Abstract Flood basalts are receiving increasing attention as possible host formations for geologic sequestration of anthropogenic CO 2 , with studies underway in the U.S., India, Iceland, and Canada. Our previous laboratory studies with Columbia River basalts showed relative quick precipitation of carbonate minerals compared to other siliclastic rocks when batch reacted with water and supercritical CO 2 . In this study, our prior work with Columbia River basalt was extended to tests with basalts from the eastern U.S., India, and Africa. The basalts are all similar in bulk chemistry and share common minerals such as plagioclase, augite, and a glassy mesostasis. Single pass flow through dissolution experiments under dilute solution and mildly acidic conditions indicate similar cation release behavior among the basalt samples tested. Despite similar bulk chemistry and apparent dissolution kinetics, long-term static experiments with CO 2 saturated water show significant differences in rates of mineralization as well as precipitate chemistry and morphology. For example, basalt from the Newark Basin in the U.S. is by far the most reactive of any basalt tested to date. Carbonate reaction products for the Newark Basin basalt were globular in form and contained significantly more Fe than the secondary carbonates that precipitated on the other basalt samples. Calcite grains with classic “dogtooth spar” morphology and trace cation substitution (Mg and Mn) were observed in post-reacted samples associated with the Columbia River basalts. Other basalts produced solid precipitates with compositions that varied chemically throughout the entire testing period. Polished cross sections of the reacted grains show precipitate overgrowths with irregular regions outlined by dark and bright layers indicative of zonations of different compositions. Chemical differences in the precipitates indicate changes in fluid chemistry unique to the dissolution The Karoo basalt appeared the least reactive, with very limited behavior of each basalt sample reacted with CO 2 saturated water. mineralization occurring during the testing period. Additional experiments conducted using mixtures of H 2 S and CO 2 unexpectedly changed the relative reactivity of the basalts. For example, the Karoo basalt was highly reactive in the presence of aqueous dissolved H 2 S and CO 2 , evident by small nodules of carbonate coating the basalt grains after 181 days of testing. However the most reactive basalt in pure CO 2 , Newark Basin, formed limited amounts of carbonate in the presence of H 2 S. Basalt reactivity in pure CO 2 appears to be controlled by the glassy mesostasis chemistry, which is the most reactive component of basalt. With the addition of H 2 S, the reactivity appears to be controlled by precipitation of insoluble iron sulfides as coatings on the basalt grains.
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