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Article Abstract
The electrocatalytic nitrate reduction reaction (NitRR) is a promising dual-functional strategy for carbon-free ammonia synthesis and sustainable wastewater treatment. The complexity of the eight-electron/nine-proton transfer process in the NitRR highlights the need for improved catalysts to optimize reaction pathways and suppress competitive side reactions. Herein, the successful growth of CuCoO nanowires with tailored defect structures is reported with the assistance of graphdiyne (GDY) through an atomic-level heterointerface engineering strategy. The synergistic interactions between GDY electron-rich sp-C atoms and electron-deficient bimetallic atoms induce self-optimized planar defects along nanowires and accelerate interfacial charge transfer via metal‒carbon covalent hybridization. These properties significantly facilitate dynamic NO adsorption-activation and completely suppress byproduct formation via intermediate stabilization. As a result, CuCoO/GDY exhibites a remarkable NitRR performance of 100% Faradaic efficiency (FE), a record-high NH yield rate (Y, 3332 µg cm h) at an ultralow operational potential (-0.132 V vs RHE), no side reactions, and long-term durability. This work pioneers atomic-level interface engineering in GDY-based systems, establishing a general method for synthesizing high-performance electrocatalysts in sustainable nitrogen cycles.
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