Over 56.55% Faradaic efficiency of ambient ammonia synthesis enabled by positively shifting the reaction potential

Mengfan Wang, Sisi Liu, Tao Qian (), Jie Liu, Jinqiu Zhou, Haoqing Ji, Jie Xiong, Jun Zhong and Chenglin Yan ()
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Mengfan Wang: Soochow University
Sisi Liu: Soochow University
Tao Qian: Soochow University
Jie Liu: Soochow University
Jinqiu Zhou: Soochow University
Haoqing Ji: Soochow University
Jie Xiong: University of Electronic Science and Technology of China
Jun Zhong: Soochow University
Chenglin Yan: Soochow University

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract Ambient electrochemical N2 reduction is emerging as a highly promising alternative to the Haber–Bosch process but is typically hampered by a high reaction barrier and competing hydrogen evolution, leading to an extremely low Faradaic efficiency. Here, we demonstrate that under ambient conditions, a single-atom catalyst, iron on nitrogen-doped carbon, could positively shift the ammonia synthesis process to an onset potential of 0.193 V, enabling a dramatically enhanced Faradaic efficiency of 56.55%. The only doublet coupling representing 15NH4+ in an isotopic labeling experiment confirms reliable NH3 production data. Molecular dynamics simulations suggest efficient N2 access to the single-atom iron with only a small energy barrier, which benefits preferential N2 adsorption instead of H adsorption via a strong exothermic process, as further confirmed by first-principle calculations. The released energy helps promote the following process and the reaction bottleneck, which is widely considered to be the first hydrogenation step, is successfully overcome.

Date: 2019
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DOI: 10.1038/s41467-018-08120-x

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