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Electrochemical nitrogen reduction reaction (eNRR) offers a sustainable route for ammonia synthesis; however, current electrocatalysts are limited in achieving optimal performance within narrow potential windows. Herein, inspired by the heliotropism of sunflowers, we present a biomimetic design of Ru-VOH electrocatalyst, featuring a dynamic Ru–O–V pyramid electron bridge for eNRR within a wide potential range. In situ spectroscopy and theoretical investigations unravel the fact that the electrons are donated from Ru to V at lower overpotentials and retrieved at higher overpotentials, maintaining a delicate balance between N2 activation and proton hydrogenation. Moreover, N2 adsorption and activation were found to be enhanced by the Ru–O–V moiety. The catalyst showcases an outstanding Faradaic efficiency of 51.48% at −0.2 V (vs RHE) with an NH3 yield rate exceeding 115 μg h–1 mg–1 across the range of −0.2 to −0.4 V (vs RHE), along with impressive durability of over 100 cycles. This dynamic M–O–V pyramid electron bridge is also applicable to other metals (M = Pt, Rh, and Pd).
Sun et al. (Wed,) studied this question.