-1 INTRODUCTION Sewage which has undergone only primary treatment, i.e. removal of grease and floatables, preliminary digestion, and treatment with Chlorine, has been discharged into the intertidal areas at Pacific Grove and Carmel, California until recently. Under an order from the State Regional Water Quality Control Board to "clean up" their sewage because of high Coliform counts, very large amounts of Chlorine were introduced into the effluent in the winter of 1969, in order to disinfect the sewage effluent. In fresh water systems, chlorination has proven to be a highly effective and relatively inexpensive method of controlling harmful bacteria. Chlorination of public swimming pools and fresh water supplies are common practices, and some cities are even chlorinating their storm sewer runoffs. (Pavia, et. al,1969) Enough information about such chlorination systems has been accumulated in order to understand both the beneficial and deleterious effects of Chlorine and Sodium Hypochlorite on the flora and fauna indigeneous to those fresh water systems. However, the effects of liquid Chlorine and Sodium Hypochlorite upon the marine flora remains largely unknown. A comprehensive study of all the effects of liquid Cl, and Naocl on marine algae is a prodigious undertaking and is clearly beyond the scope of this project. Therefore, this examination has been limited to determining the effects of Chorine residuals on the primary productivity of Prionitis lanceolata Harvey, Ulva lobata (Kützing ) Setchel and Gardner, and Macrocystis pyrifera (Linnaeus ) C.A. Agardh, a red, green, and brown alga respectively. . Chlorine residual studies and subjective observations that I made of the City of Carmel's sewage outfall suggested that a correlation between algal photosynthetic rates and the chlorine residual activity of the sea water might exist; however, a primary productivity analysis by the Winkler method for dissolved oxygen was impossible in this case, as both Cl, and OCl react very quickly with S,0,, the standard reagent in such analyses. The use of a modification of the Bean et. al. (1953) C0, uptake method circumvented this reaction, allowing the photosynthetic rates at different chlorine residual concentrations in the selected marine algae to be measured. MATERIALS AND METHODS The chlorine residual analysis was carried out using the Lodometric method with a starch endpoint described in Standard Methods for the Exam- ination of Water and Wastewater (1965). Samples were collected in 250 ml plastic reagent bottles and brought back to the lab within one hour of sampling and tested immediately. It appeared from preliminary data that in a 24- hr.period after the sampling, bacteria in the sewage capable of living on S,0, would cause the results to be much higher that they should have been. This was combatted by adding a drop of CCl, to each sample bottle along with the standard S,O, reagent and by immediate testing. The 10 sampling stations around the Carmel outfall and their relation to the onshore currents are shown in Figure 1. The results of the chlorine residuals analysis around the Carmel outfall area are presented in Figure 2. This figure shows a rapid decrease of the chlorine residuals in the sea water with increasing distance from the point of sewage discharge. Beyond 110 feet, the residual chlorine level 2/ had decreased to less than 0.1 ppm. Beyond 130 feet to either side of the sewage discharge, residual chlorine in the water was not detectable with this test. Sampling in a line parallel to the shoreline and nearly 1000 feet out to sea revealed no detectable residual chlorine; however, others (Grey and Nakata, personal communication) found chlorine residuals as far as 3000 feet to the south of the outfall. From this it might be inferred that the sewage field was staying close to shore and moving south. Figures 3,4,5, and 6 give the results of the current studies done at the Carmel outfall area. It can be seen that the currents do indeed run just offshore in the vicinity of the outfall and head south toward Monastery Beach and Whaler's Cove. After the residual chlorine levels in sea water had been established, the 3 algae, Prionitis lanceolata, Macrocystis pyrifera, and Ulva lobata were selected for the primary productivity tests. Prionitis (Rhodophyta) was selected because it was the commonest of all the algae near the Pacific Grove sewage outfall where the chlorine residuals in the water were found to be greater than 10 ppm (Remsen, personal communication). Ulva lobata (Chlorophyta) was selected because it was conspicuously absent form the