Wide-direct-band-gap monolayer carbon nitride CN2: a potential metal-free photocatalyst for overall water splitting.

Abstract

Two dimensional metal-free semiconductors with high work function have attracted extensive research interest in the field of photocatalytic water splitting. Herein, we have proposed a kind of highly stable monolayer carbon nitride CN2 with an anisotropic structure based on first principles density functional theory. The calculations of electronic structure properties, performed using the HSE06 functional, indicate that monolayer CN2 has a wide direct band gap of 2.836 eV and a high work function of 6.54 eV. And the suitable band edge alignment, high electron mobility (∼103 cm2 V-1 s-1) and visible-light optical absorption suggest that monolayer CN2 has potential on visible-light photocatalytic water splitting at pH ranging from 0 to 14. Moreover, we have observed that uniaxial strain can effectively control the electronic structure properties and optical absorption of monolayer CN2, which can further improve its solar to hydrogen efficiency from 9.6% to 16.02% under 5% uniaxial tension strain along the Y direction. Our calculations have not only proposed a new type of potential metal-free photocatalyst for water splitting but also provided a functional part with high work function for type-I and scheme-Z heterojunction applied in photocatalytic water splitting.