Reversible hydrogen electrode

Yield (engineering)

Nanotechnology

Electrode

Organic chemistry

Nitrogen fixation

Fluorine

Hydrogen

Nitrogenase

Nanorod

Engineering

Faraday efficiency

Catalysis

Physical chemistry

Inorganic chemistry

Chemistry

Metallurgy

Materials science

Reference electrode

Chemical engineering

Optoelectronics

Electrochemistry

Nitrogen

Doping

Chemical Communications

As the cheapest and one of the most abundant transition metals, Fe is not only involved in nitrogenases for biological N2 fixation but is also extensively utilized in the Haber-Bosch process for industrial-scale NH3 synthesis. However, the application of Fe-based electrocatalysts for ambient N2-to-NH3 conversion still requires exploration of effective strategies to boost the catalytic performances for simultaneously achieving a large NH3 yield and a high Faradaic efficiency (FE). Here, we report that the ambient electrocatalytic N2 reduction activity of a β-FeOOH nanorod can be greatly improved by fluorine doping. When tested at -0.60 V vs. reversible hydrogen electrode (RHE) in 0.5 M LiClO4, such a β-FeO(OH,F) nanorod obtains an optimal NH3 yield (42.38 μg h-1 mgcat.-1) and FE (9.02%), much higher than those of pristine β-FeOOH (10.01 μg h-1 mgcat.-1, 2.16%). Density functional theory calculations reveal that the enhancement in activity originates from the lower reaction energy barrier (0.24 eV) of the nanorod than that of β-FeOOH (0.59 eV).

Boosting electrocatalytic N<sub>2</sub> reduction to NH<sub>3</sub> on β-FeOOH by fluorine doping

Boosting electrocatalytic N2 reduction to NH3 on β-FeOOH by fluorine doping

Boosting electrocatalytic N₂ reduction to NH₃ on β-FeOOH by fluorine doping