immediate area around the same outfall. Finally, Macrocystis,in addition to belonging to the brown algae group, was selected because the proposed Carmel sewage outfall extension would move the effluent boil out into the kelp beds, and it would be of interest to know what effects Chlorine might have upon Macrocystis before the outfall pipe was extended. Labelling of the algae was accomplished by allowing small discs, approximately 5 mm in diameter, cut from the algae with a +2 cork borer to carry on photosynthesis in a sea water solution of Nahc 0, with and without NaoCl. In an attempt to limit the natural variation in photosyn S Janes Schreiber hetic rates from blade to blade, the dises were eut from the blades the following manner. With Macrocystis, 5 discs were cut from an area of 4 cm. near the tips off 4 blades taken from the same plant near the center of the frond. One disc of each set of 5 discs from each ade was used for each concentration of Ocl". In this way, even if one blade had a photosyntheitc activity much more or less than the other blades one disc from that blade would be in each set of the four replicates run at each of the 5 Ocl concentrations,(0, 1, 5, 10, and 15 ppm), which woul distribute any such effect equally among the results. With Prionitis, all the discs were cut from different blades because he blades were not big enough to allow more than one disc from near the apical point of the blade. The blades were chosen all of approximately he same length, from the same thallus, and from as close to the top the thallus as possible. Uva, however, was the hardest from which to get reproducible samples The dises were cut from near the margins of the blade, as close together as was feasible. It is recognized that this would not necessarily remove all the natural variabliity of photosynthetic activity in the dises, bu was assumed that such close sampling would limit it as much as was ssible. After the wet weights of the dises were taken, the dises, weighing om 1.6 mg to 2.4 mg for Ulva, from 5.6 to 6.2 mg for Prionitis, and com 5.9 to 6.3 mg for Macrocystis, were placed in 12 ml graduated centrifuge ubes with enough freshly filtered sea water (0.45 micron millipore filter make 5 ml of total solution when the 0.20 ml of 5.C/ml Nanc 0, solutior and ml of the Naocl solution were added. Naocl was chosen as the chlorine residual to work with because it is the major component of the chlorine residuals in sea water due to the following reaction; ((Baker, 1969 + HC - Hocl C19 + H,0 The NaoCl solution was made up with distilled water and not filtered sea water. It was felt that the OCl would be more stable in distilled water, as it normally will very rapidly begin to decompose in the presence of an easily oxidized material, such as would be present even in freshly filtered sea water. After weighing, 0.2 ml of 5C/ml NaHC 0, solution was added to each centrifuge tube containing the algal discs. This was immediately followed by the addition of the appropriate amount of NaoCl solution necessary to produce the proper initial concentration of hypochlorite, which was never more than 0.24 ml. The centrifuge tubes were then sealed with vaccine caps, swirled to mix the solution, and placed in the incubator for i hr. This incubator consisted of an outer plastic tub with both a water inflow and outflow tube for cooling water, an inner clear plastic box lined with aluminum foil and filled with fresh water, and a foil covered, wooden tube rack that was slanted at approximately 450 to the counter top in the hood. This slant allowed the algal discs to rest at the bottom of the tubes in a plane parallel with the counter top and perpendicular to the majority of the incident light. The water level in the inner plastic box was set such that the water would cover the centrifuge tubes up to the 5 ml mark, and the rate of flow of the cooling water through the outer plastic tub was set as necessary to keep the temperature of the inner bath at 20° c. The light source was a fluorescent light bank consisting of two 18 watt, 18 inch, soft white, G.E. bulbs in a aluminum foil covered hood. The light bank was placed over the centrifuge tube rack so that it was 4" from the algal discs. It was not possible, however, to eliminate outside radiation completely. In order to take the outside radiation into account, a complete set of runs was made only from 2 p.m. to 5 p.m. or from 11 p.m. to 2 a.m.. This was necessary because it had been observed in preliminary runs that the photosynthetic rates of those discs tested in the daylight hours of bright sunlight were consistently about 