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Transcript of Groundwater Depletion
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Long-term impact of irrigation with sewage effluents on heavymetal content in soils, crops and groundwatera case study
R.K. Rattan a,*, S.P. Datta a, P.K. Chhonkar a, K. Suribabu a, A.K. Singh b
aDivision of Soil Science and Agricultural Chemistry, Indian Agricultural Research Institute, New Delhi 110012, Indiab Water Technology Centre, Indian Agricultural Research Institute, New Delhi 110012, India
Received 15 September 2004; received in revised form 3 February 2005; accepted 22 February 2005
Abstract
There is a gradual decline in availability of fresh water to be used for irrigation in India. As a consequence, the use of sewage
and other industrial effluents for irrigating agricultural lands is on the rise particularly in peri-urban areas of developing
countries. On the other hand, there is increasing concern regarding the exceedance of statutory and advisory food standards for
trace metals throughout the world. Hence, a case study was undertaken to assess the long-term effect of sewage irrigation on
heavy metal content in soils, plants and groundwater. For this purpose, peri-urban agricultural lands under Keshopur Effluent
Irrigation Scheme (KEIS) of Delhi, India were selected where various cereals, millets, vegetable and fodder crops have
successfully been grown. Sewage effluents, ground water, soil and plant samples were collected and analysed mainly for metal
contents. Results indicated that sewage effluents contained much higher amount of P, K, S, Zn, Cu, Fe, Mn and Ni compared togroundwater. While, there was no significant variation in Pb and Cd concentrations in these two sources of irrigation water and
metal content were within the permissible limits for its use as irrigation water. There was an increase in organic carbon content
ranging from 38 to 79% in sewage-irrigated soils as compared to tubewell water-irrigated ones. On an average, the soil pH
dropped by 0.4 unit as a result of sewage irrigation. Sewage irrigation for 20 years resulted into significant build-up of DTPA-
extractable Zn (208%), Cu (170%), Fe (170%), Ni (63%) and Pb (29%) in sewage-irrigated soils over adjacent tubewell water-
irrigated soils, whereas Mn was depleted by 31%. Soils receiving sewage irrigation for 10 years exhibited significant increase in
Zn, Fe, Ni and Pb, while only Fe in soils was positively affected by sewage irrigation for 5 years. Among these metals, only Zn in
some samples exceeded the phytotoxicity limit. Fractionation study indicated relatively higher build-up of Zn, Cu, Fe and Mn in
bioavailable pools of sewage-irrigated soils. By and large, tissue metal concentrations in all the crops were below thegeneralized
critical levels of phytotoxicity. Based on the soil to plant transfer ratio (transfer factor) of metals, relative efficiency of some
cereals, millet and vegetable crops to absorb metals from sewage and tubewell water-irrigated soils was worked out. Risk
assessment in respect of metal contents in some vegetable crops grown on these sewage-irrigated soils indicated that thesevegetables can be consumed safely by human.
# 2005 Elsevier B.V. All rights reserved.
Keywords: Long-term sewage irrigation; Heavy metals; Soils; Groundwater; Crops; Hazard quotient
www.elsevier.com/locate/agee
Agriculture, Ecosystems and Environment 109 (2005) 310322
* Corresponding author. Tel.: +91 11 25841991; fax: +91 11 25841529.
E-mail address: [email protected] (R.K. Rattan).
0167-8809/$ see front matter # 2005 Elsevier B.V. All rights reserved.
doi:10.1016/j.agee.2005.02.025
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1. Introduction
India supports more than 16% of the worlds
population with only 4% of the worlds fresh waterresources (Singh, 2003). Although agriculture sector in
this country has been major user of water, share of
water allocated to irrigation is likely to be decreased by
1015% in next two decades (CWC, 2000). In this
changing scenario, reuse of domestic and industrial
waste water in agriculture for irrigating crops appears
to be a lucrative option. Besides being source of
irrigation water, these waste waters contain appreciable
amounts of plant nutrients. In India, total waste water
generated per annum from 200 cities is about
2600 Mm3 (Kaul et al., 1989) and also the use of
sewage effluents for irrigating agricultural lands is on
the rise especially in the peri-urban area. These waste
waters carry appreciable amounts of trace toxic metals
(Feign et al., 1991; Pescod, 1992; Som et al., 1994;
Gupta et al., 1998; Brar et al., 2000; Yadav et al., 2002)
and concentrations of trace metals in sewage effluents
vary from city to city (Rattan et al., 2002). Although the
concentration of heavy metals in sewage effluents are
low, long-term use of these waste waters on agricultural
lands often results in the build-up of the elevated levels
of these metals in soils (Rattan et al., 2002). Extent of
build-up of metals in waste water-irrigated soilsdepends on the period of its application (Bansal
et al., 1992; Palaniswami and Sree Ramulu, 1994).
Crops raised on the metal-contaminated soils accu-
mulate metals in quantities excessive enough to cause
clinical problems both to animals and human beings
consuming these metal rich plants (Tiller, 1986). Since
food chain contamination is one of the major routes for
entry of metals into the animal system, monitoring the
bioavailabile pools of metals in contaminated soils has
generated a lot of interest (Datta et al., 2000; Yadav
et al., 2002). Also information on the fractionation oftrace metals in soils is potentially valuable in predicting
bioavailability, metal leaching rates, and transforma-
tion between chemical forms in agricultural and
polluted soils (Jenne and Louma, 1977; McBride,
1981; Miller et al., 1986). But such information on
agricultural lands receiving sewage irrigation for quite
a long time is meagre.
Crop species exercise differentiality in accumulat-
ing metals in their tissue (Lepp, 1981; Datta et al.,
2000) and ef ficiency of different crops in absorption of
metals is judged either by plant metal uptake or by
transfer factor of metals from soil to plants. Uptake of
metals by plants may be a good indicator of efficiency
of metal absorption of different crop species grown onsoils having uniform metal levels under controlled
conditions. Whereas, transfer factor of metal from soil
to plants indicates the efficiency of crop species better
where crops are grown on soils having variable metal
contents, e.g. farmers fields. Generally, soil to plant
transfer factor of metals is computed based on total
metal contents of soils (Hooda et al., 1997). However,
total metal content in soils does not take into account
the other soil factors that modify the bioavailability of
metals. Hence, computation of soil to plant transfer
factor of metals should be based on available soil
metal pools.
