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  • Sunday, June 1, 2003
  • Impacts of Irrigation with Water Containing Heavy Metals on Soil and Groundwater – A Simulation Study
  • Published at:Water, Air, & Soil Pollution, Volume 146, Numbers 1-4 / June, 2003
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    IMPACTS OF IRRIGATION WITH WATER CONTAINING HEAVY

    METALS ON SOIL AND GROUNDWATER – A SIMULATION STUDY

    MOHAMMED M. AL-SUBU

     

     

    , MARWAN HADDAD, NUMAN MIZYED and

    INAYA MIZYED

    An-Najah National University, Nablus, Palestine, via Israel

    (

     

     

    author for correspondence, e-mail: [email protected])

    (Received 26 October 2000; accepted 19 December 2002)

    Abstract.

     

     

    This research work intended to study the impacts of irrigation water containing various

    levels of copper, lead, and zinc on adsorption capacity of soil packed in 4

     

     

    plastic columns and

    obtained from two locations around the city of Nablus: Salem (A) and Deir Sharaf (B). Results of

    simulation experiments showed an increase in the copper, lead, and zinc concentrations in soil and

    in leachate with increasing the amount of metal in irrigation water. Copper, lead, and zinc concentrations

    increased also with soil depth and duration of application. The results also indicate that the self

    purification of both soils was highly affected by physical factors, i.e. the intermittent application of

    irrigation water to the soils in the columns caused soil wetting and drying cycles which resulted in

    the formation of cracks in shrinked soils specially in the top half of the columns. Crack formation is

    common in such clay soils due to the climatic conditions (Mediterranean type: dry summers and wet

    winters) and type of clay minerals in the soil. Thus, short circuiting of water through cracks results

    in moving contaminants fast and deep in the soil profile.

    Keywords:

     

     

    groundwater, heavy metals, irrigation water, leachate, mediterranean climate, soil pollution

    1. Introduction

    Generally, wastewater is a liquid waste that is removed from residential, institutional

    and commercial establishments. Contaminants of domestic wastewater are

    categorized as: Disease causing microorganisms, essential plant nutrient elements,

    dissolved minerals and toxic chemicals and biodegradable organic matter (Manahan,

    1990). Discharging raw wastewater to the environment causes pollution

    problems, therefore, the treatment of wastewater is essential to enhance overall

    water availability and conserve water resources (Aziz

     

     

    et al

    ., 1996; Moatgomery,

    1988).

    Urban wastewater collection practices in Palestine are such that many small

    industries are located within municipal boundaries and drain their wastewater into

    the municipal systems. Due to scarcity of fresh water, farmers use raw wastewater

    in irrigation (Haddad, 1990, 1993). The long term use of land application as

    a disposal method of raw wastewater and/or sludge may result in limiting soils

    agricultural ability to produce (Martin Edward, 1991).

    Several studies were conducted on the toxicity of urban wastewater in Palestine

    and on its impacts on groundwater, plants and soils (Haddad, 1994; Radi

     

     

    et al

    .,

    1988; Environmental Protection, 2000; Haddad, 2000). The reported heavy metal

    concentrations of wastewater in Palestine range from 0 to 2075 mg L

     

     

    1

    for zinc,

    0 to 10 mg L

     

     

    1 for copper, and from 0 to 15 μg mL1

    for lead (Environmental

    Protection, 2000; Haddad, 2000; Haddad

     

     

    et al

    ., 1999). Zinc has the highest level

    due to the fact that galvanized steel tanks mounted on the roofs of buildings and

    houses are used in Palestine for water supply storage.

    In conventional wastewater treatment, considerable portions of heavy metals

    remain in the treated effluent if special advanced treatment is not conducted. Thus,

    long term effects of irrigation with wastewater might include pollution of ground

    water and soil with heavy metals such as: Pb, Cu and Zn ions (Lebourg

     

     

    et al

    ., 1998).

    Other impacts of treated wastewater in agriculture include the health impacts of

    possible contamination of crops by pathogenic bacteria and heavy metals (Farid

     

     

    et

    al

     

     

    ., 1993).

    There is a rapidly growing awareness of the threat to water resources caused by

    highway drainage and sewage effluents. Some of the most significant contaminants

    are heavy metals such as copper, zinc and lead (Farid

     

     

    et al

    ., 1993; Selim and

    Iskandar, 1992; Laxen and Harrison, 1977; Chatzoudis and Rigas, 1998; Mendoza

    et al

     

     

    ., 1996).

