Reaction Mechanism for the Aqueous-Phase Mineral Carbonation of Heat-Activated Serpentine at Low Temperatures and Pressures in Flue Gas Conditions

作者：Louis-César Pasquier, Guy Mercier, Jean‐François Blais, Emmanuelle Cecchi, Sandra Elizabeth Kentish · 发表于：Environmental Science & Technology · 年份：2014 · DOI：10.1021/es405449v · 被引用次数：81 · 研究领域：CO2 Sequestration and Geologic Interactions、Radioactive element chemistry and processing、Zeolite Catalysis and Synthesis

Mineral carbonation is known as one of the safest ways to sequester CO2. Nevertheless, the slow kinetics and low carbonation rates constitute a major barrier for any possible industrial application. To date, no studies have focused on reacting serpentinite with a relatively low partial pressure of CO2 (pCO2) close to flue gas conditions. In this work, finely ground and heat-treated serpentinite [Mg3Si2O5(OH)4] extracted from mining residues was reacted with a 18.2 vol % CO2 gas stream at moderate global pressures to investigate the effect on CO2 solubility and Mg leaching. Serpentinite dissolution rates were also measured to define the rate-limiting step. Successive batches of gas were contacted with the same serpentinite to identify surface-limiting factors using scanning electron microscopy (SEM) analysis. Investigation of the serpentinite carbonation reaction mechanisms under conditions close to a direct flue gas treatment showed that increased dissolution rates could be achieved relative to prior work, with an average Mg dissolution rate of 3.55 × 10(-11) mol cm(-2) s(-1). This study provides another perspective of the feasibility of applying a mineral carbonation process to reduce industrial greenhouse gas (GHG) emissions from large emission sources.