title: In situ infrared spectroscopic study of brucite carbonation in dry to water-saturated supercritical carbon dioxide.
abstract: In geologic carbon sequestration, whereas part of the injected carbon dioxide will dissolve into host brine, some will remain as neat to water saturated supercritical CO(2) (scCO(2)) near the well bore and at the caprock, especially in the short term life cycle of the sequestration site. Little is known about the reactivity of minerals with scCO(2) containing variable concentrations of water. In this study, we used high-pressure infrared spectroscopy to examine the carbonation of brucite (Mg(OH)(2)) in situ over a 24 h reaction period with scCO(2) containing water concentrations between 0% and 100% saturation, at temperatures of 35, 50, and 70 °C, and at a pressure of 100 bar. Little or no detectable carbonation was observed when brucite was reacted with neat scCO(2). Higher water concentrations and higher temperatures led to greater brucite carbonation rates and larger extents of conversion to magnesium carbonate products. The only observed carbonation product at 35 °C was nesquehonite (MgCO(3)·3H(2)O). Mixtures of nesquehonite and magnesite (MgCO(3)) were detected at 50 °C, but magnesite was more prevalent with increasing water concentration. Both an amorphous hydrated magnesium carbonate solid and magnesite were detected at 70 °C, but magnesite predominated with increasing water concentration. The identity of the magnesium carbonate products appears strongly linked to magnesium water exchange kinetics through temperature and water availability effects.
authors.affiliation: Pacific Northwest National Laboratory, Richland, Washington 99352, USA. john.loring@pnl.gov
authors.forename: John S
authors.initials: JS
authors.lastname: Loring
authors.forename: Christopher J
authors.initials: CJ
authors.lastname: Thompson
authors.forename: Changyong
authors.initials: C
authors.lastname: Zhang
authors.forename: Zheming
authors.initials: Z
authors.lastname: Wang
authors.forename: Herbert T
authors.initials: HT
authors.lastname: Schaef
authors.forename: Kevin M
authors.initials: KM
authors.lastname: Rosso
mesh_terms: D002245:Carbon Dioxide / Q000737:chemistry* / Q000302:isolation & purification; D057965:Carbon Sequestration; D005844:Geology; D008276:Magnesium Hydroxide / Q000737:chemistry*; D013055:Spectrophotometry, Infrared; D013696:Temperature; D014867:Water / Q000737:chemistry*
chemical_list: D014867:Water; D002245:Carbon Dioxide; D008276:Magnesium Hydroxide