environmental pathway and risk assessment studies of the musi river's heavy metal...

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Environmental Pathway and RiskAssessment Studies of the Musi River'sHeavy Metal Contamination—A CaseStudyChandra Sekhar a , N. S. Chary a , C. T. Kamala a , Shanker b & H.Frank ca Analytical Chemistry and Environmental Sciences Division, IndianInstitute of Chemical Technology (IICT) , Hyderabad, Indiab Analytical Chemistry Division, Defence Metallurgical ResearchLaboratory (DMRL) , Hyderabad, Indiac Environmental Chemistry and Ecotoxicology, University ofBayreuth , GermanyPublished online: 18 Jan 2007.

To cite this article: Chandra Sekhar , N. S. Chary , C. T. Kamala , Shanker & H. Frank (2005)Environmental Pathway and Risk Assessment Studies of the Musi River's Heavy Metal Contamination—ACase Study, Human and Ecological Risk Assessment: An International Journal, 11:6, 1217-1235, DOI:10.1080/10807030500278594

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Human and Ecological Risk Assessment, 11: 1217–1235, 2005Copyright C© Taylor & Francis Inc.ISSN: 1080-7039 print / 1549-7680 onlineDOI: 10.1080/10807030500278594

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Environmental Pathway and Risk Assessment Studiesof the Musi River’s Heavy Metal Contamination—ACase Study

Chandra Sekhar,1 N. S. Chary,1 C. T. Kamala,1 Shanker,2 and H. Frank3

1Analytical Chemistry and Environmental Sciences Division, Indian Institute ofChemical Technology (IICT), Hyderabad, India; 2Analytical Chemistry Division,Defence Metallurgical Research Laboratory (DMRL), Hyderabad, India;3Environmental Chemistry and Ecotoxicology, University of Bayreuth, Germany

ABSTRACTThe Musi River, in Hyderabad, the capital city of Andhra Pradesh state in India,

is relatively dry for most of the year except for the four monsoon months when700–800 mm of rain falls. Throughout the year, sewage, industrial, and hospitalwaste is released into the river. In the present work the Musi River from AmberpetBridge to Nallacheruvu (8 km stretch) was assessed and monitored for heavy metalcontamination attributable to sewage and industrial effluents. Twelve locations wereassessed for Zn, Cr, Cu, Ni, Co, As, Hg, Cd, and Pb in soils, waters, forage grass,milk, and vegetables. A sequential extraction scheme revealed that high levels ofZn, Cr, and Cu were associated with labile fractions, making them more mobile andphytoavailable. Human risk was assessed in people exposed to pollution by analyzingmetals concentrations in venous blood and urine. Results showed high amounts ofPb, Zn, Cr, and Ni compared to permissible limits, attributable to the consumptionof contaminated food. Metals concentrations were monitored systematically to assessrisks and support management decisions to help curtail the possible entry of metalsinto human food chains. An assessment was also made of a possible analysis of aremediation technology for lead-contaminated soils and water.

Key Words: Musi River, heavy metals, food chain, human exposure, remediation.

INTRODUCTION

The Musi River, a tributary of the river Krishna, is a part of the rich culture and di-verse heritage of Hyderabad, Andhra Pradesh, India. It originates in the Ananthagiri

Received 13 October 2004; revised manuscript accepted 31 January 2005.Address correspondence to Dr. Chandra Sekhar, Head, Analytical Chemistry Group, De-fence Metallurgical Research Laboratory, Defence Research and Development Organization,Kanchanbagh, Hyderabad 500 058, India. E-mail: [email protected]

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hills, about 90 km to the West of Hyderabad city and flows through 7 mandals (eachmandal consists of 10–12 villages in general) before reaching the Osmansagar reser-voir at Gandipet. In September 1908 the river was in flood, causing heavy loss of lifeand property. Two reservoirs, Osman Sagar and Himayat Sagar, were constructed in1920 and 1927, respectively, on the river to reduce the risk of floods. These reservoirsserve today as a water sources for drinking and irrigation (EPTRI 1997; NadanavanamProject 1999). The Musi River enters Hyderabad near Rajendranagar, southwest ofthe city, dividing Hyderabad into two parts, North of Musi (New city) and South ofMusi (Old city). The Musi flows into Hyderabad as a clean resource until it reachesthe T-main sewer where 25 million liters per day (mld) of untreated sewage is re-leased. It is from this point that the river serves as little more than a sewer drain. Dueto low levels of runoff water and encroachments in the catchment and along thebanks, it resembles a drainage canal along its flow through Hyderabad. Even dur-ing monsoon, runoff inflows are very low in comparison to the quantity of sewagedischarged into the river. During monsoon the Musi River catchment area receives700–800 mm of rainfall, but because of the large inputs of sewage, self-purificationwithin the river and dilution are minimal (EPTRI 1997; Buechler et al. 1999; Sircar2000). This once beautiful and plentiful river resource has been reduced to a trickle,supplemented with drainage and sewage, converting it into a stinking drain. Due tothe rapid unplanned development of the city of Hyderabad, the quantity of sewagegenerated is many times more than the design capacity of the Amberpet SewageTreatment Plant (STP). This results in a high percentage of under-treated and un-treated sewage entering the river. The capacity of the Amberpet STP is 115 mld, butthe plant typically receives 350 mld, which includes industrial effluents (Sircar 2000;Musi River 2001; CPCB 2002).

