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Review article
Occurrence, distribution and possible sources of organochlorine pesticide residues intropical coastal environment of India: An overview
S.K. Sarkar a,⁎, B.D. Bhattacharya a, A. Bhattacharya a, M. Chatterjee a, A. Alam a, K.K. Satpathy b, M.P. Jonathan c
a Department of Marine Science, University of Calcutta, 35 Ballygunge Circular Road, Calcutta 700019, Indiab Indira Gandhi Center for Atomic Research, Environmental and Industrial Safety Section, Safety Group, Kalpakkam 603102, Tamil Nadu, Indiac Centro de Investigaciones en Ciencias de la Tierra, Universidad Autonoma del Estado de Hidalgo, Ciudad Universitaria, Cerratera Pachuca-Tulancingo Km. 4.5, Pachuca, Hidalgo,C. Postal. 42184, Mexico
Article history:Received 27 September 2007Accepted 20 February 2008Available online 18 April 2008
Organochlorine pesticides (OCPs) are an important potential component of chemical pollutants usedextensively for agriculture and sanitation purposes in India as these are comparatively cheap and effective.These persistent organic compounds such as HCH isomers, DDT and its metabolites are the predominantchemical contaminants found along the Indian coast and thus constitute both alluring and grave areas ofscientific research. Our objective in the paper is to provide a comprehensive account of the distribution oforganochlorine pesticides in biotic and abiotic compartments of the Indian coastal environment, make somecomments on their environmental sources, their movement through the food chain and possibleecotoxicological risk of health in biota including humans.The prevalent HCH, DDT and HCB concentrations differ markedly in eastern and western coast of Indiareflecting differing agricultural and other usage and their ultimate input into the coastal environment byseveral rivers and the bioturbation activities of macrozoobenthos (bivalve mollusks, polychaetous annelids,etc.). In several cases, the DDT levels exceeded the effects range-low (ER-L) and could thus cause acutebiological impairments, in comparison with the sediment quality guidelines. Contributions of DDTmetabolites (DDT, DDD and DDE residues) vary in different Indian coastal regions predominated by pp′-DDT and pp′-DDD. Measured concentrations of HCHs were lower than DDTs that might be due to higher watersolubility, vapor pressure and biodegradability of the latter. HCH and DDT residues in fish in India were lowerthan those in the temperate countries indicating a lower accumulation in tropical fish, which might be relatedto rapid volatilization of this insecticide in the tropical environment. The concentrations of other chlorinatedpesticides (aldrin, dieldrin, eldrin, methoxychlor, endosulfan sulphate) were lower and not generally of greatconcern.
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1. Introduction
Persistent organic pollutants (POPs) such as organochlorines havebeen of great concern due to their occurrence in high concentrationeven in remote ecosystems, despite bans on production and usage(Iwata et al., 1994; Guruge and Tanabe, 2001). Organochlorinepesticides (OCPs) such as hexachlorocyclohexane (HCH) and 1,1,1-trichloro-2,2′-bis(p-chlorophenylethane (DDT) are ubiquitous anthro-pogenic environmental contaminants (Willett et al., 1998; Nakataet al., 1998). They are persistent, broad-spectrum toxicants thataccumulate in the food web with high risks to the ecosystem andhuman health. Many of these compounds are considered to act ashazardous environmental hormones, which disrupt reproductivecycles of humans and wildlife (Colborn and Smolen, 1996). Somedeveloping countries are still using these compounds because of theirlow cost and versatility in industry and agriculture for sanitationpurpose (Tanabe et al., 1994). Consequently, environmental problemsassociated with toxic contaminants in these countries are of greatconcern. It is reported that approximately three million people arepoisoned and 200,000 died each year around the world from pesticidepoisoning, and a majority of them belongs to the developing countries(WHO, 1990; FAO, 2000). It is also believed that in developingcountries, the incidence of pesticide poisoning may even be greaterthan reported due to under-reporting, lack of data and misdiagnosis(Forget, 1991).
India (Lat. 8°4′ N and 37°69′ N and Long. 68°7′ E and 97°25′ E), atropical south Asian country, has a stretch of ~7500 km coastline,excluding its island territories with 2 million km2 exclusive economiczone (EEZ). There are 14 major, 44 medium and 162 small rivers inIndia, with a mean annual run-off of 1645 km3, although not all theserivers discharge into the sea. The Arabian Sea and the Bay of Bengal aresubject to large semi-diurnal tides with amplitudes of 1–8 m and arealso influenced by the biannual reversal of the monsoonwinds. Thesetwo factors result in the flushing of Indian coastal areas which furtherhelp in dispersing pollutants (Glassby and Roonwal, 1995). Thecatastrophic effects of tsunami and supercyclones also play a majorrole in changing the coastal morphology and sediment dispersalpatterns (Bhatterchaya, 2003).
In India, organochlorine pesticides (OCPs) especially DDT and HCHwere used extensively till recently both for agricultural and sanitarypurposes (Pandit et al., 2001; Kumar et al., 2006). It is estimated thatabout 25,000 MT of chlorinated pesticides was used annually in Indiaand DDT accounted over 40% of this group (Mathur, 1993). Althoughsubstantial portions of applied pesticide are dissipated at the site ofapplication through chemical and biological degradation processes.Still, a reasonable fraction of the OCPs residues reaches the oceansthrough agricultural run-off, atmospheric transport and seweragedischarge (GESAMP, 1989). Because OCPs are known for theirpersistence, toxicity and bioaccumulation characteristics, there is aconcern about their impact on themarine environment. The transport,dispersion and finally the ultimate effects of pesticides in marinesystems depend upon the persistence of the chemicals under tropicalconditions and their bioaccumulation and biodegradation. Althoughpesticide consumption is low in India compared to the otherdeveloped countries, the indiscriminate use of these pesticides hasresulted in sporadic occurrence of the residues in biota and otherabiotic compartments. In order to understand the role of tropicaldeveloping countries as possible emission sources of POPs, it isnecessary to elucidate the distribution, behavior and fate of thesecompounds in various environmental compartments. The determina-tion of those compounds existing in water and sediment may indicatethe extent of aquatic contamination and the accumulation character-istics in the aquatic ecosystems. Hence an attempt has been made toelucidate the distribution, behavior and fate of these compounds inIndian coastal regions which are characteristically different ingeomorphological and hydrological set up with varying anthropo-
genic stresses. Authors have extracted data from different depart-ments, published literature in research journals and National reports.
