ABSTRACT Sea urchins (Strongylocentrotus purpuratus and Strong- ylocentrotus franciscanus) in the vicinity of the Los An¬ geles County sewer outfall at White's Point have abnormal spination (stunted and missing primary spines). There are very high DDT residue levels (mainly DDE) in the tissues of these animals compared with normal appearing animals found at Pigeon Point, San Mateo County. Calcification rates in regenerating spines of S. purpuratus from White's Point were one-half the rates of regenerating spines of S. purpuratus from Pigeon Point. DDT in concentrations above 1 ug/ml appears to supress calcification in regen- erating spines of S. purpuratus from Pigeon Point while no suppression of calcium uptake occurred in regenerat¬ ing spines of S. purpuratus from White's Point exposed to DDT concentrations up to 10 pg/ml. Accumulated pesti¬ cide residues contained in the spines of the White's Point urchins apparently suppresses calcification and may be a major cause of their stunted, abnormal appearing spina- tion. 35 INTRODUCTION Pearse, et.al.(1970) noted that sea urchins (both Strongylocentrotus purpuratus and Strongylocentrotus fran¬ ciscanus) in the White's Point area of Palos Verdes Pen- insula, Southern California, were without many of their major spines, suggesting an unhealthy condition. Moreover, the proportion of unhealthy sea urchins in the area appears to have increased between September 1970 and May 1971 (J.S. Pearse, personal communication). The cause of the unhealthy condition is unknown, but high levels of DDT residues in the area suggests a possible cause. Burnett (1971) found extremely high levels of DDT residues in the sand crab, Emerita analoga, only a few miles from White's Point (10 ppm in the whole animal). Swarbrick (1971) analyzed specimens of Pagurus samuelis collected at White's Point and found DDT residue levels 4 times greater than levels found in the Monterey Bay or San Francisco Bay areas. Marian (1971) also found DDT residue levels in Hermissenda crassicornis that were much higher than those found in the Monterey Bay area. Carry and Redner (1970) reported that the Los Angeles County sewer outfall located at White's Point (dispersion is - 1 - actually 1500 to 3600 meters offshore) discharged an aver¬ age of 1.44 million cubic meters (380 million gallons) of primary treated sewage per day with an average concentra¬ tion of 34 ppb of chlorinated hydrocarbons (105 lbs. per day) almost all of which were DDT metabolites. Therefore, there may be a correlation between high DDT residue con¬ centrations in the area, and the abnormal spination of sea urchins from White's Point; this is examined in the present paper by studying calcification rates of spines of S. purpuratus and S. franciscanus regenerating in vitro. Heatfield (1970) studied calcification of regenerat- ing spines of S. purpuratus using calcium-45 as a radio¬ active tracer. He examined the effects of time, tempera¬ ture, and inhibition of carbonic anhydrase on calcium up¬ take in regenerating spines. Heatfield's system was very sensitive to calcium metabolism and therefore provides a convenient method for examining the possible effect of DDT on calcification. MATERIALS AND METHODS Specimens: Specimens were collected at both White's Point on 16 May 1971, and Pigeon Point on 22 April 1971 (Fig. 1). Only specimens that appeared to be distinctly unhealthy, including both S. purpuratus and S. franciscanus, were collected at White's Point from 1 to 3 meters of water. Pigeon Point urchins (S. purpuratus only) were collected - 2 - 39 from the intertidal region; all were very healthy in ap- pearance. The urchins were maintained at Hopkins Marine Station in running sea-water kept at 15 C I I C and fed unlimited amounts of the brown algae, Macrocystis integ- rifolia. Measured Pesticide Residue Levels: Pesticide residue levels in tissues of S. purpuratus were measured by gas chromatography using the techniques developed by Stanley and LeFavoure (1965) and Kadoum (1967) except that smaller amounts of tissues were used (0.5 to 2.5 grams versus about 100 grams) and the digest medium used for the spine extraction was 12N HCl. The gonads, spines, lantern structure, and coelomic fluid of 3 Pigeon Point urchins and the spines and gonads of 2 White's Point urchins and the gonads of an additional animal were ana- lyzed for DDT residues. Only very unhealthy appearing spec¬ imens from White's Point were analyzed, while the speci¬ mens from Pigeon Point appeared normal. Measurement