Sustainable process for enhanced CO2 mineralization of calcium silicates using a recyclable chelating agent under alkaline conditions

Abstract

This study explored a key challenge of aqueous indirect CO2 mineralization: the consumption of chemicals for a large pH swing between acidic and alkaline conditions and the production of waste fluid. Herein, we proposed and experimentally examined the technical feasibility of a sustainable process for enhanced CO2 mineralization using a new potentially recyclable alkaline solution of chelating agent [N,N-dicarboxymethyl glutamic acid (GLDA)] at near-room temperatures. This process comprising the following: enhanced Ca extraction from silicates with suppressed formation of silica-rich passivation layer via the combined actions of proton and chelating agent attacks at weakly alkaline conditions; Ca carbonation using sodium carbonate at high pH and temperature; and regeneration of the extraction solution (i.e., a decrease in pH and silicon removal) via CO2 gas dissolution. Ca extraction experiments using representative calcium silicate (CaSiO3) at various GLDA concentrations and initial pHs under 50 °C demonstrated the possibility of enhanced Ca extraction with almost all GLDA molecules combining with Ca (Ca/GLDA≈1) at an optimum condition (0.1 M GLDA and pH 8 in this study). This type of extraction is desirable as it contributes to an efficient Ca carbonation in addition to a decreased stability of the Ca-GLDA complex; indeed, most of the extracted Ca were carbonated to aragonite at 80 °C. Moreover, such extraction with the relatively low pH of 8 was found to be desirable for solution regeneration that involves pH adjustment (reduction) because of low silica solubility at lower pH. It was demonstrated that room-temperature CO2 bubbling removed almost all Si as amorphous SiO2, during which CO2 captured as NaHCO3 was also occurring. The recyclability of extraction solution was also demonstrated in this paper. This study encourages further extensive studies to optimize reaction conditions, particularly for using alkaline solid wastes, to make the process both technically and economically feasible.