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Biomedical subjects

Peter H Santschi

Publications and source records attributed to Peter H Santschi.

9 recordsLinked to original sources

Carbon isotopes and iodine concentrations in a Mississippi River delta core recording land use, sediment transport, and dam building in the river's drainage basin.

Sedimentary material from coastal and nearshore areas in the Mississippi Delta region are comprised of different organic carbon sources with diverse ages that require isotopic and elemental records for resolving the various sources of plant residues. Carbon isotopic ((13)C, (14)C) values were used to differentiate contributions from plants using the C3, C4, and/or CAM (crassulacean acid metabolism) carbon fixation pathways., and iodine concentrations indicated that wetland plant residues are a significant source of organic carbon in a sediment core from the Mississippi River delta region collected at a 60 m water depth. This sediment core had been extensively described in Oktay et al. [Oktay, S.D., Santschi, P.H., Moran, J.E., Sharma, P., 2000. The (129)Iodine Bomb Pulse Recorded in Mississippi River delta Sediments: Results from Isotopes of I, Pu, Cs, Pb, and C. Geochim. Cosmochim. Acta 64 (6), 989-996.] and significantly, includes unique features that had not previously been seen in the marine environment. These special features include a plutonium isotopic close-in fallout record that indicates a purely terrestrial source for these sediment particles and the elements associated with it, and a distinct iodine isotopic peak (as well as peaks for plutonium and cesium isotopes) that indicate little bioturbation in this core. Our carbon isotopic and iodine data can thus be compared to published records of changes in drainage basin land use, river hydrology, and hydrodynamic sorting of suspended particles to elucidate if these changes are reflected in nearshore sediments. This comparison suggests a significant contribution for organic carbon (OC) from C4 plants to these sediments during the 1950's to early 1960's. Relative older carbon isotopes, and episodically high iodine concentrations (up to 34 ppm) were observed during this time period that (1) indicate sediment deposition that is coincident with the times of major hydrological changes induced from dam and levee building in both the upper and lower reaches of the Mississippi River drainage basin, and (2) suggest episodic organic carbon deposition from wetland plant residues.

Carbon Isotopes↗

Relationship between carbonaceous materials and polychlorinated biphenyls (PCBs) in the sediments of the Danshui River and adjacent coastal areas, Taiwan.

Persistent organic pollutants, POPs (e.g., polychlorinated biphenyls) can seriously and deleteriously affect environmental quality and human health. These organic pollutants are exhibiting high affinities to solid phases and thus, quickly end up in sediments. To better understand the role of carbonaceous materials in the transport and distributions of POPs in terrestrial and near-shore environments, concentrations of PCBs and carbonaceous materials (including total organic carbon, black carbon and total carbohydrates), were determined in surface sediments of the Danshui River and nearby coastal areas, Taiwan. Total concentrations of PCBs in the sediments ranged from non-detectable to 83.9 ngg(-1), dry weight, with the maximum value detected near the discharge point of the marine outfall from the Pali Sewage Treatment Plant. These results suggest that the sewage treatment plant has discharged PCBs in the past and the concentrations are still high due to their persistence; alternatively, PCBs are still being discharged in the estuarine and near-shore environment of the Danshui River. Organic carbon and black carbon concentrations correlated well with those of total PCBs in the sediments, suggesting that both organic carbon and black carbon significantly affect the distribution of trace organic pollutants through either post-depositional adsorption, or by co-transport of similar source materials. The field results demonstrate that black carbon and plays an important role in the general distribution of PCBs, while concentrations of some specific PCBs are affected by both black carbon and organic carbon concentrations.

Carbohydrates↗

Plutonium from global fallout recorded in an ice core from the Belukha glacier, Siberian Altai.