of DDT Effects on Calcification: Heatfield (1970) found no difference in calcium up¬ take rates of spines regenerating in vitro and in vivo; linear rates of calcium uptake were established in 4 days. Accordingly, spines analyzed for DDT effects on calcium¬ 45 uptake were allowed to regenerate in vivo for 4 days before being exposed to test conditions in vitro. The spines from healthy urchins (Pigeon Point) were all taken from the 2 major rows of primary spines of each of 5 in¬ terambulacral plates to minimize effects due to size differences. This was not possible for animals collected at White's Point because the extremely unhealthy specimems chosen had few spines and it was difficult to get just the 25 spines necessary for the experiment. All individual experiments were done with spines from the same animal. The spines (about 40 per animal) were fractured 3 mm above the milled rings as specified by Heatfield (1970) and allowed to regenerate for 4 days still attached to the animal. After 4 days the stubs were removed intact and gently placed in 4 250 ml beakers (about 10 spines per beaker) containing 1 uci/ml calcium-45 (Amer¬ sham/Searle - 71.4 mCi/milli-mole) in 20 ml of artificial sea-water maintained at 15 C I 1 C. Additional amounts of ethanol (0.02, 0.1, and 0.2 ml) of different concentrations of DDT (0.1 mg/ml and 1.0 mg/ml) were added to test sol¬ utions. After 24 hours the stubs were removed from the solutions and assayed for calcium-45 uptake as described by Heatfield (1970) Ethanol Controls: Since ethanol was being added to test solutions, it was essential to isolate any effects due to ethanol. Therefore, controls with varying amounts of ethanol were analyzed for effects on calcium uptake. Concentrations of ethanol up to 0.91% in sea-water had no effect on the rate of calcification (Fig. 2). Salk (1969) found a similar break at 0.95% ethanol in sea-water in his calcification experiments with S. purpuratus larvae. Therefore, in all calcification experiments on regenerating sea urchin spines, the total percentage of ethanol in sea-water was less than or equal to 0.91%. Carbon-14 DDT Uptake: In vivo DDT uptake was measured by adding 0.2 ml of 1 ug/mlC-DDT (Amersham/Searle - 19.1 mCi/milli-mole) in 95% ethanol to 2 liters of filtered sea-water in which 4 specimens of S. purpuratus form Pigeon Point were placed. These animals all weighed approximately 30 grams. At time intervals one spine (that had not been fractured) was re¬ moved from each urchin, weighed, and placed in a plastic scintilaation vial with 1 ml of NCS Solubilizer (Amersham/ Searle). After 5 minutes in NCS, 10 ml of scintillation fluid (4 grams 2,5-di-phenyloxazole (PPO) and 0.1 gram 1,4-bis- 2-(5-phenyloxazole) benzene (POPOP) per liter toluene) was added. Counts were quantified by the channel ratio technique with corrections made for quenching (nu¬ clear Chicago Liquid Scintillation Counter Mark II). For in vitro uptake measurements, spines first frac- tured as previously described and then allowed to regen¬ erate for 6 days on the urchin were then removed and placed in 250 ml beakers containing 20 ml of filtered sea-water with 0.1 ml of 1 ppm C-DDT in ethanol added. (15 stubs from 3 S. purpuratus collected at Pigeon Point were placed in 3 beakers.) The concentration of C-DDT in the in vitro experiments (5,000 ppg/ml) was 50 times higher than that in the in vivo experiment (100 pug/ml). Assay for C was done in the same way as for the in vivo experiment. - 5 RESULTS Measured Pesticide Residue Levels: In the 3 specimens collected at Pigeon Point and analyzed for pesticide residues, only the gonads showed a trace of DDE, between 0.5 and lng/g (ppb), near the detection limit of the gas chromatograph. No detectable amounts of DDE, DDD, or DDT were found in the spines, lantern structure, or coelomic fluid. In contrast to the specimens collected at Pigeon Point, 3 animals collected at White's Point, that were maintained at Hopkins Marine Station for 2 weeks and then analyzed, had measurable amounts of DDT residue (mainly DDE) in their tissues (Fig. 3). The DDT residue levels in the spines of 2 animals were about twice the levels found in their gonads. The spines of the third specimen were not analyzed but it is likely that they also had a higher content of DDT residues than the gonads, which would mean their content would be well over the 420 ppb found in the gonads. -DDT Uptake Rates: Uptake studies showed a striking difference between spines incubated in vivo and in