C COMPARISON OF DDT RESIDUE VALUES OF PLANKTONIC ORGANISMS AT THE AIR:WATER INTERFACE AND SUBSURFACE LEVELS OF MONTEREY BAY Keith G. Baxter Hopkins Marine Station of Stanford Universit running title-- S AT THE AIR:WATER INTERFACE DDT RESIDUE Send correspondence to: Hopkins Marine Station, Pacific Grove, California C ABSTRAC Plankton samplos from the surface and ten meters depth were collected in Monterey Bay and analyzed for DDT residues. The results show a trend toward higher concentration at the air-sea interface. Possible mechanisms of concentration are discussed, with some consideration given to the ecological implications. C O 4 —- INTRODUCTTON Investigation of the unique properties of the air: water interface with relation to DDT content of its resident species has generally been neglected in the scientific literature. There are, however, many important attributes of this surface layer which indicate that it might play a significant role in both the concentration and eventual biological magnification of DDT. The major difference between the surface layer and other sub-surface depth zones is its constant contact with the air. This allows significant imput of DDT residues due to atmospheric fallout (Cox, a-1971; Risebrough,1968). ly evidence suggesting this process were studies of: i) the codistillation of chlorinated hydrocarbons with water (Sowman, et.al.,1964; ibid.,1969); ii) its detection in air and rain water (Antommaria, et.al.,1965; Abbot,et.al.,1965: ibid.,1966; Wheally, et.al.,1966); iii) its appearance in atmospheric dust originating in Texas and subsequently deposited in Ohio (Cohen, et.al.,1966). More recent analysis has shown that an average of 32 X 10 g of DDT residues were present in dust particles over the Bay of Bengal (Goldberg and Griffen,1970). Risebrough (1968) has found 1.8 X 10"2 total pesticides/gram of dust in La Jolla, Calif- ornia. However, these estimates of pesticides should be considered minimal. The sampling techniques used elimin- ated particles less than one micron, which may constitute 47 the majority of the adsorptive interface of DDT residues (Dolaney, ot.al.,1967; Pfister, et.al., 1969; Routh,1971) The upper layer of the ocean in enriched with potassium, ammonium, organic nitrogen, and organic particulate matter (Wilson,1959). The latter aggregates are produced in thin films by the adsorption of dissolved organic material on rising bubbles (as those produced by wave action and active photosynthesis), other subsurface objects, and the sea surface itsolf (Riley,1963,; ibid.,et.al.,1961; Siegal & Burke, 1965; Blanchard,196; Sutcliffe, et.al.,1963.) This process allows for a mechanism of concentration of DDT residues. Seba and Corcoran (1969) have shown values of chlorinated hydrocarbns up to 13 X 10"2 g/ml in surface slicks in Biscane, Florida, mpared to approximately loi g/ml in the surrounding water. or The fact that a small crustacean has been shown to exist solely on organic aggregates (Baylor & Sutcliffe,1963) suggests a means of entry of these concentrated pesticides into various foodchains. DDT residues, being insoluble in water, have been linked with specific particulates (Pfister, et.al., 1969; Routh,1971), and hence would be ammendable to this scheme of input. The soa surface itself is a natural concentrator of detrital matter. Most debris is either heavier or lighter than sea water (Wilson, 1959). The latter rises to the tor to form an upper layer, while the heavier sinks to benthic 411 sediments. The very fact that an interface is present is significant, for they account for many of the chemical roactions ofthe ocean (Horn,1969). In most regions of the world, the surface layer is inhabitated by unique neustonic populations (David,a-1971). which have maximum contact with the interface. These in turn are preyed upon by a variety of organisms which provide for a means of both the concentration and transformation of DDT through various trophic levels. These creatures include larve, fish, vertically migrating predators, and skimming birds (Cox,a-1971). The latter, especially, are known to have very high concentrations of DDT (Tatton & Zicka,1967). The surface in unique in its chemistry and tendency to concentrate particulate matter. The chemical properties of DDT residues associate themselves with particulates. These two observations, in addition to the contribution to atmospheric fallout, lead one to believe that surface organisms leeding on surface populations and injesting and adsorbing particulates at the air:water interface would show higher levels of pesticides than organisms exposed to greater depth zones. This experiment will attempt to show this phenomenum mpling and analyzing several different groups of organ- by sa isms which are found at the surface (designated as neustonic), These will be compared to similar organisms taken from subsurface samples (labelled as plankton). 