72 to 4.59 and 3.85 to 4.13, corresponding to the class of acid strong
reaction to acid moderate. Also, the soil of Phaeozem type from Cop șa Mică , has acid
weak reaction with variation of pH, from 5. 03 to 5.94. In global samples from Zlatna,
the pH is 3.49 in Z-T, proper to soil of Dystricambosols, and of 7.64 in soil from the
location area of metallurgical factory (Z-2T). In global sample (CM-T) from Cop șa
Mică pH is 6.94. The base saturation rate increases with the depth in all soils from both
areas. The quantity of C org is, in general, very low <2% in soil profiles, the biggest
values being specific to surface horizons of 0.592 to 1.810% in Zlatna, and between
0.27 to 1.60% in Copș a Mică area. In global samples, the content of C org is moderated,
2.54% in Z-T and 2.65% in CM-T, and low in Z-2T, 0.835%.
The studied soils are poor in nutritive el ements, (Tab. 1). The content of Nt
varies from 0.056% to 0.128% in organic horizons of soil profiles from Zlatna, and
from 0.028% to 0.16% in soils from Cop șa Mică . The low content of nitrogen is the
consequence of reducing the microbial activ ity of fixation of nitrogen caused by
pollution with heavy metals, (Lorenz et al. 1992). The contents of potassium have low
values, the highest values, of 237 to 152 ppm , are related with the organic horizons of
soils, which had been treated with fertili zers, in Phaeozem and Aluviosol types (CM-1
soil profile in Cop șa Mică area and in Z-1 soil profile from Zlatna area).
Generally, the content of phosphorus in the studied soils is low. Bigger
contents of phosphorus have b een determined in sandy and sandy loam soils, poor in
clay fraction, which have determined the lo wer binding of phosphorus, (Zarcinas et al.
2003).
The mineralogical composition of the clay fractions (under 0.02 mm) in the
soil global samples from both areas was determined by X-ray diffraction studies. The
dominant clay types are: montmorillonite, illite, kaolinite. All the clay minerals present a poor crystallinity. The X-ray diffraction patterns of the clay particles indicate an
amorphous phases.

3.2 Total concentration of heavy metals

The important anthropogenic sources, by which heavy metals are introduced
into soil from both areas, have been represented by: gas emissions from the
metallurgical factories with content of metallic particles, by dissolving under the effect of acid rains; leaching of heavy metals from the tailling dumps and from the metallurgical slag. Concentration in a total and mobile form (Tab. 2) of those four
analyzed heavy metals, Pb, Cu, Zn and Cd in soil profiles and in the global samples of
both areas, Zlatna and Cop șa Mică , exceed maximum allowable limit for soils,
according to the Romanian legislation.
Concentration in a total form of those four heavy metals in different types of
soils reflects different rates of pollution on soil profiles depending on the metal species
(Tab. 2). The concentration and distribution of heavy metals have been analyzed on
soil profile in relation with certain phys ical-chemical properties of soils, which
determined mobility and bioavailability in soils, (Jiemba 2005). In soil, heavy metals
can be affected by processes of sorption/d esorption, precipitation, dissolution, redox
reaction, incorporation in the solid components of soil, (Koptsik et al. 2005).
73

Table 2. The total and mobile form of concentration of heavy metals in soil from Zlatna and
Copșa Mică areas

Pb ppm Cu ppm Zn ppm Cd ppm Soil
type/horizon/profile total mobile total mobile total mobile total mobile
Aluviosol
Z-1
Ao
A/C

66 57

41.7 31.4

45.2 24.2

16.0 4.6

102 207

35.6 187

0.95 1.01

0.60 0.70
Z-2
Ao
A/C
48
39
14.4
5.3
19.2
12.4
230 775
63.0
69.1
0.50
0.25
0.63
0.19
Dystricambosol
Z-3
Ao
Bv
C

