Artificial electrocatalytic ammonia (NH3) synthesis is recently becoming a research hotspot. It can couple with clean renewable electricity, which is considered an energy-efficient and sustainable approach for regulating the recirculation of nitrogen species and meanwhile promoting the growth of a circular nitrogen economy. In this Account, we review recent advances in electrocatalytic ammonia synthesis. Firstly, we briefly introduce the research background and significance of three electrochemical NH3 synthesis routes: electrocatalytic nitrogen reduction, nitric oxide reduction, and nitrate/nitrite reduction. And then we give a detailed discussion of the latest research advances in electrocatalysts for ambient NH3 synthesis, mainly involving catalytic mechanisms, theoretical advances, and electrochemical performance. Finally, the existing challenges and future research needs for artificial electrosynthesis of NH3 are also highlighted. 

Recent advances in electrocatalytic ammonia synthesis

Recent developments in heterogeneous electrocatalysts for ambient nitrogen reduction to ammonia: Activity, challenges, and future perspectives

The reduction of molecular nitrogen (N2) to ammonia (NH3) under mild conditions is one of the most promising studies in the energy field due to the important role of NH3 in modern industry, production, and life. The photocatalytic reduction of N2 is expected to achieve clean and sustainable NH3 production by using clean solar energy. To date, the new photocatalysts for photocatalytic reduction of N2 to NH3 at room temperature and atmospheric pressure have not been fully developed. The major challenge is to achieve high light-absorption efficiency, conversion efficiency, and stability of photocatalysts. Herein, the methods for measuring produced NH3 are compared, and the problems related to possible NH3 pollution in photocatalytic systems are mentioned to provide accurate ideas for measuring photocatalytic efficiency. The recent progress of nitrogen reduction reaction (NRR) photocatalysts at ambient temperature and pressure is summarized by introducing charge transfer, migration, and separation in photocatalytic NRR, which provides guidance for the selection of future photocatalyst selection. More importantly, we introduce the latest research strategies of photocatalysts in detail, which can guide the preparation and design of photocatalysts with high NRR activity. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/cey2.305

Recent progress in research and design concepts for the characterization, testing, and photocatalysts for nitrogen reduction reaction

Anchoring Mo Single-Atom Sites on B/N Codoped Porous Carbon Nanotubes for Electrochemical Reduction of N2 to NH3

Synergistic Enhancement of Electrocatalytic Nitrogen Reduction over Few-Layer MoSe2-Decorated Ti3C2Tx MXene

Herein, we assemble semi-metallic 1T′ phase MoS 2 on the surface Ti 3 C 2 MXene (1T′-MoS 2 /Ti 3 C 2 composite) by one-step hydrothermal method for nitrogen fixation. 1T′-MoS 2 /Ti 3 C 2 composites present a high ammonia yield rate of 31.96 µg h −1 mg −1 cat. at − 0.95 V vs. RHE and a Faradaic efficiency (FE) of 30.75% at − 0.7 V, which is much better than pure 1T′-MoS 2 and pure Ti 3 C 2 MXenes alone. Furthermore, the 1T′-MoS 2 /Ti 3 C 2 composites exhibit good selectivity and stability with no significant decrease in ammonia yield rate and FE. Density functional theory (DFT) calculations reveal that 1T′-MoS 2 /Ti 3 C 2 composite makes the activation and further reduction of *N 2 more thermodynamically favorable than pure 1T′-MoS 2 . 1 5 N isotopic labeling experiment confirms that nitrogen in produced ammonia originates from N 2 in the electrolyte. • Semi-metallic 1T′ phase MoS 2 on Ti 3 C 2 MXene is active for electrocatalytic NRR. • 1T′-MoS 2 /Ti 3 C 2 composite achieves a large NH 3 yield of 31.96 µg h −1 mg −1 cat. . • 1T′-MoS 2 /Ti 3 C 2 composite attains a high Faradaic efficiency of 30.75%. • 1T′-MoS 2 /Ti 3 C 2 composite shows high electrochemical stability. 

Enabling efficient electrocatalytic conversion of N2 to NH3 by Ti3C2 MXene loaded with semi-metallic 1 T'-MoS2 nanosheets

https://www.cjcatal.com/EN/article/downloadArticleFile.do?attachType=PDF&id=26271

Heterostructuring 2D TiO2 nanosheets in situ grown on Ti3C2T MXene to improve the electrocatalytic nitrogen reduction

P-band center theory guided activation of MoS2 basal S sites for pH-universal hydrogen evolution

Constructing three-dimensional (3D) hierarchical heterostructures is an appealing but challenging strategy to improve the performance of catalysts for electrical energy devices. Here, an efficient and robust flexible self-supporting catalyst, interface coupling of ultrathin CoFe-LDH nanosheets and Co3O4 nanowire arrays on the carbon cloth (CC/Co3O4@CoFe-LDH), was proposed for boosting oxygen evolution reaction (OER) in rechargeable liquid/solid Zn-air batteries (ZABs). The strong interfacial interaction between the CoFe-LDH and Co3O4 heterostructures stimulated the charge redistribution in their coupling regions, which improved the electron conductivity and optimized the adsorption free energy of OER intermediates, ultimately boosting the intrinsic OER performance. Besides, the 3D hierarchical nanoarray structure facilitated the exposure of catalytically active centers and rapid electron/mass transfer during the OER process. As such, the CC/Co3O4@CoFe-LDH catalyst achieved excellent OER catalytic activity in alkaline medium, with a small overpotential of 237 mV at 10 mA cm-2, a low Tafel slope of 35.43 mV dec-1, and long-term durability of up to 48 h, significantly outperforming the commercial RuO2 catalyst. More impressively, the liquid and flexible solid-state ZABs assembled by the CC/Co3O4@CoFe-LDH hybrid catalyst as the OER catalyst presented a stable open circuit voltage, large power density, superb cycling life, and satisfactory flexibility, indicating great potential applications in energy technology. This work provides a good guidance for the development of advanced electrocatalysts with heterostructures and an in-depth understanding of electronic modulation at the heterogeneous interface.

Construction of 3D Hierarchical Co3O4@CoFe-LDH Heterostructures with Effective Interfacial Charge Redistribution for Rechargeable Liquid/Solid Zn-Air Batteries.

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Enabling efficient electrocatalytic conversion of N2 to NH3 by Ti3C2 MXene loaded with semi-metallic 1 T'-MoS2 nanosheets

Heterostructuring 2D TiO2 nanosheets in situ grown on Ti3C2T MXene to improve the electrocatalytic nitrogen reduction

P-band center theory guided activation of MoS2 basal S sites for pH-universal hydrogen evolution

Construction of 3D Hierarchical Co3O4@CoFe-LDH Heterostructures with Effective Interfacial Charge Redistribution for Rechargeable Liquid/Solid Zn-Air Batteries.