Computational calculations and experimental studies reveal that the CoOOH phase and the intermediate-spin (IS) state are the key factors for realizing efficient Co-based electrocatalysts for the oxygen evolution reaction (OER). However, according to thermodynamics, general cobalt oxide converts to the CoO2 phase under OER condition, retarding the OER kinetics. Herein, we demonstrate a simple and scalable strategy to fabricate electrodes with maintaining Fe-CoOOH phase and an IS state under the OER. The changes of phase and spin states were uncovered by combining in-situ/operando X-ray based absorption spectroscopy and Raman spectroscopy. Electrochemical reconstruction of chalcogenide treated Co foam affords a highly enlarged active surface that conferred excellent catalytic activity and stability in a large-scale water electrolyzer. Our findings are meaningful in that the calculated results were experimentally verified through the operando analyses. It also proposes a new strategy for electrode fabrication and confirms the importance of real active phases and spin states under a particular reaction condition.
© 2022. The Author(s).