Surface-mediated iron on porous cobalt oxide with high energy state for efficient water oxidation electrocatalysis

摘要

Surface engineering of active materials to generate desired energy state is critical to fabricate high-performance heterogeneous catalysts.However, its realization in a controllable level remains challenging. Using oxygen evolution reaction(OER) as a model reaction, we report a surface-mediated Fe deposition strategy to electronically tailor surface energy states of porous Co_(3)O_(4)(Fe-pCo_(3)O_(4)) for enhanced activity towards OER. The Fe-pCo_(3)O_(4) exhibits a low overpotential of 280 mV to reach an OER current density of 100 mA cm^(-2), and a fast-kinetic behavior with a low Tafel slop of 58.2 mV dec^(-1), outperforming Co_(3)O_(4)-based OER catalysts recently reported and also the noble IrO_(2). The engineered material retains 100% of its original activity after operating at an overpotential of 350 m V for 100 h. A combination of theoretical calculations and experimental results finds out that the surface doped Fe promotes a high energy state and desired coordination environment in the near surface region, which enables optimized OER intermediates binding and favorably changes the rate-determining step.