articleJournal of the American Chemical SocietyFeb 28, 2025Closed access

Self-Triggering a Locally Alkaline Microenvironment of Co 4 Fe 6 for Highly Efficient Neutral Ammonia Electrosynthesis

University of Science and Technology of China · Chinese Academy of Sciences · +6 more institutions

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Abstract

Electrochemical nitrate reduction reaction (eNO3–RR) to ammonia (NH3) holds great promise for the green treatment of NO3– and ambient NH3 synthesis. Although Fe-based electrocatalysts have emerged as promising alternatives, their excellent eNO3–RR-to-NH3 activity is usually limited to harsh alkaline electrolytes or alloying noble metals with Fe in sustainable neutral electrolytes. Herein, we demonstrate an unusual self-triggering localized alkalinity of the Co4Fe6 electrocatalyst for efficient eNO3–RR-to-NH3 activity in neutral media, which breaks down the conventional pH-dependent kinetics restrictions and shows a 98.6% NH3 Faradaic efficiency (FE) and 99.9% NH3 selectivity at −0.69 V vs RHE. The synergetic…

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