Distinctive defects engineering in graphitic carbon nitride for greatly extended visible light photocatalytic hydrogen evolution

Defects modulation usually has great influence on the electronic structures and activities of photocatalysts. Here, porous structured graphitic carbon nitride materials with large amount of defects are obtained through facile 5 min thermal treatment in air without additional reactants. The resultant materials show remarkably extended light absorption in the visible light region. Theoretical calculations indicate that the distinctive origin of red-shifted intrinsic light absorption edge and newly occurred light absorption edge are attributed to cyano groups and nitrogen vacancies, respectively. Compared to pristine graphitic carbon nitride, the optimally modified material shows greatly enhanced photocatalytic hydrogen evolution rate by 21.5 times under lambda > 440 nm and the responsive wavelength is extended from 450 nm to 650 nm. This work is expected to provide guidance for rational design of graphitic carbon nitride and inspire similar attempts for the modification of nanomaterials.