Visible-Light-Driven Photocatalytic Dehydrogenation of Alcohols on TiO2 via Ligand-to-Metal Charge Transfer for Coproduction of H2 and Aldehydes

Developing visible-light-driven photocatalysts for thecatalyticdehydrogenation of organics is of great significance for sustainablesolar energy utilization. Here, we first report that aromatic alcoholscould be efficiently split into H-2 and aldehydes over TiO2 under visible-light irradiation through a ligand-to-metalcharge transfer (LMCT) mechanism. A series of TiO2 catalystswith different surface contents of the hydroxyl group (-OH)have been synthesized by controlling the hydrothermal and calcinationsynthesis methods. An optimal H-2 production rate of 18.6 & mu;mol h(-1) is obtained on TiO2 synthesizedfrom the hydrothermal method with a high content of surface -OH.Experimental characterizations and comparison studies reveal thatthe surface -OH markedly influences the formation of LMCT complexesand thus changes the visible-light-driven photocatalytic performance.This work is anticipated to inspire further research endeavors inthe design and fabrication of visible-light-driven photocatalyst systemsbased on the LMCT mechanism to realize the simultaneous synthesisof clean fuel and fine chemicals.

Automated summary

In this study, visible-light-driven photocatalysts based on the ligand-to-metal charge transfer (LMCT) mechanism were developed to efficiently split aromatic alcohols into H-2 and aldehydes over TiO2. TiO2 catalysts with different surface contents of -OH were synthesized using hydrothermal and calcination synthesis methods. Experimental characterizations revealed that the surface -OH significantly influenced the formation of LMCT complexes and thus the photocatalytic performance. This work is expected to inspire further research on the design and fabrication of visible-light-driven photocatalyst systems for the simultaneous synthesis of clean fuel and fine chemicals.