Abstract
Electrocatalytic nitrate reduction sustainably produces ammonia and alleviates water pollution, yet challenging due to the kinetic mismatch and hydrogen evolution competition. Cu/Cu2O heterojunction is proven effective to break the rate-determining NO3--to-NO2- step for efficient NH3 conversion, while it is unstable by electrochemical reconstruction. Here we report a programmable pulsed electrolysis strategy to achieve reliable Cu/Cu2O structure, where Cu is oxidized to CuO during oxidation pulse, then regenerating Cu/Cu2O upon reduction. Alloying with Ni further modulates hydrogen adsorption, which transfers from Ni/Ni(OH)2 to N-containing intermediates on Cu/Cu2O, promoting NH3 formation with a high NO3--to-NH3 Faraday efficiency (88.0 ± 1.6%, pH 12) and NH3 yield rate (583.6 ± 2.4 μmol cm-2 h-1) under optimal pulsed conditions. This work provides new insights to in situ electrochemically regulate catalysts for NO3--to-NH3 conversion.
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