1.1. Aquatic systems
OCPs can enter the aquatic system in a variety of ways, includingrun-off from non-point sources, discharge of industrial and seweragewastewater and wet/dry deposition. Because of their persistence,OCPs inwater can be transferred into the food chain and accumulate inaquatic organisms like plankton and thus enter the food chain.
In the middle stretch of the Ganges river, Nayak et al. (1995)observed DDT concentration in water exceeding the WHO prescribedsafe limit of 1 μg/l which might be attributed to enhanced municipalpublic health activities than the agricultural pest managementactivities during monsoon period.
Ramesh et al. (1990a) and Rajendran and Subramanian (1997)measured DDT and HCH residues in several rivers of South India.Neither study found significant changes in DDT residue concentra-tions in waters of the river Vellar, Kaveri and Coleroon or in thePichavaram mangrove wetland based on seasonal changes, wet or dryseason or summer, pre-, post- or monsoon season. However, therewasa significant increase in mean Σ-HCH levels during the wet season forthe Vellar River and the Pichavaram mangroves (Ramesh et al., 1990a)and among pre-monsoon season for the rivers Kaveri and Coleroon(Rajendran and Subramanian, 1997). The increase in Σ-HCH concen-trations corresponding with the time of increased agricultural use ofthe pesticide and the absence of a similar pattern of ΣDDT stronglysuggests that farmers for pest control are not employing DDT nor is itbeing excessively employed in public health programs in South India.
In west coast of India, Pandit et al. (2002) measured concentrationof HCH (range 0.16 to 15.92 ng/l) and total DDT (3.0 to 33.2 ng/l). Theelevated concentration of DDT in comparison to its metabolitesdichlorodiphenyldichloroethylene (DDE) in the seawater samplesindicates the freshwater input of DDT. The presence of HCH isomersand DDT and its metabolites can be attributed to the use of theseinsecticides in agricultural and anti-malaria sanitation activities,carried out throughout the country.
There is scarce literature on pesticide residues in seawater aroundIndia. However, a detailed comparative account of pesticide residuesinmarine, estuarine and freshwaters has been shown in Table 1whichdelineates wide variations between different regions as well asdifferent pesticides. Venugopalan and Rajendran (1984) reportedpesticide concentration ranges in Vellar estuarine water (southeastcoast of India) which ranged, for total ΣDDT (DDT+DDE+DDD) of 1.6to 14.1 ng/l, for lindane of 0.09 to 2.8 ng/l, and for endosulfan of 0.02 to1.4 ng/l. Their observations did not show any definite seasonalvariations for any of the pesticides monitored. The authors attributedthe low residue concentrations in water to high surface watertemperatures, which resulted in a high vaporization rate for thepesticides.
Sujatha et al. (1994a) assessed the distribution of DDT and itsmetabolites in the Kochi backwaters, southwest of India. Total DDTconcentration was as high as 54.4 μg/l and the predominantmetabolite was pp′-DDE. Total HCH concentration was as high as1.1 μg/l in the Kochi (former Cochin) backwaters due to a pre-monsoonal accumulation of pesticide (Sujatha et.al., 1993). However,during the monsoon Σ-HCH concentrations ranged from belowdetection level to 0.18 μg/l through the estuary followed by anincrease during post-monsoon period from 0.24 to 0.52 μg/l (Sujathaet.al., 1993). A similar seasonal pattern during pre-monsoon loadingfor endosulfan and malathion for water samples from the Kochibackwaters was recorded by Sujatha et al. (1999). Endosulfan'sdistribution throughout the estuaries varying seasonally with pre-monsoon loading always being higher than post-monsoon loading(about two fold greater), and undetectable pesticide throughout themonsoon, OCPs show a wide variations in their concentration level in
Table 1Pesticide residues in marine, estuarine and freshwaters of India
Notes.A. En dash (–) indicates no data.B. Maximum concentrations of endosulfan and malathion were primarily the result of the dose proximity of a pesticide manufacturing facility.
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various coastal zones. The distribution of malathion followed almostsimilar trend. However, in the upper reaches of the Kochi backwaters,which is largely riverine in the nature and slightly acidic, OCPpesticides are not subjected to removal by sorption onto sediments(Sujatha et al., 1994b) and malathion concentrations reached 13.1 μg/lduring pre-monsoon loading from agricultural use. Comparativelylower levels of malathion were observed in the lower reaches of theestuary where higher pH would promote biodegradation and lowlevels would be further dilutedwith seawatermoving into the estuary.The riverine nature and acidic pH of the upper estuary combined withthe industrial effluents from a pesticide manufacturing plant ac-counted for the very high concentrations of pesticides. Levels in themid-estuarine region reflected the prominent influence of agriculturalrun-off.
Using a moored in-situ sampler, Sarkar and Sen Gupta (1989) deter-mined the concentration of residues in seawater off the central westcoast of India. Shailaja and Sarkar (1992) reviewed the resultswhere theorder of distribution of different chlorinated compounds along the cen-tral West Coast of the Arabian Sea was as follows: γ-HCHNaldrinNp,p′-DDENdieldrinNo,p′-DDENp,p′-DDTNo,p′-DDTNo,p′-DDD. The ΣDDTconcentrations ranged from 15.8 to 444.0 ng/l. Among DDT isomers, p,p′-DDTwas found to bemore abundant than others in the southern partof the regionwhereaso,p′-DDTwaspresent in significant concentrationsoff the Ratnagiri Coast, western part of India. Gamma-HCH ranged from0.26 to 9.4 ng/l, whereas aldrin and dieldrin were found at concentra-tions ranging from 1.4 to 9.8 ng/l and 2.1 to 50.9 ng/l, respectively. Ingeneral γ-HCH and the two cyclodiene compounds aldrin and dieldrinwere found more consistently in seawater samples than compounds ofthe DDT family.
