Abstract
Efficient ammonium (NH4+) production from strongly acidic wastewater through electrocatalytic nitrate reduction reaction (NO3RR) holds promise, yet faces challenges due to hydrogen evolution competition and catalyst corrosion. This work reports a novel catalyst (i.e., CoSA-CoNP@N-CNA/CC), which consists of carbon cloth (CC) supporting a nitrogen-doped carbon nanotube array (N-CNA) that contains atomically dispersed Co single atoms (CoSA) and Co nanoparticles (CoNP), achieving exceptional NO3−-to-NH4+ conversion at pH 1. The resulting cathode produces NH4+ at a rate of 0.275mmolh−1 cm−2 with a Faradaic efficiency of 95.6%, without concurrent NO2− production at -0.6V (vs. RHE). The study reveals that the synergy between individual Co atoms and encapsulated Co nanoparticles facilitates electron transfer, hindering hydrogen adsorption, enhancing NO3− adsorption and activation, and reducing the energy barrier for the rate-determining step involving intermediate ⁎NO hydrogenation. Validation with real acidic samples underscores the exceptional capability of CoSA-CoNP@N-CNA/CC for NH4+ recovery via NO3RR.
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