High‐Efficiency and Carbon‐Lean Electrochemical Desalination Enabled by Nucleophilic Engineering of Organic Molecular Electrode

ABSTRACT The worsening global freshwater crisis positions seawater desalination as a critical solution. However, conventional desalination technologies remain constrained by a persistent sustainability trilemma involving high energy consumption, chemical reliance, and substantial carbon emissions. Here, we present an electrochemical strategy that overcomes these constraints by delivering high‐performance desalination behaviors while generating substantial environmental and energy benefits. Our approach utilizes a molecularly nucleophilic‐engineered dinitro‐functionalized pyrenephenazine (PPZ‐2NO 2 ) organic electrode integrated in a capacitive deionization (CDI) cell, enabling real seawater desalination. The electron‐withdrawing nitro groups precisely modulate the electronic structure and electrochemical activity of the PPZ‐2NO 2 electrode, unlocking the full utilization of redox‐active sites. The resulting organic‐based CDI configuration possesses high salt ion adsorption capacity and ultrafast rate under low‐voltage operation without chemical additives. The validation at module scale demonstrates practical viability, producing industrial‐grade freshwater at a 97.2% yield ratio in compliance with World Health Organization (WHO) criteria, while achieving an exceptional seawater desalination capacity of 349.91 mg g −1 . Furthermore, the process operates with low energy consumption and a carbon footprint of only 0.147 t CO 2 eq per ton of salt removed, which is ∼61.18% lower than state‐of‐the‐art technologies. This work offers a molecular‐level design for carbon‐lean electrochemical desalination toward sustainable water‐energy integration.