Seasonal variation of persistent organochlorine insecticide residues in Vellar River waters in Tamil Nadu, South India

Environmental Pollution 67 (1990)289-304

Seasonal Variation of Persistent Organochlorine Insecticide Residues in Vellar River Waters in Tamil Nadu, South India A. Ramesh, S. Tanabe,* H. Iwata. R. Tatsukawa Department of Environment Conservation, Ehime University, Tarumi 3-5-7, Matsuyama 790, Japan

A. N. Subramanian, D. Mohan & V. K. Venugopalan Centre of Advanced Study in Marine Biology of Annamalai University, Porto Novo-608502, Tamil Nadu, India (Received 19 March 1990; accepted 11 June 1990)

A BS TRA C T Water samples collected from Vellar river and Pichavaram mangroves at Porto Novo (11°29'N, 79°46'E), Tamil Nadu State, South India, Jrom December 1987 to Januao' 1989 were analy=ed to determine the seasonal variation of the levels o f organochlorine insecticides such as H C H ( BHC ) and DDT. Both these insecticides showed higher levels from October to Februao', although this trend was more pronounced in H C H than DDT. reflecting the application of technical H C H largely and probably small quantities ~f D D T during the .[lowering season of rice. The ~-HCH was detected as a dominant isomerJor all seasons monitoredJollowed by [~-HCH. Among D D T compounds, p,p'-DDT was the highest in river water except in the dry season when p,p'-DDD showed a higher percentage. On the other hand, in mangroves p,p'-DDE was highest during the wet season and p,p'DDD during the dry season. A ir-water partitioning data of i l C H isomers and DD T compounds in Vellar river revealed that these chemicals tend to be in the water phase. These observations may aid in understanding the role o['a tropical paddy area on the behavior and fate of man-made chemicals in view of worldwide contamination. * To whom correspondence should be addressed. 289

Environ. Pollut. 0269-7491/90/$03"50 :~ 1990 Elsevier Science Publishers Ltd, England. Printed in Great Britain

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INTRODUCTION The usage of persistent man-made chemicals in tropical countries and the associated environmental and human health hazards has been a matter of great concern (Kalra & Chawla, 1981; Edwards, 1985; Mowbray, 1986; Anon., 1989). Ironically, the demand for these chemicals is increasing; a situation remarkably reflected in the application of pesticides in developing countries. As most of the developing countries are located in the tropical belt, the tropical agroecosystem, characterized by high temperature and heavy rainfall, facilitates the rapid removal of these insecticide residues through air and water and ultimately contributes to global contamination. Our earlier studies reported the widespread contamination of these insecticide residues in air (Ramesh et al., 1989) and human breast milk (Tanabe et al., 1990) from South India. India is a representative tropical country where persistent insecticides like HCH and D D T are still used for agriculture and public health purposes. Their usage data revealed that annual consumption of H C H amounts to about 45 million kg, and that of DDT, 19 million kg (FAO, 1978-88; ICS, 1986). They together account for more than 50% of the pesticides (in quantity) currently used in the country. This has resulted in considerable contamination of the Indian environment. Further, we also observed a seasonal variation in the level of these residues in air which was in line with the agricultural activities of the area investigated. In order to understand the comprehensive behavior of organochlorine insecticides and their interaction with the water phase, the present study was undertaken to measure these chemicals in water samples from the Vellar river and Pichavaram mangroves, South India.

MATERIALS AND METHODS Water sampling in Vellar river and nearby areas (Fig. 1) was carried out in both the dry and wet seasons, i.e. July 1988 and January 1989, respectively. Periodical sampling was also made from December 1987 to January 1989 at station 5. The Vellar river joins the Bay of Bengal at Porto Novo (11 ° 29' N, 79 ° 46' E) located 200 km south of Madras city on the east coast of India. Dry and wet seasons alternate in this location. Hundreds of acres of agricultural fields (mainly paddy) are located on either side of the Vellar river. Pichavaram mangroves are situated south of the Vellar estuary. They cover approximately 1000 ha of land and are mazed with numerous creeks and channels. These mangroves receive sea water from the Bay of Bengal

Variation ~?["organochlorine insecticide residues in South India

291

llON30 ' ,

ii ° 15'

79 ° 40'

Fig. !.

