Atomically Dispersed Zinc Active Sites Efficiently Promote the Electrochemical Conversion of N2 to NH3

Yanjiao Wei; Xinyu Wang; Mengjie Sun; Min Ma; Jian Tian; Minhua Shao

doi:10.1002/eem2.12630

Energy & Environmental Materials ›› 2024, Vol. 7 ›› Issue (3) : 12630 DOI: 10.1002/eem2.12630

RESEARCH ARTICLE

Atomically Dispersed Zinc Active Sites Efficiently Promote the Electrochemical Conversion of N₂ to NH₃

Yanjiao Wei ¹
, Xinyu Wang ¹
, Mengjie Sun ¹
, Min Ma ¹
, Jian Tian ¹^,²^,^†
, Minhua Shao ²^,³^,^†

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Abstract

At present, the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia (NH₃). Herein, we synthesized atomically dispersed zinc active sites supported on N-doped carbon nanosheets (Zn/NC NSs) as an efficient nitrogen reduction reaction catalyst, which achieves a high ammonia yield of 46.62 μg h⁻¹ mg⁻¹_cat. at −0.85 V (vs RHE) and Faradaic efficiency of 95.8% at −0.70 V (vs RHE). In addition, Zn/NC NSs present great stability and selectivity, and there is no significant change in NH₃ rate and Faradaic efficiencies after multiple cycles. The structural characterization shows that the active center in the nitrogen reduction reaction process is the Zn–N₄ sites in the catalyst. DFT calculation confirms that Zn/NC with Zn–N₄ configuration has a lower energy barrier for the formation of *NNH intermediate compared with pure N-doped carbon nanosheets (N-C NSs), thus promoting the hydrogenation kinetics in the whole nitrogen reduction reaction process.

Keywords

electrocatalysis / nitrogen reduction / single-atom catalyst / Zn–N ₄

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Yanjiao Wei, Xinyu Wang, Mengjie Sun, Min Ma, Jian Tian, Minhua Shao. Atomically Dispersed Zinc Active Sites Efficiently Promote the Electrochemical Conversion of N₂ to NH₃. Energy & Environmental Materials, 2024, 7(3): 12630 DOI:10.1002/eem2.12630

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