Hematite reactivity with supercritical CO2 and aqueous sulfide

Hematite nanoparticles were reacted in a solution containing sulfide in contact with supercritical CO2, to simulate conditions relevant to carbon dioxide sequestration in the Earth's subsurface. X-ray diffraction was used to identify reaction products. Rietveld analysis of the X-ray diffractograms and thermogravimetric analysis were used to estimate the amounts of reaction product formed. Under the experimental conditions used (70 °C), a near equimolar amount of siderite (FeCO3) and pyrite (FeS2) formed. The equimolar amounts of pyrite and siderite products were consistent with the stoichiometry associated with the following overall reaction, 2Fe3+ + 2S2− + CO32– → FeS2 + FeCO3.In situ infrared spectroscopy suggested that the conversion of the hematite was rapid and largely occurred within 4 h at 70 °C. Analysis of the reaction product with electron microscopy showed the presence of framboidal pyrite and rhombohedral siderite particles that were micron-sized. The observed morphologies suggest that the transformation from hematite to siderite occurred via a dissolution–reprecipitation reaction.

Research highlights
► Hematite reacts with sulfide to form siderite and pyrite.
► Siderite and pyrite form in equal amounts.
► TGA is used to identify siderite and pyrite.