Ice cores from glaciers situated near anthropogenic sources of air pollution provide important archives of the emissions of species with short atmospheric lifetimes. Here we present the history of atmospheric Pu fallout reconstructed from an ice core from the Belukha glacier in the Siberian Altai. Fourteen ice core samples covering the time period 1941-1986 were selected for Pu analysis, chemically processed, and measured using accelerator mass spectrometry. The Pu concentration peaks in 1963, coinciding with the maximum of the nuclear weapons tests and in concordance with the 3H activity concentration peak. The shapes of the 239Pu and 3H profiles reflect two main periods of atmospheric nuclear test activity: premoratorium testing before 1958 and postmoratorium testing in 1961 and 1962. Premoratorium tests contribute about 45% of the integrated Pu inventory. The average 240Pu/239Pu isotopic ratio is 0.18 +/- 0.05, indicating that a large majority of the Pu in the Belukha glacier originates from global stratospheric fallout rather than from direct tropospheric input.

Air Pollutants, Radioactive↗

Biogeochemical behavior of organic carbon in the Trinity River downstream of a large reservoir lake in Texas, USA.

Dissolved and particulate organic carbon concentrations were measured and annual loads estimated for the Trinity River, the main freshwater input source to Galveston Bay, which lies on the upper Gulf coast of Texas, USA, during 2000-2001. This river drains the forested lowlands south of a relatively large reservoir lake, Lake Livingston. A weak relationship between dissolved organic carbon (DOC) and Q(TR) indicated hydrologic control but separation of the data, based on individual discharge events, was necessary to improve interpretation. For instance, the first rain of the season resulted in only a modest increase in DOC concentrations and led to an inverse relationship with discharge, due to decreased lateral flow and increased infiltration of rainwater, with the lower flows being more efficient at DOC leaching from soils. In contrast, a long duration high discharge river crest event resulted in an opposite trend, i.e. a linear increase in DOC with increasing discharge rates. A short duration high discharge tropical storm showed reduced Trinity River DOC concentrations and the highest POC concentrations measured, likely resulting from the relatively short duration, and minimal contact time, of this event. In contrast to DOC, the concentrations of particulate organic carbon, POC (mg C l(-1)) were linearly correlated to suspended particulate matter (SPM) concentrations and accounted for between 10 and 12% of the total suspended load at low discharge but decreased to approximately 2% at high discharge. This suggests dilution by larger particles with a reduced organic carbon content, possibly silicate minerals, more readily resuspended at elevated levels of discharge. The annual total organic carbon (TOC) load to Galveston Bay, estimated from the slope of the daily load vs. discharge relationship, was 11.2 x 10(10) g C and calculated export coefficients (g C m(-2) year(-1)) were in good agreement with previous results. Using this relationship, accurate assessments of TOC flux inputs to Galveston Bay over the past quarter-century and in the future are possible by obtaining annual Trinity River discharge rates, which are readily available from the USGS. Comparing DOC riverine inputs to benthic sources in Trinity Bay, measured directly on the same day, indicates that the sediments contribute approximately 20% of total inputs of DOC to Trinity Bay. However, assuming a constant benthic source during low-flow conditions, which can occur for periods of up to 14 months in this region of Texas, benthic fluxes would account for > 80% of the total inputs into Trinity Bay. At high levels of discharge, the Trinity River discharges approximately 1.0 x 10(9) g C day(-1) and dominates DOC inputs to Trinity Bay.

Carbon↗

129I/(127)I as a new environmental tracer or geochronometer for biogeochemical or hydrodynamic processes in the hydrosphere and geosphere: the central role of organo-iodine.

