Investigation of Tributyltin (TBT) Affinity to Sediment Under Simulated Marine and Estuarine Conditions PDF Download
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Author: James Wilson
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Languages : en
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Author: James Wilson
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Languages : en
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Author: Edward D. Burton
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Category : Electronic dissertations
Languages : en
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Abstract: An improved understanding of the geochemical partitioning of trace metals and tributyltin (TBT) in sediments is of great importance in risk assessment and remedial investigation. The aim of this thesis was to examine the distribution and partitioning behaviour of trace metals and TBT in benthic, estuarine sediments. This was achieved by a series of field- and laboratory-based studies investigating factors controlling the geochemical behaviour of trace metals and TBT in sediments from south-east Queensland, Australia. The distribution and enrichment of selected trace metals in benthic sediments of the Southport Broadwater (a semi-enclosed coastal body of water adjacent to the Gold Coast city, south-eastern Queensland, Australia) was studied. Sediment contamination for Cd, Cr, Cu, Ni, Pb, Sn and Zn was assessed by (1) comparison with Australian sediment quality guidelines, (2) calculation of the index of geoaccumulation based on regional background values, and (3) geochemical noi-malisation against Al (i.e. the abundance of alumino-silicate clay minerals). Based on this approach, several sites were found to be strongly enriched with Cu, Pb, Sn and Zn, arising from sources related to either urban runoff or vessel maintenance activities. The geochemical partitioning of Cu, Pb and Zn was examined in sediments collected from three of these sites of sediment contamination. Total Cu, Pb and Zn concentrations in coarse-textured (65 to 90 % sand sized particles), sub-oxic sediments (Eh + 120 to +260 mV) ranged from 8.3 to 194 mg/kg for Cu, 16.3 to 74.8 mg/kg for Pb and 30.1 to 220 mg/kg for Zn, and were related to vertical trends in sediment texture. The association of Cu, Pb and Zn with amorphous oxides, crystalline oxides and organic matter was linearly dependent on the abundance of each phase. For retention by amorphous oxide minerals, the trace metal retention ranged from 5.2 to 23.7 mgcjgFe oxide as Fe for Cu, 1 2.8 to 21 .5 mgpb/gFe oxide as Fe for Pb, and 23. I to 85.7 mgm/gFe oxide as Fe for Zn. Corresponding values for association with crystalline oxides were an order of magnitude less than those for amorphous oxides, indicating a weaker affinity of trace metals for crystalline oxides. The relationships describing association with organic matter ranged from 17.6 to 54.0 mgcu/gorg c for Cu, 6.1 to 9.6 mgpb/gorg c for Pb and 6.4 to 16.4 mgzn/gorg c for Zn. The in-situ solid/pore-water partitioning of TBT and the degradation products, dibutyltin (DBT) and monobutyltin (MBT), was determined for an estuarine sediment profile with previously identified elevated Sn concentrations. Total butyltin levels were (depending on depth) 220 to 8750 jig/kg for TBT, 150 to 5450 jig/kg for DBT and 130 to 4250 jig/kg for MBT. Pore-water butyltin concentrations ranged from 0.05 to 2.35 jig/L for TBT, 0.07 to 3.25 jiglL for DBT, and 0.05 to 0.53 J.tgIL for MBT. The organic carbon normalised distribution ratios (Doc) were similar for TBT, DBT and MBT, and were io to 106 L/kg. Values for the Butyltin Degradation Index (BDI) were larger than I at depths greater than 10 cm below the sediment/water-column interface, indicating that substantial TBT degradation has occurred in the sediments. This suggests that natural attenuation may be a viable sediment remediation strategy. Factors controlling the partitioning behaviour of Cu, Pb and Zn in nonsulfidic, estuarine sediments were examined in controlled laboratory-based studies with the use of combined sorption curve - sequential extraction analysis. This allowed determination of sorption parameters for Cu, Pb and Zn partitioning to individual geochemical fractions. Partitioning behaviour in sulfidic sediments was also determined by sequentially extracting Cu, Pb and Zn from synthetic sulfide minerals, and from natural sediment and pure quartz sand after spiking with acid-volatile sulfide (AVS). Trace metal sorption to the 'carbonate' fraction (pH 5, NaOAc extraction) increased with metal loading due to saturation of sorption sites associated with the 'Fe-oxide' (NH2OH. HCI extraction) and 'organic' (H202 extraction) fractions in non-sulfidic sediments. Freundlich isotherm parameters describing sorption to the 'Fe-oxide' and 'organic' fractions were dependent on the sediment Fe-oxide and organic carbon content, respectively. Sequential extraction of Cu from pure CuS, AVS-spiked sediment and AVS-spiked quartz sand showed that AVS-bound Cu was quantitatively recovered in association with the 'organic' fraction. However, some AVS-bound Pb and Zn were recovered by the NH2OH. HCI step (which has been previously interpreted as 'Fe-oxide' bound metals) in the sequential extraction procedure used in this study. This indicates that the sequential extraction of Pb and Zn in sulfidic sediments may lead to AVS-bound metals being mistaken as Fe-oxide bound species. Caution should therefore be exercised when interpreting sequential extraction results for Pb and Zn in anoxic sediments. Tributyltin (TBT) sorption to four natural sediment samples in artificial seawater was also examined under a range of modified pH and salinity conditions in controlled laboratory-based studies. Three of the sediment samples were relatively pristine with regard to TBT contamination, but the fourth was a TBT-contaminated sediment from a commercial marina. Sorption of TBT was described well by linear sorption isotherms, with distribution coefficients ranging from 6.1 to 5210 L/kg depending on pH and salinity. Sediment organic C content and particle size distribution were important determinants of sorption behaviour. The presence of resident TBT in the contaminated marina sediment caused a substantial reduction in TBT sorption due to satuaration of high selectivity sites. Desorption of TBT from the marina sediment was described by relatively large observed distribution coefficients ranging from 5100 to 9400 L/kg, suggesting that aging effects may reduce sorption reversibility. Increased artificial seawater salinity generally reduced TBT sorption at pH 4 and pH 6, but enhanced TBT sorption at pH 