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Page, D.S. 1995. A six-year monitoring study of tributyltin and dibutyltin in
mussel tissues from the Lynher river, Tamar Estuary, U.K, Mar. Pollut. Bull.

30:746-749.

Paul, J.D. ‘and I.M. Davies. 1986. Effects of copper- and tin-based anti-
fouling compounds on the growth of scallops (Pecten maximus) and oysters

(Crassostrea gigas). Aguaculture 54:191-203.

Pickwell, G.V. and S.A. Steinert. 1988. Accumulation and effects of organotin
cofmpounds in oyster and mussels: Correlation with serum biochemical and
cytological factors and tissue burdens. Mar. Environ. Res. 24:215-218.

’ Pinkney, A.E. 1988. Biochemical, histological and physiological effects of
tributyltin: compounds in estuarine fish. Ph.D. Dissertation. University of

. Maryland. 92 pp.

Pinkney, A.E., L.W. Hall, dx., M.L. Lenkevich, D.T. Burton and S. Zeger. 1985.
Comparison of avoidance responses of an estuarine fish, Fundulus heteroclitus,
and crustacean, Palaemonetes pugio, to bis(tri-n-butyltin) oxide. Water Aix

Soil Pollut. 25:33-40.

Pinkney, A.E., D.A. Wright and G.N. Hughes, 1989a. A morphometric study of the
effects of tributyltin compounds on the gills of the munnichog, Fundulus

115



the sensitive life-stage of hatching until an exposure concentration reached
72 ug/L: ,

, Larvae of the clam, Corbicula fluminea, has a 24-hr EcSO of 1, 990 ug/L
which isa “high concentration relative to most other species of tested
freshwater organisms. Another species of clam, Elliptio complanatus, also
showed low sensitivity ‘£0 {BT with a 96-hr LC50 of 24,600 wg/L (Table 1).
Various bivalve clam species may have the ability to reduce exposure to TBT
temporarily by closing the valves.

The cladoceran, paphnia magna, has 24-hr EC50s ranging from 3 to 13.6
ug/L (Polster and Halacha 1972; Vighi and Calamari 1985). When a more
sensitive endpoint of altered phototaxis was examined in a lenger-term
exposure of 8 days, the effect concentration (0.45 ug/L) was much lower
(Meador 1986). similarly, rainbow. trout (Oncorhynchus mykiss) exposed in.
short-term exposures of 24 to 48 hr have LC50 and -EC50 values from 18.9 to
30:8 ug/L (Table 6). When the exposure is increased to 110 days (Seinen et
al. 1981), the LC100 decreased to 4.46 pg/L and a 10% reduction in growth is
seen at'0.18 pg/L. De Vries et al. (1991) measured a similar response in
rainbow trout growth in another 110 day exposure. They demonstrated decreased
survival and growth at 0. 200 pg/L but not at 0.040 ug/L. Triebskorn et al.
(1994) found reduced growth and behavior changes at 21 days when exposed to

0.5 ug/L. The frog, Rana temporaria, has a LC50 of ‘28. 2 ug/L for a 5-day

exposure to TBT.

An attempt was made to measure the bioconcentration of TBT with the
green alga, Ankistrodesmus falcatus (Maguire et al. 1984). The algae are able
to degrade TBT to its di- and monobuty1 forms. As a result, the
concentrations of {TBT steadily declined during the 28-day study. During the
first seven days of exposure, the concentrations. declined from 20 to 5.2) ug/L
and the calculated BCF was 300 (Table 6)- After 28 days of exposure, the TBT
concentration had declined to 1.5 g/L and the calculated BCF was 467.

Several studies reported BCFs for fish but failed to demonstrate plateau
concentrations in the organism. In these studies, rainbow trout BCFs ranged

from 990. (Triebskorn et al. 1994) to 3, 833 (Schwaiger et al. 1992). Goldfish

13



Zucker, R.M., E.J. Massaro and K.H. Elstein. 1992. The reversibility of

tributyltin-induced toxicity in vitro as a function of concentration.and .

duration of exposure (C x T) 1. Environ. Res. 57:107-116.

guckerman, J.J., R.P. Reisdorf, H.V. Ellis III and R.R. Wilkinson. 1978.

Organotins in biology and the environment. In: Organometals and
organometaloids, occurrence and fate in the environment. American Chemical

Society, Brinkman, F.E., and J.M. Bellama (Eds). pp. 388-424.



(Crassostrea gigas) and the European flat oyster (Ostrea edulis). Int. Counc.

Explor. Sea, Mariculture Committee E:52. 8 pp. : : ' ’

Waldock, M.J., ‘I.E. Thain and M.E. Waite. 1987. The distribution and potential
toxic effects of TBT in U.K. estuaries during 1986. Appl. Organo. Chem. 1:287-
301.

Walker, K.E. 1977. Organotin contact studies. In: Controlled Release
Pesticides. Scher, H.B. (Ed.). ACS Symposium Series No, 53. American Chemical

Society, Washington, DC. pp. 124-131.

Walker; W.W. 1989a. Acute toxicity of bis(tributyltin) oxide to the sheepshead
minnow in a flow-through system. Final Report to M&T Chemcials, Inc. and

Sherex Chemical Co., Inc. 94 pp. ©

Walker, W.W. 1989b. Acute effect of bis(tributyltin) oxide on new shell.
deposition by the Eastern, oyster (Crassostrea virginica) under flow-through
conditions. Draft Report to Mer chemicals and Sherex Chemical Co., Inc. ,
Walsh, G.E. 1986. Organotin toxicity studies conducted with selected marine’
organisms at EPA'S Environmental Research Laboratory, Gulf Breeze, Florida.
In: Oceans 86, Vol. 4. Proceedings International Organotin Symposium. Marine

Technology, Society, Washington, DC. pp. 1210-1212.

141





Meador, J.P., U. Varanasi and C.A. Krone. 1993. Differential sensitivity of

marine infaunal amphipods to tributyltin. Mar. Biol. 116:231-239.

Meador, J.P., S.C. U'Ren, A.O. Valkirs, M.H. Salazar and S.A. Steinert. 1984.
A flow-through bioassay system-to study chronic effects of pollutants:

analysis with bis(tributyltin) oxide (TBTO). Mar. Environ. Res. 14:501.

Mercier, A., E. Pelletier and J. Hamel. 1994. Metabolism and subtle toxic

effects of butyltin compounds in starfish. Aquat. Toxicol. 28:259-273.
Miana, P., S. Scotto, G..Perin and E. Argese. 1993. Sensitivity of Selenastrum

capricornutum, Daphnia magna and submitochondrial particles to tributyltin.

Environ. Tech. 14:175-181.

Minchin, D., C.B. Duggan and W. King. 1987. Possible effects of organotins on

scallop recruitment. Mar. Pollut. Bull. 18:604-608.

Monaghan, C.P., E.J. O'Brien, Jr., H. Reust and M.L. Good. 1980. Current
status of the chemical: speciation of organotin toxicants in antifoulants. Dev.

Ind. Microbiol. 21:211-215.

Miniero, R. and G.D.D. Delupis. 1991. Effects of. TBT (tributyltin) on aquatic
‘microcosms. Toxicol. Environ. Chem. 31-32:425-431. .

111



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Weis, J.S., P. Weis and F. Wang. 1987b. Developmental effects of tributyltin

on the fiddler crab, Uca pugilator, and the killifish, Fundulus heteroclitus.

In: Oceans 87, Vol. 4. Proceedings International Organotin Symposium. Marine

Technology Society, Washinton, DC. pp. 1456-1460.

Weisfeld,.L.B. 1970. Evaluation of an accelerated test method for organotin
and organolead antifouling coating: guppy mortality. J. Paint Technol. 42:564-

568.

Wester, P.W. and J.H. Canton. 1987. Histopathological study of Poecilia
reticulata (guppy) after long-term exposure to bis (tri-n-butyltin) oxide (TBTO), -

and di-n-butyltindichloride (DBTC). Aquat. Toxicol. 10:143-165.

Wester, P.W. and J.H. Canton. 1991. The usefulness of histopathology in

aquatic toxicity studies. Comp. Biochem. Physiol. 100C:115-117.

Widdows, J. and D.S. Page. 1993. Effects of tributyltin and dibutyltin on the
physiological energetics of the mussel, Mytilus edulis. Mar. Environ. Res.

35:233-249.

W.H.O. 1990. International programme on chemical safety environmental health
eriteria for tributyltin. World Health Organization (ICS/EHC/89.29), Geneva,

Switzerland. 229 pp.



REFERENCES,

ABC Laboratories, Inc. 1990a. Acute 96-hour flow-through toxicity of bis(tri-

n-butyltin) oxide to rainbow trout (Oncorhynchus mykiss). ABC study number

38306. Analytical Bio-Chemistry Laboratories, Inc., Columbia, MO. 277 pp.

ABC Laboratories, Inc. 1990b. Acute 96-hour flow-through toxicity of bis(tri-

n-butyltin) oxide to bluegill (Lepomis macrochirus). ABC study number 38307.

Analytical Bio-Chemistry Laboratories, Inc., ‘Columbia, MO. 279 pp.-

ABC Laboratories, Inc. 1990c. Acute toxicity of bis(tributyltin) oxide to
Daphnia magna. ABC study number 38308. Analytical Bio-Chemistry Laboratories,.

Inc., Columbia, MO. 255 pp.

ABC Laboratories, Inc. 1990d. Chronic toxicity of bis(tributyltin) oxide to
Daphnia magna. ABC report number 38310. Analytical Bio-Chemistry Laboratories,

Inc., Columbia, MO. 318 pp.

Alabaster, J.S. 1969. Survival of fish in 164 herbicides, insecticides,
fungicides, wetting agents and miscellaneous substances. Int. Pest control

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Ali, A.A., R.K. Upreti and A.M. Kidwai. 1990. Assessment of di- and tri-

72



was supplied. Inorganic tin can be methylated by estuarine microorganisms
(Jackson et al. 1982). Maguire et al. (1984) reported that a 28-day culture
of TBT with the green alga, Ankistrodesmus falcatus, resulted in 7% inorganic
tin. Maguire (1986) reported that the half-life of TBT exposed to microbial
degradation was five months under aerobic’ conditions. and 1.5 months under
anaerobic conditions. TBT is also accumulated and metabolized by Zostera
marina (Francios et al. 1989). Chiles et al. (1989) found that much of. the
TET accumulated on the surface of saltwater algae and bacteria as well as
within the cell. The major metabolite of TBT in saltwater crabs, fish, and
shrimp was dibutyltin (Lee 1986).
{BT readily sorbs to sediments and suspended solids and can persist
there (Cardarelli and Evans.1980). In some instances, most TBT in the water
‘ column (70-90%) is associated with the dissolved phase (Valkirs et al. 1986a;
Maguire 1986; Johnson et al. 1987). The half-life for degradation of TBT from
sediments is reported to be greater than ten months (Maguire and Tkacz 1985).
In a modeling and risk assessment study of TBT, Traas et al. ; (1996) predicted
that TBT concentrations in the water and suspended matter would decrease
rapidly and TET concentrations in sediment and benthic organisms would
decrease at a much slower rate.

. Elevated TBT: concentrations in fresh and salt waters, sediments or
biota, are primarily associated with harbors and marinas (Cleary and Stebbing .
1985; Hall 1988; Hall et al. 1986; Langston et al. 1987; Maguire 1984,1986;
Maguire and Tkacz 1985; Maguire et al. 1982; Quevauviller et al. 1989; Salazar
and Salazar 1985b; Seligman et al. 1986,1989; Short and Sharp 1989; Stallard
et al. 1986; Stang and Seligman 1986; Unger et al. 1986; Valkirs et al. 1986p;
Waldock and Miller 1983; Waldock et al. 1987). Lenihan et al. (1990)
“hypothesized that changes in faunal composition in hard bottom communities in
San Diego Bay were related to boat. mooring and TBT. Salazar and Salazar
(1988) ‘found an apparent relationship between concentrations of TBT in waters
of San Diego Bay and reduced growth of mussels. Organotin concentrations in .

“the low part per trillion range have been associated with oyster shell ;

malformations (Alzieu et al. 1989; Minchin et al. 1987). Reevaluation of a

3



Ruiz, J.M., G.W. Bryan and P.E. Gibbs. 1994a. Bioassaying the toxicity of

tributyltin- (TBT) -polluted sediment to spat of the bivalve Scrobicularia

plana. Mar. Ecol. Prog. Ser. 113:119-130.

Ruiz, J.M., G.W. ‘Bryan and P.E. Gibbs. 1994b. Chronic toxicity of water
tributyltin (TBT) and copper to spat of the bivalve Scrobicularia plana:

ecological implications. Mar. Ecol. Prog. Ser. 113:105-117.

Ruiz, J.M., G.W. Bryan and P.E. Gibbs. 1995a. Acute and chronic ‘toxicity of
tributyltin (TBT) to pediveliger larvae of the bivalve Scrobicularia plana. -

Max. Biol. 124:119-126.

Ruiz, J.M., G.W. Bryan and P.E. Gibbs. 1995b. Effects of tributyltin (TBT)
exposure on the veliger larvae development of the bivalve Scrobicularia plana

(da Costa). J. Exp. Mar. Biol. Ecol. 186:53-63.

Riuz, J.M., G.W. Bryan, G.D. Wigham and P.E. Gibbs. 1995c. Effects of
txributyltin (TBT) exposure on the reproduction and embryonic development of
the bivalve Scobicularia plana. Mar. Environ. Res. 40 2363-379.

Saint-Louis, R., E. Pelletier, P. Masot and R. Fournier. 1994. Distribution
and effects of tributyltin chloride and its degredation products on the growth
of the marine alga Pavlova lutheri in continuous culture. Wat. Res. 28:2533-

120



Applications. Zuckerman, J.J. (Ed). pp. 204-226.

Sherman, L.R. 1983. A model for the controlled release of tri-n-butyltin -
fluoride from polymeric molluscicides and mosquito larvicides. J. Appl.

Polymer Sci. 28:2823-2829.

Sherman, L.R. and H. Hoang. 1981. The bioassay and analysis of tributyltin

fluoride. Anal. Proc. 18:196-198.

Sherman, L.R. and J.C. Jackson. 1981. Tri-n-butyltin fluoride as a controlled-
release mosquito larvicide. In: Controlled Release of Pesticides and

Pharmaceuticals. Lewis, D.H. (Ed.). Plenum Press, New York, NY. pp. 287-294.

Shiff, C.3., C. Yiannakis and A.C. Evans. 1975. ‘Further trials with TBTO and
other slow release molluscicides in Rhodesia. In: Proceedings of 1975
International Controlled Release Pesticide Symposium. Harris, F.W. (Ed.).

Wright State University, Dayton, OH. pp. 177-188.
Shimizu, A. and S. Kimura. 1992. Long-term effects of bis(n-tributyltin) oxide
(TBTO) on salt-water goby Chasmichothys dolichognathus. Nippon Suisan

Gakkaishi. 59:1595-1602.

Short, J.W. 1987. Measuring tri-n-butyltin in salmon by atomic absorption:

126 . ’



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be required to limit development of imposex.

Reproductive abnormalities have also been observed in the European flat

oyster (Thain 1986). After exposure for 75 days to a TBT concentration of
0.24 pg/L, a retardation in the sex change from male to female was observed
and larval production was completely inhibited: A TBT concentration of 2.6
ug/L prevented development of gonads. Salazar et al. (1987) found no
negative effects in the same species at 0.157 pg/L, but Thain and Waldock
(1985) and Thain (1986) measured reduced growth at 0.2392 ug/L and reduce
survival (30%) at 2.6 ug/L.

. Four species of snails (Hinia reticulata, Thais orbita, T. clavigera,
Qcenebra erinacea) not resident to North America also demonstrated imposex
effects when exposed to TBT in field studies (Text Table 1). The snail H.
xeticulata is less sensitive to TBT than other snails having higher body
burdens (>1.5 pg/L) before showing affects of imposex. Thais sp. showed high -
imposex incidence at tissue concentrations as low as 0.005 wg/L and no imposex
at other locations with tissue concentrations of 0.108 yg/L. Ocenebra
exinacea did not show imposex in a field study at body burdens. as high as
0.185 pg/L, but females were deformed at all higher concentrations.

Survival and growth of several commercially important saltwater bivalve
molluscs have been studied during acute and long-term exposures to TBT.
Mortality of larval blue mussels, ‘Wytilus edulis, exposed to 0.0973 yg/L was
51%; survivors were moribund and stunted (Beaumont. and Budd 1984). Similarly,
Dixon and Prosser (1986) observed 79% mortality of mussel larva after 4 days
exposure to 0.1 ywg/L. ‘Growth of juvenile blue mussels was significantly

reduced after 7 to 66 days at 0.31 to 0.3893 wg/L (Stromgren and Bongard 1987;

Valkirs et al. 1985). Growth rates of mussels transplanted into San Diego

* Harbor were impacted at sites where TBT concentrations exceeded 0.2 yng/L
(Salazar and Salazar 1990b). At ‘ecations where concentrations were less than
0.1 pg/L, the presence of optimum environmental conditions for growth appear
to limit or mask the effects of TBT. Less than optimum conditions for growth

may permit the effect of TBT on growth to be expressed. Salazar et al. (1987)

20



Gras, G. and J.A. Rioux. 1965. Structure-activity relationships. Organotin

insecticides (effects on larva of Culex pipiens L.). Arch. Inst.

Pasteur Tunis 42:9-21.

Guard, H.E., W.M. Coleman, III and A.B. Cobet. 1982. Speciation of tributyltin
compounds in seawater and estuarine sediments. In: Proceedings of the 185th
National Meeting of the American Chemical Society, Division of Environmental

\ :
Chemistry, Las Vegas, NV. 22(1):180-183.

Gutinski, H. 1986. The effect of sea surface microlayer enrichment on TBT
transport. In: Oceans 86, Vol. 4. Proceedings International Organotin
Symposium. Marine Technology Society, Washington, DC. pp. 1266-1274.
Guolan, H. and W. Yong: 1995. Effects of tributyltin chloride on marine

bivalve mussels. Wat. Res. 29:1877-1884.

Hall, L.W., dr. 1988. Tributyltin environmental studies in Chesapeake Bay.