10 % higher than those discs tested under the incubator light source alone. As soon as the testing period was finished, the sea water solution of NaHC0, and NaoCl was drawn off with a 10 ml disposable syringe. The dscs were washed vigorously with 4 5 ml portions of filtered sea water, and the water was drawn off as before. The discs, still in the centrifuge tubes, were covered with 0.5 ml of 2 N methanolic KOH, and the tubes placed in an 80°C sand bath for thirty minutes. After thirty minutes, 30 % 20 was added to the solution in the tubes in 0.05 ml increments as necessary to dissolve the disc completely. When the H,O, activity had ceased, the contents of the centrifuge tube were diluted to 3.0 ml total volume with distilled water. Two 1.5 ml aliquots of this solution were transferred quantitatively from the centrifuge tube by means of a disposable pipette with two 15 ml aliquots of Bray's scintillation fluid into 2 scintillation vials and counted for 10 minutes for C activity on a Nuclear Chicago Scintillation Counter Model Unilux II. RESULTS AND DISCUSSION The comparative rates of photosynthesis for each concentration of NaoCl were determined by dividing the total disintegrations per minute (dpm. obtained from the dissolved algal discs by the milligrams wet weight of 7 the discs. Each disc was run for exactly 1 hr, so the above rate values have the following dimensions of dpm/ mg wet weight/ hr. Comparison of these experimental rates was done by taking the mean C''0, uptake rate of the control discs (O ppm Chlorine residuals) as 100%. Dividing the mean experimental C0, uptake rates by the mean control rate gåve the values in per cent of the mean control CO, uptake rate, which were then compared by plotting them against the appropriate concentration of OCl in parts per million. The results for Macrocystis are presented in Fig. 7, those for Prionitis and Ulva are presented in Figs. 8 and 9 respectively. These figures show that the concentrations of 15 ppm and 10 ppn OCl cause a definite decrease in the photosynthetic activities of each of the 3 algae tested; however, the results for the OCl concentrations of 5 ppm and éspecially i ppm are much less certain due to a greater degree of internal variation than was observed for the control discs and the discs in 15 and 10 ppm OCl. (See Table 1) Nonetheless, the OCl" concentration of 5 ppm does show a decrease of 25% in the photosynthetic rate of Ulva lobata and a 12% decrease in the photosynthetic rate of Macrocystis pyrifera. Prionitis lanceolata, however, did not show an effect for either 5 ppm or 1 ppm OCl", and further, the reductions in photosynthetic rates of Prionitis for the 10 and 15 ppn concentrations were considerably less than those found for Macrocystis and Ulva at the same OCl concentrations. This is presented graphically in Fig. 10. It would appear that Prionitis lanceolata (Rhodophyta) can resist the effects of OCl better than Macrocsytis pyrifera (Phaeophyta) or Ulva lobata (Chlorophyta), at least in the lab. However, close observation of both the Carmel subtidal sewage outfall and the Pacific Grove intertidal sewage outfall reveals that Prionitis lanceolata Harvey and Prionitis andersonii Eaton are the dominant James Schreiber species of macroscopic plant life within 5 feet of the end of the outfall pipes. At the Pacific Grove outfall, where the chlorine residuals sometimes reach levels greater than 10 ppm (Remsen, per. comm.), Prionitis lanceolata is the only macroscopic plant within 5 feet of the sewage discharge, and they seem abundant; yet there are no green algae or brown algae within this area. This could be expected in such an area of high chlorine residuals, judging from the results of this study It should also be noted from Figure 10 that Ulva lobata shows the greatest decrease in photosynthetic activity at lower concentrations of OCl. This might be a function of the particular pigments that Ulva, a green algae, would have;oi.e. the chlorophylls may be more susceptible to chlorine than the pigments of the red and brown algae. It might alse be explained by the fact that the blades of Ulva lobata are much thinner than the blades of Prionitis lanceolata or Macrocystis pyrifera. This might have allowed the penetration of OCl into the intracellular centers of photosynthetic activity to be more pronounced in Ulva than in Prionitis or Macrocystis, but the data cannot support either of these hypotheses to the exclusion of the other. The experimental results that have been obtained do apparently show an adverse effect of chlorine residuals on the rates of photosynthesis in the