vitro (Fig. 4). While spines incubated in vitro (regenerating) took up DDT with increasing time, spines still attached to urchins (not regenerating) lost their initial content of DDT until they equilibrized after 1 hour to approximately a constant level. Spines incubated in vitro for 48 hours at 5 ng DDT/ml C showed a comparable DDT content to the levels found in White's Point urchins (see Fig. 3). DDT Effect on Calcification: There was no effect on Ca uptake by DDT on the spines of animals from Pigeon Point tested at concentra¬ tions of DDT up to 1 ug/ml. However, when the concentra¬ tion was raised above the saturation concentration of 1.2 ug/ml (Salk, 1969), there was a striking decrease (32% at 10 ug DDT/ml) in calcium absorbed between spines exposed to DDT and controls not exposed to DDT (Fig. 5). DDT, even at concentrations of 10 jg/ml, had no ef- fect on calcium uptake in spines of the White's Point S. purpuratus (6A - Fig. 6). However, the amount of Ca taken up by this specimen, even without DDT in the incu¬ bation medium, was relatively low in comparison to amounts of Ca taken up by the spines of urchins from Pigeon Point (see Fig. 5). Indeed, amounts of Ca taken up by spines of the spines of the White's Point animal incubated without DDT was most similar to that amount of Ca taken up by spines of the Pigeon Point animal incubated in 10 ng DDT/ml (Fig. 7). The uptake of Ca45 in regenerating spines of a 10 gram animal from White's Point was also measured without exposure to DDT; the value of Cat ab- sorbed was 9.6 ng f 1 ng (compared to 16.24 for the 30 gram specimen shown in Table 1 and Figs. 6A and 7). - 7 - DISCUSSION C1DDT Uptake by Spines: The results of the uptake study (see Fig. 4) show that spines regenerating in vitro do take up DDT at con- centrations of 5 ng DDT/ml and hence probably do so at the higher concentrations used during the calcification experiments. The in vivo curve of non-regenerating spines is interesting in that it shows that DDT taken up in the first 5 minutes, probably by adsorption, is somehow lost until equilibrium is reached after about 1 hour. The fate of the lost DDT is unknown. Perhaps the DDT is translocat¬ ed into the urchin until it reaches equilibrium. Another possible explanation is mucous secretion of the spines and subsequent loss of mucus containing high concentra¬ tions of DDT. DDT Effect on Calcification: The high levels of pesticide residues found in the White's Point specimens are in accordance with the high pesticide residue concentrations in the water and sedi¬ ments around the sewer outfall (Carry and Redner, 1970) Moreover, because the spines are almost 99% inert calcium carbonate by weight, the actual DDT content per weight of organic tissue is much higher than indicated in Figs. 3 and 4. Marian (1971), Burnett (1971), and Swarbrick (1971) also found very high DDT residue concentrations in other animals in the White's Point area. However, whether these high levels of DDT residues are responsi¬ - 8 - 3 ble for the unhealthy appearance of the urchins at White's Point is not certain. Statistical analysis (Table 1) shows that calcifica¬ tion in only 1 animal (50) from Pigeon Point was suppressed by DDT and suppression occurred at concentrations above jg DDT/ml. In contrast, the S. purpuratus (6A) from White's Point showed no suppression at the same concen¬ trations of DDT in sea-water (1,5,10 ug DDT/ml). However, as Figure 7 shows, calcium uptake in the regenerating spines of the White's Point specimen (6A), incubated with¬ out DDT, was similar to the suppressed calcium uptake by the spines of the Pigeon Point animal (5C). A possible explanation is the size difference between the stunted primary spines of the White's Point in comparison to the normal spines of the Pigeon Point urchin. However, the uptake of calcium by the S. franciscanus (6B) specimen collected at White's Point, which had spines at least twice the size of normal spines of S. purpuratus, was not significantly different from amounts of calcium taken up by spines of the S. purpuratus collected at White's Point (6A). This suggests that size difference is not the major cause of the different amounts of calcium taken up by spines incubated without DDT from Pigeon Point and White's Point. It seems more probable,he that the high levels of DDT residues present in the spines of the White's Point urchins (see Fig. 3) inhibit normal calcium uptake and mask the effect of additional amounts of DDT added to the water. Heatfield (1970) found that complete inhibition of carbonic anhydrase, an important enzyme involved in cal¬ cium metabolism, only resulted in a partial suppression of calcium uptake in regenerating spines of S. purpuratus. Past studies of the effect of DDT and its metabolites on calcification, specifically on the enzyme carbonic anhy¬ drase, have been conflicting. Peakall (1970) and Bitman et.al.