Biological Effects of Zosteric Acid in Solution: Barnacle Behavior and Settlement, Bacterial Attachment, and Sea Urchin Fertilization Corita R. Grudzen and Suejin Hwang Correspondence can be sent to: Corita Grudzen Suejin Hwang ABSTRACT Zosteric acid (p- sulphooxy cinnamic acid) was studied for its role as a non-toxic antifouling agent. Cypris larvae of B. amphitrite were used to study the effects of the compound on larval chemotaxis, mobility, and settlement. Zosteric acid (ZA) elicited no chemotactic response from the larvae and therefore it does not appear to inhibit settlement by deterrence. ZA and sodium acetate, a weak acid with a similar pKa, did both cause larval immobility, possibly acting as weak acids and changing intracellular pH. Both pH neutralized (8.0) and unbuffered ZA were shown to inhibit settlement by up to 30%. Because the presence of microbial films can act as settlement cues for further fouling by both larval invertebrates and algae, ZA’s effect on bacterial attachment was also investigated. Both zosteric acid, a sulfated phenolic ester, and p- coumaric acid, an unsulphated analog of ZA, were found to suppress bacterial attachment. Therefore, it can be concluded from this study that the sulphate moiety is not the necessary component for inhibiting bacterial adherance. The effects of ZA were also assayed on the attachment of sperm to the egg in the fertilization of the sea urchins Strongylocentrotus purpuratus and Litichinus pictus. It was found that the sulphate group on the ZA is necessary for the inhibition of fertilization. Another fertilization experiment, in which Protease was used to remove the vitelline layer of the egg, showed that ZA may inhibit fertilization by binding to the egg receptors on the vitelline layer, thus blocking sperm from attaching. In conclusion, it should be noted that ZA has a wide variety of effects and more than one mode of action. Multiple mechanisms seem to be involved, both individually and synergystically, in producing ZA's antifouling effect. INTRODUCTION Biofouling, the attachment of a wide variety of organisms to à submerged surface, has been and continues to be a major economic concern. Both microscopic and macroscopic organisms contribute substantially to drag and the loss of integrity of ships and other vessels. In the past, the most effective antifouling compounds have been toxic to marine life prompting continued research in this area. The recent identification and synthesis of p-(sulphooxy) cinnamic acid, commonly known as zosteric acid (ZA), by Dr. Richard Zimmerman is one of the first natural non-toxic compounds shown to prevent fouling of a wide range of organisms (Todd, Zimmerman, Crews, and Alberte, 1993). This work was inspired by the observation that new leaves of Zostera marina, from which the compound was isolated, were essentially free of fouling organisms from marine bacteria to barnacles (Harrison, P.G., 1982). The objective of this study was to determine the mechanism(s) by which zosteric acid inhibits fouling. The most prevalent form of fouling is barnacle settlement (Christie, A.O. and Dalley, R., 1987). Therefore, three Balanus amphitrite bioassays analyzing the effects of ZA on larval chemotaxis, mobility, and settlement were performed to determine the compound's mode of action of ZA. The effects of ZA on marine bacteria were also studied because the presence of microbial films was shown to act as a settlement cue in recruiting cypris larvae to surfaces (Maki et al., 1990) Cypris larvae respond to surface associated stimuli during settlement and metamorphosis. Attached bacteria can present various stimuli by changing the surface chemistry through their physical presence and or by the production of extracellular molecules. Therefore, by preventing the formation of bacterial films, the primary initiator of fouling that leads to the successive growth of both algae and marine invertebrates, ZA may inhibit barnacle settlement. Zosteric acid was also tested in another type of attachment assay, the attachment of the sperm to the egg in the fertilization of sea urchins. Gametes from both Strongylocentrotus purpuratus and Litichinus pictus were used to determine the mode of action of ZA as a possible inhibitor of attachment. MATERIALS AND METHODS The competent cyprids of Balanus amphitrite used in this study were cultured by James S. Todd at the Marine Sciences Laboratory of Duke University according to the method described in Rittschof, D., 1992. Chemotaxis Assay Chemotactic response was assayed using a 50 cm long trough of PVC pipe. Barnacle larvae were maintained at a temperature of 6-8° C to prevent settlement and kept at room temperature during the experiment. Both ends were closed with silicone gel and rubber stoppers were used to prevent water flow between the five 10 cm sections. To begin, a rubber stopper was placed at 20 and 30 cm from side #1 and from approximately 250 barnacle larvae were pipetted along with 8 ml of FSW into this section of the trough. 