LEVLES AND SITES OF CONCENTRATION OF TRACE METALS IN INSHORE FISHES OF MONTEREY BAY ABSTRACT The sites of concentration of the trace metals cadmium, lead, silver, copper, chromium, manganese, and zinc were determined for five species of inshore marine fishes. Generally, zinc and lead accumulate in the gills; copper, cadmium, and zinc accumulate in liver; and silver, zinc, manganese, chromium, and cadmium concentrate in bone. Flesh dosen't noticeably concentrate any of these elements. Concentration levels with regard to trophic levels were also examined, and it was found that manganese in the liver, and zinc in flesh and bone decrease in concentration with increasing trophic level. Cadmium in the liver may show a direct relationship of concentration with higher trophic levels. 119 LEVELS AND SITES OF CONCENTRATION OF TRACE METALS IN INSHORE FISHES OF MONTEREY BAY By James Prickett Hopkins Marine Station of Stanford University 14 INTRODUCTION Most public attention and much of the research involving pollution has centered around the introduction of pesticides, especially DDT and its derivatives, into the environment. Only recently, with the government's release of mercury levels in swordfish, has public awareness focussed on another source of pollution, that of the trace metals. Using calculations of the total amount of an element mined each year as compared to the amount of that element added to the oceans each year, Bowen (1966) has classified the pollution potential of many of the trace metals. Silver (Ag), cadmium (Cd), chromium (Cr), copper (Cu), lead (Pb), and zinc (Zn) are all classified as having a very high potential of pollution. Manganese (Mn) is classified as having a high potential of pollution. The detrimental effects of many of the trace metals have been known for years. Silver is highly poisonous, and copper, which is used in large amounts in some areas as a fungicide, is also toxic. The toxicity of manganese is reported to be moderately high. Chromium, although it may be important in activating some enzymes, is suspected of being carcenogenic. Stock's study (1960) of zinc pol- luton in industrial smoke indicates that this metal may 4/4 induce lung disease (Bowen). Cadmium, which is used extensively by man in such varied items as automobile parts, laundry equipment, and dental fillings, has been responsible for many human deaths. In Japan alone, since 1962, fifty-six deaths have resulted from "Ouchi-Ouchi" disease, which is linked to cadmium- polluted rice in areas adjacent to mining operations. On a molecular level, cadmium binds to essential SH-groups to block the functioning of many enzyme systems (Nillson, 1970). Lead has long been known to be highly toxic, and yet in 1965 alone, about 6,000 tons of lead were introduced into the air of Los Angeles as a result of the use of tetraethyl lead in gasoline (Lead in the Environment and its Effects on Humans, 1967). Lead readily co-ordinates with organic ligands, and is generally toxic to enzyme systems (Brooks and Rumsby, 1965). Both lead and cadmium are cumulative poisons, so that exposure to low levels over an extended period can allow undesirable levels to accumulate (Bowen). In an effort to determine the extent to which these metals are accumulating in marine fishes, a study was made of the concentration of Ag, Cd. Cr. Cu, Mn, Pb, and Zn in inshore fishes of Monterey Bay. It was felt that the inshore water mass, due to its proximity to pollution sources, would tend to accumulate metal pollutants at higher levels ao than those found in open ocean, and give a clearer picture of what metals are involved as pollutants. The question of trace metal accumulation was approached from two points of view. First, for each fish studied, levels of the seven metals were measured in the flesh, liver, bone, and gills to determine the principle sites of concentration of each metal. Flesh was chosen because of its use in several of the species studied as food by man. The liver, because of its use as a