Thermodynamics of Electrochemical Marine Inorganic Carbon Removal.

In recent years, marine carbon removal technologies have gained attention as a means of reducing greenhouse gas concentrations. One family of these technologies is electrochemical systems, which employ Faradaic reactions to drive alkalinity-swings and enable dissolved inorganic carbon (DIC) removal as gaseous CO2 or as solid minerals. In this work, we develop a thermodynamic framework to estimate upper bounds on performance for Faradaic DIC removal systems. To assess the fundamental mass balances of these systems, we first define unit operations in the DIC/total alkalinity (TA) space. By coupling a seawater speciation model to an electrochemical framework, we provide a generalized comparison of gas evolution and mineralization DIC removal routes, focusing on asymmetric charge/discharge systems. We then show how this framework can be extended to other processes, such as those employing dilution schemes. Finally, we provide a minimum energetic assessment of mCDR pathways relative to direct air capture. Overall, this thermodynamic framework aims to guide system and process design and to drive material discovery and engineering for future electrochemical marine DIC removal systems.