763 39
39
374 8.7
7.5
73.8 20.1
13.7
33.4 10.1
4.1
150 161
830
33.5 16.2
304
0.35 0.35
2.87
0.21 0.23
1.55
Alosol
Z-4
Ao
E
Bt
245
48
30 101
18.9
10.9 38.8
27.9
24.7 22.4
12.4
16.0 105
82
93 40.6
51.8
71.2 0.35
0.28
0.45 0.21
0.25
0.42
Aluviosol
CM-1
Ao
A/C
C
2768
26 9
1173
21.0 4.0
96.9
5.1 1.0
22.4
1.4 0.7
7500
275 37
2819
104 32.0
400
2.79 0.45
153
2.60 0.33
CM-2
Ao
C
bAo
bC
1429
61 182
21 1313
48.0 89.0
9.8 71.1
8.3 21.5
3.7 23.3
3.0 8.7
1.3 4900
1070 1808
54 2974
489 306
35.6 100
23.70 31.25
0.50 74.4
23.18 25.24
0.34
Phaeozem
CM-3
Am
Bv

561
30
498
12.1
22.4
6.
10.2
1.4
648
513
484
102
17.99
1.60
16.30
1.35
Z-T Global sample 995 876 99.7 40.7 127 26.4 0.50 0.34
Z-2T Global sample 980 378 1165 275 1377 170 5.05 2.90
CM-T Global sample 5000 2042 199 36.1 8591 2795 175 161
MAL 100 100 300 3
MAL – maximum allowable limit; Z-1-4 soil profiles in Zlatna; CM-1-3 soil profiles in
Copșa Mică.

3.2.1 Lead
The highest concentrations of lead ar e related with the organic horizons of
Dystricambosols and of Alosols from Zlatna in conditions of acid pH, (Fig. 9) and in
Aluviosols and Phaeozems from Cop șa Mică in conditions of alkaline pH, (Fig. 10).
Lead concentrations vary between 245 to 763 ppm in Zlatna, and between 561 to 2768
74

ppm in Copș a Mică . Lead contents decrease suddenly, under maximum allowable limit
(MAL) in C and Bv horizons of the soil profiles, (Fig. 11) thus proving the Pb affinity
for insoluble humic substances, (Angehrn-Bettinazzi et al. 1989).
75
Z-3
02004006008001000
0 20 47 97
Depth (cm)Pb Concentration (ppm)
3.63.653.73.753.83.853.93.95
pHPb
pH

Figure 9. Distribution of Pb and the pH
variation in soil
profile Zlatna area
CM-1
050010001500200025003000
0 20 45 90
Depth (cm)Pb Concentration (ppm)
6.877.27.47.67.888.28.4
pHPb
pH

Figure 10. Distribution of Pb and the pH
variation in soil profile Cop șa Mică area

The bigger stability
of complexes with
humic acids of Pb
and Cu (due to
coordinative
complexes) than that of complexes with Cu and Zn
(due to reactions of
ionic exchange) has been demonstrated
by Pinheiro et al.
(1994), Ladonin &
Margolina (1997). For the excessive concentrations of Pb from Aluviosols and Phaeozems, in Cop șa Mică, which have a content of humus from very low to medium
(0.48 to 2.76%), it is possible that in retaining of lead through absorption mechanisms, an important role may be played by the clay fraction demonstrated by Sipos et al. (2003). The clay content in surface horizons of the CM-1 and CM-3 profiles is of 27.9% and 23.7%. Absorption might be favoured at near-neutral to alkaline pH values,
(Voegelin et al. 2003), (pH of 5.03 in CM-3 and pH of 7.26 in CM-1) with a weak variation, (Bradl 2004) from surface horizons of soil profiles. An important role for
biding through absorption of Pb, can be played by Fe oxides and of Mn, (Bradl et al. 2005), which are presented in great quantity in surface horizons of the soil profiles from Cop șa Mică . Also, high pH could favour reactions of precipitation through which
Pb is transformed in insoluble compounds in these soils of hydroxides Pb form that are, predominantly, between pH 6 and pH 10, (B radl 2004). The immobility of Pb within
the soil profiles is also emphasized by the per cent concentrations of contents in mobile
form of the total form contents. The percent of Pb in mobile form is higher in the upper
horizon, and decreases with the depth on soil profiles of both areas. The affinity of Pb
0 200 400 600 800
Pb Concentrations47-97 cm20-47cm0-20 cm3/3 3/2 3/1Z-3 Profile/horizonsMA L
Pb

Figure 11. Distribution of Pb in soil profile and MAL of Pb

for surface horizons is emphasized by the excessive contents from global samples of
995 ppm in Z-T, 980 ppm in Z-2T, and 5000 ppm in CM-T.