Mar. Pollut. Bull. 19:431-438.

Hall, L.W. dr. 1991. A synthesis of water quality and contaminants data on
early life stages of striped bass, Morone saxatilis. Rev. Aquat. Sci. 4:261-

288.

95



Yla-Mononen 1989). .

: Alzieu (1986), Cardarelli-.and Evans (1980), Cardwell and Sheldon (1986),
Cardwell and Vogue (1986), Champ (1986), Chau (1986), Bisler (1989),
Envirosphere Company (1986), Evans ‘and Leksono (1995), Gibbs and Bryan (1987),
“Gibbs et al. (1991a), Good et al. (1980); Guard et al. (1982), Hall (1988,
1991), Hall and Pinkney (1985), Hall et al. (1991), Hodge et.al. (1979),
International Joint Commission (1976), Jensen (1977), Kimbrough (1976),
Kumpulainen and Koivistoinen (1977), Lau (1991), Laughlin (1986), Laughlin and
Linden (1985),. Laughlin ‘et al. (1984a), McCullough "et al. (1980), Monaghan et
al. (1980), North Carolina Department of Natural Resources and Community
Development ‘(1983,1985), Rexrode (1987), Salazar (1989), Seligman et al.~

* (1986), ‘slesinger and Dressler (1978), Stebbing (1985), Thayer (1984),
Thompson et al. (1985), U.S. EPA (1975,1985b), U.S. Navy (1984), Valkirs et
al. (1985y, von Rumker et al. (1974), Walsh (1986) and Zuckerman et al. (1978)
compiled data from other sources. studies: by Gibbs et al. (1987) were not
used because data were from the first year of a two-year experiment reported
in Gibbs et al. (1988).

Results were not used when the test procedures, test material, or
results were not adequately described (e.g., Bruno and Ellis 1988; Cardwell
and Stuart 1988; Chau et al. 1983; Danil'chenko and Buzinova 1982; de la Court
1980; Deschiens 1968; EG&G Bionomics 1981b; Filenko and Isakova 1980; Holwerda
and Herwig 1986; Kelly et al. 1990b; Kolosova et al. 1980; Laughlin 1983; Lee
1985; Mercier et al. 1994; Nosov and Kolosova 1979; Smith 1981c; Stroganov et
al. 1972,1977). ‘Thé 96—hr LC50 of 0.01466 ywg/L reported by Becerra-Huencho
(1984) for post larvae of the hard clam, Mercenaria meroenari: a, was not used
because results of other studies with embryos, larvae, and post larvae of the

“hard clam where acutely lethal concentrations range from 0.6 to 4.0 ug/L
(Tables 1 and 6) cast doubt on this LC50 value. Data from the life-cycle test
with sheepshead minnows (Ward et al. 1981) were not used because ratios of
measured and nominal concentrations were inconsistent within and between tests

suggesting problems in delivering TBT, analytical chemistry or both. Results

27



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vitturi,,R., C. Mansueto, E. Catalano, L. Pellerito and M.A. Girasolo. 1992.
Spermatocyte chromosome alterations in Truncatella subcylindrica (L., 1767)
(Mollusca, Mesogastropoda) following exposure to dibutyltin (Iv) and

tributyltin (Iv) chlorides. Appl. Organo. Chem. 6:525-532.

von Rumker, R., E.W. Lawless, A.F. Meiners, K.A. Lawrence,’G.L. Kelso and F.
Horay. 1974. Production, distribution, ‘use and environmental impact potential
of selected pesticides. PB-238795 or EPA-540/1-74-001. National Technical

Information Service, Springfield, VA. pp. 334-346.

wade, T.L., B. Garcia-Romero and J. Brooks. 1988. Tributyltin contamination in

bivalues from United States Coastal Estuaries. Envirion. Sci. Technol.

22:1488-1493.

Waldock, M.J. and D. Miller. 1983. The determination of total and tributyltin
in seawater and oysters in areas of high pleasure craft activity. Int. Counc.

Explor. Sea, Mariculture Committee E:12. 14 pp.

Waldock, M.J. and J.E. Thain. 1983. Shell thickening in Crassostrea gigas:

Grganotin antifouling or sediment induced? Mar. Pollut. Bull. 14:411-415.

Waldock, M.J., J. Thain and D. Miller. 1983. The accumulation and depuration

of bis (tributyltin) oxide in oysters. A comparison between the Pacific oyster

140



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Hall, L.W., dr., S.J. Bushong, W.S. Hall and W.E. Johnson. 1987. Progress -

report: Acute and chronic effects.of tributyltin on a Chesapeake Bay copepod. :

Johns Hopkins University, Shady Side, MD.

Hall, L.W., dr., S.d. Bushong,-W.S. Hall and W.E. Johnson. 1988a. Acute and
chronic effects of tributyltin on a Chesapeake Bay copepod. Environ. Toxicol.

Chem. 7:41-46.

Hall, L.W., dx., S.d. Bushong, M.C. Ziegenfuss, W.E. Johnson, R.L. Herman and
D.A. Wright. 1988b. Chronic toxicity of tributyltin to Chesapeake Bay biota.

Water Air Soil Pollut. 39:365-376.

Hall, L.W. Jx., S.A. Fischer and J.A. Sullivan. 1991. A synthesis of water
quality and contaminants data for the.Atlantic Menhaden, Brevoortia tyrannus:
implications for Chesapeake Bay. J. Environ. Sci. Health. A26:1513-1544.
Hall, L.W., dr., Mug. Lenkevich, W.S. Hall, A.E. Pinkney and S.J. Bushong.
1986. Monitoring organotin concentrations. in Maryland waters of Chesapeake
Bay. In: Oceans 86, Vol. 4. Proceedings International Organotin Symposium.

Marine Technology Society, Washington, DC. pp. 1275-1279.

Hall, L.W., Jr. and A.E. Pinkney. 1985. Acute and sublethal effects of
organotin compounds on aquatic biota: An interpretative literature evaluation.

96



Rexrode, M. 1987. Ecotoxicity of txibutyltin. In: Oceans 87, Vol. 4.
Proceedings International Organotin Symposium. Marine Technology Society,

Washington, DC. pp. 1443-1455.

Rhea, M.R., A. Proctor and R.D. Cardwell. 1995. Chronic life-cycle toxicity of
bis (tzibutyltin) oxide to Mysidopsis bahia. Elf Atochem North America, Inc.,

Philadelphia, PA. Laboratory Project No. 44-1807-16-01-MYSID. 33 pp.

Rice, C.D., M.M. Banes and T.C. Ardelt. 1995. Immunotoxicity in channel

catfish, Ictalurus punctatus , following acute exposure to tributyltin. Arch.

Environ. Contam. Toxicol. 28:464-470.

Rice, C.D. and B.A. Weeks. 1990. The influence of in vivo exposure to

tributyltin on reactive oxygen formation in oyster toadfish macrophages. Arch.

Environ, Contam. Toxicol. 19:854-857.

Rice, C.D. and B.A. Weeks. 1991. Tributyltin stimulates reactive oxygen

formation in toadfish macrophages. Dev. Comp. Immun. 15:431-436.

“Ringwood, A.H. 1992. Comparative sensitivity of gametes and early
developmental stages of a sea urchin species (Echinometra mathaei) and a
bivalve species (Isognomon californicum) during metal exposures. Arch.

Environ. Contam. Toxicol. 22:288-295.

118



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245.

Buccafusco, R. 1976a. Acute toxicity of tri-n-butyltin oxide to channel.

catfish (Ictalurus punctatus), the freshwater clam (Elliptio camplanatus), the

common mummichog (Fundulus heteroclitus) and the American oyster (Crassostrea
virginica). US EPA-OPP Registration Standard.”

Buccafusco, R. 1976b.. Acute toxicity of tri-n-butyltin oxide to bluegill
(Lepomis macrochirus). U.S. EPA-OPP Registration Standard.
Buccafusco, R., C. Stiefel, D. Sullivan, B. Robinson’ and J. Maloney, Jr. 1978.
Acute toxicity of bis(tri-n-butyl-tin) oxide to rainbow trout (Salmo
gairdneri). US EPA-OPP Registration Standard.
‘

. Burridge, T.R., T. Lavery and P.K.S. Lam. 1995. Effects of tributyltin and
formaldehyde on the germination and growth of Phyllospora comosa
(Labillardiere) Cc. Agardh (Phaeophyta: Fucales). Bull. Environ. Contam.

" Toxicol. 55:525-532.

Bushong, S.J., L.W. Hall, Jr., W.S. Hall, W.E. Johnson and R.I,. Herman. 1988.
. Acute toxicity of tributyltin to selected Chesapeake Bay fish and

invertebrates. Water Res. 22:1027-1032.

79




This document has been reviewed by the Environmental Research
Laboratories, Duluth, MN and Narragansett, RI, Office of Research and .
Development and the Health and Ecological Criteria Division, Office of Science
and Technology, U.S. Environmental Protection Agency, and approved for
publication. : :

Mention of trade names or commercial products does not constitute
endorsement or recommendation for use.

This document “is available to the public through the National Technical
Information Service (NTIS), 5285 Port Royal Road, Springfield, VA 22161.



Walsh, G-E., C.H. Deans, and L.L.- McLaughlin. 1987. Comparison of the EC50s of
algal toxicity tests calculated by four methods. Environ. Toxicol. Chem 6:767-

770.

Walsh, G.E., M.K. Louie, L.L. McLaughlin and E.M. Lorez. 1986b. Lugworm
(Azenicola cristata) larvae in toxicity tests: Survival and development when
exposed to organotins. Environ. Toxicol. Chem. 5:749-754.

Walsh, G.E., L.L. McLaughlin, E.M. Lores, M.K. Louie and C.H. Deans. 1985.
Effects of organotins on growth and survival of two marine diatoms,

Skeletonema costatum and Thalassiosira pseudonana. Chemosphere 14:383-392.

Walsh, G.E., L.L. McLaughlin, M.K. Louie, C.H. Deans and E.M. Lores. 1986a.
Inhibition of arm regeneration by Ophioderma brevispina (Echinodermata,
Ophiuroidea) by tributyltin oxide and triphenyltin oxide. Ecotoxicol. Environ.

Safety 12:95-100.

Walsh, G.E., L.L. McLaughlin, N.J. Yoder, P.H. Moody, E.M. Lores, J. Forester
and P.B. Wessinger-Duval. 1988. Minutocellus polymorphus: A new marine ‘diatom

for use in algal toxicity tests. Environ. Toxicol. Chem. 7:925-929.

Wang, W.X., J. Widdows and D.S. Page. 1992. Effects of organic toxicants on

the anoxic energy metabolism of the mussel Mytilus edulis. Mar. Environ. Res.

142



by concentrations ranging from 56.1 to 1,782 ug/L.

Acute values for 27 species of saltwater animals range from 0.61 pg/L
for the mysid, Acanthomysis sculpta, to 204.4 pg/L for adult European flat
oysters, Ostrea edulis. Acute values for the twelve most sensitive genera, .
including molluscs, crustaceans, and fishes, ‘aifter by less than a factor of
4. Larvae and juveniles appear to be more sensitive than adults. A life-
cycle toxicity test has been conducted with the saltwater mysid, nth
sculpta. The chronic value for A. sculpta was 0.1308 ug/L based on reduced
reproduction and the acute-chronic ratio was 4.664. Bioconcentration factors
for three species of bivalve molluscs range from 192.3 for soft parts of the
European flat oyster to 11,400 for soft parts of the Pacific oyster,
Crassostrea gigas. Tributyltin chronically affects certain saltwater
copepods, gastropods, and pelecypods at concentrations less than those.
predicted from "standard" acute and chronic toxicity tests. Survival of the
copepod Acartia tonsa was reduced in >0.023 ywg/L. Growth of larvae or spat of
two species of oysters, Crassostrea gigas and Ostrea edulis was reduced in
about 0.02 pg/L; some C. gigas larvae died in 0.025 ug/L. - Generally
concentrations <0.01 yg/L have not been demonstrated to affect sensitive life-
stages,of saltwater organisms. This above data demonstrate that reductions in
growth occur in commercially or ecologically important saltwater species at
concentrations of TBT less than the Final Chronic Value of 0.0500 pg/L derived
using Final Acute values and Acute-Chronic Ratios from Table 3. Therefore,
EPA believes the Final Chronic Value should be lowered to 0.01 ug/L to limit
unacceptable impacts on Acartia tonsa, Mercenaria mercenaria, Crassostrea
gigas and Ostrea edulis observed at 0.02 pg/L. At this criteria

concentration, imposex would be expected.in Ilyanassa obsoleta, Nucella
lLapillus and similarly sensitive neogastropéds; populations of N. Japilius and
similarly sensitive snails with direct development might be impacted and

growth of Mercenaria mercenaria might be somewhat lowered.

30



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Bailey, S.K., I.M. Davies, M.d.C. Harding and A.M. Shanks. 1991. Effects of

tributyltin oxide on the dogwhelk Nucella lapillus (L). The Scottish Office

Agriculture and Fisheries Department, Fisheries Research Services Report No. ~

P14/39/13/2. 153p.

Balls, P.W. 1987. Tributyltin (TBT) in the waters of a Scottish sea loch
arising from the use of antifoulant treated netting by salmon farms.

Aquaculture 65:227-237.

Batley, G.E., C. Fuhua, C.I. Brockbank and K.J. Flegg. 1989. Accumulation of
tributyltin by the Sydney rock oyster, Saccostrea commercialis. Aust. J. Mar.

Freshwater Res. 40:49-54.

Batley, G.E., M.S. Scammell and C.I. Brockbank. 1992. The impact of banning of
tributyltin-based antifouling paints on the Sydney rock oyster, Saccost: rea

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United Statés ; Office of Water ' EPA-€22-D-97-001
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AMBIENT AQUATICLIFE
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Cardarelli, N.F. 1978. Controlled release organotins as mosquito larvicides. -

Mosq. News 38:328-333.

Cardarelli, N.F. and W. Evans. 1980. Chemodynamics and environmental
toxicology of controlled release organotin molluscicides. In: Controlled
release of bioactive materials. Baker, R. (Ed.). Academic Press, New York, NY.

pp. 357-385.

Cardwell, R.D. and A.W. Sheldon. 1986. A risk assessment concerning the fate
and effects of tributyltins in the aquatic environment. In: Oceans 86, Vol. 4.

Proceedings International Organotin Symposium. Marine Technology Society,

80,



National Criteria
The procedures described in ‘the "Guidelines for Deriving Numerical

National water Quality criteria for the Protection of Aquatic Organisms and
Their Uses" indicate that, except possibly where a locally important species
is very sensitive, freshwater aquatic organisms and their uses should not be

, affected unacceptably if the four-day average concentration of tributyltin
does not exceed 0.063 ug/L more than once every three years on the average and
if the one-hour average concentration ‘does not exceed 0.46 ug ft more than once
every three years on the average. ,

The procedures described in the "Guidelines for Deriving Numerical
National Water Quality Criteria for the Protection of Aquatic Organisms and
Their Uses” indicate’ that, except possibly where a locally important species
is very sensitive, saltwater aquatic organisms and their uses should not be
affected unacceptably if the four-day average concentration of tributyltin
does not exceed 0.010 yg/L more than once every three years on the average and
if the one-hour average concentration does not exceed 0.37 pg/L more than once

every ‘three years on the average.

Implementation

As discussed’ in the Water Quality Standards Regulation (U.S. EPA 1983)
and the Foreword of this document, a water quality criterion for aquatic lite
has regulatory impact: only if it has been adopted in a state water quality
standard. such a standard specifies a criterion for a pollutant that is
consistent with a particular designated use. With the concurrence of the U.S.
“EPA, states designate one or more uses for each body of water or segment ;
thereof and adopt criteria that are consistent with the use(s) (U.S. EPA
°1987,1994). Water quality criteria adopted in state water quality standards
could have the same numerical values as criteria developed under Section 304,
of the Clean Water Act. However, in many situations states might want to
adjust water quality criteria developed under Section 304 to reflect local

environmental conditions and human exposure patterns. Alternatively, states

31



2544. °° *

Salazar, M.H. 1986. Environmental significance and interpretation of oragnotin
bioassays. Proc. Oceans 1986 Conference, Washington, D.C., 23 - 25 September |

1986, Organotin Symposium, Vol: 4.

Salazar, M.H. 1989. Mortality, growth and bioaccumulation in mussels exposed
to TBT: differences between the laboratory and the field. Proc. Oceans 1989,

Seattle, Washington. 18-21 September, 1989, Organotin Symposium, Vol. 2.

Salazar, M.H. 1992. Use and misuse of mussels in-natural resource damage
assessment. Proc. MTS '92, Washington, ‘D.C., 19-21 October, 1992, Vol. 1,

Global Ocean Resources, pp. 257-264, Marine Technology Society.

Salazar, S.M. 1985. The effects of bis(tri-n-butyltin) oxide on three species
of marine phytoplankton. NOSC-TR-1039 ‘or AD-A162-115-0. National Technical

Information Service, Springfield, VA. 17 pp.

Salazar, M.H. and D.B. Chadwick. 1991. Using real-time physical/chemical
sensors and in-situ biological indicators to monitor water pollution. In: Lc.
Wrobel and C.A. Brebbia (Eds.) water Pollution: Modelling, measuring and
‘prediction. First International Conference on Water Pollution Modeling,

Measuring and Prediction, 1991. Elsevier Applied Science; London. pp. 463.480.

121 : '



Laughlin, R.B., Jr., W: French and H.E. Guard. 1983. Acute and sublethal
toxicity of tributyltin oxide (TBTO) and its putative environmental product,
tributyltin- sulfide (TBTS) to zoeal mud crabs, Rhithropanopeus harrisii. Water

Air Soil Pollut. 20:69-79.

Laughlin, R.B., dr.,.W. French and H.E. Guard. 1986b. Accumulation of
bis(tributyltin). oxide by the’ marine mussel Mytilus edulis. Environ. Sci.

Technol. 20:884-890.

LatGghlin, R.B., Jx., W. French, R.B. Johannesen, H.E. Guard and F.E.
Brinckman. 1984a. Predicting toxicity using computed molecular topologies: The

example of triorganotin compounds. Chemosphere 13:575-584.