We attempted to study some of the above-
mentioned aspects in sewage-irrigated peri-urban
agricultural lands under Keshopur Effluent Irrigation
Scheme (KEIS) of the Delhi Government, India. Under
this scheme, sewage irrigation has been provided to the
farmers fields for more than two decades. Various
cereals, millet, leafy vegetables and fodder crops have
successfully been grown thereon. No investigation has
been carried out in sewage-irrigated soils of this peri-
urban area except one where we reported the build-up
of some of major and secondary plant nutrients in soilsas a result of sewage irrigation (Rattan et al., 2001).
The objectives of this study were: (i) to study the
chemical composition of sewage effluents emanating
from KEIS and groundwater; (ii) to assess the effects of
long-term irrigation with sewage effluents on metal
contents in soils and plants; and (iii) to assess the risk of
consuming leafy green vegetables in respect of their
heavy metal contents grown on sewage-irrigated soils
to human beings.
2. Materials and methods
2.1. Study area and collection of samples
The study area is located in the western Delhi, India,
where sewage effluents originating from Keshopur
Sewage Treatment Plant have been used for irrigation
purposes since 1979 (Fig. 1). Our study confined to six
villages, viz. Nilothi, Mundka, Ranhola, Bakarwala,
Hirankudna and Dichaonkalan covering 123, 233, 196,
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775, 183 and 98 acres of agricultural lands,respectively.
Agricultural lands offirst four villages have been under
sewage irrigation for 20 years, while in Hirankudna and
Dichaokalan, crops have been irrigating with sewage
effluents for 10 and 5 years, respectively. Sewage
effluents were collected periodically from 13 locations
spread over these six villages under study. Similarly,
groundwater samples were also collected from eight
tubewells located in these villages. First sampling wasdone on 17 January 2002 and subsequently three more
samplingswerecarriedouteachattwomonths interval.
WithactivesupportoftheRevenueOfficialsoftheDelhi
government and local farmers, land in each village was
divided into two categories, viz. sewage and tubewell
water-irrigated. Tubewell water-irrigated landswere the
ones inaccessible for sewage irrigation because of their
slight higher elevation. In all, 431 and 106 soil samples
(015 cm) were collected from sewage and adjacent
tubewell water-irrigated lands, respectively. From
sewage-irrigated sites of Nilothi, Ranhola, Mundka,
Bakarwala, Hirankudna and Dichaokalan 37, 62, 57,
213, 39 and 23 soil samples werecollected,respectively,
the corresponding number of soil samples collected
fromadjacenttubewellwater-irrigated siteswere 11, 12,
6,51,10and16.Plantsamplesofcropsgrownonsewage
and tubewell water-irrigated lands were also collected
from the soil sampling sites wherever available.
2.2. Chemical analysis of sewage effluents,
groundwater, soil and plant samples
An aliquot of 500 mL of sewage effluents and
groundwater samples with 15 mL of HNO3 was
evaporated to near dryness on a hot plate. Then
contents were digested with 15 mL of HNO3 and
20 mL HClO4 (70%) (Brar et al., 2000). The residue
was taken in 15 mL of 6N HCl and made to the volume
(50 mL) and contents were filtered. The filtrate was
R.K. Rattan et al. / Agriculture, Ecosystems and Environment 109 (2005) 310322312
Fig. 1. Map showing the area under Keshopur Effluent Irrigation System commissioned in 1979.
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analyzed for P, K, S, Zn, Cu, Fe, Mn, Ni, Pb and Cd
using inductively coupled plasma-atomic emission
spectrophotometer (ICP-AES). Sewage effluent sam-
ples were analyzed for pH and electrical conductivityusing pH meter and solu-bridge, respectively. Carbo-
nates and bicarbonates were estimated by titrating an
aliquot of effluent samples with H2SO4. Soil samples
were dried, ground and passed through 2 mm sieve.
Soil pH was measured in suspension (soil:water::1:2)
according to Datta et al. (1997). Organic carbon
contents in soil were determined by the wet digestion
method (Walkley and Black, 1934). Further, 30 soil
samples across the villages were selected and analysed
for texture by hydrometer method (Day, 1965). For
heavy metal analysis, the soil samples were extracted
with 0.005 M DTPA according to Lindsay and Norvell
(1978) and metals in the extract were determined with
help of atomic absorption spectrophotometer (AAS;
GBC 932). In all, nine surface (015 cm) soil samples
were selected from sewage effluent-irrigated lands
receiving effluent irrigation for last 20 years and three
soil samples were also selected from adjacent tubewell
water-irrigated lands. These soil samples were used
for sequential extraction of Zn, Cu, Fe and Mn
according to the scheme of Iwasaki and Yoshikawa
(1990) which is modified form of fractionation scheme
of Miller et al. (1986). Plant samples were dried at60 8C in hot air oven, ground and digested in a diacid
mixture (HNO3:HClO4::9:4) (Jackson, 1973). Metal
contents in the plant digests were determined on
AAS.
2.3. Metal transfer factor
Soil to plant metal transfer factor was computed as
ratio of the concentration of metal in plants (on dry
weight basis) to its DTPA-extractable metal contents
in soil.