79 ° 50rE

Map showingthe study area. Dotted portions represent the riverineand mangrove areas. Numbers represent the sampling stations.

through both the Vellar and Coleroon river mouths and fresh water from the irrigation channels and small drains from the nearby paddy fields. About 20 liters of water from the Vellar river and Pichavaram mangroves was collected and then passed through prewashed and dried Amberlite XAD-2 resin (Harvey, 1973) packed in a glass tube. All the solvents used in the present analysis were of analytical grade and thoroughly distilled before use to avoid contamination. HCH isomers and DDT compounds adsorbed to the resin were eluted with 150ml of ethanol. The crude extract was transferred to a separatory funnel containing 100 ml of hexane and 750 ml of hexane washed water and thoroughly shaken. After partitioning, the hexane layer was collected and concentrated to 5 ml in a Kuderna Danish concentrator. The concentrate was cleaned up with 5% fuming sulphuric acid and then washed with water. The hexane extract, if necessary, was further concentrated to 100/~1 with a microconcentrator under a stream of purified nitrogen gas. Quantification of HCH isomers and DDT compounds was performed by injecting the aliquots of final extract into a gas chromatograph (Shimadzu: Model 9A) equipped with a 63Ni electron capture detector and moving needle type injection system (splitless and solvent cut mode). The column consisted of fused silica capillary (0.25mm i.d. x 25m length) with chemically bonded OV-1701 (film thickness of stationary phase 0.3 #m).

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Temperature was maintained at 240°C isothermal. Injector and detector temperatures were kept at 260°C. Nitrogen was used both as a carrier and make-up gas (flow rate about 1.5 ml min-1). The detection limits and the recovery of the analyzed organochlorine insecticides were 0"01 ng liter-1 and about 95%, respectively.

RESULTS A N D DISCUSSION The spatial distribution of Z HCH (sum of ~, fl, 7 & 6 isomers) and Z DDT (sum ofp,p'-DDT, p,p'-DDE, p,p'-DDD and o,p'-DDT) residues obtained in the dry and wet seasons in the river and the mangroves are described in Figs 2 to 5. The mean and range of concentrations as well as percentage compositions of organochlorine insecticide residues in survey areas in both seasons are also given in Figs 6 to 9. The levels of Z HCH were found to be in the range of 110-2000 ng liter- 1 in the wet season and 14-90 ng liter- 1 in the dry season. On the other hand, E D D T levels were much lower than those of EHCH, varying from 0.12 to 0.63 ng liter- 1 in the wet season and 0-04 to 0-38 ng liter- 1 in the dry season.

11"30'1~

11"20'

79"40'

79°50'E

Fig. 2. Spatial distribution of EHCH concentrations in dry season in Vellar river and Pichavaram mangroves. Numbers on the top of each bar represent the concentrations detected at the respective sampling points.

11°30'N

11"20'

79"40'

79"50'E

Fig. 3. Spatial distribution of ZHCH concentrations in wet season in Vellar river and Pichavaram mangroves. Numbers on the top of each bar represent the concentrations detected at the respective sampling points.

11°30'N

11"20'

79°40 '

79"50'E

Fig. 4. Spatial distribution of Z D D T concentrations in dry season in Vellar river and Pichavaram mangroves. Numbers on the top of each bar represent the concentrations detected at the respective sampling points.

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ll°30'N

11o20,

79040 ,

79°50'E

Fig. 5. Spatial distribution of E D D T concentrations in wet season in Vellar river and Pichavaram mangroves. Numbers on the top of each bar represent the concentrations detected at the respective sampling points.

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Mean and range of concentrations and percentage compositions of riCH isomers in Vellar river water.

Variation o[ organochlorine insecticide residues in South India

F-o

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Mean and range of concentrations and percentage compositions of HCH isomers in Pichavaram mangrove water.

In the dry season, both Y.HCH and Y D D T revealed rather uniform distribution (Figs 2 and 4). Interestingly, H C H distribution in the wet season showed higher levels in Vellar river stations particularly where m a n y more agricultural channels empty, such as stations 4, 5 and 6, than mangroves (Fig. 3). However, such a trend was not m a r k e d in the distribution o f E D D T s (Fig. 4). When the concentrations of E H C H and E D D T were c o m p a r e d in both seasons, the variations were m u c h larger in the case of Z H C H (Figs 6 and 7) than E D D T (Figs 8 and 9). To further elucidate the temporal variation of these insecticides in water, P.P~DDT

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Mean and range of concentrations and percentage compositions of DDT compounds in Vellar river water.