Isomers of HCH, aldrin, dieldrin and DDT were detected inwater ofdifferent regions of the Indian Ocean (Shailaja and Sen Gupta, 1989).Of all organochlorine pesticides, total DDT was found to be present inconsiderable amounts (15.8–444 ng/l). There was sharp spatialvariations of organochlorine compounds in water where enrichmentwas evident in coastal regions in comparison to open oceanwater, thelater is contaminated mainly due to atmospheric transport ofpollutants (Tanabe et al., 1982a,b). The concentration of HCH wasfound to be quite low inwater as compared to that in sediment whichmay be due to the hydrophobic characteristics of these compounds aswell as dispersion of pollutants in the open ocean.
1.2. Marine sediments
Coastal sediments act as temporary or long-term sinks for manyclasses of anthropogenic contaminants and consequently act as thesource of these substances to the ocean and biota. The appliedpesticide can be transported through surface run-off, leaching andvapor phase and ultimately accumulates and settles in the bottomsediments. Hence bottom sediments represent an integrated measureof particle bound contaminants that have deposited over a longerperiod of time. Few studies have reported that contamination of OCsin the sediments from Indian coastal regions (Takeoka et al., 1991;Pandit et al., 2002; Sarkar et al., 1997; Sarkar and SenGupta, 1987,1988c, 1991) indicating the presence of their major emission sourcesin these regions.
Data on the accumulation of pesticides in marine sediments islimited, especially considering the length of India's coastline. Guzzellaet al. (2005) documented distribution of various organochlorinepesticides in the surface sediments along the stretch of the Ganges(Hooghly) estuary including Sunderban mangrove wetland, easterncoastal part of India. The results revealed a wide range of spatialvariations. The concentration of various pesticides also exhibited awiderange of fluctuations in the following range: ∑HCH 0.11–0.40 ng/g; HCBb0.05–0.98 ng/g; ∑DDT 0.18–1.9 ng/g. The presence of HCH isomersand DDT and its metabolites can be attributed to the use of theseinsecticides in agriculture as well as anti-malaria sanitary activitiescarried out throughout the country (Pandit et al., 2002). In contrast,levels of trans-eptachlorepoxide, dieldrin, endrin, mirex and meth-oxychlor were below the detection limit (either b0.05 or b0.10) inmajority of the cases. The concentration of four important isomers ofHCHs reveals a heterogenic nature of distribution. The compositionof HCH isomers α- and γ-HCH (lindane) was detected in all thesamples, whereas β- and δ-HCH were below the detection levels inmajority of the cases. This may be relative to isomerization of HCHsduring the process of transport and transformation in a marineecosystem (Chen et al., 2000; Iwata et al., 1994; Dou and Zhao,1998). The α isomer was the predominant one followed by γ-isomer, reflecting the use of a technical mixture of HCHs (Kannan etal., 1995). Isomers of α-, β-, and δ-HCHs were observed to contributeabout 33–74%, 28.5% and 26–50%, respectively, to the total HCHs. α-HCH has higher values of Henry's law constant and vapor pressure
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than β-HCH and γ-HCH, indicating greater efficiency by atmospherictransport of α-isomer than other isomers (Iwata et al., 1994)favoring existence of the isomer in all the samples.
The ratios of α- to γ-isomer were well below those in the technicalmixture (i.e., 4–7). The low HCH ratio in the sediment sample impliesthe use of lindane in this region. HCH contamination might haveoccurred through atmospheric transport from others parts of Indiawhere a large amount of technical HCHs is still being used and highconcentrations were found in biota (Ramesh et al., 1992). Concentra-tions of HCB seem to be generally uniform except for an abrupt level of0.98 ng/g at Babughat, very close to the western part of themetropolitanmegacity Kolkata (former Calcutta). High concentrationsof HCB in biota were reported near the industrialized cities such asMumbai, western coast of India, Tokyo Bay in Japan and Jiao ZhouWan, Qing Dao city in China (Monirith et al., 2003).
Recently Sarkar et al. (2008) reported the first comprehensiveaccount of the organochlorine pesticide residues (HCHs, DDTs andHCB) in core sediments (b63 µm particle size) from Sunderban whichrevealed an erratic pattern, either top to bottom or vice versa,reflecting non-homogenous input of these compounds.
HCB is not only used as fungicide but also generated as a byproductduring the production and usage of several agrochemical andindustrial chemicals. Furthermore, HCB has also been released intothe environment by waste incineration (van-Birgelen, 1998) and in avariety of reactions where it persists because of its thermodynamicstability (Breivik et al., 2004). Hence, the present result may bereflecting the levels of HCB generated in the industrial and highlypopulous city of Calcutta (with a population of 14.5 million). Theresidues of HCB in the rest of the stations might be a reflection of itslimited sources and the volatile nature of this compound. Breivik et al.(2004) rightly pointed out that HCB emissions can be expected todecrease as developing countries improve their chemical and metalproduction and handling practices.
DDTs were detected in all sediment samples, but the contributionof individual metabolites showed differences. Wide range of varia-tions in∑DDTwas also evident, with a range of 0.18 to 1.9 ng/g. Amongthe metabolites of DDT, pp′-DDT and op′-DDT were found to be muchmore significant than othermetabolites DDE and DDD. The occurrenceof DDT isomers is predominant in the following order: pp′-DDTNpp′-DDDNpp′-DDENop′-DDTNop′-DDDNop′-DDE. The dominance ofDDTs in the sediment was also reported by Pandit et al. (2002) fromthe coastal marine environment ofMumbai, western part of India. Thismay be attributed to the slow degradation of DDTs or recent input ofDDTs in this environment (Tavares et al., 1999; Yuan et al., 2001). Thedominance of either pp′-DDT or both pp′-DDT and pp′-DDE insediments was also recorded by Guruge and Tanabe (2001) from the
Table 2A comparison of OCPs concentration in surface sediment collected from different estuaries
Locations DDTs
Range Mean
Xiamen Harbor, PRC 4.45–311 42.8Minjiang River estuary, PRC l.57–13.06 6.7Yangtze River, China BDL–0.6 –
Pearl River Estuary, PRC 1.36–8.99 2.84Daya Bay, PRC 0.14–0.3 –
Wu-shi estuary, Taiwan ND–11.4 2.51Ulsan Bay, Korea 0.02–41.9 3.34Mason Bay, Korea 0.2–80.2 –
Bay of Bengal, India 0.04–4.79 –
Casco Bay, USA b0.25–20 –
Quanzhou Bay 7.37–49.3 22.27Singapore Coast 2.2–11.9 –
Notes.A. ND: not detected.B. BDL: below detection level.
