Urea
(CO(NH2)2) is the most common
nitrogen
fertilizer that is promoting food production worldwide due to its
high nitrogen content. However, the conventional urea synthesis involving
hydrogenolysis of nitrogen and C–N bond coupling requires harsh
conditions and a massive carbon footprint. Herein, we report a promising
technology for the green synthesis of urea using nitrate (NO3
–) and carbon dioxide (CO2) under ambient
conditions over Ru/Pt/Pd-modified three-dimensional copper foam (Ru/Pt/Pd-Cu
CF) electrode. The Ru-Cu CF catalyst delivers a high urea yield of
151.6 μg h–1 cm–2 at a low
onset potential of −0.3 V vs Ag/AgCl (0.13 V vs RHE) as well
as an FE of 25.4%, surpassing that of Pt/Pd-Cu CF. Moreover, it is
confirmed by operando electrocatalytic Raman spectroscopy
and theoretical calculations that the *COOH intermediate is the rate-determining
step of C–N bond coupling. Benefiting from the partial 3d states
of surface Ru sites, the Ru-Cu CF electrode possesses the lowest formation
energy of the *COOH intermediate to accelerate the urea synthesis.
This work provides an extraordinarily sustainable strategy for green
urea synthesis.
Mesoporous polydopamine/titanium dioxide (PDA/TiO2)
composite nanospheres with different polydopamine content were successfully
synthesized by a facile organic–inorganic self-assembly method.
The synthesized composite materials were characterized by N2 adsorption–desorption isotherm, X-ray photoelectron spectroscopy,
X-ray diffraction, transmission electron microscopy (TEM), energy
dispersive spectrometry, field emission scanning electron microscopy,
Fourier transform infrared spectroscopy, ζ--potential, and cyclic voltammetry. The results showed that the composite
material with the most exposure active site exhibits a spherical morphology.
The composite material could also be used as a reducing agent, and
spheres of the composite material were used as adsorbents for removing
hexavalent chromium from aqueous solutions by reducing Cr(VI) to Cr(III).
The influence of factors, including the initial solution pH, contact
time, initial ion concentration, temperature, coexisting ions, and
dose of adsorbent, was also studied. The hexavalent chromium adsorption
data fit well to a Langmuir isotherm model, and the maximum adsorption
capacity was shown to be 244.5 mg/g. The kinetics data follow a pseudo-second-order
kinetic model. The study of thermodynamics indicated that the adsorption
on the composite nanospheres was a spontaneous and endothermic process.
Moreover, a mechanism of adsorption and reduction on the composite
spheres was proposed.
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