Carbon sequestration via aqueous olivine mineral carbonation: role of passivating layer formation
- Arizona State University, Tempe, AZ (United States). Center for Solid State Science, Science and Engineering of Materials Graduate Program, Departments of Mechanical and Aerospace Engineering and Chemistry and Biochemistry
CO{sub 2} sequestration via carbonation of widely available low-cost minerals, such as olivine, can permanently dispose of CO{sub 2} in an environmentally benign and a geologically stable form. The paper reports the results of studies of the mechanisms that limit aqueous olivine carbonation reactivity under the optimum sequestration reaction conditions observed to date: 1 M NaCl + 0.64 M NaHCO{sub 3} at T {approx} 185{sup o}C and P{sub CO{sub 2}} {approx} 135 bar. A reaction limiting silica-rich passivating layer (PL) forms on the feedstock grains, slowing carbonate formation and raising process cost. The morphology and composition of the passivating layers are investigated using scanning and transmission electron microscopy and atomic level modeling. Postreaction analysis of feedstock particles, recovered from stirred autoclave experiments at 1500 rpm, provides unequivocal evidence of local mechanical removal (chipping) of PL material, suggesting particle abrasion. This is corroborated by the observation that carbonation increases dramatically with solid particle concentration in stirred experiments. Multiphase hydrodynamic calculations are combined with experiment to better understand the associated slurry-flow effects. Large-scale atomic-level simulations of the reaction zone suggest that the PL possesses a 'glassy' but highly defective SiO{sub 2} structure that can permit diffusion of key reactants. Mitigating passivating layer effectiveness is critical to enhancing carbonation and lowering sequestration process cost. 30 refs., 7 figs.
- OSTI ID:
- 20781536
- Journal Information:
- Environmental Science and Technology, Vol. 40, Issue 15; Other Information: mckelvy@asu.edu; ISSN 0013-936X
- Country of Publication:
- United States
- Language:
- English
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