Electrocatalytic nitrogen reduction reaction (NRR) is a promising approach for renewable NH 3 production, while developing the NRR electrocatalysis systems with both high activity and selectivity remains a significant challenge. Herein, we combine catalyst and electrolyte engineering to achieve a high-efficiency NRR enabled by a Se-vacancy-rich WSe 2−x catalyst in water-in-salt electrolyte (WISE). Extensive characterizations, theoretical calculations, and in situ X-ray photoelectron/Raman spectroscopy reveal that WISE ensures suppressed H 2 evolution, improved N 2 affinity on the catalyst surface, as well as an enhanced π-back-donation ability of active sites, thereby promoting both activity and selectivity for the NRR. As a result, an excellent faradaic efficiency of 62.5% and NH 3 yield of 181.3 μg h −1 mg −1 is achieved with WSe 2−x in 12 m LiClO 4 , which is among the highest NRR performances reported to date.
Electrocatalytic
NO reduction to NH3 (NORR)
offers a
prospective approach to attain both harmful NO removal and efficient
NH3 electrosynthesis. Main-group p-block metals are promising
NORR candidates but still lack adequate exploration. Herein, p-block
Sb single atoms confined in amorphous MoO3 (Sb1/a-MoO3) are designed as an efficient NORR catalyst, exhibiting
the highest NH3 yield rate of 273.5 μmol h–1 cm–2 and a NO-to-NH3 Faradaic efficiency
of 91.7% at −0.6 V vs RHE. In situ spectroscopic characterizations
and theoretical computations reason that the outstanding NORR performance
of Sb1/a-MoO3 arises from the isolated Sb1 sites, which can optimize the adsorption of *NO/*NHO to lower
the reaction energy barriers and simultaneously exhibit a higher affinity
to NO than to H2O/H species. Moreover, our strategy can
be extended to prepare Bi1/a-MoO3, showing a
high NORR property, demonstrating the immense potential of p-block
metal single-atom catalysts toward the high-performing NORR electrocatalysis.
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