Laughlin, R.B., Jr., H.E. Guard and W.M. Coleman, III. 1986a. Tributyltin in
seawater: Speciation and octanol-water partition coefficient. Environ. Sci.

Technol. 20:201-204.

Laughlin, R.B., Jr., R.G. Gustafson and P. Pendoley. 1988. Chronic embryo
' larval toxicity of tributyltin (TBT) to the hard shell clam Mercenaria

mercenaria. Mar. Ecol. Progress Ser. 48:29-36.

Laughlin, R.B., dr., R.G. Gustafson and P. Pendoley. 1989. Acute toxicity of
tributyltin (TBT) to early life history stages of the hard shell. clam,

105 -


Nosov, V:N. and L.V. Kolosova. 1979. Features of a toxicological curve as a
function of the chemical structure of hetero-organic compounds. Biol. Nauki

22:97-101.

Oceans 86. 1986. Vol. 4. Proceedings International Organotin Symposium. Marine |
Technology Society, Washington, D.C. Sept. 23-25, 1986. pp. 1101-1330.

: ’
Oceans 87. 1987. Vol. 4. Proceedings International Organotin Symposium. Marine
Technology Society, Halifax, Nova Scotia, Canada. Sept. 28-Oct. 1,.-1987. pp.

1295-1524.

‘

Oehlmann, J., P. Fioroni, E. Stroben and B. Markert. 1996. qributyltin (TBT)
effects on Ocinebrina aciculata (Gastropoda: Muricidae): Imposex development,
sterilization, sex change and population decline. Sci. Tot. Environ, 188:205-
223. , ,

Oehlmann, S., E. Stroben and P. Fioroni. 1991. The morphological expression of
imposex in Nucella lapillus (Linnaeus) (Gastropoda: Muricidae). J. Moll. stud.

57:375-390.

Osada, M., T. Nomura and K. Mori. 1993. Acute toxicity and accumulation of,
tributyltin oxide in the Japanese oyster, Crassostrea gigas. Suisanzoshoku

41:439-443.

114



Ritchie, L.S., L.A. Berrios-Duran, L.P. Frick and I.“Fox. 1964. Molluscicidal
time-concentration relationships of organo-tin compounds. Bull. W.H.O. 31:147-

149.

Roberts, M.R., dr. 1987. Acute -toxicity of tributyltin chloride to embyos and
larvae of two bivalve mollusks, Crassostrea virginica and Mercenaria

mercenaria. Bull. Environ. Contam. Toxicol. 39:1012-1019.

Robert, R. and E, His. 1981. The effects: of tributyltin acetate on the eggs
. and larvae of the two commercially important molluscs ‘Crassostrea gigas :

(Thurberg) and Mytilus» al rovincialis (Link). Int. Counc. Explor. Sea,

_Mariculture Committee F:42. 16 pp.

Roberts, M.H., Jr., M.E. Bender, P.F. DeLisle, H.C. Sutton and R.L. Williams.
1987. Sex ratio, and gamete production in American oysters exposed to ,
tributyltin in the laboratory. In: oceans 87, Vol. 4. Proceedings
International organiotin Symposium. Marine Technology Society, Washington, De.
pp. 1471-1476.

Rouleau, c., E. Pelletier and H. Tjalve. 1995. Distribution kinetics of
trophic and single doses of methylmercury, tributyltin, and corresponding
inorganic ions in the starfish’Leptasterias polaris. Mar. zcol. Prog. Ser.

124:143-158.

_ 119


34:327-331. . my

Ward, G.S., G.C. cramm, PLR, Parrish, H. Trachman and A. Slesinger. 1981. °
Bioaccumulation and chronic toxicity of .bis tributyltin oxide (TBTO) : Tests
with a saltwater fish. In: Aquatic Toxicology and Hazard Assessment. pranscn,
D.R. and K.L. Dickson (Eds .) . ASTM STP 737. American Society for Testing
Materials, Philadelphia, PA. pp. 183-200.

i . . .
Webbe, G. and R.F. Sturrock. 1964. Laboratory tests of some new molluscicides

in-Tanganyika. Ann. Trop. Med. Parasitol. 58:234-239.

Weis, J.S., J, Gottleib and J. Kwiatkowski. 1987a. Tributyltin retards
regeneration and produces deformities of limbs in the fiddler crab, Uca

pugilator. Arch. Environ. Contam. Toxicol. 16:321-326.

Weis, J.S. and K. Kim..1988. Tributyltin isa teratogen in producing

deformities in limbs of the fiddler crab, Uca pugilator. arch. Environ.

Contam. Toxicol. 17:583-587.

Weis, J.S. and J. Perlmutter. 1987. Effects of tributyltin on activity and

burrowing behavior of the fiddler crab, Uca pugilator. Estuaries. 10:342-346.

143



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DRAFT
1997

AMBIENT AQUATIC LIFE WATER QUALITY CRITERIA FOR
. TRIBUTYLTIN

CAS Registry Number (See Text)

Prepared by

University of Wisconsin - Superior
Superior, WI 54880 .

and

Great Lakes Environmental Center
Traverse City, MI 49686

Prepared for

U.S. Environmental Protection Agency
, Office of Water
Office of Science and Technology
Health and Ecological Criteria Division
Washington D.C.

Office of Research and Development
, Environmental Research Laboratories
‘ . Duluth, Minnesota
Narragansett, Rhode Island

é EPA Contract No. 68-C6~0036
soe ° ° Work Assignment No. B-04



‘Upatham,, E.S., M. Xoura, Mea. Dagal, A.H. Awad and M.D. Ahmed. 19808. Focal
control of Schistosoma haematobium-transmitting snails, pulinus (Ph.)
abyasinicus, using controlled release tri-n-butyltin fluoride and copper
sulphate. In: Controlled Release of Bioactive Materials. Baker, R. (Ed.).

Academic Press, New York, NY. pp. 449-459.

“ Utren, S.C. 1983, Acute toxicity of bis(tributyltin) oxide to a marine
D ,

copepod. Mar. Pollut. Bull. 14:303-306.

U.S. EPA. 1975. Preliminary investigation of effects on the environment of
boron, indium, nickel, selenium, tin, vanadium and their compounds. Vol. V
. : :

°

U.S. EPA. 1983. Water quality standards regulation. Federal Regist. 48:51400-

51413. November 8.

U.S. EPA. 1985a. Appendix B - Response to public comments on "Guidelines for
deriving numerical national water quality criteria for the protection of
aquatic organisms and their uses." Federal Regist. 50:30793-30796. July 29.
U.S. EPA. 1985b. Tributyltin support document. Office of Pesticides and Toxic

Substances. Washington, DC.

U.S. EPA. 1986. Chapter I - Stream design flow for steady-state modeling. In:

137,



His, E. and R. Robert. 1980. Effect of tributyltin acetate on eggs and larvae

of Crassostrea gigas. Int. Counc. Explor. Sea, Mariculture Committee F:27.

Hnath, J.G. 1970. Di-n-butyltin oxide as a vermifuge on Eubothrium crassum

(Block, 1779) in rainbow trout. Prog. Fish-Cult. 32:47-50.

Hodge, V.F., S.L. Seidel’ and E.D. Goldberg. 1979. Determination of tin(IV) and
organotin compounds in natural waters, coastal sediments, and macro algae by

atomic absorption spectrometry. Anal. Chem. 51:1256-1259.

Holm, G., L. Norrgren and 0. Linden. 1991. Reproductive and histopathological
effects of long-term experimental exposure to bis(tributyltin)oxide (TBTO) on
the three-spinned stickleback, Gasterosteus aculeatus:' linnaeus. J. Fish Biol.

38:373-386.

Holwerda, D.A. and H.d. Herwig. i986. Accumulation and metabolic effects ‘of
di-n-butyltin dichloride in the freshwater clam, Anodonta anatina. Bull.

Environ. Contam. Toxicol. 36:756-762.

Hopf, H.S. and R.L. Muller. 1962. Laboratory ‘breeding and testing of

Australorbis glabratus for molluscicidal screening. Bull. W.H.O. 27:783-389.

Horiguchi, T., H. Shiraishi, M. Shimizu, S. Yamazaki and M. Morita. 1995.

98



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Organotin Symposium, Marine Technology “Society; ‘Washington, DC. pp. 1482-1487.
. . . . . .
Gibbs, P.E., G.W. Bryan, .P.L. Pascoe and G.R. Burt. 1987. The use of the dog-
whelk, Nucella lapillus, as an indicator of tributyltin (TBT) contamination.

3. Mar. Biol. Assoc. U.K. 67:507-523.

Gibbs, P.E., G.W. Bryan, P.L. Pascoe and G.R. Burt. 1990. Reproductive
abnormalities in female Ocenebra erinacea (Gastropoda) resulting from
tributyltin-induces imposex. J. Mar. Biol. Assoc. U.K. 70:639-656.

. Gibbs, P.E., P.L. Pascoe and G.R. Burt. 1988. Sex change in the female dog-
whelk, Nucella lapillus, induced by tributyltin from antifouling paints. J.

Mar. Biol. Assoc. U.K. 68:715-731.

Gibbs, P.E., P.L. Pascoe and G.W.' Bryan. 1991a. Tributyltin- induced imposex in -
stenoglossan gastropods: pathological effects on the female reproductive
system. Comp. Biochem. Physiol. 100€:231-235.

Gibbs, P.E., B.E. Spencer and P:L. Pascoe. 1991b. The American oyster drill,
Urosalpinx cinerea (Gastropoda): evidence of decline in an imposex-affected

‘population (R. Blackwater, Essex). J. Mar. Biol. Ass: 71:827-838.

Girard, J., C. Christophe, D. Pesando and P. Payan. 1996. Calcium homeostasis

93



achieved a BCF of 1,230 (Tsuda et al. 1988b) in a 14-day exposure and carp

achieved a BCF of 295 in the muscle tissue in 7 days (Teuda et al. 1987).

TBI has been shown to produce the superimposition of male sexual-
characteristics on female neogastropod (stenoglossan) snails (Smith 1981b,
Gibbs and Bryan 1987). This phenomenon, termed "imposex," can result in
females with a penis, a duct leading to the vas deferens, and a convolution of
the normally straight oviduct “(smith 1981a). Other anatomical changes
associated with imposex are detailed in Gibbs et al. (1988) and Gibbs and
Bryan (1987). Severity of “imposex is quantified using relative penis size
(RPS; ratio of female.to male penis volume) and the Bix, developmental stages :
of the vas deferens sequence (VDS) (Bryan et al. 1986; Gibbs et al. 1987).

{BT has been shown to impact populations of the Atlantic dogwhinkle
(dogwhelk), Nucella lapillus, which has direct development. In neoglossian
snails with indirect development through planktonic larval stages, the impacts
of TBT are less certain because recruitment is facilitated. Natural
pseudohemaphiodism in neoglossans occurs (Salazar and Champ 1988) and may be
caused by other organotin compounds (Bryan et al. 1988a). However, increased
global incidence and severity of imposex has been associated with areas of
high boating activity and high concentrations of TBT in water, sediment or
snails and other biota (Alvarez and Ellis 1990; Bailey and Davies 1988a,1988b;
Bryan et al. 1986,1987,; Davies et al. 1987, Durchon 1982; Ellis and Pattisima
1990; Gibbs and Bryan 1986,1987; Gibbs et al. 1987; Langston et al. 1990;
Short et al. 1989; Smith 198la, 1981b; Spence et al. 1990a).

Although imposex has been observed in 45 species of snails worldwide
(Ellis and Pattisima 1990, Jenner 1979), definitive laboratory and field
studies implicating TBT as the cause have focused on seven North American or
cosmopolitan species; the Atlantic dogwhinkle (Nucella lapillus), file
dogwhinkle (N. lima), eastern mud snail [Ilyanassa (Nassarius) obsoleta), a
snail (Hinia reticulta), welks (Thais orbita and fT. clavigera), and the
European sting winkle (Qcenebra erinacea). Imposex has been associated with
reduced reproductive potential and altered density and population structure in

field populations of N. lapillus (Spence et al. 1990a). This is related to

14



saltwater of 0.0500 ywo/L (Table 3}. Both of these Chronic values are below
the experimentally determined chronic values from life-cycle or early life-

stage tests.

to Aquatic ants
Blanck et al. (1984) reported the concentrations of TBT that prevented

growth of thirteen freshwater algal species (Table 4). These concentrations
xanged from 56.1 to 1,782 ug/L, but most were between 100 and 250 pg/L. ‘
Fargasova and Kizlink (1996), Huang et al. (1993), and Miana et al. (1993)
measured severe reduction in growth of several green alga species at TBT
concentrations ranging from 1 to 12.4 wg/L. Several green alga species appear
to be as sensitive to TBT as many animal species (Table 1). No data are ‘
available on the effects of TBT on freshwater vascular plants.

Toxicity tests on TBT have been conducted with five species of
saltwater phytoplankton including the green alga, Dunaliella tertiolecta; the
diatoms, Minutocellus polymorphus, Nitzshia sp., Phaeodactylum tricornutum,
Skeletonema costatum, and Thallassiosira pseudonana; the dinoflagellate,
Gymnodinium splendens,, the microalga, Pavlova lutheri and the macroalga, Fucus
wesiculosus (Tables 4 and 6). The 14-day EC50 of 0.06228 ywg/L for S. costatum
(EG&G Bionomics 1981ic) was the lowest value reported, but Thain (1983)

xeported that a measured concentration of 0.9732 ug/L was algistatic to the
same species (Table 4). The 72-hr EC50s based on population growth ranged
from approximately 0.3 to <0.5 wg/L (Table 6). Lethal concentrations were
generally more than an order of magnitude greater than EC50s and ranged from
10.24 to 13.82 pg/L. Identical tests conducted on tributyltin acetate,
tributyltin chloride, tributyltin fluoride, and tributyltin oxide with Ss.
*costatum resulted in EC50s from 0.2346 to 0.4693 yg/L and LC50s ‘from 10.24 to
13.82 pg/L (Walsh et al. 1985). ; _
A Final Plant Value, as defined in the Guidelines, cannot be obtained
because no test in which the concentrations of TBT were measured and the
endpoint was biologically important has been conducted with an important

aquatic plant species. The available data do indicate that freshwater and

10



Crit. Rev. Toxicol. 14:159-209.

Hall, L.W., Jx., A.E. Pinkney, S. Zeger, E.T. Burton and M.J. Lenkevich. 1984.
: 1 ot : :

Beliavioral responses to two estuarine fish species subjected to bis(tri-n-

butyltin) oxide. Water Resour. Bull. 20:235-239.

Han, J.S. and J.H. Weber. 1988. Speciation of methyl- and butyltin compounds
and inorganic tin in oysters of hydride generation atomic absorption

spectrometry. Anal. Chem. 60:316-319.

Harding, M.J.C., S.K. Bailey and I.M. Davies. 1995. Effects of TBT on the

reproductive success of the dogwhelk Nucella lapillus.

Helmstetter, M.F. and R.W. Alden III. 1995. Passive trans-chorionic transport
of toxicants in topically treated Japanese medaka (Oryzias latipes) eggs.

Aquat. Toxicol. 32:1-13.

Henderson, R.S. 1986. Effects of organotin antifouling paint leachates on
Pearl ‘Harbor organisms: A site specific flowthrough bioassay. In: Oceans 86,
Vol. 4. Proceedings Internatiorial Organotin Symposium. Marine Technology fo

Society, Washington, DC. pp. 1226-1233.

97



al. (1988b) observed no effect of 0.579 ug/L on Gammarus sp. after 24 days.
Developmental rates and growth of larval mud crabs, Rhithropanopeus harrisii,
were reduced by a 15-day exposure to 214.60 wg/L. R.- harrisii might
accumulate more TBT via ingested food than directly from water (Evans and
Laughlin 1984). ‘TBIF, TBTO, and TBTS were about equally toxic to amphipods
and crabs (Laughlin et al. 1982,1983,1984a). Laughlin and French (1989)
observed LC50 values for larval developmental stages of 13 wg/L for crabs (R.-
Harrisii) from California vs 33.6 ywg/L for crabs from Florida. Limb
malformations and reduced purrowing were observed in fiddler crabs exposed to!
0.5 G/L (Weis and Kim 1988; Weis and Perlmutter 1987). Arm regeneration was
reduced in brittle stars exposed to 0.1 yg/L (Walsh et al. 1986a). Exposure
to >0.1 g/L during settlement -of fouling organisms reduced number of species
and species diversity of communities (Henderson 1986). The hierarchy of
sensitivities of phyla in this test was similar to that of single species
tests. , ,
Exposure of embryos of the California grunion, Leuresthes tenuis, for ©
ten days to 74 yg/L caused a 50% reduction in hatching success (Newton et al.
1985). At TBT concentrations between 0.14 and 1.72 yg/L, growth, hatching

success, and survival were significantly enhanced. In contrast, growth of

inland silverside larvae was reduced after 28 days exposure to 0.093 pg/L

(Hall et al. 1988b). Juvenile Atlantic menhaden, Brevoortia tyrannus, avoided
a TBT concentration of 5.437 pg/L and juvenile striped bass, Morone Saxatilis,
avoided 24.9 pg/L (Hall et al. 1984).  BCFs were 4,300 for liver, 1,300 for
brain, and 200 for muscle tissue of chinook salmon, Oncorhynchus tshawytscha,
exposed to 1,490 yg/L for 96 hours (Short and Thrower 1986a, 1986c).

TBT concentrations less than the Final Chronic Value of. 0.0500 pg/L
from Table 3 have been shown to affect the growth of early life-stages of
commercially important bivalve molluscs and survival of ecologically ‘important
copepods (Table 6; Text Table 2). Survival of the copepod Acartia tonsa was
significantly reduced in three tests in 0.029, 0.023 and 0.024 ug/L; 30, 27

and 51 percent of control survival, respectively (Bushong et al. 1990).

22



Vol. 4. ‘Proceedings International Tributyltin Symposium. Marine Technology

Society, Washington, DC. pp. 1494-1498.

Lawler, I,F. and:J.C. Aldrich.. 1987. Sublethal effects of bis(tri-n-

butyltin) oxide on Crassostrea gigas spat. Mar. Pollut. Bull..18:274-278.

LeBlanc, G. 1976. Acute toxicity of tributyltin oxide to Daphnia magna. US

EPA-OPP Registration Standard.

