Electrocatalytic conversion of widely distributed nitrate
from
industrial wastewater into value-added ammonia was proposed as an
attractive and sustainable alternative to harvesting green ammonia.
Herein, CuCo alloys were facilely synthesized for nitrate conversion,
while nonthermal Ar-plasma was employed to enhance the adhesion strength
between the electrocatalyst and substrate interface via regulating
the surface hydrophobicity and roughness. Based on Ar-plasma treatment,
a high ammonia yield rate (5129.29 μg cm–2 h–1) was achieved using Cu30Co70 electrocatalyst −0.47 V vs RHE, while nearly 100%
of Faradaic efficiency was achieved using Cu50Co50 electrocatalyst at −0.27 V vs RHE (reversible hydrogen electrode).
Validated by in situ spectroscopy and density functional theory calculations,
the high activity of the CuCo alloy was derived from the regulation
of Co to weaken the strong adsorption capacity of Cu and the shift
of the d-band center to lower the energy barrier, while Ar-plasma
modification promoted the formation of *NO to boost nitrate conversion.
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