There are 12 industrial areas within 30 km of Hyderabad city, which include elec-troplating, oil mills, lead extraction battery units, pharmaceuticals, leather, textilepaper, and others. The common effluent treatment plant (CETP), which was es-tablished for the industrial areas, is not able to treat the effluents adequately dueto their complex nature and the lack of adequate pretreatment facilities at the in-dividual industrial facilities. The CETP discharges to the STP at Amberpet, whichsubsequently discharges into the Musi River without further treatment. Individualindustries that do not send their effluents to the CETP also discharge directly into theMusi River. Organic pollutants in the river are partially eliminated by self-purificationand accessible dilution. The inorganic pollutants (heavy metals) are the fraction ofgreatest concern due to their persistence in sewage sludge, which later becomes apotential source of risk to the nearby soils and vegetation. Episodes of heavy metalpollution of the Musi River and its surroundings have been reported (Buechler et al.1999; Kumari et al. 1991; Venkateshwarulu and Kumar 1982; Bansal 1998). Along thebanks of the Musi intensive cultivation of fodder grass (para grass) and food cropsoccurs in the sewage sludge, and the concentrations of heavy metals are reported tobe very high (Kumari et al. 1991; Venkateshwarulu and Kumar 1982; Bansal 1998;Anjaneyulu 2001). Grass raised along the river is the fodder for most of the cattlein and around Hyderabad (Buechler et al. 1999; Sircar 2000). Because of these con-ditions, a methodical study was conducted to assess heavy metal concentrations indifferent environmental matrices and also to understand the potential risk to ani-mals and humans due to heavy metal exposures through the food chain. As part of

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Risk Assessment Studies of the Musi River

the study, a possible remediation method for lead-contaminated waters and soils wasinvestigated, using a plant identified as a hyperaccumulator of lead for extraction oflead from contaminated soils.

STUDY AREA

Investigations of heavy metal concentrations were conducted along and across theMusi River basin from Amberpet Bridge (station M1) to Nallachervu (station M12),including 2 km on either side of the river. Geologically the Musi basin is covered bygranites of archean age and intercalated with quartz veins here and there and is atan altitude of 500 m above mean sea level (M1) and 470 MSL (M12). The location ofthe Musi River stretch along with the 12 sampling sites (M1–M2) is shown in Figure 1.The study area consists of approximately 23.33 km2 under residential use, 4.95 km2

with plantations and harvested land, and 18.12 km2 land with scrub (Anjaneyulu2001).

EXPERIMENTAL

Materials and Methods

Reagents

All chemicals used were of analytical reagent grade. All solutions were preparedin deionized water (zero metal concentration). Calibration standards for each metalwere prepared by appropriate dilution of stock solution of 1,000 ppm of J.T. Baker/E.Merck standards.

Measurements of metal contents

Concentrations of Zn, Cu, Cr, Ni, Pb, As, Hg, Cd, and Co were measured in soil,water, vegetation, clinical samples (blood and urine), and sequentially extractedfractions by Ultra Mass 700 ICP-MS (Varian, Australia). Mathematical equations thatwere built into the software (Jarvis and Gray 1992) were used for isobaric inter-ference corrections. Canadian reference standards CANMET SO-1, SO-2 and SO-4and NIST (USA) water CRMs 1643b, 1643c, and 1643d were used to confirm theaccuracy of the analytical data. A 10% Rhodium solution of 1 mg/L concentrationwas added to all the soil, water, vegetation, milk, and clinical samples as an inter-nal standard (Balaram et al. 1992). Inter-laboratory testing was performed on allsamples by ICP-OES (Jobin Yvon Ultima, France at Defence Metallurgical ResearchLaboratory, Hyderabad) and FAAS (SpectrAA 500, Varian at National GeophysicalResearch Institute, Hyderabad). The values reported per sample are an average ofnine readings consisting of the three different instrumental techniques. Recoveryvalues in the range of ±2% were accepted, otherwise analyses were repeated. ForQA/QC of vegetation, milk, and clinical samples, due to the non-availability of CRMsin our laboratory, recovery studies were conducted using standard additions.

Sampling

Samples of ground and surface waters and soils were collected in 3 differentseasons for 2 years (January, May, and October of 2002 and 2003) following standard

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sampling procedures (Chen 1994). Samples were collected from 12 different loca-tions along and across the Musi River stretch and within a zone of 2 km on eitherside of river, covering a length of 8 km from Amberpet (M1) to Nallachervu (M12).

Surface samples (10–20 cm depth) were collected from the soil of the study areawith an 8 cm diameter hand auger; 1 kg of soil was collected for each sample. Sampleswere collected at each site in triplicate at 15 cm intervals on either side of the river.Soils were mainly red sandy loam and brownish sandy soil with black clay subsoil.Upon arrival in the laboratory, large stones and pebbles were removed, and thesample was air-dried, sieved (2 mm), and analyzed for physicochemical parametersusing standard methods (GANR 2004). HF/HClO4 digestion was used for total metalanalysis by ICP-MS.