2.4. Risk assessment
Risk to human health (Hazard Quotient, HQ) for
intake of Zn, Cu and Ni through consumption spinach
(Brassica oleraceae), gobhi sarson (Brassica napus)
and Indian rape (Brassica campestris) as green leafy
vegetables grown on sewage-irrigated soils was
calculated using the following relationship (Pier-
zynski et al., 2000):
HQgv = (add/RfD), where HQgv is the hazard
quotient to a human from consumption of green
vegetables, add: the average daily dose (mg metal/kg
body weight/day) and RfD the reference dose. Thevalues of RfD for Zn and Ni were used as 0.3 and
0.02 mg/kg bw/day, respectively (IRIS, 2003). For Cu,
value of provisional maximum tolerable daily intake is
0.5 mg/kg bw/day (WHO, 1982) and the same is used
as RfD (Alam et al., 2003). Daily intake of green
vegetable was considered as 200 g/person/day which
is recommended amount from nutritional point of
view (Hassan and Ahmed, 2000). A factor of 0.085
was used to convert the fresh to dry weight of these
green vegetables. Average body weight for an adult
was considered as 70 kg. Average daily dose (add) was
computed using following relationship:
add mc cf di
bw
where mc is the metal concentrations in plant
(mg kg1) on dry weight basis, cf the fresh to dry
weight conversion factor, di the daily intake of green
vegetable (kg) and bw the body weight (kg). Assess-
ment of risk as computed here is not complete since,
metal accumulation to soil organisms, groundwater,
surface water, direct uptake of soil by human and
animal are some of the other risks which have not beenconsidered here.
2.5. Statistical analysis
The differences between DTPA-extractable metal
contents in sewage and tubewell water-irrigated soils
were statistically evaluated by applying t-test accord-
ing to Snedecor and Cochran (1967). Simple correla-
tion and multiple regression analyses were also carried
out to assess the relationships of DTPA-extractable
metal with plant metal concentration, soil pH andorganic carbon.
3. Results and discussion
3.1. Physico-chemical properties of sewage
effluents and groundwater
Plant nutrients and heavy metal contents in sewage
effluents and groundwater samples of first sampling
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are presented in Table 1. Data for second, third and
fourth sampling were not shown, since similar values of
these elements were obtained except S. In first
sampling, on an average, P, K, and S contents were
0.22, 3.58 and 14.3 mg L1, respectively in ground-
water samples, whereas, corresponding values for
sewage effluents were 2.57, 11.7 and 15.9 mg L1.
Among these plant nutrients, sewage effluents con-
tained about 12 and 3 times more P and K, respectively
compared to ground water. Sulphur contents in sewage
effluents in second, third and fourth sampling were
about two- to three-folds higher than that of ground-water. On an average, sewage effluents contained 5.5,
3.6, 2.6, 6.4 and 1.3 times higher amounts of Zn, Cu, Fe,
Mn and Ni, respectively compared to groundwater.
There were no appreciablevariations between these two
sources of irrigation water in respect of Pb and Cd. The
sewage effluents contain appreciable amounts of useful
major plant nutrients, viz. P, K and S, which was also
reflected in the appreciable build-up of these nutrients
in sewage-irrigated soils of this study area (Rattan et al.,
2001). According to Pescod (1992), threshold values of
heavy metals in irrigation water leading to crop damageare 2000 mg L1 for Zn, 200 mg L1 for Cu,
5000 mg L1 for Fe, 200 mg L1 for Mn, 200 mg L1
for Ni, 5000 mg L1 for Pb and 10 mg L1 for Cd.
Although sewage effluents had elevated concentrations
of some of the metals compared to groundwater, the
concentrations of these metals in these two sources of
irrigation water were within the permissible limits for
their use as irrigation water.
Some additional physico-chemical parameters
were determined in sewage effluent samples. Results
indicate that sewage effluents were acidic in reaction
with pH values ranging from 5.8 to 6.5 (data not
shown). The tolerance limit of pH for irrigation water
ranged from 6.0 to 9.0 (Patel et al., 1990). Thus, pH ofall the effluent samples is within the permissible limit.
Electrical conductivity of sewage effluents in all
samples exceeded 1 dS m1 (1.362.88 dS m1) indi-
cating that these effluents were saline in nature. The
carbonate and bicarbonate contents in effluent samples
varied from traces to 0.8 and 4.4 to 9.8 me L1,
respectively. Carbonate concentrations in all the
samples were much lower as compared to bicarbonate
concentrations, which is also reflected in acidic
reaction of effluents. The values of residual sodium
carbonate (RSC) varied from traces to 1.2, i.e. RSC in
all the samples were below 1.25 me L1 (safe limit for
irrigation water). These effluents can safely be used
for irrigation purpose as far as RSC is concerned.
3.2. Soil texture
Mechanical analysis of soil samples indicated that
sand and silt contents ranged from 56 to 86 and 8 to
28%, respectively, while maximum 18% clay was
recoded. Out of 30 samples analysed, 7 samples
belong to loamy sand and 23 samples were classified
as sandy loam. Thus, it is obvious that soils of thisstudy area are coarse to moderately coarse in texture.
3.3. Effect of long-term use of sewage effluents
3.3.1. Soil pH and organic carbon
Across the villages, soil pH varied from 5.1 to 9.9
and 6.2 to 9.1 in sewage and tubewell water-irrigated
soils, respectively with the corresponding average
values of 7.5 and 7.9 (data not shown). On an average,
soil pH was dropped by 0.4 unit. The organic carbon
content varied from 0.14 to 3.71% (average 0.65%) insewage-irrigated soils, the corresponding values for
tubewell water-irrigated soils were 0.140.76 (average
0.39%) (data not shown). Thus, organic carbon was
increased by 59% as result of long-term sewage
irrigation. These results concurred the findings of
Singh and Verloo (1996). After pH, soil organic
carbon (SOC) is the most important indicator of soil
quality and in addition to acting as a store-house of the
plant nutrients, plays a major role in nutrient cycling.
