Enhancing Electrochemical Nitrate Reduction to Ammonia over Cu Nanosheets via Facet Tandem Catalysis

Abstract Electrochemical conversion of nitrate (NO 3 − ) into ammonia (NH 3 ) represents a potential way for achieving carbon‐free NH 3 production while balancing the nitrogen cycle. Herein we report a high‐performance Cu nanosheets catalyst which delivers a NH 3 partial current density of 665 mA cm −2 and NH 3 yield rate of 1.41 mmol h −1 cm −2 in a flow cell at −0.59 V vs. reversible hydrogen electrode. The catalyst showed a high stability for 700 h with NH 3 Faradaic efficiency of ≈88 % at 365 mA cm −2 . In situ spectroscopy results verify that Cu nanosheets are in situ derived from the as‐prepared CuO nanosheets under electrochemical NO 3 − reduction reaction conditions. Electrochemical measurements and density functional theory calculations indicate that the high performance is attributed to the tandem interaction of Cu(100) and Cu(111) facets. The NO 2 − generated on the Cu(100) facets is subsequently hydrogenated on the Cu(111) facets, thus the tandem catalysis promotes the crucial hydrogenation of *NO to *NOH for NH 3 production.