west coast of India and by Booij et al. (2001) from the northwest coastof Java, Indonesia. The ratio of concentrations of pp′-DDT to ∑DDT(0.36–0.75) showed a definite indication of recent use of the DDT. Thecontribution of pp′-DDT over 50% of the total DDT at some stationsseems to be associated with vegetable growing activities. The use ofpesticides in agriculture and aquaculture has generally been increas-ing due to rising population and demand for more agrochemicals atthese sites. The Hugli (Ganges) River passes through relatively denseindustrial and residential areas where pesticides are sprayed duringthe public health campaign against malaria and also for otherpurposes. The relative concentration of the parent DDT compared toits biological metabolites, DDD and DDE can be used as indicativeindices for assessing the possible pollution sources. Since the ratio of(DDE+DDD)/∑DDT is always b0.5, weathering in the source areas hasvirtually no role in their concentration (Hites and Day, 1992; Honget al., 1999; Zhang et al., 1999).
The high percentage composition of op′-DDT and pp′-DDT withrespect to total DDT clearly illustrates that DDT usage has not beeneradicated yet in the country, and there might be new input of DDT tothe coastal estuary as asserted by Aguilar (1984) and Dimond andOwen (1996). India is ranked the biggest consumer and manufacturerof HCH and DDT in the world (Mehrotra, 1993) as these are cheap aswell as effective chemicals (Bashkin, 2003).
Sarkar and Sen Gupta (1987) measured pesticide residues insediments along the west-central coast of India in the Arabian Seashowing the following decreasing order: HCHNaldrinNpp′-DDENpp′-DDTNop′-DDENpp′-DDDNdieldrin. HCH was detected in almost allsediment samples at concentrations ranging from 0.44 to 17.9 ng/gww. Aldrinwas found at concentrations ranging from 0.95 to 35.7 ng/gww. Among the metabolites of DDT, residues of pp′-DDE and op′-DDEwere found to be much more significant than DDD in the marineenvironment. Total DDT detected ranged from 7.01 to 179.10 ng/g ww.It is worthwhile to mention that HCH was found in 11 of 12 sampleswhile DDT and its metabolites were found only in 5 of 14 sedimentsamples.
Sarkar and Sen Gupta (1991) collected sediment samples off thewest coast of India in the Arabian Sea and recorded the residue levelsin the following order: DDTNHCHNaldrinNdieldrin. The concentra-tion of ΣDDTwas relatively high inmost of the samples. However, DDTcould not be detected in a few sediment samples that contained themaximum percentage of silt and sand. Aldrin was much moreprevalent than dieldrin and γ-HCH was dominant over its otherisomers.
In the east and west coast of India, Pandit et al. (2001) observedthat HCH isomers and DDT and its metabolites are the predominantlyidentified compounds in majority of the surface sediment samples.
and bays (ng/g dry wt)
HCHs References
Range Mean
0.14–1.12 0.45 Hong et al. (1995)2.99–16.21 8.62 Zhang et al. (2003)– – Liu et al. (2003)0.28–1.23 0.68 Hong et al. (1999)0.32–4.16 – Zhou et al. (2001)0.99–14.5 3.78 Doong et al. (2002)0.02–4.55 0.64ND–1.3 – Hong et al. (2003)0.17–1.56 – Babu Rajendran et al. (2005)b0.25–0.48 –
0.55–3.74 1.63 Gong et al. (2007)3.3–46.2 – Wurl and Obbard (2005)
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The predominance of α- and β-HCH reflects the use of technical gradeHCH in India. An overall low level of DDT, DDD and DDE residues insediments were recorded in sediments where DDE followed by DDTconstituted the bulk portion. Comparable residue levels of thesepesticides have earlier been reported in the Indian marine environ-ment (Sarkar and Sen Gupta, 1987, 1988). They attributed thesignificant concentrations of DDE in coastal sediments to the presenceof various kinds of marine benthic organisms which accelerate thebiodegradation process and the alkaline nature of marine systemswhich is highly favorable for such types of transformations.
To evaluate the relative degrees of OCP contamination in coastalsediments in India, a comparison has made against the available datain Asian context as shown in Table 2. Although, the direct compar-ability is somewhat compromised by the fact that different studiesconsidered different DDT metabolites, still it is important to evaluatethe OC contamination to get a sense of regional similarity. It is evidentthat Indian coastal regions present low tomoderate OC contaminationin sediments.
Sarkar et al. (1997) found higher mean concentration of ΣDDT anddieldrin (by factors of 1.7 and 2.4 respectively) in estuarine sedimentsof the Arabian Sea areas compared to offshore sediments while meanconcentrations of ΣHCH, aldrin, and endrin were similar for bothoffshore and estuarine samples. In both offshore and estuarinesediments, α-HCH was the most dominant isomer and for the DDTs,pp′-DDE was the most predominant metabolite except near Canna-nore and Murmugao where op′-DDE and pp′-DDT were significant inoffshore samples. Their overall assessment revealed that Zuari andKali estuaries are the most susceptible to DDT as compared to otherestuaries.