    Though copper is not a cumulative systemic poison, large dose (>100 mg) of

    copper are harmful to humans and might cause central nervous system disorder,

    failure of pigmentation of hair and adverse effects on Fe-metabolism that results

    in liver damage. Excess copper may also be deposited in the eyes, brain, skin,

    pancreas and myocardium (McAnally

     

     

    et al

    ., 1997). Lead is a cumulative poison to

    humans. Its major effects are impairment of hemoglobin and porphyries synthesis.

    Zinc cause muscular weaknesses and pain, irritability and nausea (AWWA, 1990).

    In Palestine, the availability of renewable water resources to maintain various

    human needs is poor and scarcity is accelerating with time. Therefore, alternative

    water resources development options such as brackish water desalination and the

    reuse of treated wastewater is gaining much importance at present. The use of these

    options is expected to be obligatory with time.

    The present work aims to conduct a column study to simulate Pb, Cu and Zn

    ions adsorption on soil and in leachate from two locations near the city of Nablus

    in order to recommend if these soils are suitable for wastewater application, based

    on simulation results.

    2. Methodology

    All chemicals were Analytical Grade reagents, deionized water was used for preparation

    and dilution of metal solutions. All bottles and other containers (except

    columns) were treated with 1 M HNO

     

     

    3

    solution before being washed with de

    ionized water and dried.

    2.1. E

     

     

    XPERIMENTAL SETUP

    The experimental setup consisted of 20 PVC columns, 4

     

     

    in diameter and 2 m long.

    Soil samples from the top 100 cm layer soil were collected from the two locations

    near Nablus city, Salim (A) and Deir Sharaf (B), before winter 1998. Small stones

    (if any) were removed by hand from soil samples and 19 kg of soil was mixed and

    then placed in each column in layers of 10 cm.

    To allow drainage flow freely without eroding soil from columns, a thin layer

    of gravel and sand was placed in the lower end of the column, with a plastic mesh

    screen at the bottom of the column. A plastic container was placed under each

    column to collect drainage water.

    For each soil, three treatments were carried out. These treatments represent

    simulation of irrigation for 2, 10 and 20 yr periods in triplicates. Two other columns

    were used as blanks. Rainwater was simulated for the blanks by applying 250 mL

    of rainwater to each column as needed.

    2.2. W

     

     

    ATER AND HEAVY METALS APPLICATIONS

    To each column, a solution containing known combinations of Pb

     

     

    2+, Cu2+

    and

    Zn

     

     

    2+

    was added. The concentration of each metal was estimated based on following

    (Table I):

    1. Average rainfall, evapotranspiration, crop irrigation requirements and leaching

    in Nablus area.

    2. Volume of irrigation water = 1025 mm (m

     

     

    3

    /dunum), assuming fruit trees will

    be planted in these areas.

    3. Volume of leaching water = 403 mm (m

     

     

    3

    /dunum). Considering the column

    volume, the volume of irrigation water for simulation was 8.05 L per column

    per year.

    2.3. W

     

     

    ATER APPLICATION

    Two, 10 and 20 yr were selected for simulation to study short, medium and long

    terms’ effects of simulation. Details are found in Table I.

    2.4. H

     

     

    EAVY METAL APPLICATION

    Metal solutions were prepared from their nitrate salts and stored in polyethylene

    bottles.

    The amount of heavy metals applied in irrigation was based on the maximum allowable

    limit by FAO (10, 5 and 10 mg L

     

     

    1 for Zn2+, Cu2+ and Pb2+

    , respectively)

    (FAO, 1980). Details are shown in Table I.

    TABLE I

    Water and heavy metal application in both soils

     

     

    a

    Description Years

    1 2 10 20

    Depth of irrigation water (mm) 1025 2050 10250 20500

    Depth of leachate water (mm) 403 806 4030 8060

    Volume of irrigation water (L/column) 8.05 16.1 80.5 161

    Volume of leachate water (L/column) 3.17 6.34 31.7 63.4

    Weight of zinc added to each column (mg) 80.5 161 805 1609

    Weight of copper added to each column (mg) 40.25 80 402 805

    Weight of lead added to each column (mg) 80.5 161 805 1609

    Duration (from 28-12-1998 to 23-4-1999 8-5-1999 19-5-1999

    a

     

     

    Humidity was 49–69% and pan evaporation was 2.4–7.8 mm day1

    .

