agricultural water management 84 (2006) 147–152

available at www.sciencedirect.com

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

Cadmium in soil–rice system and health risk associated

with the use of untreated mining wastewater for
irrigation in Lechang, China

Q.W. Yang a, C.Y. Lan b, H.B. Wang b, P. Zhuang b, W.S. Shu b,*
a
Department of Resource and Environmental Sciences, School of River & Sea Architectural Engineering,
Chongqing Jiaotong University, Chongqing 400074, PR China
b
School of Life Sciences and State Key Laboratory of Bio-control, Sun Yat-sen (Zhongshan) University, Guangzhou 510275, PR China

article info abstract

Article history: Using untreated mining wastewater to irrigate paddy field around Lechang lead/zinc mine in
Accepted 15 January 2006 the upper Wu Jiang River basin, Guangdong Province, southern China, caused cadmium
Published on line 9 March 2006 transport onto paddy soils and crop contamination. This study characterized Cd concen-
tration in soil–rice system irrigated with the wastewater mentioned above and evaluated
Keywords: potential ecotoxicological hazardous risk to humans and animals. All soil and plant samples
Cadmium were analyzed using atomic absorption spectrophotometer (AAS; Model 3030, Perkin-Elmer,
China USA). The results showed that all soil samples were extremely contaminated by cadmium,
I-geo soil Cd occurred primarily in the residual fraction. Using synthetic stomach fluid simulating
Health risk gastrointestinal condition, result showed that 28.4% of the total soil cadmium concentration
Paddy soil would be ingested in human/animal gastrointestinal tract. Mean Cd concentrations in plant
Oryza sativa L. tissues (DW) ranged from 0.24 (unpolished rice) to 8.21 mg g
1 (root). Dietary intake of
cadmium through contaminated rice consumption was calculated to be 2.2 and 1.5 mg kg
1
body weigh per day for a 60-kg adult and 40-kg child, respectively. The values were much
higher than the provisional tolerable daily intake (PTDI; 1 mg kg
1 body weight by FAO/WHO in
1989). Present results indicated that the paddy soil–rice system irrigated with untreated
mining wastewater in Lechang lead/zinc mine area was heavily contaminated by Cd
and would pose a human/animal health risk through Cd mobility in the food chain. Therefore,
local mine wastewater should be decontaminated before being irrigated to surrounding
farmland.
# 2006 Elsevier B.V. All rights reserved.

1. Introduction
As a great concern, water and soil contamination by heavy
metals from various mining activities in the upper Wu Jiang
River basin is not well documented. It is well known that heavy
metal, such as cadmium (Cd), in agricultural soils may influence
crop yield and quality. Consumption of heavy metal contami-
nated food and water posed severe foodborne illness for several
hundred millions of humans in the world (WHO, 2004). With
increasing improvements of economy and living levels, the
demand for ‘food safety’ is increasing. However, heavy metal
contamination in agricultural soils has increased due to
disposal of sewage sludge and municipal wastes, irrigation
with industrial wastewater, and precipitation of air pollutants

