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Article Abstract
The electrocatalytic conversion of wastewater nitrate (NO) to ammonia (NH) under industrial-grade current densities at ambient conditions presents a sustainable alternative to the energy-intensive Haber-Bosch process, yet remains fundamentally challenging. Here, a highly efficient NO to NH electrocatalyst with single Fe atoms dispersed on graphdiyne (GDY) is constructed through an growth method. Experimental analysis demonstrates the formation of high-density atomic active sites on GDY, ensuring the high intrinsic activity of the electrocatalyst. Besides, the newly formed sp-C-Fe chemical bonds bridged GDY and Fe atoms providing a well-defined channel for selectively and efficiently transferring electrons from the active sites to the reactants/key intermediates, allowing for selective NO activation and efficient protonation. This atomic-scale electronic modulation enables exceptional nitrate reduction performance, achieving record-high faradaic efficiency (45.48%) and ammonia yield (202.34 μmol h cm) while maintaining operational stability.
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