(1970) noted that DDT induced inhibition of carbon- ic anhydrase in the shell glands of birds. Keller (1952) observed inhibition of carbonic anhydrase extracted from bovine red blood cells and Nance (1969) found DDT inhibit¬ ed carbonic cnhydrase purified from Mytilus californianus and Tequla funebralis as well as bovine red blood cells. However, Anderson and March (1956) found no inhibition by DDT of carbonic anhydrase extracted from cockroaches, and recnetly Maren, et.al.(1971) retested the effects of DDT on carbonic anhydrase taken from bovine red blood cells and found no effect in concentrations less than 500 mg DDT/ml. Maren did observe a partial suppression of calcium uptake, however, at concentrations above 500 mg DDT/ml where DDT was found to precipitate out of solution. Precipitation of DDT from sea-water was also noted to take place in experiments done in concentrations above 1 ug DDT/ml (5C and 6A). The partial effect (32% in Pigeon Point urchins and 50% between controls of speci¬ mens 50 and 6A could then possibly be due to a carbonic anhydrase-independent element of the calcification mechanism. - 10 2 DDT is toxic because of its tendency to accumulate in tissues and hence cause an effect over a longer period of time. This long range effect is probably responsible for the lower calcification rates of regenerating spines of the White's Point urchin. Longer time studies of the effect of pesticide residues should be done - and ideally on more animals than analyzed here. Trace metal effects should also be studied. Cadmium especially has been known to effect calcium metabolism (Nilsson, 1970) and should be examined in the animals at White's Point. In conclusion, it is not certain whether DDT is the major cause of the abnormal spination of the sea urchins at White's Point; however it probably is at least partly responsible because there are high DDT residue concen¬ trations in the spine tissues, and high DDT concentrations do seem to inhibit calcification rates. SUMMARY . 1. Sea urchins found at White's Point, Los Angeles County, were missing many of their major spines and appeared to be in an unhealthy condition. Very high levels of DDT residues (mainly DDE) were found in animals collect¬ ed around the White's Point area, especially in the spines which had more than 200 ppb. In contrast, DDT residues were barely detectable in healthy appearing animals from Pigeon Point, San Mateo County. 2. Uptake studies using C-DDT showed that non-regener¬ ating spines incubated in vivo tended to lose initially absorbed levels of DDT and equilibrate at about O.5 ppb after 1 hour. Regenerating spines incubated in vitro showed the opposite trend, concentrating DDT with time; levels of 419 ppb were reached in 48 hours, Calcium uptake by regenerating spines in vitro from animals collected at Pigeon Point was not affected significantly by DDT concentrations less than 1 g/ml but was affected by concentrations greater than 1 ug/ml, when the drug precipitated from the sea-water. 4. Calcium uptake rates by spines of one specimen of S. purpuratus collected at White's Point was lower than that in the specimens collected at Pigeon Point and, although they were not affected by external DDT con¬ centrations up to 10 g/ml, levels already present in the spines may have suppressed calcification. 5. It is suggested that the stunted spination of the sea - 12 - urchins of White's Point, may be due, in part, to high DDT residue levels in their spine tissues. 