Electrostatic Focusing Enables Directed Active Hydrogen Delivery for pH‐Universal Nitrate Electroreduction

ABSTRACT Achieving pH‐universal electroreduction of nitrate to ammonia remains a fundamental obstacle for practical nitrate remediation in aqueous environments. The central challenge is to achieve efficient utilization of the scarce reactive hydrogen (*H) under alkaline conditions while preventing *H recombination that promotes hydrogen evolution in acidic media. Herein, electrostatic focusing is introduced to regulate the directional delivery of *H toward nitrate‐bound sites through the electrostatic potential (ESP) landscape established upon nitrate coordination. A copper‐halide cluster catalyst achieves selective nitrate electroreduction across pH 1–13, delivering NH 3 Faradaic efficiencies (FE) of 92.9%–100%. Electrochemical, spectroscopic, and density functional theory (DFT) analyses reveal that nitrate binding generates a single, localized ESP minimum at the nitrate oxygen, which biases *H delivery toward productive hydrogenation. Moreover, quantitative correlations between ESP extrema and pH‐dependent onset potentials indicate that an appropriately moderated ESP magnitude promotes proton‐sensitive hydrogenation kinetics. This work establishes electrostatic focusing as a viable strategy for achieving pH‐universal and selective nitrate electroreduction.