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

Wei Liu, Mengyang Xia, Chao Zhao, Ben Chong, Jiahe Chen, He Li, Honghui Ou and Guidong Yang ()
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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

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-47765-9

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