Two-dimensional Confined Topotactic Transformation to Produce Co-Pi/Co3O4 Hybrid Porous Nanosheets for Promoted Water Oxidation

Exploring advanced electrocatalyst for the oxygen evolution reaction (OER) is of great importance in pursuing efficient and sustainable hydrogen production via electrolytic water splitting. Considering the structure-activity-stability relationship for designing advanced OER catalysts, two-dimensional (2D) porous catalyst with single crystallinity is deemed to be an ideal platform which could simultaneously endow enriched active sites, facile mass and charge transport ability as well as robust structural stability. Herein, we proposed a facile 2D confined topotactic phase transformation approach, which realizes the fabrication of highly porous single-crystalline Co3O4 nanosheets with in-situ surface modification of amorphous Co-Pi active species. Benefitted from the highly exposed undercoordinated cobalt sites, facilitated mass transport and facile 2D charge transfer pathway, the Co-Pi/Co3O4 hybrid porous nanosheets display enhanced OER activity with obvious pre-oxidation-induced activation. In addition, the operational stability was significantly improved owing to the strengthened structural stability which effectively buffers the internal strains and avoids the structural collapse during the electrochemical process. This work proposed a facile and mild method for the synthesis of amorphous/single-crystalline hybrid porous materials, and the achievement of synergistic modulation of active site density and charge transfer ability via targeted microstructural construction will shed light on catalyst design in the future.