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This work demonstrates a nickel-based catalyst achieving >80% Faradaic yield for ammonia from nitrogen, indicating potential for efficient nitrogen reduction.
Activation and reduction of N2 to NH3 are a formidable challenge. While there have been several reports of metal complexes that can bind and activate N2, very few catalysts have been reported to catalyze the electrochemical reduction of N2 to NH3 selectively, under ambient conditions, and with reasonable yields. A trinuclear Ni complex with a bulky thiolate ligand and a boat-shaped cavity is synthesized and characterized. This complex can electrocatalytically reduce N2 selectively by 6e-/6H+ to NH3 using phenol as a proton source with a Faradaic yield of >80% at -2.3 V vs Fc+/0 in CH3CN solvent. The selective 6e-/6H+ reduction of N2 contrasts with a previous report of an analogous complex with propanethiolate ligands that could reduce N2 by 4e-/4H+ to N2H4.
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Das et al. (2025) studied this question.
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