Triplicate water samples (1L) from the surface and from the tube wells werecollected in polyethylene bottles pre-washed with nitric acid and water (1:1), followedby copious rinse with double-distilled water. Groundwater samples were collected asthe first drawn water from the hand pump of tube wells, which were already presentand being used by the local residents. Water drawn for the initial 5 minutes wasdiscarded and sample bottles were filled to the brim under overflowing conditions.The purpose of the triplicate samples is to ensure the precision of samples andanalysis. All groundwater samples were collected at a depth of 10–24 m. Immediatelyafter sampling, nitric acid (1.0 mg/L) was added to all the samples as a preservative.pH was measured on the spot with a field pH probe (Yellow Springs, USA). Thevalues presented here are an average of 18 samples, 3 samples for each season overa period of 2 years.

Vegetation

A variety of crops are grown along the Musi in the study area. The predominantcrop is forage grass/para grass (Panicum maximum) (65%), followed by coconut(Cocus nucifera) (10%), banana (Musa domestica) (15%), vegetables (9%), and others(1%) (Buechler et al. 1999). Vegetables are grown on small sections of land both forsubsistence and for sale in nearby markets. Because rice is the staple food and leafyvegetables constitute a major portion of local diets, samples of spinach (Bagella rubra),amaranthus (Amaranthus graecizans.), coriander leaves (Coriandrum sativum), mintleaves (Mentha spicata), and other vegetables including ladies finger (Abelmoschusesculentus), brinjal (Solonum melengina), and ginger (Zingiber officinale) were collectedat marketable stages of development to assess the human dietary intake of heavymetals. Also, forage grass samples from the 12 sampling sites were collected andanalyzed for total metal content. All vegetation samples were washed carefully underrunning water, followed by double distilled water. One gram of dried (65◦C) samplewas wet ashed (HNO3/ HClO4/H2SO4 10:1:1) and solutions were made up to 50 ml(Bech et al. 1997) and analyzed for metals content.

Milk

A major part of land in the study area is used for fodder cultivation. Approximately60% of the fodder grass grown is sold at market. The other 40% is used directly by thefarmers for their livestock. Buffalo’s milk is locally preferred over cow’s milk, and hasrelatively low cholesterol and high fat content (Ismail 2004; Indian Dairy 2004). Thus,


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most of the fodder is consumed by buffaloes (Buechler et al. 1999, 2002; Buechler andDevi 2003). The forage grass harvested along the river is chopped into small piecesand fed to the cattle. As mentioned previously, this is the only fodder for the cattleof Hyderabad. Milk samples were collected soon after calving during early hours ofthe day before milking. Samples of milk (200 ml) were collected from buffaloes aswell as cows fed on forage grass. Milk samples were collected in sterile polyethylenesampling bottles with KMnO4 as preservative. No pretreatment was given to thesamples. After collection, the samples were transferred to the lab in an ice-coldbox and then digested for metals analysis. Milk samples were digested followingthe method suggested by Ayyaduria et al. (1998). For reference samples, milk wascollected from cattle that were fed on pastures away from the city of Hyderabad.

Control samples

Samples of water, soil, forage grass, and vegetables were collected from the resi-dential campus area of our research laboratory covering an area of 18 km2, whichis free from obvious sources of industrial and vehicular pollution. This area is onthe outskirts of the city of Hyderabad and is distant from the most intense pollutionzone. The campus area is situated 7 km away from the main road, which forms a sub-route from the national highway, and traffic density is very low. Because this campusis located in a residential area, movement of heavy vehicles is restricted, which helpsminimize pollution. All the samples were collected in triplicate from 10 differentsampling sites in this area.

Fractionation studies of soil

A six-step modified Tessier sequential extraction scheme (Chwastowska andSkalmowski 1997) for the extraction of metals in soil samples was used for assess-ing the mobility of the metals. As the concentrations of As, Hg, and Cd are very low,fractionation studies were not performed for these three metals in the present study.

Human Exposure Assessment

Residents of the study area and people who consume milk from cattle fed onlocally grown forage grass were asked to complete a questionnaire. The questionsincluded their occupation, duration of stay, their diet and its source, and they wereasked to keep a dietary document of the precise food and drinks ingested over aperiod prior to providing blood and urine samples. As the migration of populationis significant, samples were collected from residents only if their length of residencein the community was more than 5 years.

Urine samples and venous blood samples were collected from people of varyingage groups and analyzed for metals content using ICP-MS (Chandra Sekhar et al.2000). Upon collection the venous blood and urine samples were placed in an icecool box (4◦C), transferred to the lab, and then refrigerated until further analysis.Samples were digested according to the method suggested by Chandra Sekhar et al.(2000).

For control, samples of blood and urine were collected from 30 participants re-siding in the campus area of our research laboratory and from the authors.


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RESULTS AND DISCUSSION

Soil

The pH of the soil examined ranged from near neutral to moderately acidic(M3 and M9) cation exchange capacity (CEC) ranged between 22.7 to 33.3 c.molkg−1, respectively. CEC did not vary much in these 12 sites, however, a low CEC wasreported for site M6 (22.7 c. mol kg−1), indicating low metal retention potential atthis location. Organic matter was high due to constant sewage flows and rangedbetween 7.9–10.9%. Metal retention was found to be high in almost all the sites dueto high percentage of organic matter, which is in concurrence with our fractionationresults. The metal contents of the soil along with the normal ranges and permissiblelimits for agricultural and residential purpose and background values are presentedin Table 1. As the concentrations of As, Hg, and Cd were appreciably low comparedto the permissible limits, these metals were not considered in the risk assessmentstudies.