* Corresponding author. Tel.: +86 20 8403 6296; fax: +86 20 8411 3652.
E-mail address: ls53@zsu.edu.cn (W.S. Shu).
0378-3774/$ – see front matter # 2006 Elsevier B.V. All rights reserved.
doi:10.1016/j.agwat.2006.01.005
148 agricultural water management 84 (2006) 147–152
(MacNicol and Beckett, 1985; Jinadasa et al., 1997). As a well-
known toxic element, cadmium is nonessential and poisonous
for plant, animal and human (Gupta and Gupta, 1998). Elevated
Cd in soils may compromise soil productivity, and inhibit vital
plant processes (Kabata-Pendias and Pendias, 1992).
Rice (Oryza sativa L.), as a primary cereal crop in China,
contributes to about 40% of the national grain yield. The yield
of about 200 million tonnes per year and sowing area of around
30 million ha per year since 1995 rank the first and the second
in the world, respectively (Hu et al., 2002). In addition, rice is a
major staple for more than 60% of the population of China
(Ying, 1997). There are 20 million ha accounting for about 20%
of total area under cultivation contaminated by heavy metals
from various human activities in China (Chang and Shi, 2001)
and about 1700,000 ha of farmland contaminated by heavy
metals released from local mining activities in northern
Guangdong Province of China (Shu, 1997), which accounted for
7.3% of the total cultivated land in this area. Thus, heavy metal
such as Cd in rice production may cause potential long-term
health risk through rice consumption. The objectives of this
study were to examine Cd contaminations in paddy soil–rice
plant system influenced by mining activities, and to evaluate
the potential ecotoxicological hazardous risk to local animal
and human from ingestion.
2. Materials and methods
2.1. Study area description
Lechang lead/zinc mine (248400 N, 1138200 E) is located in north-
ern Guangdong Province, southern China (Fig. 1). This mine area
has a humid subtropical climate with a long-term average
annual temperature of 19.6 8C and an average annual precipita-
tion of 1522 mm. The major ore minerals are sphalerite (ZnS
with some cadmium, iron and manganese), galena (PbS), pyrite
(FeS2) and chalcopyrite (CuFeS2). As a conventional under-
ground operation, this ore mine was opened in 1959 and is still
in operation with a cover area of 1.5 km2 and produces of
250,000 tonnes of waste rocks and 30,000 tonnes of tailings
occupying respective 8300 and 60,000 m2 (Shu et al., 2001). Most
of the dumping area is bare and lacks vegetation cover.
Therefore, the surrounding farmlands, including the present
study area involving six adjacent rectangle paddy fields and
covering an area of 0.8 ha (Fig. 1), were seriously affected by the
continuing usage of untreated black mining wastewater lifted
from mines and filtrated from tailings for irrigation all year
around. Both polluted and unpolluted soils in the study area are
the same zonal soil, i.e., red soil, with pH value of 4.38 and
33.8 g organic matter (O.M.) kg
1 for unpolluted (Xu and Liu,
1996) and 7.46 (pH) and 12.4 g O.M. kg
1 for polluted soils (Yang
et al., 2003), respectively. In the study area, rice plant has been
grown continuously on these soils since 1959 when the mine
opened. Rice plant is submerged with the polluted water
occasionally during growing season.
2.2. Soil and plant sampling and preparation
As presented in Fig. 1, at harvest, six adjacent rectangle paddy
fields were selected for collection of 60 soil (10 from each plot)
and 40 rice (just from plots 2 to 5 and 10 from each plot) samples.
Note that there was no any crop in plots 1 and 6. Plot distance
from the inlet is clearly plotted in Fig. 1. Each soil sample (about
1 kg) was taken from the plough layer (0–20 cm) and each rice
plant sample was collected from the corresponding soil-
sampling site. Aerial parts of rice plant were sampled using
stainless steel scissors, roots were scooped up using a stainless
steel shovel within a cylinder of approximately 20 cm in
diameter and in depth. Plant samples were washed with tap
water to remove adhered soil. Ten random samples of paddy
soil were also collected from control area about 2 km away from
the study area and without the use of the mining wastewater
(Yang et al., 2003). Soil sampling in background area was also
collected and analyzed by Xu and Liu (1996).
Soil samples were air-dried, pulverized and passed through
60 mesh sieve. All samples of rice plants were washed with
deionized water to remove soil particles or dusts adhering to the
plant surface. Aerial parts were separated into straw, stalk, hull,
grain with hull, and grain without hull (namely, unpolished
rice). All aerial parts and roots were oven-dried at 70 8C for 72 h,
then ground in a stainless steel mill to fine powder.
2.3. Chemical analysis
Total soil Cd was measured by the method from McGrath and
Cunliffe (1985). DTPA-extractable soil Cd was extracted using
DTPA solution introduced by Lindsay and Norvell (1978).
Exchangeable, carbonate, Fe/Mn oxides, organic and residual
form of Cd in soils was determined by a sequential extraction
procedure described by Tessier et al. (1979), and the likely post-
ingestion bioavailability of soil Cd in human/animal gastro-
intestinal tract was examined by a simple bioavailability
extraction test (SBET), which using synthetic stomach fluid. A
detailed description of this program has been published
elsewhere (Kim et al., 2002). Plant samples were digested with
concentrated HNO3 and HClO4 (5:1, v/v). Cadmium in all
extracts was analyzed using atomic absorption spectrophot-
ometer (AAS; Model 3030, Perkin-Elmer, USA). Quality control
was assured by the use of reagent blanks, duplicates and
standard reference material (NIST SRM 2709).
2.4. Soil Cd pollution assessment
Soil Cd pollution severity was assessed by the geo-accumula-
tion index (I-geo;) using the following equation (Muller, 1969;
Ntekim et al., 1993):
 