3.2.2. Copper
Copper is the heavy metal, strongly bou nd of soil’s phases, which determines a
contamination on long term, (Koptsik et al. 2005), caused by formation of some
constituents of soil of no exchangeab le components, (Bradl et al. 2005).
Copper contents in studied soil profiles present low concentrations, under the maximum allowable limit of 100 ppm, but ove r the normal values. The contents close
to maximum allowable limit are specific fo r Dystricambosols (73.8 ppm) profile and
global sample Z-T (99.7 ppm) and for Aluviosols from Cop șa Mică (71.1 to 96.9 ppm).
Copper concentration from Cop șa Mică global sample exceeds maximum allowable
limit, being of (199 ppm), and the Cu conten t in global sample Z-2T exceeds this limit
for 11.65 times. Association of bigger conten ts of copper with surface horizons of soil
profiles (Tab. 2) and concentrations of the global samples sustains the role of organic
material, in the form of humic and fulvic aci ds as mechanisms for Cu in soil retention,
(Bradl et al. 2005). The repartition of Cu cont ents in quantities close to horizons, in the
soil profiles of Dystricambosols and Aluvisols from Zlatna area, is related with Fe, Mn, and clay increases with depth. In these conditions, the weak mobility of Cu (in Z-4 soil profile) is associated with low values of pH (3.85, 4.13), which prevent the adsorption
on clay fraction (Bradl et al. 2005). At bigger concentrations of Cu, it is obvious the
bigger retention capacity of horizons rich in organic material of 68.58% in soil profiles
for Dystricambosol and 94.07% in soil profile for Aluviosol type from Cop șa Mică
area. The mobility of Cu in soils from Cop șa Mică was limited as shown by reduction
in their concentration within the soil pr ofiles in relation with decrease of humus
content (Fig. 12). Association of Cu in high proportions (from 40 to 74%) with organic
matter, Fe, Mn oxides and carbonate was dem onstrated in sequential extraction by Ma
& Rao (1997).

CM-1
020406080100120
0 18 47 73
Depth (cm)Cu Concentration (ppm)
00.511.522.5
HumusCu
Humus

Figure 12. Distribution of Cu and the humus
variation in soil profile from Cop șa Mică area
Z-3
02004006008001000
0 20 47 97
Depth (cm)Zn Concentration (ppm)
05101520
TZn
CEC
Figure 13. Distribution of Zn and CEC
variation in soil profile from Zlatna area
The series of bivalent elements with affinity for the most stable complexes
with humic acids is the following: Cu>Pb>Fe>Ni=Co=Zn>Mn=Ca, (Adriano 2001).
The high percent of sand from soils of both areas could negatively influence the sorption of Cu, (Kabala & Singh 2001). Th e low concentrations of Cu from soil
profiles of Zlatna area are due to losses fro m topsoil through eros ion of flow that
76

removed the fine part of the material from the surface. Concentrations of Cu from
Zlatna area increase very much towards the site of smelter and near the tailing dump, in the lowest area of Aluviosols.
3.2.3. Zinc
The behaviour of Zn on soil profiles is different in the two areas, possible
under the influence of pH values, (Catlett et al. 2002). In organic horizons of soils from Zlatna, where the pH varies from neutral to aci d, Zn concentrations in total form do not
represent significant values for pollution. The va riation within the soil profile (Z-2 and
Z-3) of the total content of zinc in rela tion with the content of humus and with the
variation of pH, has emphasized the Zn concentration (775 ppm and 820 ppm) in
quantities that exceed the maximum allowable limit of 300 ppm at C horizons rich in
clay minerals, with high cation exchange capacity (CEC), (Fig. 13). Mobility on soil profiles in conditions of acid pH can be ensu red by the ability of Zn to form complexes
with mobile organic substances, with low molecular weight, (Angehrn-Bettinazzi et al.
1989). The role of the clay and of Fe and Mn oxides in Zn adsorption was
demonstrated by Kuo et al. (1983), Narwal et al. (1999) and Bradl et al. (2005).
In conditions of neutral to alkaline pH (pH 5.03, 7.10, 7.26) in soils from Copșa Mică , the pollution with Zn is excessive at the surface horizons level of soil
profiles. The immobilization effect of Zn in excessive quantities at surface horizons level, 7500 ppm, 4900 ppm, in Aluviosols and 684 ppm in Phaeozem type, is
associated with values of humus content, between very low to moderate (from 0.48%
to 2.27%). In presence of a relative lo w content of humus, through adsorption
mechanisms, an important role in retention of Zn can be played by fine clay fractions
that are 29% in Aluviosols and 23.75% in Phaeo zem type. In alkaline soils Zn retention
is due to the precipitation of Zn hydroxide or carbonates, (Adriano 2001).
The mobility of Zn is emphasized in all soil profiles from Cop șa Mică ,
especially in profile CM-2, where the contam ination rate with heavy metals is in
relation with the development of soil under the influence of flooding. With all these, the biggest quantity of zinc is bounded to the surface horizons of soil, especially in the case of Aluviosols, also emphasized by the Zn content of global sample that is 8591 ppm, in conditions of alkaline pH, high content of humus, 4.56%, and of C
org, 2.64%.