Fractionation of Soil

Whether an element is present naturally in the soil or has been introduced bypollution, a measure more useful than total elemental content for most purposes isan estimation of “availability” or “lability” of the element (McBride 1994). It is thisproperty that can be related to mobility and uptake by plants and extractability bychemical treatments. Chemical soil tests are designed to extract a quantity of elementfrom the soil solids that correlates statistically to the size of the “available pool” inthe soil defined by the quantity of element taken up by the plants (Earnest 1984).The mobility and phytoavailability of metals are governed by soil properties thatinclude pH, composition and content of organic matter, clay minerals, Fe-Mn andAl oxides and hydroxides, redox potential and cation exchange capacities (Berrowand Burridege 1991; Salomans and Stigliani 1995). Chemical extraction techniques

Table 1. Environmental quality criteria for soils compared with Musi soils(µg/g).

Musi soil values

Concentrations fromBackground values@ our study area

Zn 200 250 1–100 6.5–13 26–60 227–401Cr 8 8 0.03–14 2.7–8.5 1.4–2.5 26–38Cu 150 100 5–20 1.8–5.7 12–30 21–35Ni 60 80 0.02–5.2 0.9–2.3 10–20 33–63Co 40 40 5–20 6.5–13 4–10 12–19Pb 200 300 5–15 11–23 15–25 303–637As 10 20 0.2–10 0.002–0.01 0.3–0.8 0.08–0.14Hg 0.8 2 0.05–5 0.005–0.01 0.03–0.2 0.03–0.06Cd 3 5 0.25–15 0.01–0.08 0.04–0.5 0.12–1.12

$: Ashwathanarayana (1999); #: Alloway (1990); Mc Bride (1994); @: Venkateshwarlu(1981); Venkateshwarulu and Kumar (1982); Syamala (1999); Stephanie (2002).


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provide a well established means of identifying and characterizing different fractionsof heavy metals in the soil (Evans 1989; Van Straalen and Denneman 1989; Ure et al.1995). Results of the geochemical partitioning using a modified Tessier schemerevealed high concentrations of Zn, Cr, and Cu to be associated with the mobilefraction of the soil. The sum of metal extracted in each sequential extraction schemewas compared with the total digestion procedure for the recovery studies.

Nearly 40% of zinc was associated with readily soluble and exchangeable frac-tions. Locations M5, M7, and M9–M11 showed high concentrations of zinc in mobilefractions attributed to the high CEC values of the respective sites, in agreement withearlier studies (Ramos et al. 1994). The organic bound fraction was also found to behigh at these sites, which is in concurrence with the percentage of organic matterin the soils. Chromium was associated with mobilizable fractions (30–35%) and 10–12% of chromium was associated with organic matter of soil. Approximately 10% ofCr was associated with the carbonate bound fraction, which may become availableto plants with changes in pH and Eh of respective soils (Kimbrough et al. 1999). ForCu, only 15–25% was bioavailable. High CEC values are reported to release Cu, mak-ing it mobile. In the soils of the present study, CEC values were reported to be low,resulting in moderate mobility of the metal. For Co and Ni, major portions of thesemetals were associated with the non-mobile fraction of soil. Only 10–20% of Co andNi were associated with labile fractions. These two metals are reported to mobilizein acidic soils. Because Pb binds strongly with organic matter and chemisorbs onoxides of Fe, Mn, and Al, it is a low mobility metal in soil. Studies have reported thataccumulation of Pb in plants occurs only with high concentrations of lead in soils(Cambier 1997; Chandra Sekhar et al. 2001). All the samples along the Musi Rivershowed 75–80% lead associated with non-mobile fractions due to the high organiccontent of the soils. Because the soil concentration of lead was very high, the nearbyvegetation is prone to accumulate lead.

Based on these fractionation studies of metals using a modified Tessier scheme in12 soil/sludge samples, the elements under study can be arranged in the followingorder from more bioavailable to less bioavailable.

Zn > Cr > Cu > Ni > Co > Pb

Surface Water and Groundwater

The pH of surface and groundwater ranged between 6.9–7.7 throughout the studyarea. The heavy metal concentrations were low and well within the permissible limitsof the irrigation water quality, confirming findings of earlier studies (Venkateshwarlu1981; Buechler et al. 1999; Anjaneyulu 2001).

Hydrogeological Conditions

The study area is in hard rock terrain where groundwater is available under watertable conditions. Water table fluctuates in an undulating fashion generally followingthe topography. Open wells are dug to weathered rock, and tube wells penetrate thefractured portion in which water is under semi-confined conditions (Prem Chandet al. 2002). There seems to be a connection between weathered layers and fractured


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layers, as it was observed that whenever over-pumping through tube wells occurs,nearby dug wells become dry (Anjaneyulu 2001; Venkateswara Rao et al. 2001).

