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Efficient ammonia synthesis from the air using tandem non-thermal plasma and electrocatalysis at ambient conditions

Author

Listed:
  • Wei Liu

    (Xi’an Jiaotong University)

  • Mengyang Xia

    (Xi’an Jiaotong University)

  • Chao Zhao

    (Xi’an Jiaotong University)

  • Ben Chong

    (Xi’an Jiaotong University)

  • Jiahe Chen

    (Xi’an Jiaotong University)

  • He Li

    (Xi’an Jiaotong University)

  • Honghui Ou

    (Xi’an Jiaotong University)

  • Guidong Yang

    (Xi’an Jiaotong University)

Abstract

While electrochemical N2 reduction presents a sustainable approach to NH3 synthesis, addressing the emission- and energy-intensive limitations of the Haber-Bosch process, it grapples with challenges in N2 activation and competing with pronounced hydrogen evolution reaction. Here we present a tandem air-NOx-NOx−-NH3 system that combines non-thermal plasma-enabled N2 oxidation with Ni(OH)x/Cu-catalyzed electrochemical NOx− reduction. It delivers a high NH3 yield rate of 3 mmol h−1 cm−2 and a corresponding Faradaic efficiency of 92% at −0.25 V versus reversible hydrogen electrode in batch experiments, outperforming previously reported ones. Furthermore, in a flow mode concurrently operating the non-thermal plasma and the NOx− electrolyzer, a stable NH3 yield rate of approximately 1.25 mmol h−1 cm−2 is sustained over 100 h using pure air as the intake. Mechanistic studies indicate that amorphous Ni(OH)x on Cu interacts with hydrated K+ in the double layer through noncovalent interactions and accelerates the activation of water, enriching adsorbed hydrogen species that can readily react with N-containing intermediates. In situ spectroscopies and density functional theory (DFT) results reveal that NOx− adsorption and their hydrogenation process are optimized over the Ni(OH)x/Cu surface. This work provides new insights into electricity-driven distributed NH3 production using natural air at ambient conditions.

Suggested Citation

  • Wei Liu & Mengyang Xia & Chao Zhao & Ben Chong & Jiahe Chen & He Li & Honghui Ou & Guidong Yang, 2024. "Efficient ammonia synthesis from the air using tandem non-thermal plasma and electrocatalysis at ambient conditions," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47765-9
    DOI: 10.1038/s41467-024-47765-9
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