Single Unit Cell Bismuth Tungstate Layers Realizing Robust Solar CO₂ Reduction to Methanol.

Liang, Liang; Lei, Fengcai; Gao, Shan; Sun, Yongfu; Jiao, Xingchen; Wu, Ju; Qamar, Shaista; Xie, Yi

Solar CO2 reduction into hydrocarbons helps to solve the global warming and energy crisis. However, conventional semiconductors usually suffer from low photoactivity and poor photostability. Here, atomically-thin oxide-based semiconductors are proposed as excellent platforms to overcome this drawback. As a prototype, single-unit-cell Bi2WO6 layers are first synthesized by virtue of a lamellar Bi-oleate intermediate. The single-unit-cell thickness allows 3-times larger CO2 adsorption capacity and higher photoabsorption than bulk Bi2WO6. Also, the increased conductivity, verified by density functional theory calculations and temperature-dependent resistivities, favors fast carrier transport. The carrier lifetime increased from 14.7 to 83.2 ns, revealed by time-resolved fluorescence spectroscopy, which accounts for the improved electron-hole separation efficacy. As a result, the single-unit-cell Bi2WO6 layers achieve a methanol formation rate of 75 µmol g-1 h-1, 125-times higher than that of bulk Bi2WO6. The catalytic activity of the single-unit-cell layers proceeds without deactivation even after 2 days. This work will shed light on designing efficient and robust photoreduction CO2 catalysts.

CARBON dioxide reduction; BISMUTH compounds; CHEMICAL synthesis; METHANOL; TUNGSTATES; PHOTOREDUCTION; DENSITY functional theory

Angewandte Chemie International Edition, 2015, Vol 54, Issue 47, p13971

1433-7851

Academic Journal

10.1002/anie.201506966