Abstract
It is of great significance to controlled synthesis of high activity, selectivity and durable electrocatalysts. In this work, for the first time, the ultrathin (0.9 nm) of interstitial metallene with controlled vacancies and lattice hydrogen atoms are successfully gained. With the optimal lattice hydrogen atoms and composition, the interstitial VPd-PdH0.41 metallene exhibits the great nitrogen reduction (NRR) activity in Li2SO4 solution, among interstitial PdHx with different extent of vacancies, interstitial PdH0.41 without vacancies and Pd nansheets. The density functional theory (DFT), in situ Raman and Attenuated total reflection surface-enhanced infrared absorption spectrum (ATR-SEIRAS) tests further display that the VPd on the interstitial VPd-PdH0.41 metallene can urges the adsorption and arousal of N2, while lattice hydrogen atoms as active hydrogen source to follow an association mechanism rather than a dissociation mechanism, showing nice NRR performance at low overpotential.
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