Over 56.55% Faradaic efficiency of ambient ammonia synthesis enabled by positively shifting the reaction potential
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Open Access
- 20 January 2019
- journal article
- research article
- Published by Springer Science and Business Media LLC in Nature Communications
- Vol. 10 (1), 1-8
- https://doi.org/10.1038/s41467-018-08120-x
Abstract
Ambient electrochemical N-2 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 (NH4+)-N-15 in an isotopic labeling experiment confirms reliable NH3 production data. Molecular dynamics simulations suggest efficient N-2 access to the single-atom iron with only a small energy barrier, which benefits preferential N-2 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.Keywords
This publication has 29 references indexed in Scilit:
- Progress in the Electrochemical Synthesis of AmmoniaCatalysis Today, 2017
- Nanostructured photoelectrochemical solar cell for nitrogen reduction using plasmon-enhanced black siliconNature Communications, 2016
- Challenges in reduction of dinitrogen by proton and electron transferChemical Society Reviews, 2014
- Photo-illuminated diamond as a solid-state source of solvated electrons in water for nitrogen reductionNature Materials, 2013
- An Earth-system perspective of the global nitrogen cycleNature, 2008
- Trends in the Exchange Current for Hydrogen EvolutionJournal of the Electrochemical Society, 2005
- Hydrogenation and cleavage of dinitrogen to ammonia with a zirconium complexNature, 2004
- Electrosynthesis of ammoniaNature, 1985
- Microbial production of ammonium ion from nitrogen.Proceedings of the National Academy of Sciences of the United States of America, 1975
- Spectrophotometric Method for Determination of HydrazineAnalytical Chemistry, 1952