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Aquatic Geochemistry (v.5, #3)
Eh ph Diagrams for mn, fe, co, ni, cu and as Under Seawater Conditions: Application of two new Types of eh ph Diagrams to the Study of Specific Problems in Marine Geochemistry by Geoffrey P. Glasby; Horst D. Schulz (pp. 227-248).
EH pH diagrams have been calculated using the PHREEQC programme in order to establish the predominance fields of Mn, Fe, Co, Ni, Cu and As in bottom waters from the Angola Basin. Predominance fields are presented separately for both aquatic species and solid mineral phases in order to simplify interpretation of the data. The diagrams show significant differences from standard EH pH diagrams for these elements calculated for freshwater at 25 °C and 1 bar which assume an element concentration of 10-6 M. In particular, our diagrams show that Mn2+ and NiCO 3 0 are the predominant aquatic species for Mn and Ni in bottom seawater and FeOOH, Fe2O3, Fe3O4, CoFe2O4, CuFe2O4, CuFeO2, and Ba3 (AsO4)2 the predominant solid phases for Fe, Co, Cu and As, respectively. Mn and Ni are therefore undersaturated and Fe, Co, Cu and As supersaturated in bottom seawater from the Angola Basin. Neither rhodochrosite (MnCO3) nor siderite (FeCO3) can form in this marine environment in equilibrium with seawater. A mixed Mn-Ca carbonate is therefore formed within the pore waters of reducing sediments. The high Ni/Cu ratios in cobalt-rich manganese crusts formed adjacent to the oxygen minimum zone may be explained by the change from Cu2+ to CuCl 3 2- as the dominant aquatic species of Cu in seawater at an EH of +0.48 V.
Keywords: EH pH diagrams; seawater
Stable Sulfur Isotopic Evidence for Historical Changes of Sulfur Cycling in Estuarine Sediments from Northern Florida by Volker Brüchert; Lisa M. Pratt (pp. 249-268).
Data on abundance and isotopic composition of porewater and sedimentary sulfur species are reported for relatively uncontaminated and highly contaminated fine-grained anoxic sediments of St. Andrew Bay, Florida. A strong contrast in amount and composition of sedimentary organic matter at the two sites allows a comparative study of the historical effects of increased organic loading on sulfur cycling and sulfur isotopic fractionation. In the contaminated sediments, an increase in organic loading caused increased sedimentary carbon/sulfur ratios and resulted in higher rates of bacterial sulfate reduction, but a lower efficiency of sulfide oxidation. These differences are well reflected in the isotopic composition of dissolved sulfate, sulfide, and sedimentary pyrite. Concentration and isotopic profiles of dissolved sulfate, organic carbon, and total sulfur suggest that the anaerobic decomposition of organic matter is most active in the upper 8cm but proceeds at very slow rates below this depth. The rapid formation of more than 90% of pyrite in the uppermost 2 cm which corresponds to about 3 years of sediment deposition allows the use of pyrite isotopic composition for tracing changing diagenetic conditions. Sediment profiles of the sulfur isotopic composition of pyrite reflect present-day higher rates of bacterial sulfate reduction and lower rates of sulfide oxidation, and record a profound change in the diagenetic cycling of sulfur in the contaminated sediments coincident with urban and industrial development of the St. Andrew Bay area.
Keywords: sulfate; stable sulfur isotopes; delta 34S; porewaters; bacterial sulfate reduction; diffusion modeling; sulfide reoxidation; pyrite; anthropogenic effects; organic contamination; stable carbon isotopes; delta 13C; estuarine sediments; Florida; St. Andrew Bay; pulp mill effluent; lignin; lignocellulose
Biochelates as a Cause of Metal Cycling Across the Redoxcline by Rolf O. Hallberg; Carin Larsson (pp. 269-280).
The sharp concentration peak of the metals Cu, Cd and Zn at the redoxcline of the Framvaren Fjord, Norway, is described as an effect of chelation/complexation with organic ligands. The most dominating ligand is 2-mercaptobenzothiazole (MBT), which binds with a 2 : 1 ligand to metal stoichiometric ratio. MBT has the highest concentrations at the vicinity of the redoxcline where the oxidation of sulfide to elemental sulfur and sulfate is most extensive. We suggest the production being caused by sulfide oxidizing bacteria as we have not been able to detect MBT in pure cultures of sulfate reducing bacteria. Ni does not exhibit the same distribution as the other three metals due to lower preference for coordination with S and N donor atoms and a much lower rate for loss of water than Cu, Cd and Zn.
Keywords: metal chelation; redoxcline; sulfur bacteria; 2-mercaptobenzothiazole; benzothiazole
Chemical Composition and Geologic History of Saline Waters in Aux Vases and Cypress Formations, Illinois Basin by Ilham Demir; Beverly Seyler (pp. 281-311).
Seventy-six samples of formation waters were collected from oil wells producing from the Aux Vases or Cypress Formations in the Illinois Basin. Forty core samples of the reservoir rocks were also collected from the two formations. Analyses of the samples indicated that the total dissolved solids content (TDS) of the waters ranged from 43,300 to 151,400 mg/L, far exceeding the 35,400 mg/L of TDS found in typical seawater. Cl-Br relations suggested that high salinities in the Aux Vases and Cypress formation waters resulted from the evaporation of original seawater and subsequent mixing of the evaporated seawater with concentrated halite solutions. Mixing with the halite solutions increased Na and Cl concentrations and diluted the concentration of other ions in the formation waters. The elemental concentrations were influenced further by diagenetic reactions with silicate and carbonate minerals. Diagenetic signatures revealed by fluid chemistry and rock mineralogy delineated the water-rock interactions that took place in the Aux Vases and Cypress sandstones. Dissolution of K-feldspar released K into the solution, leading to the formation of authigenic illite and mixed-layered illite/smectite. Some Mg was removed from the solution by the formation of authigenic chlorite and dolomite. Dolomitization, calcite recrystallization, and contribution from clay minerals raised Sr levels significantly in the formation waters. The trend of increasing TDS of the saline formation waters with depth can be explained with density stratification. But, it is difficult to explain the combination of the increasing TDS and increasing Ca/Na ratio with depth without invoking the controversial ''ion filtration'' mechanism.
Keywords: Illinois Basin; Aux Vases; Cypress; saline formation waters; ion filtration; brine chemistry