The water table is situated in the weathered zone and the fractured zone withgreater thickness (Venkateswara Rao et al. 2001; Anwar et al. 2002). The facturedzone thickness and weather zone thickness is reduced moving downstream alongthe Musi following the topography (M1 to M12). As we move down stream, the leftbank (M3, M6, M7, M10, M12) and aquifers are at a lower elevation compared to theright bank (M1, M2, M4, M5, M8, M9). The aquifers have greater thickness on theleft bank, therefore in general the left bank is more susceptible to groundwaterpollution (Anjaneyulu 2001; Venkateswara Rao et al. 2001; Prem Chand et al. 2002;Anwar et al. 2002). In addition, the right side is underlain by both factured rockand solid basement (Venkateswara Rao et al. 2001). It can be concluded from theseobservations that pollutants entering at the surface on either side of the river willmigrate toward the river and ultimately travel downstream toward Nallachervu (M12).Our results clearly indicate that metals concentrations are higher in groundwaterthan in surface water. Groundwater samples showed higher concentration of metalsin location numbers M3, M6, M7, and M10–M12 when compared to those on the rightside of the river. Among the six metals studied, concentration of lead and zinc werehighest. Lead contents in groundwaters ranged between 4.2–10.2 µg/mL and zinc inthe range of 2.4–8.9 µg/mL. Concentration of metals were also found to be higherat sampling site M5(Pb = 9.2; Zn = 7.2 µg/mL), which may be attributed to anindustrial effluent channel confluence with the Musi at this point that has resultedin percolation of metals into groundwater.

Forage Grass

Table 2 presents concentrations of metals in forage grass samples along with thenormal range of metal accumulation in plants and control values. These data arefurther assessed by calculating the plant-to-soil ratios commonly known as transfercoefficients, a convenient way of quantifying relative differences in bioavailability of

Table 2. Metal concentration in fodder grass (µg/g) and plant soil transfercoefficient values.

Transfer coefficientGeneral transfer Musi fodder values from Musi

Metal Normal ranges ∗ coefficient values # Control values grass values river plant

Zn 1–100 1–10 2.4–8.2 164.2–212.4 0.53–0.68Cr 0.03–14 0.01–0.1 0.06–0.91 20.2–36.7 0.70–0.95Cu 5–20 0.01–0.1 0.02–0.26 15.7–29.6 0.76–0.84Ni 0.02–5 0.01–1.0 0.23–1.6 10.7–18.3 0.29–0.38Co 2–10 0.01–0.1 0.01–0.11 3.7–7.1 0.28–0.33Pb 5–10 0.01–0.2 2.8–10.6 66.7–101.7 0.21–0.35As 0.02–5 0.01–0.1 0.006–0.08 0.002–0.006 0.03–0.07Cd 0.1–2.4 1–10 0.005–0.05 0.03–0.06 0.05–0.11Hg 0.005–0.17 0.1–1 BDL 0.01–0.04 0.01–0.04

∗Kabata-Pendias and Pendias (1984); # Kloke et al. (1984); Alloway and Ayres (1993); BDL:Below detection limit.


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metals to plants. Farago and Thornton (1997) considered that plant/soil ratios forany particular element of 0.1 indicate that the plant is excluding the element fromits tissues. Although soil concentrations may be high and source metals may be takenup in the roots, only a portion of the root uptake is translocated to the leaves, givinga leaf/soil concentration ratio of about 0.2. Based on this, we suggest that transferfactors above 0.2 indicate anthropogenic contamination of the plants. Kloke et al.(1984) gave a generalized transfer coefficient for soils and plants based on the rootuptake of metals. However, soil pH, soil organic matter, CEC, and plant genotypecan markedly affect metal uptake. The generalized coefficients were in concurrencewith the studies of Forago and Thornton (1997) except for Cd and Zn, which hadmaximum transfer factors of 10. This is due to high mobility and phytoavailabilityof these two metals, which is a reflection of their relatively poor sorption in soils. Incontrast, metals such as Ni, Co, and Pb have low transfer coefficients because they arestrongly bound, usually to the soil colloids. The results of our study (Table 2) werein good agreement with the earlier two hypotheses and that of our fractionationstudies of soils, which clearly indicates high concentration of Zn, Cu, and Cr inplants and high transfer coefficient values compared to Ni, Co, and Pb. Table 2 alsocontains the metal concentrations in control samples, which is generally free fromanthropogenic contamination. Among As, Cd, and Hg, the highest transfer factorwas recorded for Cd, a reflection of its relatively high mobility and phytoavailabilityin soil.

Milk

Concentrations of metals in milk are presented in Table 3, which clearly indicateshigh concentrations of all six metals and of Zn, Cu, Cr in particular. The concentra-tion of cadmium ranged between 0.02–0.04 µg/mL in milk samples, a consequenceof the values in the forage grass. Concentrations of metals were high in buffalo milkcompared to cow milk and this can be attributed to the high fat content in buffalo’smilk (Indian Diary 2004), which helps in metal retention due to the formation ofbioactive (lipophilic) complexes (Leeuwen and Pinheiro 2001; Buechler et al. 1999,2002). These concentrations of metals in milk are clear reflections of the fraction-ation data and respective concentrations in forage grass. Repeatedly feeding this

Table 3. Concentration of metals in milk (µg/mL) from the study area.

Metal Control Cow’s milk Buffalo milk

Zn 0.06–1.0 1.9–4.3 2.7–6.3Cr 0.06–0.08 1.2–2.7 1.6–3.9Cu 0.03–0.06 0.96–2.2 1.1–2.4Ni 0.02–0.05 0.69–2.0 0.8–1.9Co BDL 0.4–0.9 0.6–1.1Pb 0.03–0.09 1.4–3.9 1.6–4.9As BDL BDL BDLCd 0.0001–0.002 0.02–0.03 0.02–0.04Hg BDL BDL BDL

BDL: Below detection limit.


