A Hierarchical Z‑Scheme α‐Fe2O3/g‐C3N4 Hybrid for Enhanced Photocatalytic CO2 Reduction

Abstract

The challenge in the artificial photosynthesis of fossil resources from CO 2 by utilizing solar energy is to achieve stable photocatalysts with effective CO 2 adsorption capacity and high charge‐separation efficiency. A hierarchical direct Z‐scheme system consisting of urchin‐like hematite and carbon nitride provides an enhanced photocatalytic activity of reduction of CO 2 to CO, yielding a CO evolution rate of 27.2 µmol g−1 h−1 without cocatalyst and sacrifice reagent, which is >2.2 times higher than that produced by g‐C 3 N 4 alone (10.3 µmol g−1 h−1). The enhanced photocatalytic activity of the Z‐scheme hybrid material can be ascribed to its unique characteristics to accelerate the reduction process, including: (i) 3D hierarchical structure of urchin‐like hematite and preferable basic sites which promotes the CO 2 adsorption, and (ii) the unique Z‐scheme feature efficiently promotes the separation of the electron–hole pairs and enhances the reducibility of electrons in the conduction band of the g‐C 3 N 4. The origin of such an obvious advantage of the hierarchical Z‐scheme is not only explained based on the experimental data but also investigated by modeling CO 2 adsorption and CO adsorption on the three different atomic‐scale surfaces via density functional theory calculation. The study creates new opportunities for hierarchical hematite and other metal‐oxide‐based Z‐scheme system for solar fuel generation.