Comprehensive analysis of direct aqueous mineral carbonation using dissolution enhancing organic additives

Direct aqueous mineral carbonation using organic anions has been presented by many as a promising strategy for mineral carbonation, on the basis that additives such as oxalate increase the rate and extent of dissolution of magnesium silicates several folds. Through geochemical modelling and detailed solid characterisation, this paper discusses and extends our current understanding of this process. The role of disodium oxalate as a dissolution enhancing agent for olivine is thoroughly examined through experiments in which all phases are carefully analysed. We show that under 20 bar of CO2 pressure formation of strong oxalate–magnesium complexes in solution and precipitation of MgC2O4·2H2O (glushinskite) impede any chance of obtaining significant amounts of magnesium carbonate. Other promising ligands from a dissolution perspective, namely citrate and EDTA salts, are also investigated. Contrary to oxalate, these ligands do not form any solid by-products with magnesium, and yet they do not produce better carbonation results, thereby casting strong doubts on the possibility of developing a direct aqueous mineral carbonation process using organic salts. Geochemical modelling permits successful simulation of the dissolution kinetics of magnesium silicate using a shrinking particle model that accounts for the precipitation of glushinskite, amorphous silica and a magnesium phyllosilicate at advanced stages of the dissolution process.

► Investigation of direct aqueous mineral carbonation with organic salts.
► Reaction mechanisms explained by analytical measurements and geochemical modelling.
► Magnesite formation impeded by complexation of Mg with dissolution additives.
► Mineral carbonation with polyacid salts not a viable mineral carbonation process.