14 ml of FSW were then added to the 0-20 cm section and 16 ml to the 30-50 cm section. At time zero 2 ml of 30 mM ZA were added at 0 cm and the two rubber stoppers removed allowing the movement of the cyprids and the diffusion of ZA throughout the trough. At 60 minutes, a rubber stopper was placed at each 10 cm mark from side f1 (10 cm, 20 cm,...) and the number of larvae in each of the five 10 cm sections were counted (0-10 cm, 10-20 cm....). Experiments were disregarded if the number of larvae was less than 100 or if the two rubber stoppers were not released at the same moment. The side in which the ZA was added (f1 or f2) was reversed every other experiment. A control experiment was run exactly as above with one exception¬ 16 ml of FSW was added to the 0-20 cm section and no ZA was used. Cyprid Mobility Plastic Falçon petri dishes were used to evalute the effects of ZA, p coumaric acid (CA) and sodium acetate on B. amphitrite motility. From 10 to 30 larvae were used in each dish containing 2 ml of solution. 2, 4, 6, 8, and 10 mM concentrations of ZA and 3, 5, and 7 mM of CA were used in both buffered (pH 8) and unbuffered (pH 3.9 for CA and pH 5.2-5.7 for ZA) solutions. Sodium acetate was used at 10 mM both buffered with Trisma as above (pH 8) and unbuffered (pH 5.7). Cyprids were considered motile if they were noticeably active under the microscope and/or their appendages were extended after 15 minutes. Two types of control experiments were used: one contained 2 ml FSW and the other a buffered solution of MES (pH 5.6), both absent of any of the above weak acids. Two replicate dishes were analyzed for each concentration, buffered and unbuffered. Barnacle Settlement Assay Attachment of cyprids of B. amphitrite was assayed against ZA, CA, and sodium acetate in plastic dishes (Falcon 43001) containing 20-60 larvae and 5 ml of solution at room temperature. Each experiment was stopped after 24 hours using a few drops of 1 N HCI and the number of attached barnacles were counted using a dissecting microscope. Varying concentrations of buffered and unbuffered ZA, CA, and sodium acetate were assayed with 6 replicates for each unbuffered ZA concentration and 4 for each buffered one. CA and sodium acetate assays were done once. Experiments were disregarded if there were less than 20 larvae in a petri dish. Bacterial Attachment Two different assays were done to test the effects of ZA on bacterial attachment. The first was a hemagglutination assay done with red blood cells and bacteria to test for the ability of zosteric acid to prevent agglutination of red blood cells due to the adherence of bacteria. The experiment was carried out in eppendorf tubes with an overnight culture of Vibrio cholerae and human type O- whole blood that was centrifuged at 3000 rpm for five minutes, washed, and resuspended in phosphate buffered slution (PBS) three times to arrive at a 5% solution of red blood cells. A 1% solution of fucose, and 6 mM zosteric acid neutralized to pH 8.0 were additional components. The first tube contained 15 ul of bacteria and 50 ul of red blood cells in PBS, the positive control for hemagglutination. The second tube consisted of bacteria, red blood cells, and 100 ul of fucose (a sugar known to inhibit hemagglutination). The third tube contained bacteria, red blood cells and 100 ul of 6mM zosteric acid (3mM final concentration in tube). The last two tubes acted as controls containing red blood cells and either zosteric acid or fucose, to make sure that these compounds were not affecting the red blood cells. Appropriate amounts of PBS were added to each tube for a final volume of 200 ul. The tubes were left to sit for 30 min and then samples were removed and checked under the microscope to observe for bacterial induced agglutination of the red blood cells. The second bacterial attachment assay was set up to determine the relationship between varying doses of zosteric acid in solution and the density of attached bacteria on a surface. Coumaric acid, an analog of zosteric acid without the sulphate group, was also tested for the ability to prevent bacterial attachment to surfaces. Five 50 ml Falcon tubes were set up, each containing 200 ul of three marine bacterial isolates of the strain Shewanella. The control tube contained 600 ul of the bacterial strains and SSW, for a total volume of 30 ml. The four experimental tubes contained bacteria, and three different concentrations of pH neutralized zosteric acid (0.03mM, O.3mM, 3.OmM) or coumaric acid (3.0 mM), and the appropriate amount of SSW for a final volume of 30 ml each. A glass