Lee, R.F. 1985: Metabolism of tributyltin oxide by crabs, oysters and fish.

Max. Environ. Res. 17:145-148.

Lee, R.F. 1986. Metabolism of bis(tributyltin) oxide by ‘estuarine animals. In:
Oceans 86, Vol. 4. Proceedings International Organotin Symposium. Marine

Technology Society, Washington, DC. pp. 1182-1188.

Lee, R.F., A.O. Valkius and P.F. Seligman. 1987. In: Oceans 87, Vol. 4.

Proceedings International Organotin Symposium. Marine Technology Society,

Washington, DC. pp. 1411-1419.

Lee, R.F., K. O'Malley and Y. Oshima. 1996. Effects of toxicants on developing
oocytes and embryos of the blue crab, Callinectes sapidus. Mar. Environ. Res.

42:125-128.



Short, J.W. and F.P. Thrower. 1986c. Accumulation of butyltins in muscle

tissue of chinook salmon reared in sea pens treated with tri-n-butyltins. Mar.

Pollut. Bull. 17:542-545.

Short, J.W. and F.P. Thrower. 1987. Toxicity of tri-n-butyl-tin to chinook

salmon, Oncorhynchus tshawytscha, adapted to seawater. Aquaculture 61:193-200.

Slesinger, A.E. and I. Dressler. 1978. The environmental chemistry of three
organotin chemicals. In: Report of the Organotin Workshop. Good, M. (Ed.).
University of New Orleans, New Orleans, LA. pp. 115-162.

Smith, S.B. 1981a. Male characteristics on female mud snails caused by

antifouling bottom paints. a. Appl. Toxicol. 1:22-25.

Smith, S.B. 1981b. Reproductive anomalies in stenoglossian snails related to

pollution from marinas. J. Appl. Toxicol. 1:15-21.

Smith, S.B. 1981c. Tributyltin compounds induce male characteristics on female

mud snails Nassarius obsoletus = Ilyanassa obsoleta. J. Appl. Toxicol. 1:141-

144.

Smith, P.J., A.d. Crowe, V.G. Kumar Das and J. Duncan. 1979. Structure-
activity relationships for some organotin molluscicides. Pestic. Sci. 10:419-

128



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oxganotin compounds to crab zoea, Rhithropanopeus harrisii. Abstract from

Annual Meeting of the American Society of Zoologists, Philadelphia, PA.

23:1004.

Laughlin, R.B., dr. 1986. Bioaccumulation of tributyltin: The link between
environment and organism. In:_ Oceans 86, Vol. 4. Proceedings International

Oxganotin Symposium. Marine Technology Society, Washington, DC. pp. 1206-1209.

Laughlin, R.B., dr. and W.J. French. 1980. Comparative study of the acute
toxicity of a homologous series,of trialkyltins to larval shore crabs,
Hemigrapsus nudus, and lobster, Homarus americanus. Bull. Environ. Contam.

Toxicol. 25:802-809.

Laughlin, R.B., ox. and W. French. 1988. Concentration dependence of

bis (txributyltin) oxide accumulation in the mussel, Mytilus edulis. Environ.

Toxicol. Chem. 7:1021-1026.

Laughlin, R.B., Jr. and W.d. French. 1989. Population-related toxicity
xesponses to two butyltin compounds by zoea of mud crab Rhithropanopeus

hharrisii. Mar. Biol. 102:397-401.



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of the molluscicide tributyltin oxide to control bilharziasis. Bull. Soc.’ ©
Pathol. Exot. 59:968-973.

Deschiens, R., H. Brottes and L: Mvogo. 1966b. Effectiveness of field
applications of the molluscicide tributyltin oxide (in the control of

bilharziasis). Bull. Soc. Pathol. Exot. 59:231-234.

Deschiens, R. and H.A. Floch. 1968. Comparison of 6 chemical molluscicides as

to theix control of bilharziasis. Conclusions. Bull. Soc. Pathol. Exot.

612640-650.

Deschiens, R. and H.A. Floch. 1970. Molluscicidal use of polyethylene

impregnated with tributyltin oxide. Bull. Soc. Pathol. Exot. 63:71-78.

Deschiens, R., H. Floch and T. Floch. 1964. The molluscicidal properties of
tributyltin oxide and acetate for prophylaxis of bilharziasis. Bull. Soc.

Pathol. Exot. 57:454-465.

de Sousa, C.P. and E. Paulini. 1970. Absorption of molluscicides by. calcium
carbonate. Rev. Bras. Malariol. Doencas Trop. 21:799-818.

Q
de Vries, H., A.H. Penninks, N.J. Snoeij and W. Seinen. 1991. Comparative
toxicity of organotin compounds to rainbow trout (Oncorhynchus mykiss) yolk

86



TABLES

2. Acute Toxicity of Tributyltin to Aquatic Animals .....-..--+.+.-+ 33
2. Chronic Toxicity of Tributyltin to Aquatic Animals ..- ....-+.-- 50
3. Ranked Genus Mean Acute Values with Species Mean Acute-Chronic

Ratios bo ee ee ee BB
4. Toxicity of Tributyltin to Aquatic Plants eee . rs : 56
5. Bioaccumulation of Tributyltin by Aquatic Organisms ......-.- 58
6. Other Data on Effects of Tributyltin on Aquatic Organisms . . ev §6=$621

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Beaumont, A.R. and M.D. Budd. 1984. High mortality of the larvae of the common.

mussel at low concentrations of tributyltin. Mar. Pollut. Bull. 15:402-405.

Beaumont, A.R. and P.B. Newmann. 1986. Low levels of tributyltin reduce growth

of marine micro-algae. Mar. Pollut. Bull. 17:457-461."

Becerra-Huencho, R.M. 1984. The effect of organotin and copper sulfate on the
late development and presettlement behavior of the hard clam Mercenaria

mercenaria. Master's thesis, University of Maryland, College Park, MD. 85 pp.

Becker, K., L. Merlini, N. de Bertrand, L.F. de Alencastro and J. Tarradellas.
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organism. Bull. Environ. Contam. Toxicol. 48:37-44.

Blaix, W.R., G.d. Olson, F.E. Brinckman and W.P. Iverson. 1982. Accumulation

and fate of tri-n-butyltin cation in estuarine bacteria. Microb. Ecol. 8:241-
)

251.

Blanck,: H. 1986. University of: Goteborg, Goteborg, Sweden. (Memorandum to D.J.
Call, Center for Lake Superior Environmental Studies, University of Wisconsin-

Superior, Superior, WI. March 11.).



ACKNOWLEDGMENTS

Larry, T. Brooke

(freshwater author)

University of Wisconsin-Superior
Superior, Wisconsin

Robert L. Spehar

(document coordinator)
Environmental Research Laboratory
Duluth, Minnesota

David J. Hansen

(saltwater author)

Environmental Research Laboratory
Narragansett, Rhode Island

Glen Thursby

(saltwater coordinator)
Environmental Research Laboratory
Narragansett, Rhode Island



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Jackson, J.A., W.R. Blair, F.E. Brinkman and W.P. Iverson. 1982. Gas-
chromatographic speciation of methylstamnanes in the Chesapeake Bay using
purge and trap sampling with a tin-selective detector. Environ. Sci. Technol.

16:110-119.
Jantataeme, S. 1991. Some effects of the molluscicide bis (tri-n-butyltin)

oxide (TBTO) on the snail ‘Oncomelania qQuadrasi and the larval stages of its

trematodé parasite Schistosoma japonicum. Dissert. Abst. Internat. 52:1290-B.

99


Curtis, L.A. and A.M. Barse. 1990. Sexual anomalies in the estuarine snail
Zlyanassa obsoleta:, imposex in females and associated phenomena in males.

Oecologia. 84:371-375.

Danil'chenko, 0. 1982. A comparison of the reaction of fish embryos and

prolarvae to certain natural factors and synthesized compounds. J. Ichthyol.

(Engl. Transl. Vopr. Ikhtiol.) 22(1) :123-134.

Danil'chenko, 0. and N.C. Buzinova. 1982. Effect of pollution on the mollusc

Lyfmaea stagnalis. I. Survival, reproduction and embryonic development. Biol.

Nauki 25:61-69. . fF

Davidson, B.M., A.O. Valkirs and P.F. Seligman. 1986a. Acute and ‘chronic
effects of tributyltin on the mysid Acanthomysis sculpta (Crustacea,
Mysidacea). NOSC-TR-1116 or AD-A175-294-8. National Technical Information

Service, Springfield, VA.

Davidson, B.M., A.O. Valkirs and P.F. Seligman. 1986b. Acute and chronic
effects of tributyltin on the mysid Acanthomysis sculpta .(Crustacea,
Mysidacea). In: Oceans 86, Vol. 4. Proceeding International Organotin

Symposium. Marine Technology Society, Washington, DC. pp. 1219-1225.

Davies, I.M., S.K. Bailey and D.C.’ Moore. 1987. Tributyltin in Scottish sea

84



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is the fathead minnow, Pimephales promelas, which has a SMAV of 2.6 wg/L from
a single 96-hr flow-through measured test (Brooke et al. 1986). . Rainbow
trout, Oncorhynchus mykiss, were tested by four groups with good agreement.
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three tests (Brooke et al. 1986; Martin et a1. 1989; ABC Laboratories, Inc.
1990a) which were conducted flow-through and concentrations were measured.
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ug/L. ,

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genera which vary by more than 21,000 times from the least sensitive to the
most sensitive. Removing the least sensitive genera, Elliptio, the remainder
differ from one another by a maximum factor of 11.2 times. Based upon the
twelve available GMAVs the Final Acute Value (FAV) for freshwater organisms is
0.9177 g/L. The FAV is lower thar the lowest freshwater SMAV.

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saltwater species ‘that are useful for deriving water quality criteria
concentrations have been performed with 23 species of invertebrates and six
species of fish (Table 1). The range of acute toxicity to saltwater animals
is a factor of about 672. Acute values range from 0.42 ywg/L for juveniles of
the mysid, Acanthomysis sculpta (Davidson et al. 1986a,1986b) to 282.2 ug/L
for adult Pacific oysters, Crassostrea gigas (Thain 1983). The 96-hr Les0s
for six saltwater fish species range from 1.460, pg/L for juvenile chinook
salmon, Oncorhynchus tshawytscha (Short and Thrower 1986b) to 25.9 wg/L for
subadult sheepshead minnows, Cyprinodon variegatus (Bushong et al. 1988).

Larval bivalve molluscs and juvenile crustaceans appear to be much

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butyltin interaction with ‘skeletal muscle membranes. Bull. Environ. Contam.
Toxicol. 4429-38.

Allen, A.J., B.M. Quitter and C.M. Radick. 1980. The biocidal mechanisms of
controlled release bis(tri-n-butyltin) oxide ‘in Biomphalaria glabrata. In:
Controlled release of bioactive materials. Baker, R. (Ed.). Academic Press,

New York, NY. pp. 399-413.

Alvarez, M.M.S. and D.V. Ellis. 1990. Widespread neogastropod imposex in the
Northeast Pacific: Implications for TBT contamination surveys. Mar. Pollut.

Bull. 21:244-247.

Alzieu, C. 1986. TBT detrimental effects on oyster culture in France -
Evolution since antifouling paint regulation. In: Oceans 86, Vol. 4.

Proceedings International Organotin Symposium. Marine Technology Society,

Washington, DC. pp. 1130-1134.

Alzieu, C., J. Sanjuan, P. Michel, M. Borel and J.P. Dreno. 1989. Monitoring
and assessment of butyltins in Atlantic Coastal waters. Mar. Pollut. Bull.

20:22-26.

Alzieu, C., ¥. Thibaud, M. Heral and B. Boutier. 1980. Evaluation of the risks
of using antifouling paints near oyster zones. Rev. Trav. Inst. Peches Marit.

44:301-348.

72



Thrower, F.P. and J.W. Short. 1991. Accumulation and persistence of tri-n-
butyltin in pink and chum salmon -fry cultured in marine net-pens. Aquaculture.

96:233-239. .

Tin. EPA-560/2-75-005. National Technical Information Service, Springfield,

VA.

Trass, T.P., J.A. Stab, P.R.G. Kramer, W.P. Cofino and T. Aldenberg. 1996.
Modeling and risk assessment of tributyltin accumulation in the food web of a

shallow freshwater lake. Environ. Sci. Technol. 30:1227-1237.

Triebskorn, R., H. Kohler, J. Flemming, T. Braunbeck, R. Negele and H.
Rahmann. 1994. Evaluation of bis(tri-n-butyltin) oxide (TBTO) neurotoxicity in
xainbow trout (Oncorhynchus mykiss). I. Behaviour, weight increase, and tin

content. Aguat. Toxicol. 30:189-197.

Tsuda, T., H. Nakanishi, S. Aoki and J. Takebayashi. 1986. Bioconcentration of

butyltin compounds by round erucian carp. Toxicol. Environ. Chem. 12:137-143.

Tsuda, T., H. Nakanishi, S. Aoki and J. Takebayashi. 1988a. Bioconcentration

and metabolism of butyltin compounds in carp. Wat. Res. 22:647-651.

Tsuda, T., S. Aoki, M. Kojima and H. Harada. 1990a. The influence of ph on the

134



* Analysis with and without gas chromatography. Bull. Environ. Contam. Toxicol.
39:412-416.

: . . .
Short, J.S., S.D. Rice; €.C. Brodersen and W.B. Stickle. 1989. Occurrence of
tri-n-butyltin-caused imposex in the Pacific marine snail Nucella lima in Auke

Bay, Alaska. Mar. Biol. 102:291-297.

Short, J.W. and J.L. Sharp. 1989. ‘Tributyltin in bay mussels (Mytilus edulis)

of the Pacific coast of the United States. Environ. Sci. Technol. 23:740-743.

Short, J.W. and F.P. Thrower. 1986a. Accumulation of butyltins. in muscle
tissue of chinook salmon reared in sea pens treated with tri-n-butyltin. In:
Oceans 86, Vol. 4. Proceedings International Organotin Symposium. Marine _

Technology Society, Washington, DC. pp. 1177-1181.

Short, J.W. and F.P. Thrower. 1986b. Tri-n-butyltin caused mortality of
chinook salmon, Oncorhynchus tshawytscha, on transfer to a TBT-treated marine
net pen. In: Oceans 86, Vol. 4. Proceedings International Organotin Symposium.

Marine Technology Society, Washington, DC. pp. 1202-1205.

127


introduction
Organotins are compounds consisting of one to four organic moieties

attached to a tin atom via carbon-tin covalent bonds. When there are fewer
than four carbon-tin: bonds, the organotin compound will be a cation unless the
remaining valences of tin are occupied by an’ anion such as acetate, carbonate,
chloride, fluoride, hydroxide, oxide, or sulfide. Thus a species such as
tributyltin (77) is ‘a cation whose formula is (C4Hy)38n*. In sea water TBT
exists mainly as a mixture of the chloride, the hydroxide, the aquo complex,
and the carbonate complex ‘(Laughlin et al. 1986a).

i Several review papers have been written which cover the production,
use, chemistry, toxicity, fate and hazards of TBT in the aquatic environment
(Clark et al. 1988; Eisler 1989; Oceans 86 1986; Oceans 87 1987; WHO 1990).
The toxicities of organotin compounds are related to the number of organic a
moieties bonded to the tin atom and to the number of carbon atoms in the
organic moieties.” Toxicity to aquatic organisms generally increases as the
number of organic moieties increases from one to three and decreases with the
incorporation of a fourth, making triorganotins more toxic than other forms.
Within the triorganotins, toxicity increases as the number of carbon atoms in
the organic moiety increases from one to four, then decreases. Thus the
organotin most toxic to aquatic life is TBT (Hall and Pinkney 1985; Laughlin

and Linden 1985; Laughlin et al. 1985). TBTs inhibit Nat and K* ATPases and

are ionophores controlling exchange of Cl, Br, F’ and other ions across cell
membranes (Selwyn 1976). : : :
Organotins are used in several manufacturing processes, for example, as
an anti-yellowing agent in clear plastics and as a catalyst in poly(vinyl
chloride) products (Piver 1973). One of the more extensive uses of organotins
is as biocides (fungicides, bactericides, insecticides) and as preservatives
’ for wood, textiles, paper, leather and electrical equipment. The use of TBT
in antifouling paints on ships, boats, docks and cooling towers probably

contributes most significantly to direct release of organotins into the

aquatic environment . (Clark et al. 1988; Hall and Pinkney 1985; Kinnetic

Laboratory 1984).



422.

Spence, S.K.,, G.W. Bryan, P.E. ‘Gibbs, D. Masters, L. Morris and S.J. Hawkins.
1990a. Effects of TBT contamination on Nucella populations. Funct. Ecol.

4:425-432.

Spence, S.K., S.J. Hawkins and R.S. Santos. 1990b. The mollusc Thais
hhaemastoma -an exhibitor of ‘imposex' and potential biological indicator of
tributyltin pollution. Mar. Ecol. 11:147-156.
Springborn Bionomics. 1984a. Acute and chronic toxicity of tributyltin
fluoride to Pacific oyster (Crassostrea gigas). Report submitted to M&T
Chemicals Inc., Rahway, Nd.

)
Springborn Bionomics. 1984b. Effects of tributyltin fluoride on survival,
growth, and development of sheepshead minnow (Cyprinodon variegatus). Report

B4-84-7 to M&T Chemicals Inc., Rahway, NJ.
Stab, J.A., M. Frenay, I.L. Freriks, U.A. Brinkman and W.P. Cofino. 1995.
‘survey of nine organotin compounds in The Netherlands using the zebra mussel

(Dreissena polymorpha) as biomonitor. Environ. Toxicol. Chem. 14:2023-2032.

