Bimetallic Cu11Ag3 Nanotips for Ultrahigh Yield Rate of Nitrate-to-Ammonium

doi:10.1002/anie.202415259

Bimetallic Cu11Ag3 Nanotips for Ultrahigh Yield Rate of Nitrate-to-Ammonium

2024-11-06

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DOI：10.1002/anie.202415259

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Electrochemical reduction of nitrate to ammonia (NRA) offers a sustainable approach for NH3 production and NO3- removal but suffers from low NH3 yield rate (<1.20 mmol h(-1) cm(-2)). We present bimetallic Cu11Ag3 nanotips with tailored local environment, which achieve an ultrahigh NH3 yield rate of 2.36 mmol h(-1) cm(-2) at a low applied potential of -0.33 V vs. RHE, a high Faradaic efficiency (FE) of 98.8 %, and long-term operation stability at 1800 mg-N L-1 NO3-, outperforming most of the recently reported catalysts. At a NO3- concentration as low as 15 mg-N L-1, it still delivers a high FE of 86.9 % and an NH3 selectivity of 93.8 %. Finite-element method and density functional theory calculations reveal that the Cu11Ag3 exhibits reduced adsorption energy barrier of *N intermediates, favorable water dissociation for *H generation and high energy barrier for H-2 formation, while its tip-enhanced enrichment promoting NO3- accumulation.

Keywords:

Electrocatalytic nitrate reduction

ammonia production

high yield rate

tip-enhanced enrichment

finite-element method

Bimetallic Cu11Ag3 Nanotips for Ultrahigh Yield Rate of Nitrate-to-Ammonium

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