Besides, some estimates show that increase in the SOC
R.K. Rattan et al. / Agriculture, Ecosystems and Environment 109 (2005) 310322314
Table 1
Plant nutrients and heavy metals content in sewage effluents and
groundwater collected at first sampling
Element Sewage ef fluents Groundwater
P (mg L1
) 0.565.91 (2.57) 0.110.36 (0.22)
K (mg L1
) 9.3323.1 (11.7) 0.845.03 (3.58)
S (mg L1) 7.7122.9 (15.9) 9.8519.4 (14.3)
Zn (mg L1
) 6151 (61) 338 (11)
Cu (mg L1
) 9116 (29) 79 (8)
Fe (mg L1
) 6393793 (1464) 100745 (557)
Mn (mg L1
) 24122 (64) 115 (10)
Ni (mg L1) 3967 (49) 955 (37)
Pb (mg L1
) 2267 (33) 2241 (30)
Cd (mg L1
) 1.172.44 (1.53) 1.071.76 (1.42)
Figures in parenthesis indicate the mean values.
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content by 0.01% could lead to the carbon sequestra-
tion equal to the annual increase in the atmospheric
CO2-C (Lal et al., 1998). Such a long-term application
of the sewage effluents is a carbon-building/seques-tering and soil quality sustaining practice. Farmers of
the area have expressed that over a period of time, the
soils, which were not productive (because of the
problems of Kallarsodicity) had started giving
improved yields. Such an observation could be
explained on the basis of counteraction of alkalinity
through sewage-induced acidification and improve-
ment in soil organic carbon status.
3.3.2. Heavy metals in soils
In Nilothi, Ranhola, Mundka and Bakarwala, there
were substantial build-up of DTPA-extractable Zn,
Cu, Fe, Pb and Ni in sewage-irrigated soils over
tubewell water-irrigated ones (Table 2). Whereas, Mn
contents in soils of Nilothi, Mundka, Bakarwala were
declined by 44, 18 and 51%, respectively, as a result of
sewage irrigation. In Hirankudna, on an average,
sewage irrigation resulted in 113, 117, 29 and 81%
increase Zn, Fe, Pb and Ni, respectively, however, Cu,
Mn and Cd did not show any significant change.
Significant effect of irrigation through sewage water
was only observed in case of Fe, where 254% increase
was recorded over the tubewell water-irrigated soils ofDichaonkalan. Cadmium content was not affected by
sewage irrigation except in soils of Mundka.
To assess the impact of duration under sewage
irrigation, build-up of heavy metals in soils was
computed separately for villages receiving irrigation
for 20, 10 and 5 years (Fig. 2). In soils of Dichaokalan,
which has been under sewage irrigation for 5 years, on
average 254% build-up in Fe content was recorded and
corresponding values for Hirankudna which has been
receiving sewage irrigation for 10 years was 117%.
Whereas, as a result of sewage irrigation for 20 years,Fe increased by 170% in soils of Nilothi, Ranhola,
Mundka and Bakarwala. Zinc was not affected by
sewage irrigation for 5 years, while 113 and 208%
increases were observed in soils under sewage
irrigation for 10 and 20 years, respectively. Significant
build-up in Cu was recorded under sewage irrigation
of 20 years only, value being 170%. Sewage irrigation
for 10 and 20 years increased the Ni contents in soils
by 81 and 63%, respectively and corresponding values
for Pb in both the cases was 29%. However, sewage
irrigation for 5 years could not change the available
pool of both of these metals. Although 5 and 10 years
of sewage irrigation could not change the Mn content
in soil significantly, on an average 31% decline wasrecorded in soil which has been receiving sewage
irrigation for 20 years.
In case of Nilothi and Dichaonkalan, average
DTPA-extractable Fe content in the tubewell-irrigated
soils is below the critical limit of deficiency of
4.5 mg kg1 (as suggested by Lindsay and Norvell,
1978 and used extensively in India for delineating Fe-
deficient soil), increased more than three to five times
in the sewage-irrigated soils. It leads one to logically
conclude that the enhancement of crop productivity in
the sewage-irrigated soils of this village could partly
be due to alleviation of Fe-deficiency syndrome. In
other four villages, i.e. Mundka, Ranhola, Bakarwala
and Hirankudna, there has been an enormous build-up
in the available Fe content in the sewage-irrigated
soils. Since Fe does not cause phytotoxicity in neutral
to alkaline soils of this area, the build-up of available
Fe is not likely to limit the use of sewage effluents for
irrigation purpose. The sewage-irrigated soils are still
maintaining higher levels of DTPA-Mn than the
critical limit of Mn deficiency of 2.0 mg kg1 (being
used currently in this country for separating the Mn-
deficient soils from the non-deficient ones); however,this is a cause of concern and steps need to be
undertaken to monitor Mn deficiency and include Mn
in the fertilization schedule.
All the soils, both under tubewell and sewage
irrigation are well supplied with Zn and Cu as their
levels are generally higher than their critical levels of
deficiency of 0.6 and 0.20.5 mg kg1, respectively.
In case of the sewage-irrigated soils, some of the soils
have accumulated more than 10 mg kg1 DTPA-Zn,
which has been listed as critical level of phytotoxicity
(Rattan and Shukla, 1984). Accumulation of Zn andCu in soils coupled with decrease in soil pH has a
potential of aggravating the nutritional disorders
associated with toxicity of these metals in the long run.