Sarkar and Sen Gupta (1988a,b) determined residues of organo-chlorine pesticides in sediments from the Bay of Bengal. Thecompounds and concentrations detected were aldrin at 20 to530 ng/g (all sample weights expressed as ww), γ-HCH at 10 to210 ng/g, dieldrin at 50 to 510 ng/g (Sarkar and Sen Gupta 1988b), andΣDDT at 20 to 790 μg/g (Sarkar and Sen Gupta 1988a). The variabilityin pesticide residue concentrations was attributed to the presence of
Fig. 1. Map showing distribution of major rivers and important s
numerous rivers along the east coast of India including the Hugli,Mahanadi, Vamsodhara, Godavari, Krishna, Pennar and Palar Rivers, asevidenced in Fig. 1. All these rivers bring copious amount ofagricultural discharges containing persistent organic pollutantsincluding organochlorine pesticides and empties into the Bay ofBengal. The highest concentration of aldrin (0.53 ppm) was present ina sample collected from the mouth of the river Palar, whereas thehighest concentrations of HCH (0.21 ppm), dieldrin (0.51 ppm) andΣDDT (0.79 ppm)were found in samples from themouth ofMahanadi,Hooghly and Palar rivers respectively. Amongmetabolites of DDT, bothpp′-DDE and op′-DDE, were consistently found along the east coast ofIndia, attributed to the degradation of DDT to DDE in the coastalsediments. Sarkar and Sen Gupta (1988a) suggested that the followingphenomenon, either singly or in combination, are responsible for thedegradation of DDT to DDE: the ability of marine benthic organisms tobiodegrade DDT: the alkaline nature of the marine system thepresence of chemical constituents and their characteristics, e.g.salinity, clay mineral concentration, major elements and the presenceand concentration of organic matter; and stored thermal energy inoceanwaters, DDT isomers and their metabolites were detected in thesediments of coastal Bay of Bengal in the following order: op′-DDENpp′-DDENpp′-DDTNop′-DDDNpp′-DDDNop′-DDT. Venugopalan andRajendran (1984) showed that DDT concentration was in the rangeof 1.8 to 25.8 ng/g ww and HCH in the range of 0.4 to 7.1 ng/g ww insediment samples of Vellar Estuary.
Shailaja and Sarkar (1992) attributed the high concentration ofresidues, especially ΣDDT, in the Bay of Bengal to the rapid transportby rivers of their high-suspended sediment load (about 8.1 mg/l)compared to rivers emptying into the Arabian Sea, where suspendedparticulate loads are 1.6mg/l. Several studies havemeasured sedimentconcentration of pesticide in Indian rivers, including the Vellar,Ganges, Kaveri and Mahanadi rivers, and Lake Kolleru. Ramesh et. al.(1991) found higher sediment loads of DDTs and HCHs in the VellarRiver during the wet season (3, 4 and 12.4 ng/g dw, respectively)compared to dry season (1.0 to 2.3 ng/g dw, respectively). Senthilk-umar et al. (1999) found mean sediment concentrations in the Ganges
ites in peninsular India and southeast Asia cited in the text.
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of 5.6 and 2.6 ng/g dw DDT and HCH, respectively. Rajendran andSubramanian (1999) measured chlorinated pesticide residues insurface sediments from the Kaveri River on the southeastern coastof India. Total DDT was low and showed no wide variations amongsampling sites, reflecting its ban from agriculture and use formosquitocontrol. The concentrations of HCHs (39.4 to 158.4 ng/g dw) at thevarious collection sites reflected its agricultural use, with peak valuesreflecting the application of HCH for rice crops during the monsoonand subsequently to grams during the post-monsoon season.
Iwata et al. (1994) analyzed air, river, water, and sediment samplesfrom eastern and southern Asia (India, Thailand, Vietnam, Malaysiaand Indonesia) and Oceania (Papua, New Guinea and the SolomonIslands) for the presence of OC pesticides to elucidate theirgeographical distribution (Fig. 1). The distribution patterns insediments showed smaller spatial variations on global terms, indicat-ing that OCs released in the tropical environment are dissipatedrapidly through air and water and retained less in sediments. Theynoted that atmospheric and hydrospheric concentrations of HCHs(hexachlorocyclohexanes) and DDTs (DDT and its metabolites) intropical developing countries were higher than those observed indeveloped nations.
There are only a few studies on the fate and behavior of OPpesticides in marine sediments (Sarkar and Sen Gupta 1985; Sarkarand Sen Gupta 1986; Sujatha and Chacko 1991) from Indian waters.They found that the stability and fate of the pesticides monocroto-phos, phosphamidon and DDVP in sediment samples were influencedby pH, salinity and exchangeable cations. The low stability of thesepesticides in sea sediments indicates that major element cations havereduced the toxic effects of these pesticides in marine organisms(Sarkar and Banerjee 1987).
A review of published data of pesticide residues in sedimentsindicates that isomers of DDTand its metabolites, HCH, aldrin, dieldrinand endrin are present but that, while all may not be found in everysample, the most common and abundant pesticide residues werealdrin, HCHs and DDTs. Furthermore, there is a striking contrast inpesticide residue concentrations in sediments of the east and westcoasts of India. Sediment samples of the east coast contain pesticideresidue concentrations in magnitude higher than samples from off thewest coast of India the cause of which might be attributed to severalfactors. All major Indian rivers flow east and drain through fertileagricultural lands, which receive a considerable input of pesticides,and carry their sediment loads to marinewaters on the coast. Also, theuse pattern of pesticides shows a predominance of pesticides to landsbordering the eastern coast.
James and Ramesh (2002) emphasized on the significant role of thesedimentological characteristics i.e., texture and total organic mattercontrolling the leaching process in sediments. In general fine grainedsediments inhibit pesticide leaching because of low permeability orhigher surface area and enhance adsorption of pesticides. Theyestablished correlation between grain size and organic matter insurficial sediments of a river basin of South India. They had alsoobserved a high concentration of gamma-HCH near the agricultural
Table 3OC pesticide residues in zooplankton samples from Indian waters
Location Concentration range and mean (ng/g w
Year of sampling DDT
Vellar Estuary 1979 1.2–47.3Southeast Bay of Bengal Kaveri and ColeroonRiver mouths
1990 4.0–6.2 (5.2)
Northern Bay of Bengal Mahanadhi and HooglyRiver mouths
1991 310.2–1587.8 (844.6
Notes.A. Figures in parentheses indicate mean values.B. En dash (–) indicates no data.
non-point source area and beta-HCH was always higher than gamma-HCH confirming the characteristic feature of more stability andresistance to microbial degradation (Rajendran and Subramanian,1997). Recently, Sarkar et al. (in press) established negative correla-tions for all the organochlorines (HCH, DDT, HCB) with sand in coresediments from Indian Sunderban wetland (Fig. 1) which reveals thatcoarse particles have less adsorption capacity for OCs.
