Simultaneous anchoring of Ni nanoparticles and single-atom Ni on BCN matrix promotes efficient conversion of nitrate in water into high-value-added ammonia

Realize the reuse of nitrate waste in sewage through electrocatalysis, including the sustainable production of high value-added ammonia and the effective purification of nitrate sewage. • Achieved the anchoring of single-atom Ni on the BCN through structural confinement engineering. • Ammonia yield rate reaches milligram level and the selectivity is as high as 91.5% • Achieve high-efficiency and high-selectivity production of ammonia in the full-pH range. • BCN@Ni has strong electrochemical cycle stability and long-term durability. Electrochemical synthesis of ammonia driven by clean energy is expected to realize the supply of ammonia for distributed production of industry and agriculture. Here, nickel nanoparticles and nickel in the form of single atoms were simultaneously anchored on the electrochemically active carrier BCN matrix through a structured domain strategy, which realized a high-efficiency, high-value-added, conversion of nitrate in sewage. Specifically, the electrochemical nitrate reduction reaction (NIRR) driven by BCN@Ni in alkaline media achieves an ammonia yield rate as high as 2320.2 μg h −1 cm −2 (at −0.5 V vs RHE), and Faraday efficiency as high as 91.15% (at −0.3 V vs RHE). Even in neutral and acidic media, the ammonia yield rates of NIRR driven by BCN@Ni are as high as 1904.2 μg h −1 cm −2 and 2057.4 μg h −1 cm −2 , respectively (at −0.4 V vs RHE). The 15 NO 3 - isotope labeling experiment verified that the recorded ammonia all came from the electrochemical reduction of NO 3 – on BCN@Ni. Density functional theory (DFT) calculations show that both nano-Ni and single-atom Ni in BCN@Ni have the ability to electrochemically convert NO 3 – into NH 3 , and that the addition of BCN can further promote the NIRR on Ni.