Iodine is a biophilic element, with several short-lived isotopes (e.g. (131)I, t(1/2)=8 days), one long-lived isotope, (129)I (t(1/2)=15.6 million years) and one stable isotope, (127)I. The inventory of (129)I in surface environments has been overwhelmed by anthropogenic releases over the past 50 years. Iodine and its isotopes are important for a number of reasons: (1) The largest fraction of the short-term and long-term dose from accidental releases and fallout from atomic bomb tests was from iodine isotopes. (2) (129)I is one of the two long-lived nuclides with highest mobility in stored radioactive waste. (3) (129)I could provide the scientific community with a new geochemical tracer and new geochronological applications in environmental science. (4) A better assessment of iodine deficiency disorders, mineralization in exploration geochemistry, and the transfer of volatile organic greenhouse-active and ozone-destroying iodine species from the oceans to the atmosphere is needed. One of the most promising future applications for the (129)I/(127)I ratio is not only as a new geochronometer, but also as a new source tracer for terrestrial organic matter with ages of 50 years or less. This is especially attractive, since radiocarbon can be, at times, an ambiguous chronometer for the 50-year time-scale, whereas (129)I concentrations during this time are overwhelming previous levels by orders of magnitude. Iodine is to a significant extent involved in the cycle of organic matter in all surface environments. Its biophilic nature is demonstrated by a relative enrichment of iodine in seaweed and dissolved macromolecular organic matter. Because of the close coupling of iodine and organic carbon cycles, our understanding of the underlying molecular mechanisms of the processes regulating iodination reactions in aquatic systems is still limited. The binding of iodine by organic matter has the potential to modify the transport, bioavailability and transfer of iodine isotopes to man. Equilibration times for (129)I in many reservoirs are likely long enough that (129)I could be used as a new source tracer for organic matter of terrestrial origin, and as a geochronometer. Current tracer applications of (129)I are limited by our knowledge of the effects of UV-radiation, microbial activity and geochemical redox conditions on organo-I compounds and overall iodine speciation. The biogeochemical behavior of iodine and its isotopes appears to be different in North America and European waters, possibly due to climatic, source and speciation differences.

Environmental Monitoring↗

Inverse dependency of particle residence times in ponds to the concentration of phosphate, the limiting nutrient.

234Th, a commonly used short-lived particle-reactive tracer in marine systems, was measured in three different holding pond series at the Rocky Flats Environmental Technology Site (RFETS), Colorado, along with its parent nuclide 238U, to determine steady-state residence times of particle-reactive actinides such as Pu, and of particles. Series B ponds, which received industrial effluent that includes ortho-phosphate (PO4) and actinides, differed from series A and C ponds, which did not. This difference was also evident in the calculated particle residence times, which were <1 day for the ponds B4 and B5, where PO4 concentrations were higher (1.4 and 1.8 mg/l), and 3 and 3.4 days for ponds A3 and C2, respectively, where ortho-phosphate concentrations were lower (<0.1 mg/l). Particle residence times thus showed an inverse relationship with the concentration of ortho-phosphate, the limiting nutrient in fresh water systems. The same relationship to the concentration of ortho-phosphate or any of the other nutrient elements was not evident for the residence times of dissolved 234Th, which ranged between 0.1 and 2 days. This can be attributed to higher concentrations of dissolved and particulate ligands with greater binding potential for actinides such as four-valent Th and Pu in ponds with higher ortho-phosphate concentrations. Regardless of actual ortho-phosphate concentration, however, at water residence (holding) times of 1 month in these ponds, particles and associated actinides would be expected to be completely removed from the pond water to sediments.

Adsorption↗

Organic nature of colloidal actinides transported in surface water environments.

Elevated levels of (239,240)Pu and 241Am have been present in surficial soils of the Rocky Flats Environmental Technology Site (RFETS), CO, since the 1960s, when soils were locally contaminated in the 1960s by leaking drums stored on the 903 Pad. Further dispersion of contaminated soil particles was by wind and water. From 1998 until 2001, we examined actinide ((239,240)Pu and 241Am) concentrations and phase speciation in the surface environment at RFETS through field studies and laboratory experiments. Measurements of total (239,240)Pu and 241Am concentrations in storm runoff and pond discharge samples, collected during spring and summer times in 1998-2000, demonstrate that most of the (239,240)Pu and 241Am transported from contaminated soils to streams occurred in the particulate (> or = 0.45 microm; 40-90%) and colloidal (approximately 2 nm or 3 kDa to 0.45 microm; 10-60%) phases. Controlled laboratory investigations of soil resuspension, which simulated storm and erosion events, confirmed that most of the Pu in the 0.45 microm filter-passing phase was in the colloidal phase (> or = 80%) and that remobilization of colloid-bound Pu during soil erosion events can be greatly enhanced by humic and fulvic acids present in these soils. Most importantly, isoelectric focusing experiments of radiolabeled colloidal matter extracted from RFETS soils revealed that colloidal Pu is in the four-valent state and is mostly associated with a negatively charged organic macromolecule with a pH(IEP) of 3.1 and a molecular weight of 10-15 kDa, rather than with the more abundant inorganic (iron oxide and clay) colloids. This finding has important ramifications for possible remediation, erosion controls, and land-management strategies.

