Seawater alkalization via an energy-efficient electrochemical process for CO₂ capture

Electrochemical pH-swing strategies offer a promising avenue for cost-effective and energy-efficient carbon dioxide (CO₂) capture, surpassing the traditional thermally activated processes and humidity-sensitive techniques. The concept of elevating seawater's alkalinity for scalable CO₂ capture without introducing additional chemical as reactant is particularly intriguing due to its minimal environmental impact. However, current commercial plants like chlor-alkali process or water electrolysis demand high thermodynamic voltages of 2.2 V and 1.23 V, respectively, for the production of sodium hydroxide (NaOH) from seawater. These high voltages are attributed to the asymmetric electrochemical reactions, where two completely different reactions take place at the anode and cathode. Here, we developed a symmetric electrochemical system for seawater alkalization based on a highly reversible and identical reaction taking place at the anode and cathode. We utilize hydrogen evolution reaction at the cathode, where the generated hydrogen is looped to the anode for hydrogen oxidation reaction. Theoretical calculations indicate an impressively low energy requirement ranging from 0.07 to 0.53 kWh/kg NaOH for established pH differences of 1.7 to 13.4. Experimentally, we achieved the alkalization with an energy consumption of 0.63 kWh/kg NaOH, which is only 38% of the theoretical energy requirements of the chlor-alkali process (1.64 kWh/kg NaOH). Further tests demonstrated the system's potential of enduring high current densities (~20 mA/cm²) and operating stability over an extended period (>110 h), showing its potential for future applications. Notably, the CO₂ adsorption tests performed with alkalized seawater exhibited remarkably improved CO₂ capture dictated by the production of hydroxide compared to the pristine seawater.