Realizing high visible-light-induced carriers mobility in TiO2-based photoanodes

Abstract

Increasing the quantum conversion efficiency in visible-light region is a key issue for the efficient usage of solar energy in the process of photoelectrochemical (PEC) water splitting. Here, based on the N anion and S cation codoped TiO2 thin film photoanodes, we find experimentally and theoretically that the transport ability of visible-light-induced carriers can be notably enhanced by engineering the dopant electronic energy states. The hole transport resistivity is decreased from 6.8 × 104 to 1.3 × 104 Ω m via delocalizing the introduced bands, leading to an evident increase of the internal quantum efficiency from 5% to 20% at the visible-light region of 450–550 nm. Further DFT calculations exhibit that the split of the isolated band is induced by a strong N and S hybridization, which favors to decrease the hole effective mass and to improve the hole mobility by three times. The photocurrent of N − S codoped TiO2 thin film is thus twice that of monodoping cases, the best value for doping modified TiO2 thin film photoanodes. This work may provide not only a design principle but also a candidate for tailoring and optimizing TiO2 towards high PEC activity.