1.3. Marine zooplankton
Kureishy et al. (1978) studied the samples of zooplankton in theeastern Arabian Sea and found residues of DDT, HCH and otherunidentified compounds. In their study area south of Mumbai (formerBombay), west coast of India, ΣDDT was found in the range of 0.50 to3.21 μg/g ww. They could detect op′-DDT, pp′-DDT, op′-DDE, pp′-DDEbut no DDD. Subsequently Kannan and Sen Gupta (1987) collectedzooplankton samples off the Saurashtra Coast, Gujarat (north ofBombay) in the northern Arabian Sea and observed that ΣDDT rangedfrom 0.38 to 1.6 μg/g ww and from 17.5 to 379.5 μg/g ww lipid. DDDwas the major metabolite detected in most of the samples.
Shailaja and Singbal (1994) determined residues in zooplanktonsamples from two oceanographic cruises, viz. during the southwestmonsoon covering the southeast coast and during the northeastmonsoon covering the northern coast of the Bay of Bengal. In samplesfrom the southeast coast, ΣDDT concentrations ranged from 4.0 to6.2 ng/g ww while aldrin levels varied between 0.36 and 0.78 ng/gww. However, in samples from the northern Bay of Bengal, DDTranged from 310.2 to 1587.8 ng/g ww and aldrin was not detected.Shailaja and Sen Gupta (1990) had confirmed the presence of DDT andits metabolites, DDD and DDE, in their study on samples obtainedfrom three stations in a transect off Mumbai. In this study, DDD wasthe major product formed in zooplankton, indicating DDTmetabolismin zooplankton. They observed that ΣDDT concentrations showed adeclining trend from near-shore to offshore while DDD concentrationsincreased from the coast to offshore. The concentration of ΣDDT washigher in zooplankton than in both plankton-feeding and carnivorousfish from coastal as well as open ocean regions of the Arabian Sea. Thisindicates that zooplankton did not act as an important link in thetransfer of organic material from the primary producers to plankton-feeding fish. In zooplankton samples collected from the coastalregions of Bay of Bengal, ΣDDT was 5.2 ng/g and aldrin 0.6 ng/g ww.Venugopalan and Rajendran (1984) detected ΣDDT in the range of 1.2to 47.3 ng/g ww. HCH from 0.3 to 8.5 ng/g ww, and endosulfan from0.1 to 0.4 ng/g ww. Toxicity studies with zooplankton indicated thatDDT was more toxic than either lindane or endosulfan (Venugopalanand Rajendran 1984; Rajendran and Venugopalan 1988). The authorsranked zooplankton sensitivity in the order of Acartia sp.NEucalanussp.NLucifer sp.NSagitta sp. Shailaja and Sarkar (1993) summarizedtheir analyses of zooplankton residues, with reference to the influenceof themonsoon, from coastal and offshore sampling in the Arabian Seaand the coastal region of the Bay of Bengal. For pre-southwestmonsoon samples from the Arabian Sea, ΣDDT of zooplankton varied
w) References
HCH Aldrin Endosulfan
0.3–8.5 – 0.1–0.4 Venugopalan and Rajendran (1984)– 0.36–0.78 (0.6) – Kannan and Sen Gupta (1987)
) – – – Shailaja and Singbal (1994)
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from 3.36 to 38.8 ng/g ww. However, for the post-monsoon periodΣDDT ranged from 31.8 to 614.8 ng/g ww. DDT accounted for nearly83% of ΣDDT in the post-monsoon samples but only about 70% ofΣDDT in the pre-monsoon samples. The increase in DDTs contributionto ΣDDT for the post-monsoon samples may be attributed to land run-off carrying DDT during monsoon period to coastal waters. DDD,which contributed 29% of ΣDDT in pre-monsoon samples, contributedonly 16% to the post-monsoon samples. They hypothesized thatbecause DDD could be further metabolized to DDE, there was no food-chain magnification in samples tested from this region (Shailaja andSen Gupta 1990).
Venugopalan and Rajendran (1984) in their studies of the VellarEstuary recorded that residue levels were low during the monsoonseason and that it is likely that residues swiftly reach the Bay of Bengal.In fact, Shailaja and Nair (1997) observed higher residues in oceanplankton during the post-monsoon season. Wide variations ofzooplankton in Indian coastal waters have been evidenced from Table 3.
1.4. Marine bivalves
Bivalves have been widely accepted and used as sentinel organismsto monitor the concentration of pollutants in coastal marine environ-ments. Different species of oysters, mussels and clams have been usedas bioindicators for Mussel Watch Programme in different countries tomonitor marine pollution from pesticide residues. Also, Ramesh et al.(1990b) suggest that the bioaccumulation of OCPs by mussels mighthave implications for human exposure, because mussels are marketedimmediately following collection and without depuration.
Ramesh et al. (1990b) measured the concentrations of OC residuesin green-lipped mussels Perna viridis L. (Mollusca: Bivalvia) collectedfrom nine locations along the South Indian Coast, which includes theeast and west coasts covering the Bay of Bengal and the Arabian Sea,respectively. They found that HCH isomer (α, β and γ) concentrationsranged from 4.3 to 16 ng/g whereas ΣDDT (the sum of pp′-DDT, pp′-DDE, pp′-DDD and op′-DDT) varied from 2.8 to 39 ng/g. Musselscollected from thewest coast had higher levels of DDT, suggesting DDTused for vector control in urban locales, eventually dispersed or areasis in storm water run-off from coastal cities. However, in Porto Novoand Pondicherry harbors on the east coast and Suratkal on the westcoast, HCH levels were slightly higher than DDT, which is indicative ofthe use of HCH for agricultural purposes in the nearby areas. Rameshet al. (1989, 1991) observed considerable pesticide contamination inair and water, especially in agricultural areas. The highest levels ofHCH in Indian mussels are comparable to those reported from HongKong and Taiwan and this is probably attributed to the large-scale useof HCH in Mainland China and its eventual transport to the SouthChina Sea.
