Electrocatalytic Oxidative Dehydrogenation Of Benzylamine To Nitriles And Catalytic Mechanism Exploration

The oxygen evolution reaction(OER)is a crucial half-reaction that produces protons for electrochemical and photoelectrochemical water splitting,CO₂ reduction,and N₂ reduction.Unfortunately,the OER is a kinetically sluggish half-reaction owing to its four-proton and four-electron process.The development of highly efficient,robust,and cost-effective OER catalysts is one of the biggest challenges in this field.(1)Electrocatalytic water oxidation requires efficient catalysts to reduce the overpotential and accelerate the sluggish kinetics of oxygen formation.Here,NiFeBa trimetal material was prepared by the co-electrodeposition of Ba²⁺,Ni²⁺,and Fe³⁺as an efficient catalyst for electrocatalytic water oxidation.NiFeBa showed enhanced water oxidation performance compared with NiFelayered double hydroxide and NiFeoxide,delivering a current density of 10 m A cm^-2 at an overpotential of 180 m V.Doped Ba ions played a key role in stabilizing the electro-generated Ni³⁺species,producing more octahedral Ni-O structures for water oxidation,adjusting the catalytic mechanism,and finally leading to an enhancement of catalytic efficiency.(2)Inspired by the active Ni³⁺intermediates involved in electrocatalytic water oxidation by Ni-based materials,we prepared Ni(OH)₂ nanosheets as a catalyst and used water as the oxygen source for the oxygenations of various organics.The electrically driven Ni(OH)₂successfully realized the selective electrooxidation of aryl primary amines to the corresponding nitriles at the anode in an aqueous solution,with the conversions efficiencies and selectivity reached more than 98%.Ni²⁺/Ni³⁺can be used as the redox active substance for the conversion of aryl primary amines.