2026-04-13T07:21:18Zhttps://recercat.cat/oai/request

oai:recercat.cat:2072/4755672025-10-13T11:41:44Zcom_2072_98col_2072_378192

00925njm 22002777a 4500 dc Beiler, A.M. author Denisiuk, A. author Holub, J. author Sánchez-Baygual, F.J. author Gil-Sepulcre, M. author Ertem, Mehmed Z author Moonshiram, Dooshaye author Piccioni, A. author Llobet Dalmases, Antoni author 2023 Molecular catalysts can promote ammonia oxidation, providing mechanistic insights into the electrochemical N cycle for a carbon-free fuel economy. We report the ammonia oxidation activity of carbon anodes functionalized with the oligomer {[Ru(bda-κ-NO)(4,4'-bpy)](4,4'-bpy)}, Rubda-10, where bda is [2,2'-bipyridine]-6,6'-dicarboxylate and 4,4'-bpy is 4,4'-bipyridine. Electrocatalytic studies in propylene carbonate demonstrate that the Ru-based hybrid anode used in a 3-electrode configuration transforms NH to N and H in a 1:3 ratio with near-unity faradaic efficiency at an applied potential of 0.1 V vs Fc, reaching turnover numbers of 7500. X-ray absorption spectroscopic analysis after bulk electrolysis confirms the molecular integrity of the catalyst. Based on computational studies together with electrochemical evidence, ammonia nucleophilic attack is proposed as the primary pathway that leads to critical N-N bond formation. Ammonia Catalysts Electrodes Electrolysis Oligomers Heterogeneous Electrochemical Ammonia Oxidation with a Ru-bda Oligomer Anchored on Graphitic Electrodes via CH-π Interactions