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

Abstract

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.

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Fig. 1: Amines used to capture CO2 in aqueous solution.
Fig. 2: The aqueous alkaline-amine-looping approach for CO2 mineralization.
Fig. 3: Carbon mineralization by aqueous alkaline-amine looping is affected by the solid precursor, temperature and amine concentration.
Fig. 4: Polymorphism in calcium and magnesium carbonate products of carbon mineralization.
Fig. 5: Comparison of the reactivity of Ca-bearing and Mg-bearing silicate and aluminosilicate minerals and rocks.
Fig. 6: Coupled reaction pathways in the conversion of silicates into carbonates and H2.
Fig. 7: Characterization over multiple length scales reveals reaction-induced chemo-morphological coupling.

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Acknowledgements

This research was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division.

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Correspondence to Greeshma Gadikota.

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Provisional patents have been filed by Cornell University on the process for directed hydrogen synthesis starting with calcium and magnesium silicate precursors and the reactive separation of CO2 using amine-bearing solvents.

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Gadikota, G. Multiphase carbon mineralization for the reactive separation of CO2 and directed synthesis of H2. Nat Rev Chem 4, 78–89 (2020). https://doi.org/10.1038/s41570-019-0158-3

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