3.3.3. Fractionation
In view of appreciable build-up in DTPA-
extractable Zn, Cu and Fe and depletion in Mn,
distribution of these metals in different soil pools
were studied and presented in Table 3. In tubewell
water-irrigated soils, lower proportions of Zn were
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R.K. Rattan et al. / Agriculture, Ecosystems and Environment 109 (2005) 310322316
Table 2
Effect of long-term irrigation with sewage effluent on the DTPA-extractable heavy metal status of soil (mg kg1)
Metals Sewage-irrigated Tubewell-irrigated
Range Mean S.D. # (%) Range Mean S.D.Nilothi
Zn 2.5218.6 7.31** 4.14 638 0.531.84 0.99 0.34
Cu 1.9411.9 4.91** 2.60 416 0.651.23 0.95 0.18
Fe 8.4841.6 20.1** 9.13 554 1.784.04 3.08 0.63
Mn 1.308.26 3.29** 1.45 44 4.596.95 5.87 0.99
Cd 0.110.37 0.20 0.06 0.070.44 0.14 0.10
Pb 1.252.58 1.91** 0.38 46 0.661.96 1.31 0.44
Ni 0.062.46 1.19** 0.70 284 0.090.67 0.31 0.20
Ranhola
Zn 1.5636.9 9.28** 9.27 189 1.107.50 3.21 2.01
Cu 2.2632.3 7.04** 4.96 162 1.364.13 2.69 1.16
Fe 8.6576.8 43.1** 18.57 214 4.8534.2 13.7 9.08
Mn 1.5810.7 4.19 1.87 1.524.79 3.82 1.05Cd 0.050.41 0.15 0.07 0.080.24 0.16 0.04
Pb 0.917.09 2.37** 0.99 25 1.532.37 1.90 0.24
Ni 0.0083.98 1.04** 0.77 131 0.160.86 0.45 0.17
Mundka
Zn 0.5716.17 3.68** 4.22 247 0.691.49 1.06 0.26
Cu 1.4117.03 4.39** 3.29 181 1.232.19 1.56 0.36
Fe 9.96115.5 50.2** 24.3 341 9.2017.1 11.4 2.99
Mn 4.7314.7 7.46** 2.05 18 7.7610.1 9.10 0.92
Cd 0.020.46 0.11* 0.07 38 0.050.11 0.08 0.02
Pb 1.123.79 2.60** 0.67 44 1.472.29 1.81 0.44
Ni 0.051.83 0.58** 0.40 123 0.070.39 0.26 0.12
Bakarwala
Zn 1.018.9 6.38** 5.29 186 0.757.73 2.23 1.04
Cu 1.539.7 6.53** 5.53 158 1.184.28 2.53 0.57
Fe 10.2113 62.2** 23.1 144 7.2876.2 25.4 16.1
Mn 2.6918.4 8.43** 3.03 51 4.121.2 12.7 4.3
Cd 0.040.85 0.22 0.12 0.070.85 0.19 0.11
Pb 0.507.92 2.64** 0.99 19 1.183.62 2.22 0.48
Ni 0.159.76 1.29** 1.22 14 0.061.58 0.54 0.29
Hirankudna
Zn 0.819.18 2.72* 2.00 113 0.981.51 1.28 0.20
Cu 0.494.94 1.71 0.94 1.101.79 1.41 0.18
Fe 1.8028.5 11.3** 6.67 117 2.439.75 5.22 2.58
Mn 1.0923.3 5.67 4.90 1.9113.1 6.47 3.08
Cd 0.010.90 0.14 0.18 0.010.23 0.09 0.06
Pb 0.761.46 1.21** 0.16 29 0.661.10 0.94 0.12
Ni 0.010.67 0.29* 0.19 81 0.010.35 0.16 0.13
Dichaonkala
Zn 1.1212.2 5.02 4.06 2.3118.8 6.46 4.74
Cu 0.528.59 2.65 2.47 0.995.78 3.04 1.67
Fe 2.8642.9 15.6** 12.2 254 1.7818.6 4.42 3.98
Mn 1.0320.5 6.92 5.98 1.0612.8 3.76 2.98
Cd 0.040.26 0.14 0.06 0.090.39 0.17 0.08
Pb 0.572.17 1.11 0.37 0.932.02 1.30 0.30
Ni 0.011.34 0.36 0.42 0.010.91 0.27 0.23
#(%), increase or decrease over tubewell-irrigated soils; S.D., standard deviation; (*) and (**) indicate that differences between means of sewage
and tubewell water-irrigated soils are significant at 5 and 1% probability levels, respectively.
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recorded in all the fractions except residual compared
to that of effluent-irrigated soils. Labile pool of Zn,
i.e. adsorbed fractions [(water soluble + exchange-
able) + Pb displaceable (specifically adsorbed) + a-
cid soluble] constituted higher share of total Zn
(38.3%) in sewage-irrigated soils than that in
tubewell water-irrigated ones (22.1%). Unlike Zn,
share of adsorbed Cu was more 61.2% of total Cu for
tubewell water-irrigated soils compared to effluent-
irrigated soils. However, immediately bioavailable
pools, i.e. water soluble + exchangeable Cu (Mathurand Levesque, 1983) was much higher 23.8% in
sewage-irrigated soils than that in tubewell water-
irrigated ones (1.16%). Generally, less than 10% of
total soil micronutrients are present in water soluble
and exchangeable forms (Lake et al., 1984).
Relatively higher amount of Zn and Cu in bioavail-
able forms in our study may be attributed to reduction
in soil pH as well as increase in organic carbon as a
result of long-term use of sewage effluents whichmay be a cause of concern in future.
Residual fraction of Fe constituted major share of
total soil Fe in both the categories of soils, followed by
crystalline Fe-oxide occluded and amorphous Fe-
oxide occluded fractions. Contribution of remaining
fractions to total soil Fe was meagre, ranging from
0.01 to 2.34%. Various researchers also reported that
most of the Fe resides in the amorphous Fe-oxide,
crystalline Fe-oxide occluded and residual fractions
(Hoffman and Fletcher, 1978; Shuman, 1985). Never-
theless, build-up of Fe was relatively more in first five
fractions in effluent irrigated soils indicating relatively
more lability of Fe in sewage-irrigated soils compared
to tubewell water-irrigated ones. More or less similar
pattern of distribution of Mn in different fractions was
observed in both the categories of soils, except water
soluble + exchangeable and residual fractions. Sew-
age-irrigated soils exhibited comparatively higher
share of water soluble + exchangeable Mn than that in
tubewell water-irrigated ones, while trend was reverse
for residual fractions. This may be attributed to the
decrease in pH associated with increase in organic
carbon as a result of long-term use of sewage effluents,which might have remobilized the Mn from structural
pools to more labile fractions. This probably can
explain the reason for depletion of Mn in these
sewage-irrigated light textured soils due to leaching
over the years. Takkar and Nayyar (1981) also
R.K. Rattan et al. / Agriculture, Ecosystems and Environment 109 (2005) 310322 317
Fig. 2. Effect of period of sewage irrigation on the build-up/deple-
tion of DTPA-extractable metals (%) over tubewell water-irrigated
soil.