Venugopalan and Rajendran (1984) detected pesticide residues inthree molluscs (the oyster Crassostrea madrasensis and the clamsMeretrix casta and Katalysia opima) collected from Vellar Estuary. Themean pesticide residues in these three species were 3.4 ng/g ww forDDT, 0.8 ng/g ww for lindane and 0.42 ng/g ww for endosulfan. Therewas no correlation between the pesticide concentration in themolluscs and the concentration in solution or in particulate fraction
Table 4OC pesticide and PCB residues in bivalves from Indian waters
Location Concentration range and mean (ng/g ww)
HCH DDT
Vellar Estuary 0.1–3.1 (0.8) 0.3–7.3 (3.4)East Coast (Bay of Bengal) 4.3–16.0 (7.9) 2.8–33 (26.6)West Coast (ArabIan Sea) 4.9–9.7 (6.7) 6.0–39 (27.3)Porto Novo and Cuddalore 6.6 15
Notes.A. Figures in parentheses indicate mean values.B. En dash (–) indicates no data.
of water. The authors also studied the toxicity of DDT, lindane andendosulfan using the same three species of molluscs and found theorder of toxicity was DDDNendosulfanN lindane and the sensitivity ofthe bivalves was in the order: C. madrasensisNK. opimaNM. casta.
As part of the Asia Pacific Mussel Watch Programme, Senthilkumaret al. (2001) measured the concentrations of persistent organicpollutants in green mussel tissues collected from coastal regions ofIndia, Thailand and the Philippines from 1994 to 1997. Among all thepesticide concentrations, DDTs, were highest followed by HCHs,chlordane and HCB, and the trends were comparable to an earlierstudy by Ramesh et al. (1991). However, an overall uniformconcentration of pesticide residues was observed in the bivalvesfrom Indian coastal waters excepting a few cases (Table 4).
1.5. Marine fish
Fish have been selected for monitoring because (i) they concen-trate pollutants in their tissues directly from water and also throughdiet, thus enabling the assessment and transfer of pollutants throughthe pelagic food web (Bruggeman, 1982), (ii) they generally exhibit alow metabolism for organochlorines and consequently should reflectthe levels of pollution in the aquatic environment (Muir et al., 1990)and (iii) they occupy different habitats in the same ecosystem andhave different feeding behaviors, thus offering the potential to studythe influence of environmental and biological factors in the bioaccu-mulation of pollutants (Porte and Albaiges, 1993).
Shailaja and Sen Gupta (1989) measured HCHs and DDTs in variousfish species collected from different regions of the seas aroundpeninsular India. However, the concentration of the isomers of HCHswas too low to be quantified. The concentration of total DDT wasfound to be in the range of 8.1–204 ng/g (dry wt) and the meanconcentration level was 59.2 ng/g. They observed highest amount of t-DDT residues burden (344.7 ng/g) from the estuarine regions followedby the coastal varieties of the 23 fish species. Among the metabolitesof DDT, DDE constitutes a major proportion. Shailaja and Nair (1997)pointed out a strong influence of the feeding habit and habitat of thefish on the residue levels of OCs. They recorded highest t-DDTconcentration in two carnivore species, barracuda (Sphyraena acuti-pinnis) and shark (Scoliodon sorrakowah) from the Arabian Sea andsuggested a rapid dissemination through the water column of thepesticides entering the northern Arabian Sea in the monsoon season.They had also established that the liver generally accounted for thehighest level of total DDTon awet wt basis, followed by the gills while,on a lipid basis, the residue content in the muscle was the highestamong the different fish tissues. Das and Das (2004) observed positivecorrelation between total organochlorine residues and the % of fatcontent in muscle of River Shad Hilsa ilisha from the south patches ofthe Bay of Bengal which was also endorsed by other workers(Georgakopoulos-Gregoriades et al., 1991; Stout, 1980). Pesticideresidues were found to be higher in the muscle of larger fishes asthey content more fat than the smaller ones (Georgakopoulos-Gregoriades et al., 1991; Stout, 1980).
Venugopalan and Rajendran (1984) studied the pesticide residuesin fish samples obtained from Vellar Estuary of South India adjoining
References
PCB Endosulfan
5.0 2.1–0.8 (0.4) Venugopalan and Rajendran (1984)1.0–7.1 (3.3) – Ramesh et al. (1990b)1.03 4.2–5.7 (4.7) Venugopalan and Rajendran (1984)1 – Senthilkumar et al. (2001)
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the Bay of Bengal including the grey or striped mullet Mugil caphalusL. (Perciformes: Mugilidae), therapon or targetfish Therapon jarbou(Forsskål) Klunzinger (Perciformes: Terapontidae), spine foot Siganusjavus L. (Perciformes: Siganidae), and the catfishes Mystus gulioHamilton (Siluriformes: Bagrinae) and Arius (Tachysurus) sp. (Silur-iformes: Ariidae). Residue concentrationswere in the following ranges(ng/g ww): ΣDDT, 0.4 to 89.27; lindane, 0.05 to 4.64; and endosulfan,0.02 to 2.47. Between DDT and its metabolites, pp′-DDE was thedominant degradation product. There was no significant variation inthe concentration of various pesticides between fish species and theyobserved no obvious variations in pesticide concentrations betweenherbivorous and carnivorous fish species. They studied the toxicity ofthese pesticides under laboratory conditions and found that the orderof toxicity was DDTN lindaneNendosulfan. M. cephalus was moresensitive than M. gulio to all three pesticides.
Considering different feeding habits, Pandit et al. (2001) studiedaccumulation of OCPs in the muscle tissues of different finfishes andshell fish (prawn) from Alibagh and Mumbai, west coast of India. Theyobserved predominance of α- and γ-HCH which reflected the use oftechnical grade HCH in India. They detected low concentration of OCPsin comparison to other temperate countries suggesting a loweraccumulation in tropical fish which could be due to rapid volatilizationand degradation of these compounds in the tropical environment. Also,thehigher temperature in the tropics could enhance the elimination rateof chemicals from fish due to the influence of temperature on theirrespiratory requirements, as the biological half-lives of compounds suchas HCH and DDT are shorter at high temperature. The data on thedistributionofOCPs infishes is importantnot only for ecological reasons,but also because of their impact on human health.
