Efficient conversion of CO2 to value-added
fuels or
chemicals using electricity from renewable sources is an appealing
approach to realize carbon neutrality. Under this background, it is
crucial to design efficient and low-cost catalysts for CO2 electroreduction. Herein, we fabricated an electrocatalyst with
the structure of Cu–Ni alloy nanoparticles grown on nitrogen-doped
carbon nanotubes (Cu
x
Ni/NCNT, x = 2.4, 1, and 0.36) for electrochemical CO2 reduction reaction (CO2RR) via a hydrothermal method
followed by pyrolysis. The optimized CuNi/NCNT demonstrates a favorable
CO2RR performance with a CO Faradaic efficiency (FECO) of 94.8% and a current density of 26.6 mA cm–2 at −0.9 V versus the reversible hydrogen electrode (vs RHE)
in the H-cell, far superior to those of single metal counterparts.
Density functional theory (DFT) calculations unravel that the Cu–Ni
alloys possess much lower free energy changes for the formation of
the key COOH* intermediate than those of the Cu metal, thereby facilitating
CO2 reduction into CO. Additionally, the CO2RR performance of CuNi/NCNT was further evaluated in the gas diffusion
electrode (GDE) involved in the flow cell to examine the practical
application of the prepared catalyst, which can deliver a current
density of 124.6 mA cm–2 with a FECO of
92.8% at −1.1 V vs RHE. This work enriches electrocatalysts
for highly efficient CO2 electroreduction to CO.
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