Ferro/Nonferroelectric Vertical Heterostructure Superlattice as a Visible-Light-Responsive Photocatalyst: A DFT Prediction.

Abstract

Developing narrow-band-gap ferroelectric semiconducting photocatalysts is a promising strategy for efficient photocatalytic water splitting with high energy conversion efficiency. Within this context, six ferro/nonferroelectric vertical heterostructure superlattices (VHSs) are constructed in this work by stacking ferroelectric SiS or GeS with nonferroelectric layered organic photocatalysts (C2N, g-C3N4, and melon), layer by layer. The geometry and electronic structures of these six VHSs are systematically investigated by density functional theory calculations. Consequently, four VHSs (SiS/g-C3N4, GeS/C2N, GeS/g-C3N4, and GeS/melon) are predicted to simultaneously possess several important and highly desirable features for photocatalytic water splitting, namely excellent visible-light adsorption, remarkable spontaneous polarization (0.49-0.70 C/m2), spatial charge separation, as well as suitable band-edge positions, thus serving as potential candidates for photocatalytic water splitting to produce hydrogen. This work not only provides a new strategy to use narrow-band-gap ferroelectric semiconductors for photocatalytic water splitting but also offers inspiration for developing photocatalysts with high energy conversion efficiency.