Table 3
Mean values of Zn, Cu, Fe and Mn fractions in sewage and tubewell water-irrigated soils
Fractions Zn Cu Fe Mn
Sewage Tubewell Sewage Tubewell Sewage Tubewell Sewage Tubewell
Water soluble +
exchangeable
2.91 (3.8) 1.77 (3.4) 9.69 (23.8) 0.30 (1.16) 7.27 (0.07) 1.8 (0.01) 44.9 (12.1) 2.55 (0.77)
Pb-displaceable 16.9 (22.2) 5.92 (11.3) 7.34 (18.04) 11.7 (45.3) 5.48 (0.06) 4.33 (0.04) 42.1 (11.3) 43.2 (13.1)
Acid soluble 9.32 (12.3) 3.88 (7.4) 6.12 (15.04) 3.81 (14.7) 27.4 (0.30) 18.9 (0.18) 47.8 (12.8) 40.7 (12.3)
Mn-occluded 2.64 (3.47) 0.46 (0.88) ND ND 33.4 (0.37) 23.6 (0.23) 31.5 (8.46) 26.4 (8.0)
Organically bound 22.6 (29.7) 19.1 (36.6) 1.72 (4.22) 0.35 (1.33) 215 (2.34) 128 (1.26) 8.87 (2.38) 6.04 (1.83)
Amorphous Fe-oxide
occluded
6.84 (8.99) 4.68 (9.0) 3.96 (9.73) 0.73 (2.82) 566 (6.16) 396 (3.9) 5.78 (1.55) 5.82 (1.76)
Crystalline Fe-oxide
occluded
8.20 (10.7) 4.74 (9.1) 0.94 (2.31) 0.053 (0.20) 1000 (10.9) 1071 (10.6) 18.3 (4.91) 17.5 (5.31)
Residual 6.63 (8.7) 11.5 (22.0) 10.9 (26.8) 8.90 (34.4) 7304 (79.7) 8492 (83.8) 173 (46.5) 187 (56.9)
Figures in parenthesis indicate percentage of total metal content in soils; ND: not detectable in flame AAS.
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reported Mn deficiency in some light textured soils of
Punjab because of the leaching losses of Mn from the
surface soil layer.
3.3.4. Metal contents in plants
Mean contents of metals in the dry matter of
various crops grown on sewage effluent and tubewell
water-irrigated soils are summarized in Table 4. Rice
grain accumulated much higher amount of Zn and Cu
grown on sewage-irrigated soils compared to tubewell
water-irrigated soils, while slight increase in Ni
content was recorded. Manganese content in rice grain
for sewage-irrigated soils was much lower than that
for tubewell water-irrigated soils. In general, this trend
is in concurrence with the levels DTPA-extractableMn in both categories of soils. Although sewage
effluent-irrigated soils exhibited much higher amount
of DTPA-Fe, it was not reflected in Fe content of rice
grain. From this study, it is difficult to elucidate the
reasons for this anomaly. Iron content in rice straw to
some extent reflected the variations in DTPA-Fe
between sewage and tubewell water-irrigated soils.
Rice straw accumulated almost two times more Ni
produced with sewage water over that of tubewell
water irrigation. However, Zn and Cu contents in the
rice straw produced on the sewage-irrigated soils
appeared to be rather marginally lower than its
background level. Wheat had elevated contents of Zn,
Cu, Fe, Mn and Ni grown on sewage-irrigated soilscompared to that produced with tubewell irrigation.
Sorghum accumulated higher amount of Fe, Cu and Ni
on sewage effluent irrigated soils, while Zn and Mn
contents were lower than its background level. Maize
showed higher accumulation of all the elements on
sewage effluent irrigated soils. Similar trends were
observed in gobhi sarson and oats with only exception
of Mn, where plant contents of Mn conformed to the
DTPA-Mn in both the categories of soils. Spinach
grown on sewage-irrigated soils accumulated higher
amount of Zn, Cu and Ni than those grown on tubewellwater-irrigated soils, whereas reverse were the trends
for Fe and Mn. Comparison of metal contents in Indian
rape, cauliflower, cucumber, Egyptian clover and
radish for both of these soils could not be made as
these crops were not grown with tubewell irrigation in
this study area at the time of sampling. Cadmium and
lead contents in tissue of all the crops under study,
were below the analytical detection limits, hence no
data were reported. Similar were the observations of
Datta et al. (2000) and Yadav et al. (2002) for some
R.K. Rattan et al. / Agriculture, Ecosystems and Environment 109 (2005) 310322318
Table 4
Heavy metal contents in crops grown on sewage effluents and tubewell water-irrigated soils
Crops Metal contents (mg kg1
)
Zn Cu Fe Mn NiS T S T S T S T S T
Rice (Oryza sativa L.)
Grain 49.6 (27) 29.6 (4) 51.6 23.0 122 186 53.3 88.1 10.1 9.85
Straw 58.9 (27) 61.9 (4) 57.2 59.8 233 202 208 229 10.4 5.27
Wheat (Triticum aestivum L.) 65.3 (88) 47.5 (27) 9.39 7.45 404 336 15.3 13.6 20.0 19.7
Sorghum (Sorghum vulgare Pers.) 54.2 (38) 73.4 (9) 16.9 115.5 526 485 40.6 44.8 14.8 11.6
Maize (Zea mays L.) 78.8 (15) 67.6 (1) 14.9 13.3 531 99.0 26.0 15.3 16.5 5.20
Oats (Avena sativa L.) 59.0 (7) 44.3 (2) 8.71 6.35 458 400 23.8 29.2 18.3 37.3
Gobhi sarson (Brassica napus) 66.9 (17) 38.7 (3) 23.1 14.1 454 401 69.0 104 12.0 3.73
Spinach (Spinacea oleraceae L.) 77.1 (17) 38.4 (2) 20.6 16.1 711 734 39.3 87.8 18.4 13.2
Indian rape (Brassica campestris
var. toria Dutch)
52.5 (10) 5.42 475 42.6 8.78
Cauliflower (Brassica oleracea L.) 46.7 (11) 10.8 328 31.8 14.4 Cucumber (Cucumis sativus L.) 79.4 (5) 19.3 932 19.9 21.5
Radish (Raphanus sativus L.)
