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Fakultät für Biologie, Chemie und Geowissenschaften

Umweltgeochemie - Prof. Dr. Britta Planer-Friedrich

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Mehlhorn, J; Beulig, F; Küsel, K; Planer-Friedrich, B: Carbon dioxide triggered metal(loid) mobilisation in a mofette, Chemical Geology, 382, 54-66 (2014), doi:10.1016/j.chemgeo.2014.05.027
Abstract:

Carbon capture and geologic storage is a frequently discussed option to reduce atmospheric CO2 concentrations with the long-term risk of leakage from storage sites to overlying aquifers and soils. We chose natural CO2 exhalations, so-called mofettes, in a wetland area in the Czech Republic as analogues to follow the fate of metal(loid)s under CO2-saturated conditions. Compared to the reference fluvisol at the study site, mofette soils exhibited lower pH (4.9 ± 0.05) and redox potential (300 ± 40 mV), as well as higher organic carbon contents. Poorly crystalline and crystalline Fe (hydr)oxides, the most important metal(loid) sorbents in the CO2-unaffected soils (7.9 ± 5.9 g kg-1), showed significantly lower concentrations under the acidic and reducing conditions in the mofettes (1.2 ± 0.4 g kg-1). In turn, this increased the mobility of As and resulting concentrations were up to 2.5 times higher than in the CO2-unaffected pore water (58 ± 18 µg L-1). Methylation (up to 11 % of total As) and thiolation (up to 9 %) contributed to net As mobilisation. Dissolved Mn (131 ± 53 µg L 1), Ni (9.1 ± 3.1 µg L-1) and especially Cu (2.2 ± 1.0 µg L 1) concentrations remained low, likely due to complexation and/or adsorption to organic carbon and the small amount of Fe (hydr)oxides. A one-month-in-situ mobilisation experiment showed mobilisation of all investigated elements to the aqueous phase suggesting that desorption is the faster and initially dominating process while resorption is a secondary, slower process. We conclude that the CO2-induced mobilisation of toxic As and net-immobilisation of essential micro-nutrients (Mn, Ni, Cu) constitute serious risks and must be tested for transferability and relevance at geologic carbon storage sites.

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