Suitability of Existing Numerical Model Codes and Thermodynamic Databases for the Prognosis of Calcite Dissolution Processes in Near-Surface Sediments Due to a CO2 Leakage Investigated by Column Experiments     

Christoph Haase  Andreas Dahmke  Markus Ebert  Dirk Schäfer  Frank Dethlefsen 《Aquatic Geochemistry》2014,20(6):639-661

Among the risks of CO₂ storage is the potential of CO₂ leakage into overlaying formations and near-surface potable aquifers. Through a leakage, the CO₂ can intrude into protected groundwater resources, which can lead to groundwater acidification followed by potential mobilisation of heavy metals and other trace metals through mineral dissolution or ion exchange processes. The prediction of pH buffer reactions in the formations overlaying a CO₂ storage site is essential for assessing the impact of CO₂ leakages in terms of trace metal mobilisation. For buffering the pH-value, calcite dissolution is one of the most important mechanisms. Although calcite dissolution has been studied for decades, experiments conducted under elevated CO₂ partial pressures are rare. Here, the first study for column experiments is presented applying CO₂ partial pressures from 6 to 43 bars and realising a near-natural flow regime. Geochemical calculations of calcite dissolution kinetics were conducted using PHREEQC together with different thermodynamic databases. Applying calcite surface areas, which were previously acquired by N₂-BET or calculated based on grain diameters, respectively, to the rate laws according to Plummer et al. (Am J Sci 278:179–216, doi:10.2475/ajs.278.2.179, 1978) or Palandri and Kharaka (US Geol Surv Open file Rep 2004–1068:71, 2004) in the numerical simulations led to an overestimation of the calcite dissolution rate by up to three orders of magnitude compared to the results of the column experiments. Only reduction of the calcite surface area in the simulations as a fitting procedure allowed reproducing the experimental results. A reason may be that the diffusion boundary layer (DBL), which depends on the groundwater flow velocity and develops at the calcite grain surface separating it from the bulk of the solution, has to be regarded: The DBL leads to a decrease in the calcite dissolution rate under natural laminar flow conditions compared to turbulent mixing in traditional batch experiments. However, varying the rate constants by three orders of magnitudes in a field scale PHREEQC model simulating a CO₂ leakage produced minor variations in the pH buffering through calcite dissolution. This justifies the use of equilibrium models when calculating the calcite dissolution in CO₂ leakage scenarios for porous aquifers and slow or moderate groundwater flow velocities. However, the selection of the thermodynamic database has an impact on the dissolved calcium concentration, leading to an uncertainty in the simulation results. The resulting uncertainty, which applies also to the calculated propagation of an aquifer zone depleted in calcite through dissolution, seems negligible for shallow aquifers of approximately 60 m depth, but amounts to 35 % of the calcium concentration for aquifers at a depth of approximately 400 m.  相似文献   

Alteration and chemical U-Th-total Pb dating of heterogeneous high-uranium zircon from a pegmatite from the Aduiskii massif,middle Urals,Russia     

Zamyatin  Dmitry A.  Shchapova  Yuliya V.  Votyakov  Sergey L.  Nasdala  Lutz  Lenz  Christoph 《Mineralogy and Petrology》2017,111(4):475-497

Mineralogy and Petrology - The U-Th-Pb isotope system in the accessory mineral zircon may be disturbed, as for instance by the secondary loss of radiogenic lead. The recognition of such alteration...  相似文献   

Physical laboratory analyses of intergravel flow through brown trout redds (Salmo trutta fario) in response to coarse sand infiltration          下载免费PDF全文

Wolfgang Obruca  Christoph Hauer 《地球表面变化过程与地形》2017,42(4):670-680

In the spawning environment of salmonids, the quality of the intergravel flow is an essential abiotic requirement for the survival success of incubated embryos. As one of the most frequently investigated anthropogenic environmental impacts, the enhanced mobilization of fine sediments (<1 mm) and their entry into riverine ecosystems is considered as a major cause for the degradation of a variety of biological processes and habitats, including the spawning habitats of salmonids. In catchments draining crystalline bedrock, however, like the Bohemian Massif in the northern part of Austria, the excessive loading of river channels with coarse sand and fine gravel sediments (D = 1–10 mm) and less cohesive than fines is common as a consequence of altered catchment land use. Here, far less understanding exists of the mechanism and the possible implications of coarse sand infiltration on the functioning of the intergravel flow in salmonid redds. To investigate the intergravel flow hydraulics in response to coarse sand infiltration (D₅₀ = 2 mm) in brown trout spawning redds (Salmo trutta fario ) under controlled conditions, a laboratory flume experiment with three infiltration scenarios was conducted: (1) no infiltration; (2) segmental infiltration; and (3) full section infiltration. A more than two times drop in the average intergravel flow velocity was documented from scenario 1 (5.85 cms^?1) to scenario 2 (2.53 cms^?1) and another clear reduction was seen from scenario 2 (2.53 cms^?1) to scenario 3 (1.61 cms^?1). Moreover, in scenario 3, a clear reduction of the intergravel flow distance traveled was observed. Based on the findings we conclude that future considerations regarding the sustainable catchment management of salmonid fisheries should include programs to reduce not only the excessive entry of fines, but, in the relevant catchments, also the entry of excessive coarse sand into the riverine ecosystem. Copyright © 2016 John Wiley & Sons, Ltd.  相似文献   

Sediment budgeting of short-term backfilling processes: The erosional collapse of a Carolingian canal construction     

Johannes Schmidt  Lukas Werther  Johannes Rabiger-Völlmer  Franz Herzig  Birgit Schneider  Ulrike Werban  Peter Dietrich  Stefanie Berg  Sven Linzen  Peter Ettel  Christoph Zielhofer 《地球表面变化过程与地形》2020,45(14):3449-3462

Sediment budgeting concepts serve as quantification tools to decipher the erosion and accumulation processes within a catchment and help to understand these relocation processes through time. While sediment budgets are widely used in geomorphological catchment-based studies, such quantification approaches are rarely applied in geoarchaeological studies. The case of Charlemagne's summit canal (also known as Fossa Carolina) and its erosional collapse provides an example for which we can use this geomorphological concept and understand the abandonment of the Carolingian construction site. The Fossa Carolina is one of the largest hydro-engineering projects in Medieval Europe. It is situated in Southern Franconia (48.9876°N, 10.9267°E; Bavaria, southern Germany) between the Altmühl and Swabian Rezat rivers. It should have bridged the Central European watershed and connected the Rhine–Main and Danube river systems. According to our dendrochronological analyses and historical sources, the excavation and construction of the Carolingian canal took place in AD 792 and 793. Contemporary written sources describe an intense backfill of excavated sediment in autumn AD 793. This short-term erosion event has been proposed as the principal reason for the collapse and abandonment of the hydro-engineering project. We use subsurface data (drillings, archaeological excavations, and direct-push sensing) and geospatial data (a LiDAR digital terrain model (DTM), a pre-modern DTM, and a 3D model of the Fossa Carolina] for the identification and sediment budgeting of the backfills. Dendrochronological findings and radiocarbon ages of macro remains within the backfills give clear evidence for the erosional collapse of the canal project during or directly after the construction period. Moreover, our quantification approach allows the detection of the major sedimentary collapse zone. The exceedance of the manpower tipping point may have caused the abandonment of the entire construction site. The spatial distribution of the dendrochronological results indicates a north–south direction of the early medieval construction progress. © 2020 The Authors. Earth Surface Processes and Landforms published by John Wiley & Sons Ltd  相似文献