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Institute
We performed leaching tests at elevated temperatures and pressures with an Alum black shale from Bomholm, Denmark and a Posidonia black shale from Lower Saxony, Germany. The Alum shale is a carbonate free black shale with pyrite and barite, containing 74.4 mu g/g U. The Posidonia shales is a calcareous shale with pyrite but without detectable amounts of barite containing 3.6 mu g/g U. Pyrite oxidized during the tests forming sulfuric acid which lowered the pH on values between 2 and 3 of the extraction fluid from the Alum shale favoring a release of U from the Alum shale to the fluid during the short-term and in the beginning of the long-term experiments. The activity concentration of U-238 is as high as 23.9 mBq/ml in the fluid for those experiments. The release of U and Th into the fluid is almost independent of pressure. The amount of uranium in the European shales is similar to that of the Marcellus Shale in the United States but the daughter product of U-238, the Ra-226 activity concentrations in the experimentally derived leachates from the European shales are quite low in comparison to that found in industrially derived flowback fluids from the Marcellus shale. This difference could mainly be due to missing Cl in the reaction fluid used in our experiments and a lower fluid to solid ratio in the industrial plays than in the experiments due to subsequent fracking and minute cracks from which Ra can easily be released.
Shrub encroachment has far-reaching ecological and economic consequences in many ecosystems worldwide. Yet, compositional changes associated with shrub encroachment are often overlooked despite having important effects on ecosystem functioning. We document the compositional change and potential drivers for a northern Namibian Combretum woodland transitioning into a Terminalia shrubland. We use a multiproxy record (pollen, sedimentary ancient DNA, biomarkers, compound-specific carbon (delta C-13) and deuterium (delta D) isotopes, bulk carbon isotopes (delta(13)Corg), grain size, geochemical properties) from Lake Otjikoto at high taxonomical and temporal resolution. We provide evidence that state changes in semiarid environments may occur on a scale of one century and that transitions between stable states can span around 80 years and are characterized by a unique vegetation composition. We demonstrate that the current grass/woody ratio is exceptional for the last 170 years, as supported by n-alkane distributions and the delta C-13 and delta(13)Corg records. Comparing vegetation records to environmental proxy data and census data, we infer a complex network of global and local drivers of vegetation change. While our delta D record suggests physiological adaptations of woody species to higher atmospheric pCO(2) concentration and drought, our vegetation records reflect the impact of broad-scale logging for the mining industry, and the macrocharcoal record suggests a decrease in fire activity associated with the intensification of farming. Impact of selective grazing is reflected by changes in abundance and taxonomical composition of grasses and by an increase of nonpalatable and trampling-resistant taxa. In addition, grain-size and spore records suggest changes in the erodibility of soils because of reduced grass cover. Synthesis. We conclude that transitions to an encroached savanna state are supported by gradual environmental changes induced by management strategies, which affected the resilience of savanna ecosystems. In addition, feedback mechanisms that reflect the interplay between management legacies and climate change maintain the encroached state.
Recultivation of disturbed oil sand mining areas is an issue of increasing importance. Nevertheless only little is known about the fate of organic matter, cell abundances and microbial community structures during oil sand processing, tailings management and initial soil development on reclamation sites. Thus the focus of this work is on biogeochemical changes of mined oil sands through the entire process chain until its use as substratum for newly developing soils on reclamation sites. Therefore, oil sand, mature fine tailings (MFTs) from tailings ponds and drying cells and tailings sand covered with peat-mineral mix (PMM) as part of land reclamation were analyzed. The sample set was selected to address the question whether changes in the above-mentioned biogeochemical parameters can be related to oil sand processing or biological processes and how these changes influence microbial activities and soil development.
GC-MS analyses of oil-derived biomarkers reveal that these compounds remain unaffected by oil sand processing and biological activity. In contrast, changes in polycyclic aromatic hydrocarbon (PAH) abundance and pattern can be observed along the process chain. Especially naphthalenes, phenanthrenes and chrysenes are altered or absent on reclamation sites, Furthermore, root-bearing horizons on reclamation sites exhibit cell abundances at least ten times higher (10(8) to 10(9) cells g(-1)) than in oil sand and MFF samples (10(7) cells g(-1)) and show a higher diversity in their microbial community structure. Nitrate in the pore water and roots derived from the PMM seem to be the most important stimulants for microbial growth. The combined data show that the observed compositional changes are mostly related to biological activity and the addition of exogenous organic components (PMM), whereas oil extraction, tailings dewatering and compaction do not have significant influences on the evaluated compounds. Microbial community composition remains relatively stable through the entire process chain. (C) 2014 Elsevier B.V. All rights reserved.
