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On the interaction of pure and impure supercritical CO2 with rock forming minerals in saline aquifers: An experimental geochemical approach

  • The aim of this experimental study was to evaluate and compare the geochemical impact of pure and impure CO2 on rock forming minerals of possible CO2 storage reservoirs. This geochemical approach takes into account the incomplete purification of industrial captured CO2 and the related effects during injection, and provides relevant data for long-term storage simulations of this specific greenhouse gas. Batch experiments were conducted to investigate the interactions of supercritical CO2, brine and rock-forming mineral concentrates (albite, microcline, kaolinite, biotite, muscovite, calcite, dolomite and anhydrite) using a newly developed experimental setup. After up to 42 day (1000 h) experiments using pure and impure supercritical CO2 the dissolution and solution characteristics were examined by XRD, XRF, SEM and EDS for the solid, and ICP-MS and IC for the fluid reactants, respectively. Experiments with mixtures of supercritical CO2 (99.5 vol.%) and SO2 or NO2 impurities (0.5 vol.%) suggest the formation of H2SO4 and HNO3, reflectedThe aim of this experimental study was to evaluate and compare the geochemical impact of pure and impure CO2 on rock forming minerals of possible CO2 storage reservoirs. This geochemical approach takes into account the incomplete purification of industrial captured CO2 and the related effects during injection, and provides relevant data for long-term storage simulations of this specific greenhouse gas. Batch experiments were conducted to investigate the interactions of supercritical CO2, brine and rock-forming mineral concentrates (albite, microcline, kaolinite, biotite, muscovite, calcite, dolomite and anhydrite) using a newly developed experimental setup. After up to 42 day (1000 h) experiments using pure and impure supercritical CO2 the dissolution and solution characteristics were examined by XRD, XRF, SEM and EDS for the solid, and ICP-MS and IC for the fluid reactants, respectively. Experiments with mixtures of supercritical CO2 (99.5 vol.%) and SO2 or NO2 impurities (0.5 vol.%) suggest the formation of H2SO4 and HNO3, reflected in pH values between 1 and 4 for experiments with silicates and anhydrite and between 5 and 6 for experiments with carbonates. These acids should be responsible for the general larger amount of cations dissolved from the mineral phases compared to experiments using pure CO2. For pure CO2 a pH of around 4 was obtained using silicates and anhydrite, and 7-8 for carbonates. Dissolution of carbonates was observed after both pure and impure CO2 experiments. Anhydrite was corroded by approximately 50 wt.% and gypsum precipitated during experiments with supercritical CO2 + NO2. Silicates do not exhibit visible alterations during all experiments but released an increasing amount of cations in the reaction fluid during experiments with impure CO2. Nonetheless, precipitated secondary carbonates could not be identified.show moreshow less

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Metadaten
Author:Franziska D. H. Wilke, Monica Vasquez, Thomas Wiersberg, Rudolf Naumann, Jörg Erzinger
DOI:https://doi.org/10.1016/j.apgeochem.2012.04.012
ISSN:0883-2927 (print)
Parent Title (English):Applied geochemistry : journal of the International Association of Geochemistry and Cosmochemistry
Publisher:Elsevier
Place of publication:Oxford
Document Type:Article
Language:English
Year of first Publication:2012
Year of Completion:2012
Release Date:2017/03/26
Volume:27
Issue:8
Pagenumber:8
First Page:1615
Last Page:1622
Funder:Federal Ministry of Education and Research [03G0671A-C]
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Erd- und Umweltwissenschaften
Peer Review:Referiert