filtering organ, and because of its many physiological roles, might be expected to act as an accumulation site. Bone was chosen since due to its mineral composition, it might offer a matrix suitable for the concentration of an entirely dif- ferent group of metals than those found in the other tissues. Finally, gills, because of their large surface area and use as an exchange organ, would be predicted to be another site of concentration. The second focus of attention involved trace metal behavior in food chains. Although the fishes used in this study do not lie necessarily in the same food chain, they do fall into general trophic levels. The fish studied were the top smelt, Atherinops affinis; shiner perch, Cymatogaster aggregata; starry flounder, Platichthys stellatus; striped bass, Roccus saxatilis; and the leopard shark, Triakis semifasciata. The food of these fishes are 444 found in Table 1, along with an indication of the approximate trophic level of each fish. MATERIALS AND METHODS The geographic location of this study is shown in Figure 1. Elkhorn Slough enters into the central portion of Monterey Bay. Although there is a small amount of fresh water entering the slough, generally the physical character- istics are those of an inshore marine environment (Rote, 1968). The Pajaro River enters into Monterey Bay about three miles north of Elkhorn Slough, and is a typical estuarine environ- ment, with salt water intrusion occuring up to two miles above the mouth of the river. The shiner perch (12-14 cm; all were females with young) and the leopard sharks (100 cm) were captured using gill nets at Kirby Park in Elkhorn Slough, shown as station 1 in Figure 1. The starry flounder (22-26 cm) were captured with a beach seinein the yacht harbor of the slough, shown as station 2. Finally, the top smelt (22-25 cm; all were females with young) and striped bass (24 cm) were taken using gill nets, about one mile up from the mouth of the Pajaro river at station 3. Tissues were either dissected on the day of capture, or the whole fish was frozen in a plastic bucket for later dissection. It should be noted that due to the small 14 size of the gills in some of these fishes, the whole gill basket, including bone, had to be used. Thus, gills can be said to accumulate a metal only when that metal's con- centration in the gills is greater than its concentration in the bone of the same fish. Samples were prepared for analysis using a modification of the wet digestion procedure of Middleton and Stuckey as described in Christion and Feldman (1970). Samples were dried at 90'C and powdered with mortar and pestle. one gram aliquot was dissolved in 5 ml of 90% HNO3 and refluxed at low temperature. HCl was used to dissolve any remaining calcareous particles. Two ml of 30% Ho09 were added and the sample was refluxed again before bringing to volume with distilled water. All samples were analyzed on a Perkin-Elmer Model 303 atomic absorption spectrophotometer using an air-acetylene flame. Standard conditions were followed for each element. For each set of tissues, the mean value was calculated, and all variation was reported in terms of one standard deviation. Those tissues for which N = 1 or N = 2 represent a composit value of five samples which were too small to be run individually. RESULTS AND DISCUSSION The concentrations found for each of the metals by 1/66 species are given in Tables 2A-20. Values determined by Ting (1967) for albacore and skipjack tunas are found in Table 3. Ting's values are given as a comparison, since his fish were pelagic and from a different region (Peru). His values generally compare closely with the values found by this study of inshore fishes, with the exception of manganese. The inshore fishes were often one order of magnitude higher for manganese than the tunas. This could possibly be due to manganese accumulation in the inshore waters, since manganese levels would be expected to be approximately equal if they were only involved with natural systems. Veith's