Bionic Design of a Mo(IV)-Doped FeS₂ Catalyst for Electroreduction of Dinitrogen to Ammonia

Abstract

Highly effective catalysts are of great importance for artificial nitrogen fixation. Inspired by the natural nitrogenase, we biomimetically designed an inorganic catalyst, Mo­(IV)-doped FeS2, for electroreduction of dinitrogen to ammonia. The Mo­(IV) ions favor the adsorption and activation of N2, while the FeS2 substrate depresses the competitive hydrogen evolution reaction, and the two factors jointly endow the catalyst with a high Faraday efficiency of 14.41% at −0.2 V versus RHE.

Intrinsic Electron Localization of Metastable MoS2 Boosts Electrocatalytic Nitrogen Reduction to Ammonia

“…[ 26,27 ] Therefore, lots of efforts including heteroatom doping and defect engineering are made to strengthen the MoN interaction to enhance NRR activity. [ 26–29 ] In fact, there is still a gap with the actual application due to the insufficient catalyst efficiency as well as the lack of understanding the mechanism of the NRR. Basically, most of the latest works on MoS 2 for NRR are based on stable 2H phase only.…”

Multi‐Site Electrocatalysts Boost pH‐Universal Nitrogen Reduction by High‐Entropy Alloys

“…[ 10–13 ] Later, new ammonia production methods appeared. [ 14–17 ] Electrocatalytic nitrogen reduction reaction (NRR) is a nitrogen fixation technology that generates NH 3 under relatively mild conditions using N 2 and water as raw materials. [ 18–20 ] It has become a new research hotspot in the field of electrocatalysis due to its environmentally friendly characteristics.…”

FeTe2 as an earth-abundant metal telluride catalyst for electrocatalytic nitrogen fixation

“…Fe-based organometallic or homogeneous catalysts are known to be effective NRR catalysts but have the inherent drawbacks of poor stability, complicated synthesis and difficulty in grafting them onto electrodes [25]. Promisingly, these issues can be well alleviated in the heterogeneous catalysts and thus great efforts have been recently devoted to developing Febased heterogeneous catalysts, especially Fe oxides (Fe 2 O 3 [26][27][28][29], F 3 O 4 [30,31]) and sulfides (FeS 2 [32][33][34], Fe 3 S 4 [35]). Nonetheless, the NRR activity of these Fe oxides/sulfides is still much unsatisfactory for either NH 3 production rate or Faradaic efficiency (FE) due possibly to their low conductivity and poor intrinsic activity.…”