Theoretical modeling of electrochemical carbon mineralization.

Global warming, driven by the accumulation of greenhouse gases such as carbon dioxide (CO2), has spurred significant interest in carbon sequestration strategies to mitigate its impact. One promising approach is the conversion of CO2 into value-added materials, with electrochemical carbon mineralization emerging as a particularly effective method. This process converts CO2 into carbonate minerals, fixing CO2 in a solid form and resulting in a class of carbon-negative composites with unique material properties, including high toughness, fire resistance, self-healing capabilities, and reprocessability. Despite its advancements and potential, the theoretical understanding of electrochemical carbon mineralization remains incomplete. To bridge this gap, this study establishes theoretical and phase-field modeling frameworks to elucidate the fundamental mechanisms underlying electrochemical carbon mineralization. By integrating experiments, analytical modeling, and phase-field simulations, we investigate key factors influencing mineral growth, including electrode diameter, applied voltage, Ca2+ concentration, and electrode cross-sectional shape. The results show strong agreement among experimental observations, theoretical analyses, and phase-field simulations, laying a solid foundation for optimizing electrochemical carbon sequestration in manufacturing.