study of trace metal introduction into Monterey Bay (1971) shows that manganese is one of the principle trace metals found in the sewage effluent. In addition, he found manganese to be the highest of the metals studied in sediments near the Monterey sewage outfall. Manganese concentrations in the two water bodies would have to be determined before any definite hypotheses could be made. The concentrations of each metal by tissue are plotted in Figure 2 - Figure 8. From these, it can be seen that certain tissues are accumulating much more of particular metals than others. Flesh is the site of lowest concentration for all of the metals. Lead and zinc concentrate in the 4/ gills at levels above those found in bone, so that the gill filaments themselves may be said to accumulate these metals. Ting's data also shows this trend. Manganese is possibly accumulating in the gills, but the values are too close to those of bone to make a definite statement. These observations are similar to those made in studies by Pringle, et. al. (1968) and Brooks, et. al. (1965), which indicate that the gills of bivalves, due to their mucous secretions, tend to be sites of concentration of Cutt, Zn, and Mnt. One theory for the toxicity of the trace metals upon fish attributes them with causing asphyxiation. When in high enough concentrations, the metals have been found to precipitate in the mucous layers of the gills, blocking respiratory transfers (Pringle, et. al.). The liver seems to be accumulating cadmium, zinc, and copper. The copper levels are especially interesting, since they range from two to twenty times the levels of copper in the other tissues. Among the catalytic trace elements, Bowen includes copper, manganese, and zinc. Thus, considering the many enzymatic functions of the liver, the relatively high levels of zinc and copper would be expected. Bone concentrates the largest number of the elements studied, including silver, zinc, manganese, chromium, and 44 cadmium. Chromium and silver especially are found in bone as opposed to the other tissues. Since much of bone is inorganic material, concentration of these generally non- enzymatic elements is not unusual. However, no definite explanation can be found for the high manganese and zinc levels. These, too, could be accumulating in the inorganic fractions of the bone, or they could be involved in some physiological functions of bone cells. No information could be found in the literature which could distinguish between these or other hypotheses. No general conclusions can be made concerning the behavior of trace metals as a class in regard to food chain magnification. As a whole, no single pattern emerged, with most of the elements in each tissue showing much scatter between different trophic levels. Hovever, a few patterns for specific elements in specific tissues are seen in Figure9- Figure 12. Manganese in the liver, and zinc in the flesh and bone all show decreasing concen- trations with increasing trophic levels. This is the same pattern ovserved in an experiment by Baptist and Lewis (1969) for both 2n65 and Cr5l in an artificial food chain of four levels. Although at first this inverse relationship might appear to be due to decreasing surface/volume ratios with increasing size, this does not explain the scattered behavior of most of the other elements with regard to trophic level. 2/0 A rather interesting behavior is observed for cadmium in the liver, shown in Figure 12. Of the twenty-eight metal-organ systems studied with regard to food chains, only cadmium showed any kind of direct relationship between trophic level and concentration. Although the uncertainty of Figure 12 is rather large, due to the high toxicity of cadmium in enzymatic reactions, and the essential physiological role of the liver, this trend of cadmium to accumulate at higher trophic levels deserves further study. Although some conclusions have been reached concerning the two questions set forth in this study, no definite statement can