The discovery of stable and noble-metal-free catalysts toward efficient electrochemical reduction of nitrogen (N ) to ammonia (NH ) is highly desired and significantly critical for the earth nitrogen cycle. Here, based on the theoretical predictions, MoS is first utilized to catalyze the N reduction reaction (NRR) under room temperature and atmospheric pressure. Electrochemical tests reveal that such catalyst achieves a high Faradaic efficiency (1.17%) and NH yield (8.08 × 10 mol s cm ) at -0.5 V versus reversible hydrogen electrode in 0.1 m Na SO . Even in acidic conditions, where strong hydrogen evolution reaction occurs, MoS is still active for the NRR. This work represents an important addition to the growing family of transition-metal-based catalysts with advanced performance in NRR.
Conversion of naturally abundant nitrogen to ammonia is a key (bio)chemical process to sustain life and represents a major challenge in chemistry and biology. Electrochemical reduction is emerging as a sustainable strategy for artificial nitrogen fixation at ambient conditions by tackling the hydrogen- and energy-intensive operations of the Haber–Bosch process. However, it is severely challenged by nitrogen activation and requires efficient catalysts for the nitrogen reduction reaction. Here we report that a boron carbide nanosheet acts as a metal-free catalyst for high-performance electrochemical nitrogen-to-ammonia fixation at ambient conditions. The catalyst can achieve a high ammonia yield of 26.57 μg h–1 mg–1cat. and a fairly high Faradaic efficiency of 15.95% at –0.75 V versus reversible hydrogen electrode, placing it among the most active aqueous-based nitrogen reduction reaction electrocatalysts. Notably, it also shows high electrochemical stability and excellent selectivity. The catalytic mechanism is assessed using density functional theory calculations.
It is vitally essential
to design highly efficient and cost-effective
bifunctional electrocatalysts toward water splitting. Herein, we report
the development of P-doped Co3O4 nanowire array
on nickel foam (P-Co3O4/NF) from Co3O4 nanowire array through low-temperature annealing, using
NaH2PO2 as the P source. As a 3D catalyst, such
P-Co3O4/NF demonstrates superior performance
for oxygen evolution reaction with a low overpotential (260 mV at
20 mA cm–2), a small Tafel slope (60 mV dec–1), and a satisfying durability in 1.0 M KOH. Density
functional theory calculations indicate that P-Co3O4 has a reaction free-energy value that is much smaller than
that of pristine Co3O4 for the potential determining
step of the oxygen evolution reaction. Such P-Co3O4/NF also performs efficiently for hydrogen evolution reaction,
and a two-electrode alkaline electrolyzer assembled by P8.6-Co3O4/NF as both anode and cathode needs only
1.63 V to reach a water-splitting current of 10 mA cm–2.
MoO3 nanosheets act as an efficient electrocatalyst for N2 fixation to NH3 with excellent selectivity at ambient conditions. In 0.1 M HCl, they show high activity with an NH3 yield of 4.80 × 10−10 mol s−1 cm−2 (29.43 μg h−1 mgcat.−1) and a faradaic efficiency of 1.9%.
The synthesis of
NH3 is mainly dominated by the traditional
energy-consuming Haber–Bosch process with a mass of CO2 emission. Electrochemical conversion of N2 to
NH3 emerges as a carbon-free process for the sustainable
artificial N2 reduction reaction (NRR), but requires an
efficient and stable electrocatalyst. Here, we report that the Mo2C nanorod serves as an excellent NRR electrocatalyst for artificial
N2 fixation to NH3 with strong durability and
acceptable selectivity under ambient conditions. Such a catalyst shows
a high Faradaic efficiency of 8.13% and NH3 yield of 95.1
μg h–1 mg–1cat at −0.3 V in 0.1 M HCl, surpassing the majority of reported
electrochemical conversion NRR catalysts. Density functional theory
calculation was carried out to gain further insight into the catalytic
mechanism involved.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.