Stallard, N., V. Hodge and E.D. Goldberg. 1986. TBT in California coastal

129



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blockage of the oviduct by the vas deferens, hence, “prevention of release of
egg capsules, sterilization of the female or change into an apparently
fuctional male (Bryan et al. 1986; Gibbs et al. 1987,1988; Gibbs and Bryan
1986,1987).” ‘TBT may reduce populations of N. lima as snails were absent from
marinas in Auke Bay, AK. At intermediate distances from marinas, about 25
were caught per hour of sampling and 250 per hour were caught at sites distant
from marinas (Short et al. 1989). Snails from intermediate sites had blocked
oviducts. Reduced proportions of female I. ebsoleta in Sarah Creek, VA algo
suggests population impacts (Bryan et al. 1989). However, other causes may .
explain this as oviducts were ‘not blocked and indirect development .
facilitating recruitment may Limit impacts. ; ;
Several field studies have used transplantations of snails between
sites or snails painted with TBT paints to investigate the role of TBT or
proximity to marinas in the development of imposex without defining actual
exposure concentratiotis of TBT. Short et al. (1989) painted Nucellus Lima
with TBT-based paint, copper paints or unpainted controls. For 21 females
painted with TBT paint, seven developed penises within one month, whereas
penises were absent from 35 females from other treatments. Smith (1981a)
transplanted I. obsoleta between marinas and "clean" locations and found that
"incidence of imposex was unchanged after 19 weeks in snails kept at clean
locations or marinas, increased in snails. transplanted from clean sites to
marinas and decreased gomewhat in transplants from marinas to clean sites.
Snails exposed in the laboratory to TBT-based paints in two-separate
experiments developed imposex: within one month with maximum impact within 6 to
12 months (Smith 1981a). Snails painted with non-TBT paints were unaffected.
Concentration-response data demonstrate a similarity in the response
of snails to TBT in controlled laboratory. and field studies (Text Table 1).
Eastern mud snails, Illyanassa obsoleta, collected from the York River, VA
near Sarah Creek’ had no incidence of imposex (Bryan et al. 1989) and contained
no detectable TBT, (<0.020 ug/g dry weight). The average TBT concentrations
of York River water was 0.0016 ug/L. In ‘contrast, the average TBT ,

concentrations from four locations in Sarah Creek, VA were from 0.010 to 0.023

15



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Book VI -.Design conditions. In: Technical guidance manual for performing

waste load allocation. Office of Water, Washington, pe. August.
U.S. EPA. 1987. Permit writer's guide to water quality-based permitting for

toxic pollutants. EPA-440/4-87-005. Office of Water, Washington, DC.

U.S. EPA. 1991. Technical support document for water quality-based toxics
control. Office of Water, Washington, DC, March 1991, EPA 505/2-90-001 or

PB91-127415, National Technical Information Service, Springfield, VA.

U.S. EPA. 1994. Water Quality Standards Handbook: 2nd ed. EPA-823-B-94-

005a,b. Washington, DC.

U.S. Navy. 1984. Environmental assessment. Fleetwide use of organotin

antifouling paint. U.S. Naval Sea Systems Command, Washington, DC. 128 pp.

vValkirs, A., B. Davidson and P. Seligman. 1985. Sublethal growth effects and
mortality to marine bivalves and fish from long-term exposure to tributyltin.
NOSC-TR-1042 or AD-A162-629-0. National Technical Information Service,

Springfield, VA.



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par reproductive day was significantly reduced at the same concentrations

affectiny survival. The chronic limits are set at 0.19 where no effects were

seen and 0.34 ywg/L where survival and reproduction were reduced. The Chronic

Value is 0.2542 pg/L and the Acute~Chronic Ratio is 44.06 when calculated from
the acute value of 11.2 ug/L from the same test. The Acute-Chronic Ratio for
D. magna is 36.60 which is the geometric mean of the two available Acute-
Chronic ratios (30.41 and 44.06) for D. magna. .

In an early life-stage test (32-day duration) with the fathead minnow,
Pimephales promelas, all: fish exposed to the highest exposure concentration of
2.20' pg/L died during the test (Brooke et al. 1986). Survival was reduced by
2% at the next lower TBT concentration of 0.92 yg/L, but was higher than in
the controls and at 0.45 wg/L and lower concentrations. The mean weight of
the surviving fish was reduced 4% at 0.08 ug/L, 9% at 0.15 wo/L, 26% at 0.45
ug/L, and 48% at 0.92 pg/L. Mean length of fry at the end of the test was
significantly reduced at concentrations >0.45 wg/L. The mean biomass at the
end of the test was higher at the lowest TBT concentrations (0.08 and 0.15
ug/L) than in the controls, but was reduced by 13 and 52% at .TBT .
concentrations of 0.45 and 0.92 pg/L, respectively. Because the reductions in
weight of individual fish were small at the two lowest concentrations (0.08
and 0.15 pg/L) and the mean biomass increased at these same concentrations,
the chronic limits are 0.15 and 0.45 ug/L based upon growth (length and
weight) . Thus the chronic value is 0.2598 yg/L and the acute-chronic ratio
10.01 calculated using the acute value of 2.6 ug/L from the same study.

Two partial life-cycle toxicity tests were conducted using the
copepod, Eurytemora affinis (Hall et al. 1987;1988a). Tests began with egg-
carrying females and lasted 13 days. In the first test, mean brood size was
reduced from 15.2 neonates/female in the control to 0.2 neonates/female in
0.479 ywg/L. Percentage survival of neonates relative to controls was 21% in
0.088 g/L (nominal concentration of 0.100 ug/L), and 0% in 0.479 pg/L. The
chronic value is <0.088 ywg/L in this test.

In the second copepod test, percentage survival of neonates was

significantly reduced (27% relative to controls) in 0.224 ug/L; brood size was

8



Survival decreased with _Anerease in exposure concentration but was not
significantly affected in the 0.012 pg/L exposure concentration. .
Laughlin et’ al. (1987, 1988) observed a significant decrease in growth
of hard clam (Mercenaria mercinaria) larvae exposed for 14 days to 20.01 ug/L
(Text Table 2). Growth rate (increase in vaive length) was 75% of controls in
0.01 ug/L, 63% in oO. 025 Hg/Le 59% in 0.05 pg/L, 45% in 0.1 ug/L, 29% in 0.25
pg/L and 2.2% in 0.5 ug/L. A five-day. exposure followed by nine. aays in TBT-
free water produced similar responses and little evidence of recovery.
Pacific oyster (Crassostrea gigas) spat exhibited shell thickening in
0.01 and 0.05 wg/L and reduced valve lengths in >0.02 pg/L (Lawler and Aldrich
1987; Text Table 2). Increase in valve length was 101% of control lengths in
“9.02 jig/L, 72% in 0.02 g/L, 17% in 0.05 ug/l 35% in 0.1 yg/L and 0% in 0.2
ug/L. Shell thickening was also observed in this species exposed to 20.02 pg/L
for 49 days (Thain et al. 1987). they predicted from these data that
approximately 0.008 pg/L would be the maximum TBT concentration permitting
culture of commercially acceptable adults. their field studies agreed with
laboratory results showing wacceptable" shell thickness where TBT ;
concentrations averaged 0.011 and 0.015 ug/L but not at higher concentrations.
Decreased weights of oyster meats were associated with locations where there
was shell thickening. Survival’ of Crassostrea giqas larvae exposed for 21°
days was reduced in 0.025 ug/L (Springborn Bionomics 1984a). No larvae
survived in 20.050 pg/L. :
Growth of spat of the European oyster (Ostrea edulis) was reduced at
20.02 ug/L (Thain and Waldock 1985; Text Table 2). Spat exposed to TBT in
static tests were 82% of control lengths and 75% of control weights; extent. of
impact increased with increased exposure. In these static and flow-through
tests at exposures at about 0.02 ug/L, weight gain was identical; i.e., 35% of
controls. Growth of larger. spat was marginally reduced by 0.2392 ug/L (Thain
1986; Thain and Waldock 1985).
The National Guidelines (Stephan et al. 1985; pp 18 and 54) requires

that the criterion be lowered if sound scientific evidence indicates that

25



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saltwater ‘plants will be protected by TBT concentrations that adequately

protect freshwater and saltwater animals. . o

ac ation
Bioaccumulation of TET’ has been measured in one species of freshwater
“ molluse and four species of freshwater fish (Table 5). The zebra mussel,

Dressena 1: ha, was monitored ‘in cages in a marina and at an
uncontaminated site in a lake for 105 days (van ‘Slooten and Tarradellas 1994).
The organisms reached steady-state concentrations after 35 days. The BCF/BAF
was 180,427 for TBT at an average water exposure concentration of 0. 0703 ug/L.
Growth of the TBT-exposed organisms may have been slightly reduced. Martin et
al. (1989) determined the whole body bioconcentration factor (BCF) for rainbow
trout to be 406 after a 64-day exposure to 0.513 yg TBT/L. Equilibrium of the
Tar concentration was achieved in the fish in 24 to 48 hrs. In a separate
exposure to 1.026 ygTBT/L, rainbow trout organs were assayed for TBT content ,
after a 15-day exposure. ‘the BCFs ranged from 312 for muscle to 5,419 for
peritoneal fat. TBT was more highly concentrated than the metabolites of di-
and monobutyltin or tin. Carp and guppy demonstrated a plateau BCF in 14 days
and BCFs of 501.2°and 460, respectively. Goldfish reached a much higher BCF
(1,976) in the whole body than the other fish species tested.

The extent to which TBT is accumulated by saltwater animals from the
field or from laboratory tests lasting 28 days or more has been investigated
with three species of bivalve ‘molluscs, a snail, and a fish (Table 5). Thain
and’ Waldock (1985) reported a BCF of ‘6,833 for the soft parts of blue mussel
spat exposed to 0.24 yg/L for 45 days. In other laboratory exposures of blue
mussels, Salazar and Salazar (1987) observed BCFs of 10,400 to 37,500 after 56
days. BAFs from field deployments of mussels were similar to BCFs from
laboratory studies; 11,000 to 25,000 (Salazar and Salazar 1990a) and 5,000 to
60,000 (Salazar and Salazar 1991). Laboratory BCFs for the snail Nucella
lapillus (11,000 to 38,000) were also similar to field BAFs (17,000) (Bryan et
al. 1987). The soft parts of the Pacific oyster exposed to TBT for 56 days

contained 11,400 times the exposure concentration of 0.146 ywg/L (Waldock and

11



Unger,+M.A., W.G. MacIntyre, J. Greaves and R.J. Huggett. 1986. GC determina-
tion of butyltins in natural waters by flame photometric detection of hexyl .

derivatives with mass spectrometric confirmation. Chemosphere 15:461-470.

Unger, M.A., W.G. MacIntyre and R.J. Huggett. 1987. Equilibrium sorption of
tributyltin chloride by Chesapeake Bay sediments. In: Oceans 87, Vol. 4.
Proceedings International Organotin Symposium. Marine Technological Society,

Washington, DC. pp. 1381-1385.

Unger, M.A., W.G. MacIntyre and R.J. Huggett. 1988. Sorption behavior of
tributyltin on estuarine and freshwater sediments. Environ. Toxicol. Chem.

7:907-915.

Upatham, E.S. 1975. Field studies on slow-release TBTO-pellets (Biomet SRM)
against St. Lucian Biomphalaria glabrata. In: Proceedings of 1975
international controlled release pesticide symposium. Harris, F.W. (Ed.).
Wright State University, Dayton, OH. pp. 189-195.

Upatham, E.S., M. Koura, M.D. Ahmed and A.H. Awad. 1980b. Laboratory trials of
controlled release molluscicides on Bulinus (Ph.) abyssinicus, the
intermediate host of Schistosoma haematobium in Somalia. In: Controlled
Release of Bioactive Materials. Baker, R. (Ed.). Academic Press, New York, NY.

pp. 461-469.

136



Chau, ¥.K. 1986. Occurrence and speciation of organometallic compounds in

freshwater systems. Sci. Total Environ. 49:305-323.

Chau, ¥.K., R.d. Maguire and P.T. Wong. 1983. Alkyltin compounds in the
aquatic environment.-In: Proceedings of the ninth annual aquatic toxicity
workshop. Mckay, W.C. (Ed.). Canadian Technical Report of Fisheries and

Aquatic Sciences No. 1163. Department of Fisheries and Oceans, Ottawa,

Ontario, Canada. p. 204.

Chiles, T., P.D. Pendoley and R.B. Laughlin,’ Jr. 1989. Mechanisms of tri-n-
butyltin bioaccumulation by marine phytoplankton. Can. J. Fish. Aquat. Sci.

46:859-862.

Chliamovitch, Y.P. and C. Kuhn. 1977. Behavior, haemotological and
histological studies on acute toxicity of bis(tri-n-butyltin) oxide on Salmo

gairdneri Richardson and Tilapia rendalli Boulenger. Jd. Fish Biol. 10:575-585.

Clark, J.R., J.M. Patrick, Jzr., J.C. Moore and E.M. Lores. 1987. Waterborne
and sediment-source toxicities of six organic chemicals to grass shrimp .

(Palaemonetes pugio) and amphioxus - (Branchiostoma caribaeum). Atch. Environ.

Contam. Toxicol. 16:401-407.

Clark, E.A., R.M. Sterritt and J.N. Lester. 1988. The fate of tributyltin in

82



may use different data and assumptions than EPA in deriving numeric criteria
that are scientifically defensible and protective of designated uses. State
water quality standards include both numeric and narrative criteria. A state
may adopt a numeric exiterion within ite water quality standards ‘and apply it
either state-wide to all waters designated ‘gor the use the criterion is
designed to protect or to a specific site. A state may use an indicator
parameter or the national exiterion, supplemented with other relevant
information, to interpret its narrative criteria within its water quality
standards when developing NEDES effluent limitations under 40 CFR
122.44(d) (1) (vi) -2

Site-specific criteria may include not only site-specific criterion
concentrations (U.S. EPA 1994), but also site-specific, and possibly
pollutant-specific, durations of averaging periods and frequencies of allowed
excursions (U.S. EPA 1991). The averaging periods of "one hour" and "four
days" were selected by the U.S. EPA on the basis of data concerning the speed
with which some aquatic species ean react to increases in the concentrations
of some aquatic pollutants, and "three years" is the Agency's best scientific
judgment of the average amount of time aquatic ecosystems ‘should be provided
between excursions (Stephan et al. 1985; U.S. EPA 1991). However, various
species and ecosystems react and recover at greatly differing rates.
Therefore, if adequate justification is provided, site-specific and/or
pollutant-specific concentrations, durations, and frequencies may be higher or
lower than those given in national water quality criteria for aquatic lite.

Use of criteria, which have been adopted in state water quality
standards, for developing, water quality-based permit limits and for designing
waste treatment facilities requires selection of an appropriate wasteload
“allocation model. Although dynamic models are- preferred for the application
of these criteria (U.S. EPA 1991), limited ‘data or other considerations might
require the use of a steady-state model (U.S. EPA 1986).

Guidance on mixing zones and the design of monitoring programs is also

available (U.S. EPA 1987, 1991).

32



Philadelphia, PA. Laboratory Project No. 55-1807-05 (02A). 20 pp.

Brooke, L.T., D.d. Call, S.H. Poirier, T.P. Markee, C.A. Lindberg, D.J.
McCauley and P.G. Simonson. 1986. Acute toxicity and chronic effects of
bis(tri-n-butyltin) oxide to several species of freshwater organisms. Center
for Lake Superior Environmental Studies, University of Wisconsin-Superior,

: Superior, WI. 20 PP.

Bruno, D.W. and A.E. Ellis. 1988. Histopathological effects in Atlantic

salmon, Salmo salar L., attributed to the use of tributyltin antifoulant.

Aquaculture 72:15-20.

Bruschweiler, B.J., F.E. Wurgler and K. Fent..1996. Inhibition of cytochrome

P4501A by organotins in fish hepatoma cells PLHC-1. Environ. Toxicol. Chem.
. yO .

15:728-735.

Bryan, G.W., D.A. Bright, L.G. Hummerstone and G.R. Burt. 1993. Uptake tissue
distribution and metabolism of ‘c-labelled tributyltin (TBT) in the dog-

whelk, Nucella lapillus. J. Mar. Biol. Assoc. U.K. 73:889-912.

Bryan, G.W., P.E. Gibbs and G.R. Burt. 1988a. A comparison of the
effectiveness of tri-n-butyltin chloride and five other organotin compounds in

4
promoting the development of imposex in the dog-whelk, Nucella lapillus. J.

77



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Max. Biol. Assoc. U.K. 68:733-744.

Bryan, G.W., P.E. Gibbs, G.R. Burt and L.G. Hummerstone. 1987a. The effects of

tributyltin (TBT) accumulation on adult dog-whelks, Nucella lapillus: Long-

term field and laboratory experiments. J. Mar. Biol. Assoc. U.K. 67:525-544.

Bryan, G.W., P.E. Gibbs, R.J. Huggett, L.A. Curtis, D.S. Bailey and D.M.
Dauer. 1989a. Effects of tributyltin pollution on the mud snail, Ilyanassa

ebsoleta, from the York River and Sarah Creek, Chesapeake Bay. Mar. Pollut.

Bull. 20:458-462.

Bryan, G.W., P.E. Gibbs, L.G. Hummerstone and G.R. Burt. 1986. The decline of
the gastropod Nucella lapillus around south-west. England: Evidence for the
effect of tributyltin from antifouling paints. J. Mar. Biol. Assoc. U. K.

66:611-640.

Bryan, G.W., P.E. Gibbs, L.G. Hummerstone and G.R. Burt. 1987b. Copper, zinc
and organotin as long-term factors governing, the distribution of organisms in

the Fal Estuary in southwest England. Estuaries. 10:208-219.

Bryan, G.W., P.E. Gibbs, L.G. Hummerstone and G.R. Burt. 1989b. Uptake and
transformation of 14c-Jabelled tributyltin chloride by the dog-whelk, Nucella
lapillus: Importance of absorption from the diet. Mar. Environ. Res. 28:241-

78



commercialis (Iredale and Roughley) and Pacific oysters Crassostrea gigas

 ghunberg. Sci. Total Environ. 125:193-201.

Newton, F., A. Thum, B. Davidson, A. Valkirs and P, Seligman. 1985. Effects on
the growth and survival of eggs and: embryos of the California grunion
(Leuresthes tenuis) exposed to trace levels of tributyltin. NOSC-TR-1040 or

AD-A162-445-1. National Technical Information Service, Springfield, VA. 17 pp-

Nias, D.d., S.C. McKillup and K.S. Edyvane. 1993. Imposex in Lepsiella vinosa

from southern Australia. Mar. Pollut. Bull. 26:380-384.

