Reduction of nitrogen to ammonia under mild conditions
is recognized
as one key step in the NH3-economy. The Haber–Bosch
process, the typical ammonia production technique, is energy-intensive
and high carbon-emitting. Intense efforts have been devoted to searching
for sustainable options for decarbonized ammonia generation. Wherein,
the electrocatalytic nitrogen fixation route driven by renewable energy
is extremely anticipated. Herein, the integrated concept for ammonia
production powered by direct solar energy is outlined and proposed.
Responding to the limited yield rate and reasonable Faraday efficiency
in ammonia synthesis, non-precious Cu-electrocatalysts with porous
carbon as substrates are fabricated and Ce is introduced as a modulator
which could facilitate electron conduction and nitrogen trapping.
By optimizing the proportion of metal sources, strongly synergistic
metallic effect of Ce and Cu is structured, further enhancing nitrogen
reduction performance of electrocatalysts and inhibiting hydrogen
evolution reaction. A satisfactory NH3 yield rate of 30.60
± 3.04 μg h–1 mgcat
–1 is achieved at −0.3 V vs reversible hydrogen electrode (RHE)
in 0.1 M KOH and the corresponding FE is about 8.20 ± 0.22%.
The solar self-driven NH3 generation system presents a
total yield of 104 μg mgcat
–1 and
a solar-to-ammonia efficiency of 1% at ∼1.2 V in daylight.
This work offers a rational energy-utilizing strategy for the preparation
of high-grade NH3 chemical via solar system employing non-precious
metal catalysts in zero-carbon emission footprint.