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A. Ramesh

et al. Wet Season

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Fig. 9. Mean and range of concentrations and percentage compositions of DDT compounds in Pichavaram mangrove water. H C H and E D D T concentrations obtained from station 5, a representative area of Vellar river, were shown in Figs 10 and 11, respectively. In this station, concentrations of E H C H varied from 26 to 3900 ng liter- 1 whereas Z D D T ranged from 0.06 to 4.8ngliter -1. H C H values were high in December 1987, then showed a decline until July 1988 (Fig. 10). The levels started to increase apparently from October 1988, reaching a peak in December 1988. The relatively high values o f r i C H from October to January 3900

1200

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Jan.

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May June JuLy Aug. Sept. 1988

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Nov. Dec, Jan. 1989

Fig. I0. Seasonal variation of ZHCH concentrations in Vellar river.

297

Variation ~["organoehlorine insecticide residues in South India

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Seasonal variation o f ' ~ . D D T concentrations in Vcllar river.

reflect the large scale application of HCH during the flowering season of paddy in this area. A similar trend in H C H levels has already been observed in air samples from this area (Ramesh et al., 1989). On the other hand, concentrations of E D D T in water (Fig. 11) showed a trend similar to that of EHCH. However, the extent of variation among different seasons was not prominent in EDDT. Under the National Malaria Eradication Program of the Government of India, D D T is now mainly used for vector control (Gupta, 1986). About 85% of the D D T produced in India is used for mosquito control (Singh et al., 1988). Hence, the much lower level of Y D D T observed in the present paddy cultivating areas could be attributed to the relatively smaller quantity of D D T used in agricultural activities. Regarding percentage composition of H C H isomers in river and mangrove water, a high percentage of~ isomer was recorded followed by fi, 7 and 6 in both seasons (Figs 6 and 7). The high level of~ isomer might be due to its high percentage in technical H C H (c. 70%) sprayed on rice crops. Although the contribution of fl-HCH in technical HCH is smaller (c. 9%) than 7 (c. 14%) and slightly higher than 6-HCH (7%), its concentration was apparently high in water (next to ~). It is known that/~-HCH has lowest water solubility and vapor pressure, but is most stable among H C H isomers and also resistant to microbial degradation. Considering these physicochemical and biochemical properties it could be assumed that 7- and 6-HCH rather rapidly escape from agricultural areas through air and water and

A. Ramesh et al.

298

hence higher levels of them in water are expected to continue for a short while after application. On the contrary, /%HCH is the most persistent isomer in soil and crops and hence its contribution to water bodies is likely to continue for a long time. The persistent tendency of/~-HCH in agricultural soil and water bodies has also been reported from temperate areas (Tatsukawa et al., 1972; Chessells et al., 1988). Hence, present data on the behavior of HCH isomers in tropical water might be interpreted in a similar fashion to its behavior in temperate environments. Regarding the composition of D D T and its metabolites in the Vellar river in the wet season the percentage of p,p'-DDT increased more than the other D D T compounds (Fig. 8). Since a technical formulation of D D T is applied to crops (even though in little quantities) during this period, the same might have entered the water. Another possible reason is that D D T used in vector control operations during the monsoon period might have gained an entry into the coastal water bodies or drainage system of the nearby areas and ultimately into the river. On the other hand, during the dry season the percentage of p,p'-DDD was high in river water. D D D is known to be formed in reductive environments such as waterlogged paddy soil and sediment. Most of the paddy fields have little water during the dry season and hence formation ofp,p'-DDD is a great deal less in this season. Although there is no plausible explanation of this, the bottom river sediment might play a role, being the possible source of p,p'-DDD in its formation and release even in the dry season, p,p'-DDE showed a high percentage in TABLE 1 Mean Values o f A i r - W a t e r Partition Coefficients in Vellar River from Porto Novo, South India

Compound :~-HCH /#HCH ,'-HCH 6-HCH p,p'-DDE

o,p'-DDT p,p'-DDD p,p'-DDT

A 1"8 x 8'9 X 3-2 x 2"4 x 1"8 x 1"1 x 1"4 x 7"9 x

10 -4 10 . 4

10 -5 10 -5 10 -3 10 -3 10 . 4 10 . 4

B 4"3 X 1'6 x 6"2 x 4"9 x 1"0 x 2"6 x 7"1 × 1'2 x

10 . 6

10 -6 10 -~ 10 -6 10 . 4 10 -4 1 0 -'5

10 4

C 42 560 5"2 4'9 18 4'2 20 6"6

A: Theoretical values o f a i r - w a t e r partition coefficient (atm-m3/mol). B: Annual mean values o f a i r - w a t e r partition coefficient (atm-m3/mol). C: Values s h o w n in column A divided by those in column B.