4 ETIIODS MATERIALS AND! Samples were collected using a nouston sled towed at the surface (David,b-1965) and a small zooplankton net simultaneously towed about ten meters below the surface. The two nets had openings of similar area (0.016 M- for the sled, 0.061 M for the plankton net) and similar mesh (220.5 microns -- sled, 291 microns -- plankton net). The sled was either towed off to the side of the boat by moans of a boom, or was trailed far enough aft so that the wake had little effect. Tows lasted from one-half hour to one hour. All inshore tows were taken at about the same time of day. Boat speed was recorded and used in the cal- culations of relative biomass density. While on board, the fresh samples were taken from the net and placed in acid- cleaned (M-6 N HNO,) glasswear, covered with aluminum foil, and stored on ice. In the lab, major groups of organisms were seperated from each other. This usually consisted of seperating calaniod copepods from ctenaphores (Pleurobrachia bachii) jatina). This was easily done and medusea (especially Oct by the sample through a course (inch mesh) net. The remaining sample was strained through a ring of phytoplankton netting, retaining the copepod segment of the sample. Excess water was removed and wet weights recorded. Initial preparation of the samples was done by the method described by Burnett (1971). The only deviation 50 C M-2 was the addition of 0.05g of acid washed Nuchar Attaclay to the silica gol (Grade 950,mesh 60-200, dessicant-activated) microcolumn to remove additional pigments and impurities. In addition, the samples in tow number 5 were mixed with metalic mercury to remove sulfur compounds. Pesticide analysis was accomplished by a Beckman Go-I gas liquid chromatograph. The solid support for the colunn was 80-100 mesh Chromosorb W, acid washed and DMOS treated. It was a mixed bed arrangoment, employing equal parts ol 65 QF 1 and 8% DC 200. Initialidentification of peaks was based on retention times as determined by known injected standards. Various samples throughout the experiment were analyzed by Pesticidequality hexane and acetonitrile partition coefficients to supplement retention times. 5 5 RESULT The rosults of three inshore and two offshore tows are summarized in Figure 1 and Table 1. Table 2 gives probability values for the following comparisons: I. Examination of concentrations of all neustonic copepods ys. all planktonic copepods yields p values of .10 for DDD and.20 for DDT. II. There is a significant difference between inshore copepods and offshore copepods for DDE (p-.02) and DDT (p-.001). —-+ 111. Comparison of ctenaphores (Pleurobrachia bachii) in the neuston and plankton samples showed no signilicant correlation (pp.10). IV. A comparison between Euphasia pacifica in the neuston and plankton samples yields p values y.30. V. As the relative density of neustonic copepods decreased in a series of runs, there was a corresponding increase in the relative density of planktonic calanoid copepods (Figure 2). VI. There is an inverse correlation between relative densit and concentration for individual DDT residues and sums in neustonic calanoid copepods (Figures 3,1, & 5). DISCUSSION A comparison of the results with other values in the literature is difficult because of the scarsity of the latter. Woodwell etal. (1967) did find 10 ppb total DDT residues in plankton from a polluted esturary on the East Coast. Cox (a-1971) found 30 ppb in large pooled copepod samples in Monterey Bay. (Converted to wet weight concentrations as shown by Martin, 1971). These values compare with the range of 10-37 ppb for individual samples in the three inshore tows. The differences between the neustonic and planktonic populations were not as great as expected. This is undoubt- edly due to sampling techniques which did not allow collection of those organisms that are uniquely and consistently found at the air :water interface. Instead of true "neustonic" residenis, the organisms consisted primarily of vertically migrating calanoid copepods. However, the fact that a trend towards higher values (especially with DDT) was found in the upper layers is encouraging. Here one