Leaf 60.8 (7) 14.6 358 41.9 9.26
Root 58.9 (7) 10.4 166 16.7 11.5
Egyptian clover (Trifolium
alexandrinum L.)
91.9 (15) 18.3 623 20.7 20.6
Figures in parenthesis indicate number of samples analysed; S: sewage-irrigated; T: tubewell water-irrigated.
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sewage-irrigated soils of India. By and large,
concentrations of metals in all the crops grown on
sewage effluent-irrigated soils were below the general-
ized critical levels of phytotoxicity (as summarized by
Datta et al., 2000) except Fe. Although no toxicity
symptoms were noticed, Fe contents in sorghum,
maize, spinach, cucumber and Egyptian clover
exceeded the phytotoxicity limit (> 500 mg kg1;
on dry weight basis). Crop species exercised
differentiality in accumulating metals in their tissues.
Similar were the observations of Lepp (1981),
Sauerback (1991), Smith (1994), Hooda et al.(1997), Datta et al. (2000) and Yadav et al. (2002).
Since DTPA is the most commonly used soil test
for assessing bioavailability of metals in contaminated
soils (Hooda et al., 1997; Datta et al., 2000; Yadav
et al., 2002; Patel et al., 2004), simple correlation
coefficients were worked out between plant metal
concentrations and DTPA-extractable metals in soil.
Results indicate that DTPA-Zn had most consistent
positive relationships with tissue metal concentrations
of all the crops as listed in Table 5, except sorghum.
DTPA-extractable Cu positively contributed to thetissue concentration of Cu in case of wheat, sorghum
and cucumber. DTPA-extractable Fe contents were not
related to the Fe contents in any of the crops.
Manganese contents in plants did not exhibit any
relationship with soil Mn, except rice grain. Nickel
contents in sorghum, Indian rape and cauliflower were
positively related with DTPA-Ni in soils. Failure of
DTPA extractant in some cases in the present study
may be attributed lesser number of observations and
variations in the management practices among the
farmers of the study area. Even under controlled
conditions, ability of extractants to predict plant
available metals depends on the crop species, the
metal and extractant used (Hooda et al., 1997). In
several studies, it is established that solubility of
metals in soils mainly depends on soil pH and organic
carbon (Ma and Lindsay, 1993; Jopony and Young,
1994; Hough et al., 2003; Tye et al., 2003). Hence, in
the present investigation, effect of these two important
soil properties on the lability of metals was studied
(Table 6). Results show that soil pH had negative
influence on the extractability of metals from soils byDTPA. While increase in soil organic carbon content
enhanced the DTPA-extractable metals, except Mn.
However, inclusion of pH and organic carbon in
multiple regression equation along with DTPA-
extractable metals as predictor variables to predict
plant metal concentrations, could not improve the
values of prediction coefficients except spinach (data
not shown). It appears that available metal content in
soils is the principal factor predicting its concentration
R.K. Rattan et al. / Agriculture, Ecosystems and Environment 109 (2005) 310322 319
Table 6
Simple correlation coefficients of DTPA-extractable metals with soil
pH and organic carbon
Metals pH Organic carbon
Zn 0.37** 0.55**
Cu 0.37**
0.71**
Fe 0.50**
0.54**
Mn 0.31**
0.02
Ni 0.46**
0.73**
Pb 0.09**
0.32**
Cd 0.29**
0.42**
(**) significant at 1% probability level.
Table 5
Simple correlation coefficients (r) between DTPA-extractable metals and metal contents in crops
Crops Metal contents in crops
Zn Cu Fe Mn NiRice (Oryza sativa L.)
Grain 0.58**
0.05 0.04 0.38**
0.20
Straw 0.58**
0.06 0.25 0.02 0.15
Wheat (Triticum aestivum L.) 0.35**
0.43**
0.14 0.04 0.12
Sorghum (Sorghum vulgare Pers.) 0.25 0.38**
0.25 0.04 0.28*
Gobhi sarson (Brassica napus) 0.45* 0.12 0.26 0.27 0.38
Spinach (Spinacea oleraceae L.) 0.51*
0.43 0.03 0.09 0.03
Indian rape (Brassica campestris var. toria Dutch) 0.86**
0.21 0.25 0.35 0.61**
Cauliflower (Brassica oleracea L.) 0.72* 0.67* 0.41 0.34 0.66*
Egyptian clover (Trifolium alexandrinum L.) 0.57*
0.28 0.01 0.027 0.03
(*) and (**) significant at 5 and 1% probability levels, respectively.
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in plants. Regression analysis according to Snedecor
and Cochran (1967) revealed that DTPA-Zn, soil pH
and organic carbon could explain the variability in
Zn content in spinach to the extent of 79% [Zncontent in spinach (mg kg1) = 241 + 2.11 (DTPA-Zn
mg kg1) 25.9 (pH) + 54.7 (organic carbon %);
R2 = 0.79; significant at 1% probability level].
Transfer factors (TF), i.e. the ratio of metal
concentration in plants to DTPA-extractable metal
in soil, varied considerably among the crops (Table 7).
In case of Zn and Fe, TFs for all the crops grown on
sewage effluent-irrigated soils were lower than that for
crops produced with tubewell water irrigation.
However, for other metals, such consistent variations
in TFs were not obtained. This indicates that uptake ofmetals by crops does not increase linearly with
increasing concentrations of metals in soils. This is in
concurrence with the findings ofHooda et al. (1997).
