Modulating Dynamic Atomic Hydrogen Generation and Utilization for Selective Electrocatalytic Ammonia Recovery from Low-Concentration Nitrate-Containing Wastewater
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY（2025）
Abstract
Herein, a copper-doped nickel phosphide (CuxNi2-xP) electrode with a tailored metal d-band center was designed to boost ammonia (NH3) selectivity during electrocatalytic nitrate (NO3-) reduction (NO3RR) by modulating atomic hydrogen (H*) behavior. The Cu doping accelerated both the Volmer step of water splitting to form H* and the H*-mediated hydrogenation steps for NH3 production, addressing the mismatch between H* supply and utilization. Consequently, the CuxNi2-xP electrode achieved 100 % NO3- conversion efficiency and 99.2 % NH3 selectivity at a low NO3- concentration of 50 mg L- 1, outperforming Ni2P and Cu counterparts. The crucial role of H* in the performance enhancement was elucidated via in-situ characterizations and density functional theory (DFT) calculations. Furthermore, an integrated device combining NO3RR, organic pollutant degradation and NH3 recovery was constructed, demonstrating its scalability for practical wastewater treatment. This study paves the way for collaboratively addressing environmental and energy challenges through improving NH3 recovery from nitrate-laden wastewater.
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Key words
Electrocatalytic nitrate reduction,Atomic hydrogen,Ammonia synthesis,d -Band center modulation,Cu x Ni 2-x P
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