Sulfide Binding Characteristics of.. Abstract The sulfide binding characteristics of blood serum were studied in¬ vitro in two deep-sea vesicomyid clams, Calyptogena pacifica and Vesicomya gigas. Both the C. pacifica and the V. gigas serum concentrated sulfide at least an order of magnitude above ambient levels. V. gigas accumulated sulfide faster than C. pacifica, reaching saturation at 5000 M after an hour. C. pacifica bound sulfide at half the rate of V. gigas, reaching saturation in about two hours at a substantially higher concentration of sulfide. The observed distribution of the animals near cold seeps in the Monterey Submarine Canyon can be explained by their different sulfide binding abilities. The hypothesis that cold seeps are actually much more unstable sources of sulfide than previously assumed is explored. Sulfide Binding Characteristics of. Introduction Calyptogena pacifica and Vesicomya gigas are members of the deep-sea clam family Vesicomyidae. Both burrow in the soft, sulfide-rich benthic substrate surrounding hydrothermal vents or cold seeps. In the last four years, they have been discovered in the Monterey Submarine Canyon near cold seeps between 550 and 900 meters depth. The large sulfur-rich gills of the animals contain intracellular symbiotic chemoautotrophic bacteria. The clams' feeding grooves and guts are simple and reduced in size, suggesting that they rely on nutritional supplements from their symbionts. This is corroborated by isotopically light carbon isotope levels, as are typical of chemosynthetically derived carbon (J. P. Barry, pers. comm.). The clams are oriented with their feet buried in the reducing substrate and their siphons exposed to the relatively sulfide-free bottom water. It has been hypothesized that they take up sulfide through the foot and obtain carbon dioxide and oxygen from overlying ambient seawater (Arp et al. 1984). This would require a system to transport the sulfide through the clams' circulatory system from the foot to the bacteria in the gills without poisoning the surrounding tissues or oxidizing the reduced, energy-rich form of sulfur. Sulfide, even at nanomolar concentrations, is a potent inhibitor of aereobic respiration through the cytochrome-c oxidase system (National Research Council 1979). Sulfide inhibition of cytochrome¬ c oxidase from the giant hydrothermal vent clam C. magnifica has been shown to be offset by the re-addition of the clam's blood to the system (Powell and Somero 1986), suggesting that the binding agents serve to protect the animals' tissues as well as provide Sulfide Binding Characteristics of.. sulfide for their symbionts. The circulatory systems of vesicomyid clams contain ample quantities of blood with hemoglobin containing red blood cells. Studies of C. magnifica and C. elongata have found a sulfide-specific binding moiety in the animals' blood serum (Childress et. al 1993, Arp et. al 1984); preliminary research on C. ponderosa and V. cordata indicates that their blood has a similar capacity for sulfide accumulation (Fisher 1990). I set out to explore the binding characteristics, over different concentrations and times of incubation, of C. pacifica and V. gigas blood serum. Materials and Methods Experimental Animals Organisms were collected using Monterey Bay Aquarium Research Institute’s (MBARI) remote operated vehicle RÖV Ventana from cold seep locations around the Monterey Canyon. Collection sites ranged from 550-900 meters in depth. The two clams studied, Vesicomya gigas and Calyptogena pacifica, are associated with sulfide-rich seeps. Animals were maintained from one to ninety days in 4° C reduced oxygen sea water at atmospheric pressure until they were sacrificed. Animal shells were scrubbed clean and shaken to evacuate water before dissection. All blood was aspirated in syringes, pooled, and stored at 4° C. Sample Preparation Initial studies concluded that whole blood and extracted serum displayed the same binding sensitivity, so experiments were Sulfide Binding Characteristics of. performed using clam serum. Whole blood was centrifuged for ten minutes at 62006. The serum was extracted and diluted ten fold with 0.2 um filtered, UV-sterilized sea water. The dilutions were then aliquoted in 1 ml quantities in dialysis membrane tubing (MWCO 12-14,000, Spectra/Por 42). All visible air bubbles were evacuated and both ends of the dialysis tubing were clamped. A 0.4 M hydrogen sulfide stock solution was made with de¬ oxygenated filtered sea water and sodium sulfide crystals. Ten percent HCI was added to re-establish a pH of 8. This stock was used for all subsequent working concentrations of sulfide. Sulfide Incubations For each measurement of sulfide binding as a function of external concentration, 750 ml of filtered sea water was bubbled with nitrogen for ten minutes to remove all oxygen. The appropriate amount of sulfide stock was then added to achieve the desired sulfide concentration. One dialysis bag each of C. pacifica and V. gigas dilute serum was added and the jars were sealed with Parafilm and screw caps. After at least six hours of incubation at 4° C, the serum samples and the dialysate were analyzed for sulfide content using a HP5890 Series II gas chromatograph modified for quantitation of dissolved gases in liquid samples (Childress et al., 1984) as descibed below. 