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Article Abstract
Activation and reduction of N to NH are a formidable challenge. While there have been several reports of metal complexes that can bind and activate N, very few catalysts have been reported to catalyze the electrochemical reduction of N to NH 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 N selectively by 6e/6H to NH using phenol as a proton source with a Faradaic yield of >80% at -2.3 V vs Fc in CHCN solvent. The selective 6e/6H reduction of N contrasts with a previous report of an analogous complex with propanethiolate ligands that could reduce N by 4e/4H to NH.
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