Litcius/Paper detail

Biomimetic Design of a Dynamic M–O–V <i>Pyramid</i> Electron Bridge for Enhanced Nitrogen Electroreduction

Yuntong Sun, Xuheng Li, Zhiqi Wang, Lili Jiang, Bingbao Mei, Wenjun Fan, Junjie Wang, Junwu Zhu, Jong‐Min Lee

2024Journal of the American Chemical Society72 citationsDOI

Abstract

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 N 2 activation and proton hydrogenation. Moreover, N 2 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 NH 3 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).

Topics & Concepts

ChemistryFaraday efficiencyElectrocatalystCatalysisElectrochemistryAmmonia productionNitrogenElectron transferNanotechnologyPhotochemistryElectrodePhysical chemistryMaterials scienceOrganic chemistryAmmonia Synthesis and Nitrogen ReductionAdvanced Photocatalysis TechniquesNanomaterials for catalytic reactions