Nishiuchi, ¥. and K. Yoshida. 1972. Toxicities of pesticides to fresh water

“snails. Bull. Agric. Chem. Insp. Stn. (Tokyo) 12:86-92.

North Carolina Department of Natural Resources and Community Development.
1983. Investigation of the effects and uses of biocides and related compounds
in North carolina. Report No. 83-09. Division of Environmental Management,

Water Quality Section, Raleigh, NC. 60 pp.
North Carolina Department of Natural Resources. and Community Development.
1985. Triorganotin regulations in North Carolina. Division of Environmental

Management, Water Quality Section, Planning Branch, Raleigh, NC.

113


heteroclitus. J. Fish Biol. 34:665-677.

Pinkney, A.E., L.L. Matteson and D.A. Wright. 1990. Effects of tributyltin on
survival, growth, morphometry and RNA-DNA ratio of larval striped bass, Morone

gaxatilis. Arch. Environ. Contam. Toxicol. 19:235-240.

Pinkney, A.E., D.A. Wright, M.A. Jepson and D.W. Towle. 1989b. Effects of
tributyltin compounds on ionic regulation and gill ATPase activity in

estuarine fish. Comp. Biochem. Physiol. 92C:125-129.

Piver, W.T. 1973. Organotin compounds: industrial applications and biological

investigation. Environ. Health Perspect. 4:61-79.

Polster, M. and K. Halacha. 1972. Hygenic-toxicological problems of some

antimicrobially.-used organotin compounds. Ernaehrungsforschung ,16:527 +535.

Pope, D.H. 1981. Effect of biocides on algae and legionnaires disease
bacteria. DE81-028768. National Technical Information Service, Springfield,

VA.

Quevauviller, P., R. Lavigne and M. Ostruc. 1989. Organotins in sediments and

mussels from the Sado estuarine system (Portugal). Environ. Pollut. 57:149-

116



ug/L, snails contained about 0.1 to 0.73 pg/g.and there was a 40 to 100%
incidence of imposex. Short et al. (1989) collected file dogwinkle snails,
Nucella lima, from Auke Bay, AK and did not detect imposex or TBT in snails
from sites far “from marinas. Snails from locations near. marinas all exhibited
_imposex and contained 0.03 to 0.16 ug/g. a . . ;
The effects of TBT on the development of imposex has been studied most
in the Atlantic dogwhinkle, Nucella lapillus. Bryan et al. (1987a) exposed
* adult snails for two years to 0.0036 (control), 0.0083, 0.046 and 0.26 ug/L in
the laboratory and compared responses to a field control." Imposex was present
in laboratory "control" snails exposed to 0.0036 ug/L and extent of penis and
vas deferens development increased’ significantly with increase in TBT
_ exposure; sterility occurred in some snails exposed to 0.26 ug/L. Ina
similar laboratory experiment that began with snail egg capsules and lasted
two years (Gibbs et al. 1988), imposex development was more severe. Field
controls. spawned and females were normal in <0.0012 ug/L. In the laboratory,
one-third of the snails exposed to 0.0036 yg/L were sterile and 160 egg cases
were produced. At >0.0093 pg/L all females were sterile with only two
” undersized egg capsules ‘Produced. Concentrations of TBT in females were 0.19
ug/g in the field, 0.58 wg/g in the 0.0036 ug/L treatment and from 1.39 to_
(7.74 ug/g in >0.0093 ‘wg/L. Similar concentrations of TBT (9.7 ug/g) were
found in snails which became sterile after they were placed in the Dart
Estuary, UK where TBT concentrations range from 0.022 to 0.046 pg/L. Gibbs
and Bryan (1986) and Gibbs et al. (1987) report imposex and reproductive
failures at other marine 7
sites where TET concentrations in female snails range from 0.32 to 1.54 ywg/g.
; In summary, in both field and laboratory studies, concentrations of TBT
in water of about 0.001 pg/L or less and in tissues of about 0.2 ug/g or less
appear to not cause imposex in N. lapillus. Imposex begins to occur, and
_ cause some reproductive failure at about 0.004 ug/L with complete sterility
occurring after chronic exposure of .sensitive early life-stages at >0.009 pg/L
and for ‘less sensitive stages at 0.02 wg/L in some studies and greater than

0.2 ug/L in others. If N. lapillus or similarly sensitive species are

ecologically important at specific sites, TBT concentrations <0.001 pg/L may



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CONTENTS

. Rage
FOLEWOLd. oe ccc c eee cece wenn cece te rscconccccecssecccccececcccssccscccscoes Adi
Acknowledgments.......- eee ecccecccccceee Av
“Tables...ecseee nace cece ewe ecw cece ese c ca ecescesesscccccccscccccesesses | VE

Text Tables ..cccccecececscccccccscccccecccececeecccscncccnscsscecesesens Vid

Introduction.......--- a biceceeetees
Acute, Toxicity to Aquatic Animals.......seeseeeccecereccccoccccsocs

Chronic Toxicity to Aquatic Animals.......s cess ccc c cece ec cec cece eteeeees

“Toxicity to Aquatic PlantG... cece csc cece ccc cn cece ec cecesecncesccccsseece

Bioaccumulation. ..-.+++ssse++e+

Other Data......see cece sees ceeceeec eee eceeneeeececeeceseesseseeeecenseees
Unused Data..... sees eee cece ccc ce eter eee eeceee cece ecsecsecseseresescene
Summary.....-

National Criteria........

Implementation. ... 2s cece cece ccc cree cece nce c ences eccccscsseeesescnseces

References.



Stephan, C.E., D.I. Mount, D.J. Hansen, J.H. Gentile, G.A. Chapman and W.A.
Brungs. 1985. Guidelines for deriving numerical national water quality
_ eriteria for the protection of aquatic organisms and their uses. PB85-227049.
National Technical Information Service, Springfield, VA. 90 pp.

Stephenson, M. 1991. A field bioassay approach to determining tributyltin

toxicity to oysters in California. Mar. Environ. Res. 32:51-59.

Stephenson, M.D., D.R. Smith, J. Goetzl, G. Ichikawa and M. Martin. 1986.
Growth abnormalities in mussels and oysters from areas with high levels of
tributyltin in San Diego Bay. In: Oceans 86, Vol. 4. Proceedings International

Organotin Symposium. Marine Technology Society, Washington, pe. pp. 1246-1251.

Stroben, E., J. Oehlmann and P. Fioroni. 1992a. The morphological expression
of imposex in Hinia reticulata (Gastropoda: Buccinida): A potential indicator

of tributyltin pollution. Mar. Biol. 113:625-636.

Stroben, E., J. Oehlmann and P. Fioroni. 1992b. Hina reticulata and Nucella

lapillus comparison, of two gastropod tributyltin bioindicators. Mar. Biol.

114:289-296.
Stroganov, N.S., 0. Danil'chenko and E.H. Amochaeva. 1977. Changes in
developmental metabolism of the mollusc Lymnaea stagnalis under the effect of

131



Valkirs, A.O., B.M. Davidson and P:F. Seligman. 1987.:Sublethal growth effects

. * .
and mortality to marine bivalves from long-term exposure to tributyltin.

Chemosphere 16:201-220.

Valkirs, A.O., P.F. Seligman and R.F. Lee. 1986a. Butyltin partitioning in
‘marine waters and sediments. In: Oceans 86, Vol. 4. Proceedings International
Organotin Symposium. Marine Technology Society, Washington, DC. pp. 1165-1170.
Valkirs, A.O., P.F. Seligman, P.M. Stang, V. Homer, S.H. Lieberman, G. Vafa
and C.A. Dooley. 1986b. Measurement of butyltin compounds ain San Diego Bay.

Mar. Pollut. Bull. 17:319-324. '

van Slooten, K. B. and J. Tarradellas. 1994. Accumulation, depuration and
growth effects of tributyltin in the’ freshwater bivalve Dreissena polymorpha

under field conditions. Environ. Toxicol. Chem. 13:755-762.

Vighi, M. and D. Calamari. 1985. QSARs for organotin compounds on Daphnia’

magna. Chemosphere 14:1925-19 32.

Virkki; L. and M. Niknmaa. 1993. Tributyltin inhibition of adrenergically
activated sodium/proton exchange in erythrocytes of rainbow trout

“ (Oncorhynchus mykiss). Aquat. Toxicol. 25:139-146.



Wishkovsky, A., E.S. Mathews and B.A. Weeks. 1989. Effect of tributyltin on
the chemiluminescent response of phagocytes from three species. of estuarine

fish. Arch. Environ. ‘Contam. Toxicol: 18:826-831.

Wolniakowski, K.U., M.D. Stephenson and G.S. Ichikawa. 1987. Tributyltin
’ concentrations and Pacific oyster deformations in Coos Bay, Oregon. In: Oceans
87, Vol. 4. Proceedings International Organotin Symposium. Marine Technology
Society, Washington, DC. pp. 1438-1442.

Worig, P.T., ¥.K. Chau, 0. Kramar and G.A. Bengert. 1982. Structure-toxicity
relationship of tin compounds on algae. Can. J. Fish. Aquat. Sci. 39:483-488.

‘
Yamada, H. and K. Takayanagi. 1992. Bioconcentration and elimination of
bis (tributyltin) oxide (TBTO) and triphenyltin chloride (TPTC) in several

marine fish species. Wat. Res. 36:1589-1595.

Yamada, H., M. Tateishi and K. Takayanagi. 1994. Bioaccumulation of organotin
compounds in the ‘red sea bream ‘(pagrus maior) by two uptake pathways: dietary

uptake and direct uptake from water. Environ. Toxicol. Chem. 13:1415-1422. ,

Yla-Mononen, L. 1989. The effects of tri-n-butyltin chloride (TBTC) on the

early life stages of perch (Perca fluviatilis L.) in brackish water. Aqua.

Fenn. 19:129-133.

145



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of some laboratory tests were not used because the tests were conducted in :
distilled or deionized water without addition of appropriate salts (e.g., Gras
and Rioux 1965; Kumar Das et al. 1984). The concentration of dissolved oxygen
was too low in tests reported by EG&G Bionomics (1981a). Douglas et al.
(1986) did not observe sufficient mortalities to calculate a useful LC5O.

Data were not used when TBT was a component of a formulation, mixture,
paint, or sediment (Boike and Rathburn 1973; Cardarelli 1978; Deschiens and
Floch 1970; Goss et al. 1979; Laughlin et al. 1982; Maguire and Tkacz 1985;
Mattiessen and Thain 1989; ‘North Carolina Department of Natural Resources and
Community Development 1983; Pope 1981; Quick and Cardarelli 1977; Salazar and
Salazar 1985a, 1985b; Santos et al. 1977; Sherman 1983; Sherman and Hoang
1981; Sherman and Jackson 1981; Walker 1977; Weisfeld 1970), unless: data were
available to show that the toxicity was the same as for TBT alone. Data were
not used when the organisms were exposed to TBT by injection or gavage (e.g-,
Fent and Stegeman 1991, 1993; Rice et al. 1995; Rice and Weeks 1990; Rouleau
et al.' 1995). Caricchia et al. (1991), Salazar and ‘Chadwick (1991), Salazar
and Salazar (1990a, 1990b, 1991), and Steinert and Pickwell (1993), did not
identify the organism exposed to TBT. Some studies did not report toxic.
effects of TBT (e.g., Balls 1987; Gibbs 1993; Meador et al. 1984; Page 1995; -
Salazar 1986; Salazar and Champ 1988).

Data were not used when the test organisms were infested with tapeworms
(e-g-, Hnath 1970). Mottley (1978) and Mottley and Griffiths (1977) conducted
tests with a mutant form of an alga. Results of tests in which enzymes,
excised or homogenized tissue, or cell cultures were exposed to the test
material were not used (e.g., Avery et al. 1993; Blair et al. 1982;
Bruschweiler et al. 1996; Falcioni ‘et al. 1996; Fent and Bucheli 1994; Fent
and Stegeman 1991; Fisher et al. 1990; Josephson et al. 1989; Joshi and Gupta

1990; Pickwell and Steinert 1988; Reader et al. 1994, 1996; Rice and Weeks

1991; Virkki and Nikinmaa 1993; Wishkovsky et al. 1989; Zucker et al. 1992).

Tests conducted with too few test organisms were not used (e.g., EG&G

Bionomics 1976; Good et al. 1979). High control mortalities occurred in tests

28



Moore, -DiW., T.M. Dillon and B.C, Suedel. 1991. Chronic toxicity of

tributyltin to the marine polychaete worm, Neanthes arenaceodentata. Aquat.

Toxicol. 21:181-198.

Mottley, J. 1978. Studies on the modes of action of n-alkylguanidines and.
triorganotins on. photosynthetic energy: conservation in the pea and the-
unicellular alga Chlamydomonas reinhardi Dangeard. Pestic. Biochem. Physiol.

9:340-350.

Mottley, J. and D.E. Griffiths. 1977. Minimum inhibitory concentrations of a
broad range of inhibitors for the unicellular alga Chlamydomonas reinhardi

Dangeard. J. Gen. Microbiol. 102:431-434.

Nagabhushanam, R., P.S. Reddy and R. Sarojini. 1991. Tissue specific
alterations in glycogen profiles by tributyltin oxide induced stress in the

prawn, Caridina rajadhari. J. Anim. Morphol. Physiol. 38:153-156.

Nagase, H., T. Hamasaki, T. Sato, H. Kito, ¥. Yoshitada and Y. Ose. 1991.
Structure-activity relationships for organotin compounds on the red killfish

Oryzias latipes. Appl. Organo. Chem. 5:91-97.

Nell, J.A. and R. Chvojka. 1992. The effect of bis-tributyltin oxide (TBTO)

and copper on the growth of juvenile Sydney rock oysters Saccostrea

112



Pacific oysters, Crassostrea gigas, was 1.557 pg/L, whereas the value for
adults | was 282.2 ug/L (Thain 1983). The 96-hr LC50s for larval and adult blue
mussels, Mytilus: edulis, were 2. 238 and 36.98 ywg/L, respectively (Thain 1983).
Juveniles of the crustaceans Acanthomysis sculpta and Metamysidopsis elongata
were slightly more sensitive to TBT than adults (Davidson et al. 1986a,1986b;
Valkirs et al. 1985; Salazar and Salazar, Manuscript). Four genera of .
amphipods were tested and sensitivity to TBT ranged from 1.3 to 22.8 pg/L. As
with bivalve molluscs and other crustaceans, one genus (Gammarus) demonstrated
greater sensitivity to TBT at the younger life-stage (Bushong et al. 1988).
Genus Mean Acute values for 27 saltwater genera range from 0.61 ug/L
for Acanthomysis to 204.4 wg/L for ‘Qstrea (Table 3). Genus Mean Acute Values
for the 13 most sensitive genera differ by a factor of less than four.
Included within these genera are four species of molluscs and nine species of

crustaceans. The saltwater Final Acute Value for TBT was calculated to be

0.7347 pg/L (Table 3), which is greater than the lowest saltwater Species Mean
Acute Value of 0.61 ug/L. :

Chronic Toxicit: to atic Anima:

The available data that are usable, according to the Guidelines,
concerning the chronic toxicity of TBT are presented in Table 2. Brooke et
al. (1986) conducted a 21-day life-cycle test with a freshwater cladoceran and
reported that the survival of adult Daphnia magna was 40% at a TBT
concentration of 0. 5 ug/L, and 100% at 0.2 pg/L. The mean number of young per
adult per reproductive day was reduced 30% by 0. 2 ug/L, and was reduced only
6% by 0.1 pg/L. The chronic limits are 0.1 and 0.2 pg/L based “upon the

. reproductive effects on / adult daphnids. The chronic value for Daphnia magna
is calculated to be 0.1414 pg/L, and the acute-chronic ratio of 30.41 is ;
calculated using the acute value of 4.3 yg/L from the same study.

Daphnia ‘pagna were exposed in a second 21-day life-cycle test to TBI
(ABC Laboratories, Inc. 19904) . Exposure concentrations ranged from 0.12 to

1.27 ug/L as TBT. Survival of adults was significantly reduced (45%) from, the

controls at 20:34 pg/L but not at 0.19 po/L.- Mean number of young per adult



The U.S. Navy (1984) proposed application of some paints containing TBT

to hulls of naval ships. Such paint formulations have been shown to be an
effective and relatively long-lived deterrent to adhesion of barnacles and
other fouling organisms. Encrustations of these organisms on ships’ hulls
reduce maximum speed and increase fuel consumption. According to the U.S.
Navy (1984), use of TBT paints, relative to other antifouling paints, would
not only reduce fuel consumption by 15% but would also increase time between
repainting from less than 5 years to.5 to 7 years. Release of TBT to water
occurs during repainting in shipyards when old paint is sand-blasted off and
new paint applied: BT would also be released continuously from the hulls of
the painted ships. Antifouling paints in current use contain copper as the :
primary biocide, whereas the proposed TBT paints would contain both copper and
TBI. Interaction between the toxicities of TBT and other ingredients in the
paint apparently is negligible (Davidson et al. 1986a). . ,

The solubility of TBT compounds in water is influenced by such factors
as the oxidation-reduction potential, pH, temperature, ionic strength, and
concentration and composition of the dissolved organic matter (Clark et al. .
1988; Corbin 1976). The solubility of tributyltin oxide in water was reported
to be 750 Hg/L at pH of 6.6, 31,000 pg/L at pH of 8.1 and 30,000 pg/L at pH
2.6 (Maguire et al. 1983). The carbon-tin covalent bond does not hydrolyze in
water (Maguire et al. 1983,1984), and the half-life for photolysis due to
sunlight is greater than 89 days (Maguire et al. 1985; Seligman et al. 1986).
Biodegradation is the major breakdown pathway for TBT in water and sediments
with half-lives of several days in water to several weeks in sediments (Clark
et al. 1988; Lee et al. 1987; Maguire and Tkacz 1985; Seligman et al. 1986,
1988, 1989; Stang and Seligman 1986). Breakdown products include di- and
monobutyltins with some butylmethyltins detected..