1.6. Marine mammals
From Porto Novo coastal areas, southern coastal regions of India,Tanabe et al. (1993) detected residues of all the four HCH isomers, DDT(pp′- and op′-DDT), pp′-DDE, HCB and PCBs in the blubber of dolphinsfrom the Bay of Bengal. Interestingly, DDT concentrationwas higher inthese cetaceans than HCH which might be ascribed to several factors,including that the former being more lipophilic, less biodegradable,and thus less likely to undergo atmospheric transport, due to itsrelatively low vapor pressure. Kannan et al. (1993; 1994) also recordedsimilar trend of pesticide residues in the Gangetic dolphin (Platanistagangetica), distributed in Ganga, Brahmaputra and Indus rivers andtheir larger tributaries and Irrawaddy dolphin (Orcaella brevirostris)distributed in Chilika Lake, India (Kannan et al., 2005). Populations ofIrrawaddy dolphins are constrained by the species narrow habitatrequirements – lagoons, estuaries, rivers and lakes – and as thereforeparticularly vulnerable to the effects of human activities. The similartrend of contamination was evident in blubber from bottle-nosedolphins, spinner dolphins, humpback dolphin (Tursiops truncates,Stenella longirostris and Sousa chinensis) inhabiting Bay of Bengal(southeast coast of India), reported by Karuppiah et al. (2005). Thedominance of DDT might be attributed to extensive use of DDT formalaria and Kala-azar vector control in India.
Pesticides are toxic entities that enter the human body through thefood chain and cause serious health problems. From northern part ofIndia, Nair et al. (1996) and Kumar et al. (2006) reported both HCH andDDT residues in humanmilk, exceeding the tolerance limit of gamma-HCH and DDT in milk as prescribed by FAO/WHO (2000) of 0.01 and0.02 μg/g respectively.
1.7. Ecotoxicological concerns
The sediment quality guidelines (SQG) specified by the USEPA(1997) and by Canadian Council of Ministers of the Environment(CCME, 2002) were used to assess the potential ecotoxicologicalimpacts of organic contaminants. Effects range-low (ER-L) and effects
range-medium (ER-M) values are used to predict potential impacts ofcontaminants in sediments, as devised by Long et al. (1995) whereasER-L values correspond to the lower 10 percentile and ER-M values tomedian values, when the chemical concentrations of a contaminant inmarine sediments are sorted according to the degree of their effectlevels. ER-L represents the value at which toxicity may begin to beobserved in sensitive marine species, whereas ER-M value representsthe concentration below which adverse effects are expected to occuronly rarely. For ∑DDT the levels for samples of few sites of thepeninsular India exceed the ER-L value, but are lower than the ER-Mvalues leading to an intermediate ranking of sediment toxicity.Recently, Sarkar et al. (in press) observed that for ∑DDT the levelsexceed the ER-L value, but are lower than the ER-M values leading toan intermediate ranking of sediment toxicity in Sunderban wetland.For γ-HCH the threshold value (TEL) is much higher than the certifiedvalue and the ecotoxicological impacts to marine environment.Probable effect level value of γ-HCH also exceeds the PEL valueindicating, there is an every chance of contamination to the marineenvironment and the habitants inhabiting into the sediment.
1.8. Recommendations to improve the understanding of the situation
1. The authors recommend that a reliable monitoring, assessmentand reporting procedures shall be implemented in accordancewith appropriate environmental policies, laws and regulations inorder to minimize the pesticide exposure. Though cost-effective,effort should be undertaken in the development of biodegradablepesticides with the help of mechanical and electronic devices.
2. Studies are to be carried out to elucidate and quantify the subtleeffects of pesticides on humans and wildlife, including molecularmodeling of biodegradation, transformation and toxicity mechan-isms. As devised very recently by Leach and Mumford (2008), thePesticide Environmental Accounting (PEA) tool should beemployed for monetary estimate of environmental and healthimpacts per hectare-application for any pesticide.
3. Epidemiological studies of pesticides should be carried out so thatthe biological indices (Maroni et al., 2000) of pesticide compoundsmay be effectively used to monitor exposure to pesticide of fieldworkers.
4. Adulteration of food items by pesticides should be controlledthrough food regulation as has been done in developed countries.
5. The authors suggest an extensive awareness programme for safeuse of pesticides through potential paper and electronic media i.e.,television, radio, schools and colleges, agriculture and municipalstaff. Government and other agencies should educate farmers onGood Agricultural Practices (GAP) in the use of pesticides inagriculture.
2. Conclusion
The review work summarizes and synthesizes the significantamount of data on the organochlorine pesticide residues in abiotic andbiotic compartments in Indian coastal regions. This reveals a betterunderstanding of the current levels and spatiotemporal trends ofcontaminants including the fish species which the coastal peopleconsume largely. The east coast, on an average, is found to be muchmore contaminated than the west coast, which might be attributed toresidues carried by the major rivers along the former coast. OCPsresidues were also present in food commodities (Mukherjee andGopal, 1996), water (Agnihotri, 1993), mothers' milk (Nair et al., 1996;Kumar et al., 2006), in human blood (Subramaniam and Solomon,2006) and blubber of endangered Gangetic dolphin (Tanabe et al.,1993) in different parts of India. It has been revealed that a significantbioaccumulation of DDT and HCH residues in the breast milk and thenewborn is a recipient of this bioconcentrated form of pesticides. Theauthors suggest that a regular monitoring, assessment and reporting
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machineries should be implemented in accordance with appropriateenvironmental policies, laws and regulations. The Government andother related agencies should educate farmers and agriculturemanagers on Good Agricultural Practices (GAP). The authors alsorecommend for Good Laboratory Practices (GLP) and LaboratoryStandard Operating Procedures (SOPS) for reliable and dependableanalytical systems and standardization of facilities for analysis.
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