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Aquatic Geochemistry (v.7, #1)
Mercury in the Tinto-Odiel Estuarine System (Gulf of Cádiz, Spain): Sources and Dispersion by D. Cossa; F. Elbaz-Poulichet; J. M. Nieto (pp. 1-12).
The Tinto and Odiel are small rivers draining one of the largest sulphide deposits in the world. As a result of these deposits and a large industrial complex, the adjacent marine area receives a high amount of metal input. Mercury distribution in the Tinto-Odiel estuary, the Huelva Ría and the Gulf of Cádiz was assessed in water and suspended particulatematter (SPM) and sediments. In the rivers and estuaries, dissolved (HgD)and particulate (HgP) mercury showed wide variations (13 to 200 pM and0.3 to 330 nmol g-1 respectively) depending on the presence or notof sulphidic waters, phosphogypsum deposits, detrital pyrite and oxyhydroxides.In the Ría, concentrations were lower than 10 pM and 4.5 nmol g-1 for HgD and HgP respectively. In surface waters of the Gulf of Cádiz, the average HgD concentration (pm standard deviation) was 2.9 pm 0.9 pM, which is similar to that of North Atlantic Central Waters. The surface sediments collected in the rivers, the Ría and the Gulf showed systematically enriched mercury compared to pre-industrial levels. Vertical mercury profiles in dated sediment cores were typical of anthropogenically influenced environments starting in the early Roman age. These distribution features suggest that most of the Hg discharged by the Huelva Ría is trapped in the sediments of the Gulf of Cádiz.
Keywords: mercury; Gulf of Cádiz; estuary; sulphide deposit; phosphogypsum
Surface Charge Concentrations on Silica in Different 1.0 M Metal-Chloride Background Electrolytes and Implications for Dissolution Rates by Magnus Karlsson; Colin Craven; Patricia M. Dove; William H. Casey (pp. 13-32).
The empirical rate laws formulated to describe the dissolution rates of oxide minerals include the surface charge concentration that results from the protonation and deprotonation of surface functional groups. Previous experiments on quartz and silica have shown that dissolution rates vary as a function of different background electrolyte solutions, however, such experiments are often conducted at elevated temperatures where it is difficult to estimate surface charge along with the dissolution rates. In the present study we measuresurface charge concentrations for silica in different electrolyte solutions at 298 K in order to quantify the extent to which the different counterions could affect the dissolution rates through their influence on the surface charge concentrations. The experimental solutions in the electrolyte series: LiCl, NaCl, KCl, RbCl, CaCl2, SrCl2 and BaCl2 were prepared to maintain a constant metal concentration of 1.0 M. For the alkali-metal chlorides, the surface charge concentrations correlate with the size of the hydrated alkali metal, consistent with the idea that these counterions affect charge via outer-sphere coordination that shield proton surface complexes from one another. The reactivity trend for alkaline-earth cations is less clear, but the data demonstrate distinct differences in the acid-base propertiesof the silica surface in these different electrolytes. We then discuss how these trends are manifested in the rate equations used to interpret dissolution experiments.
Keywords: oxide surface chemistry; dissolution kinetics; silica
Adsorption and Desorption of Phosphate on Calcite and Aragonite in Seawater by Frank Millero; Fen Huang; Xiaorong Zhu; Xuewu Liu; Jia-Zhong Zhang (pp. 33-56).
The adsorption and desorption of phosphate on calcite and aragonite were investigated as a function of temperature (5–45 °C)and salinity (0–40) in seawater pre-equilibrated with CaCO3. An increase in temperature increased the equilibrium adsorption; whereas an increase in salinity decreased the adsorption. Adsorption measurements made in NaCl were lower than the results in seawater. The higher values in seawater were due to the presence of Mg2+ and Ca2+ ions. The increase was 5 times greater for Ca2+ than Mg2+. The effects ofCa2+ and Mg2+ are diminished with the addition of SO4 2- apparently due to the formation of MgSO4 and CaSO4 complexes in solution and/or SO4 2- adsorption on the surface of CaCO3. The adsorbed Ca2+ and Mg2+ on CaCO3 (at carbonate sites) may act as bridges to PO4 3- ions. The bridging effect of Ca2+is greater than Mg2+ apparently due to the stronger interactions of Ca2+ with PO4 3-.The apparent effect of salinity on the adsorption of PO4 was largely due to changes in the concentration of HCO3 - in the solutions. An increase in the concentration of HCO3 - caused the adsorption of phosphate to decrease, especially at low salinities. The adsorption at the same level of HCO3 - (2 mM) was nearly independent of salinity. All of the adsorption measurements were modeled empirically using a Langmuir-type adsorption isotherm[ [PO4]ad = KmCm[PO4]T/(1 +Km [PO4]T) , ]where [PO4]ad and [PO4]T are the adsorbed and total dissolved phosphate concentrations, respectively. The values of Cm (the maximum monolayer adsorption capacity, (mol/g) and Km (the adsorption equilibrium constant, g/(mol) over the entire temperature (t, °C) and salinity (S) range were fitted to[ Cm = 17.067 + 0.1707t - 0.4693S + 0.0082S2 (σ = 0.7) ][ ln Km = - 2.412 + 0.0165t - 0.0004St - 0.0008S2 (σ = 0.1) ]These empirical equations reproduce all of our measurements of[PO4]ad up to 14 μmol/g and within ±0.7 μmol/g.The kinetic data showed that the phosphate uptake on carbonate minerals appears to be a multi-step process. Both the adsorption and desorption were quite fast in the first stage (less than 30 min) followed by a much slower process (lasting more than 1 week). Our results indicate that within 24 hours aragonite has a higher sorption capacity than calcite. The differences between calcite and aragonite become smaller with time. Consequently, the mineral composition of the sediments may affect the short-term phosphate adsorption and desorption on calcium carbonate. Up to 80 % of the adsorbed phosphate is released from calcium carbonate over one day. The amount of PO4 left on the CaCO3 is close to the equilibrium adsorption. The release of PO4 from calcite is faster than from aragonite. Measurements with Florida Bay sediments produced results between those for calcite and aragonite. Our results indicate that the calcium carbonate can be both a sink and source of phosphate in natural waters.
Impact of Ditching in a Small Forested Catchment on Concentrations of Suspended Material, Organic Carbon, Hydrogen Ions and Metals in Stream Water by Mats Åström; Eeva-Kaarina Aaltonen; Juhani Koivusaari (pp. 57-73).
Stream-water samples were collected during a 4-year-period in twosmall streams, one whose catchment was ditched for forestry halfway through the sampling period and another nearby reference stream whose catchment was not ditched during this period. The main aim was to study the impact of forest ditching on stream-water quality. Whereas the artificial drainage did not change the hydrograph pattern, it had a large effect on stream hydrochemistry: the concentrations of suspended material, Mn, Ca, Mg and Al increased, theconcentrations of total organic carbon decreased, and pH increased by approximately one unit, from an average of 4.4 to 5.4. The increase in suspended material, Mn and Al concentrations is explainedby the physical mobilisation of mineral particulates/colloids from mineral soils (till) exposed on the ditch slopes beneath the peat layer, while the increase in Ca and Mg loads is explained by the release of Ca2+ and Mg2+ in exchange reactions in this same soil layer. The increase in pH and decrease in TOC concentrations after ditching are related to changes in hydrological flow paths in the catchments, and most likely to immobilisation of both hydrogen ions and humic substances in the near neutral till horizon exposed beneath the peat layer. Only the aquatic abundance of Fewas not significantly affected by the ditching.
Keywords: stream; hydrochemistry; ditching; leaching; catchment; artificial drainage