Abstract
The synthesis of intermetallic compounds with small size and defective structures is rigorous challenge. In this work, the small size (< 10 nm) of intermetallic PdM (M = Pb, Sn, In) with ordered vacancies (OVs) are successfully prepared by ultrafast and solvent-free microwave method for the first time. With the optimized vacancies, atomic arrangement and components, the intermetallic OVs-Pd3Pb-2 shows the best nitrogen reduction (NRR) performance among intermetallic OVs-PdM (M = Sn, In), intermetallic OVs-Pd3Pb with various degrees of vacancies, intermetallic Pd3Pb with vacancies-free, Pd3Pb/CNT and Pd/CNT in Li2SO4 solution. In situ Raman spectroscopy, in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) technique and density functional theory (DFT) further demonstrate the synergy mechanism of good NRR activity at low overpotentials on OVs-Pd3Pb-2 catalysts.
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