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Aquatic Geochemistry (v.17, #3)

Physical Controls on Spatial Variability in Decomposition of Organic Matter in Lake Kinneret, Israel by Ami Nishri; Alon Rimmer; Udi Wagner; Zvi Rosentraub; Peter Yeates (pp. 195-207).

High resolution chemical data collected during summer 2003 indicate that the lower water mass (LWM) of the thermally stratified Lake Kinneret (LK) can be subdivided into three layers: a benthic boundary layer (BBL), overlain by the hypolimnion (HYP), and on top, the lower part of the metalimnion (ME-L). After onset of thermal stratification, the BBL is the first layer that turns anoxic, followed shortly afterward by the ME-L, while the HYP remains oxic and has relatively higher pH until later in summer. Thus, during the early summer, the HYP forms an oxygen-containing layer in-between two DO-deficient layers. Somewhat later, the HYP is characterized by still having significant levels of nitrate NO₃, while in both adjacent layers nitrate is already removed through denitrification. The mechanisms controlling the gradual decline of dissolved oxygen (DO) in the HYP during the summer were studied. The seasonal mean lake-wide vertical eddy diffusion coefficient in this layer, evaluated from heat flux measurements, is approximately 4 × 10⁻⁶ m² s⁻¹. The vertical oxygen flux due to diffusion from within the HYP toward its oxygen-deficient upper and lower boundaries accounts for most of the slow summer decline in DO in this layer. A smaller portion of this decline can be attributed to in-layer respiratory processes. The low turbidity, relatively high pH, and slow accumulation rate of NH₄ in the HYP support the notion that the slower mineralization processes occurring in this layer result from relatively low ambient concentrations of biodegradable organic matter, most probably due to the short residence time of the particles settling through this layer.

Keywords: Stratified Lake; Hypolimnion; Oxygen consumption; Degradation of organic matter

Impact of Alkaline Earth Metals on Aqueous Speciation of Uranium(VI) and Sorption on Quartz by Sreejesh Nair; Broder J. Merkel (pp. 209-219).

The effect of Mg-, Ca-, and Sr–Uranyl-Carbonato complexes with respect to sorption on quartz was studied by means of batch experiments with U(VI) concentration of 0.126 × 10⁻⁶ M in the presence and absence of Mg, Ca, and Sr (each 1 mM) at pH from 6.5 to 9. In the absence of alkaline earth elements, 90% of the U(VI) sorbed on the quartz surface at all pH. In the presence of Mg, Ca, and Sr, the sorption of U(VI) on quartz decreased to 50, 10, and 30%, respectively. Sorption kinetics of U(VI) on quartz is faster in the absence of alkaline earth elements and reached equilibrium after 12 h, whereas in the presence of Mg, Ca and Sr, the kinetics of U(VI) sorption on quartz is pH dependent and attained equilibrium after 24 h. Aqueous speciation calculations for alkaline earth uranyl carbonates were carried out by using PHREEQC with the Nuclear Energy Agency thermodynamic database (NEA_2007) by adding constants for MUO₂(CO₃) ₃ ²⁻ and M₂UO₂(CO₃) ₃ ⁰ (M = Ca, Mg, Sr). This study reveals that alkaline earth elements can have a significant effect on the aqueous speciation of U(VI) under neutral to alkaline pH conditions and subsequently sorption behavior and mobility of U(VI) in aqueous environments.

Keywords: Uranium(VI); Alkaline earth elements; Sorption; Alkaline earth uranyl carbonates; Quartz

Weathering regime associated with subsurface circulation on volcanic islands by Sétareh Rad; Karine Rivé; Claude Jean Allègre (pp. 221-241).

Volcanic islands, being characterized by highly porous basaltic/andesitic lava flows and pyroclastic deposits, are subject to important chemical weathering by subsurface waters. Moreover, such subsurface weathering is impacted by hydrothermal springs in both active and non-active volcanic areas, thus increasing dissolved load concentrations. Here, we focus on the subsurface water chemistry in the volcanic islands of the Lesser Antilles and Réunion and on the origin of these subsurface flows. We are able, through the use of various isotopic tools (C, Sr, U–Th), to identify hydrothermal influences in river water. For example, Li concentrations show a positive correlation with temperature of hot and cold springs and also a relationship with δ¹³C; from this, we can show that several sources of hydrothermal activity influence the rivers of the Lesser Antilles and that some rivers also reveal an important organic influence. As much as 20% of the subsurface hydrothermal springs go to feed the rivers. The increasing temperatures result in more dissolved elements being mobilized and an increase in chemical weathering rates. In addition, using the (²³⁰Th/²³⁸U) isochron for the well and river dissolved loads in Martinique, Guadeloupe and Réunion, we can evaluate residence times in the river water, i.e. the average residence time in the water along the circulation path to the sampling point. Alteration takes longer when the water circulates through thick soil, for example, 400–5,000 years when circulating under an ash profile and 1,200–15,000 years when circulating through a collapse zone. It would appear that waters circulation is globally three times longer for subsurface water than for surficial water. The weathering regime in tropical volcanic environments seems to be controlled mainly by such subsurface circulation with high chemical concentration from hydrothermal inputs. The origin of these compositions is varied and not controlled by a single hydrothermal spring. Consequently, it is subsurface circulation that determines the weathering regime in tropical volcanic islands with the main controlling parameters being temperature and residence time.

Keywords: Subsurface weathering; Hydrothermal springs; Volcanic islands; Residence time

Chemical and Strontium Isotopic Compositions of the Hanjiang Basin Rivers in China: Anthropogenic Impacts and Chemical Weathering by Zhifang Xu; Chao Shi; Yang Tang; Hongyin Han (pp. 243-264).