must conclude that the differences in residue values is attributable to exposure to the concentrating capacity of the surface. Marian (1971) found similar results when analyzing Hermissinda ssicornis collected from floats and wharf pilings at O.3-7.0 meters. The organisms at the surface had residue values of 2.3 X that of the mean of the piling population. The significant difference between inshore and offshore 53 copopods may be duo to the location of the sewer outfalls, other effulonts, and the marina inshore relative to off- shore (Figure 1). Large differences in DDT values further substantiate this rolationship, since the organisms immediate responso to the onvironment would be reflected in these values. In addition, the largest DDT values were found in the tow nearest the two outfalls, with levels decreasing as a function of distance from the effulents. The same correlation with distance was found in Tow 1 away from the mouth ofthe marina. Swarbrick (1971) found a similar falloff in the same transect in DDT analysis of Pagurus samuelis. The ctenaphores sampled from both dopths were showm to be from the same population. Because of their sensitivity to sunlight and weather conditions (Hyman,1910,p662, they are in continual movement in the water column. This is substantiated by observation of changing densities throughout the five tows. This consistent fluctuation may eliminate the possibility for effective concentration. In addition, the high S/V ratio and high water content (95-97%) minimizies the amount of adsorptive and assimilative surfaces. i Similarity of the neustonic and planktonic E. oifica may be a result of the strength of migration of the population. The 0030-0230 runs of Tow 5 resulted in 99% E. pacilica at both the surface and 10 meters. The 0600-0700 netted only scattered euphausids in both samples. Accompaning these movements is undoubtedly a large amount of mixing, which would tend to mask differences in concentration levels. Examination of Figure 2 shows an inverse relationship between the rolative densities of the neustonic and planktonic copepod populations. This is what one might expect from a partly migrating species. That their migration is not total is shown by their presence in different densities in all tows at all times of the day. It is likely that some organisms seldom leave the surface, while others spend most of their time at subsurface depths. This is reasonable, since in any migrating population, there will be member: which are skowed to either side of the mean movement of the population. There is some evidence that this distribution may be physiologically determined. Marshall and Orr (1955) have noted that copepod females migrate to the surface to lay their eggs. Moreover, females tend to migrate more regularly than males. Bainbridge (1952) noted two distinct layers of copepods in a summer bloom: a dense population in the top 30 cm, and a subsurface layer in which the copepods were more sparsley distributed. That the relative density may be an indication of residence time of the members in any one layer is shown by the inverse relationship between concentration and density in neustonic copepods (Figures345). As the relative density of the neuston layer is decreased by downward movement, the relative concentration of DDT residues is increased, since the remaining animals will have been exposed to the surface for a longer period. 63 Supplementing the residence time with respect to concontration are the proporties of injestion and adsorption at the surface. Both of these properties are taking place simultanoously (Cox,c-1971). As density increases, loss pollutants are available/organism, and the concentration values drop per unit weight. The fact that Cox (b-1971) showed similar slopes for the density vs. concentration of organic particulate matter may indicate that while at the surface, adsorption contributes significantly to the total DDT levels. A third contribution to the inverse density:concentration relationship is the location of the various tows. Location of effluents could have completely determined the concentration values irrespective of density. However, Lopez (1971) found no correlation between values for heavy metals as a function of location. He did demonstrate the same relationship for y and concentration. This indicates that something dens more than location is responsible for this phenomenum. That the planktonic samples did not exhibit this relation- ship is presumably due to scattering after leaving the two dimensional confinements of the surface. 