Monodisperse Cu Cluster-Loaded Defective ZrO2 Nanofibers for Ambient N2 Fixation to NH3

Electrocatalytic nitrogen reduction to ammonia has attracted increasing attention as it is more energy-saving and eco-friendly. For this endeavor, the development of high-efficiency electrocatalysts with excellent selectivity and stability is indispensable to break up the stable covalent triple bond in nitrogen. In this study, we report monodisperse Cu clusters loaded on defective ZrO2 nanofibers for nitrogen reduction under mild conditions. Such an electrocatalyst achieves an NH3 yield rate of 12.13 mu g h(-1) mg(cat).(-1) and an optimal Faradaic efficiency of 13.4% at -0.6 V versus the reversible hydrogen electrode in 0.1 M Na2SO4. Density functional theory calculations reveal that the N-2 molecule was reduced to NH3 at the Cu active site with an ideal overpotential. Meanwhile, the interaction between bonding and antibonding of the Cu-N bond promotes activation of N-2 and maintains a low desorption barrier.

Automated summary

In this study, monodisperse Cu clusters loaded on defective ZrO2 nanofibers were used as an electrocatalyst for nitrogen reduction, achieving high NH3 yield rate and optimal Faradaic efficiency. Density functional theory calculations revealed that N-2 molecule was reduced to NH3 at Cu active site with an ideal overpotential. The interaction between bonding and antibonding of Cu-N bond promoted activation of N-2 and maintained a low desorption barrier.