Tuning the Electronic Structure of a Novel 3D Architectured Co-N-C Aerogel to Enhance Oxygen Evolution Reaction Activity

Hydrogen generation through water electrolysis is an efficient technique for hydrogen production, but the expensive price and scarcity of noble metal electrocatalysts hinder its large-scale application. Herein, cobalt-anchored nitrogen-doped graphene aerogel electrocatalysts (Co-N-C) for oxygen evolution reaction (OER) are prepared by simple chemical reduction and vacuum freeze-drying. The Co (0.5 wt%)-N (1 wt%)-C aerogel electrocatalyst has an optimal overpotential (0.383 V at 10 mA/cm²), which is significantly superior to that of a series of M-N-C aerogel electrocatalysts prepared by a similar route (M = Mn, Fe, Ni, Pt, Au, etc.) and other Co-N-C electrocatalysts that have been reported. In addition, the Co-N-C aerogel electrocatalyst has a small Tafel slope (95 mV/dec), a large electrochemical surface area (9.52 cm²), and excellent stability. Notably, the overpotential of Co-N-C aerogel electrocatalyst at a current density of 20 mA/cm² is even superior to that of the commercial RuO₂. In addition, density functional theory (DFT) confirms that the metal activity trend is Co-N-C > Fe-N-C > Ni-N-C, which is consistent with the OER activity results. The resulting Co-N-C aerogels can be considered one of the most promising electrocatalysts for energy storage and energy saving due to their simple preparation route, abundant raw materials, and superior electrocatalytic performance.