Engineering the Metal‐Support Interaction and Oxygen Vacancies on Ru@P‐Fe/Fe3O4 Nanorods for Synergetic Enhanced Electrocatalytic Nitrate‐to‐Ammonia Conversion
Advanced Functional Materials(2024)
摘要
AbstractRuthenium (Ru) loaded catalysts show high activity and selectivity for ammonia (NH3) synthesis via electrochemical reduction of nitrate (NO3−), but their practical application is still restricted by their high cost and insufficient stability. Herein, a multi‐component electrocatalyst of Ru nanoclusters loaded on phosphorus‐doped/phosphate‐modified and oxygen vacancy (OV)‐rich Fe/Fe3O4 composite nanorods (Ru@P‐Fe/Fe3O4) to synergistically promote electrocatalytic NO3− reduction reaction (NO3−RR)‐to‐NH3 performance via strong metal‐support interaction (SMSI) is reported. Impressively, the best Ru@P‐Fe/Fe3O4 catalyst exhibits outstanding NO3−RR activity, selectivity, and durability in 0.1 M KNO3 + 0.5 M KOH solution, with an NH3 yield rate of 14.37 ± 0.21 mgNH3 h−1 cm−2 (1710.71 ± 25 mgNH3 h−1 mgRu−1) at −0.75 V versus reversible hydrogen electrode (vs. RHE), an NH3 Faradaic efficiency (FE) of 97.2% at −0.55 V vs. RHE, and a superior stability over 50 h, suppressing most of reported Fe‐based and Ru‐based electrocatalysts. The characterizations and theoretical calculations unveil that the SMSI between Ru nanoclusters and P‐Fe/Fe3O4 composite nanorods can promote the generation of OV, tune the electronic structure of Ru species, and stabilize Ru nanoclusters, thereby reducing the reaction energy barrier of NO3−RR‐to‐NH3, inhibiting the competitive hydrogen evolution reaction, and boosting the NH3 yield rate NH3 FE, and stability.
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