Ionic Liquid‐Assisted Electrocatalytic NO Reduction to NH₃ by P‐Doped MoS₂

Abstract

Ambient NH 3 electrosynthesis from NO reduction reaction (NORR) is attractive in replacing the industrial Haber-Bosch route; however, the competitive hydrogen evolution reaction (HER) in aqueous electrolyte typically induces a limited selectivity and activity toward NH 3 production. Herein, hierarchical P-doped MoS 2 nanospheres are developed as the NORR electrocatalyst in an ionic liquid (IL) electrolyte for catalyzing the reduction of NO to NH 3 with a maximal Faradaic efficiency of 69 % (À 0.6 V vs RHE) and a peak yield rate of 388.3 μg h À 1 mg cat.À 1 (À 0.7 V vs RHE), both of which are comparable to the best-reported results. Moreover, the catalyst also shows stable NORR activity over 30 h and 6 cycles. Theoretical analyses further reveal that the P dopants in MoS 2 facilitate the activation and hydrogenation of NO. Besides, the employment of hydrophobic IL electrolyte also slows down the HER kinetics effectively.

Asymmetric Coordination Environment Engineering of Atomic Catalysts for CO2 Reduction

“…For over a decade, significant advancements have been accomplished in the structural design and fundamental electrocatalytic investigation of SACs as next-generation catalysts with a maximum of nearly 100% atomic utilization [ 139 , 140 , 141 ]. However, for the CO 2 RR, the simplicity of the conventional MN 4 structure severely restricts the substantial improvement of its electrocatalytic activity.…”

Self‐Supported Pd Nanorod Arrays for High‐Efficient Nitrate Electroreduction to Ammonia

“…[ 1–5 ] However, the classic Haber–Bosh process, which accounts for the majority of ammonia production and the 2% global energy usage, causes severe environmental issues and affects people's health and normal life. [ 6–9 ] Renewable electricity such as wind and solar energy, offers the available energy sources for the electrocatalytic nitrate (NO 3 − ) reduction reaction (NO 3 − RR), which is considered to be a sustainable alternative to the energy‐intensive Haber–Bosh process. [ 10–12 ] Then NO 3 − becomes a more suitable source material for NH 3 synthesis owing to its high solubility in aqueous solvents.…”

“…[1][2][3][4][5] However, the classic Haber-Bosh process, which accounts for the majority of ammonia production and the 2% global energy usage, causes severe environmental issues and affects people's health and normal life. [6][7][8][9] Renewable electricity such as wind and solar energy, offers the available energy sources for the electrocatalytic nitrate (NO 3…”

Main-group indium single-atom catalysts for electrocatalytic NO reduction to NH3

“…Diverse transition metal-based materials have been reported as active NORR catalysts, [26][27][28][29] by virtue of their partially occupied d-orbitals to enhance NO adsorption and dissociation. Nonetheless, d-orbitals also contribute to *H binding on the catalyst surface, which is benecial for the competitive HER and unfavorable for FE NH 3 .…”