Mineralization of Basalts in the CO2–H2O–SO2–O2 System

• Published in: Environmental science & technology Vol. 48; no. 9; pp. 5298 - 5305
• Main Authors: Schaef, Herbert T, Horner, Jake A, Owen, Antoinette T, Thompson, Chris J, Loring, John S, McGrail, Bernard P
• Format: Journal Article
• Language: English
• Published: Washington, DC American Chemical Society 06-05-2014
• Subjects: Carbon Dioxide - chemistry; Climatology. Bioclimatology. Climate change; Earth, ocean, space; Exact sciences and technology; External geophysics; Mass Spectrometry; Meteorology; Minerals - chemistry; Oxygen - chemistry; Silicates - chemistry; Spectrophotometry, Infrared; Sulfur Dioxide - chemistry; Water - chemistry; X-Ray Diffraction; Sulfur compounds; Laboratory study; Co-contaminant; volcanic rocks; Carbon dioxide; CO2 sequestration; Geological formation; igneous rocks; fluid injection; Supercritical state; Carbon sequestration; Sulfur dioxide; greenhouse gas; sustainable development; Mitigation; Geoengineering; basalts; Carbonation; climate change
• ISSN: 0013-936X; 1520-5851
• DOI: 10.1021/es404964j

Sequestering carbon dioxide (CO2) containing minor amounts of co-contaminants in geologic formations was investigated in the laboratory through the use of high pressure static experiments. Five different basalt samples were immersed in water equilibrated with supercritical CO2 containing 1 wt % sulfur dioxide (SO2) and 1 wt % oxygen (O2) at reservoir conditions (∼100 bar, 90 °C) for 48 and 98 days. Gypsum (CaSO4) was a common precipitate, occurred early as elongated blades with striations, and served as substrates for other mineral products. In addition to gypsum, bimodal pulses of water released during dehydroxylation were key indicators, along with X-ray diffraction, for verifying the presence of jarosite–alunite group minerals. Well-developed pseudocubic jarosite crystals formed surface coatings, and in some instances, mixtures of natrojarosite and natroalunite aggregated into spherically shaped structures measuring 100 μm in diameter. Reaction products were also characterized using infrared spectroscopy, which indicated OH and Fe–O stretching modes. The presences of jarosite–alunite group minerals were found in the lower wavenumber region from 700 to 400 cm–1. A strong preferential incorporation of Fe­(III) into natrojarosite was attributed to the oxidation potential of O2. Evidence of CO2 was detected during thermal decomposition of precipitates, suggesting the onset of mineral carbonation.