Controlled Hydrogen Delivery by Single‐Atom Ru Accelerates Electrocatalytic Ammonia Synthesis

ABSTRACT Electrocatalytic nitric oxide reduction to ammonia (NORR) offers a dual opportunity for NO remediation and decentralized NH 3 production, yet its efficiency is often limited by competing pathways and unclear structure–function relationships. Here we introduce a reactant‐shunting strategy that installs a guiding electrocatalytic step via isolated Ru atoms to supply surface‐bound * H species and enforce a Langmuir–Hinshelwood (LH) hydrogenation pathway. Using Ru 1 /Co 3 O 4 as a model catalyst, we show that single Ru sites promote water adsorption and dissociation, forming stable Ru‐H intermediates that thermodynamically and kinetically accelerate the coupling‐hydrogenation steps in NORR. The optimized catalyst delivers an NH 3 yield of 533.49 µmol cm −2 h −1 with a 97.19% faradaic efficiency, surpassing state‐of‐the‐art systems. The reactant‐shunting principle further generalizes across multiple oxide hosts, enhancing NH 3 productivity by up to threefold. These findings establish pathway steering through controlled hydrogen delivery as a powerful strategy for high‐efficiency electrocatalytic ammonia synthesis.