The apparent advantage of this phenomenon is that
although long-term sewage irrigation resulted into
elevated concentration of metal in soil, the same
would not be proportionately transferred to food
chain. Taking all the crops together, relative orders of
transfer of metals from soil to plants grown on sewage-
irrigated soils were Ni > Zn > Fe > Mn > Cu. These
results show that as far as entry of these metals to food
chain plants is concerned, Ni has the greatest potential,
followed by Zn, Fe, Mn and Cu. Based on the TFs,
relative efficiency of crops to absorb metals fromsewage-irrigated soil could be arranged in the
following order:
Zinc: Egyptian clover> spinach> sorghum> rice
leaf> Indian rape > wheat > rice grain > gobhi sar-
son> oats > radish root > maize > cucumber> rad-
radish leaf.
Copper: Rice leaf> rice grain> sorghum > spi-
spinach > gobhi sarson> Indian rape> Egyptian
clover > cucumber > radish leaf> maize > wheat
>
radish root>
cauliflower>
oats.Iron: Sorghum > spinach > gobhi sarson > cucum-
ber > radish leaf> Indian rape > cauliflower > mai-
ze > Egyptian clover > wheat> oat > radish root >
rice leaf> rice grain.
Manganese: Rice leaf> gobhi sarson > Indian ra-
pe> radish leaf> sorghum > spinach > rice grain >
cauliflower > radish root> cucumber > maize > oa-
ts > Egyptian clover > wheat.
Nickel: Sorghum > cucumber > spinach > wheat >
rice leaf> Egyptian clover> Indian rape > radish
R.K. Rattan et al. / Agriculture, Ecosystems and Environment 109 (2005) 310322320
Table 7
Transfer factor (TF) for crops grown on sewage effluents and tubewell water-irrigated soils
Crops Transfer factor of metals
Zn Cu Fe Mn NiS T S T S T S T S T
Rice (Oryza sativa L.)
Grain 16.5 21.2 12.9 7.46 2.30 4.43 8.69 10.9 15.9 20.2
Straw 20.8 47.5 15.2 21.9 4.46 5.92 31.5 26.8 23.1 12.1
Wheat (Triticum aestivum L.) 18.3 22.6 2.35 16.7 7.91 16.2 1.93 1.27 24.3 47.8
Sorghum (Sorghum vulgare Pers.) 23.7 33.4 8.48 6.80 57.8 104 10.9 16.3 145 457
Maize (Zea mays L.) 14.4 32.0 2.81 8.59 11.8 19.6 3.58 3.85 18.9 11.4
Oats (Avena sativa L.) 15.5 29.6 1.69 2.48 7.17 15.3 2.65 1.90 15.2 37.3
Gobhi sarson (Brassica napus) 16.1 43.5 5.57 14.3 25.6 123 21.2 23.2 16.0 31.7
Spinach (Spinacea oleraceae L.) 24.6 27.7 6.18 16.1 26.0 255 9.07 15.3 32.3 52.2
Indian rape (Brassica campestris
var. toria Dutch)
19.1 55.6 5.42 18.1 15.8 200 15.6 20.2 22.1 94.3
Cauliflower (Brassica oleracea L.) 7.25 1.91 14.7 8.59 15.6 Cucumber (Cucumis sativus L.) 13.1 3.16 22.5 3.98 37.3
Radish (Raphanus sativus L.)
Leaf 9.55 3.05 22.4 13.7 9.00
Root 15.0 2.32 6.00 4.77 19.7
Egyptian clover (Trifolium
alexandrinum L.)
25.1 4.71 11.8 2.60 22.5
S: sewage-irrigated; T: tubewell water-irrigated.
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root > maize > gobhi sarson> rice grain > cauli-
flower > oats > radish leaf.
This information will be very useful in selecting thesuitable crops to be grown on metal-contaminated
soils.
3.4. Risk assessment
In this study area, spinach, gobhi sarson and Indian
rape are produced and marketed as leafy green
vegetables. Also there was a substantial build-up of
Zn, Cu and Ni sewage-irrigated soils. Hence, hazard
quotients (HQgv), i.e. the ratio of average daily dose to
the reference dose (Pierzynski et al., 2000) for intake
of metals by human through the consumption of these
leafy green vegetables were worked out. The values of
HQgv for gobhi sarson varied from 0.040 to 0.068 for
Zn, 0.004 to 0.021 for Cu and 0.027 to 0.442 for Ni
(data not shown). In case of spinach, HQgv varied from
0.035 to 0.152, 0.008 to 0.015 and 0.046 to 0.502 for
Zn, Cu and Ni, respectively. The values of HQgv for
Indian rape ranged from 0.027 to 0.053, 0.004 to 0.014
and 0.016 to 0.429 for Zn, Cu and Ni, respectively.
Although, Ni exhibited relatively higher HQ for all the
crops compared to other two metals, most of the values
were far less than 1. Hence, these green vegetables arenot likely to induce any health hazard to consumers
(human) as far as its metal contents are concerned.
4. Conclusions
From this study, it can be concluded that besides
use as irrigation water, these sewage effluents are also
a potential source of plant nutrients. Build-up of heavy
metals, particularly Zn, Cu and Ni in sewage-irrigated
soils needs to be monitored periodically in view oftheir significant accumulation in bioavailable pool
associated with decline in pH. Appreciable depletion
in available Mn under these intensively cultivated
sewage-irrigated soils is likely to induce unsustain-
ability in soil productivity and thus, Mn needs to be
included in balanced fertilization programme. There is
a great respite that accumulation of dreaded metals
like Cd and Pb has not posed any threat even after such
long-term use of these sewage effluents. As far as
metal contents are concerned, the leafy green
vegetables grown on these sewage-irrigated soils are
still safe to be consumed by human beings.
Acknowledgement
Authors would like to place on record their sincere
thanks to Indian Council of Agricultural Research,
New Delhi, India for funding this study as a part of AP
Cess Fund project.
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