Variation o[ organochlorine insecticide residues in South India

299

mangrove waters in the wet season (Fig. 9). The addition of preformed p,p'-DDE into the mangrove system by sewage channels from the nearby villages is open to speculation• As in river water during the dry season the p,p'-DDD percentage was high in mangrove water also, suggesting the existence of reductive conditions in mangrove sediment during this season. In order to understand the equilibration of organochlorine contaminants between aqueous and vapor phases and also to know the transport of pollutants through water bodies and atmosphere, air-water partition coefficients (Kh) were calculated for HCH isomers and D D T compounds. These were estimated from the HCH and D D T residue levels in air (Ramesh et al., 1989) and water (station 5 in present study) and compared with the theoretical values (Henry's Law Constants) computed from vapor pressure and solubility of the compounds (Tateya, 1987). :~-HCH and p,p'-DDT were chosen to represent the seasonal variation of Kh values of HCH isomers and D D T compounds, respectively (Figs 12 and 13). These insecticides were found to have lower values in the field than the theoretical ones over a year. All the other residues behaved in a similar fashion (Table 1). The lower field values indicate that the partition of organochlorines tends to be in water rather than air. This might be due to the fact that these insecticides are largely and directly applied into the aquatic realms such as rice fields, land drainage, municipal sewage, roadsides, ditches and other stagnant water bodies• A m o n g the HCH isomers and D D T compounds, the difference between the theoretical and the field K h values is higher in :~-HCH,/3-HCH, p,p'-DDE -3

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theoretical value

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A i r - w a t e r partition coefficients o f ~ - H C H in Vellar river over a year.

A. Ramesh et al.

300

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Fig. 13. Air-water partition coefficientsofp,p'-DDT in Vellar river over a year. and p,p'-DDD. If the theoretical K h values are assumed to express the actual equilibrium state in field conditions, these chemicals are expected to be transferred more to the atmospheric phase. On the other hand, other chemicals like 7-HCH, 6-HCH, o,p'-DDT and p,p'-DlgT which showed smaller differences have a tendency to be relatively less transportable through atmosphere. These findings indicate that tropical areas contribute organochlorine insecticide residues to remote areas through long-range atmospheric transport. To understand the status of organochlorine contamination in Indian waters, concentrations of E H C H and E D D T determined in the present study were compared with earlier reports from India and those of other countries (Table 2). A m o n g the Indian data the residue levels of E H C H recorded in our study also showed higher levels than those of others whereas E D D T levels were low. Most of the data on organochlorine residue levels reported from India deal with the levels from urban localities whereas our study was the first carried out in a rural and predominantly agricultural area. In urban areas of India, both H C H and D D T are still being used for vector control. On the other hand, in rural areas HCH is mainly used for agriculture, but the utilization of D D T is less for this purpose and frequency of its application for mosquito control is also less (Singh et al., 1988). This could be the reason why our D D T levels are lower than other places in India. A perusal of data in Table 2 also revealed that organochlorine insecticide contamination in India is high by comparison with those of other countries. Our earlier studies also revealed that concentration of HCH and D D T were highest in Indian air (Ramesh et al., 1989). The high concentration of these insecticides in air and water reiterates the contention that now India is one of the major point-source countries of organochlorine insecticide pollution. To

TABLE2

" year not known. NA: not analyzed. ND: not detected.

1976-1978 1982-1984 1982 1984 1982-1984 1985 1986 1985 1986 1987 1989

a

1-4

1"0

1 120

3-82 1~-00 50-9 300 104 600 26-3 900

8 2 000 2 560 70-25 000 40-47 000 0.051 ~4.8

3-2 000

ND 900 40-3 400

NA 1'1 20-70 ND-3"3 <2'0 260 33 22-211 7 90 210-530 <100 <100 100-300 3 1.2

22 15 NA ND-50 1-8 20 0"1-15 NA NA NA NA NA 100-900 72 0.94

1987 1985 1985 1981 1983 1976 1984 1982 1986 1986 1986 1974 1975 1981 1984 1984 1984 1984 < 1.00-56 890 NA

NA 2"5 NA

220 NA 920

1974 1970 1970-1973

lshite river, Matsuyama, Japan Chikuma river, Nagano, Japan Onga, Higashitani, Nishitani & Murasaki rivers, Kitakyushu, Japan Yodo river, Osaka, Japan Pontchartrain lake, USA Yakima river, USA Niagara river, Canada Rhine-Meuse estuary, The Netherlands Donana National Park, Spain Nile river, Egypt Shattal-Arab river, lraq Tigris river, lraq Euphrates river, lraq McIlwaine lake, Zimbabwe Nakuru lake, Kenya Paddy field water, Malaysia Stream water, Bali, Indonesia Bengawan Solo river, Indonesia Kali Porong river, Indonesia Chao Phraya river, Thailand Stream water, Ludhiana, India Jamuna river, India Urban water sources, Delhi, India Urban water sources, Kanpur, India Hooghly river, Calcutta, India Mahalon lake, Jaipur, India Jalmahal lake, Jaipur, India Vellar river, Tamil Nadu, India

