Table 1 Reagents of Organotin Compounds Temporal trends of tributyltin concentrations in seawater at the Port of Osaka and the Port of Takamatsu, Japa

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1 Distribution and Origin of Organotin Species in Seawater of the Seto Inland Sea, Japan Hiroaki TAO, Ramaswamy Babu RAJENDRAN, Ryuichi NAGANAWA, Tetsuya NAKAZATO, Akira MIYAZAKI, Masayuki KUNUGI* and Akira HARASHIMA* National Institute for Resources and Environment (16-3 Onogawa, Tsukuba, Ibaraki ) *National Institute for Environmental Studies (16-2 Onogawa, Tsukuba, Ibaraki ) [Received June 30, 1999] Summary Organotin species in seawater, collected by using a ferry between Osaka and Beppu, were determined by gas chromatography combined with inductively coupled plasma mass spectrometry after the ethylation with sodium tetraethylborate. Distributions of 9 organotin species below 1 ng Sn/l in the Seto Inland Sea were clarified for the first time. The concentrations of tributyltin (TBT) and triphenyltin (TPhT) were in the range of 0.21 `1.02 ng Sn/l and ng Sn/l, respectively. Three unknown species among them were identified as mono-, di-, and tri-octyltin species, which were used as plastic stabilizers. Butyltin and phenyltin species except for TPhT were found to occur as dissolved form, but di- and tri-octyltin species were found to occur as particular form. Principal component analysis revealed the origin of pollution at each sampling station, i.e., whether it come from antifouling paints or from plastic stabilizers. Key words: Organotin, TBT, GC-ICP-MS, Seawater, Seto Inland Sea

2 Table 1 Reagents of Organotin Compounds Temporal trends of tributyltin concentrations in seawater at the Port of Osaka and the Port of Takamatsu, Japan. This graph was derived from the data in ref. 2. The bar indicates standard deviation of three analyses.

3 Table 2 Sampling station and sample conditions

4 Fig. 2 Chromatograms of (a) a mixed standard, (b) a seawater sample (collected at Stl), and (c) blank

5 Table 3 Concentrations of Organotins in Seawater (pg/g as Sn)

6 Fig. 3 Distribution of butyltin and phenyltin species in seawater of the Seto Inland Sea The numbers on the map indicate the station number listed in Table 3.

7 Fig. 4 Chromatogram of a mixed standard of octyltins, tricyclohexyltin, fenbutatin and bis (tributyltin) oxide

8 Fig. 5 Distribution of octyltin species in seawater of the Seto Inland Sea

9 Fig. 6 Score plots and loading plots of principal components 1 and 2 derived from the concentrations of oranotin species in seawater of the Seto Inland Sea Fig. 7 Dendrogram of hierarchical cluster analysis Proportions of MBT, DBT, TBT, PhT, and OT in seawater of the Seto Inland Sea PhT=MPhT+DPhT+TPhT DOT +TOT and OT=MOT+

10 12) Tao, H., Rajendran, R. B., Quetel, C. R., Nakazato, plasma conditions. Anal. Chem., (in printing) 13) Tao, H., Murakami, T., Tominaga, M, and Miyazaki, Huggett, R. J., Unger, M. A., Seligman, P. F, and Valkirs, A.O.: The marine biocide tributyltin. Environ. Sci. Technol., 26, (1992) 5) Horiguchi, T., Shiraishi, H., Shimizu, M., Yamazaki, S. and Morita, M.: Imposex in Japanese gastropods (neogastropoda and mesogastropoda): effects of tributyltin and triphenyltin from antifouling paints. Mar. Pollut. Bull., (1995) Harino, H., Fukushima, M., Yamamoto, Y., Kawai, S. and Miyazaki, N.: Contamination of butyltin and phenyltin compounds in the marine environment of Otsuchi Bay, Japan. Environ. Pollut., 101, (1998) 9) Harino, H., Fukushima, M. and Kawai, S.: Temporal trends of organotin compounds in the aquatic environment of the Port of Osaka, Japan. Environ. Pollut., 105, 1-7 (1999) 10) Mizuishi, K., Takeuchi, M, and Hobo, T.: Trace analysis of tributyltin and triphenyltin compounds in sea water by gas chromatography-negative ion chemical ionization mass spectrometry. J. Chromatogr. A, 800, (1998) 11) Hashimoto, S., Watanabe, M., Noda, Y., Hayashi, T., Kurita, Y., Takasu, Y. and Otsuki, A.: Concentration and distibution of butyltin compounds in a heavy tanker route in the Strait of Malacca and in Tokyo Bay. Mar. Environ. Res., 45, (1998) T., Tominaga, M. and Miyazaki, A.: Tin speciation in the femtogram range in open ocean seawater by gas chromatography-inductively coupled plasma mass spectrometry using a shield torch at normal A.: Mercury speciation in natural gas condensate by gas chromatography-inductively coupled plasma mass spectrometry. J. Anal. At. Spectrom., 13, (1998) 670

11 ŠÂ Šw Vol. 9, No. 3 [1999] 14) Szpunar, J., Schmitt, V. O., Lobinski, R. and Monod, J-L.: Rapid speciation of butyltin compounds in sediments and biomaterials by capillary gas chromatography-microwave-induced plasma atomic emission spectrometry after microwave-assisted leaching/digestion. J. Anal. At. Spectrom., 11, (1996) 15) Moens, L., De Samele, T., Dams, R., Van Den Broeck, P. and Sandra, P.: Sensitive, simultaneous determination of organomercury, -lead, and -tin compounds with headspace solid phase microextraction capillary gas chromatography combined with inductively coupled plasma mass spectrometry. Anal. Chem., 69, (1997) and Chau, Y. K.: Speciation and genotoxicity of butyltin compounds. Analyst, 120, (1995) 21) Stang, P. M., Lee, R. F. and Sellgman, P. F.: Evidence for rapid, nonbiological degradation of tributyltin compounds in autoclaved and heat-treated fine-grained sediments. Environ. Sci. Technol., 26, (1992) 22) Stab, J. A., Cofino, W. P., Van Hattum, B. and Brinkman, U. A. T.: Comparison of GC/MSD and GC/AED for the determination of organotin compounds in the environment. Fresenius J. Anal. Chem., 347, (1993) 18) Randall, L. and Weber, J. H.: Adsorptive behavior of butyltin compounds under simulated estuarine conditions. Sci. Total Environ., 57, (1986) 19) Kuballa, J., Wilken, R-D., Jantzen, E., Kwan, K. K. 25) Kuballa, J., Jantzen, E. and Wilken, R-D.: Organotin compounds in sediments of the River Elbe and Mulde. pp , gsediments and Toxic Substances hedited by Calmano, W. and Forstner, U., Springer, Tokyo (1995)

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