In:
Nature Communications, Springer Science and Business Media LLC, Vol. 10, No. 1 ( 2019-01-21)
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 15 NH 4 + in an isotopic labeling experiment confirms reliable NH 3 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.
Type of Medium:
Online Resource
ISSN:
2041-1723
DOI:
10.1038/s41467-018-08120-x
Language:
English
Publisher:
Springer Science and Business Media LLC
Publication Date:
2019
detail.hit.zdb_id:
2553671-0
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