56 C CONCLUSTO The rosults presented here favorthe hypothesis that DDT residues are concentrated at the air:water interface relative to the subsurface zones. Problems encountered in sampling, analysis, and population structure of the study orcanisms tended to mask these dil ferences. The implications from this surface concentrating effect may be significant. Any organism that is subjected to this region will be brought into contact with higher concentrations of DDT residues than its usual medium. Therefore surface feeding larve, filter feeders, and skimming birds may be receiving relatively high levels of pesticides in their food. By this method an important means of DDT input to both marine and terrestrial food webs is established. O 5 C Acknowledgements I would like to thank the entire staff of Hopkins Marine Station for their valuable assistance and encouragement, especially Dr. Malvern Gilmartin, Mr. Phillip Murphy, Mr. Robin Burnett, and the crew of the R/V Proteus. This would was made possible by grant GY 8950 of the Undergraduate Research Program of the National Science Foundation. Literature Cited Abbot, R.B., (1965), Organochlorine Pesticides in the Atmospheric Environment, Mature, 208:1317. , et.al., (1966), Organochlorine pesticides in the mosphere, Nature, 211:259. Antommaria, P., et.al., (1965), Airborn Particulates in Pittsburg: Association with p,p' DDT, Science, 150:1176. Bainbridge, (1952), Underwater Observations on the Swimming of a Marine Zooplankton, J. Mar. Bio. Ass. U.K., 31: 107. Baylor, E.R., & W.H. Sutcliffe, (1963), Dissolved Organic Matter in Sea Water as a Source of Particulate Food, J5. mnol. and Oceanog., 8:369. Li Blanchard, D.C., (1964), Sea to Air Transport of Surface Active Material, Science, 1146:396. Bowman, M.C., et.al., (1964), Chlorinated Insecticides Fate in Aqueous Suspensions Containing Mosquito Larve, Science, 116:1180. Burnett, R., (1971), DDT residues: Their Distribution Along Coastal California, Science, submitted. J.H., & C. Pinkerton, (1966), Widespread Translocation Cohen, of Pesticides by Air: Transport and Rainout, p 163, icides in the ic Pes in R.F. Gould (ed.), 0 nvironment, American Chemical Society, Washington 5 D.C., 309 pp. Cox, J.L., (a-1971), DDT Residues in Coastal Marine Phyto¬ plankton and Their Transfer in Pelagic Food Chains, Ph. D. Thesis, Stanford University. . (5-1971), DDT Residues in Sea Water and Particulate Matter in the California Current System, Fish. Bull. submitted. (c-1971), Uptake, Assimilation, and Loss of DDI Residues by E. pacifica, a Euphasid shrimp, Fish. Bull., submitted. P.M., (a-1965), The Surface Fauna of the Ocean, Endeavour David, 21:95. . (b-1965), The Neuston Net, a Device for Sampling the Surface Fauna of the Ocean, J. Mar. Bio. Assoc., U.K.,15:313. A.C., et.al. (1967), Airborn Dust Collected at Barbados, Delan Geo m. Cosmochim. Acta., 31:885. riffen, (1970), The Sediments of the Northern Goldberg & ( Sea Res., 17:513. Indian Ocean, Dee y, John Wiley & Sons, R.T., (1969), Marine Chemistr Horne, New York, 566 pp. The Invertebrates: Protozoa throu? man, L.H., (1940), tenophora, MoGraw Hill, New York, 726 pp. Lopez, G. (1971), Analysis of Heavy Metal Concentrations at the Air: Water Interface and Subsurface Waters of Monterey Bay, unpublished. rine Biology of aM Marshall, S.M. and A.P. Orr (1955), The! 60 Copepod: Calanus fenmarchicus (Gunnerus), Oliver and Boyd, London, 188 pp. Marian, R., (1971), Assimilation and Transfer of DDT Residues in a Hydroid-Nudibranch-Tetribranch Food Chain, un- published. Martin, J.H., (1970), The Possible Transport of Trace Metals Via Molting Copepod Exoskeletons, Limnol. Oceanog., 15:756. Pfister, R.M., et.al., (1969), Microparticulates:Isolation From Water and Identification of Associated Chlorinated Pesticides, Science, 166:878. Riley G.A., (1963), Organic Aggregates in Sea Water and the Dynamics of Their Formation, Limnol Oceanog., 6:372. , et.al., (1964), Organic Aggregates in Tropical & Subtropical Surface Waters of the North Atlantic Ocean, imnol. Oceanog, 9:516. Risebrough, (1968), Pesticides: Transatlantic Movement in the Northeast Trades, Scjence 159:. Seba & Corcoran, (1969), Surface Slicks as Concentrators of Pesticides in the Marine Environment, Pest. Monit. J., 3:190. Siegal, A, & B. Burke (1965), Sorption Studies of Cations on Bubble Produced Organic Aggregates in Sea Water, Deep Sea Res., 12:789. Sutclille, W.H., et.al., (1963), Sea Surface Chemistry and Langmuir Circulation, Deep Sea Res. 