~)

EDDT

C o n c e n t r a t i o n s (ng liter EHCH

Survey year

Locality

C o n c e n t r a t i o n s ( R a n g e / M e a n ) o f E H C H and E D D T i n W a t e r f r o m D i ~ r e n t P l a c e s i n t h e

Fukushima et al. (1988) McFall et al. (1985) Johnson et al. (1988) Oliver & Nicol (1984) Duinker & Hillebrand (1979) Rico et al. (1989) Et-Dib & Badawy (1985) Dou Abul et al. (1988) Dou Abul et al. (1988) Dou Abul et al. (1988) Greichus e t a / . (1978a) Greichus et al. (1978b) Meier et al. (1983) Ohsawa et al. (1985) Hillebrand et al. (1989) Hillebrand et al. (1989) Onodera & Tabucanon (1986) Kalra & Chawla (1981) Agarwal et al. (1986) Thakkar (1986) Thakkar (1986) Thakkar (1986) Kumar et al. (1988) Kumar et al. [1988) Present study

Ueda et al. (1976) Ueda et al. (1976) Suzuki et al. (1974)

Refi'rences

World

O

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r.~

7

e~

5

e~

5"

302

A. Ramesk et al.

increase food production, currently more area is brought under cultivation in India and hence a concomitant increase in the usage of insecticides is expected in the future. Since air and water are highly mobile components of the environment, it is envisaged that these chemicals from a point-source country like India are carried away to far off places. Such a process, accentuated by the continuous input o f these insecticides into the environment from agricultural and public health activities, might be alarming in the context of global contamination by organochlorines.

ACKNOWLEDGEMENTS We wish to record our deep sense of gratitude to Professor Rm. Sethunarayanan, Vice-chancellor, Annamalai University, for his wholehearted cooperation and keen interest in our work. Our thanks are also due to the Director, staff and research fellows of Marine Research Laboratory, Porto Novo, for their help. This research was supported by a Grant-in-Aid from the International Scientific Research Programme o f the Ministry of Education, Science and Culture of Japan (Project Nos 62042017 and 63041094).

REFERENCES Agarwal, H. C., Mittal, P. K., Menon, K. B. & Pillai, M. K. K. (1986). DDT residues in the river Jamuna in Delhi, India. Water, Air, Soil Pollut., 28, 89-104. Anon. (1989). Poison in your food. India Today, 14, 74-83. Chessells, M. J., Hawker, D. W., Connell, D. W. & Papajcsik, I. A. (1988). Factors influencing the distribution of lindane and isomers in soil of an agricultural environment. Chemosphere, 17, 1741 9. DouAbul, A. A. Z., AI-Saad, H. T., AI-Timari, A. A. K. & Al-Rekabi, H. N. (1988). Tigris-Euphrates Delta: A major source of pesticides to the Shatt al-Arab River (Iraq). Arch. Environ. Contam. Toxicol., 17, 405-18. Duinker, J. C. & Hillebrand, M. T. J. (1979). Behaviour of PCB, pentachlorobenzene, hexachlorobenzene, :t-HCH, 7-HCH, fl-HCH, dieldrin, endrin and p,p'-DDD in the Rhine-Meuse estuary and the adjacent coastal area. Neth. J. Sea Res., 13, 256-81. Edwards, C. A. (1985). Agrochemicals as environmental pollutants. In Control of Pesticide Applications and Residues in Food. A Guide and Director)', ed. B. V. Hofsten & G. Ekstrom. Swedish Science Press, Uppsala, Sweden, pp. 1 19. El-Dib, M. A. & Badawy, M. I. (1985). Organochlorine insecticides and PCBs in river Nile water, Egypt. Bull. Environ. Contam. Toxicol., 34, 126-33. Food and Agricultural Organization of the United Nations (1978-88). Production Yearbooks, 31 41, Rome, Italy. Fukushima, M., Kawaii, S., Yamamoto, O., Oda, K. & Morioka, T. (1988).

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