be made concerning the more important and general question: Is trace metal pollution occuring in these marine fishes? To draw such a conclusion, base- lines of natural concentrations must exist for comparison. Ting's study on tuna was used to partially fill this need, and indeed, as mentioned earlier, there is the possibility that manganese is acting as a pollutant. Perhaps cadmium and silver, since they have no known physiological functions are also occuring due to pollution. But no such conclusions can be made for the other four metals, and it is quite possible that all of the levels measured are simply natural levels. Hopefully, the data obtained in this study will be of use to other investigators as comparison values, so that some idea of natural levels 450 can be obtained. Knowing these, more conclusive measure- ments can be made of trace metal pollution of marine fishes. SUMMARY The sites of concentration of the trace metals cadmium, lead, silver, copper, chromium, manganese, and zinc were determined for five species of inshore marine fishes. Generally, zinc and lead accumulate in the gills; copper, cadmium, and zinc accumulate in liver; and silver, zinc, manganese, chromium and cadmium concentrate in bone. Flesh dosen't noticeably concentrate any of these elements. Concentration levels with regard to trophic levels were also examined, and it was found that manganese in the liver, and zinc in flesh and bone decrease in concentration with increasing trophic level. Cadmium in the liver may show a direct relationship of concentration with higher trophic levels. ACKNOWLEDGEMENTS This work was made possible by Grant GY-8950 of the Undergraduate Research Participation Program of the National Science Foundation. I would like to thank James Rote for his help throughout the project, and Dr. John Martin and George Knauer for their help with atomic absorption analysis. Also, I would like to thank Gary Kukowski of 45 Moss Landing Marine Lab for his aid in collecting materials for this study. REFERENCES Ackerman, L. T. 1970. Variations in food habits with length of leopard sharks in Elkhorn Slough. From an unpublished paper at Moss Landing Marine Lab. Baptist, J. P., and C. W. Lewis. 1969. Transfer of 65- Zn and 51- Cr through an estuarine food chain, p. 420- 430. In D. J. Nelson and F. C. Evans (eds.), Proc. 2nd. Natl. Symp. on Radioecology, Ann Arbor. Baxter, J. L. 1966. Inshore Fishes of Californea. State of Calif., The Resources Agency, Dept. of Fish and Game. 80 p. Trace elements in biochemistry. Bowen, H. J. M. 1966. Academic Press. 241 p. Brooks, R. R., and M. G. Rumsby. 1965. The biogeochemistry of trace element uptake by some New Zealand bivalves. Limnol. Oceanogr., 10: 521-537. Christian, G. D., and F. J. Feldman. 1970. Atomic Absorption Spectroscopy: Applications in Agriculture, Biology, and Medicine. John Wiley & Sons, New York, 490 p. Lead in the Environment and its Effects on Humans. Air Resources Board, Sacramento, Calif. 1967. Nilsson, R. 1970. Aspects on the toxicity of cadmium and its compounds. Swedish Natural Science Research Council, Ecological Research Committee Bull. No. 7. Pringle, B. H., D. E. Hissong, E. L. Katz, and S. T. Mulawka. 1968. Trace metal accumulation by estuarine mollusks. J. Sanit. Eng. Div., 94: 355-475. Rote, J. W., 1968. Ecological Studies of the Cirratulid Worm Cirriformia Spirabrancha at Elkhorn Slough. Paper submitted to Hopkins Marine Station, Pacific Grove, California, for Biol. 175h. 450 Ting, R. Y. 1967. Appendix A. p. A-1 - A-191. In F. G. Lowman, D. K. Phelps, R. Y. Ting. J. H. Martin. D. J. Swift, R. M. Escalera. Puerto Rico Nuclear Center Marine Biology Program Progress Summary Report No 5, 1967. Veith, R. 1971. Trace Metals in Monterey Peninsula Sewerage. Paper submitted to Hopkinc Marine Station, Pacific Grove, California, for Bio. 175h. 6 TABLE LEGEND Food and Trophic Levels of Five Species of Table 1. Inshore Fishes. Table 2A. Trace Metal Concentrations in ug/gram Dry Weight. Table 2B. Trace Metal Concentrations in ug/gram Dry Weight. Table 20. Trace Metal Concentrations in ug/gram Dry Weight. Table 3. Trace Metal Concentrations in ug/gram Dry Weight as reported by Ting, 1967. Table 4. Key to Figures. TASLE FOOD AND TROPHIC LEVELS OF FIVE SPECIES OF INSHORE FISHES Top Smelt: Small planktonic crustacea. 