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.
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%.
Electrochemical N 2 reduction reaction (NRR) under ambient conditions offers us an environmentally friendly route for artificial synthesis of NH 3 . However, up to now, few noble-metal-free electrocatalysts with satisfactory catalytic activities have been explored. In this Letter, we demonstrate that MoN nanosheets array on carbon cloth (MoN NA/CC) acts as a high-performance NRR electrocatalyst toward NH 3 electrosynthesis in 0.1 M HCl under ambient conditions. This catalyst achieves a large NH 3 yield of 3.01 × 10 −10 mo1 s −1 cm −2 and a Faradaic efficiency of 1.15% at −0.3 V vs reversible hydrogen electrode with strong electrochemical durability and selectivity. Density functional theory calculations reveal that MoN NA/CC catalyzes NRR via the Mars−van Krevelen mechanism.
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