slide was then placed in each tube such that it would float horizontally once the tubes were placed on their sides. The tubes were placed on a rocker at room temperature for two hours. Each glass slide was removed and dipped in SSW three times to remove much of the excess unattached bacteria. The underside of each slide was examined to ensure that the bacteria were specifically attaching themselves as opposed to settling due to gravity. The slides were then examined and photographed under the microscope. The number of bacteria per unit area was counted to quantify the density of the bacteria attached to the surface of the slide. Sea Urchin Fertilization Several experiments were done to determine the effects of zosteric acid on sea urchin fertilization and the possible mechanism by which it functions. A dose response experiment for both ZA and CA was performed with eggs and sperm of Strongylocentrotus purpuratus. Four different concentrations of ZA and CA were tested: 1mM, 2mM, 3mM, and 4mM. Replicate dishes were set up for each concentration. Control dishes with just sperm and eggs were also set up. 1ml of a 2% egg solution in FSW was placed in each dish. ZA neutralized to pH 7.8 or CA neutralized to pH 7.6 was added to the dishes in appropriate volumes such that once the final volume of 5 ml was reached by adding FSW the desired concentration was established. Sperm were then added to the dishes at a 1/10,000 dilution. The solutions were stirred and the sperm and eggs were allowed to fertilize. Samples were removed from the dishes and examined under the microscope. The number of fertilized and unfertilized eggs were recorded to compare percent fertilization at the varying concentrations of the two compounds. These dose response experiments for ZA and CA were done twice with Strongylocentrotus purpuratus and also once with Litichinus pictus for ZA. A comparative analysis was done with Litichinus pictus and ZA, CA, and Heparin, to compare the effects on fertilization of a known compound such as Heparin with the compounds under study. All dishes were set up in replicates. Controls were set up with sperm (diluted 1/100,000), eggs (2% solution in FSW), and FSW for a final volume of 5 ml. The experimental dishes were set up similiarly except that they contained a final concentration of 3mM ZA, CA, or Heparin. Once the gametes were allowed to fertilize, samples were removed from the dishes and examined. The number of fertilized and unfertilized eggs were recorded to compare the variability in percent fertilization due to the effects of the different compounds. One last fertilization experiment was done to determine the mechanism by which zosteric acid inhibits fertilization. A protease was used to remove the vitelline layer of the unfertilized eggs to determine whether or not ZA was inhibiting fertilization by acting on the egg, as opposed to the sperm. In the control dishes, untreated eggs with intact vitelline layers were placed in 0 mM, 1mM, and 3 mM concentrations of ZA. The experimental dishes contained ZA at the same concentrations mentioned above with eg whose vitelline layers were removed. The vitelline layer of the eggs were removed by treating dejellied eggs with Protease (100 ug/1 ml egg solution) for 10 minutes. The eggs were then washed three times to remove excess Protease. Sperm (1/10,000 dilution) were added to the untreated and treated eggs. After four hours samples were removed and percent fertilization was recorded. The Protease treated eggs were checked for fertilization by observing for cleavage. RESULTS Chemotaxis Assay The chemotactic effects on the cypris larvae did not differ between the control and ZA experiments (fig. 1). The number of larvae was greatest in the 20-30 cm range (100% at time zero) and then evenly distributed among the 10- 20 cm and 30-40 cm sections and the 0-10 cm and 40-50 cm sections. Despite the ZA concentration gradient that was established after sixty minutes between sides #1 and #2 (2.05 mM and .004 mM respectively) the larvae swam evenly in both directions. Cyprid Motility The motility of the cyprids differed greatly between buffered and unbuffered ZA, CA, and sodium acetate. Regardless of which of the three compounds was assayed, the larvae were motile at pH 8 (tab. 1). At 8 mM ZA and above (pH 5.7 and below), the larvae were 100% reversibly immotile with appendages contracted upon contact. When placed in FSW, there was almost 100% recovery after 10 minutes. At 5 mM CA and above (pH 3.9 and below), the larvae were 100% irreversibly immotile upon contact, probably dead. In 10 mM sodium acetate (pH 5.7) the larvae were almost 100% reversibly immotile after 40 minutes. The acidity of the final solution differed between the same concentrations of the same compound depending on the molarity