Photocatalytic
lignocellulose-to-H2 conversion is highly
attractive but remains a huge challenge due to the absence of efficient
photocatalysts. Herein we report the use ultrathin anatase TiO2 nanosheets with a thickness of 2.1 nm and 94.5% exposed (001)
facets (TiO2-1) as highly active photocatalysts for photocatalytic
lignocellulose-to-H2 conversion. The ultrathin structure
of TiO2 not only provides abundant active sites for the
photocatalytic H2 production reaction but also benefits
photogenerated charge transfer to the surface. Furthermore, as proven
by theoretical calculations and fluorescence experiments, the ●OH radicals acting as the key species for the oxidation
of lignocelluloses can be easily generated on the (001) facets owing
to the low activating energy for the ●OH generation
reaction. Notably, the highest photocatalytic H2 generation
rates of 275 and 26 μmol·h–1·g–1 were achieved, respectively, in 250 mL of 4g·L–1 α-cellulose solution and poplar wood chip aqueous
solution consisting of 100 mg of 1.0% Pt-loaded TiO2-1
photocatalyst, and an apparent quantum yield of 1.89% at 380 nm was
achieved in α-cellulose aqueous solution. The photocatalytic
H2 production activity of TiO2-1 is about 2.4
and 2.1 times higher than that of reference TiO2 nanosheets
(TiO2-2) in α-cellulose solution and poplar wood
chip solution, respectively. Our findings demonstrate the feasibility
of establishing rapid ●OH generation to boost the
oxidation of lignocelluloses and to enhance lignocellulose-to-H2 conversion.