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forage grass as fodder to cattle may result in the exposure of humans through thefood chain (Chandra Sekhar et al. 2003a).

Vegetables

Table 4 presents the concentration of metals in samples collected from the MusiRiver, along with control samples. From the values it is clear that Zn, Cr, Ni, andPb are in high concentrations, making them a direct source of human exposure.Concentrations of Hg and As were found to be below the detection limit, whereasthe Cd concentrations ranged between 10–50 µg/kg. Concentration factors (CF)were calculated using the equation suggested by Chandra Sekhar et al. (2003a) andpresented in Table 4 from which it can be concluded that Zn, Cr, and Pb show highCF compared to other metals. Because pesticides are not in use and air pollution inthis area is minimum (Anjaneyulu 2001; Buechler and Devi 2003), the concentrationof metals in vegetables is generally from soils.

A comparison of heavy metal concentration in soils and waters of the Musi Riverdrainage and its surrounding environs from earlier studies with our study is pre-sented in Table 5. The table clearly indicates the degraded status of Musi and sur-rounding environs with the potential amplification of heavy metal concentrationsfor a consecutive 5-year period. Our studies clearly indicate the progressive increaseof metal concentrations in the past 5 years.

Human Exposure Pathways

For each of the metals there exist several exposure pathways that depend onthe particular contaminated media of air, water, soil, and food and on the receptorpopulation (Caussy et al. 2003). Food is an important pathway for several metals,particularly in populations consuming regionally contaminated foods. This wouldbe true for people consuming vegetables or grains grown on soils contaminated withmetals.

To understand the risk and associated hazard due to heavy metal toxicity and assessadverse effects on human health, samples of blood and urine were collected from 105male and female participants of different age groups. In Figure 2 are presented theage-to-sex distribution of the participants exposed to pollution. Metal contents wereanalyzed using ICP-MS and the results are presented in Table 6. It is evident fromour questionnaire that the participants are exposed to metal pollution and peoplein the age group of 35–60 years were found to be most affected. The participantshad a variety of reactions indicating possible health risks. Irritation of skin with blackrashes was among the commonest symptoms, which may be attributed to exposureto Pb, Cr, and Zn (Abbasi et al. 1998; Syamala 1999). Urban and periurban farmersare less exposed to contaminated water and soils than rural farmers, who spendlong hours standing in sewage waters and sludges during puddling, transplanting,and harvesting (Buechler et al. 1999; Sircar 2000; Buechler et al. 2002; Buechler andDevi 2003). Concentrations of Pb, Zn, Cr, and Ni were high in the blood and urinein the aforementioned age group with higher concentrations in males compared tofemales. Earlier studies on toxic metals in farmers working on sludge farms (Srikanthet al. 1994) indicated high concentrations of Pb, Zn, and Cr. The high concentrationof metals in blood and urine of the participants compared to control individuals


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Tab

le4.

Con

cen

trat

ion

ofh

eavy

met

als

inve

geta

bles

(µg/

g,dr

y.w

t)an

dco

nce

ntr

atio

nfa

ctor

.

App

roxi

mat

ein

take

byh

uman

Vege

tabl

es(g

/wee

k)dr

y·w

t(@

)Z

nC

rC

uN

iC

oPb

Spin

ach

1.6–

11.2

0.6–

3.1

0.1–

1.1

0.2–

3.6

0.06

–0.1

71.

3–3.

6C

ontr

ol0.

06–0

.09

0.03

–0.0

50.

02–0

.03

0.00

1–0.

02B

DL

0.05

–0.0

9C

F1.

60.

670.

230.

140.

060.

99A

mar

anth

us1.

2–8.

90.

8–2.

90.

1–1.

70.

17–3

.30.

03–0

.11

1.1–

3.1

Con

trol

0.04

–0.0

60.

02–0

.04

0.01

–0.0

20.

002–

0.01

BD

L0.

04–0

.09

CF

1.2

0.54

0.21

0.1

0.04

1.1

Min

tlea

ves

1.3–

6.7

0.3–

1.7

0.2–

1.3

0.2–

2.9

0.02

–0.0

60.

9–2.

7C

ontr

ol0.

02–0

.06

0.00

4–0.

020.

002–

0.01

BD

LB

DL

0.03

–0.0

8C

F0.

940.

610.

210.

080.

030.

81C

oria

nde

rle

aves

1.1–

5.8

0.2–

2.4

0.3–

1.6

0.1–

3.1

0.01

–0.0

40.

6–3.

4C

ontr

ol0.

03–0

.06

0.02

–0.0

40.

005–

0.02

0.00

2–0.

005

BD

L0.

02–0

.05

CF

0.71

0.55

0.22

0.1

0.02

0.69

Gin

ger

2.3–

12.9

0.6–

4.1

0.2–

1.8

1.1–

4.5

0.06

–1.1

1.9–

6.5

Con

trol

0.06

–0.2

60.

05–0

.10.

01–0

.06

0.00

2–0.

06B

DL

0.02

–0.2

1C

F1.

60.

740.

440.

210.

031.

11B

rin

jal

1.1–

4.9

0.2–

1.3

0.2–

0.9

0.7–

3.4

BD

L0.