of the stock solution from which it was made. The above pH's were calculated after a 1:1 dilution of ZA or sodium acetate with FSW while CA dishes were all made from an 8 mM stock solution due to the compound’s low solubility in sea water. A solution buffered with MES (pH 5.6) or FSW titrated down to pH 5.2 did not cause larval immotility and in the control experiments (2 ml FSW) larvae were almost 100% motile. Barnacle Settlement Assay Figure 2 shows the dose-effectiveness of pH neutralized and unbuffered ZA against barnacle settlement. The error bars were determined by calculating the error (0) using the binomial distribution equation, o squared=npq, where n equals the total number of replicate experiments, p equals the fraction of larvae that settled, and q equals the fraction that didn’t. Four experiments were conducted in which there were more than 20 larvae in each petri dish. A stock solution of 20 mM ZA (pH 4.2-4.3) was used and then diluted to 0.05, 0.1, 1, 2, and 3 mM. The pH's of the final solutions were 8.0 in all buffered dishes and 6.5 to 7.6 for 3 mM unbuffered ZA, 7.8 to 7.9 for 2 mM, and 8.0 for 1 mM. pH neutralized and unbuffered percent settlement were similar at 1, 2, and 3 mM although buffered ZA (pH 8) was a slightly more powerful inhibitor than unbuffered ZA (pH 6.5 to 7.6) on average and at each concentration. Neither sodium acetate nor CA significantly inhibited settlement. Bacterial Attachment In the hemagglutination assay, the positive control tube containing Vibrio cholerae and red blood cells showed significant agglutination due to the attachment of bacteria (tab. 2). The negative control tube containing bacteria, red blood cells, and fucose, a known inhibitor of hemagglutination, showed no agglutination and the red blood cells were free of bacteria. The red blood cells in the other control wells containing red blood cells and either hypothetical inhibitor of bacterial attachment, fucose or zosteric acid, without bacteria were normal. The experimental tube containing bacteria, red blood cells, and 3mM zosteric acid showed agglutinated red blood cells with bacteria attached, just as in the positive control. The second assay showed a difference in the density of bacteria attached to the glass slides in response to the varying concentrations of zosteric acid in solution. Bacteria were counted from the photographs taken of the glass slides immediately after they were washed of excess unattached bacteria in SW. These numbers were then normalized to the control. Figure 3 shows a negative correlation between the concentration of zosteric acid and bacterial density. The lower concentrations (0.03 mM and 0.3 mM) of the zosteric acid seemed to have a small, yet noticeable effect on the density of attached bacteria by 18.2% and 24.3% respectively. The highest concentration of zosteric acid (3 mM) had a more significant effect in preventing bacterial attachment, decreasing the density of attached barnacles by 36.4%. Sea Urchin Fertilization In the dose response experiments with the Strongylocentrotus purpuratus, ZA decreased percent fertilization while CA did not. The mean fertilization rates for each concentration were normalized to the percentage of the control and plotted in Figure 4. The figure shows a negative correlation between the concentration of ZA and percent fertilization. The data at 2 mM, 3 mM, and 4 mM ZA dishes were statistically different from the control, having P values of 0.023, 0.006, and 0.00 respectively. The dose response experiment for ZA on Litichinus pictus showed a similiar negative correlation between increasing concentrations of ZA and percent fertilization. Figure 4 also shows the relationship between CA and fertilization in S. purpuratus. Increasing concentrations of CA have no statistically different effect on the percentage of eggs fertilized (P value: 0.147) as compared to the control. 10 The fertilization experiment comparing the effects of CA, Heparin, and ZA showed a variance in percent fertilization due to the effects of the different compounds. Figure 5 shows the effects of these compounds at 13 mMl on fertilization of L. pictus. CA decreased the percentage of fertilized eggs by 14.1% as compared to the control. Heparin decreased fertilization by 36.9% and ZA by 74.8%. Figure 6 shows the results of the Protease treatment experiment. 