Rational Design of Cobalt–Iron Selenides for Highly Efficient Electrochemical Water Oxidation

Exploring active, stable, earth-abundant, low-cost, and high-efficiency electrocatalysts is highly desired for large-scale industrial applications toward the low-carbon economy. In this study, we apply a versatile selenizing technology to synthesize Se-enriched Co1–xFexSe2 catalysts on nickel foams for oxygen evolution reactions (OERs) and disclose the relationship between the electronic structures of Co1–xFexSe2 (via regulating the atom ratio of Co/Fe) and their OER performance. Owing to the fact that the electron configuration of the Co1–xFexSe2 compounds can be tuned by the incorporated Fe species (electron transfer and lattice distortion), the catalytic activity can be adjusted according to the Co/Fe ratios in the catalyst. Moreover, the morphology of Co1–xFexSe2 is also verified to strongly depend on the Co/Fe ratios, and the thinner Co0.4Fe0.6Se2 nanosheets are obtained upon selenization treatment, in which it allows more active sites to be exposed to the electrolyte, in turn promoting the OER performance. The Co0.4Fe0.6Se2 nanosheets not only exhibit superior OER performance with a low overpotential of 217 mV at 10 mA cm–2 and a small Tafel slope of 41 mV dec–1 but also possess ultrahigh durability with a dinky degeneration of 4.4% even after 72 h fierce water oxidation test in alkaline solution, which outperforms the commercial RuO2 catalyst. As expected, the Co0.4Fe0.6Se2 nanosheets have shown great prospects for practical applications toward water oxidation.