250 ul of each sample was injected using a gas-tight syringe (Hamilton) into a heated, teflon-sealed, glass extraction chamber pre-loaded with dilute, gas stripped phosphoric acid and silicon anti-foam. As the sample entered the extraction chamber, dissolved carbonates (CO32“, HCO3-, H2CO3) and sulfides (82-, HS) were Sulfide Binding Characteristics of.. converted to CO2 and H2S (respectively), and were stripped, along with other dissolved gases (e.g. O2, N2, CH4, CO), by helium carrier gas flowing through the chamber. This gas mixure was then carried directly to a packed column (6' x 1/8” teflon-lined stainless steel, packed with Unibeads 1S 80/100) where CO2 and H2S were separated from the remaining gases, which passed through an automatically¬ actuated valve onto a second column (18' x 1/8" stainless steel, packed with Mol Seive 5A 60/80) for further separation. Upon elution from the columns, concentrations of all gases were determined using a thermal conductivity detector. To determine the time course of sulfide uptake, several serum samples from both species were placed in a 1-liter volume of 300450 UM sulfide solution. The dialysate was stirred continuously to ensure uniform sulfide distribution. At each time point, one pair of serum samples was removed and immediately placed in air tight syringes to prevent the sulfide from oxidizing. The initial and final dialysate and the samples were then analyized for sulfide content. Serum bound sulfide concentrations were calculated as follows: bound sulfide = (serum sample sulfide content - dialysate sulfide content) + 10 This compensated for both the ten fold dilution of blood serum and for the unbound sulfide present in the serum due to free diffusion across the dialysis membrane. Results Both the C. pacifica and the V. gigas serum concentrated sulfide substantially above ambient levels (Fig. 1). At low external sulfide concentrations (below 500 UM), all bound sulfide concentrations Sulfide Binding Characteristics of were at least an order of magnitude above the ambient levels. V. gigas appeared to reach saturation at about 5000 uM, but three outlying data points prohibit conclusive assertions. C. pacifica consistently bound higher levels of sulfide than V. gigas. Again, quantitative comparison between the two clams is difficult as there appear to be some outlying points. The range of external sulfide concentrations used in these trials may not have saturated the serum of C. pacifica, as the upward trend did not approach an asymptote similar to that evident in V. gigas. V. gigas accumulated sulfide faster than C. pacifica, but reached saturation at a lower sulfide concentration than C. pacifica (Fig. 2). V. gigas initially bound sulfide at a rate of 350 umolel serumemin¬ ', while C. pacifica concentrated it a little less than half the speed, at 156 umolsl serummin". V. gigas appeared to reach saturation at a concentration of approximately 5000 uM, which is consistant with the trend seen in the study of sulfide binding as a function of external concentration. Again, C. pacifica did not clearly reach saturation, as the serum sulfide concentrations at the highest external sulfide levels still show an upward trend. Discussion Sulfide binding in vesicomyid clams serves three vital functions. It prevents sulfide poisoning of aerobic metabolism, concentrates sulfide and transports it from the uptake site in the foot to the symbiotic bacteria in the gill, and preserves the most reduced, energy-rich form of sulfur by preventing the spontaneous oxidation of sulfide during transport. As animals sacrificed the day after collection displayed the same sulfide binding curve as those Sulfide Binding Characteristics of maintained for 90 days, I suggest that sulfide binding levels may be constitutive and species-specific rather than highly regulated, although this is certainly an area for further experimentation. The two aspects of sulfide binding discussed in this paper--absolute level bound and rate of binding--deserve further exploration. My data suggest that the blood of both species binds sulfide at least an order of magnitude above ambient levels. However, the two species differ considerably in binding characteristics. C. pacifica consistently bound more sulfide than V. gigas when both were allowed to reach equilibrium at comparable external sulfide concentrations. In situ, V. gigas inhabits areas of high sulfide concentration, while C. pacifica is more abundant at sites with lower sulfide levels (R. E. Kochevar, pers. comm.). As blood binding of sulfide may be an important defense against sulfide toxicity (Powell and Somero 1986), elevated sulfide levels may inhibit aerobic respiration in C. pacifica, while the lower sulfide levels on which C. pacifica thrives may not be sufficient for V. gigas to supply adequate sulfide to its symbionts. C. pacifica also survives better and longer in the laboratory. This may be partially linked to its ability to bind the lower levels of sulfide characteristic of aquarium maintenance. Saturation was evident in V. gigas after an hour and in C. pacifica after approximately two hours. Rate studies on the blood serum C. magnifica suggest that it binds sulfide more slowly than the C. pacifica and V. gigas. Arp et al. (1984) discovered that C. magnifca, which wedges its foot into hydrothermal vent fissures and is in close contact with warm, sulfide