Actinoid Series Elements↗

Metal partitioning between colloidal and dissolved phases and its relation with bioavailability to American oysters.

Kinetics and the extent of metal partitioning between colloidal and dissolved phases and coagulation of metals associated with colloids were examined to determine their effects on the bioavailability of selected metals (Cd, Co, Hg, Ag, Fe, and Zn) to American oysters (Crassostrea virginica) using radiotracer and short term exposure experiments. After dispersion of radiolabeled colloids into low molecular weight (LMW, < 1 kDa) seawater, metal partitioning between dissolved (<1 kDa) and colloidal (1 kDa-0.2 microm) phases resulted in a consistent pattern, with a relatively constant percentage in the colloidal phase for each metal. On average, about 90% of Hg and Fe, approximately 60% of Ag and approximately 40% of Zn, Co, and Cd were measured in the colloidal fraction during a short term exposure experiment, consistent with their partitioning in natural waters. Controlled laboratory experiments carried out in parallel using radioactively tagged colloids showed that coagulation of colloidal species, quantified as the fraction retained by a 0.2 microm filter, was insignificant for most metals under the conditions and time periods of the uptake experiments. The bioavailability of colloidally complexed metals, measured in terms of dry weight concentration factor (DCF, ml g(-1)) and uptake rate constant (ml g(-1) h(-1)), was somewhat depressed compared with their counterpart in the LMW treatment, but could be well predicted from the results of the LMW treatment and metal partitioning. Both DCF values and uptake rate constants were higher in the LMW treatment than in the colloidal treatment. In addition, B-type metals, such as Ag, Hg, and Zn, all had higher values of DCF and uptake rate constants, regardless of treatments, except for Cd which had a lower DCF and uptake rate constant. In contrast, Co and Fe had significantly lower DCF values and uptake rate constants. Most of Hg and Ag (60-80%) were measured in the soft tissue of oysters in both LMW and colloidal treatments. In contrast, 80% of Fe, 75% of Co, and approximately 60% of Cd were observed on the shell, while Zn was found evenly distributed between shell and soft tissue of oysters. These results agree well with the variation pattern of both DCF value and uptake rate constant for these two groups of metals.

Animals↗

Silver concentrations in Colorado, USA, watersheds using improved methodology.

River water samples were collected at five sites in the state of Colorado, USA, to assess the impact of municipal and industrial discharges on Ag concentrations and speciation in surface waters. Samples were collected and analyzed for total (unfiltered collections), filtered (0.1 and 0.4 microm), particulate (> or = 0.45 microm), and colloidal Ag (3 kDa-0.1 m) using ultraclean protocols. A series of laboratory experiments were conducted to assess bias from sample storage, digestion, and preconcentration protocols. In general, upstream unfiltered and particulate Ag concentrations fell within a fairly narrow range, 3.1 to 21 ng/L and 0.2 to 1.7 microg/g, respectively. Downstream unfiltered and particulate Ag concentrations showed a more broad range, 2.8 to 1,110 ng/L and 0.5 to 104 microg/g, respectively, and reflected attenuated impacts of Ag-laden discharge effluents. However, Ag concentrations in the 0.1-microm filter-passing fraction 0.8 to 1.2 km downstream from major treatment plant effluents were all below the chronic silver criteria. On average, more than 60% of the 0.1-microm filter-passing Ag was associated with colloidal macromolecular organic matter. Silver concentrations in colloids (microg/g) were, on average, the same as those in suspended particulate matter. The percentage abundance of colloidal Ag was similar to that of dissolved organic carbon, suggesting that strong Ag binding ligands exist in both the colloidal and the particle size fractions, as these macromolecular ligands likely play a major role in Ag speciation.

Chemical Industry↗