algae examined; however, other interpretations are possible. Since no attempt was made to make the OCl solution isotonic with the filtered sea water used in the experiments, it might be argued that the gradient of salinity present in the samples caused these effects. But the greatest decrease in the salinity was present in the 15 ppm OCl test solution. Only 0.24 ml of 312.4 ppm OCl and 0.20 ml of Nac Ho, solutions were added to 4.56 ml of filtered sea water in order to make up this 15 ppm 2 9 - James Schreiber OCl experimental solution. This represents a decrease of only 8.8 % in the total salt concentration of the experimental media from the control media, but this would hardly account for the 80 % decrease in the photo¬ synthetic activity of Macrocystis pyrifera at 15 ppm OCl or the 40 % decrease of Prionitis lanceolata at 15 ppm OCl". The variability of the results for 1 and 5 ppm OCl can be explained using the fact that only the initial concentration of OCl in the centrifuge tubes was known. Since OCl is a highly reactive ion that rapidly undergoes reduction in the presence of any easily oxidized substance, the actual residual OCl concentration could have varied due to the different levels of oxidizable materials in each centrifuge tube. Furthermore, no additional OCl could be added to the tubes after the run was started because this would have changed the critical concentration of available NahcO, in the tubes; consequently, any natural variation in the resistance of an alga¬ to the chlorine effects might have been accentuated by the variable lowering of the actual OCl concentrations in the centrifuge tubes. If this were the case, one would expect to see the standard deviation of the replicates decreasing with increased OCl concentrations because the small deviations from the initial OCl concentrations would become less important and because the differences in the resistance to chlorine would be less at higher Ocl concentrations. The experimental results show rather definitely that the standard deviations do decrease with increasing OCl concentration. (See Table 1 ) The experimental results suggest several types of experiments that need to be done before the mechanism of this effect can be understood. One such experiment would be to expose an entire plant to a concentration of OCl found previously to be detrimental to that plant for several hours, remove the plant to a fresh sea water aquarium, and then sample that plant a 10 James Schreiber for C0, uptake experiments at 1 hour intervals or so. In this way, it might be determined whether the chlorine residuals were affecting the plant reversibly or not. This experiment could then be coupled with a concurrent analysis of the plant pigments, in order to ascertain if the exposure to OCl had caused any damage to these crucial parts of the photosynthetic apparatus. From the results of these experiments, it might be possible to decide if the chlorine was primarily attacking the pigments or other vital components of the photosynthetic process. However, until such time as these types of experiments can be performed, it is only possible to state that residuals Chlorine levels of 5 ppm and greater de adversely affect the photosynthetic activities of the three algae studied, Prionitis lanceolata, Ulva lobata, and Macrocystis pyrifera 11 James Schreiber SUMMARY This project involved the determination of the persistence of residual Chlorine in sea water and the determination of any effects, either adverse or positive, of residual Chlorine from chlorinated sewage effluents on the photosynthetic activities of three representative algae, Prionitis lanceolata, (Rhodophyta ), Ulva lobata (Chlorophyta), and Macrocystis pyrifera (Phaeophyta ). By using the technique of quantitative C0, uptake to measure the rates of photosynthesis, a correlation between the concentrations of Sodium Hypochlorite in the experimental media and the experimental rates of photosynthetic activity was discovered. The results show that a residual level of 5 ppm Chlorine in sea water does adversely affect the photosynthetic activities of these algae. in the case of Ulva lobata by as much as 25 %. Higher concentrations of residual Chlorine have even greater effects,with 15 ppm residual Chlorine giving an 80 % reduction in the photosynthetic rate of Macrocystis pyrifera. 