Abstract
Ammonia is a key chemical feedstock worldwide. Compared with the well-known Haber-Bosch method, electrocatalytic nitrogen reduction reaction (ENRR) can eventually consume less energy and have less CO2 emission. In this study, a plasma-enhanced chemical vapor deposition method is used to anchor transition metal element onto 2D conductive material. Among all attempts, Ru single-atom and Ru-cluster-embedded perovskite oxide are discovered with promising electrocatalysis performance for ENRR (NH3 yield rate of up to 137.5±5.8µgh-1 mgcat -1 and Faradaic efficiency of unexpected 56.9±4.1%), reaching the top record of Ru-based catalysts reported so far. In situ experiments and density functional theorycalculations confirm that the existence of Ru clusters can regulate the electronic structure of Ru single atoms and decrease the energy barrier of the first hydrogenation step (*NN to *NNH). Anchoring Ru onto various 2D perovskite oxides (LaMO-Ru, MCr, Mn, Co, or Ni) also show boosted ENRR performance. Not only this study provides an unique strategy toward transition-metal-anchored new 2D conductive materials, but also paves the way for fundamental understanding the correlation between cluster-involved single-atom sites and catalytic performance.
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