8. Regardless of salinity, maximum sorption of TBT was observed at pH 6, which is attributed to an optimal balance between abundance of the cationic TBT species and deprotonated surface ligands. Consideration of aqueous TBT speciation along with octanol-water partitioning behaviour suggest that hydrophobic partitioning of TBTCI to non-polar organic matter was important for pH (up to) 6, whilst partitioning of TBTOH was important at higher pH. The effect of aging on the solid/pore-water partitioning and desorption behaviour of TBT in sediments was examined. Three sediment samples with contrasting physical and chemical properties were spiked with 10 mg/kg TBT and aged under sterile conditions for periods of time ranging from I to 84 days. Aging had a negligible effect in a sandy sample with very low organic carbon content (0.2 % w/w). In contrast, for samples with larger amounts of organic carbon (2.6 and 4.8 % w/w), the effect of aging on the solid/pore-water partitioning behaviour was significant. For these samples, the apparent distribution coefficients (Ks) obtained from sequential two hour desorption experiments exhibited a two-fold increase between spiked sediments subjected to aging for 1 day and 84 days. This study demonstrates that aging effects may be an important aspect of TBT fate in contaminated sediments. Overall, the results described in this thesis demonstrate that environmental factors (i.e. pH, salinity, Eh, aging) and sediment composition (i.e. abundance of fine alumino-silicate minerals, organic matter, Fe-oxides, reactive sulfides) exert substantial effects on trace metal and TBT partitioning. The current reliance on measurement of total trace metal and TBT concentrations in contaminated sediment management may consequently lead to inaccurate estimates of environmental risk and inappropriate remediation measures if other factors regulating contaminant distribution and partitioning are ignored.
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Languages : en
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Progress is reported in research dealing with the biogeochemical behavior of technetium in marine and estuarine ecosystems. Studies were planned to elaborate the biokinetic behavior of Tc as TcO4− in selected marine and estuarine organisms and to determine the affinity of TcO4− for different marine sediments under oxygenated conditions. It is concluded that concentration factors for TcO4− in bivalve molluscs (oysters and mussels) do not exceed 2 when calculated for whole animals and when uptake is directly from water. Direct uptake from water by limpets (archeogastropod) are very much lower than have been reported for red abalone (archeogastropod). Whole body concentration factors for TcO4− in the plaice, Pleuronectes platessa, where uptake is directly from labeled seawater, do not exceed 10 at equilibrium. Both the lobster, Homarus gammaris and the polychaete, Nereis diversicolor appear to concentrate Tc efficiently from water labelled intially with TcO4−. Both plaice and rays (Raja clavata) fed /sup 95m/Tc labeled Nereis show an initial rapid loss of the isotope for approximately five days. Thereafter, loss is much reduced. Shrimp (Palaemon elegans), Cragnon sp.) and Crab (Cancer pagurus) show concentration factors similar to plaice (C.F. is less than 10). Isopods, however, have concentration factors of only 3 following four weeks exposure to labeled seawater. Uptake of TcO4− by phytoplankton is extremely low, which precludes experiments in which TcO4− labeled phytoplankton can be fed to either bivalve molluscs or microzooplankton. Sediment distribution coefficients for TcO4− are essentially zero and are independent of sediment type in well oxygenated seawater. Experiments to date have shown that it is not possible to make generalizations concerning the bioavailability of TcO4− to marine organisms.
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Category : Environmental chemistry
Languages : en
Pages : 726
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Author: Allen P. Hennigar
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Category :
Languages : en
Pages : 18
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Author: Donna J. Westbrook
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Category : Tributyltin
Languages : en
Pages : 0
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This report presents data gathered in a program designed to monitor tributyltin (TBT) levels in water and sediment from areas in the southern Chesapeake Bay which experience high boating activities. The concentrations reported will hopefully give an insight into the extent and magnitude of TBT contamination in these areas.
Author: Graeme Batley
Publisher: CSIRO PUBLISHING
ISBN: 1486303862
Category : Science
Languages : en
Pages : 332
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Contaminated sediments represent an ongoing threat to the health of aquatic ecosystems. The assessment of sediment quality is, therefore, an important concern for environmental regulators. Sediment quality guidelines are now well established in regulatory frameworks worldwide; however, practical guidance that covers all of the key aspects of sediment quality assessment is not readily available. In 2005, CSIRO published its highly cited Handbook for Sediment Quality Assessment. In the ensuing period, the science has advanced considerably. This practical guide is a revised and much expanded second edition, which will be a valuable tool for environmental practitioners. Written by experts in the field, it provides coverage of: sediment sampling; sample preparation; chemical analysis; ecotoxicology; bioaccumulation; biomarkers; and ecological assessment. In addition, detailed appendices describe protocols for many of the tests to be used.
Author: Stephen de Mora
Publisher: Cambridge University Press
ISBN: 1108422373
Category : Business & Economics
Languages : en
Pages : 397
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A comprehensive, global review of the impact ships have on the environment, covering pollutant discharges, non-pollutant impacts and international legislation.
Author: Stuart L. Simpson
Publisher:
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Category :
Languages : en
Pages : 117
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Author: Frederick T. Short
Publisher: Univ of California Press
ISBN: 9780520240476
Category : Nature
Languages : en
Pages : 336
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Seagrasses are a vital and widespread but often overlooked coastal marine habitat. This volume provides a global survey of their distribution and conservation status.
