Micropore-Boosted Layered Double Hydroxide Catalysts: EIS Analysis in Structure and Activity for Effective Oxygen...

Since the oxygen evolution catalysis process is vital yet arduous in energy conversion and storage devices, it is highly desirous but extremely challenging to engineer earth-abundant, noble-metal-free nanomaterials with superior electrocatalytic activity toward effective oxygen evolution reactions (OERs). Herein, we construct a prismlike cobalt-iron layered double hydroxide (Co-Fe LDH) with a Co/Fe ratio of 3:1 utilizing a facile self-templated strategy. Instead of carbon-species-coupled treatment, we focus on ameliorating the intrinsic properties of LDHs as OER electrocatalysts accompanied by the hierarchical nanoflake shell, well-defined interior cavity, and numerous microporous defects. In contrary to conventional LDHs synthesized via a one-pot method, Co-Fe LDHs fabricated in this work possess a huge specific surface area up to 294.1 m² g^-1, which not only provides abundant active sites but also expedites the kinetics of the OER process. The as-prepared Co-Fe LDH electrocatalysts exhibit advanced electrocatalytic performance and a dramatic stability of the OER in an alkaline environment. In particular, the contribution of micropore defects is clearly discussed according to the electrochemical impedance spectroscopy analysis, in which the time constant of the OER at the micropore defect is several orders of magnitude smaller than that at the exterior of Co-Fe LDHs, forcefully verifying the intrinsic catalytic activity enhancement derived from the micropore defects. This work provides a promising model to improve OER electrocatalyst activity via produce defects and research the contribution of micropore defects.