The study reported here evaluates the degree to which metals, salt anions and organic compounds are released from shales by exposure to water, either in its pure form or mixed with additives commonly employed during shale gas exploitation. The experimental conditions used here were not intended to simulate the exploitation process itself, but nevertheless provided important insights into the effects additives have on solute partition behaviour under oxic to sub-oxic redox conditions.
In order to investigate the mobility of major (e.g. Ca, Fe) and trace (e.g. As, Cd, Co, Mo, Pb, U) elements and selected organic compounds, we performed leaching tests with black shale samples from Bornholm, Denmark and Lower Saxony, Germany. Short-term experiments (24 h) were carried out at ambient pressure and temperatures of 100 degrees C using five different lab-made stimulation fluids. Two long-term experiments under elevated pressure and temperature conditions at 100 degrees C/100 bar were performed lasting 6 and 2 months, respectively, using a stimulation fluid containing commercially-available biocide, surfactant, friction reducer and clay stabilizer.
Our results show that the amount of dissolved constituents at the end of the experiment is independent of the pH of the stimulation fluid but highly dependent on the composition of the black shale and the buffering capacity of specific components, namely pyrite and carbonates. Shales containing carbonates buffer the solution at pH 7-8. Sulphide minerals (e.g. pyrite) become oxidized and generate sulphuric acid leading to a pH of 2-3. This low pH is responsible for the overall much larger amount of cations dissolved from shales containing pyrite but little to no carbonate. The amount of elements released into the fluid is also dependent on the residence time, since as much as half of the measured 23 elements show highest concentrations within four days. Afterwards, the concentration of most of the elemental species decreased pointing to secondary precipitations. Generally, in our experiments less than 15% of each analysed element contained in the black shale was mobilised into the fluid. (C) 2015 Elsevier Ltd. All rights reserved.
Soil degradation is a severe and growing threat to ecosystem services globally. Soil loss is often nonlinear, involving a rapid deterioration from a stable eco-geomorphic state once a tipping point is reached. Soil loss thresholds have been studied at plot scale, but for landscapes, quantitative constraints on the necessary and sufficient conditions for tipping points are rare. Here, we document a landscape-wide eco-geomorphic tipping point at the edge of the Tibetan Plateau and quantify its drivers and erosional consequences. We show that in the upper Kali Gandaki valley, Nepal, soil formation prevailed under wetter conditions during much of the Holocene. Our data suggest that after a period of human pressure and declining vegetation cover, a 20% reduction of relative humidity and precipitation below 200 mm/year halted soil formation after 1.6 ka and promoted widespread gullying and rapid soil loss, with irreversible consequences for ecosystem services.
Oxidation of particulate organic carbon (POC) during fluvial transit releases CO2 to the atmosphere and can influence global climate. Field data show large POC oxidation fluxes in lowland rivers; however, it is unclear if POC losses occur predominantly during in-river transport, where POC is in continual motion within an aerated environment, or during transient storage in floodplains, which may be anoxic. Determination of the locus of POC oxidation in lowland rivers is needed to develop process-based models to predict POC losses, constrain carbon budgets, and unravel links between climate and erosion. However, sediment exchange between rivers and floodplains makes differentiating POC oxidation during in-river transport from oxidation during floodplain storage difficult. Here, we isolated inriver POC oxidation using flume experiments transporting petrogenic and biospheric POC without floodplain storage. Our experiments showed solid phase POC losses of 0%-10% over similar to 10(3) km of fluvial transport, compared to similar to 7% to >50% losses observed in rivers over similar distances. The production of dissolved organic carbon (DOC) and dissolved rhenium (a proxy for petrogenic POC oxidation) was consistent with small POC lasses, and replicate experiments in static water tanks gave similar results. Our results show that fluvial sediment transport, particle abrasion, and turbulent mixing have a minimal role on POC oxidation, and they suggest that POC losses may accrue primarily in floodplain storage.