1 carnivore (Baxter, 1966). Shiner Perch: Small crustacea and invertebrates. 2° carnivore (Baxter). Starry Flounder: Small crustacea, clams; small fish. 2° - 3° carnivore (Baxter). Striped Bass: Shrimp, anchovies, small fish. 30 carnivore (Baxter). Leopard Shark: Crabs, Urechis; fish (scavenger). 3+ carnivore (Ackerman, 1971). TABLE àA TRACE METAL CONCENTRATIONS IN ug/gram DRY WEIGHT Species: Atherinops affinis, Top Smelt N = 3 N = 3 N = 3 liver flesh bone O.8 + 0.2 O.9 + 0.2 N.D. Pb N. D. 0.5 + 0.7 N.D. 2.0 f 0.1 Ag N.D. 3.4 + 0.3 4.9 + 0.2 90.0 + 20 Cu 0.8 + 0.1 N.D N.D 3.9 + 1.5 0.7 + 0.1 15.0 + 4.5 71.0 + 9 Mn 66.0 + 6 98.0 + 10 146.0 + 12 Species: Cymatogaster aggregata, Shiner Perch N = 1 N = 10 N = 2 liver flesh bone O.3 +O 0.2 + 0.3 0.2 1.6 1.4 + 1.4 1.3 f 0.1 Pb 2.7 + 0.2 0.2 + 0.2 N.D. 5.1 f 1.4 Cu 3.6 + 1.7 16.0 8.5 + 0.5 Cr N.D. 3.7 + 6.7 2.0 + 0.7 7.6 30.0 + 4 13.0 + 13 Zn 103.0 118.0 + 4 N = 3 gill 0.5 + 0.2 2.5 + 2.0 2.0+ 0.8 4.1 + 0.9 3.5 + 0.9 73.0 + 10 102.0 + 13 N = 2 gill 0.2 + 0.1 3.7 + 3.1 1.7 + 0 6.0 + 0.5 10.0 + 1.3 30.0 + 6 108.0 + 9 16 Species: Cd Pb Ag Mn Zn Species: Pb Cu Cr Mn Zn TABLE 2B TRACE METAL CONCENTRATIONS IN ug/gram DRY WEIGHT Platichthys stellatus, Starry Flounder N = 5 N = 5 N = 5 lag flesh liver bone 0.5 +0.2 1.6 + 0.8 O.9 + 0.7 N.D. N.D. 0.5 + 0.1 N.D. N.D. 2.7 + 0.7 4.3 + 1.3 111.0 + 14 1.5f0.2 1.3 + 1.2 6.4 + 2.0 7.0 + 3.7 1.0 +0.2 38.0 + 15 5.8 + 0.8 N.D. 238.0 + 6 112.0 + 18 Roccus saxatilis, Striped Bass N = 3 N = 3 N = liver bone flesh N.D. 1.0 f0.2 1.5 +O.1 N.D. N.D. 5.1 + 1.3 2.5 + 0.2 N.D. N.D. 1.2 + 0.4 5.0 +0.2 11.0 + 2 N.D. N.D. 3.4 + 2.4 46.0 + 4 1.5+0.6 7.1 + 0.8 20.0 + 2 94.0 + 11 73.0 f 11 N = 5 gill 0.9 + 0.6 3.6 + 2.5 1.0 +0.1 2.7 + 0.9 2.5 + 1.1 15.0 + 6 194.0 + 18 N = gill 0.5 + O.1 4.8 + 0.3 1.3 + 0.4 4.7 + 2.1 1.4 + 0.8 32.0 + 3 73.0 + 10 465 Species: Cd Pb Ag Cu Cr Mn Zn TASLE ac TRACE METAL CONCENTRATIONS IN ug/gram DRY WEIGHT riakis semifasciata, Leopard Shark N = 5 N = 5 N = 3 liver cartilage flesh N.D. 7.0 + 6.0 0.9 + 0.2 4.0 + 0.3 N.D. N.D. 1.3 + 0.2 N.D. 0.1 + 0.1 1.6 + 0.6 1.6 + 0.5 3.8 + 1.2 12.3 + 8.7 N.D. N.D. 0.5 + 0.5 2.5 + 1.2 15.0 + 3 44.0 + 3 19.0 + 2 33.0 + 13 N = 5 gill 0.7 + 0.3 N.D. 0.2 + 0.1 4.2 + 0.9 3.4 + 1.8 6.7 + 0.6 61.0 + 3 4 C Species: cd Pb Cu Mn Zn Species: Cd Pb Cu Mn Zn TABLE 3 TRACE METAL CONCENTRATIONS IN ug/gram DRY WEIGHI (Taken from Ting, 1967) Thunnus albacares, Albacore N = 10 N = 20 N = 10 flesh bone gill 1.0 f O 1.8 + 0.5 1.5 + 0.5 4.7 + 0.5 N.D. 9.8 + 6.2 1.7 + 0.4 1.8 + 0.4 2.9 + 0.1 O.4+0.5 8.5 + 0.7 7.0 +0.8 65.0 + 2.7 156.0 + 9 134.0 + 36 Katsuwonus pelamis, Skipjack N =10 N -10 N = 10 bone flesh gill 0.9 + 0.3 3.0 f 1.0 3.2 + 0.4 8.4 + 3.4 N.D. 14.0 + 6 1.6 f 0.7 5.4 + 1.2 6.6 + 0.5 0.9 + 0.3 2.5 + 1.3 5.4 + 0.4 24.0 + 3 142.0 + 6 55.0 + 9 169 e TABLE A Key to Figures = Top Smelt P = Shiner Perch = Starry Flounder B = Striped Bass = Leopard Shark flesh = liver - bone g = gill 660 FIGURE LEGEND Fig. 1. Map of Monterey Bay area. Fig. 2. Sites of concentration of cadmium in ug/g. Fig. 3. Sites of concentration of lead in ug/g. Fig. 4. Sites of concentration of silver in ug/g. Fig. 5. Sites of concentration of copper in ug/g. Fig. 6. Sites of concentration of chromium in ug/g. Fig. 7. Sites of concentration of manganese in ug/g. Fig. 8. Sites of concentration of zinc in ug/g. Fig. 9. Concentration of manganese in liver. Fig.10. Concentration of zinc in flesh. Fig.11. Concentration of zinc in bone. Fig.12. Concentration of cadmium in liver. 2o Santa Cryz Monterey Bay Montere carmel Pajaro River Elkhorn Slough oille Salinas River 4 Miles 462 o0 e 163 e oe H oe ve ce ve 26 . 222 ve ve oe 16 oe ve 5 26 2 te e ve S 46 LV ug/g o 16 2n (bnc oo (ver 9