Porous Cobalt Oxynitride Nanosheets for Efficient Electrocatalytic Water Oxidation

Exploring efficient and cheap oxygen evolution reaction (OER) electrocatalysts is of great significance for electrochemical water splitting. Herein, we successfully prepared an efficient ternary electrocatalyst of porous cobalt oxynitride (Co3OxNy) nanosheets by a simple nitridation strategy. Specifically, CoONPNS-400 (cobalt oxynitride with porous nanosheet structure obtained at 400(degrees)C) offered a low OER overpotential of 0.23V to achieve the catalytic current density of 10 mA cm(-2) and a small Tafel slope of 48m V dec(-1) in alkali media, outperforming most of the first-row transition-metal-based OER electrocatalysts. The calculated density of states (DOS) analysis and electron spin resonance (ESR) measurements revealed that the introduction of foreign N atoms into pristine Co3O4 nanosheets can optimize the electronic structure and create more oxygen vacancies, thus leading to enhanced electrical conductivity. Density functional theory (DFT) calculations demonstrated that the foreign N atoms can also improve the energetics for OER by modulating the free energy for adsorbed intermediates (OOH*, OH*, O*), further improving the OER electrocatalytic activity of CoON PNS-400. This work provides a possibility for rationally designing ternary transition-metal compounds as advanced OER electrocatalysts.