Journal
NATURE COMMUNICATIONS
Volume 10, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-018-08120-x
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Funding
- National Natural Science Foundation of China [51622208, 21703149, 51872193]
- Shanghai Synchrotron Radiation Facility (SSRF)
- Taiwan Light Source (TLS)
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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.
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