Enhanced light harvesting and charge separation of carbon and oxygen co-doped carbon nitride as excellent photocatalyst for hydrogen evolution reaction.

ABSTRACT

Solar-driven water splitting has been regarded as a promising strategy for renewable hydrogen production. Among many semiconductor photocatalysts, graphitic carbon nitride (g-C3N4) has received tremendous attention due to its two-dimensional structure, appropriate band gap and decent photocatalytic activity. However, it suffers severe charge recombination problems, affecting its practical performance. In this work, we demonstrated that dual heteroatoms (C and O) doped g-C3N4 can exhibit about 3 times higher catalytic performance for hydrogen evolution than that of the normal g-C3N4 with a hydrogen evolution rate reaching 2595.4 umol g-1h-1 and an apparent quantum efficiency at 420 nm of 16.6%. The heteroatoms (C and O) doped g-C3N4 photocatalyst also exhibited superior removal performance when removing Rhodamine B (RhB) . X-ray photoelectron spectroscopy (XPS), solid-state nuclear magnetic resonance (ssNMR) and X-ray absorption near-edge structure (XANES) spectroscopy reveal that the carbon and oxygen dopants replace the sp2 nitrogen and bridging N atom, respectively. DFT calculations demonstrate the codoping of carbon and oxygen- induced the generation of mid-gap state, leading to the improvement of light harvesting and charge separation.