8–3.

4C

ontr

ol0.

02–0

.09

0.01

–0.0

5B

DL

0.02

–0.0

5B

DL

0.03

–0.0

8C

F0.

660.

480.

050.

09B

DL

0.54

Lad

ies

fin

ger

1.3–

3.7

0.1–

1.7

0.3–

0.7

0.6–

2.7

BD

L0.

61–4

.1C

ontr

ol0.

05–0

.10.

005–

0.02

0.01

–0.0

50.

02–0

.05

BD

L0.

06–0

.11

CF

0.81

0.59

0.06

0.02

BD

L0.

61

CF:

Con

cen

trat

ion

fact

or;B

DL

:Bel

owde

tect

ion

Lim

it;@

Bas

edon

the

data

colle

cted

from

the

ques

tion

nai

re.

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Table 5. A contrast of heavy metal concentrations in soils and waters of Musi andsurrounding environs.

Previous studies∗ Present study

Soil Groundwater Surface Soil Groundwater Surface(mg/kg) (mg/L) water (mg/L) (mg/kg) (mg/L) water (mg/L)

Zn 63–126 0.8–1.6 0.6–1.2 227–401 2.6–7.6 1.1–2.6Cu 8–16 0.6–1.1 0.4–1.4 20–35 1.7–6.3 1.1–2.9Cr 7–18 0.5–1.8 0.3–0.8 26–38 2.2–5.9 0.9–3.1Ni 12–28 0.4–0.9 0.1–0.5 33–63 2.7–7.2 0.1–0.8Pb 22–280 0.9–3.4 0.2–2.1 303–637 4.1–10.1 1.3–3.9Co 6–10 0.5–1.1 0.2–0.6 12–19 2.3–6.3 0.4–0.9

∗(Srikanth and Reddy (1991); Srikanth et al. (1992); Syamala (1999); Anjaneyulu (2001).

(Table 6) may be attributed to the consumption of contaminated vegetables, milk,and other foods. Due to slow accumulation rates of these metals in the human body,concentrations were found to be higher in the age group of 35–60. From our surveyand questionnaire it is evident that the participants are exposed to higher-than-acceptable concentration of metals.

REMEDIATION FOR LEAD CONTAMINATION

Waters from the Musi Study Area

Our group has identified a plant, Hemidesmus indicus, for the removal of leadfrom aqueous solutions (Chandra Sekhar et al. 2003b). Experiments were conductedfor the removal of lead from contaminated ground and surface waters using theimmobilized biomass of this plant for better recovery and regeneration. Resultsindicate that immobilized plant biomass (IPBFIX) under certain flow conditions can

Figure 2. Age to sex distribution of the participants.


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Tab

le6.

Con

cen

trat

ion

ofm

etal

sin

clin

ical

sam

ples

(µg/

L).

Hea

vym

etal

con

cen

trat

ion

ran

ge

Exp

osed

Zn

Cr

Cu

Ni

Co

PbA

sC

dH

g

Blo

od Age

/Yrs

No.

ofsa

mpl

es10

–30

3595

0–10

5676

5–99

688

9–11

5039

0–66

526

0–42

065

5–89

516

–22

10–1

611

–23

30–4

530

1200

–125

6010

00–1

540

1265

–145

056

0–88

930

0–45

576

6–14

5047

–106

20–3

545

–107

45–6

035

1000

–950

011

00–1

452

1150

–155

090

0–11

5041

0–56

696

5–13

6082

–165

28–4

288

–145

Con

trol

10–3

015

225–

340

220–

310

310–

452

110–

275

89–1

2922

0–31

0N

FN

FN

F30

–45

1031

0–45

635

2–42

026

6–51

032

4–39

811

0–19

933

5–66

915

–32

10–2

330

–40

45–6

012

369–

490

254–

366

355–

500

300–

434

140–

210

665–

720

30–4

015

–22

46–5

5Pe

rmis

sibl

elim

its

#80

–400

50–2

0060

–240

40–1

1038

–99

60–3

0010

–20

Uri

ne

Age

/Yrs

No.

ofsa

mpl

es10

–30

3540

–100

30–1

1020

–60

10–4

412

.5–2

545

.3–9

9.5

NF

NF

NF

30–4

530

60–3

8042

–290

52–1

1037

–89

28.3

–43.

860

.5–1

86.3

10.4

–49.

210

–25

1.6–

6.6

45–6

035

100–

760

65–3

9576

–283

53–1

2541

.3–9

4.2

75.3

–289

44.2

–80.

222

–40

2.7–

10.2

Con

trol

10–3

015

1.1–

2.7

2.2–

6.5

1.7–

6.3

NF

NF

20–6

5N

FN

FN

F30

–45

1010

–40

20–4

415

.8–5

5.3

2.2–

103.

3–6.

944

.3–8

3.6

10.2

–16.

6N

FN

F45

–60

1230

–90

65–1

1048

–100

20–4

6.3

25–4

5.3

75.3

–105

.715

.5–2

2.8

10.2

–17.

11.

6–5.

2Pe

rmis

sibl

elim

its

$20

–100

30–1

5030

–120

50–8

025

–90

30–1

0015

–25

NF

=N

otfo

und;

#A

bbas

ieta

l.(1

998)

;$Iy

enga

r(1

984)

.

