Electrocatalytic
nitrogen reduction reaction (NRR) represents a
highly promising process to ammonia synthesis for artificial N2 fixation. However, the yield rate for NH3 production
and Faradaic efficiency (FE) are still low, which greatly hinder its
widespread applications. Until now, although a variety of catalysts,
including single-atom catalysts, have been developed for NRR in the
pursuit of suppressing hydrogen evolution reaction (HER) and the corresponding
higher FE, the limited NH3 yield rate makes them uncompetitive
for the synthesis of ammonia. Herein, we report a Fe single-atom catalyst
anchoring on a nitrogen-doped carbon substrate (Fe SAC/N–C)
as a highly efficient NRR catalyst. The catalyst achieves a high FE
of 39.6% in 0.1 M KOH under room temperature, particularly a dramatically
enhanced NH3 yield rate of 53.12 μgNH3
h–1 mgcat
–1. The isotopic labeling (15N2) experiment confirms
that the NH3 production completely originates from N2 reduction. Meanwhile, theoretical calculations and X-ray
fine structure analysis reveal that the Fe–N3 coordination
of Fe SAC/N–C is indeed responsible for the suppression of
HER, particularly resulting in a maximum activation of NRR intermediates
to produce ammonia with a high yield rate.
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