Abstract
It is a great challenge to design and synthesize catalysts that can regulate both adsorption and desorption processes for electrocatalytic nitrate reduction to ammonia (NRA). Herein, amorphous Cu-Ni-Al nanometallic glasses (NG) were synthesized using a facile thermal evaporation coupled Joule heating method. The Cu50Ni25Al25-NG exhibits remarkable Faradaic efficiency (98.81 %) and NH3 yield-rate (211.14 μmol h−1cm−2) at an outstanding positive potential of −0.15 V vs. RHE. Aluminum atoms of low work-function when intercalated at different positions in Cu50Ni25Al25-NG enhance both adsorption and desorption processes during NRA. The oscillatory properties of surface potential detected by Kelvin-probe force microscopy demonstrate the diversity of active sites on Cu50Ni25Al25-NG. Two potential-regulated reaction mechanisms in NRA on the surface of Cu50Ni25Al25-NG were proposed using in-situ electrochemical Raman spectra. This work provides a new method for the preparation of multi-element NG enriched with low work-function metals and a new idea for the synthesis of synergistic catalytic-sites for NRAs.
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