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Table 7. Phytoremediation of lead from five different contaminated sites of Musi.

Concentration of Pb taken up by plant (µg/g)

Root Shoot Total

M2 540 (200)∗ 106.2 ± 2.3 80.3 ± 1.5 186 ± 2.6M5 577 (206)∗ 110.5 ± 2.9 82.6 ± 2.3 192 ± 3.1M6 623 (211)∗ 100.2 ± 1.3 83.4 ± 2.2 183 ± 2.2M7 637 (220)∗ 114.6 ± 2.2 83.7 ± 1.3 197 ± 1.9M9 583 (215)∗ 116.3 ± 3.1 75.4 ± 2.8 191 ± 2.1

∗Phytoavailable fraction; All values are a mean of three different experiments.

yield 99.8% removal of lead from ground as well as surface water samples (ChandraSekhar et al. 2004a). An attempt was made to remove lead from the ground andsurface waters of the present study area using IPBFIX and it was observed that 100%of lead could be removed from the waters successfully (Chandra Sekhar et al. 2004a).

Soils from the Musi Study Area

Tests were also conducted for the phytoremediation of lead contaminated soilsof Musi using this plant under laboratory conditions (“pot studies”). Soil samplesfrom five different sites (M2, M5, M6, M7, M9) were collected and pot experimentswere conducted to test the lead decontamination potential of Hemidesmus indicus.Results reveal efficient removal of lead from contaminated soil (Table 7). Studiesare underway for the decontamination of chromium and zinc from contaminatedwaters and soils and will be communicated separately.

CONCLUSIONS

The information presented in this article is a systematic evaluation of the metalpollution status of the 8-km Musi River stretch from Amberpet (M1) to Nalla Cheruvu(M12). Results of the periodic monitoring of metals concentrations of soils, waters,vegetation, milk, and human exposure studies are presented and discussed. Thisstudy confirms the degraded quality of the river and its environs. Concentrations ofmetals were found to be high in soils with special reference to Pb and Zn content,which were found to be very high. Much research has been conducted on the effectsof heavy metals on soil and vegetation attributed to sewage irrigation (Bansal 1998).The pH of surface waters was near neutral, which resulted in low metal concentra-tions in river waters. The groundwater concentrations of metals were found to behigh and in agreement with topography and slope, which resulted in higher concen-trations of metals on the left side of the Musi River (M3, M6, M7, M10–M12). Due toreduced thickness of fractured and weathered zones, the left bank is more suscep-tible to metals contamination. From these studies we infer that pollutants enteringthe surface on either side of the Musi will migrate toward the river and ultimatelytravel down stream to the north east, that is, M10–M12. The fractionation studies ofsoil clearly indicate that Zn, Cr, and Cu are more mobile and in other ways morephytoavailable, reflected by high plant transfer coefficients. Srikanth et al. (1992)


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conducted studies on forage grass cultivated in sewage sludge along the banks ofthe Musi River and reported accumulation of heavy metals by the fodder grass. Thesame authors further reported high concentrations of Pb, Cr, and Zn in variousvegetables grown on urban sewage sludge, indicating possible health hazards forconsumers (Srikanth and Reddy 1991). As this forage grass is fed to most of thecattle in and around Hyderabad, the risk of metal toxicity is not limited to the Musienvirons. Our studies clearly indicated high concentrations of metals in vegetablesgrown on the banks of the Musi River. Samples of milk collected from cattle fed oncontaminated grass indicated high amounts of Zn, Pb, and Cr, which is in agreementwith studies conducted by Ayyadurai et al. (1998).

Analysis of human exposure pathways revealed that concentrations of Zn, Pb, Cr,and Ni are in higher concentrations than the permissible limits (Abbasi et al. 1998;Iyengar 1984) in the participants of the study area. In general it is very difficult todraw a correlation between metals contents of blood and urine with age and num-ber of people. Many factors such as intake of metals-contaminated water, quality ofmetals-contaminated food (vegetables, milk), health and financial status of people,and nutritional quality of food all play important roles. The results of the currentstudy will be helpful for the local pollution control authorities and policy-makers inmanaging the intrusion of industrial effluents into the Musi River. Further, remedialmeasures may be taken to abate the metal pollution and also restrict the cultivationof vegetables on contaminated soils.

Even though As, Hg, and Cd are very important from the point of ecotoxicologicalstudies, we did not perform a detailed study due to their low concentrations in thesoil, water, vegetation, and the clinical samples. It is surprising to see As and Hg inblood and urine samples, whereas these metals are absent in milk and vegetation,which are the main sources of entry into the human food chain. The authors are notable to identify the source of these two metals (As and Hg) as there are no knownindustrial sources for them. Further study of this matter is required.

ACKNOWLEDGMENTS

The authors are grateful to the Director, Indian Institute of Chemical Technology,for his encouragement and for providing the facilities for carrying out this work andpermitting us to publish our findings. The authors are thankful to Dr. V. Balaram,Deputy Director, NGRI, Hyderabad, for extending the support for inter-laboratorytesting. Two of the authors (N. S. Chary and C. T. Kamala) thank the Council for Sci-entific and Industrial Research (CSIR), India, for providing fellowship for carryingout this work. The authors are thankful to Dr. A. Siva Shanker, Research Associate,Jawaharlal Nehru Technological University, Hyderabad, for his help in preparationof the maps.

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