rich water, appears to accumulate sulfide in a linear fashion over at least 20 hours. Timed binding Sulfide Binding Characteristics of.. studies performed on the sulfide binding hemoglobin of the vestimentiferan Riftia pachytila suggest continuous sulfide accumulation until saturation, which occurs after about 16 hours (Arp and Childress 1983). The sulfide concentrations surrounding the animals are intermittant, but their vascular blood levels indicate that substantial quantities of sulfide are availible in their environments (Arp and Childress 1983). Sulfide binding rates in both Riftia and C. magnifica are an order of magnitude slower than the rates observed in C. pacifica and V. gigas. It has been assumed that the cold seep environment has a low, steady, continuous flow of sulfide in comparison to the concentrated, capricious sulfide in hydrothermal vents. In this scenario it seems that selection would favor high sulfide affinities with little regard for rapid binding rates. In light of the fact that the sulfide binding rates in C. pacifica and V. gigas are much higher than those of the aforementioned hydrothermal vent species, this may be called into question. One possible explanation of the fast binding rates of seep animals may be that the sulfide levels of cold seeps, as well as being lower than those of vents, are highly variable. Selective pressure would then favor clams that could concentrate sulfide in large quantities as quickly as possible. This reconsideration of the seep environment is supported by time lapse videos of clam fields in which it has been observed that occasionally, a patch of mud within a clam field will suddenly turn black and then fade to its normal color over several hours (J. P. Barry, pers. comm.). These data suggest that the cold seeps may be more dynamic systems then previously recognized. C. ponderosa and V. cordata are found associated with Sulfide Binding Characteristics of... hydrocarbon seeps in the Gulf of Mexico. Both animals leave characteristic trails of up to 205 cm (Rosman et al. 1987). It has been suggested that this burrowing behavior is necessary to provide a constant source of sulfide to the clams’ symbionts (Fisher 1990). As this foraging behavior is not evident in C. pacifica and V. gigas, the cold seeps must provide sufficient net amounts of sulfide, but sulfide levels may fluctuate considerably over short temporal scales. It is hypothesized that the distribution of C. pacifica and V. gigas may be in part controlled by their sulfide binding characteristics. The comparatively rapid sulfide binding evident in the clam serum suggests that the cold seeps may have ephemeral bursts of sulfide. This is a radical deviation from current dogma. Further observation of animals with chemotrophic symbionts in conjunction with studies of their environments may support the hypothesis that the sulfide binding characteristics of the animals may be indicative of the surrounding sulfide availibilities. Acknowledgements I would like to give a hearty thanks to all the people who made my research possible: Dr. Randy Kochevar, for his guidance, assistance, and patience Dr. Jim Barry and the crew of the Pt. Lobos and the RÖV Ventana for animal retrevial MBARI for facilities, reagents, and equipment Dr. Jim Watanabe for his tireless cheer and editing assistance and 10 Sulfide Binding Characteristics of. Connie Kim, Alan Lam, and Edwardo Martinez for their unflagging support. Sulfide Binding Characteristics of. Literature Cited Arp, A.J., J.J. Childress, and C.R. Fisher Jr. 1984. Metabolic and blood gas transport characteristics of the hydrothermal vent bivalve, Calyptogena magnifica. Physiological Zoology. 57:648-662. Arp, A.J. and J.J. Childress. 1983. Sulfide binding by the blood of the hydrothermal vent tube worm Riftia pachytila. Science. 219:295¬ 297. Childress, J.J., C.R. Fisher Jr., J.A. Favuzzi, A.J. Arp and D.R. Oros. 1993. The role of a zinc-based, serum-borne sulphide-binding component in the uptake and transport of dissolved sulphide by the chemoautotrophic symbiont-containing clam Calyptogena elongata. Journal of Experimental Biology. 179:131-158. Fisher, Charles R. Jr. 1990. Chemoautotrophic and methanotrophic symbioses in marine invertebrates. Reviews in Aquatic Sciences. 399-436. National Research Council: Hydrogen Sulfide. Baltimore: University Park Press 1979. (Committee on Medical and Biological Effects of Environmental Pollutants. Subcommittee on Hydrogen Sulfide: Division of Medical Sciences. Assembly of Life Sciences). Powell, M.A. and G.N. Somero. 1986. Adaptations to sulfide by hydrothermal vent animals: sites and mechanisms of detoxification and metabolism. Biological Bulletin. 171:274-290. Rosman, I., G.S. Boland and J.S. Baker. 1987. Epifaunal aggregations of Vesicomyidae on the continental slope off Louisiana. Deep-Sea Research. 34: 1811. Sulfide Binding Characteristics of. Figure Legends Figure 1: Serum bound sulfide as a function of external sulfide concentration Figure 2: Time dependence of sulfide binding. Experiment performed with dialysate concentration of 300450 UM sulfide solution. 15000 : 1oo00 5000 o C. pacifica A V. gigas o A A A 200 Figure 1 A A A A A 400 600 800 external sulfide concentration UM A 1000 8000 - 6000 4000 2000 A 32 -2000 - -4000 20 Ae A A 40 Figure 2 A e A C. pacifica A V. gigas m v 100 120 m mv time min