Rivers regulate the global carbon cycle by transferring particulate organic carbon (POC) from terrestrial landscapes to marine sedimentary basins, but the processes controlling the amount and composition of fluvially exported POC are poorly understood. We propose that hydrodynamic sorting processes modify POC fluxes during fluvial transit. We test this hypothesis by studying POC transported along a similar to 1,200 km reach of the Rio Bermejo, Argentina. Nanoscale secondary ion mass spectrometry revealed that POC was either fine, mineral-associated organic matter, or coarse discrete organic particles. Mineral-associated POC is more resistant to oxidation and has a lower particle settling velocity than discrete POC. Consequently, hydraulic sorting and downstream fining amplify the proportion of fine, mineral-associated POC from similar to 55% to similar to 78% over 1,220 km of downstream transit. This suggests that mineral-associated POC has a greater probability of export and preservation in marine basins than plant detritus, which may be oxidized to CO2 during transit.
Origin and migration of fluoride in the area of the Aluto Volcanic Complex (Main Ethiopian Rift)
(2022)
Fluoride-enriched ground and surface waters represent a major health risk for the local population in many areas along the East African Rift.
The present study investigates the origin of fluoride and the reason for its accumulation in the rift waters, following two hypotheses: (i) fluid-rock-interactions release fluoride from minerals into the water and (ii) magmatic-derived fluoride-containing liquids and gases migrate along permeable fault zones until they dissolve in ground-and surface water or be released to the atmosphere.
Rock-, gas, water-, soil-, and plant samples were collected from the area within and close by the Aluto Volcanic Complex, which is part of the Main Ethiopian Rift. Most analyzed waters showed fluoride concentrations above the drinking water limit (> 1.5 mg/L) with the highest values in hot springs (up to 70 mg/L) and the geothermal well (76 mg/L).
In the solid phase, a high fluoride content was found in acid volcanic rocks (ignimbrite: 4391 ppm; rhyolite: 3248 ppm) as well as in pumice (up to 1955 ppm). The fluoride content of soil samples collected within the volcanic complex varied between 82 and 1036 ppm, whereas former lake sediments from outside the Aluto Volcanic Complex showed higher fluoride contents ranging from 674 to 8171 ppm. Identified fluoride-rich minerals are various amphiboles (about 3 wt.-% F-), fluor-apatite (about 3 wt % F-), minerals of the fluorcaphite group (about 5 wt.-% F-), parisite (up to 9 wt.-% F-), and fluorite (CaF2).
Elevated fluoride concentrations were also measured in some gas samples from fumaroles (up to 50 ppm) and in plant samples collected next to the fumaroles (up to 65 ppm). Leaching experiments of solid samples with deionized water demonstrated that fluoride can easily be mobilized from pumice and sediments but hardly from consolidated rocks.
This fluoride release increased with temperature (up to 150 C) and correlated roughly with dis-solved silica indicating the binding of some fluoride to the amorphous or weakly crystalline silica fraction. Based on these results it was concluded that fluoride migrates via different pathways through the environment: At the depth of the magma chamber during magmatic differentiation fluoride enriches initially in the magmatic melt and accumulates in some late-crystallizing minerals of igneous rocks such as fluorite or mica. Upon volcanic eruption fluoride is predominantly incorporated in the glass (ignimbrite) and ash phase (pumice).
On the surface, these rocks are exposed to weathering and fluoride leaches partly out into the aqueous phase. Soft and porous rocks such as pumice release fluoride first whereas hard extrusive/igneous rocks are less prone to weathering and retain the fluoride. Pumice and (lake) sediments might act both, as source and as sink for fluoride in the area.
Although some fluoride might drain from the surface into the deeper subsoil, we conclude that magmatic fluids (liquid and gas) contribute more substantially to the overall fluoride ground water content because (i) of the much higher fluoride content in deep geothermal waters and hot springs as compared to surface-near waters; (ii) active geothermal surface manifestations located along fault zones indicate that fluids migrate from deep magmatic intrusions (as gas and liquid) towards the surface, where fluoride dissolves in groundwater; (iii) and the good correlation between bicarbonate (deriving from dissolution of magmatic CO2) and fluoride content in all analyzed water samples.