Single-atom Fe anchored graphdiyne for high-efficiency nitrate-to-ammonia conversion under ambient conditions

Abstract

The electrocatalytic conversion of wastewater nitrate (NO₃⁻) to ammonia (NH₃) 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 NO₃⁻ to NH₃ electrocatalyst with single Fe atoms dispersed on graphdiyne (GDY) is constructed through an in situ 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 NO₃⁻ 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⁻¹ cm⁻²) while maintaining operational stability.