The Hanjiang River, the largest tributaries of the Changjiang (Yangtze) River, is the water source area of the Middle Route of China’s South-to-North Water Transfer Project. The chemical and strontium isotopic compositions of the river waters are determined with the main purpose of understanding the contribution of chemical weathering processes and anthropogenic inputs on river solutes, as well as the associated CO₂ consumption in the carbonate-dominated basin. The major ion compositions of the Hanjiang River waters are characterized by the dominance of Ca²⁺ and HCO₃ ⁻, followed by Mg²⁺ and SO₄ ²⁻. The increase in TDS and major anions (Cl⁻, NO₃ ⁻, and SO₄ ²⁻) concentrations from upstream to downstream is ascribed to both extensive influences from agriculture and domestic activities over the Hanjiang basin. The chemical and Sr isotopic analyses indicate that three major weathering sources (dolomite, limestone, and silicates) contribute to the total dissolved loads. The contributions of the different end-members to the dissolved load are calculated with the mass balance approach. The calculated results show that the dissolved load is dominated by carbonates weathering, the contribution of which accounts for about 79.4% for the Hanjiang River. The silicate weathering and anthropogenic contributions are approximately 12.3 and 6.87%, respectively. The total TDS fluxes from chemical weathering calculated for the water source area (the upper Hanjiang basin) and the whole Hanjiang basin are approximately 3.8 × 10⁶ and 6.1 × 10⁶ ton/year, respectively. The total chemical weathering (carbonate and silicate) rate for the Hanjiang basin is approximately 38.5 ton/km²/year or 18.6 mm/k year, which is higher than global mean values. The fluxes of CO₂ consumption by carbonate and silicate weathering are estimated to be 56.4 × 10⁹ and 12.9 × 10⁹ mol/year, respectively.

Keywords: Hanjiang River; South-to-North water transfer project; Sr isotopic ratio; Chemical weathering; CO₂ consumption

Modeling Geochemically Caused Permanent Stratification in Lake Waldsee (Germany) by Santiago Moreira; Bertram Boehrer; Martin Schultze; Severine Dietz; Javier Samper (pp. 265-280).

A geochemical model was incorporated into a stratification model for lakes to create the model package: DYCD-CORE, a numerical code that couples the thermal and hydrodynamic capabilities of DYRESM and the geochemical capabilities of the reactive transport model CORE2DV4. Based on the chemical composition of solutes calculated in each node for each time step, density was computed using specific partial molal volumes of all considered solutes and fed back into the stratification module of the program package. The density calculated each time step leads to a strong coupling of hydrodynamics and hydrogeochemistry and reflects the complex interaction as it is present in all lakes. To demonstrate the functionality of the numerical approach, an example of an iron-meromictic lake was chosen, where the reactivity of the dissolved iron kept the water body perennially stratified. To critically validate the model results, temperatures were continously measured at high vertical and temporal resolution in a field investigation of Waldsee (near Döbern, Germany). Multiparameterprobe profiles and water samples confirmed the continous chemical stratification and served as initial and boundary conditions for the simulation period. The model package DYCD-CORE could reproduce the permanent stratification as it were in the lake. A demonstration run using the standard UNESCO equation for density, and hence assuming non-reactive solutes, failed entirely. Hence, stratification models using salinity for density are not suited for simulating density created by lake-internal geochemical transformation of solutes. However, density can be based directly on the simultaneous numerical simulation of lake geochemistry. Predictive modeling of changing lake circulation in a variable climate or considering change of use will require a proper inclusion of the geochemistry as demonstrated in this paper.

Keywords: Meromictic lake; Stratification; Stability; Hydrodynamic model; Geochemical model

Interacting Effect of pH, Phosphate and Time on the Release of Arsenic from Polluted River Sediments (Anllóns River, Spain) by David A. Rubinos; Luz Iglesias; Francisco Díaz-Fierros; María Teresa Barral (pp. 281-306).

The interacting effect of pH, phosphate and time on the release of arsenic (As) from As-rich river bed sediments was studied. Arsenic release edges and kinetic release experiments (pH range 3–10), in the absence and presence of phosphate, coupled with sequential extraction procedures, SEM/EDX analyses and geochemical calculations, were carried out to evaluate As remobilisation and to elucidate the mechanisms involved. The results showed that As release underwent pronounced kinetic effects, which were strongly influenced by pH and phosphate. Remobilisation of As after 24 h was low (between ~1 and 5%) and varied slightly with pH, whereas alkaline conditions generally promoted As remobilisation after 168 h, with up to 12–21% of total As released. The results showed that depending on the pH and sediment considered, the release of As increased dramatically after ~48–72 h, suggesting that different processes are involved at different reaction periods. The addition of phosphate (1 mM) increased both the amount of As released (between 2 and 8 times) and the rate of As release from the sediments within the entire pH range (3–10) and period (168 h) studied. Moreover, in some cases, it also affected the shape of the As release edges and kinetic profiles. The similarities in the release profiles and the positive correlations between As and some sediment components, especially Fe and Al hydroxides, and organic matter—which appears to play a key role at high pH—suggest that As release from the studied sediments may be associated with solid phase dissolution processes under both acid and alkaline pH, whereas desorption plays a key role in the short term and at natural pH conditions, especially in the presence of phosphate, which acts as an As-displacing ligand. Evaluation of As mobility based on short-time leaching experiments may seriously underestimate the mobilisation of As from sediments.

Keywords: River; Sediment; Arsenic; Phosphate; Remobilisation; pH; Kinetics

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Aquatic Geochemistry (v.17, #3)

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Aquatic Geochemistry (v.17, #3)