Abstract

AbstractAmbient NH3 electrosynthesis from NO reduction reaction (NORR) is attractive in replacing the industrial Haber‐Bosch route; however, the competitive hydrogen evolution reaction (HER) in aqueous electrolyte typically induces a limited selectivity and activity toward NH3 production. Herein, hierarchical P‐doped MoS2 nanospheres are developed as the NORR electrocatalyst in an ionic liquid (IL) electrolyte for catalyzing the reduction of NO to NH3 with a maximal Faradaic efficiency of 69 % (−0.6 V vs RHE) and a peak yield rate of 388.3 μg h−1 mgcat.−1 (−0.7 V vs RHE), both of which are comparable to the best‐reported results. Moreover, the catalyst also shows stable NORR activity over 30 h and 6 cycles. Theoretical analyses further reveal that the P dopants in MoS2 facilitate the activation and hydrogenation of NO. Besides, the employment of hydrophobic IL electrolyte also slows down the HER kinetics effectively.

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