Spatial Proximity in Single Atomic Co Sites Boosts Water‐Derived Active Hydrogen for Efficient Neutral Nitrate‐to‐Ammonia Electrosynthesis

Résumé fourni par la source

ABSTRACT Single‐atom catalysts (SACs) are promising for nitrate reduction reaction (NO 3 RR) to ammonia (NH 3 ), given their high atomic efficiency and tunable, well‐defined structures. Yet, interactions between proximate atomic sites in NO 3 RR are poorly understood. Here, we demonstrate the spatial proximity effect over N, P coordinated Co single atomic centers to boost NO 3 RR catalytic activity. The adjacent configuration with CoN 4 ‐P‐CoN 4 atomic structures of the closest inter‐site distance of ∼4.5 Å balance the water dissociation and NO 3 RR via a dual‐driven cascade mechanism in a neutral electrolyte. P site located at the shared second coordination shell dissociates water molecules to supply ample *H for the following hydrogenation process, while Co single site with optimized electronic state adsorbs and converts NO 3 − to NH 3 . This study underscores the critical role of spatial proximity in SACs for NO 3 RR, and may extend to diverse electrochemical transformations.

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