    2.5. L

     

     

    EACHATE

    Water leaching from the columns drained into the plastic containers under the

    columns. To illuminate evaporation of drainage water, the containers were covered

    by plastic sheets. Depth of drainage water in the collection containers was monitored

    and when it reach about 10–15 cm (this depth equals the height of the small

    layer of gravel and sand in the bottom of each column), water was collected and

    transferred into storage containers. Storage containers were polyethylene bottles of

    4 L in volume. To each storage bottle, 10 mL of 1 M HNO

     

     

    3

    has been added.

    2.6. M

     

     

    ETALS IN SOIL

    Metal concentrations in each soil were measured before treatment. After simulation

    was finished, soil was evacuated from the PVC column, which was cut into three

    pieces or 4 cross sections at 10, 67, 133 and 200 cm heights. Each soil patch was

    dried and the metal ions were extracted from a given weight using NH

     

     

    4

    Ac/EDTA

    solutions. The extracts were then analyzed for Pb, Zn and Cu ions. Extractable ions

    were determined as this research is concerned with the amounts adsorbed on soil

    surfaces which could be a fraction of total amounts of metals in the soil. Adsorbed

    metals influence plant and environment as they interact with soil solution and plant

    roots.

    2.7. S

     

     

    OIL ANALYSIS

    Soils were analyzed for chloride, carbonate, sodium, potassium, magnesium, calcium,

    copper, zinc, lead, phosphorus, total dissolved salts (TDS), organic matter

    content and pH according to standard procedure (Laboratory Manual, 1992; Reeve,

    1994). Concentrations of chlorides, sodium, potassium, magnesium and copper

    were determined in soil extracts. Concentrations of zinc, lead and copper were

    determined from extracts by NH

     

     

    4

    Ac/EDTA.

    Moisture content, particle size distribution, bulk density and specific gravity of

    soils were also measured following standard methods (Das Braja Soil Mechanics,

    1941).

    2.8. I

     

     

    NSTRUMENTATION

    Analysis of Cu, Zn, and Pb were carried out by atomic absorption spectrophotometry

    using Atomic Absorption Spectrophotometer VIDEO 11, which was calibrated,

    using supplied standards, prior to each use. Electrical conductivity was

    measured using Conductivity Meter 4010 instrument. pH was recorded using a

    Corning pH Meter Model 12.

    3. Results and Discussion

    3.1. C

     

     

    HEMICAL ANALYSIS

    Results of soil chemical analysis are shown in Table II. The concentration of total

    dissolved solids (TDS) and electrical conductivity readings were low for both soils,

    which indicate that neither soil is saline (FAO, 1980; McNeal

     

     

    et al

    ., 1982). It also

    indicate that the average precipitation in the area of 600 mm yr

     

     

    1

    is sufficient with

    time to wash salts from soil especially that both soils showed low sodicity and good

    permeability, in spite of soil clay nature.

    The conductivity readings are supported by the low concentration found for

    calcium, magnesium, potassium, sodium, copper, zinc, lead, phosphorous chlorides

    and nitrates. For all cations and anions tested, the found concentration was below

    the acceptable limits of agricultural soil.

    The relatively high percentage composition of calcium carbonates in soil (13–

    20%) is attributed to the fact that parent materials of these soils were originated

    from rocks rich in calcium carbonates such as limestone and dolomite. The soil pH

    (7–8) and the high buffer capacity make soils suitable for most plants, as the nutrient

    availability of most macronutrient is high at this pH, though some micronutrient

    such as iron and manganese demand more acidic soil.

    The low sodicity resulting from low sodium carbonate content indicates that

    both soils were not alkaline (pH < 8.3) (Schwab

     

     

    et al

    ., 1993). The high calcium

    carbonate content and the low exchangeable sodium on the surfaces of these soils

    result in the formation of highly stable aggregates with suitable permeability and

    hence good drainage ability (Sposito, 1989).

    TABLE II

    Chemical and physical analysis of soil

    Type of analysis Salim Deir Sharaf

    Electric conductivity of soil extract (mmho cm

     

     

    1

    ) 1.2 1.3

    Total dissolved solids for soil extracts (mg g

     

     

    1

    ) 3.84 4.16

    Soil extract pH 7.29 7.11

    Chlorides in soil extract (

     

     

    μg g1

    ) 87.5 175

    Calcium and magnesium in soil extract (meq L

     

     

    1)a

    11.5 10

    % Organic matter content 2 12

    Phosphorous in soil extract (

     

     

    μg g1

    ) 460 240

    Potassium in soil extract (

     

     

    μg g1

    ) 140 180

    Sodium in soil extract (

     

     

    μg g1

    ) 1140 880

    % CaCO

     

     

