Abstract

Improving our ability to predict the interactions between CO₂ and reservoir rocks at geological time scales is of key importance if carbon capture and storage (CCS) is to have a role in climate-change mitigation, particularly in the light of likely regulatory requirements. Understanding and identifying the relevant geological processes over long time scales can be obtained only at natural-analogue sites. At one such site, in the Salt Wash Graben area of Utah, USA, widespread bleaching affects the Middle Jurassic red-bed “wet dune” Entrada Sandstone. Previous work has proposed a genetic link between the bleaching and spatially concomitant recent and modern CO₂-rich fluids. The results presented here challenge some of the previous models and come from a detailed petrographic examination of mineralized fractures in the Entrada Sandstone that are centered in vertical extensions to the bleaching. These fractures typically contain complex mineralization assemblages. Pyrite was a paragenetically early phase, identifiable from common pseudomorphs of mixed iron oxides and oxyhydroxides that rarely contain relict pyrite. The pyrite contains up to 3 wt% arsenic. The volume of fracture-adjacent bleached sandstone is sufficient to have been the source of iron for the pyrite originally present in the fracture. The pyrite pseudomorphs occur at the center of fracture- and pore-filling cements that comprise intergrowths of hematite–goethite–jarosite–gypsum, an assemblage that suggests that their formation resulted from the oxidative alteration of pyrite, a genetic link supported by the arsenic present in the iron-bearing minerals. The presence of jarosite and proximal removal of earlier, sandstone-hosted carbonates are consistent with, and indicative of, the low-pH conditions associated with pyrite oxidation reactions. Calcite- and gypsum-cemented fractures crosscut, and contain fragments of, the pyrite-pseudomorphic and -oxidation assemblages, proving that they postdate pyrite formation and its subsequent oxidation, and that pyrite oxidation was not a result of modern weathering reactions. In outcrop, some calcite- and gypsum-cemented fractures link with travertine deposits associated with the modern and recent CO₂-rich fluids. The mineral assemblages observed here, and the paragenetic sequence that we have inferred, suggest that the fracture-associated bleaching patterns result from the fracture-fed movement of sulfur-bearing reducing fluids, with hydrogen sulfide the most likely bleaching agent. We conclude that bleaching adjacent to fractures is not genetically related to modern CO₂-bearing fluids despite the spatial relationship. The bleaching was already present when the modern fluids utilized the same fracture-based fluid pathways. We suggest that the more widespread regional bleaching formed contemporaneously with the fracture bleaching and followed similar mechanisms. This study highlights the complexity of interpreting analogue sites and the importance of using field and petrographic observations to unravel textures and events that are juxtaposed spatially but not temporally.