Some species of algae, bacteria, and fungi have been shown to degrade
TBT by sequential dealkylation, resulting in dibutyltin, then monobutyltin,
and finally inorganic tin (Barug 1981; Maguire et al. 1984). Barug (1981)
observed the biodegradation of TBT to di- and monobutyltin by bacteria and

fungi only under aerobic conditions and only when a secondary carbon source



FOREWORD

Section 304(a)(1) of. the Clean Water Act of 1977 (P.L. 95-217) requires
the Administrator of the Environmental Protection Agency to publish water
quality criteria that accurately reflect the latest scientific knowledge on
the kind and extent of all identifiable effects.on health and welfare that
might be expected from the presence ,of pollutants in any body of water,
including ground water. This document -is a revision.of proposed criteria
based upon consideration of comments received from other federal agencies,
state agencies, special interest groups, and individual scientists. Criteria
contained in this document replace any previously published EPA aquatic life
criteria for the same pollutant(s)- . .

The term "water quality criteria" is used in two sections of the Clean
Water Act, section 304(a)(1) and section 303(c)(2). The term has a different
program impact in each section. In section 304, the term represents a non-
regulatory, scientific assessment of ecological effects. Criteria presented
in this document are such scientific assessments. If water quality criteria
associated with specific stream uses are adopted by a state as water quality
standards under section 303, they represent maximum acceptable pollutant
concentrations in ambient waters within that state that are enforced through
issuance of discharge limitations in NPDES permits. Water quality criteria
adopted in state water quality standards could have the same. numerical values
as’ criteria developed under section 304. However, in many situations states
might want to. adjust water quality criteria developed under section 304 to _
reflect local environmental conditions and human exposure patterns.
Alternatively, states may use different data and assumptions than EPA in
deriving numeric criteria that are scientifically defensible and protective of
designated uses. It is not until their. adoption as part of state water
quality standards that criteria become regulatory. Guidelines to assist the
States and Indian tribes in modifying the criteria presented in this document
are contained in the Water Quality Standards Handbook (U.S. EPA 1994). This
handbook and additional guidance on the development of water quality standards

and other water-related programs of this Agency have been developed by the
Office of Water. . .

. This document, if finalized, would be guidance only. It would not
establish or affect legal rights or obligations.. It would not establish a
binding norm and would not be finally determinative of the issues addressed.
Agency decisions in any particular situation will be made by applying the
Clean Water Act and EPA regulations on the basis of specific facts presented
and scientific information then available.

Tudor T. Davies
Director ;
Office of Science and Technology



Santos, A.T., M.d. Santos, B.L. Blas and E.A. Banez. 1977. Field trials using
slow release rubber molluscicide: formulations. MT-1E (Biomet SRM) and CBL-9B.
In: Controlled release pesticides. Scher, H.B. (Ed.). ‘ACS Symposium Series No.”

53. American Chemical Society, Washington, DC. pp. 114-123.

Sarojini, R., B. Indira and R. Nagabhushanam, 1991. Effect of antifouling
organometallic compounds on the brain of mature female prawn Caridina weberi.

a. Adv. Zool. 12:93-99. *

Sarojini, R., P.S. Reddy and R. Nagabhushanam. 1992. Acute and chronic
tributyltin induced alterations in digestive enzymes of the prawn, Caridina

gajadhari. Uttar Pradesh J. Zool. 12:20-24.

Scadding, $.R. 1990. Effects of tributyltin oxide on the skeletai structures
of developing and regenerating limbs of the axolotl larvae, Ambystoma .

Mexicanum. Bull. Environ. Contam. Toxicol. 45:574-581.

Scammell, M.S., G.E. Batley and C.I. Brockbank. 1991. A field study of the
impact on oysters of tributyltin introduction and removal-in a pristine lake.

Arch. Environ. Contam. Toxicol. 20:276:281.

Schwaiger, J., F. Bucher, H. Ferling, W. Kalbfus and R. Negele. 1992. A

prolonged toxicity study on the effects of sublethal concentrations of

124



Khan, A.T., J.S. Weis, C.E. Saharig and A.E. Polo. 1993. Effect of tributyltin
on mortality and telson regeneration of grass shrimp, Palaemontetes pugio.

Bull. Environ. Contam. Toxicol. 50:152-157.

Kimbrough, R.D. 1976. Toxicity and health effects of selected organotin

compounds: a review. Environ. Health Perspect. 14:51-56.
Kinnetic Laboratory. 1984. Status of knowledge concerning environmental
concentrations and effects of tributyltin in aquatic systems. Final Report to

Electric Power Research Institute: KLI-R-84-9. KLI, Santa Cruz, CA.

Kolosova, L.V., V.N. Nosov and I.Q. Dobrovolskii. 1980. Structure of hetero-

organic compounds and their effect on Daphnia. Hydrobiol. J. (Engl. Transl.

Gidrobiol. Zh.) 16 (3) :184-193.

Kubo, ¥., H. Asano, H. Kumai and G. Fuse. 1984. Studies on the toxic effects
of wood preservatives on the aquatic organisms (Part 2). Soc. Antibac.

Antifum. Agents, Jpn. 12:551-559.

Kumar Das, V.G., L.¥. Kuan, K.I. Sudderuddin, C.K. Chang, V. Thomas, C.K. Yap,
M.K. Lo, G.C. Ong, W.K. Ng and Y. Hoi-sen. 1984. The toxic effects of
triorganotin(IV) compounds on the- culicine mosquito, Aedes aegypti (L.).

Toxicology 32:57-66..



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Thain 1983). A BCF of 6,047 was observed for the soft ‘parts of the Pacific
oyster exposed to 0.1460 pg/L for 21 days (Waldock et al. 1983). The lowest
steady-state BCF reported for a bivalve was 192.3 for the soft parts of the
European flat oyster, Ostrea edulis, exposed to a TBT concentration of 2.62
ng/L for 45 days (Thain 1986; Thain and Waldock 1985). Other tests with the
same species (Table 5) resulted in BCFs ranging from 397 to 1,167. One
species of saltwater fish was exposed to 0.28 yg/L for 14 days and a plateau
BCF of 240 was demonstrated (Tsuda et al. 1990b). ;

No U.S. FDA action level or other maximum acceptable. concentration in
tissue, as defined in the Guidelines, is available for TBT, and,, therefore, no

Final Residue Value can be calculated.

other Data

Additional data on the lethal and sublethal effects of TBT on aquatic
species are presented in table 6. Two microcosm studies were conducted by
Delupis and Miniero (1989, 1991) in which single dose effects were measured on’
natural assemblages of organisms. In both studies the effects were immediate.
Daphnia magna disappeared soon. after a 80 yg/L dose of TBT, ostracods
increased, and algal species increased immediately then gradually disappeared.
In the second study metabolism was monitored by measuring oxygen consumption.
Doses of TBT (4.7 and 14.9 pg/L) were administered once and. metabolism was
reduced by 2.5 days and returned to normal in 14.1 days in the lower exposure.
In the higher exposure, metabolism was reduced in one day and returned to ;

normal in 16 days.

Wong et al. (1982) exposed a natural assemblage of freshwater algae

and several pure cultures of various algal” species to TBT in 4-hr exposures.
Effects (EC50s) were seen in all cases on the production or reproduction at
concentrations ranging from 5 to 20 ug/L which demonstrates a high sensitivity
to TBT.

Freshwater rotifers (Brachionus calycifiorus) and coelentrate (Hydra
sp.) showed widely differing sensitivites to TBT. Hydra sp. were affected at

0.5 yg/L resulting in deformed tentacles, but the rotifer was not affected at

12



accumulation of tri-n-butyltin chloride and triphenyltin chloride in carp.

comp. Biochem. Physiol. 95C:151-153.

Tsuda, T., S. Aoki, M. Kojima and T. Fujita. ‘1991a. Accumulation and excretion
of tri-n-butyltin chloride and. triphenyltin chloride by willow shiner. Comp.

Biochem. Physiol. 101C:67-70.

Tsuda, Tee S. Aoki, M. Kojima and H. Harada. 1991b. Accumulation of tri-n-
butyltin chloride and triphenyltin chloride by oral and via gill intake of

goldfish (Carassius. auratus). Comp. Biochem. Physiol. 99C:69-72,

Tsuda, T., S. Aoki, M. Kojima and H. Harada. 1990b. Differences between
freshwater and seawater -acclimated guppies in the accumulation and excretion

of tri-n-butyltin chloride and triphenyltin chloride. Wat. Res. 24:1373-1376.

Tsuda, T., M. Wada, S. Aoki and Y. Matsui. 1887. Excretion of bis(tri-n-
butyltin) oxide and triphenyltin chloride from carp. Toxicol. Environ. -Chem.

16:17-22. . ~

“Tsuda, T.,'M. Wada, S. Aoki and Y. Matsui. 1988b. Bioconcentration, excretion
and metabolism of bis (tri-n-butyltin) oxide and triphenyltin chloride by

goldfish. Toxicol. Environ. Che,. 18:11-20.

135 oy





, Thain, J-E. 1986. Toxicity of TBT ‘to bivalves: Effects on reproduction, growth

and survival. In: Oceans 86, Vol. 4. Proceedings International Organotin

Symposium. Marine Technology Society, Washington, DC. pp. 1306-1313.

Thain, J.E. and M.Jd. Waldock. 1985. The growth of bivalve spat exposed to
organotin leachates from antifouling paints. Int. Counc. Explor: Sea,

Mariculture Committee E:28. 10 pp.

Thain, J.E., M.J. Waldock and M.E. Waite. 1987. Toxicity and degradation
studies of tributyltin (TBT) and dibutyltin (DBT) in the aquatic environment.

In: Oceans 87, Vol. 4. Proceedings International Organotin Symposium. Marine

Technology Society, Washington, DC. pp. 1398-1404.

Thain, J.E. and M.J. Waldock. 1986. The impact of tributyl tin (TBT)

antifouling paints on molluscan fisheries. Wat. Sci. Tech, 18:193-202.

Thayer, J.S. 1984. Organometallic compounds and living organisms. Academic

Press, Orlando, FL. 245 pp.

Thompson, J.A.J., M.G. Sheffer, R.C. Pierce, Y.K. Chau, J.J. Cooney, W.R.
Cullen and R.J. Maguire. 1985. Organotin compounds in the aquatic environment:
Environmental quality. NRCC 22494. National Research Council Canada, Ottawa,

Canada. 287 pp.



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growth of the freshwater alga Scenedesmus quadricauda. Ecotoxicol. Environ.°

Safety. 34:156-159.

Fent, K. 1991. Bioconcentration and elimanation of tributyltin chloride by

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Toxicol. 28:107-126.

Fent, K. and J. Hunn. 1993. Uptake and elimination of tributyltin in fish-

yolk-sac larvae. Mar. Environ. Res. 35:65-71.

Fent, K. and P.W. Looser. 1995. Bioaccumulation and bioavailability of

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Fent, K. and W. Meier. 1992. Tributyltin-induced effects on early life stages

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Fent, K. and J.J. Stegeman.. 1991. Effects of tributyltin chloride in vitro on

90



tributyltin chloride in low concentrations. Biol. Nauki 20:75-78.

Stroganov, N.S., V.G. Khobotev and L.V. Kolosova. 1972. Study of the
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Sujatha, C.H., S.M. Nair and J. Chacko. 1996. Tributyltin oxide induced
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TAI Environmental Sciences Inc. 1989b. Toxicity of tri-butyl tin oxide to

Hydra littoralis and Chlorohydra yviridissima. Mobile, Al, 13 September. 25 pp.

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Cleary, J.J. and A.R.D. Stebbing. 1985. Organotin and total tin in coastal

water of southwest England. Mar. Pollut. Bull. 16:350-355.

Cleary, J.J. and A.R.D. Stebbing. 1987. Organotin in the surface microlayer

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83



TEXT TABLES

Summary of available laboratory and field studies

relating the extent of imposex of female snails,

measured by relative penis size (volume female

penis + male penis = RPS) and the vas deferens

sequence index (VDS),.as a function of tributyltin

concentration in water and dry tissue... - - 2 + + s+ 2 8 16

Summary of laboratory and field data on the effects
of tributyltin on saltwater organisms at concentrations

less than the Final Chronic. Value of 0.0500 ug/L .....- - 23

vii



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, _ - 89)



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Ecol. 174:227-242.



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harbor in the United Kingdom show that since the 1987 restrictions on
tributyltin use, oyster culture has returned in the harbor (Dyrynda 1992). In
some cases the water surface microlayer contained a much higher concentration
of TET than the water column (Cleary and Stebbing 1987; Hall et al. 1986;
Valkirs et al. 1986a). Gucinski (1986) suggested that this enrichment of the
surface microlayer might increase the bioavailability of TBT. TBT accumulates
in sediments with sorption coefficients which may range from 1.1x10? to
8.2x10? L/Kg:and desorption appears to be a two step process (Unger et al.
1987,1988). No organotins were detected in the muscle tissue of feral chinook
salmon, Oncorhynchus tshawytscha, caught near Auke Bay, Alaska, | but
concentrations as high as 900 yg/kg were reported in muscle tissue of chinook
salmon held in pens treated with TBT (Short 1987; Short and Thrower 1986a).

. Only data generated in toxicity and bioconcentration tests on TBTC
(tributyltin chloride; ‘CAS 1461-22-9), TBTF (tributyltin fluoride; CAS 1983-
10-4), TBTO [bis(tributyltin) oxide; CAS 56-35-9], commonly called :
"tributyltin oxide" and TBTS [bis(tributyltin) sulfide; CAS 4808-30-4),
commonly called “tributyltin sulfide" were used in the derivation of the water
quality criteria concentrations for aquatic life presented herein. All
concentrations from such tests are expressed as TBT, not as tin and not as the
chemical tested. Therefore, many concentrations listed herein are not those
in the reference cited but are concentrations adjusted to TBT. A
comprehension of the "Guidelines for Deriving Numerical National Water Quality
Criteria for the Protection of Aquatic Organisms and Their Uses" (Stephan et
al. 1985), hereinafter referred to as the Guidelines, and the response to
public comment (U.S. EPA 1985a) is necessary to understand the following text,
tables, and calculations. Results of such intermediate calculations as’
“yecalculated LCSO0s and Species Mean Acute Values are’ given to four significant
figures to prevent roundoff error in subsequent calculations, not to reflect
the precision of the value. fhe Guidelines requires that all available
pertinent laboratory and field information be used to derive a criterion

consistent with sound scientific evidence. The saltwater criterion for TBT

follows this requirement by using data from chronic exposures of copepods and

2



the hepatic microsomal monooxygenase system in the fish Stenotomus chrysops.
Aquat. Toxicol. 20:159-168.
Fent, K. and J.J. Stegeman. 1993. Effects of tributyltin-in vivo on hepatic

cytochrome P450 forms in marine fish. Aquat. Toxicol. 24:219-240.

Filenko, O.F. and E.F. reakova. 1980. The prediction of the effects of
pollutants: on aquatic organisms based on the data of acute toxicity
experiments. In: Proceedings of the third USA-USSR symposium on the effects of
pollutants upon aquatic ecosystems. Swain, W.R. and V.R. ‘Shannon (Eds.). EPA- .
600/9-80-034. National Technical Information Service, springfield, VA. pp.

138-155.

Fisher, W.S., A. Wishkovsky and F.E. Chu. 1990. Effects of tributyltin on
defense-related activities of oyster hemocytes. Arch. Environ. Toxicol.

19:354-360.

Foale, S. 1993. An evaluation of the potential of gastropod imposex as a
bioindicator of tributyltin pollution in Port Phillip Bay, Victoria. Mar.

Pollut. Bull. 26:546-552.

694



unaffected in any tested concentration (0.018-0.224 ug/L). Although no
statistically significant effects were detected in 0.100 ug/L; percentage
survival of neonates appears reduced; 76% vs 90% in controls.” The chronic
value in this test is 0.150 ug/L. Survival of neonates in both tests in the
0.100 ug/L nominal concentration (mean measured concentration =. 0.094 ug/L)
averaged 42% relative to controls. If this is the best estimate of the upper
chronic value, and the 0.056 pg/L treatment from the second test is the best
estimate of the lower chronic value, the overall chronic value for the two
tests is 0.0725 pg/L. . The overall acute-chronic ratio is 27.24 when the acute
value of 1.975 ywg/L (mean of acute values of 1.4, 2.2 and 2.5 yg/L) is used.

: Life-cycle toxicity tests have been conducted with the. saltwater
mysid, Acanthomysis sculpta (Davidson et al. 1986a,1986b). The effects of TBT
on.survival, growth, and reproduction of A. sculpta were determined in five
separate tests lasting from 28 to 63 days. The tests separately examined
effects of TBT on survival (1 test), growth (3 tests) and reproduction (1
test) instead of the approach of examining all endpoints in one life-cycle
test. All tests began with newly released juveniles and lasted through
maturation and spawning, therefore, are treated as one life-cycle test. The
number of juveniles released per female at a TBT concentration of 0.19 yg/L
was 50% of the number released in the control treatment, whereas the number
released at 0.09 ywg/L was higher than in the control treatment. Reductions in
juveniles ‘released resulted from deaths of embryos within brood pouches of
individual females and not from reduced fecundity. Numbers of females
releasing viable juveniles was reduced in 0.19 and 0.33 ug/L. At
concentrations of 0.38 yg/L and above, survival and weight of female mysids
were reduced; all mysids in 0.48 ywg/L died. The chronic value is 90-1308 ug/L,
“and the acute-chronic ratio is 4.664 (Table 2).

The Final Acute-Chronic Ratio of 14.69 was calculated as the geometric
mean of the acute-chronic ratios of 36.60 for Daphnia magna, 10.01 for '
Pimephales promelas, 4.664 for Acanthomysis sculpta and 27.24 for Eurytemora
affinis. Division of the freshwater and saltwater Final Acute Values by 14.69

results in Final Chronic Values for freshwater of 0.0625 wog/L and for

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sac fry. Sci. Total. Environ. 103:229-243.
Dixon, D,.R.’ and H. Prosser. 1986. An investigation of ‘the genotoxic effects of
an organotin antifouling compound (bis(tributyltin) oxide) on the chromosomes

of the edible mussel, Mytilus edulis. Aquatic Toxicol. 8:185-195.

Douglas, M.T., D.O. Chanter, I.B. Pell and G.M. Burney. 1986. A proposal for
the reduction of animal numbers required for the acute toxicity of fish test

(Lcso determination). Aquat. Toxicol. 8:243-249.

