Constructing porous carbon nitride nanosheets for efficient visible-light-responsive photocatalytic hydrogen evolution.

The photocatalytic performance of polymeric carbon nitride (CN) is mainly restricted by the poor mass charge separation efficiency and poor light absorption due to its polymeric nature. The conventional strategies to address these problems involved constructing a nanosheets structure would result in a blue shifted light absorption and increased exciton binding energy. Here, with combination of ammonia etching and selectively hydrogen-bond breaking, holey carbon nitride nanosheets (hCNNS) were constructed, thus widening the light absorption range, and spontaneously shortening the migration distance of electrons and holes in the lateral and vertical directions, respectively. Further analysis also found out the reserved atomic structure order endowed hCNNS with the relatively high redox potential. When irradiated with visible light (λ > 420 nm) and loaded with 3 wt% Pt as the cocatalyst, the hydrogen evolution rate of hCNNS was about 40 times higher than the bulk CN, and the apparent quantum yield (AQY) of hCNNS is 1.47% at 435 ± 15 nm. We expect this research can provide a new sight for achieving highly efficient solar utilization of CN-based photocatalysts.