Cn
I-geo ¼ log2 ;
1:5Bn
where Cn is the measured total concentration in soils, Bn the
background value (0.03 mg Cd kg
1 in this case; Xu and Liu,
1996) and 1.5 is the correction factor compensating the back-
ground data due to lithogenic effects. The I-geo is classified
into seven grades: 0 (class 0) indicates the uncontaminated
stage; 0–1 (class 1) shows the uncontaminated to moderately
contaminated; 1–2 (class 2) the moderately contaminated, 2–3
(class 3) the moderately to strongly contaminated; 3–4 (class 4)
the strongly contaminated; 4–5 (class 5) the strongly to extre-
mely contaminated; and 5–10 (class 6) the extremely contami-
nated (Muller, 1969; Ntekim et al., 1993).
 agricultural water management 84 (2006) 147–152 149

Fig. 1 – Sampling location map of the study area.

study paddy field, was 21 mg g
1. The comparison suggested

3. Results and discussion
3.1. Total and bioavailable cadmium in contaminated
paddy soil
Although not generally well correlated with metal mobility
and bioavailability data, total soil metals can be used to
estimate the degree of soil exposure to heavy metal pollution
(Kuo et al., 1983). As shown in Table 1, the lowest Cd
concentration (2.01 mg g
1) at one point in plot 6 was 67 times
higher than the local background value (0.03 mg g
1; Xu and
Liu, 1996), and the highest one (29.68 mg g
1) at one point in
plot 2 was 9.9 times higher than the critical level referring to
the presence of toxic effects above the concentration in soils
(3.0 mg g
1; Kabata-Pendias and Pendias, 1992).
Total Cd concentration in different plots ranged from
6.59 mg g
1 (plot 6) to 17.97 mg g
1 (plot 2) (Fig. 2), and the lowest
and the highest average concentrations of Cd were about 7.0
times and 19.1 times higher than the average (0.94 mg g
1;
Yang et al., 2003) in the control paddy soils, respectively.
According to Shu et al. (2001), mean Cd concentration in local
Pb/Zn mine tailings, from which filtrate containing toxic heavy
metals originated and was used as a great part to irrigate the
that Cd contamination in study soils was originated from the
use of untreated mining wastewater for irrigation and not
from the geochemical baseline. According to the regression
model (Fig. 2), cadmium concentration of soil decreased
significantly with distance from the inlet, which suggested a
necessity for precipitation of the mining wastewater contain-
ing toxic heavy metals before use for vegetables and crop
plants. The value of I-geo ranged from 5.5 to 9.4 (Fig. 3) which
indicated that all the 60 soil samples were in I-geo class 6 and
thus the paddy soils were extremely contaminated by Cd from
the mining wastewater.
The amount extracted by a chelating agent like DTPA is
considered to be the plant-available portion (Baker, 1990).
Mean percentage of DTPA-extractable Cd in soils of local
tailings (TS), the present study paddy soils (PS) and local
natural soils (NS) is TS (3.5%; Shu et al., 2001) < PS (4.4%;
Table 1) < NS (10.8%;Ye et al., 2002), while total Cd is NS
(1.2 mg g
1;Ye et al., 2002) < PS (13.59 mg g
1; Table 1) < TS
(21 mg g
1; Shu et al., 2001). This may be due to pH, O.M. and
other soil conditions (Harter, 1983; Berrow and Burridge, 1991;
Salomons and Stigliani, 1995; Manz et al., 1999). Although
absolute DTPA-Cd concentrations (0.39–1.28 mg g
1) found
here was lower than the phytotoxically excessive level