    3

    13.75 20

    Copper extracted by NH

     

     

    4Ac/EDTA (μg g1

    ) 4.84 2.52

    Zinc extracted by NH

     

     

    4Ac/EDTA (μg g1

    ) 2.86 1.24

    Lead extracted by NH

     

     

    4Ac/EDTA (μg g1

    ) 2.66 0.94

    % Moisture content 9.4 8.5

    Specific gravity (gm cm

     

     

    3)

    2.6 2.7

    Bulk density (gm cm

     

     

    3

    ) 1.7 1.8

    % Silt 43.2 41.6

    % Clay 37.6 35.6

    % Sand 19.2 22.8

    Soil texture Clay loam Clay loam

    a

     

     

    5.0 g dry soil was extracted with 100 mL NH4

    Ac (1 N).

    3.2. P

     

     

    HYSICAL ANALYSIS

    Due to the formation of aggregates, sieve analysis was not suitable to determine soil

    texture. Therefore, hydrometer analysis was utilized and results are summarized in

    Table II.

    Soil from both locations was found to contain high clay percentage and classified

    as clay loam soil based on textural triangle (Beaton

     

     

    et al

    ., 1975; Fitzpatrick,

    1986). Both sites from which soil was collected are located within alluvial plains

    of wadis. The low erosion in these plains and the high annual precipitation allow

    the formation of clay. However, medium weathering rates are characteristics of

    the environmental conditions of the area in these plains. These conditions result in

    forming montmorollinite clay minerals in the area. This could be easily observed

    in the Plains of the West Bank and the response of soils there to the weather conditions.

    The most common response of such clay minerals is the formation of cracks

    in summer (dry weather) and the expansion of soils in winter (wet weather). Depth

    of these cracks exceeds 1 m in these soils and might reach several meters in some

    deep soil profiles due to the long dry summer which might exceed 6 months. The

    soil bulk density is high due to shrinkage and formation of aggregates during the

    long months of the dry hot summer season. However, the specific gravity of soil

    particles is typical for such soils with calcium carbonates parent materials.

    3.3. S

     

     

    OIL ANALYSIS AFTER SIMULATION

    Application of heavy metals was carried out to simulate their impact on soil and

    leachate.

    The concentrations of metals were analyzed before and after the simulation

    experiment and the results are presented in Table III.

    Because the industrial zone is located in the eastern side of Nablus City, Soil A

    was more polluted with the three heavy metals than in Soil B.

    After simulation experiments, soil samples were taken from columns at different

    depths (10, 67, 133 and 200 cm), thereafter analyzed for copper, zinc and lead

    content (Table III).

    For all metals employed in the three terms of treatments, the metal concentration

    increased with depth. This could be attributed to one or more of the following

    factors:

    1. The experimental setup allows better ion exchange between applied solution

    and soil particles in the lower part of the column.

    2. The applied metal concentrations could be low enough to be washed by the

    running water of irrigation.

    3. The possibility of short circulating on the walls of the PVC column and through

    the soil cracks due to wetting and drying conditions and thus preventing ion

    exchange between soil and applied solution in the upper part of the column.

    Heavy metals residue was calculated for each element in each column (Table IV).

    In all cases, the residue increased with increasing the concentration of metal applied

    and simulation period. This indicates that heavy metals application in irrigation

    water is accumulative. However, Soil A retained more heavy metals than

    Soil B.

    Although the present results show an increase in heavy metals concentrations

    with depth, the actual increase in the field might be different as a result of different

    evapotranspiration rates from different soil layers depending on plant physiology

    and distribution of plant roots.

    3.4. L

     

     

    EACHATE ANALYSIS

    Figure 1 shows the changes in electrical conductivity of soil with time for the long

    term treatment for both soils. The electrical conductivity of soil was enhanced with

    duration of treatment whereas salinity decreased.

    TABLE III

    Concentrations of copper, zinc and lead in soil at different depths at the end of simulation

    period

    Column Residue concentration in soil batches (

     

     

    μg g1

    ) Total

    Lower Middle Upper (mg)