96.0% fertilization was observed in the control eggs with intact vitelline layers and no ZA. The ZA treated dishes suppressed fertilization by up to 83% as was seen in the previous dose response curves. In the experimental dishes containing the protease treated eggs, fertilization was not inhibited by ZA. DISCUSSION Although previous investigations (Todd et al., 1993) demonstrated that p-(sulphooxy) cinnamic acid inhibited settlement of competent cyprids of B. amphitrite the mechanism was unknown. A bioassay of chemotactic response to ZA in B. amphitrite was the first step in determining the compound's mode of action. Analysis of cyprid distribution in the chemotaxis assay indicated that ZA exhibited no chemotactic response. Because the larvae did not move in response to a concentration gradient of ZA, the compound does not appear to be chemorepellent to the cyprids and therefore does not inhibit settlement by deterrence. During this experiment it was observed that the larvae in the 0-25 cm range (those exposed to a much higher concentration of ZA) were noticeably less active than those in the 25- 50 cm range. A second possible mode of action for the inhibition of settlement by ZA was therefore hypothesized to be through effects on swimming behavior. If a 11 cyprid can not swim it will never find a suitable substrate on which to settle and will simply remain in the water column until it recovers or dies. A necessary distinction must be made between toxic and non-toxic compounds that cause immobility. Although both cause immobility, a narcotic effect was differentiated from a toxic one in that the former is reversible and the latter is not (Rittschof et al., 1992). The results from this assay indicate that at 8 mM ZA and 10 mM sodium acetate the larvae are 100% reversibly immotile and therefore inhibited from settling. The CA caused complete irreversible immotility at 5mM. This is clearly because CA is more acidic (pH 3.9) than both ZA and sodium acetate and too far from the pH of normal sea water for the larvae to survive. Because a FSW solution of pH 5.7 did not cause immobilization, acidic extracellular pH does not appear to be the sole component in producing this behavioral effect. ZA and sodium acetate may act as weak acids by partitioning across the cell membrane and changing intracellular pH. The uncharged species is present in higher concentrations as the pH decreases in approaching the pKa of a weak acid- 4.0 for ZA and 4.74 for sodium acetate. Therefore, the uncharged species is expected to cross the cell membrane and in this way could affect intracellular pH possibly resulting in larval immobility. Non-toxic antifoulers such as ZA seem to be more variable than toxic agents in their ability to inhibit settlement (Rittschof et al., 1992). Although high variability existed among the barnacle inhibition assays, it is apparent from Figure 2 that both buffered and unbuffered ZA inhibited settlement up to 30%. Because neither CA nor sodium acetate produced the same inhibitory effect, the mechanism by which ZA prevents settlement cannot be attributed to larval immobility in which all three compounds were effective. Therefore, larval settlement appears unrelated to external pH. However, this does 12 implicate a role for the sulfate moiety of ZA in inhibition of settlement which may be a key to the compound’s mode of action. The results of the hemagglutination assay showed no agglutination of the red blood cells in the negative control with fucose. In the experimental tube with the zosteric acid, agglutination was not prevented and bacteria attached to the red blood cells, as in the control. Therefore, the only conclusion that can be made is that ZA at a 3 mM strength does not prevent bacterial attachment in this assay. These results do not prove that ZA does not inhibit bacterial attachment, as can be seen in Figure 3. These results show that at a 3 mM concentration, ZA can suppress the attachment of bacteria onto glass surfaces by up to 40%. However, coumaric acid was also shown to suppress attachment by up to 50%. Because both ZA and CA seemed effective in suppressing the adherence of bacteria, it can be concluded that the sulfate group on ZA is not the portion of the compound necessary for inhibiting bacterial attachment. In the dose response experiments of ZA and CA with S. purpuratus and L. pictus, a negative correlation was observed between the concentration of ZA and percent fertilization. As the concentration of ZA increased, percent fertilization decreased. CA, however, did not show this effect. Because ZA, the sulphated phenolic ester, was effective and CA, the unsulfated analog of ZA, was not, it seems that the sulfate group may play a critical role in inhibiting fertiliation. The fertilization experiment with Heparin further supports this hypothesis that the sulfate moiety of ZA is a necessary component in inhibiting fertilization. Heparin was chosen for this experiment because it is a highly sulfated polysaccharide, known for its anticoagulant properties. Figure 5 shows that the fertilization inhibiting action of Heparin is intermediate to the effects of CA and ZA. CA is 13 unsulfated and has no effect in inhibiting fertilization. Heparin and ZA are similar