posted on 2021-08-23, 16:04authored byTingshuai Li, Jiaojiao Xia, Qiru Chen, Ke Xu, Yang Gu, Qian Liu, Yonglan Luo, Haoran Guo, Enrico Traversa
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 μg h–1 mgcat.–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 N2 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 N2 and maintains a low desorption
barrier.