3.2.4. Cadmium
Generally, on soil profiles of both areas, variation of Cd concentration is
identical with that of Zn, and opposed to Pb and Cu. In Zlatna area, the content of 5.05
ppm for Cd exceeds the maximum allowable limit in global sample Z-2T. The
concentration of Cd, increase within soil prof iles, related with several soil properties
with depth, including increased clay content, in conditions of acid pH from 3.72 to 4.59. The adsorption mechanisms for Cd specific to clay minerals, was demonstrated by Dudley et al. (1991). In Bv horizon of Dystricambosols, the content of Cd reaches
2.87 ppm in comparison with the content unde r 1 ppm of the surface horizon, (Fig. 14).
Contents of Cd under 1 ppm of horizons ri ch in humus (from 1.02 to 12% in profiles
and 4.38% in global sample Z-T) sustain th e idea of low adsorption of Cd by the
organic material at low pH.

77

Z-3
00.511.522.533.5
0 20 47 97
Depth (cm)Cd Concentration (ppm)
05101520
TCd
CEC

Figure 14. Distribution of Cd and CEC
variation in soil profile from Zlatna area
CM-2
020406080100120
0 25 32 49 61
Depth (cm)Cd Concentration (ppm)
6.606.807.007.207.407.607.808.008.20
pHCd
pH

Figure 15. Distribution of Cd and pH
variation in soil profile from Cop șa Mică area

In soils from Cop șa Mică area, the Cd content from surface horizons exceeds
the intervention limit for 80 times. The retention of Cd in horizons ri ch in humus is due
to the biding capacity of humic substances in conditions of high pH, (Reuter & Perdue
1997). In comparison with lead and copper, in the case of cadmium, it is observed
mobility on soil profile in maintaining the contents over the maximum allowable limit values, and of intervention limit in interm ediate horizons in the CM-2 profile, (Fig.
15). In conditions of high pH, (determined by the content of carbon introduced in soils from Cop șa Mică by polluting with carbon black), th ere have been created conditions
of precipitation of certain compounds of the analyzed heavy metals, which maintain the excessive rate of soil pollution at longe r distances from the metallurgical factory.
The sandy soils with a low content of orga nic material, with alkaline pH with high
content of Cd, favours formation of CdCO
3, which controls solubility and
concentration of Cd, (McBride 1980).

4. CONCLUSIONS
Distribution of heavy metals in studied soils within soil profiles is influenced
by the soil’s properties, determined by the pedogenetic processes and by the modifications under the influence of anthropogenic activities. The atmospheric
emissions, with content of metallic particles and sulphur oxides, have determined the
strong acidity of soil profiles in Dystricambosols and Alosols in Zlatna area (pH 3.72 to 4.59, 3.85 to 4.13). The same effects have been decreased in the case of Aluviosols
from this area, which are situated in the floodable areas of rivers, where pH varies from
6.39 to 7.78 in soil profiles.
In Cop șa Mică area, a severe impact on soils has had the emissions of black
carbon, in a long period of time, simultane ously with the gas emissions from the
metallurgical factories of Pb and Zn. In these soils, the reaction is neutral (pH from 5.3
to 5.94) (in Phaeozem type) to alkaline (pH 7.10, 7.26 in surface horizons with a light
increase on soil profiles with depth) (in Aluviosol type). In these conditions, in Cop șa
Mică, soils have been produced a severe pollu tion with heavy metals in both surface
horizons and soil profiles, over 1m deep.
78