Table 1 – Concentrations and percentages of Cd in different fractions of paddy soils

Metal fraction Meana Maximuma Minimuma Median Mode S.D. Nb

Total Cd (mg g
1) 13.59 (plot 5) 29.68 (plot 2) 2.01 (plot 6) 13.55 19.54 6.50 60
DTPA-Cd (%) 4.4 (plot 4) 7.20 (plot 2) 3.10 (plot 1) 3.8 1.2 2.02 16
SBET-Cd (%) 28.4 (plot 4) 73.5 (plot 1) 7.70 (plot 6) 27.1 29.1 13.33 16
Exchangeable (%) 15.1 (plot 4) 40.6 (plot 1) 0.6 (plot 2) 19.9 0.4 10.85 16
Carbonate (%) 18.8 (plot 4) 32.0 (plot 4) 7.6 (plot 6) 18.2 7.6 6.54 16
Fe/Mn oxides (%) 5.1 (plot 4) 10.0 (plot 4) 1.9 (plot 6) 4.8 3.4 2.34 16
Organic (%) 4.2 (plot 4) 17.4 (plot 4) 0.6 (plot 6) 2.9 2.4 3.57 16
Residual (%) 56.8 (plot 3) 83.0 (plot 2) 21.4 (plot 1) 56.3 54.7 16.9 16
a
To which in parentheses the value corresponds.
b
N, number of samples.
150 agricultural water management 84 (2006) 147–152
Fig. 2 – Soil Cd concentrations in six paddy fields with
distance from the inlet. Values are mean W S.D.
(3.0 mg g
1; Kabata-Pendias and Pendias, 1992), the positive
correlation (Fig. 4) between Cd concentration in DTPA-
extractable and total fraction indicated that the elevated Cd
in the paddy soils might increase its toxicity for crops such as
rice plant. Cadmium in soils occurred primarily in the residual,
carbonate and exchangeable fractions (Table 1) and about
37.3% of total Cd would be bioavailable to plants as the
exchangeable, carbonate, Fe/Mn oxides and organic forms
would be released under some conditions, while the residual
form would not because it was strongly bounded in the crystal
lattice of the minerals (Tessier et al., 1979; Kersen and
Förstner, 1991).
3.2. Cadmium in rice plants
Cadmium in root was over 4-, 2-, 11-, 12- and 34-fold higher
than that in straw, stalk, hull, grain with hull and grain
without hull (namely, unpolished rice), respectively (Table 2).
The result indicated that Cd was mostly accumulated in rice
root, Cd in rice grass was mainly distributed in stalk, and Cd in
rice grain largely in hull.
Average Cd concentration in hull, grain with hull and grain
without hull of rice plant exceeded the normal range of 0.013–
0.22 mg g
1 for all cereal grains and Cd in straw and stalk was
much higher than that of 0.07–0.27 mg g
1 for grass (Kabata-
Pendias and Pendias, 1992); also, concentration of Cd
Fig. 3 – The distribution of I-geo values of soil samples in
the study area.
Fig. 4 – Correlation between total and DTPA-extractable Cd
concentrations in soils.
(0.24 mg g
1; Table 2) in unpolished rice was slightly higher
than the environmental quality guideline of 0.2 mg g
1 for Cd
in cereals in China (Wang, 2000).
3.3. Potential health risk of cadmium to human and
livestock
Environmental mediums containing toxic or excessive che-
mical metals, such as food, drinking water, atmosphere, and
soil/dust, can affect human health when occasional ingestion
and inhalation occurred (Bowie and Thornton, 1985). Accord-
ing to the simple bioavailability extraction test (SBET; Kim
et al., 2002), the likely bio-availability of soil Cd in the
gastrointestinal tract of local resident and/or livestock was
examined (Table 1). Comparison with the result (61.7–72.8%)
reported by Kim et al. (2002) showed that result in the present
study (Table 1) was comparatively lower. However, children
can consume up to 10 g (i.e., 10  106 mg) per day (cf. Mercier
et al., 2002). Based on the average SBET-extractable Cd
concentration (3.86 mg g
1 = 13.59 mg g
1  28.4%; Table 1),
theoretic 0.965 mg kg
1 body weigh per day for a 40-kg person
(i.e., children) can be calculated, which approximated the
provisional tolerable daily intake (PTDI; 1 mg kg
1 body weight;
FAO/WHO, 1989). Therefore, potential health hazards may be