13 - 40 ACKNON LEDGEMENTS This work was done as undergraduate research in Biology 175H at Hopkins Marine Station of Stanford Uni¬ versity. I would like to thank the entire staff and grad¬ uate students of Hopkins Marine Station for all the under- standing and help they gave so generously. Especially I would like to thank Dr. John S. Pearse for his help in collecting specimens at White's Point, designing exper¬ ments, and for critically reading this manuscript. I would also like to thank Dr. Vicki B. Pearse for her help in using the Automatic Scintillation Counter, Phillip R. Murphy for his help with preparing necessary equipment, and Robin Burnett for his invaluable background study of the White's Point area. - 14 - REFERENCES CITED ANDERSON, A.D. AND MARCH, R.B., 1956, Inhibitors of Car¬ bonic Anhydrase in the American Cockroach, Periplaneta americana, Canad. J. Zool., 34:68-74. BITMAN, J., CECIL, H.C., AND FRIES, G.F., 1970, DDT-Induc¬ ed Inhibition of Avian Shell Gland Carbonic Anhydrase: A Mechanism for Thin Eggshells, Science, 168:594-596. BURNETT, R., 1971, DDT Residues: Their Distribution Along Coastal California, submitted to Science. CARRY, C.W. AND REDNER, J.A., 1970, Pesticides and Heavy Metals, Progress Report, December 1970, County Sani¬ tation District of Los Angeles County, 51 pp. HEATFIELD, B.M., 1970, Calcification in Echinoderms: ef¬ fects of temperature and diamox on incorporation of calcium-45 in in vitro regenerating spines of Strong- ylocentrotus purpuratus, Biol. Bull., 139:151-163. KADOUM, A.M., 1967, A Rapid Micromethod of Sample Cleanup for the Gas Chromatograph Analysis of Pesticidal Res¬ idues in Plant, Animal, Soil, Surface and Ground Water Extracts, Bull. Environ. Contam. Toxicol., 2:264-267. MAREN, T.H., DVORCHIK, B.H. AND ISTEN, M., 1971, Does DDT Inhibit Carbonic Anhydrase?, Science, 172:728-729. MARIAN, R., 1971, Assimilation and Transfer of DDT Res¬ idues in a Hydroid:Nudibranch:Tectibranch Food Chain from the California Coast, (unpublished MS. on file at Hopkins Marine Station Library). NANCE, P., 1969, Inhibition of Carbonic Anhydrase by DDT and DDE, (unpublished MS. on file at Hopkins Marine Station Library), pp. 241-250. NILSSON, R., 1970, Aspects on the Toxicity of Cadmium and its Compounds, Swedish Natural Science Research Council, Ecological Research Committee Bulletin No. 7, 48 pp. PEAKALL, D.B., 1970, p-p'-DDT: Effect on Calcium Metabol¬ ism and Concentration of Estradiol in the Blood, Science, 168:592-594. PEARSE, J.S., CLARK, M.E., LEIGHTON, D.L., MITCHELL, C.T., AND NORTH, W.J?, 1970, Marine Waste Disposal and Sea Urchin Ecology IN: Kelp Habitat Improvement Project, Ann. Rept., 1 July 1969 - 30 June 1970, Appendix, pp. 1-93, Calif. Inst. Tech., Pasadena, Calif. 4 SALK, D., 1969 Methods for Assessing the Effects of DDT on Larval Skeletal Development in the Sea Urchin, strongylocentrotus purpuratus, (unpublished MS. on file at Hopkins Marine Station Library), pp. 291-310. STANLEY, R.F. AND LEFAVOURE, H.T., Rapid Digestion and Cleanup of Animal Tissues for Pesticide residue anal¬ ysis, J. Assoc. Offic. Agr. Chem., 48:666-667. SWARBRICK, S., 1971, DDT Residues in the Marine Intertidal Hermit Crab Pagurus samuelis (Crustacea:Decapoda) in California Waters, (unpublished MS. on file at Hopkins Marine Station Library). 40 0 o 0 1+ 1+ 1+ 0 0 9 8 6 6 1+ 16 5 1+ i 0 O 8 11 — 10. 1 H 1 t 3 5 4 H + 82 22 3H 1 AH 0 - c9 0 O H 9 0 1+ 1+ O A 14 LEGEND OF FIGURES 1. Map of California showing collection sites of Pigeon Point and White's Point. 2. Effect of ethanol of Calcium-45 uptake by regenerating spines of Strongylocentrotus purpuratus;the means and standard deviations are shown. 3. Measured DDT residue levels found in Strongylocentrotus purpuratus collected at White's Point. T-DDT, D-DDD. E-DDE, 4. Carbon-14 DDT uptake rates by spines of Strongylocen¬ trotus purpuratus in vivo (not regenerating) and in vitro (regenerating). 5. Effect of DDT on Calcium-45 uptake by in vitro regen¬ erating spines of 3 specimens of Strongylocentrotus purpuratus (A,B,C) collected at Pigeon Point; the means and standard deviations are shown. 6. Effect of DDT on Calcium-45 uptake of in vitro regen¬ erating spines of Strongylocentrotus purpuratus (A) and Strongylocentrotus franciscanus (B) collected at White's Point; the means and standard deviations are shown. Comparison of Calcium-45 uptake of in vitro regener¬ ating spines of Strongylocentrotus purpuratus from White's Point and Pigeon Point exposed to the same concentrations of DDT; the means and standard devia¬ tions are shown. 40. 25 130— kt CAPE MENDOCINO FRANCISCO PIGEON. POINT POINT /CONCEPTION DIEGO WHITE'S —.—— POINT FIGURE 1205 405 5 50 40 30 20 10 0.09 FIG. 2 91 % ETHANOL 2.25 4.5 9.1 40 5 450 300 250 200 150 100 50 FIG. 3 TDEEDT I TDEEDI SPECIMEN 1DE SPINES GONADS 41 i - - - o- S 2 ng DOIg -N 50 40 20 10 (A) 0 0.1 0,5 1.0 FIG. 5 COLLECTED AT PIGEON POINT 50 (B) 401 20 104 0 0.1 0,5 1.0 ug DDTm 50 40 30 20 10 (C) L 0 1 5 10 41 40 30 20 10 COLLECTED AT WHITES POINT S. PURPURATUS 40 (A) 304 20 ug DOTm FIG. 6 S. FRANCISCANUS (B) 0.1 0.5 1.0 474 50 40 301 20 10 FIG. 7 WHITE'S POINT (4A) PIGEON POINT (50) ug DOT/m 415