Multiphase carbon mineralization for the reactive separation of CO₂ and directed synthesis of H₂

There is a need to capture, convert and store CO₂ by atom-efficient and energy-efficient pathways that use as few process configurations as possible. This need has motivated studies into multiphase reaction chemistries and this Review describes two such approaches in the context of carbon mineralization. The first approach uses aqueous alkaline solutions containing amine nucleophiles that capture CO₂ and eventually convert it into calcium and magnesium carbonates, thereby regenerating the nucleophiles. Gas-liquid-solid and liquid-solid configurations of these reactions are explored. The second approach combines silicates such as CaSiO₃ or Mg₂SiO₄ with CO and H₂O from the water-gas shift reaction to give H₂ and calcium or magnesium carbonates. Coupling carbonate formation to the water-gas shift reaction shifts the latter equilibrium to afford more H₂ as part of a single-step catalytic approach to carbon mineralization. These pathways exploit the vast abundance of alkaline resources, including naturally occurring silicates and alkaline industrial residues. However, simple stoichiometries belie the complex, multiphase nature of the reactions, predictive control of which presents a scientific opportunity and challenge. This Review describes this multiphase chemistry and the knowledge gaps that need to be addressed to achieve 'step-change' advancements in the reactive separation of CO₂ by carbon mineralization.