10:233. Gwarbrick, S., (1971), DDT Residues in the Marine Intertidal 61 C s in California Wators, Hormit Crab P gurus sane unpublished. Tatton, J O'G., & J.H. Ruzicka, (1967), Organochlorine o 215:316. Posticides in Anarctica, Matu Wheatley, G.A., & J.A. Hardman, (1965), Indication of tho Presence of Organochlorine Insecticides in Rainwater in Central England, Nature, 207:166. Wilson, A.T., (1959), Surface of the Ocean as a Source of Air Born Nitrogenous Material and Other Plant Nutrients, Nature, 164:99. Woodwell, et.al., (1967), DDT Residues in an East Coast Estuary:A Case of Biological Concentration of a Persistent Insecticide, Science, 156:871. C C Table jl - Mean values obtained for p,p' DDE, p,p'DDD, us of all p.p' DDT, andthe means of the si three residues in samples collected during five tows in Monterey Bay. The standard error was computed as follows : SE - (P N-1 TABLE 1 SAMPLS POPULATTON DD Nouston copenods .611.7 Plankton copepods 6.111.3 Inshore N.copepods 6.1+1.8 Inshore P. copepods 6.211.5 Inshore copepods 6.311.1 Offshore copepods 2.2+0.1 Neuston E.paci 3.110.5 ia Plank aEpaifice 5.312.8 All E.paci 1.311.1 Neu. ctenaphores O.6+0.3 — Plan. ctenaphores O.5+0.2 All copepods 16 5.8-1.0 All ctenaphores O.5+0.1 09 CONCENTRATIONg/1 Total residues DDT 8.9+2.1 3.310.8 17.912.9 13.212.9 5.6-1.1 1.9-0.1 10.012.1 20.041.3 3.6-0.9 6.211. 11.513.0 2.1+0.1 6.111.3 2.840.5 17.212.6 1.1+0.2 1.1+0.7 2.211.1 8.1-0.8 2.712.1 2.0+1.7 2.911.9 9.710.8 1.510.2 —— 6.9+0.7 1.8+0.6 2.8+1. O.6+0.3 O.7-0.2 1.6-1.3 O.5+0.3 0.340.1 1.3+0.3 15.612.5 7.311.3 1.1+0.8 1.1+O.8 O.6+0.5 O.1+0.2 C Table 2 - The probability that the two populations compared are from the same general population, as computed by the "t" test, ie. t- 2-X. — 2 61 n- + n- 6 C POPULATTONS COMPARE All neuston copopods All plankton copepods Inshore N. copepods Inshore P. copepods Neuston E. pac ica Plankton E. ie Inshore copepods Offshore copepods Neuston ctenaphores Plankton ctenaphores TABLE 12 DDE .50 .90 .50 .02 .90 DDI .10 .20 .80 .60 .80 DDT .20 .10 .90 .001 .10 66 2SIDU TAL REIDOD .10 .30 .30 .O1 C Figure 71 - Species composition and towing conditions for the 11 runs in Monterey Bay. Abundance scale is: +++ most abundant; ++ frequently observed; seldom observed. Circles indicate sewer effluents, corresponding numbers show treatment (ie. primary, secondary, etc.) San Lorenzo 68 FIGURE T River SANTA CRUZ Tow j-3 runs 1./29/7 0715-0915 Calm-overcast Calano oe +++ + ++ P. bachi Tow 2-1 run o8oo-0830 5/61 Overcast,cold,windy Plankton: (10-15 M) Neuston: Calanoid oppods +++ Calnid oed +++ surface)P. bachii ++ bachii ++ Iarval shrimp ++ larval shrimp + larval crab (zoa) + Elkhern larval crab + Leptomedusae + Gammarid amphipod + Beroe forskali ish + Slough larval uphausid + To 3-3 runs 5/1 0830-1030 Calm,overcast. Plankton: Calanoid coper Heuston:alnoid oepod ++ P. bachii ++ + ++ bace larval crab (megalops) amphapods + Tow -3 run Salinas River 5/11/7 o900-1300 par ly cloudy,choppy Plankton:Calanoid copepods +++ euston:alanoid opepods +++ perid amphapods + honophores - larval fish+ Hyperid amphapods + Euphausid bachii lomopterus+ 3runs Tor 2 10w1 0030-02 TOW3 Windy,choppy,cold Sron + ++ Neuston: E. paifica la: rval crab (megalopa sh (small) MONTEREY Siphonophores + Medusae + Calanoid copepod Tow 15 (con);0600-0700 H.paifica + +++ Windy,choppy,cold Plankton: euston:Calanoid copepods ++ P. bachi. (10 M) crab larve (megalops Calanoid copopods ica squid (juvenile) d amphapods+ Pla ton-10 M: tarmel Rivef Calanoid copepods: honophores + Medusae ++ P. bachi TOW 5 larval fish + C Figure j2 - Neuston copepod relative density vs. plankton copepod relative density for tows j1,3,811. 6 -0.0 -10.0 -11.C 9.O FIGURE II o-701 o -101 2 X -101 4 -7.0 -8.0 log plankton density (g/m3) 70 C Figure 3 - A graph of the concentrations of the means of neustonic DDE, DDD, and DDT residues vs. relative density as collected on inshore tows il & 42. Wach point represents seven pooled samoles, c 58+ 38 -104/ DDT RESIDUES NEUSTONIC COPEPODS LOG DENSITY - / 9.37 FIGURE 3 72 C Figure 31 - A graph of neustonic DDT residue concentrations ys, relative density as collected on inshore tows jl & 13. Each point represents two pooled ples. 10.4 O.O 8.6 7.2 54 40- -10.47 DDT NEUSTON COPEPODS -9.77 10G DENSITY - 6/M FIGURE 4 -9.37 C 74 O Figure 75 - A graph of neustonic DDD concentrations ys. relative density as collected on inshore tows 1 8. 13. Each point represents two pooled samples. 0 147 43 -10 082 078 -10.47 DOD NEUSTON COPEPODS 9.77 LOG DENSITY /m -9.37 FIGURE 5 76