Aqueous carbonation of natural brucite: relevance to CO2 sequestration

Carbonation of natural brucite in H2O and diluted HCl is investigated at room temperature and moderate pCO2 to explore the products' mineralogy and reaction kinetics. Results show nesquehonite is by far the dominant carbonate species formed, despite its poorer thermodynamic stability relative to magnesite and possibly hydromagnesite. Time-dependent measurements reveal carbonate formation within 30 min, regardless of the original acidity of the slurry. However, while the fraction of reacted brucite in H2O increases gradually over time and approaches unity ( approximately 98%) at 2.5 h, it rises rapidly in HCl within the first hour and levels off thereafter, leaving a significant amount of brucite unreacted. Such behavior suggests that the initial quantity of Mg2+ affects the reaction kinetics. Fitting a pseudo first-order rate law to the data yields a higher rate constant for the HCl experiments. These observations may imply that the carbonation does not proceed through heterogeneous reaction between gaseous CO2 and solid brucite. Solution chemistry analysis indicates that most CO2 stays in aqueous phase in both media; however, the concentration of HCO3(-) becomes high in H2O after about 2 h, agreeing with the observed inferior carbonation extent in HCl.