Heavy metals concentrations determined in the studied soil types from both
areas, Zlatna and Cop șa Mică exceed the Romanian reference limits from the Order
(756/1997). The great quantity of heavy metals from Cop șa Mică is comparable with
the excessive pollution of organic horizons due to the exceeding of maximum allowable limit for Pb of 5.61 up to 27.68 times, for Zn of 2.16 up to 25 times, and for
Cd of 5.99 up to 133.3 times. For Zn and Cd the concentration in the total form
exceeded of maximum allowable limit and an intervention threshold the clay-rich
horizons at variable depths in both areas.
In global samples from Zlatna, concentrations of heavy metal exceed the maximum allowable limit for all four metals. The concentrations of Cu are the highest
in global sample Z-2T, nearby the smelter and tailing dump, being of 1165 ppm.
Copper is associated with Pb, 980 ppm, Zn 1377 ppm and Cd 5.05 ppm. Global sample
Z-T, representative for the development area of Dystricambosols type, presents high
concentrations of Pb, 995 ppm, and lower of Cu, 96.9 ppm, Zn 127 ppm and Cd 0.50.
The migration of Zn and Cd in depth, obser ved in soil profile, is confirmed by the low
content in the global sample.
The study on the heavy metals behaviour in soil profiles from nearby of those
two smelters of copper (Zla tna) and of lead-zinc (Cop șa Mică), has demonstrated the
pH influence and that of the humus content from surface horizons on polluting these with Pb and Cu. The sudden decrease of Pb contents in soil profiles, under the horizon
rich in humus, up to normal values, indicate high stability in surface horizons,
determined by biding Pb to insoluble or ganic fractions (Angehrn-Bettinazzi et al.
1989). Soils from Cop șa Mică are characterised by excessive pollution with four
heavy metals, Pb, Cu, Zn, Cd. Arsenic is a dded to these, being analyzed in the CM-T,
global sample and its content is of 1500 ppm. The highest contents are related with the surface horizons of soil profiles.
Mobility on soil profiles has been obser ved for Zn and Cd in conditions of
weak acid to neutral pH, in relation with the increase of clay fraction, and of Fe and
Mn in Dystricambosols and Alosols, and w ith the increase of cation exchange capacity,
in the soil profiles in Zlatna area. Distribu tion of Zn and Cd in soil profiles in both
areas, from all types of soils, is variable w ith depth due to the high quantity of these
metals in total form and of the high percent of mobile form at the level of horizons from the depth. In soils from Cop șa Mică area, the conditions of neutral to alkaline pH
are favourable to biding Zn under the form of secondary compounds with iron
oxyhydroxides or under the form of anhydry silicates, which have been frequently identified in polluted soils by sme lting processes, (Manceau et al. 2002,
Kirpichtchikova et al. 2006). Retention of great quantities of Zn and Cd on surface
horizons might be in relation with the conten ts of Fe and Mn from soil profiles, taking
into consideration the moderate or reduced quantity of organic material from these
horizons and alkaline pH. Mobility on soil profil es of Zn might be also determined by
the formation of some compounds of Zn, which become soluble with the increase of pH with the depth. In Phaeozem type, re partition of Zn in comparable quantities,
between horizon A and B, is associated with equal repartition of clay fraction in the
two horizons.
79

5. ACKNOWLEDGEMENTS

This research was supported by Financial Assistance CNCSIS – National
Council of Research University in Grant c ode 138-2008. We woul d like to thank dr.
Peter Andráš from the Geological Institute, Slovak Academy of Science and from the
Department of Ecology and Environmental Education, Matej Bel University, Banská
Bystrica, Slovakia for the technical assi stance of heavy metal analyses in Cop șa Mică
Global Sample.

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Received at: 01. 09. 2008 Revised at: 08. 10. 2008
Accepted for publicatio n at: 23. 10. 2008