This perspective proposes a potential pathway to diminish atmospheric CO₂ accumulations which is distinct from traditional carbon capture and geological sequestration strategies and from existing negative emissions technologies (NETs). Unlike conventional sorbent- or solvent-based CO₂ capture processes where substantial energy expenditures are associated with demixing and desorbing CO₂, the single-step carbon sequestration and storage (sCS²) approach relies on electrolytic carbonate mineral precipitation using renewable energy within a simple and scalable process design. Although numerous approaches have implied electrolysis for carbon management, the sCS² approach is unique in the following ways: (1) CO₂ mineralization for promoting solid carbonate formation: The thermodynamic and kinetic barriers to carbonate precipitation are overcome by direct and in situ electrochemical forcing to stabilize dissolved inorganic carbon and divalent cations [Ca,Mg] to form carbonate minerals. (2) Flow-through membraneless electrolysis: A flowing electrolyte (seawater) is dissociated while in motion. The process utilizes cost-effective mesh electrodes while also decreasing the number of components and assembly steps and reducing the risk of device failure. (3) Integrated electrolytic reactor–rotary drum filter: An electroactive thin-film mesh cathode (eTFC) is suggested to be integrated within a rotary drum filter configuration, allowing for the filtration of dilute and polydispersed mineral precipitates at a low energy cost. These attributes render sCS² as an approach worthy of more detailed evaluation, development, and scaling for global-scale carbon management.

We present the mass balances associated with carbon dioxide (CO₂) removal (CDR) using seawater as both the source of reactants and as the reaction medium via electrolysis following the "Equatic" (formerly known as "SeaChange") process. This process, extensively detailed in La Plante E.C.; ACS Sustain. Chem. Eng.2021, 9, ( (3), ), 1073-1089, involves the application of an electric overpotential that splits water to form H⁺ and OH^- ions, producing acidity and alkalinity, i.e., in addition to gaseous coproducts, at the anode and cathode, respectively. The alkalinity that results, i.e., via the "continuous electrolytic pH pump" results in the instantaneous precipitation of calcium carbonate (CaCO₃), hydrated magnesium carbonates (e.g., nesquehonite: MgCO₃·3H₂O, hydromagnesite: Mg₅(CO₃)₄(OH)₂·4H₂O, etc.), and/or magnesium hydroxide (Mg(OH)₂) depending on the CO₃^2- ion-activity in solution. This results in the trapping and, hence, durable and permanent (at least ∼10 000-100 000 years) immobilization of CO₂ that was originally dissolved in water, and that is additionally drawn down from the atmosphere within: (a) mineral carbonates, and/or (b) as solvated bicarbonate (HCO₃^-) and carbonate (CO₃^2-) ions (i.e., due to the absorption of atmospheric CO₂ into seawater having enhanced alkalinity). Taken together, these actions result in the net removal of ∼4.6 kg of CO₂ per m³ of seawater catholyte processed. Geochemical simulations quantify the extents of net CO₂ removal including the dependencies on the process configuration. It is furthermore indicated that the efficiency of realkalinization of the acidic anolyte using alkaline solids depends on their acid neutralization capacity and dissolution reactivity. We also assess changes in seawater chemistry resulting from Mg(OH)₂ dissolution with emphasis on the change in seawater alkalinity and saturation state. Overall, this analysis provides direct quantifications of the ability of the Equatic process to serve as a means for technological CDR to mitigate the worst effects of accelerating climate change.

The Cl⁻-induced corrosion of metals and alloys is of relevance to a wide range of engineered materials, structures, and systems. Because of the challenges in studying pitting corrosion in a quantitative and statistically significant manner, its kinetics remain poorly understood. Herein, by direct, nano- to micro-scale observations using vertical scanning interferometry (VSI), we examine the temporal evolution of pitting corrosion on AISI 1045 carbon steel over large surface areas in Cl⁻-free, and Cl⁻-enriched solutions. Special focus is paid to examine the nucleation and growth of pits, and the associated formation of roughened regions on steel surfaces. By statistical analysis of hundreds of individual pits, three stages of pitting corrosion, namely, induction, propagation, and saturation, are quantitatively distinguished. By quantifying the kinetics of these processes, we contextualize our current understanding of electrochemical corrosion within a framework that considers spatial dynamics and morphology evolutions. In the presence of Cl⁻ ions, corrosion is highly accelerated due to multiple autocatalytic factors including destabilization of protective surface oxide films and preservation of aggressive microenvironments within the pits, both of which promote continued pit nucleation and growth. These findings offer new insights into predicting and modeling steel corrosion processes in mid-pH aqueous environments.