in that they both significantly suppppress fertiliation and contain sulfate groups. There is evidence from the work of DeAngelis and Glabe (1987), that the egg surface ligands for bindin, a protein secreted from the acrosomal granule of sea urchin sperm that mediates the sperm’s adhesion to the egg, have been characterized as containing substantial amounts of carbohydrate and esterified sulfate. Because zosteric acid is a sulphated phenolic ester, it may be suppressing fertilization because it is similiar in structure to the egg surface ligands, thereby tying up sperm and preventing them from fertilizing. The Protease treatment experiment further elucidated the mechanism by which ZA inhibits fertilization. By removing the vitelline layer of the eggs with Protease, the egg receptors for the sperm were also removed. Figure 6 shows that ZA inhibits fertilization by up to 83.0% when using eggs with intact vitelline layers. It also showed that ZA lost its inhibitory effect on fertilization once the vitelline layer was removed. These results suggest that ZA inhibits fertilization by binding to the egg receptors on the vitelline layer. Once the vitelline layer is removed, the ZA can no longer bind to the egg receptors located on this layer and therefore can no longer shield it from sperm. The sperm can then freely swim to the plasma membrane, where other egg receptors may also be located, and fertilize. This assay therefore suggests that the vitelline layer and the receptors on it may be the critical components affected by ZA in the inhibition of fertilization. CONCLUSION The experiments conducted in this study show that zosteric acid produces a wide variety of effects: on barnacle behavior and settlement, 14 bacterial attachment, and sea urchin fertilization. The results from these experiments suggest that there may be more than one mode of action. Zosteric acid not only functions in both its buffered and unbuffered forms, but also as a sulfated compound and/or simply as a weak acid. Thus, multiple mechanisms seem to be involved, both individually and synergistically for an overall antifouling effect. REFERENCES Christie, A. O. and Dalley, R., 1987. Barnacle fouling and its prevention. Barnacle Biology, Crustacean Issues, 5, pp. 419-433. DeAngelis, P. L. and Glabe, C. G., 1987. Polysaccharide structural features that are critical for the binding of sulfated fucans to bindin, the adhesive protein from sea urchin sperm. The Journal of Biological Chemistry, Vol. 262, No. 29, pp. 13946-13952. Harrison, P. G., 1982. Control of microbial growth and of amphipod grazing by water-soluble compounds from leaves of Zostera marina. Marine Biology, Vol. 67, pp. 225. Maki, J. S., et. al., 1990. Effect of marine bacteria and their exopolymers on the attachment of barnacle cypris larvae. Bulletin of Marine Science, Vol. 46, No. 2, pp. 499-511. Pawlik, J. R., 1992. Chemical ecology of the settlement of benthic marine invertebrates. Oceanogr. Mar. Biol. Annu. Rev., 30, pp. 273-335. Rittschof, D., et. al., 1992. Barnacle in vitro assays for biologically active substances: toxicity and settlement inhibition assays using mass cultured Balanus amphitrite amphitrite Darwin. Biofouling, Vol. 6, pp. 115-122. Todd, J. S., Zimmerman, R. C., Crews, P., and Alberte, R. S., 1993. The antifouling activity of natural and synthetic phenolic acid sulphate esters. Phytochemistry, Vol. 34, No. 2, pp. 401-404. 15 gure 1. Lack of ZA Chemotaxis in Barnacle Larvae Figure 2. ZA Inhibits Barnacle Settlement Figure 3. ZA Effects Bacterial Attachment to Surface gure 4. ZA Inhibits Sea Urchin Fertilization Figure 5. Effects of CA, Heparin, and ZA on Sea Urchin Fertilization Figure 6. The Effect of the Vitelline Layer on ZA's Inhibition of Fertilization Table 1. Effects of ZA, CA, and Sodium Acetate on Cyprid Mobility Table 2. Hemagglutination Assay: Test for Bacterial Attachment + of Larvae 250 200 150- 100 Figure 1. .... 0-10 40-50 2.5 -1.5 ZA Concentration (mM) 0.5 10-20 20-30 30-40 Position in Trough (cm) ZA concentration (mM) of Larvae 140 120 - O 1004 80 O —— 60 O 40 0 88 20 Figure 2. -4- 2 Concentration (mM) 4 pH 8.0 unbuffered 100 80 .— 0 60 O 40 C •— 20 Figure 3. 1 3 ZA in mM 1004 75 50 25 8 CA 5 8 ZA 4 Concentration (mM Figure 4. + 100 80.0 60.0 400. 20.0- 0.0)+ Treatment (3 mM) contro Eca hep E Z4 Figure 5. 100.0 80.0 60.0 40.0 20.0 (0.0 + igure 6. ZA Concentration — protease treated untreated Table 1. Zosteric Acid Coumaric Acid Sodium Acetate Control-FSW Neutralized (pH 8) Motile Motile Motile Motile Unbuffered (pH) Immotile (5.7) Dead (3.9) Immotile (5.7) Motile (5.7) Table 2. Positive Control : Vibrio strain Red Blood Cells Negative Control : Vibrio strain Red Blood Cells Fucose Experimental : Vibrio strain Red Blood Cells Z4 Agglutination No Agglutination A lutination