Unlocking Lattice Oxygen\non Selenide-Derived NiCoOOH\nfor Amine Electrooxidation and Efficient Hydrogen Production

In pursuit of advancing the electrooxidation\nof amines,\nwhich is\ntypically encumbered by the inertness of C(sp<sup>3</sup>)–H/N(sp<sup>3</sup>)–H bonds, our study introduces a high-performance\nelectrocatalyst that significantly enhances the production efficiency\nof vital chemicals and fuels. We propose a novel electrocatalytic\nstrategy employing a uniquely designed (Ni<sub><i>x</i></sub>Co<sub>1–<i>x</i></sub>)Se<sub>2</sub>-R electrocatalyst,\nwhich is activated through Se–O exchange and electron orbital\nspin manipulation. This catalyst efficiently generates M<sup>4+</sup> species, thus enabling the activation of lattice oxygen and streamlining\nthe electrooxidation of amines. Empirical evidence from isotope labeling,\nmolecular probes, and computational analyses indicates that the electrocatalyst\nfosters the formation of energetically favorable peroxy radical intermediates,\nwhich substantially expedite the reaction kinetics. The refined electrocatalyst\nachieves an exceptional current density of 20 mA cm<sup>–2</sup> at a potential of 1.315 V, with selectivity surpassing 99% for propionitrile,\nwhile demonstrating remarkable stability over 560 h. This work emphasizes\nthe criticality of deciphering the fundamental mechanisms of amine\nelectrooxidation and charts a more sustainable pathway for the nitrile\nand hydrogen production, marking a substantial advancement in the\nfield of electrocatalysis.