Pulsed Electrocatalysis Driven Efficient Ammonia Synthesis by Facilitating *NOOH Formation and Balancing *H Supply

Electrochemical nitrate reduction emerges as a promising approach for ammonia generation; however, its efficiency is hindered by the sluggish hydrogenation of nitrogen‐containing intermediates and limited active hydrogen supply at constant applied potentials. Driven by the pulsed electrocatalysis, in this work, efficient nitrate‐to‐ammonia conversion is realized by facilitating *NOOH formation and balancing *H supply on a Janus Cu@Co/NC electrocatalyst. In detail, the Cu sites could activate NO 3 − at low overpotentials, while the Co sites could facilitate *NOOH formation with sufficient *H provided by the Co sites at high overpotentials. Promoted by the pulsed electrocatalysis technique, a maximum Faradaic efficiency of 98.32% with NH 3 yield rate of 12.75 mg h −1 mg cat −1 is attained, and the scaled‐up pulsed electrosynthesis at industrial current densities is also achieved. This work underlines the feasibility of pulsed electrolysis for regulating intermediate hydrogenation, offering a promising approach for the synthesis of ammonia or other important chemicals.