caused by incidental oral ingestion of soil when local farmers
and cattle are working or children playing in paddy fields.
In this study area, cattle are fed with unwashed rice straw
harvested from the contaminated paddy fields in the winter.
Cadmium concentration in washed rice straw (1.69 mg g
1) or
stalk (3.41 mg g
1) (Table 2) exceeded the tolerable level
(0.5 mg g
1) recommended for livestock consumption (Chaney,
1989). Other domestic animals, including duck, geese, chicken,
and swine, are fed with other tissues containing elevated Cd
concentration, such as hull (0.73 mg g
1), grain with hull
(0.67 mg g
1) or/and unpolished rice (0.24 mg g
1; Table 2).
Thus, all these tissues of local rice crop might pose adverse
effects on the health of local domestic animals.
For local population, rice is consumed as the staple food,
and hence, concentration of Cd in rice contributes a major part
to the total daily intake of this element. Average daily dietary
intake of unpolished rice grown in their own land by local
residents is 550 g for adults aged fewer than 40 and 250 g for
 agricultural water management 84 (2006) 147–152
Table 2 – Cd concentrations in rice plants (mg gS1)
Tissue Mean Maximum
Root 8.21 23.47
Straw 1.69 6.24
Stalk 3.41 5.86
Hull 0.73 0.81
Grain with hull 0.68 1.15
Grain without hull 0.24 0.46
(unpolished hull)
a
N, number of samples.
children aged 8–10 years old. According to Cd concentration
(0.24 mg g
1; Table 2) in unpolished rice, the dietary intake of
cadmium through rice consumption may be calculated to 2.2
and 1.5 mg kg
1 body weigh per day for a 60 kg (adults) and for
40 kg (children) person, respectively. The values were much
higher than the PTDI of 1 mg kg
1 body weight recommended
by FAO/WHO (1989).
Above calculation of Cd daily intake through soil (i.e., SBET-
Cd) and rice consumption implied that, although obvious
health problems have not been found, long-term exposure to
Cd through regular consumption of rice and incidental oral
ingestion of soil may pose a potential health risk. This study
recommends that remediation should be performed before
crops are grown on the land.
4. Conclusions
The paddy soils around Lechang Pb/Zn mine contained
elevated Cd mainly through the irrigation with wastewater
discharged from the mine waste dumps. Total concentrations
of Cd were high but DTPA-extractable Cd concentration was
relatively low. Soil cadmium was dominated by the residual,
carbonate and exchangeable fraction. The SBET analysis
showed that the local farmers, cattle, and/or children might
be severely affected through ingestion and inhalation of Cd
when plowing and weeding in paddy plots or through the
inadvertent ingestion by so-called hand-to-mouth behavior.
Cadmium in rice plant was mainly enriched in the root and Cd
concentrations in components including rice straw, stalk,
hull, grain with hull and grain without hull (namely,
unpolished rice) all exceeded the safe guidelines. Elevated
Cd in soil (e.g. total, DTPA- and SBET-Cd) and rice plants may
pose potential health risk to the local population and
livestock through food chain, for example, the daily intake
of Cd from rice was far above the allowable levels for either
adults or children.
Acknowledgements
This project was supported by Fok Ying Tung Education
Foundation (No. 94022), the National Natural Science Founda-
tion of China (No. 30170178, 40471117), Science Foundation of
Chongqing Educational Committee (KJ050410) and Doctoral
Startup Foundation of Chongqing Jiaotong University (RC2004-
03). We wish to thank the editor and unknown referees for
providing valuable help.
151
Minimum S.D. Na
1.79 5.63 40
0.50 1.23 12
0.95 1.32 12
0.55 0.10 12
0.35 0.24 12
0.03 0.16 12
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