Long-Term Efficient Ammonia Synthesis by Cu-Co Tandem Active Sites at High Current Density

2026-06-18

PRE

Dongqi Liu

Chunqi Yang

Chuqian Xiao

Sheng Hu

Shaoyan Wang

Xiuming Bu

Yuhang Li

Xianying Wang

DOI：10.1039/D6GC02381A

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Electrocatalytic nitrate reduction reaction (NO3RR) holds significant promise for both sustainable ammonia (NH3) synthesis and industrial wastewater treatment. However; its efficiency in neutral electrolytes is severely limited by the insufficient supply of reactive hydrogen species (*H); leading to the accumulation of nitrite (NO2-); which not only deactivates catalysts but also suppresses subsequent hydrogenation steps. In addition; under high-current-density conditions; the competing hydrogen evolution reaction (HER) intensifies; leading to a decrease in the Faradaic efficiency (FE) for NH3. In this work; we present a Cu-Co3O4 tandem catalyst; where trace Cu doping into octahedral sites of Co3O4 promotes nitrate adsorption; while the altered coordination environment of Co facilitates water dissociation to generate *H. The Cu-Co active sites facilitate the efficient transfer of *H to adsorbed nitrate species; consequently enhancing both the ammonia production rate and catalytic stability under high-current-density and neutral conditions. The optimized catalyst can achieve a maximum FE of 93.2% and a high ammonia yield rate of 11.3 mg h-1 cm-2. Furthermore; we coupled nitrate reduction (NO3RR) with 5-hydroxymethylfurfural oxidation (HMFOR) in a membrane electrode assembly (MEA) electrolyzer; and a comprehensive techno-economic analysis demonstrates the profitability and commercial viability of this coupled system.

Long-Term Efficient Ammonia Synthesis by Cu-Co Tandem Active Sites at High Current Density

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