2 -12 LITERATURE CITED Characteristics of Chlorine Compounds. Journal Robert J., 1969. Baker, of Water Pollution Control Federation 41-3: 182 - 485. Bean, R. C.,,E. W. Putnam, R. D. Trucco and W. Z. Hassid, 1953. Preparation 4 labbelled d-galactose and glycerol. J. Biol. Chem., Of 204: 411 - 425. Pavia, Edgar H., Crawford T. Powell, Storm water disinfection at New Orleans. Pollution Control Federation, 41 - 4: 591 - 605. Journal of Water des - 13 - ACKNOWLEDGEMENTS My sincere thanks go to Dr. Isabella A. Abbott for her excellent advice and timely encouragement. I would also like to thank Dr. John H. Phillips and Phillip Murphy for their advice and technical assistance without which this project could not have been completed. This project was supported in part by the National Science Foundation's Undergraduate Research Program Grant No. GY - 7288. -14. CAPTIONS Figure 1: Chlorine residuals sampling stations: Detailed map of the Carmel outfall area showing the onshore currents and the sampling stations. Figure 2: Chlorine residual levels at the Carmel outfall: Curve A represents the values found for high tide. Curve B represents the values found for low tide. Figure 3: Surface currents 1000 feet offshore from the Carmel outfall: 12 drift bottles filled with fresh water were released from a skiff and followed from shore. Dotted lines show the path of the bottles. Figure 1: Surface currents near Monastery Beach: 12 bottles were released in a line perpendicular to the beach. Dye packets were attached to drift bottles to follow their paths. Dotted lines represent the path that the bottles followed. Figure 5: Bearings to the bottles at selected times: Both currents studies were carried out by taking a bearing to the bottle at a specified time and plotting these on a map. Figure 6: Drift bottle recoveries: Location and dated of recovery are listed along with bottle number. Figure 7: 0, uptake rate of Macrocystis vs the concentration of OCl : Curve represents the closest fit to the mean values. Standard deviation of the replicates is presented as a range of values around the mean. symbolizes the mean value. Figure 8: Standard 0, uptake rate of Prionitis vs the concentration of Ocl : symbolizes deviation presented as a range around the mean value. the mean values. 0, uptake rate of Ulva vs the concentration of OCl : Standard deviation Symbolizes the means presented as a range around the mean values. values. Figure 10: Mean values are plotted Comparison of Prionitis, Ulva, and Macrocystis; Prionitis and the curves are fitted to these mean values. Macrocystis. Ulva. Table 1 Results of the tests for each alga: Values for individual replicates are listed along with the mean values and the relative standard and standard deviations. 75 a( 5 — J ap 2 2 6 Carmel Bay CURRENT 5 STUDY May 11,1970 O930-1600 Mission Point 18 lee 0 50 1 e 1 V S Pt. Lobos Scale O REF.PT. Outfall OREF. PT. 2 6 Monastery Beach 1:10000 N 1 2 Fie Mission Point Carmel Ba Hen STUDY CURRENT II May 25,1970—1100-1300 Outfall 4 o H -- g-. - ---- ---+ 17 a 4 REF PT 3 Scale Pt. Lobos N Monastery Beach 1:10000 A Time 1032 1039 1102 1122 1132 1142 1232 1252 B Time 1115 1130 1145 1215 124 Ref. Pt. — 2 2 2 Ref. Pt. 200 185 197 185 210 206 205 200 188°205 178 185 182 181 34 22 15 12 20 12 8 10 CURRENT STUDY I No. Bottle 4 215 222 205 212 207 215 218 206 210 202 214 216 227 230 222 213 209 212 208 218 215 206 215 212 205 216 210 193 198 200 187 195 195 187 189 190 168 CURRENT STUDY II Bottle No. 4 925 345 330 310 339 345 342 34 353 350 35/ 350 358 350 4 355 0 355 3 3 7 10 244 233 236 224 229 222 214 24 233 214 215 238 2/0 °228 215 224 208° 202 200 202 195 20 195 8 10 322 318 320 335 335 337 339 331 345 354 353 353 254 230 240 224 218 210 199 183 3/6 334 336 350 358 12 260 238 248 248° 235 230 12 315 330 335 350 358 3, O C Stuc II Bottle No. 8 12 10 12 Location Monastery Beach N. Pt. Lobos Monastery Beach Approx. 50 yds. off north end of Monastery Beach Date 5/21/70 5/25/70 5/22/70 70 5/27 5/27/70 P1e 05 9. 5 u 95 00 3 60 50 40 20 100 ppm of Chlorine F16 1 - 00 jomof Chlorine Residuals N 2 3 . 932 2. 90 1000 90 80 2 10 60 50 5 40 S 30 20 ppin of Chlorine Ple. 8 8 95. 9 1004 50 — ppm of Chlorine F16. 932 X 90 14 20 E 50 110 100 ppm of Chlorine Fie 10 Macrocystis ave. rel. 5. Prionitis ave, rel. §. Ulva ave re 5 dom 940 ma 1037 870 104 987.5 6t.7 6.7 % 603.4 521. 6 911. 0 620.0 66+.o 147.4 227 8100 632.6 403.6 530. 627. 718.1 7711.0 147. 3 21% TABLE om Chlorine pp 15 44 54 23 158 119.8 56. 5.6% 328 442 334 443 399 10.6 11.6% 242.8 343.9 217.6 135.6 247.5 78.7 169 10 443 495 352 674 603.5 14 II.3 % 484.8 649.5 574.0 468.2 546.7 18.2 16%0 410.8 318.4 125. — 121.2 21% 09 1293 505 173 835 274.7 28% 818.0 674.3 57.3 43.6 156.7 23% 384.0 1014.0 343.0 54.0 591.3 290 41 7 770 1066 368 /301 873.5 347. 37.3 % 418.3 640.3 868.6 (42.3 186.2 28.470 278. 119.5 07.2 357.4 621.1 180.6 25 7