\

Durchon, M. 1982. Experimental activation of the neuroendocrine mechanism
governing the morphogenesis of ‘the penis in the females of Ocenebra erinacea
(a dioecious prosobranch mollusc) by a marine pollutant (tributyltin). C.R.

Seances Acad. Sci. 295 (III) :627-630.

’ Dyrynda, E. 1992, Incidence of abnormal shell thickening in the pacific oyster
Crassostrea gigas in Poole Harbour (UK), subsequent to the 1987 TBT

restrictions. Mar. Pollut. Bull. 24:156-163.

EG&G: Bionomics. 1976. Acute toxicity of tri-n-butyltin oxide to channel
catfish (1ctalurus punctatus), the fresh water clam (Elliptic complanatus) ,
the common mummi hog (Fundulus heteroclitus) and the American oyster
‘(Crassostrea virginica) . Final Report to M&T Chemical Co., Rahway, NJ. EPA

87



observed that 0.157 yg/L reduced growth of mussels after 56 days exposure in
the laboratory; a concentration within ess than a factor of two of that
reducing growth in the field. Similarly, Salazar and ‘salazar (1987) observed
reduced growth of mussels exposed to 0.070 ug/L for 196 days in the
laboratory. The 66-day LC50 for 2.5 to 4.1 cm blue mussels ‘was 0.97 ug/L
(Valkirs et al. 1985,1987). Alzieu et al. (1980) ‘reported 30% mortality and
abnormal shell thickening among Pacific oyster larvae exposed to 0.2 pg/L for
113 days. Abnormal development was also observed in exposures of embryos for
24 hrs or less to TBT concentrations 20.8604 pg/L (Robert and His 1981).
Waldock and Thain (1983) observed reduced growth and thickening of the upper
shell valve of Pacific oyster spat exposed to 0.1460 pg/L for 56 days. Shell
thickening in Crassostrea gigas was associated with tissue concentrations of
20.2 mg/kg (Davies et al. 1988). Abnormal shell- development was observed in
an exposure to 0.77 yg/L that began with embryos of the eastern oyster,
Crassostrea virginica, and lasted for 48 hours (Roberts, 1987). ‘Adult eastern
oysters were also sensitive to TBT with reductions in condition index after
exposure for 57 days to >0.1 ug/L (Henderson 1986; Valkirs et al. 1985).
Salazar et al. (1987) found no effect. onTM growth after 56 days exposure to
0.157 pg/L to the oysters C. virginica, Ostrea edulis and 9. lurida..
Condition of adult ‘clams, Macoma 7 suta, and scallops, Hinmites multirugosus
were not affected after 110 days exposure to 0.204 ug/L (Salazar et al. 1987).
’ Long-term exposures have been conducted with a number of saltwater ;
crustacean species. Johansen and Mohlenberg (1987) exposed adult Acartia

tonsa’ for five. days to TBT and observed impaired.egg production on days 3, 4.

and 5 in 0.1 pg/L and only on day 5 ‘in 6.01 and 0.05 pg/L. For the five days,
overall egg production was reduced markedly (25%) only in 0.1 ug/L. Davidson
et al. (1986a,1986b), Laughlin et al. (1983, 1984b), and Salazar and Salazar
(1985a) reported that TBT acts slowly on crustaceans and that behavior might
be affected several days before mortality occurs. Survival of larval
amphipods, Gammarus oceanicus, was significantly reduced after eight weeks of

‘exposure to TBT concentrations 20.2816 ug/L (Laughlin et al. 1984b). Hall et

21



‘pis (tri-n-butyltin) oxide (TBTO): Histopathological and histochemical findings

in rainbow trout (Oncorhynchus mykiss). Aquat. Toxicol. 23:31-48.

Seiffer, E.A. and H.F. Schoof. 1967. Tests of 15 experimental molluscicides

against Australorbis glabratus. Public Health Rep. 82:833.-839.

; Seinen, W., T. Helder, H. Vernij, A. Penninks.and P. Leeuwangh..1981. Short
_tezm toxicity of tri-n-butyltin chloride in rainbow trout (Salmo gairdneri
Richardson) yolk sac fry. Sci. Total Environ. 19:155-166.

Seligman, P.F., J.G. Groohoug, A.O. Valkirs, P.M. Stang, R. Fransham, M.O.
Stelland, B. Davidson and R.F. Lee. 1989. Distribution and fate of tributyltin
in the United States marine environment. Appl. Organometallic Chem. 3:31-47.
Seligman, P.F:, A.O. Valkirs and R.F. Lee. 1986. Degradation of tributyltin in
San Diego Bay, CA waters. Draft Report. Naval Ocean Systems Center, San Diego,

CA. 7 pp.

Seligman, P.F., A.O. Valkirs, P.M. Stang and R.F. Lee. 1988. Evidence for

rapid degradation of ‘tributyltin in a marina. Mar. Pollut. Bull. 19:531-534.

Selwyn, M.J. 1976. Triorganotin compounds as ionophores and inhibitors of ion

translocating ATPases. In: Organotin Compounds: New Chemistry and

125


molluses rather than Final Acute Values and Acute-Chronic Ratios to derive the
Final Chronic Value. The Federal Insecticide, Fungicide, and Rodenticide Act
(FIFRA) data base of information from the pesticide industry was searched and
: some useful information was located for deriving the criteria. The latest .
comprehensive literature search for information for this document was :

conducted in January 1997 ‘for fresh- and saltwater organisms.

ute Toxicity to Aquat. yn.ima:

_Data that may be used, according to the Guidelines, in the derivation
of Final Acute Values for TBT are presented in Table 1. Acute values are
available for thirteen freshwater species representing twelve genera. The
acute yalues range from 1.14 pg/L for a. hydra, Hydra oligactis, to 24,600 pg/L
for a freshwater calm, Elliptio complanatus. The relatively low sensitivity
of the freshwater clam to TBT is surprising due to the mollusicidal qualities
of TBT. The organism likely closes itself to the environment, minimizing
chemical intake, and is able to tolerate high concentrations of TBT
temporarily. :

: The most sensitive freshwater organisms tested are hydras (Table 3).
Three species were tested and have Species Mean Acute Values (SMAVs) ranging
from 1.14 to 1.80 pg/L. Other invertebrate species tested are an amphipod, a
cladoceran, an annelid and a dipteran larvae. ‘Brooke et al. (1986) conducted
flow-through measured tests with an amphipod, Gammarus pseudolim inaeus, and an

annelid, Lumbriculus variegatus, and a static measured test with larvae of a

. mosquito, Culex sp. The 96-hr LC50s and SMAVs are 3.7, 5.4 and 10.2 ug/L,
respectively. Six tests with the daphnid, Daphnia magna, were conducted. The
48-hr EC5O value of 66.3 wg/L (Foster 1981) was considerably less sensitive
than those from the other tests which ranged from 1.58 ug/L (LeBlanc 1976) to
18 yg/L (Crisinel et al. 1994). ‘The SMAV for D. ‘magna is 4.3 yg/L because,
according to the Guidelines, when test results are available from flow-through °
and concentratign measured tests, these have. precedence over other types of
acute tests. :

All the vertebrate species tested are fish. The most sensitive species

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Salazar, M.H. and M.A. Champ. 1988. Tributyltin and water quality: A question

of environmental significance. In: Oceans 88, Vol. 4. Proceedings
International Organotin Symposium. Marine Technology Society, Washington, Dc.

10 pp.

Salazar, S.M., B.M. Davidson, M.H. Salazar, P.M. Stang and K.J. Meyers-
Schulte. 1987. Effects of tributyltin on marine organisms: Field assessment of
a new site-specific bioassay system. In: Oceans 87, Vol 4. Proceedings
International Organotin Symposium. Marine Technology Society, Washinton, pe.

pp: 1461-1470.

Salazar, M.H. and S.M. Salazar. 1985a. The effects of sediment on the survival
of mysids exposed to organotins. Proc. 11th U.S./Japan Experts meeting,
Management of bottom sediments containing toxic substances. 4-6 November,

1985, Seattle, Washington. T.P. Patin, (Ed.).

Salazar, M.H. and S.M. Salazar. 1985b. Ecological evaluation of organotin-
contaminated sediment. NOSC-TR-1050 or AD-A160-748-0. National Technical

Information Service, Springfield, VA. 22 pp.

Salazar, M.H. and S.M. Salazar. 1987. Tributyltin effects on juvenile mussel
growth. In: Oceans 87, Vol. 4. Proceedings International Organotin Symposium.
Marine Technology Society, Washington, DC. pp. 1504-1510.

122



Mercenaria mercenaria. Bull. Environ. Contam. Toxicol. 42:352-358.

Laughlin, R.B., Jz., R.B. Johannesen, W. French, H. Guard and F.E. Brinckman.

1985. Structure-activity relationships for organotin compounds. Environ.

Toxicol. Chem. 4:343-351.

Laughlin, R. and 0. Linden. 1982. Sublethal responses of the tadpole of the
European frog, Rana temporaria, , to two tributyltin compounds. Bull. Environ.

Contam. Toxicol. 28:494-499.

Laughlin, R.B., dr. and 0. Linden. 1985. Fate and effects of organotin

compounds. Ambio 14:88-94.

Laughlin, R.B., dr., 0. Linden and H.E. Guard. 1982. Acute toxicity of
tributyltins and tributyltin leachates from marine antibiofouling paints.

Bull. Liaison Comite Int. Perm. Recher. Reser. Mater. Milieu Marin 13:3-26.

Laughlin, R.B., ar., K. Nordlund and 0. Linden. 1984b. Long-term effects of
tributyltin compounds on the Baltic amphipod, Gammarus eceanicus. Mar.

Environ. Res. 12:243-271.

Laughlin, R.B., Sx., P. Pendoley and R.G. Gustafson. 1987. Sublethal effects
of tributyltin on the hard shell clam, Mercenaria mercenaria. In: Oceans 87,

106



Lenihan,. .S., J.S. Oliver and M.A. Stephenson. 1990, Changes in hard bottom
communities related to boat niooring and tributyltin in San Diego Bay: a

natural experiment. Mar. Ecol. Prog. Ser. 60:147-159.

Levine, S.N., D.T. Rudnick, J.R. Kelly, R.D. Morton and L.A. Buttel. 1990.
Pollutant dynamics as influenced by seagrass beds: Experiments with

tributyltin in Thalassia microcosms. Mar. Environ. Res. 30:297-322.

Lewis, J.W., A.N. Kay and N.S. Hanna. 1995. Responses of electric fish (family
mormyridae) in inorganic nutrients and tributyltin oxide. Chemosphere.

31:3753-3769.

Lindblad, C., U. Kauatsky, C. Andre, N. Kautsky and M. Tedengren. 1989.
Functional response of Fucus vesiculosus communities to tributyltin measured

in an in situ continuous flow-through system. Hydrobiologia 188/189 1277-283.

Linden, E., B. Bengtsson, 0. Svanberg and G. Sundstrom. "1979. The acute
toxicity of 78 chemicals and pesticide formulations against ‘two brackish water

organisms, the bleak (Alburnus alburnus) and the harpacticoid Nitocra

gpinipes. Chemosphere 8:843-851.

108





locks, as indicated by degree of imposex in the dog-whelk, Nucella lapil lus

(L). Mar. Pollut. Bull. 18:400-404.

Davies, I.M., 3. Drinkwater and J.C. McKie..1988. Effects of tributyltin
compounds from antifoulants on Pacific oysters (Crassostrea gigas) in Scottish

sea lochs. Aquaculture 74:319-330.

Davies, I.M. and J.C. McKie. 1987. Accumulation of total tin and tributyltin

in.muscle tissue of formed Atlantic salmon. Mar. Pollut. Bull. 18:405-407.

de la Court, F.H. 1980. The value of tributyltin fluoride as a toxicant in

antifouling formulations. J. Col. Chem. Assoc. 63:465-473.

Delupis, G.D.D., P.M.B. Gucci and L. Volterra. 1987. Toxic effects of bis-

tributyltinoxide on phytoplancton. Main Group Met. Chem. 10:77-82.

Delupis, ‘“G.D.D. and R. Miniero. 1989. Preliminary studies on the TBTO effects

on fresh water biotic communities. Riv. Idrobiol. 28:1-2.

Deschiens, R. 1968. Control of infectious microorganisms with chemical

molluscicides. C.R. Hebd. Seances Acad. Sci. 266D:1860-1861.

Deschiens, R., H. Brottes and L. Mvogo. 1966a. Field application in Cameroon

85°



adverse effects might be expected on important species. The above data
demonstrate that the reductions in growth occur in commercially or
ecologically important saltwater species at concentrations of TBT less than
the Pinal Chronic Value of 0.0500 ug/L derived using Final Acute Values and
Acute-Chronic Ratios from Table 3. Therefore, EPA believes the Final Chronic
Value should be lowered to 0.01 pg/L'to limit unacceptable impacts on Acartia
tonsa, Mercenaria mercena: ja, Crassostrea gigas and Ostrea edulis observed at
0.02 wg/L. At this criteria concentration, imposex would be expected in
Zlyanassa obsoleta, Nucella lapillus and similarly sensitive neogastropods; —
populations of N. lapillus and similarly sensitive snails with direct
development might be impacted and growth of Mercenaria mercenaria might be
somewhat lowered.
Unused Data

Some data concerning the effects of TBT on aquatic organisms were not
used because the tests were conducted with species that are not resident in
North America (e.g., Ali et al. 1990; Allen et al. 1980; Axiak et al. 1995b;
Batley et al. 1989,1992; Burridge et al. 1995; Camey and Paulini 1964;
Danil'chenko 1982; Deschiens and Floch 1968; Deschiens et al.
1964,1966a,1966b; de Sousa and Paulini 1970; Fent 1991, 1992; Fent and Hunn
1993; Fent and Meier 1992; Frick and DeJimenez 1964; Girard et al. 1996;
Harding et al. 1995; Helmstetter and Alden 1995; Hopf and Muller 1962;
Jantataeme 1991; Karande and Ganti 1994; Karande et al. 1993; Kubo et al.
1984; Langston and Burt 1991; Lewis et al. 1995; Nagabhushanam et al. 1991;
Nagase et al. 1991; Nias et al. 1993; Nishuichi and Yoshida 1972; Oehlmann et
al. 1996; Reddy et al. 1992; Ringwood 1992; Ritchie et al. 1964; Ruiz et al.
1994a, 1994b, 1995a, 1995b, 1995¢; Sarojini et al. 1991, 1992; Scadding 1990;
Scammell et al. 1991; Seiffer and Schoof 1967; Shiff et al. 1975; Shimizu and
Kimura 1992; Smith et al. 1979; Spence et al. 1990b; Stebbing et al. 1990; —
Sujatha et al. 1996; Tsuda et al. 1986, i991a; Upatham 1975; Upatham et al.

1980a,1980b; Vitturi et al. 1992; Webbe and Sturrock 1964; Yamada et al. 1994;

26



166.

Quick, T. and N.E.. Cardarelli. 1977. Environmental impact of controlled
_ release molluscicides and their degradation products: a preliminary report.
In: Controlled release pesticides. Scher, H.B. (Ed.). ACS Symposium Series No.

53. American Chemical Society, Washington, DC. pp. 90-104.

Reader, S., R.S. Louis, E. Pelletier and F. Denizeau. 1996. Accumulation and
biotransformation of tri-n-butyltin by isolated rainbow trout hepatocytes.

Environ. Toxicol. Chem. 15:2049-2052.

Reader, S. and E. Pellitier. 1992. Bioabsorption and degradation of butyltin
compounds by the marine diatom Sksletonene Sostabum and the associated
bacterial community at low temperatures. Bull. Environ. Contam. Toxicol.

48:599-607.

Reader, s., H.B.. Steen and F. Denizeau. 1994. Intracellular calcium and pH

alterations induced by tri-n-butyltin chloride in isolated rainbow trout

hepatocytes: a flow cytometric analysis. Arch. Biochem. Biophys. 312:407-413.
- 4 .

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92



reported by Rhea et al. (1995), Salazar and Salazar (Manuscript) and Valkirs
et al. (1985). Some data were not used because of problems. with the.
concentration of the test material (e.g., Springborn Bionomics 1984b;
Stephenson et al. 1986; Ward et al. 1981) or low survival in the éxposure
organisms (Chagot et al. “1990; Fent and Looser 1995). BCFs were not used when
the concentration of TBT in the test. solution was not measured (Laughlin et
al. 1986b; Paul and Davies 1986) or were highly variable (Becker et al. 1992;
Laughlin and French 1988). Reports of the concentrations in wild aquatic
animals were not used if concentrations in water were unavailable or '
excessively variable (e.g., Curtis and Barse 1990; Davies et al. 1987, 1988;
Davies and leKie 1987; Gibbs et al. 1991b; Hall 1988; Han and Weber 1988;
Kannan et al. 1996; Oehlmann et al. 1991; stab et al. 1995; Thrower and Short :

1991; .Wade et al. 1988).

Summar: . . oO

/ The acute toxicity values: for thirteen freshwater animal species range
from 1.14 pg/L for a hydra (Hydra oligactis) to 24,600 wg/L for a clam
(ELliptio complanatus). There was no apparent trend in sensitivities with
taxonomy; fish were nearly as sensitive as the most ‘sensitive invertebrates
and more sensitive than others. When the much less sensitive clam was not’

. considered, the remaining species sensitivities varied by a maximum of 11.2
times. Three chronic toxicity tests have been conducted with freshwater
animals. Reproduction of Daphnia magna was reduced by 0. 2: “pg/L, but not ‘by
0.1 pg/L, and the Acute-Chronic Ratio:is 30.41. In another test with D. magna
reproduction and survival was reduced at 0.34 wg/L but not at 0.19, and the
Acute-Chronic Ratio is 44.06. Weight of fathead minnows was reduced by 0.45
pg/L, but not by 0.15 ywg/L, and the acute-chronic ratio for this species was
10.01. ° Bioconcentration of TBT was measured in zebra mussels, Dressena
polymorpha, at 180,427 times the water concentration for the soft parts and in
rainbow trout, Oncorhynchus mykiss, at 406 times the water concentration for

the whole body. Growth of thirteen species of freshwater algae was inhibited

29