Ambient N₂ fixation to NH₃ electrocatalyzed by a spinel Fe₃O₄ nanorod

Abstract

Industrially, NH3 is mainly produced via the Haber-Bosch process which is not only energy-consuming but emits a large amount of CO2. Electrochemical reduction is regarded as an environmentally-benign alternative for sustainable NH3 synthesis, and its efficiency heavily depends on the identification of Earth-abundant catalysts with high activity for the N2 reduction reaction (NRR). In this work, we report that a spinel Fe3O4 nanorod on a Ti mesh (Fe3O4/Ti) acts as an efficient and durable NRR electrocatalyst under ambient conditions. When tested in 0.1 M Na2SO4, such Fe3O4/Ti achieves a high faradaic efficiency of 2.6% and a NH3 yield 5.6 × 10-11 mol s-1 cm-2 and at -0.4 V vs. a reversible hydrogen electrode.

Nitrogen‐Doped NiO Nanosheet Array for Boosted Electrocatalytic N2 Reduction

“…The detailed comparison is provided in Table S1 (Supporting Information). Nevertheless, at potentials more negative than −0.5 V, the NH 3 yield and FE of N‐NiO/CC both decrease remarkably, which are ascribed mainly to the elevation of the selectivity toward competing HER at more negative potential, leading to the hindrance of efficient N 2 adsorption and activation. The NRR performance of N‐NiO/CC is further compared with that of NiO/CC without N‐doping at the same potential ranges (Figure S15).…”

A Biomass‐Derived Carbon‐Based Electrocatalyst for Efficient N2 Fixation to NH3 under Ambient Conditions

“…Electrochemical N 2 reduction is regarded as a sustainable alternative for ambient NH 3 production, but efficient electrocatalysts are needed to meet the challenge to break the strong N≡N triple bond of N 2 . Up till now, great efforts have been made to explore earth‐abundant transition‐metal‐based catalyst materials . Nevertheless, transition metals that bind N 2 too weakly have poor capability for activating N 2 .…”

Greatly Improving Electrochemical N2 Reduction over TiO2 Nanoparticles by Iron Doping

“…[5][6][7][8] Noble metals perform the NRR efficiently;however, their scarcity and high cost limits their application in large-scale N 2 reduction. [33] Fe compounds have been widely utilized as catalysts for artificial N 2 fixation in the Haber-Bosch [4] and electrochemical [34][35][36][37][38][39] processes.I ti st hus natural for us to explore use of Fe as ad opant for TiO 2 ,w hich has not been reported before.Herein, we report on our recent experimental results that Fe-doped TiO 2 is superior in performances for electrocatalytic N 2 reduction under ambient conditions.I n 0.5 m LiClO 4 ,t his catalyst achieves ah igh FE of 25.6 %a nd al arge NH 3 yield of 25.47 mgh À1 mg cat À1 at À0.40 Vv ersus ar eversible hydrogen electrode (RHE), outperforming pristine TiO 2 as well as all Ti-and Fe-based NRR electrocatalysts reported to date.Remarkably,the catalyst also demonstrates high electrochemical and structural stability.T he NRR mechanism on the Fe-doped TiO 2 (101) surface is further discussed using density function theory (DFT) calculations. [12][13][14][15][16][17][18][19][20][21][22][23][24] TiO 2 is highly adaptable as asemiconductor catalyst because of its long-term thermodynamic stability,n atural abundance,a nd nontoxicity.…”