Efficient tandem electroreduction of nitrate into ammonia through coupling Cu single atoms with adjacent Co3O4

Yan Liu, Jie Wei, Zhengwu Yang, Lirong Zheng, Jiankang Zhao, Zhimin Song, Yuhan Zhou, Jiajie Cheng, Junyang Meng, Zhigang Geng () and Jie Zeng ()
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Yan Liu: University of Science and Technology of China
Jie Wei: University of Science and Technology of China
Zhengwu Yang: University of Science and Technology of China
Lirong Zheng: Chinese Academy of Sciences
Jiankang Zhao: University of Science and Technology of China
Zhimin Song: University of Science and Technology of China
Yuhan Zhou: University of Science and Technology of China
Jiajie Cheng: University of Science and Technology of China
Junyang Meng: University of Science and Technology of China
Zhigang Geng: University of Science and Technology of China
Jie Zeng: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract The nitrate (NO3−) electroreduction into ammonia (NH3) represents a promising approach for sustainable NH3 synthesis. However, the variation of adsorption configurations renders great difficulties in the simultaneous optimization of binding energy for the intermediates. Though the extensively reported Cu-based electrocatalysts benefit NO3− adsorption, one of the key issues lies in the accumulation of nitrite (NO2−) due to its weak adsorption, resulting in the rapid deactivation of catalysts and sluggish kinetics of subsequent hydrogenation steps. Here we report a tandem electrocatalyst by combining Cu single atoms catalysts with adjacent Co3O4 nanosheets to boost the electroreduction of NO3− to NH3. The obtained tandem catalyst exhibits a yield rate for NH3 of 114.0 mg $${}_{{{{{{\rm{NH}}}}}}_3}$$ NH 3 h−1 cm−2, which exceeds the previous values for the reported Cu-based catalysts. Mechanism investigations unveil that the combination of Co3O4 regulates the adsorption configuration of NO2− and strengthens the binding with NO2−, thus accelerating the electroreduction of NO3− to NH3.

Date: 2024
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DOI: 10.1038/s41467-024-48035-4

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