Abstract

Fractures in basalt can provide substantial surface area for reactions, and limited mass transfer in fractures can allow accumulation of cations to form carbonate minerals in geologic carbon sequestration. In this study, flood basalt and serpentinized basalt with engineered fractures were reacted in water equilibrated with 10MPa CO2 at 100°C or 150°C for up to 40 weeks. Carbonation in basalt fractures was observed as early as 6 weeks, with Mg- and Ca-bearing siderite formed in both basalts reacted at 100°C and Mg-Fe-Ca carbonate minerals formed in the flood basalt reacted at 150°C. X-ray μCT segmentation revealed that precipitates filled 5.4% and 15% (by volume) of the flood basalt fracture after 40 weeks of reaction at 100°C and 150°C, respectively. Zones of elevated carbonate abundance did not completely seal the fracture. Limited siderite clusters (<1% volume fraction) were found in localized areas in the serpentinized basalt fracture. A 1-dimensional reactive transport model developed in CrunchTope examined how geochemical gradients drive silicate mineral dissolution and carbonate precipitation in the fracture. The model predicts that siderite will form as early as 1day after the addition of CO2. The predicted location of maximum siderite abundance is consistent with experimental observations, and the predicted total carbonate volumes are comparable to estimates derived from CT segmentation.

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