    Cu

    2 yr Salim 11.111.07 3.630.46 3.450.12 115.149.77

    D. Sharaf 10.000.07 2.030.16 2.250.08 90.481.53

    10 yr Salim 37.610.47 4.450.58 3.570.59 288.979.84

    D. Sharaf 36.490.77 3.030.74 2.670.84 267.2713.6

    20 yr Salim 81.610.81 5.031.13 4.500.82 577.1811.70

    D. Sharaf 78.670.19 3.381.02 2.830.55 53057 9.38

    Zn

    2 yr Salim 19.890.36 1.670.22 1.800.16 147.9 2.91

    D. Sharaf 17.410.99 0.990.41 0.840.34 121.9 5.07

    10 yr Salim 93.941.35 2.040.15 1.870.27 619.7 9.91

    D. Sharaf 91.291.05 1.300.05 1.090.15 593.3 5.93

    20 yr Salim 181.331.85 4.150.06 2.290.22 1189.2 13.43

    D. Sharaf 170.137.99 1.850.49 1.430.17 1089.2 21.25

    Pb

    2 yr Salim 18.610.99 2.510.08 2.290.05 148.2 5.8

    D. Sharaf 17.750.62 1.750.66 1.370.17 132.2 8.1

    10 yr Salim 90.690.72 3.530.08 3.040.17 615.9 4.79

    D. Sharaf 88.970.71 2.030.24 1.590.30 586.4 1.40

    20 yr Salim 184.600.53 5.570.81 3.360.26 1225.7 6.89

    D. Sharaf 176.6411.29 2.750.32 2.090.30 1149.4 68.52

    The amount of heavy elements in leachate (Table IV) was also dependent on the

    simulation period as expected. However, no significant difference in the amount of

    heavy elements was found in leachate from the two soils. This could result from

    similar physical and chemical characteristics of the two soils. Therefore their selfpurification

    capacities are also similar. The threat to groundwater, if happens, will

    rather depend on the hydrogeological characteristics of the two areas.

    Mass balance of metal requires that the added amount in irrigation water plus

    that present initially in soil, should equal to the metal residue in soil plus that in

    TABLE IV

    Mass balance of copper, zinc and lead

    Actual Mass balance calculations

    Initial Applied Leachate Residue

    (mg) (mg) (mg) (mg)

    Cu

    2 yr Salim 115.14 91.96 80.00 2.21 169.75

    D. Sharaf 90.48 47.88 80.00 3.25 124.64

    10 yr Salim 288.97 91.96 402.00 38.45 455.51

    D. Sharaf 267.27 47.88 402.00 39.43 410.45

    20 yr Salim 577.18 91.96 805.00 45.12 845.23

    D. Sharaf 537.57 47.88 805.00 46.61 806.27

    Zn

    2 yr Salim 147.9 54.37 161 1.01 214.36

    D. Sharaf 121.9 23.55 161 1.41 183.14

    10 yr Salim 619.7 54.37 805 17.07 842.30

    D. Sharaf 593.3 23.55 805 18.12 810.43

    20 yr Salim 1189.2 54.37 1609 66.33 1597.0

    D. Sharaf 1098.2 23.55 1609 82.32 1550.2

    Pb

    2 yr Salim 148.2 50.578 161 0.61 210.96

    D. Sharaf 132.2 17.805 161 1.01 177.80

    10 yr Salim 615.9 50.578 805 19.08 836.49

    D. Sharaf 586.4 17.805 805 19.67 805.88

    20 yr Salim 1225.7 50.578 1609 33.18 1623.1

    D. Sharaf 1149.4 17.805 1609 34.26 1592.5

    leachate (Table IV). The difference between the amount of metal found by mass

    balance calculations and that found experimentally in soil, especially for two years

    treatment could be explained by one or more of the followings:

    1. Precipitation of metal ions as insoluble salts.

    2. Adsorption of heavy metals on the columns’ surfaces.

    3. The variation in temperature during the experimental period.

     

    Figure 1.

     

     

    Electric conductivity (mmho cm1

    ) of the leachate versus date of experiment for the 20 yr

    term treatment.

    4. Conclusions

    The two soils were found to have similar chemical and physical properties and thus

    showed similar response to simulation experiments.

    The nature of metal, soil properties and the metal loading level affected redistribution

    of metals in soil. The three metals used showed cumulative effect on soil

    and in leachate, and thus the possibility of groundwater contamination does exist.

    The concentrations of these elements and other heavy metals should be reduced as

    much as possible and industrial waste should be either separated or treated before

    dumped in domestic wastewater.

    The clay nature of soils and their high content of montmorollinites were responsible

    for the formation of large and deep cracks due to wetting and drying

    weather conditions. As a result, cation exchange between soil and running solution

    was not allowed which reduces self-purification capacity of soil. Continuous

    monitoring of wastewater, soil and groundwater qualities are essential for any

    sustainable reuse of wastewater in Palestine.

    Acknowledgements

    Authors are thankful to An Najah N. University for financial support of the present

    work.

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

     

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